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OBERLIN COLLEGE Precision Spectroscopy of Atomic Lithium by Donal Sheets in the lab of Jason Stalnaker Department of Physics April 2015 Abstract The atomic structure of lithium has aroused a significant amount theoretical and experimental interest as a system in which precision atomic calculations and spectroscopic measurements can be combined to yield scientifically significant results. While there have been many experimental investigations of Li spectroscopy, particularly of the isotope shift between 6 Li and 7 Li as well as the hyperfine structure of the 2 S1/2 →2 P1/2,3/2 (D1, D2) transitions, they suffer from significant disagreements and systematic effects. By utilizing the optical-to-microwave frequency conversion made possible by a stabilized optical frequency comb, we will be able to measure the optical frequencies of the D1 and D2 transitions and resolve the discrepancies. This experiment investigates the D1 and D2 transitions by probing an atomic beam with a single mode extended cavity diode laser at approximately 671 nm. The difficulty in this experiment comes from precisely measuring the frequency of this probe laser. This is accomplished by referencing our diode laser to an optical frequency comb which acts as an optical to microwave synthesizer allowing the precise measure of optical frequencies referenced to an SI time standard. The optical frequency comb is generated by a Ti:Sapphire pulsed laser which which is broadened to span an optical octave using microstructure fiber. The frequency comb is referenced to a GPS steered Rubidium atomic clock. This system we can measure optical frequencies with a accuracy of 1 × 10−12 . This work reports on the progress made on the experiment. In particular, we discuss improvements to the system and the evaluation of the systematics associated with the measurements. Systematics associated with the alignment of the beam, Zeeman shift, and ac Stark shift have been evaluated and we have set upper limits on their effects on the measurement. Measurements of absolute frequencies of the D1 transition as well as isotope shift and hyperfine splitting measurements are also presented. Acknowledgements First and foremost I would like to thank my advisor Jason Stalnaker. His support, encouragement, and dedication have made this work possible. As a never ending source of knowledge I am grateful for the opportunity to have worked with and learned from him. I would like to thank my lab mate Peter Elgee for his company, insight, and support. I would also like to acknowledge the previous students that have worked no this and related projects. This work could not have been possible with out the contributions from but not limited to Mike Rowan, Jacob Baron, Sophia Chen, José Almaguer, and Sean Bernfeld. The information contained in their thesis was also a great resource throughout the project. I would also like to thank my friends and fellow physics majors for their company and support throughout my time at Oberlin. Lastly I would like to thank my family for their never ending support and understanding. ii Contents Abstract i Acknowledgements ii List of Figures vi List of Tables viii 1 Introduction 1.1 Lithium . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1.2 Previous Measurments . . . . . . . . . . . . . . . . . . . . . . . . . 1.3 Measuring Optical Frequencies . . . . . . . . . . . . . . . . . . . . . 2 Background Theory 2.1 Notation . . . . . . . . . . . . . . . . . . . . . 2.2 Atomic Theory . . . . . . . . . . . . . . . . . 2.2.1 Hydrogen Atom . . . . . . . . . . . . . 2.2.1.1 Quantum Defect . . . . . . . 2.2.1.2 Central-Field Approximation 2.2.2 Isotope Shifts . . . . . . . . . . . . . . 2.2.3 Fine Structure . . . . . . . . . . . . . . 2.2.4 Hyperfine Structure . . . . . . . . . . . 2.2.5 Quadrupole Interaction . . . . . . . . . 2.3 Multi-Electron Atoms . . . . . . . . . . . . . . 2.4 Precision Spectroscopy: Fields and Atoms . . 2.4.1 Quantization of Electromagnetic Fields 2.4.2 Interaction of Light with Atoms . . . . 2.4.3 Emmission . . . . . . . . . . . . . . . . 2.4.4 Absorption . . . . . . . . . . . . . . . 2.4.5 Saturation . . . . . . . . . . . . . . . . 2.4.6 Zeeman Effect . . . . . . . . . . . . . . 2.5 Wigner-Eckart Theorem . . . . . . . . . . . . 2.6 Relative Transition Strengths . . . . . . . . . iii . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1 1 1 3 6 6 7 7 9 10 11 14 17 19 20 21 21 23 23 26 27 29 30 31 Contents 2.7 iv 2.6.1 AC Stark Effect . . . . . . . . . . . . . . . . . . . . . . . . . 33 Doppler Shift . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37 3 Frequency Comb 3.1 Overview . . . . . . . . . . . . . 3.2 Dispersion . . . . . . . . . . . . 3.3 Kerr Lens Modulation . . . . . 3.4 Oscillator Cavity . . . . . . . . 3.4.1 Pump Laser . . . . . . . 3.4.2 Oscillator Cavity . . . . 3.4.3 Lasing and Modelocking 3.4.4 Microstructure Fiber . . 3.5 Stabilization . . . . . . . . . . . 3.5.1 Repetition Rate . . . . . 3.5.2 Offset Frequency . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4 Experimental Setup 4.1 Diode laser . . . . . . . . . . . . . . . . 4.1.1 Diode Laser Theory . . . . . . . . 4.1.2 Diode Laser Experimental Setup 4.1.3 Frequency Stabilization . . . . . . 4.1.4 Fabry-Perot Interferometer . . . . 4.1.5 Optical Spectrum Analyser . . . . 4.1.6 Power Stabilization . . . . . . . . 4.1.7 Electro-Optic Modulators . . . . 4.2 Atomic Beam . . . . . . . . . . . . . . . 4.3 Vacuum System . . . . . . . . . . . . . . 4.3.1 Interaction Region . . . . . . . . 4.3.2 Ion Pump . . . . . . . . . . . . . 4.3.3 Helmholtz Coils . . . . . . . . . . 4.4 Data Aquisition . . . . . . . . . . . . . . 4.5 Collection Procedure . . . . . . . . . . . 5 Analysis and Results 5.1 Analysis . . . . . . . . . . . . . . . . 5.2 Test of Frequency Standard . . . . . 5.3 Test of locks . . . . . . . . . . . . . . 5.4 Magnetic Field Evaluation . . . . . . 5.5 Evaluation of Probe Beam Alignment 5.5.1 Correction of Misalignment . 5.6 AC Stark Measurement . . . . . . . . 5.7 Isotope Shift and Hyperfine Structure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . Splitting . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40 41 42 44 45 45 45 48 49 50 50 50 . . . . . . . . . . . . . . . 55 56 56 57 60 62 64 65 66 68 71 72 73 75 77 77 . . . . . . . . 79 79 81 83 84 86 89 92 92 6 Conclusions 99 6.1 Improvements to Apparatus . . . . . . . . . . . . . . . . . . . . . . 99 Contents 6.2 6.3 v AC Stark Measurement . . . . . . . . . . . . . . . . . . . . . . . . . 100 Finalize Uncertainties . . . . . . . . . . . . . . . . . . . . . . . . . . 100 Bibliography 102 List of Figures 1.1 1.2 1.3 Energy Levels of Lithium . . . . . . . . . . . . . . . . . . . . . . . . Previous Measurements of Lithium fine structure splitting and isotope shifts for the D1 and D2 transitions. . . . . . . . . . . . . . . . Output Spectrum of Optical Frequency Comb . . . . . . . . . . . . 2.1 2.2 2.3 Fine Structure of 6 Li and 7 Li . . . . . . . . . . . . . . . . . . . . . . 12 Saturation Curves . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28 Doppler Broadening . . . . . . . . . . . . . . . . . . . . . . . . . . . 38 3.1 3.2 3.3 3.4 3.5 3.6 3.7 3.8 3.9 Pulse Generation . . . . . . . Kerr Lensing . . . . . . . . . Oscillator Cavity . . . . . . . Chirped Mirror . . . . . . . . Crystal Holder . . . . . . . . Microstructure Fiber . . . . . Microstructure Fiber Pictures Diagram of frep stabilization. Diagram of f0 stabilization. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41 44 46 46 47 48 49 51 54 4.1 4.2 4.3 4.4 4.5 4.6 4.7 4.8 4.9 4.10 4.11 4.12 4.13 4.14 4.15 4.16 4.17 Experimental Setup Block Diagram . . . . . . . . . . . . . . Extended Cavity Diode laser configurations . . . . . . . . . Picture of ECDL Cavity . . . . . . . . . . . . . . . . . . . . Power vs Current Plot for Diode Laser . . . . . . . . . . . . Block Diagram for ECDL Optics . . . . . . . . . . . . . . . Block Diagram of f0 stabilization. . . . . . . . . . . . . . . Confocal and Planar Fabry-Perot Cavity . . . . . . . . . . . Fabry-Perot peaks for scan of ECDL . . . . . . . . . . . . . Response of Electro-optic modulator to applied electric field. Diagram of Power Stabilization Optics . . . . . . . . . . . . Diagram of Electrooptic Modulator . . . . . . . . . . . . . . Lithium Vapor Density vs Temperature . . . . . . . . . . . . Lithium Oven . . . . . . . . . . . . . . . . . . . . . . . . . . Atomic Beam . . . . . . . . . . . . . . . . . . . . . . . . . . Comparison of Atomic Beams . . . . . . . . . . . . . . . . . Interaction Region . . . . . . . . . . . . . . . . . . . . . . . Vacuum Chamber Picture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 55 56 58 59 60 61 63 64 65 66 67 68 69 70 71 72 73 . . . . . . . . . vi . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2 3 4 List of Figures vii 4.18 Vacuum System . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 74 4.19 Ion Pump . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75 4.20 Helmholtz Coils . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76 5.1 5.2 5.3 5.4 5.5 5.6 5.7 5.8 5.9 5.10 5.11 Comparison of Data with different atomic beams Comparisons of Frequency Standard . . . . . . . . Magnetic Field Calibration . . . . . . . . . . . . . Magnetic Field Correction . . . . . . . . . . . . . Saturation dip from retro-reflected probe beam . Saturation Data . . . . . . . . . . . . . . . . . . . Line shape model data . . . . . . . . . . . . . . . Data fit to interpolated line shape . . . . . . . . . 7 Li D1 F = 1 → F 0 transitions . . . . . . . . . . . 7 Li D1 F = 2 → F 0 transitions . . . . . . . . . . . 6 Li D1 transitions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 80 82 84 85 87 88 90 91 96 97 98 List of Tables 2.1 2.2 2.3 Quantum Numbers . . . . . . . . . . . . . . . . . . . . . . . . . . . 7 Relative transition Amplitudes . . . . . . . . . . . . . . . . . . . . . 33 Estimated AC Stark Shifts . . . . . . . . . . . . . . . . . . . . . . . 37 4.1 Conversion from applied current to magnetic field at interaction region. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76 5.1 5.2 5.3 5.4 5.5 5.6 5.7 Correction Current for Magnetic Fields Magnetic Field Comparison . . . . . . Estimated AC Stark Shifts . . . . . . . Optical Frequencies . . . . . . . . . . . Measurement Uncertainty Budget . . . Isotope Shift Frequencies . . . . . . . . Hyperfine Splitting . . . . . . . . . . . viii . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 85 86 92 93 93 94 95 Chapter 1 Introduction 1.1 Lithium Spectroscopy of atomic lithium has gained renewed interested as a system for testing atomic theory of few electron systems as well as insight into the charge radii of the nuclei [7] [8] [9] [10]. This has prompted a need of precision measurements of fine structure intervals and isotope shifts. As a three electron atom with two stable isotopes, 6 Li and 7 Li, measurements of the isotope shift, fine structure splitting, and hyperfine structure splitting provide a window for information on charge radii of the nucleus, magnetic dipole distribution of the nucleus, and nuclear structure. 1.2 Previous Measurments While there have been several published high precision measurements of the D1 (22 S1/2 → 22 P1/2 ) and D2 (22 S1/2 → 22 P3/2 ) transitions (Fig. 1.1) there is still significant discrepancy between the published results. The current theory predictions are also more precise then the experimental limit for the isotope shift. As shown in Fig. 1.2 the discrepancy between the two most recent measurements of the isotope shift is several times their combined uncertainties for both the isotope shift and 7 Li fine structure measurements. The data presented by Brown et al [1] and Sansonetti et al. [2] is the same data present with different analysis based on the evaluation of systematics in the system. The two most recent independent measurement are presented by Sansonetti et al. [2] and Das et al. [3]. 1 Introduction 2 4d 4d 4s 3p 3p 3d 3d 3s 2p 2p 2s 2S 1/2 2PO 1/2 2P O 3/2 2D 3/2 2D 5/2 Figure 1.1: Energy levels of Lithium. This experiment is focused on measuring the 2 S1/2 →2 P1/2 (D1) and 2 S1/2 →2 P3/2 (D2) transitions in both 6 Li and 7 Li. The approximate transitions wavelengths are given for each transition. The disagreement in the D2 measurements can be partially attributed to a lack of resolution between peaks, making line shape models difficult. When multiple resonance are separated by less then the natural line width of the transition, 6 MHz for Lithium, there is a possibility for interference in the fluorescence leading to more complex line shapes that depend on the geometry of the experiment. This was addressed by Sansonetti et al.[2] who investigated the effect of probe laser polarization relative to detection angle on line shape as well as the effect of quantum interference on atomic spectra [11]. This effect is not present in the D1 lines and there persists significant disagreements so more investigation is still needed in order to resolve the discrepancy. The absolute frequency measurements of the transitions also have significant disagreements. Since these disagreements appear as linear shifts in the optical frequencies, the isotope shift measurement has less uncertainty as it is a relative frequency between two optical transitions. Introduction 3 7 Fine Structure of Li 6 Fine Structure of Li (g) (a) (a) (b) (b) (c) (c) (e) (d) (d) (e) (f) -0.8 -0.6 -0.4 -0.2 0.0 0.2 -1.2 Deviation from Weighted Mean of Measurements (MHz) -1.0 -0.8 -0.6 -0.4 -0.2 0.0 0.2 Deviation from Weighted Mean of Measurements (MHz) 7 6 Isotope Shift between Li and Li for the D1 Transition (a) (b) (e) (d) 0.0 0.1 0.2 0.3 0.4 0.5 Deviation from Weighted Mean of Measurements (MHz) Figure 1.2: Previous Measurements of Lithium fine structure splitting and isotope shifts for the D1 and D2 transitions. The red points are experimental results and the purple are theory calculations. There is clear disagreement between the experimental results as well as between experimental measurements and theory predictions. Points (a) and (b) are publications of the same data with different analysis techniques. (a) Brown PRA 87, 032504 (2013)[1] (b) Sansonetti PRL 107, 023001 (2011)[2] (c) Das PRA 75, 052508 (2007)[3] (d) Noble PRA 74, 012502 (2006)[4] (e) Walls EPJD 22, 159 (2003)[5] (f) Orth ZPA 273, 221 (1975)[6] (g) Puchalski PRL 113, 073004 (2014)[7] 1.3 Measuring Optical Frequencies The precision measurement of atomic transition frequencies relies on the ability to determine optical frequencies of hundreds of THz and reference the frequencies to the SI second. These measurements have long been a difficult task because the frequencies are so large. Earlier techniques including harmonic frequency chains,while Introduction 4 Ι νn = n frep + f0 f0 0 ν frep Figure 1.3: The optical frequency comb acts as a microwave to optical frequency synthesizer. The output frequency spectrum is a series of evenly spaced comb modes, each of which can be defined by two microwave frequencies f0 and frep as well as a mode number. accurate, only allowed the measurement of limited frequencies and were difficult to use. This experiment uses an optical frequency comb which acts as an optical to microwave synthesizer, allowing the measurement of optical frequencies in terms of two microwave frequencies (Chapter 3). A frequency comb is a light source that has a frequency spectrum consisting of a series of discrete lines with a regular spacing. This spacing is defined as the repetition rate of the optical frequency comb and it is dependent on the cavity length of the oscillator. The entire mode structure is offset by offset frequency. If the output of the comb spans an optical octave these two frequencies can be measured and stabilized. From this we can determine the frequency of any mode of the comb νn = nfrep + f0 , (1.1) where n is a integer mode number, frep is the repetition rate of the comb, and f0 is the offset frequency. This ruled output is shown in Fig. 1.3. Both the offset frequency and repetition rate are microwave frequencies which can easily be measured to high accuracy [12]. This gives a consistent and relatively easy method of measuring optical frequencies in terms of the SI second. This experiment probes atomic lithium using an extended cavity diode laser locked to the optical frequency comb. Atoms from a collimated atomic beam are excited by tuning the frequency of the probe laser across the transition frequencies. The fluorescence is then recorded using a photomultiplier tube. We have improved the stability of the extended cavity diode laser as well as collimated our atomic beam Theory 5 (Chapter 4). With this system we have established preliminary error bounds on the systematics and present optical frequencies for the D1 transitions, isotope shift and hyperfine splittings. Chapter 2 Background Theory 2.1 Notation When referring to the energy state of an atom we use the term notation 2S+1 LJ , (2.1) where S is the spin quantum number, L is the the orbital angular momentum quantum number, and J = L + S is the total electronic angular momentum. These values are capitalized as they are the totals for the system not the state of one electron. Since we are mainly concerned with lithium, a three electron atom, we will use this notation. The allowed values of J are given by |L − S| < J < L + S, (2.2) where all integer steps between are also allowed. The intrinsic angular momentum or nuclear spin is represented by I. Protons and neutrons are fermions and so have an intrinsic spin of 1/2, this means that nuclei of odd mass number will have half integer spin. The total momentum of the atom is given by F and is the combination of the nuclear spin I and the total angular momentum J. When considering a one-electron atom, each state can be defined by four quantum numbers n l j M where n is the principle quantum number, l the orbital angular 6 Theory 7 Quantum Number Desciption n Principal Quantum Number Spin Angular Momentum S Spin Quantum Number MS L Orbital Angular Momentum I Nuclear spin ~ +S ~ J Total Electron Angular Momentum: J~ = L F Total Atomic Angular Momentum F~ = I~ + J~ Table 2.1: Table of quantum numbers. moment, j the total momentum, and mj is the projection of the angular momentum. The n quantum number is used to refer to the shell that the electron resides in. For each n there are n2 orbitals. 2.2 Atomic Theory 2.2.1 Hydrogen Atom To start we will look at the simplest atom, Hydrogen which consists of a heavy proton of charge +e and a significantly lighter electron with charge −e. The proton is assumed to motionless. Starting with Schrödinger’s equation in spherical coordinates ~2 1 d 1 d δψ 1 d δ2ψ 2 δψ − r + 2 sin θ ++ 2 2 sin θ 2 +V ψ = Eψ. 2m r2 dr δr r sin θ dθ δθ δφ r sin θ dφ (2.3) Here V is the potential energy and E is the total energy and m is the mass of the electron. We can look for solutions using separation of variables in the form ψ(r, θ, φ) = Rl (r)Yl,m (θ, φ), (2.4) where Rl (r) is the radial portion and Yl,m (θ, φ) is the spherical harmonic. It can then be shown that the radial portion of Eq. (2.3) must be equal to a constant which is defined as l(l + 1). 1 d 2mr2 2 dR r − 2 [V (r) − E] = l(l + 1). R dr dr ~ (2.5) Theory 8 Here the potential energy of the configuration is given by Coulomb’s law V (r) = − e2 1 . 4πo r (2.6) To simplify this further we define u(r) = rR(r) ~2 d2 u ~2 l(l + 1) e2 1 u(r)E = − + u(r) + − 2m dr2 4πo r 2m r2 (2.7) We now need to solve this for u(r) and determine the allowed energies. To simplify Eq. (2.7) we divide through by E and make the following substitutions r ρ= −2mr2 E me2 and ρ = 0 ~2 2πo ~2 ρ (2.8) giving d2 u ρ0 l(l + 1) = 1− + u(r). dρ2 ρ ρ2 (2.9) We can now look at solutions of the form uρ = Ae−ρ + Beρ . (2.10) We start by looking at the boundary condition ρ → inf, we see that eρ blows up at infinity so we set B = 0. As ρ → 0 Eq. 2.9 is dominated by the centrifugal term l(l + 1) d2 u = u(r), dρ2 ρ2 (2.11) which leads to solutions of the form u(ρ) = Cρl+1 + Dρ−l . (2.12) As ρ → inf, ρ−l blows up and so we set D = 0 and look for solutions of the form u(ρ) = ρl+1 e−ρ X cj ρ j . (2.13) j We find that the eigenvalues of Eq. (2.9) are given by ρ0 = 2n, (2.14) Theory 9 where n is an integer. Therefore the allowed energies are 2 2 e 1 m E1 En = − = , 2~2 4πo n2 n2 2.2.1.1 n = 1, 2, 3, 4... (2.15) Quantum Defect The hydrogen system is a reasonable model for lithium as like any alkali atom lithium has one valence electron and then completely filled inner shells. These inner shells are extremely stable and so the excitation spectra are due to the transitions in the outer electron. This inner shell causes a shielding effect such that the outer electron does not see the complete charge of the nucleus and so it is more likely to be excited into a higher energy level as the binding energy is less. For this model the potential seen by the valence electron is no longer of the Coulomb form used above. When considering the potential for lithium at large distances from the nucleus the potential is simply the Coulomb potential but near the nucleus the shielding does not play a role V (r) → −e2 4π0 r −Ze2 4π0 r r→∞ . r→0 Therefore the further the electron is from the nucleus the closer to the field is to that of hydrogen. The energy levels of any alkali atom can be described by Enl = − Ry n2∗ (2.16) where Ry is the Rydberg energy and n∗ is the effective principal quantum number. This can be represented by n∗ = n − ∆l , (2.17) where ∆l is the quantum defect. The quantum defect is simply an angular momentum (l) dependent correction to the energy levels due to incomplete shielding of the nuclear charges by the inner electron shell. For small values of l this has a larger effect as the valence electron is closer to the nucleus and so sees more of the charge. This shift removes the degeneracy found in the hydrogen atom as it is only dependent on l not n. For lithium in the 2s, (l = 1) state the quantum defect is found to be .41 [13]. This lowers the ionization energy for lithium in comparison to hydrogen for low l states. Theory 2.2.1.2 10 Central-Field Approximation In the previous section we approximated the correction to the energy levels of lithium by considering the valence electron orbiting a shielded core. This approach only addressed the energy of the valence electron. Now we need to look at the energy due to all electrons in the atom. This approximation adds the correction due to the electrostatic interactions between the electrons. As long as the inner shell remains closed there is no angular momentum coupling as the inner shell has zero total angular momentum. This leads to a solution which is composed of a product of one-electron states. Given a system of three electrons, the Hamiltonian assuming Coulomb potential is given by H= 3 X i=1 3 X ~2 2 Ze2 e2 − ∇ − + . 2m i 4π0 ri 4π0 rij j>i (2.18) Here the first term is the kinetic energy of each electron, the second is the potential due to the interaction of each electron with the nucleus, and the third is the repulsion between electrons. The distance between each electron is given by rij . Next we make the assumption that the repulsion between the electrons is radially symmetric as the interaction between the inner shell, a spherical charge distribution, and valence electron is spherically symmetric. This allows the potential energy to be expressed such that it is only dependent on r and we assume a central potential S(r). VCF (r) = − Ze2 + S(r). 4π0 r (2.19) Under this approximation, the Hamiltonian for the system can then be expressed as HCF = 3 X i=1 ~2 2 − ∇ + VCF (ri ) . 2m i (2.20) From this form of the Hamiltonian the wave function can be separated into one part for each electron ψatom = ψ1 ψ2 ψ3 leaving three equations of the form ~2 2 − ∇ + VCF ψi = Eψi . 2m (2.21) From this we look for solutions of the form ψi = R(ri )Γl,m . (2.22) Theory 11 Again assuming that the potential is spherically symmetric we are left with ~2 d2 ~2 l(l + 1) − R(r) = ER(r). + VCF (r) + 2m dr2 2mr2 (2.23) This leads to a similar conclusion in the last section, where the energy is given by ECF = Zef f e 4π0 r2 (2.24) We can place limits on Zef f although it is difficult to calculate. Once again as r → 0 then Z= 3 and as r → ∞, Z = 1. For a derivation and more information see Ref. [14]. 2.2.2 Isotope Shifts Changes in mass of an atom from changes in neutron number yield different isotopes of the same element with a corresponding shift in energy levels. Lithium has two stable isotopes 6 Li and 7 Li, where 7 Li has an abundant of 92.5% and 6 Li at 7.6%. The energy shift is caused by both a change in mass of the nucleus as well as the distribution of charge within the nucleus know as the volume effect. The mass shift is the dominant contributor to the isotope shift in light atoms but decreases with mass number by A−2 . The volume shift is 10,000 times smaller in this isotope shift but increases as Z 2 A−1/3 and so is dominant in heavier atoms [15]. If we start by looking at a single-electron atom, hydrogen, the energy levels are given by: En = Where a0 = 4π0 ~2 µe2 e2 1 4π0 a0 n2 n = 1, 2, 3, 4, ... (2.25) and we have assumed the mass of the proton to be much greater then the electron and so set µ = me . If we assume that the mass of the nucleus is not infinite then we can replace the electron mass with the reduced mass µ: µ= me M A me + M A (2.26) where me is the mass of the electron, M is the nucleon mass, and A is the atomic number. We can then say that since any energy level is proportional to this mass, Theory 12 2.83 MHz 2p 2P3/2 F=0 2p 2P3/2 F=1 5.89 MHz 2p 2P3/2 F=2 9.39 MHz 2p 2P3/2 F=3 10 534.194 MHz 10 053.184 MHz 2p 2P1/2 F=2 2p 2P3/2 F=1/2 1.71 MHz 2p 2P3/2 F=3/2 92.03 MHz 2.91 MHz 2p 2P 3/2 F=5/2 10 534.039 MHz 2p 2P1/2 F=1 10 052.76 MHz 2p 2P1/2 F=3/2 26.063 MHz 2p 2P1/2 F=1/2 2s 2S1/2 F=2 2s 2S1/2 F=3/2 228.205 259 MHz 803.504 086 MHz 2s 2S1/2 F=1/2 6Li 7Li 2s 2S1/2 F=1 Figure 2.1: Fine structure for lithium D1 and D2 of 6 Li and 7 Li. the energy levels shift due to changes in the atomic mass. For two isotopes of mass number A and A + ∆N the frequency is shifted by ∆ω = ω0 m m − + M A + M ∆N MA (2.27) where w0 is the frequency of the transition. For this experiment we are considering transitions around 670nm and ∆N = 1 this results in a normal mass shift of ∼ 5 GHz. There is also a specific mass shift that is on the same order as the normal Theory 13 mass shift but this is more difficult to calculate [13],[14]. When a system contains more then two particles, the center of mass of the system is no longer the same as the center of mass between a particular electron and the nucleus. This means the interaction can no longer be treated as center of mass motion. This correction is referred to as the specific mass shift. The volume shift is due to a change in the distribution of charge in a finite volume. Since the protons and neutrons are distributed within the nucleus we cannot assume that the electrostatic potential has the 1/r dependence of a point charge. To estimate this effect, assume the that the change is evenly distributed in a sphere of radius R given by R = r0 A1/3 (2.28) where r0 is defined to be 1.2 × 10−15 m. This model gives a potential given by V (r) = Ze2 (4π0 )2R − r2 R2 −3 r<R (2.29) Ze2 (4π0 )r R < r. Now we can use this as a perturbation to the Hamiltonian with potential given by the Coulomb potential such that the correction to the Hamiltonian is the difference between the Coulomb potential and the model. H0 = Ze2 (4π0 )2R r2 R2 + 2R r −3 r<R 0 . (2.30) R<r The energy shift to first order is found using the expectation value of the Hamiltonian ∆E = hψ|H 0 |ψi. (2.31) This is found to be [16] ∆E = Z 5 e2 4R ∆R, 4π0 5a3µ n3 (2.32) where aµ = a0 (m/µ) and δR is the difference in radius between the two isotopes. For the D1 and D2 lines the total isotope shift between 6 Li and 7 Li is about 10.5 GHz as shown in Fig. 2.1. Theory 2.2.3 14 Fine Structure The fine structure splitting of energy levels is due to the addition of magnetic interactions and relativistic corrections in the kinetic energy of the Hamiltonian. ~ that results in a magnetic The electron can have an orbital angular momentum L, dipole moment, µ ~ . The electron also has an intrinsic magnetic moment µ ~ S = g~µB S. The coupling between these magnetic moments leads to the fine structure splitting. In Section 2.2.1 the energy levels of hydrogen are shown to be 2 2 m e 1 E1 En = − = , 2~2 4πo n2 n2 n = 1, 2, 3, 4... (2.33) were the Hamiltonian was taken to be H=− e2 1 ~2 2 ∇ − . 2m 4π0 r (2.34) This was derived using the classical expression for kinetic energy. To understand the relativistic corrections we use the relativistic expression for kinetic energy mc2 T =p − mc2 2 1 − (v/c) (2.35) mv . p= p 1 − (v/c)2 (2.36) and relativistic momentum The first term in the kinetic energy expression is the total relativistic energy due to the motion and the second term is the rest energy. We can now express the kinetic energy in terms of the relativistic momentum to get T = p p2 c2 + m2 c4 − mc2 . (2.37) We then Taylor expand this for small values of p/mc and get r p 2 1 p 2 1 p 4 2 T = mc 1 + ( ) − 1 = mc 1 + ( ) − ( ) ... − 1 mc 2 mc 8 mc 2 T = p2 p4 − + ... 2m 8m3 c2 (2.38) (2.39) The first term is the nonrelativistic kinetic energy and the second is the relativistic correction to lowest order. From this the relativistic correction to the En can be Theory 15 calculated to be Er1 4n (En )2 −3 =− 2mc2 l + 1/2 (2.40) where l is the orbital angular momentum quantum number [17]. Note that the relativistic correction is 2 × 105 smaller then En and that it will be a negative shift in energy. Now to look at the spin-orbit coupling from the magnetic dipole moment of the electron. When considering the electron’s rest frame the proton orbits around it ~ This field creates a torque on the electron which tries creating a magnetic field B. to align the magnetic moment of the electron µ with the field. The Hamiltonian of this configuration is given by ~ H = −~µ · B. (2.41) From here we need to find the magnetic field created by the proton and the magnetic dipole moment of the electron. The magnetic dipole moment of electron can be found by considering a charge spinning with angular momentum from its spin S. If we look at the configuration using classical electrodynamics and assume that a charge q is distributed around a ring of radius r rotating with period τ , the magnetic dipole moment of the configuration is qπr2 τ µ= (2.42) as the current in the ring is q/T and the area of the ring is πr2 . The angular momentum, again found classically is given by the moment of inertia of the ring, mr2 , times the angular velocity 2π/τ . 2πmr2 S= τ (2.43) q S. 2m (2.44) This classical derivation yields µ= However this is slightly off, in reality the magnetic moment is µe = e S. m (2.45) Theory 16 This factor of two is known as the g factor of the electron and was explained by Dirac [18]. To find the magnetic field due to the relative motion of the proton we consider the reference frame of the electron and treat the proton as a continuous charge loop with current e/τ . The period can be found by looking at the orbital angular momentum L = rmv = 2πmr2 . τ Thus the magnetic field is given by e ~ ~ = µ0 I = 1 B L. 2r 4π0 mc2 r3 (2.46) We can now go back to our Hamiltonian H = −µ · B = e2 1 ~ ~ S · L. 2 4π0 m c2 r3 (2.47) This calculation assumes that the electron’s frame is an inertial frame, however it is an accelerating frame and so an additional correction known as the Thomas precession factor [17] must be added, this adds a factor of 1/2 yielding ~ = Hso = −~µ · B 1 ~ ~ e2 S · L. 2 8π0 m c2 r3 (2.48) ~ and L, ~ this It is important to not that the Hso depends on the orientation of S causes a splitting in states that would be degenerate without this interaction. The ~ + S. ~ We simplify Eq. 2.48 using the total angular momentum is defined as J~ = L following identity ~ ·S ~ J 2 = L2 + S 2 + 2L (2.49) ~ ·S ~ = 1 (J 2 − L2 − S 2 ). L 2 (2.50) The eigenvalues of L · S are given by ~2 [J(J + 1) − L(L + 1) − S(S + 1)]. 2 (2.51) l From this we can find the correction to the energy Eso given by l Eso = hHso i = e2 1 2 8π0 m c2 r3 ~2 [J(J 2 + 1) − L(L + 1) − S(S + 1)] . L(L + 1/2)(L + 1)n3 a3 (2.52) Theory 17 By adding Eq. 2.52 and Eq. 2.40 we find the total shift to be Efl s En2 4n = 3− . 2mc2 J + 1/2 (2.53) Here both corrections although stemming from completely different effects happen to be on the scale of 2 En . 2mc2 Adding this correction to the original Bohr formula, the energy levels with the fine structure correction can be expressed as Enj E1 3 α n =− 2 1+ 2 − . n n J + 1/2 4 (2.54) Where α is the fine structure constant. For lithium, all of the states are doublets except the 2 S states which does not split. The allowed J are therefore J = L ± 1/2 [19]. This gives the degeneracy in the transition 2 S1/2 →2 P1/2,3/2 which are the D1 and D2 transitions we are interested in measuring. 2.2.4 Hyperfine Structure The hyperfine structure splitting occurs because like the electron the proton and neutron have an intrinsic magnetic dipole moment. The reason this effect is so much smaller then the fine structure splitting is that the mass of the proton is much greater. For the proton the magnetic moment is given by µp = gp e Sp , 2mp (2.55) where gp is the g-factor of the proton which is measured as 5.59 [17]. The proton has a much more complex structure because it is made of three quarks and so the gyromagnetic ratio is not as easily calculated. In classical electrodynamics the magnetic field from a dipole is given by B= 2µ0 3 µ0 3(~ µ · r̂)r̂ − µ ~ + µ ~ δ (r), 4πr3 3 (2.56) where δ 3 is the three dimensional the delta function which is is 0 everywhere except for (0, 0, 0) where it is one, see Ref. [20] in depth derivation of the field of a dipole. Theory 18 The Hamiltonian for the electron in the magnetic field of the nucleus is then given by 0 Hhf ~ 3(I · r̂)(J~ · r̂) − I~ · J~ µ0 gp e2 ~ ~ 3 µ0 gp e2 + = µe · B = J · Iδ (r). 4πr2 mp me r3 3mp me (2.57) To find the first order correction to the energy we find the expectation value of the Hamiltonian given by 0 Ehf = 0 hHhf i ~ µ0 gp e2 ~ ~ µ0 gp e2 3(I · r̂)(J~ · r̂) + J · I |ψ(0)|2 = 2 3 4πr mp me r 3mp me (2.58) For the ground state the wave function is spherically symmetric and so the expectation value of first term in the the Hamiltonian is zero. For (l=0) it is found that the expectation value of the wave function is |ψ100 (0)|2 = 1 πa3 (2.59) as found in Ref. [17]. From this we can plug in to find the energy correction 0 Ehf = µ0 gp e 2 J · I . 3mp me a3 (2.60) This is known as the spin-spin coupling term because of the dependance on the dot product of the spin of the the proton and electron. We can define the total spin as F = J + I and then find J · I by squaring and simplifying to get 1 J~ · I~ = [F 2 − J~2 − I~2 ] 2 (2.61) For Hydrogen since S for both the proton and electron are 1/2 and there are two possible states with spins aligned or anti aligned the value for the total spin can be 0 or 1. These are the singlet or triplet states respectively. Thus the possible values of J · I are J ·I = ~2 Triplet, F = 1 −3~2 Singlet, F = 0 4 4 To find the shift due to the hyperfine splitting the triplet state is shifted up and the singlet is shifted down. Theory 2.2.5 19 Quadrupole Interaction The other important characteristic when considering the structure of the nucleus is the electric quadrupole moment. Since the nucleus has only positve charge it does not have a electric dipole moment due to symmetry under time reversal however if it is not spherically symmetric there is a quadrupole term. The Hamiltonian for the interaction between a proton at r~p and and electron at r~e is given by H0 = − e2 , 4π0 |~ re − r~p | (2.62) where the position is taken from the center of mass of the nucleus. We can assume that re >rp and so we will Taylor expand Eq. (2.62) in terms off rp /re . This gives the interaction Hamiltonian to be rp2 e2 1 rp 0 H =− P0 (cos θ) + 2 P1 (cos θ) + 3 , P2 (cos θ) 4π0 re re re (2.63) where θ is the angle between re an rp and Pi is the Legendre polynomial. The first term in this series is the monopole moment given by the Coulomb potential. If we sum over all protons we see that the interaction between the nucleus and electron is given by 0 Hmono Ze2 1 =− . 4π0 re (2.64) The second term is nuclear dipole interaction, which is zero due to the reversal invariance. The last term is the electric quadruple interaction which is a combination of the nuclear electric quadruple moment and electric field gradient tensor. This can be simplified to give the nuclear quadrupole moment Q as [21] X 2 Q = hI, MI = I| Q02 (pj )|I, MI = Ii, e j (2.65) where Qi2 is the electric quadrupole tensor and is summed over all protons. We can then define the average field gradient at the nucleus as δ 2 Ve δz 2 = X 2 JMJ = J F0 (ei )JMJ = J , (2.66) i where the sum is over the valence electrons.We can now combine the quadruple moment and the average electric field gradient to show that the electric quadrupole Theory 20 interaction Hamiltonian is [21] Hquad = where BJ ~ 2 + 3 (I~ · J) ~ − I(I + 1)J(J + 1)], [3(I~ · J) 2I(2I − 1)J(2J − 1) 2 δ 2 Ve BJ = eQ δz 2 (2.67) (2.68) is the electric quadrupole interaction coefficient. The energy shift due to the quadruple interaction is then given by 0 ∆E = hψ|Hquad |ψi = BJ K(K + 1) − I(I + 1)J(J + 1) , 8 I(2I − 1)J(2J − 1) (2.69) where K = F (F + 1) − I(I + 1) − J(J + 1). (2.70) For excited states where the electron charge distribution is spherically symmetric the electric field gradient at the nucleus vanishes and so there is not quadrupole shift. Thus p states do exhibit the shift and s states do not. 2.3 Multi-Electron Atoms The theory in the previous sections was all derived using hydrogen as the model atom which only has one electron except for the quadrupole moment which is not present in hydrogen. While this may not seem like the most useful in understanding lithium which has three electrons there are many similarity which make the hydrogen atom a reasonable starting point. When considering lithium we know as an alkali metal that it consists of a filled shell plus one valence electron. For this experiment we are only looking at transitions from the ground state of lithium to the 2 P1/2 and 2 P3/2 states which have S = 1/2 and L = 1. These states exhibit similar characteristics to the corresponding states in the hydrogen atom. Theory 2.4 2.4.1 21 Precision Spectroscopy: Fields and Atoms Quantization of Electromagnetic Fields ~ r, t) in the coloumb gauge with no Consider a field given by a vector potential A(~ free currents or charges. Thus we can set the scaler potential equal to zero. Using ~ satisfies the wave equation Maxwells equations we find that A ~− ∇2 A ~ 1 ∂ 2A = 0. c2 ∂t2 (2.71) Lets now consider a single mode of light as a plane wave with polarization ˆ. Normalizing the potential to a box with volume V in order to deal with the infinite extent of a plane wave, the general solution to the wave equation is given by 1 ik·r ∗ ∗ −ik·r ~ r, t) = √ C(t)ˆe + C (t)ˆ e A(~ , V (2.72) C(t) = C0 e−iωt . (2.73) where We know that the energy of an electromagnetic wave is given by 1 E= 8π Z ε2 + B 2 dV (2.74) V and the electric and magnetic fields can be related to the vector potential by ~ 1 ∂A iω ik·r ∗ ∗ −ik·r ε= = √ C(t)ˆe − C (t)ˆ e c ∂t c V (2.75) i ik·r ∗ ∗ −ik·r ~ ×A ~ = √ C(t)(~k × ˆ)e − C (t)(~k · ˆ e B=∇ V (2.76) Plugging these back into our energy equation we find that E= 2 1 ω 2 . C(t) 2P i c2 (2.77) Breaking E into its complex and imaginary components E= 2 1 ω 2 + Im C(t) 2 ). Re C(t) 2P c2 (2.78) Theory 22 Now lets consider the Hamiltonian for a classical simple harmonic oscillator Hsho = p2 mω 2 2 + x 2m 2 (2.79) where x is the position and p is the momentum of the particle. In order rearrange H to make it of a similar form to Eq. 2.78 we will make the variable substitution √ p = mωP and x = √X . This gives mω Hsho = We also know that p = dx m dt or ωP = ω 2 (X + P 2 ). 2 dX dt (2.80) and we can define P (t) and X(t) to be X(t) = C0 cos ωt (2.81) P (t) = −C0 sin ωt (2.82) which is the same as the real and imaginary parts of C(t) as defined by Eq. 2.73. Now we can define C(t) in terms of P and X giving r C(t) = πc2 X + iP ). ω (2.83) Putting this together with the Hamiltonian for the simple harmonic oscillator we can find the Hamiltonian for a electromagnetic wave in terms of X and P. Hem = ω 2 X + P 2) 2 (2.84) This is the Hamiltonian of a single mode of the electromagnetic field. As usual the energy eigenstates of the simple harmonic oscillator have energies 1 En = ~ω(n + ). 2 (2.85) Since each photon has energy ~ω the number of photons in a given mode of the light field is given by En /~ω. This also shows the existence of a zero point energy ~ω/2 for a mode with no photons. Theory 23 2.4.2 Interaction of Light with Atoms 2.4.3 Emmission This section will derive the emission rate of an atom from an initial sate |ii to a final state |f i. To start we look at Fermi’s Golden Rule which gives a differential transition rate of an atom in an external field from a initial state i to final state f . dWf i = 2π |hf |H 0 |ii|2 ρ(E)P (E)dE. ~ (2.86) Here ρ(E) is the density of states or number of final states for a given energy. P (E) is the distribution of energies which will be derived below. The density of states refers to both the photon state, as derived in the previous section as well as the atomic state. To find this density consider the incident light with polarization ˆ with wave vector ~k. For a given slice of volume the number of photon states is given by dN = 1 d3 xd3 p (2π)3 ~3 (2.87) If we integrate over some volume V and substitute p~ = ~~k we get dN = V k 2 dk dΩ, (2π)3 (2.88) where dΩ is the the differential solid angle for the emission of the photons. We can then substitute k = ω/c = E/(~c) giving dN = V E 2 dE dΩ. (2π)3 ~3 c3 (2.89) Now to find ρ(E) we simply want the number of photon states for a change in energy dE so ρ(E) = dN V E2 = dΩ. dE (2π)3 ~3 c3 (2.90) The next step is to find the distribution of energies which will allow the transition to occur. Here we will assume that there is no line broadening other then the Theory 24 natural line width given by the lifetime of the transition 1/γ, where γ is the spontaneous emission rate. Spontaneous emission is the process where an atom decays without being triggered by an external field. For this process if the atom is originally in an excited state it will naturally decay to a lower energy state and so emit a photon with energy equal to the decay gap. This experiment detects the fluorescence due to spontaneous emission. Since the excited state has a lifetime this results in a natural broadening of spectral peaks given by the Heisenberg uncertainty principle. ∆E ∆T = ~ . 2 (2.91) The average lifetime of the the D1 and D2 lines is 27 ns giving a natural line width of 6 MHz. In order for spontaneous emission to occur both the atomic levels and the electromagnetic field must be quantized. From this uncertainty in the energy, the decay is then given by a Lorentzian distribution P (ω) = γ/(2π) . (ω − ω0 )2 + (γ/2)2 (2.92) Here γ is the width of P (ω), as γ → 0 the with of the P (ω) tends to zero and the amplitude given by (2/(πγ)) goes to infinity. This leads to P (ω) → δ(ω − ω0 ) as γ → 0. More intuitively as the line width goes to zero the only way for excitation to occur is through an energy exactly equal to the transition. Plugging Eq. (2.90) and Eq. (2.92) back into Eq. (2.86) and substituting in terms of energy dWf i = 2π |hf |H 0 |ii|2 ρ(E)δ(~ω0 − E)dE. ~ (2.93) We can then integrate over the photon energies and get Wf i = 2π ~|hf |H 0 |ii|2 ρ(~ω0 ). ~ (2.94) To find the matrix element hf |H 0 |ii we need to find the Hamiltonian for an electron in an electric field given by H = H0 + H 0 where H0 is the the unperturbed Hamiltonian for the electron and H 0 is the perturbation due to the electric field. Theory 25 For a one electron atom the Hamiltonian is given by H= p2 Ze2 − 2m r (2.95) and the perturbation due to the electric field is H0 = e ~ p~ · A. mc (2.96) Here the binding energy between the nucleus and the electron is much stronger then the the force due to the electric field and so we can treat the electric field as a perturbation, for a formal proof see Ref. [22]. As stated before it is important to consider the state of both the incident light and the atom as |ii and |f i describe the combined state. In order to find the Hamiltonian for the entire system, we must consider the electric field state as well as the atomic state given by 2.96. Htotal = H0 + H 0 + Hem (2.97) The meaning of this Hamiltonian can be thought of as the unperturbed state of both the atom and the electric filed plus a cross term which describes their interaction. We can now solve for the emission rate by plugging in the total Hamiltonian and solving for the matrix elements. This derivation is done in detail in Ref. [22] and gives the rate for spontaneous emission for any incident polarization is given by γ= 4ω03 |hg, J|d|e, J 0 i|2 . 3~c3 2J 0 + 1 (2.98) Stimulated emission occurs when an atom is already in an excited state E2 . This process requires an incident photon with an energy equal to the energy gap between this higher energy state and some lower state E1 . The incident photon can stimulate the upper level atom causing it to decay and emit a second photon with the same energy. Theory 2.4.4 26 Absorption This section will use the notation and derivation in the previous two sections to derive the absorption rate for a transition. Here we consider an atom in the ground state with an incident field. When matter is irradiated with a photon there is a probability that an atom will absorb the photon and transition to a higher energy level. For this to occur the quantum energy of the photon must match the energy gap between the initial energy of the atom and some final state. If there is no such level then the matter will not absorb the light and so be transparent to the radiation. We will assume the incident photon is of a single mode and that we are only considering one allowed transition. Again we start with Fermi’s Golden Rule dWf i = 2π |hf |H 0 |ii|2 ρ(E)P (E)dE. ~ (2.99) To find the absorption rate for we substitute the resonance amplitude (2/~πγ) into Eq. (2.99) to find Weg = 4 |hf |H 0 |ii|2 . 2 γ~ (2.100) where the initial and final states are given by |ii = |g, F, MF i|ni (2.101) |f i = |e, F 0 , MF0 i|n − 1i. (2.102) and Where n is the number of photons in the resonant mode of the incident light. We now need to find the number of photons in mode n to the electric field amplitude ε0 . The intensity of the light is given by the time averaged magnitude of the pointing vector. I= cε20 8π (2.103) For a given flux of photons nc/V with energy ~ω the intensity can be expressed as I= n ~ωc V (2.104) n= V ε20 . 8π~ω (2.105) and so solving for n we find Theory 27 The matrix element can found in terms of the electric field and the rate of absorption is given by Weg = 2.4.5 1 |he, F 0 MF0 |d~ |g, F, MF i|2 ε20 γ ~2 (2.106) Saturation Considering an atom in a two level system with an incident electric field, if the incident field is strong enough the field will perturb the properties of the atoms. This causes the system to exhibit different characteristics based on the perturbation of the the population of states. The parameter which characterizes this perturbation is the saturation parameter κ given by [22] κ= excitation rate . relaxation rate (2.107) For a two level system the excitation rate is given by Γ= d2 ε20 , γ0 (2.108) where d is the dipole matrix element, ε0 is the amplitude of the incident field, and γ0 is the spontaneous decay rate. For this system the only contribution to the relaxation rate is the spontaneous decay rate and so the saturation parameter is given by [22] κ= Γ d 2 ε2 = 20 γ0 γ0 (2.109) To find the fluoresence intensity we look at the number of atoms in both the excited state Ne and ground state Ng . These can be described by the rate equations dNg = −ΓNg + (γ0 + Γ)Ne dt (2.110) dNe = ΓNg − (γ0 + Γ)Ne . dt (2.111) and In equilibrium it is found that the total number of atoms in the excited state is given by Ne = κ Ntot , 1 + 2κ (2.112) Theory 28 Amplitude Saturation Parameter — .1 —1 — 10 800 600 400 200 -4 2 -2 4 Detuning (MHz) Figure 2.2: Line shape of atomic transition for different saturation parameters. As the saturation parameter increases the width of the peak broadens as more atoms are in the excited state. where Ntot is the total number of atoms in the system. Since the intensity of the fluorescence is proportional to the number of atoms in the upper state we see a dependance on the line shape due to the strength of the incident electric field. When tuning a laser across a transition from the ground to an excited state the detuning dependent saturation parameter is given by γ02 /4 κef f (∆) = κ 2 ∆ + γ02 /4 (2.113) where κ is the on resonance saturation parameter [22]. By substituting the effective saturation parameter into the rate equations we can find the intensity as a function of probe detuning from resonance given by I(∆) ∝ γ0 Ne = κ(∆) γ02 /4 Ntot = κNtot 2 . 1 + 2κ(∆) ∆ + (1 + κ)γ02 /4 (2.114) This give a Lorentzian profile with width given by √ γ = γ0 1 + κ. (2.115) When tuning a laser over a transition where the value of κ is small, the line shape Theory 29 is given by a Lorentzian with width γ0 . For large values of κ we see a broadened line shape as shown in Fig. 2.2. This is known as the power-broadened line shape. 2.4.6 Zeeman Effect The Zeeman effect is the splitting of spectral lines into several components in the presence of a static magnetic field. In the presence a magnetic field the magnetic moment of the atom shifts in energy and so there is a shift in the overall energy. The treatment of the Zeeman effect is dependent on the strength of the external field in comparison with the internal field associated with the spin orbit coupling. If the external field is less then the internal then the internal field dominates and the external field can be treated as a small perturbation to the Hamiltonian. If the external field is much larger then the Zeeman effect dominates and the spin orbit field becomes the perturbation. For a single electron the perturbation to the Hamiltonian is given by a sum of the electronic and nuclear components ~ ~ ~ ext , H = − gJ µB J + +gI µN I · B 0 (2.116) where gJ is the Lande g factor. For Bext << Bint the hyperfine coupling dominates with the good quantum numbers N, F, J, I. The Zeeman correction to the the energy levels is E 0 = hN F JI|H 0 |N F JIi = e ~ Bext · hJ~ + Ii 2m (2.117) To find the expectation value of J~ + I~ is not quite as simple as only F~ is conserved. ~ which we know to be constant we are left only needing By plugging in F~ = J~ + I, ~ The time average of I~ is simply its projection to find the expectation value of I. along F~ . I~ · F~ ~ I~ave = F F2 (2.118) Theory 30 From this it can be found that the expectation value of J~ + I~ is given by ~ ~ ~ · I~ F · J F ~ = hJ~ + Ii + F~ F2 F2 F (F + 1) + J(J + 1) − I(I − 1) F (F + 1) − J(J + 1) + I(I + 1) ~ + hF i = 2F (F + 1) 2F (F + 1) (2.119) as derived in Ref. [17]. Here the square bracketed term is the Lande g-factor, gj . Finally the energy correction is E0 = e~ gF Bext MF , 2m (2.120) where gF = gJ F (F + 1) + J(J + 1) − I(I − 1) me F (F + 1) − J(J + 1) + I(I − 1) − gI . 2F (F + 1) M 2F (F + 1) (2.121) Here we are choosing the z axis to lie along the external field and so MF can be F, F − 1, ... − F . 2.5 Wigner-Eckart Theorem In atomic physics many calculations require the calculation of matrix elements of tensor operators with respect to an angular momentum basis. The Wigner-Eckart theorem is useful because it states that the matrix elements of an irreducible spherical tensor operator Tqκ can be expressed as [19] F 0 −MF0 hγ 0 F 0 MF0 |Tqκ |γF MF i = (−1) hγ 0 F 0 ||T κ ||γF i F0 −MF0 κ F ! q MF , (2.122) where γ refers to any other quantum numbers that define the state, hγ 0 F 0 ||T κ ||γF i is the reduced matrix element which is independent of MF , MF0 , and q. The term on the right hand side of the equation in parentheses is the Wigner 3-j symbol which can be related to the Clebsch-Gordan coeffients by the following [22] J1 J2 J M1 M2 M ! = (−1)J1 −J2 −M √ 1 hJ1 M1 J2 M2 |J − M i. 2J + 1 (2.123) Theory 31 Here the Clebsch-Gordon coefficients are real and so the 3-j symbol is also real. For this experiment we are interested in calculating the transition strengths which are ˆ This is the electric dipole moment depended on the transition dipole operator, d. associated with the transition between states |ii and |ji. This is defined as dˆ = dx x̂ + dy ŷ + dz ẑ (2.124) in Cartesian coordinates. The direction of this vector gives the polarization of the transition and how it will interact with a external field. To use the Wigner-Eckart Theorem we need to transform this into the spherical basis defined as 1 ê1 = − √ (x̂ + iŷ) 2 ê0 = ẑ (2.125) 1 ê−1 = √ (x̂ − iŷ), 2 giving 1 d1 = − √ (dx + idy ) 2 d0 = dz 1 d−1 = √ (dx − idy ). 2 (2.126) We have now expressed the dipole operator as an irreducible spherical tensor operator. In the next section we use this to find the relative strengths of different transitions. 2.6 Relative Transition Strengths This section derives the relative strength of transitions for lithium D1 and D2 lines. In general the transition from a ground state |gi = |γ S L I J F MF i to and excited state |ei = |γ 0 S 0 L0 I 0 J 0 F 0 MF0 i is determine by Fermi’s Golden Rule as given by Eq. (2.100) which requires the calculation of he|H 0 |gi. Here the Hamiltonian is simply the dipole matrix operator dˆ defined in the previous section. To find the relative transition amplitude we can simplify this matrix element by applying the Theory 32 Wigner-Eckart theorem. hγ 0 S 0 L0 I 0 J 0 F 0 MF0 |dq |γ S L I J F MF i = (−1)F −MF hγ 0 S 0 L0 I 0 J 0 F 0 ||d||γ S L I J F i ! F0 1 F × . −MF0 q MF (2.127) We now want to decouple the angular momentum components. This can be done by either applying the Wigner-Eckart theorem twice and recombining or using the relation [19], hn0 I 0 J 0 F 0 ||d||n I J F i = (−1)J+1+F +I hn0 J 0 |d|n Ji ( ) 0 0 0 p J F I . × (2F + 1)(2F 0 + 1) F J 1 (2.128) The bracketed term is the Wigner 6j symbol. We can apply this to Eq. (2.127) to to reduce the |J I F i to |Ji and get hγ 0 S 0 L0 I 0 J 0 F 0 ||d||γ S L I J F i = (−1)J+1+F +I hγ 0 S 0 L0 J 0 ||d||γ S L Ji ( ) 0 0 p J F I × (2F + 1)(2F 0 + 1) . F J 1 (2.129) By applying this relation a second time we are left with 0 hγ 0 S 0 L0 I 0 J 0 |dq |γ S L I Ji = (−1)L+S +J+1 hγ 0 L0 |dq |γ Li ( ) 0 0 0 p L J S × (2J + 1)(2J 0 + 1) . J L 1 (2.130) This leaves the only matrix element depend on the overall quantum number n and the orbital quantum number L. Plugging the matrix elements back in we are left with 0 hγ 0 S 0 L0 I 0 J 0 F 0 MF0 |dq |γ S L I J F MF i = (−1)2+2J+S +L+2F +I+MF hγ 0 L0 |dq |γ Li p p × (2J + 1)(2J 0 + 1) (2F + 1)(2F 0 + 1) ( )( ) ! L0 J 0 S 0 J0 F 0 I F0 1 F . J L 1 F J 1 −MF0 q MF (2.131) Theory 33 For both the D1 and D2 transitions all of the hyperfine levels have the same L and n and so this term cancels when looking at relative amplitudes. We also can say that S = S 0 and I = I 0 and so the transition rate is given by ( × L0 J Wge ∝ (2J + 1)(2J 0 + 1)(2F + 1)(2F 0 + 1) )2 ( )2 !2 J 0 S0 J0 F 0 I F0 1 F . L 1 F J 1 −MF0 q MF (2.132) This equation can then be used to calculate the relative amplitudes of different transitions. The atoms in this system behave according to the Boltzmann distribution and so all the group states will be evenly populated. This means that the F states will not be equal because of the difference in degeneracies for the different states, to account for this there is an extra factor of (2F + 1) in Eq. (2.132) which cancels the term from the denominator of Eq. (2.127). This equation is trivial to solve using the built in 3j and 6j symbols in Mathmatica to find that the normalized relative transition amplitudes for the D1 lines are shown in Table 2.2. F 2 2 1 1 7 Li 6 Li 3/2 3/2 1/2 1/2 F0 2 1 2 1 Amplitude .37 .37 .22 .05 3/2 1/2 3/2 1/2 .44 .36 .18 .02 Table 2.2: Relative amplitudes for transitions from ground state for D1 transitions. These values align with the expectation that transitions with higher values of F should have greater transition amplitudes. For more in-depth derivations and more more information see Refs. [19] and [23]. 2.6.1 AC Stark Effect The Stark effect is the shift in the spectral lines of atoms in an electric field. When a time varying electric field is applied to an atom the energy levels will be split Theory 34 and shifted as the field polarizes the atom. This derivation will follow that of Ref. [22] looking at the case of the electric field being near the resonance frequency of the atoms. This will use the rotating wave approximation to find the energy level splittings. We will start with a two level atom with energy seperation ω0 . The atom is subject to at time varying electric field given by ε0 sin(ωt) and the states are coupled through the electric dipole operator d~ = −hi|ε0 z|f i, (2.133) where z is the quantization axis. The Hamiltonian for this system is given by H= 0 −dε sin(ωt) −dε sin(ωm t) ~ω0 ! . (2.134) In order to find the shift due to the applied electric field we will look at the system using the rotating wave approximation by making a unitary transformation [22] . U= 1 0 0 e−iωm t ! . (2.135) and so the Hamiltonian becomes H 0 = U † HU. (2.136) The states of the atom are also transformed by |ψ 0 i = U † |ψi. (2.137) In order to transform our standard time dependent Schrodinger Equation to this basis we multiply both sides by U † and utilize the fact that U † U = 1 to transfer bases. ∂ |ψi ∂t ∂ U † HU U † |ψi = iU † U U † |ψi ∂t H|ψi = i (2.138) Theory 35 Now substitute H 0 = U † HU and |ψ 0 i = U † |ψi. ∂ U |ψ 0 i ∂t ∂ 0 0 0 † ∂U 0 H |ψ i = iU |ψ i + U |ψ i ∂t ∂t ∂U ∂ H 0 − iU † |ψ 0 i = i |ψ 0 i. ∂t ∂t H 0 |ψ 0 i = iU † (2.139) From this we define the effective Hamiltonian of the system as H̃ = H 0 − iU † ∂U . ∂t (2.140) We can now can plug in Eq. (2.134) and (2.135) to find the effective Hamiltonian in the rotating frame. H̃ = −dε (1 2i 0 dε (1 2i − e2ωm t ) − e−2ωm t ) ~ω0 − ~ωm ! . (2.141) This Hamiltonian has two terms, an oscillatory component as well as static component. We will now make the approximation that the oscillating terms average to zero leaving that Hamiltonian as H̃ = 0 −dε 2i dε 2i ~ω0 − ~ωm ! . (2.142) Diagonalizing the Hamiltonian gives the shift for a two level system in an applied electric field of ε/2 for the near resonance case. The shift for a time varying field is given by [22] X d2 2 ik ∆Ek = . Ek − Ei i (2.143) For our system we have a energy difference of ~(w0 − wm ) and so our energy shift is ∆E = ± d 2 ε2 . 4~(ω0 − ωm ) (2.144) Here the plus and minus correspond to the shift to the upper and lower states. For our system we are assume the coupling is only occurring between the upper Theory 36 states because the hyperfine splitting of the excited state is much less then the ground state. In order to estimate the AC stark shift we need to find the dipole matrix element for each transition given. First we find the dipole element for each MF → MF0 given by d~MF ,MF0 = h2 P1/2 F 0 Mf0 |d|2 S1/2 F MF i. (2.145) Using the Wigner-Eckart theorem outlined in the previous section, we can combine Eq. (2.127) and Eq. (2.129) to find that dMF ,MF0 = (−1) f 0 −MF0 F0 1 F ! −MF0 q MF p h2 P1/2 ||d||2 S1/2 i (2F + 1)(2F 0 + 1) ( × J0 F 0 I0 F J 1 ) , (2.146) where the reduced matrix element h2 P1/2 ||d||2 S1/2 i = 3.33 ea0 and ea0 = 1.28 MHz V/cm [23]. Now we find the total d2 for the transition from F → F 0 by summing overexcited states and then averaging over the ground states to find the total dipole element. This is given by F X 1 d= 2F + 1 M =−F F " 0 F X f 0 −MF0 F0 1 F ! (3.33ea0 ) −MF0 q MF ( ) #2 0 0 0 p J F I × (2F + 1)(2F 0 + 1) F J 1 (−1) MF0 =−F 0 (2.147) We can now find an expected AC Stark Shift by plugging the dipole element into Eq. (2.144) where ∆ is given as the hyperfine splitting of the upper states. The expected stark shift is given by [24] d 2 ε2 . 4∆ (2.148) Theory 37 For the D1 transitions the expended Stark shift is given in Table 2.3. The shifts for the 6 Li transitions are larger because the hyperfine splitting is ≈ 26 MHz compared to ≈ 90 MHz for 7 Li. Transition 6 Li F = 1/2 → 1/2 F = 1/2 → 3/2 F = 3/2 → 1/2 F = 3/2 → 3/2 )) Expected Shift (kHz/( mW cm2 -20.5 2.6 -10.3 10.3 7 Li F =1→1 F =1→2 F =2→1 F =2→2 -5.5 1.1 -3.3 3.3 Table 2.3: Estimation of AC Stark shift for D1 transitions in 6 Li and 7 Li. )) of intensity in for the incident laser These estimates are kHz shift per ( mW cm2 light. 2.7 Doppler Shift As an atomic beam travels through a vacuum it diverges and we see a spread in the velocity classes caused by different Doppler shifts. This cumulative effect is referred to a doppler broadening. The frequency shift due to the Doppler effect is given by f = f0 (1 + k̂ · ~v ) c (2.149) where f is the frequency experienced by the atom, f0 is the frequency in the rest frame, and k̂ · ~v is component of the atom’s velocity along the direction of propagation of the light. In the limit that all of the atoms are propagating directly perpendicular the laser this this would just be f0 . In the case of a vapor cell there is a distribution of velocities both toward and away from the probe laser, this results in a net effect of broadening the lines. If we take Pv (v)dv to be the fraction of particles with a speed between v and v + dv the distribution in frequencies is Pf (f )df = Pv (vf ) dv df df (2.150) Theory 38 (a) Probe laser on resonance with transition. (b) Probe laser detuned from resonance. Figure 2.3: As the probe laser is swept of the resonance of the atoms, if the laser is slightly detuned from resonance two velocity classes will be excited creating a broadening in line shape as more atoms are excited. where v can be found through Eq. (2.149). For a lithium vapor cell where there is equal chance of velocities from either direction the broadened line with is given by the Maxwell distribution shown by r Pv (v)dv = m − mv2 e 2kT dv, 2πkT (2.151) where m is the mass of the particle, T is the temperature, and k is Boltzmann’s constant. Using the full width at half maximum as given by the width of a 700 K lithium vapor would be r fF W HM = 8kT ln2 f0 ≈ 320 MHz. mc2 (2.152) For an atomic beam source the width is dependent on the geometry of the beam. First we can find the vrms of the beam given by r vrms = 3kT . M (2.153) From this we can find the the transverse velocity using Eq. 2.154 which can then be plugged into Eq. 2.149 to get the line width. r vT = v sin θ = l r 3kT M (2.154) Frequency Combs 39 We tried various nozzles designed to give narrow line widths. The set up that is currently used is a simple one hole nozzle with a collimation plate directly before the interaction region. Without the collimation plate we observed line widths of 120 MHz. With the collimation plate the line width is 16 MHz as calculated by finding the full width at half max of the spectral peaks, see Chapter 5 for detailed analysis and comparison of different nozzles. Chapter 3 Frequency Comb This experiment uses an optical frequency comb as an optical frequency reference to stabilize a probe laser used to excite the atomic transitions. Optical frequency combs are light sources that consist of a series of equally spaced discrete frequencies. The frequency comb used in this experiment is generated by a mode locked Ti:Sapphire oscillator which produces a series of pulses with a pulse duration of tens of femtoseconds. The pulses occur at a repetition rate of ∼ 1 ns. The output spectrum of the Ti:Sapphire oscillator is broadened using a microstructure fiber such that it spans an optical octave. This is necessary for the self referencing and stabilization of the offset frequency as described below. The microstructure fiber is the key element to making frequency combs possible as it allows the comb to serve as an optical reference for light in the visible spectrum and in doing so allows for self referential stabilization. While there are some frequency combs which are octave spanning without the use of a microstructure fiber they are more difficult to construct and maintain [25]. The frequency comb is locked to a GPS steered atomic clock that allows measurements of optical frequencies with a precision of a part in 1012 . This precision in a relatively small system make high precision frequency measurements possible for smaller labs. The frequency comb has become a valuable tool as a frequency standard for many different applications. Stabilized optical frequency combs were first developed for spectroscopy in 1999 by Jones et al. [26] and have become widely used in various fields. 40 Frequency Combs 3.1 41 Overview The optical frequency comb is a laser source whose spectral output consists of ≈ 100, 000 evenly spaced discrete frequencies. This structure can be thought of as as set of evenly spaced teeth. To develop this picture consider a optical resonator with length L with pulse propagating through the cavity described by an envelope function A(t). If we look at one pulse with carrier frequency fc propagating through the cavity it is easy to see that A(t) = A(t + T ) where T is found from the cavity group velocity T = 2L/vg . From this we can define our pulse repetition time as frep = 1/T . The cavity can support light with wavelengths of 2L/n where n is an integer. These modes correspond to frequencies that are multiples of the repetition rate. If the waves have the proper phase relationship this series of harmonic waves forms a pulse, as more frequencies are added the pulse narrows this is shown in Fig. 3.1. Ι Ι Ι Ι Pulse Formation Spectrum of lasing light ν ν ν ν Figure 3.1: A pulse of light in the time domain can be view in the frequency domain as series of discrete frequencies. As more frequencies are added the pulse becomes shorter and so ultrafast pulsed lasers contain a wide range of frequencies. Frequency Combs 42 Now looking at the frequency space picture of A(t) we see a spectrum of comb modes separated by the repetition rate. This is shown in Fig. 1.3. As the pulse propagates through the cavity the dispersion of the cavity causes a phase difference between the phase and group velocities of the pulse. This results in a constant phase shift between the carrier and envelope waves in successive pulses. This constant phase shift ∆φ between pulses is equivalent to a overall offset in frequency space. This is know as the offset frequency where f0 < frep , given by f0 = ∆φ frep . 2π (3.1) Now we are able to relate the frequency of any comb mode to frep and f0 fn = nfrep + f0 , (3.2) this is know as the comb equation as described in Ref [26]. The phase slip is difficult to experimentally detect so the offset frequency is detected directly. This is most easily accomplished if the frequency comb spans an optical octave. If we frequency double light given by fn = nfrep + f0 and compare it to light of twice the frequency given by f2n = 2nfrep + f0 see that 2fn = 2nfrep + 2f0 −2fn = 2nfrep +f0 (3.3) f0 . This means we can directly measure the offset frequency of the frequency comb by referencing two optical frequencies within the frequency comb separated by an optical octave. The frequency comb in this experiment uses a Ti:Sapphire laser and has ∼ 4 × 105 modes with a repetition rate of ≈ 920 MHz and an offset frequency ≈ 300 MHz. 3.2 Dispersion Dispersion is the optical phenomenon by which the index of refraction of all materials in dependent on frequency. Since the group velocity of light with a given frequency is dependent on the index of refraction of the medium that means that Frequency Combs 43 a packet of light with a range of frequencies will spread out in time due to a difference in optical path length due to a change in the index of refraction. Consider the propagation constant defined as k= 2πf n(ω) 2π = . λ c (3.4) Since the index of refraction is frequency dependents we will Taylor expand this around ω0 . This gives dk 1 d2 k k = k(ω0 ) + (ω0 − ω) + (w0 − w)2 . 2 dω 2 dω (3.5) Here the first order term is related to the group velocity, vg , 1 dk = . dω vg (3.6) The second order term is known as the group velocity dispersion (GVD), and describes how the various frequencies spread apart as a pulse propagates through a medium, d2 k 1 dvg =− 2 . 2 dω vg dw (3.7) In a normal medium this means that the pulses will spread out in time as each frequency component experiences a different index of refraction. In most mediums this causes higher frequency light to travel slower then lower frequency. For frequency combs it is necessary to have negative GVD in the cavity in order to correct for the positive GVD caused by the gain medium. This is typically done using chirped mirrors which have longer optical paths for lower frequencies of light and so serve to maintain the phase relationship between different frequencies of light. Frequency Combs 3.3 44 Kerr Lens Modulation The optical frequency comb relies on self lensing through the optical Kerr effect to generate ultrafast pulses of light. The optical Kerr effect relies on the nonlinear response of an a medium to an incident electromagnetic wave. This is given by n = n0 + n2 I. (3.8) For 800 nm in a Ti:Sapphire crystal n0 = 1.76 and n2 ∼ 3 × 10−16 m2 /W [27]. Since the n2 term is negligible at anything but very high powers this term only becomes important for pulsed operation as the peak intensity in pulsed operation is much higher than cw, even though the average power is about the same. In cw operation, the frequency comb has a intracavity power of ∼ 250 W, and a single pulse in mode locked operation has a peak power of ∼ 25 MW. Thus the effect will only be important for pulsed operation. Figure 3.2: Hard aperture Kerr lensing. The CW and pulsed beam both enter the medium with the same gaussian profile, since the peak intensity of the pulsed light is much higher there nonlinear index of refraction in the medium focuses the light through the aperture. The CW beam has lower peak intensity and so is not effected. This effect makes the cavity favorable for pulsed operation as more light is passed. [28] The optical Kerr effect relies on the Gaussian profile of the beam to create a variation in the index of refraction as a function of distance from the center of the beam width. The index of refraction will be greatest at the center of the beam and decrease at the tails. This serves to refocus the light when in pulsed operation. In order to achieve pulsed operation the cavity is set up such that pulsed operation is preferred. This can be done through either a soft or hard aperture. Frequency Combs 45 The first designs for a mode locked laser used a hard aperture which cut off part of the beam to make pulsed operation preferable by increasing the losses to cw operation. This is shown in Fig. 3.2. Soft apertures use a change in the overlap between the cavity mode and the pump beam in the gain medium which also favors pulsed operation by increasing the overlap in pulsed operation. 3.4 3.4.1 Oscillator Cavity Pump Laser The pump laser used for this experiment is a Nd:YVO4 (neodymium yttrium orthovandate) Verdi G8 manufactured by Coherent. This laser outputs 532 nm light with a maximum power output of 8 W. Typically it is run around 5 W. The pump beam passes through an acousto-optic modulator (AOM) and a half wave plate before entering the oscillator cavity. The half wave plater rotates the incident light going into the oscillator cavity from the vertically polarized light from the pump. The AOM is used for stabilization of the offset frequency described below. 3.4.2 Oscillator Cavity The resonator is a bowtie configuration cavity with a path length of ∼ 30 cm. This is housed in a 10 × 20 × 30 box which is watercooled in the baseplate as well as crystal holder to improve temperature stability. The cavity length dictates a repetition rate of ≈ 1 GHz. The bowtie configuration is used because it allows tighter focusing of the beam to increase the Kerr-Lensing effect. It also is compact and so can be used for higher repetition rate cavities. Frequency combs with repetition rates of 100-200 MHz are commercially available, less common are frequency combs with repetition rates of ≈ 1 GHz. While higher repetition rate combs have the advantage of higher power output per mode, the pulse energy must decrease by 1/10, assuming the average power through the cavity is constant. This means that the steady state pulse duration is 10 times longer. This results in a overall pulse intensity which is 100 times less then the 100 MHz system. This makes Kerr lensing more difficult as the nonlinearity in the crystal is depended on peak intensities. There are two ways this has been Frequency Combs 46 M3 OC lens Pump M1 M2 Figure 3.3: The oscillator cavity used is a bowtie configuration. This configuration allows for a high repetition rate because it can be made compact and the repetition rate is based on the length of the cavity. compensated for in this laser. The output coupler is 98% reflective as opposed to 90% used in most 100 MHz systems. The dispersion of the cavity mirrors is negative such that the light maintain ultra short pulses. This helps to increase max intensity even with lower Ep . Figure 3.4: Chirped Mirrors are used to compensate for the dispersion light experiences when traveling through a medium. They are normally specially coated dielectric mirrors which provide longer optical paths for lower frequencies of light and so compensate for the increased group velocity. These mirrors are used to maintain the phase relationship between multiple frequency components of pulsed lasers. Frequency Combs 47 In order to achieve negative GDD the cavity is tuned using negative dispersive mirrors. These reflect different wavelengths of light from different layers of the mirror in order to refocus the light. Longer wavelengths are reflected deeper in the coating of the mirror. This is illustrated in Fig. 3.4. The crystal is 2 mm × 3 mm × 1.5 mm and is placed at Breuster’s angle between M1 and M2. Mirrors M1 and M2 are GDD oscillation compensated and have a GDD of -50 fs2 ± 20fs2 and a radius of curvature of 3.0 cm. Mirror M3 is flat and a GDD of -40 fs2 The output coupler is 98 percent reflective. Ti:Sapphire Crystal Crystal Holder Cooling Water X-Y Translation Stage Figure 3.5: The crystal mount for the Ti:Sapphire oscillator is shown. The mount is made of copper and has water channels cut through the center section for cooling. This is mounted to an X-Y translation stage used to center the crystal in the beam wast of the cavity. This is important as the beam is the most focused at the beam wast and so the intensity is higher increasing the nonlinear effects in the crystal. The crystal is attached to a copper holder which is mounted on an x-y translation stage to allow the crystal to be positioned at the waist of the resonator shown in Fig. 3.5. There are channels cut in the copper block to allow cooling water to circulate. Frequency Combs 3.4.3 48 Lasing and Modelocking In order to achieve lasing and mode locking of the oscillator, several aspects of the cavity can be adjusted. The cavity is first alined to achieve cw lasing by altering the angles of M1 and M2 as well as the crystal position. Mirror M2 is the then adjusted using a translation stage such that the cavity is more stabile in mode locked operation. The cavity then requires an external perturbation to interrupt the beam in the cavity to allow the build up of pulses. This is done by taping on M2 with the back of a screwdriver. Once mode locked, pulses propagate in only one direction through the cavity. This is the easiest way to tell if the laser is mode locked. The properties of the laser can be carefully tuned by adjusting the crystal position and M2. The output power in mode locked operation is ∼ 500 mW and ∼ 600 mW in continuos wave operation. The output spectrum of the oscillator cavity is ∼ 50 nm centered at 790 nm. This output does not span an optical octave which is necessarily for stabilization, explained in section 3.5, so we use a microstructure fiber to broaden the output of the oscillator to an optical octave. Figure 3.6: Silicon microstructure fiber. The microstructure fiber spectrally broadens the output of the oscillator cavity such that it spans an optical octave. Picture taken from Ref. [29]. Frequency Combs 3.4.4 49 Microstructure Fiber In order to stabilize the offset frequency of the frequency comb, we need it to be self referential. This means we need to be able to compare comb light separated by an optical octave such that light can be double and compared against itself. The output spectrum of the comb does not span an optical octave, so to achieve this we broaden the spectrum using a air-silica microstructure fiber. In conventional optical fibers light is transmitted using total internal refraction. Here the index of refraction of the core of the fiber is higher then that of the cladding and so the light is guided through the fiber with minimal loss. Microstructure fibers use optical waveguides to transmit the light. By manipulating the geometrical dispersion of the waveguide the material dispersion of the fiber can be cancelled. These fibers are made up of a series of air holes in a solid core, the arrangement of these holes can be used to tune the fiber for different purposes an example of which is shown in Fig. 3.6. The fiber is designed to have zero GVD as well as broadening, both of which are extremely important for our application. Figure 3.7: The light from the Ti:Sapphire oscillator is focused into the fiber using a microscope objective. The broadened light from the output of the fiber is shown, on the far left there is blue light present but it is difficult to see because of the strength of the green light. More discussion of the development of microstructure fibers can be found in Ref. [29] as well as detailed discussion of the particular optics setup used in this experiment in Ref. [28] and [30]. The output of the fiber spans the visible spectrum as shown in Fig. 3.7. Frequency Combs 3.5 50 Stabilization The optics post cavity serve to broaden and stabilize the comb from the output of the oscillator. The following section outlines the optics and electronics setup for the stabilization of f0 and frep . 3.5.1 Repetition Rate The repetition rate of the frequency comb is dependent only of the optical path length of the cavity. Thus it can be stabilized by tuning the length of the cavity. This is achieved using a feedback loop controlling a piezo ceramic on M3 of the resonator cavity. Broadened laser light is picked off from the main comb beam and sent onto a photodetector (Electro-Optics Technology ET-2030A) in order to detect the repetition rate. The repetition rate as well as integer multiples of frep is present in the comb light from interference of neighbor comb modes yielding a difference frequency of frep as well as higher harmonics. This signal is then sent through a bandpass filter to remove the higher harmonics (2frep , 3frep , ...) and then sent to a mixer where it is mixed down with the signal from an radio frequency generator. This generator is referenced to the atomic clock and allows the control and tuning of the repetition rate. The output of the mixer produces an error signal for the loop filter which can then output a correction to the high voltage amplifier to tune the cavity length by tuning the piezo. In this application the piezo ceramic used is a Noliac CMAR03 PZT. This then stabilizes frep at the frequency dictated by the synthesizer. This setup is illustrated in Fig. 3.8. This set up has yielded a consistent and stable lock which can easily stay locked for several hours. This is the most consistent of all locks. 3.5.2 Offset Frequency The stabilization of the offset frequency is a more complicated setup and is not as stable as the frep lock. Unlike frep , f0 is not inherently accessible in the comb light. In order to measure f0 we frequency double a lower frequency ν1 = n1 frep + f0 and then beat it against a higher frequency ν2 = n2 frep + f0 where n2 = 2n1 . When these frequencies are heterodyned together we are left with a difference frequency Frequency Combs 51 Piezo Ceramic Photodetector High Voltage Amplifier M3 Pump Loop Filter OC lens M1 M2 Bandpass Filter Mixer Splitter Divide by 8 Counter rf Signal Generator Figure 3.8: Diagram of frep stabilization. Light from the frequency comb is detected using a photodetector. This signal is then amplified and filtered to remove higher order harmonics. The signal is mixed with the output of an rf synthesizer to get a error signal. This is sent to the loop filter used to tune the feedback to the comb cavity. A piezo ceramic is mounted to M3 in the cavity and can be tuned to provide small changes in cavity length and so change the repetition rate. of f0 . For this method to work the comb must span at least an optical octave to have two frequencies to compare. The comb in this experiment does not span an optical octave without the use of a microstructure fiber. After the fiber the comb light spans a range of 530 nm (green) to 1060 nm (infrared) giving an optical octave. The 1060 nm light is frequency doubled using a nonlinear periodically poled lithium niobate (PPLN) crystal and then beat against the original 530 nm light. The crystal is designed to double light at ∼ 1064 nm. Dispersion caused by the various elements causes a relative time delay between the two pulses. To compensate for this delay an interferometer is used to alter the path length of one pulse. The beam is split using a mirror that reflects light between 420 nm and 630 nm and transmits frequencies between 750 nm and 1200nm. The 530 nm and 1060 nm light are seperated and the phase offset can be corrected by adjusting the path length of the 530 nm light. The two pulses of original 530 Frequency Combs 52 nm light and doubled 1060 nm light are heterodyned onto a photodetector for the beat note signal. The signal from the detector first passes through a tunable bandpass filter in order to remove some of the other frequencies present in the comb light. This is then mixed up to 1240 MHz with the rf synthesizer and then sent through a frequency divide by eight to give 155 MHz. This is then mixed with a synthesizer at 155 MHz in the digital phase detector to get our error signal. The process of mixing up to 1240 MHz and then dividing by eight is used to help increase the capture range of lock as deviation from the lock frequency will appear as a smaller fraction of the phase of the error signal. The error signal goes through a loop filter that is used to tune the gain response of the feedback. The offset frequency can be tuned by changing the pump power going into the Ti:Sapphire crystal because of the non-linear gain in the crystal. There are two methods for tuning this input power. The first is changing the output power of the pump beam. This is normally in the range 5 to 6 W. The second is an acousto-optical modulator (AOM) placed in the pump beam before the cavity. Acousto-optic modulators use radio frequency waves to vibrate a piezo ceramic attached to a quartz crystal, producing sound waves in the glass. These act as density waves in the glass creating regions of expansion and contraction and so varying the index of refraction in the glass. The incoming light scatters off periodically modulated index of refraction into multiple orders of beams. The diffracted light emerges at an angle θ dependent on the wavelength of the incident light, λ, and the radio frequency, fm , as shown in Eq. 3.9. This diffracted light does not couple into the resonator cavity and so by tuning the power in each order the power to the resonator can be altered. The intensity of light in each order is proportional to the applied rf voltage. B(θ) = mλ 2fm (3.9) The advantage of this setup is that AOM’s are much faster then any mechanical feedback. We use a Interaction Corp. Acoustic-Optic modulator model AOM405AF1 in this experiment. The pulse rise time and depth of modulation for this Experimental Setup 53 AOM with acoustic velocity V = 3.63 mm/µsec are given by Tr = 177D nsec (3.10) and M = e−.0936D 2f 2 m , (3.11) where D is the beam size in mm and fm is the modulated frequency in MHz. Experimental Setup 54 Pump Laser AOM M3 OC lens Pump M1 rf Signal Generator 155 MHz AOM Driver Loop Filter Cavity Filter M2 Digital Phase Detector Divide by 8 Photodetector Bandpass Filter Mixer Splitter Counter rf Signal Generator 1240MHz - fo Figure 3.9: Diagram of f0 stabilization. The frequency doubled light and non doubled light from the frequency comb are combined is detected with a photodetector. The beat note between these two frequencies is the offset frequency. This signal is mixed up to 1240 MHz with the output of a rf synthesizer. This is then frequency divided by 8 such that the signal is at 155 MHz. This is mixed with the output of a second synthesizer at 155 MHz to get an error signal. This is sent to a loop filter used to control the feedback to the AOM which modulates the pump beam to the oscillator and controls the offset frequency. Chapter 4 Experimental Setup Figure 4.1: Overview of the experimental setup for this measurment. The extended cavity diode laser is frequency stabilized to the optical frequency comb. This allows the precise measurement of the frequency of the diode laser that is used to excite the lithium atoms. The main components of this experiment are the atomic beam, frequency comb used as the frequency standard, and extended cavity diode laser for probing the atoms. The lithium oven is used to create the atomic beam that propagates through the vacuum chamber and intersects with probe laser. The frequency of the probe laser is tuned over the transitions we are interested in measuring and then the fluorescence from the atoms decay is recorded using a photo multiplier tube 55 Experimental Setup 56 (PMT). The probe laser is locked to the optical frequency comb which provides a precise measurement of the optical frequency of the diode laser. 4.1 Diode laser The extended cavity diode laser has become an extremely useful tool for atomic and optical physics [31]. Precision atomic spectroscopy requires the ability to excite single transitions with a tunable source. Diodes are available at many different frequencies and so have made many transitions easily accessible. While the frequency comb provides an absolute frequency standard, the power per comb mode is low, making spectroscopy using the comb light directly difficult. The diode laser provides a reasonably powerful probe beam that can then be stabilized to the frequency comb. Output Mirror Zero Order Diffraction Grating Tuning Mirror Zero Order First Order Diode Controller First Order Collimation Lens (a) Littrow Configuration Diode Controller Diffraction Grating Collimation Lens (b) Littman-Metcaff Configuration Figure 4.2: There widely used configurations for ECDL’s are shown. Both configurations use a diffraction grating for feedback. The two configurations differ in that the cavity length is tuned by displacing diffraction grating in the Littrow configuration and a tuning mirror for the Littman-Metcaff in order to scan the frequency with small adjustments in cavity length. This experiment uses the Littrow configuration. 4.1.1 Diode Laser Theory For precision spectroscopy, the diode laser must be single mode such that it outputs a single frequency. Ideally this laser width is as narrow as possible so that the laser line width does not broaden the spectral peak width. It is also required that this frequency be tunable over a range sufficient to scan over the transitions. Experimental Setup 57 Laser diodes are electrically pumped laser which uses a p-n junction of a semiconductor diode as the gain medium. Normally laser diodes has two reflective surfaces that serve as the resonating cavity for the laser, by coating one surface of the diode with an antireflective coating the outer surface provides no feedback and so an external cavity is used to provide feedback. This results in a frequency tunable cavity that can be scanned over a large range of frequencies. This means that without the external feedback the diode will not lase or have a very low output power as the power within the cavity is much lower. The Littrow configuration shown in Fig. 4.2a, uses a diffraction grating as the frequency tuning element. In this configuration the first order light is reflected back into the diode to provide optical feedback. By changing the angle of the grating the laser can be tuned in frequency over a range of ∼ 10nm. For finer adjustment the grating is displaced using a piezo ceramic to proved small changes in the cavity length. The zero order is reflected off the grating as the output. One of the limitations of this configuration is that in changing the angle of the grating to change the frequency the alignment of the output beam is also slightly moved. The second common configuration is the Littman-Metcaff configuration shown in Fig. 4.2b. In this configuration the output of the diode is reflected off the grating such that the first order light goes to tuning mirror and then light is reflected back off the grating into the diode as optical feedback. In this configuration the grating remains stationary and so the output alignment does not change as the beam is scanned. The mirror position is displaced to tune the cavity length and so tune the frequency. The limitation with this setup is the output efficiency is lower then the Littrow configuration and it is a more complicated system. 4.1.2 Diode Laser Experimental Setup The ECDL used in this experiment was constructed using a AR-coated diode from Eagle Yard with a wavelength of 670nm and a specified maximum output of 18mW at 25◦ C however this is dependent on configuration. This is mounted in a ThorLabs LDM21 TEC-cooled laser diode mount. The housing of the LDM21 has been replaced with a heavier brass shell to improve mechanical stability. The temperature and current are controlled using a ThorLabs TED200C temperature controller and LCD205C current controller. A lens with x-y translation stages with z adjustment is attached to the brass housing and then an 1800 groove/mm ruled Experimental Setup 58 Diode Mount Collimation Lens on Translation Stage Diffraction Grating Figure 4.3: The diode laser used in this experiment is shown. The components are mounted to a heavy steal box which is isolated from the optics table with a rubber pad. This is to reduce vibrations and so increase stability. grating with 500 nm blaze is used for feedback. Here z is the axis of propagation for the light, x is horizontal, and y is vertical. This grating was decided experimentally as it produced higher output power than other gratings that were tried. This is mounted to a piezo ceramic on a stainless steel disc. The disc is mounted in a Polaris Low Drift Kinematic Mirror Mount. When a voltage is applied to the piezo it changes the length of the cavity and so allows for tuning over a frequency range of ∼ 8 GHz. The diffraction grating provides frequency tunable feedback to the diode laser by specially separating light based on wavelength. By tuning the angle at which the light is sent back into the diode cavity the frequency can be tuned. The spacing of the grooves determines the frequency spread as well as the amount of power reflected into the 1st order which is used for feedback to the cavity. The grating used in this experiment has an efficiency of 70%. This configuration gives a maximum output power of 27 mW as shown in Fig. Experimental Setup 59 25 Power (mW) 20 15 10 5 0 80 100 120 Current (mA) 140 Figure 4.4: The output power for the ECDL as a function of applied current at 19◦ C is shown. This is using a 1800nm grating for external feedback. Normal operating current is between 130 and 140mA. 4.4 however when running we typically operate with an output power of ∼ 20mW at 671nm. A combination of temperature tuning and grading feedback is used to bring the diode laser to the desired frequency. In order to increase the wavelength the temperature is raised which results in lower output power. This laser normally was run between 19◦ and 20◦ C. The overall stability of the diode laser is very important for data taking. Both over short times scales to be able to collect single runs of data but also over the course of a day. The cavity has been made as small as possible in order to improve stability. The collimation lense mount has been changed from a x-y-z stage to a x-y stage in order to make the cavity smaller. This setup shown in Fig. 4.3. The configuration of this diode laser has been upgraded in order to improve tuning and stabilty. We originally used diodes that we had AR coated which output 1215mW. These diodes had more problems then the current setup with both stability and beam profile. This led to the decision to replace the homemade AR coated diodes with the commercially coated Eagle Yards diodes. We have also improved the mounts in the cavity to decrease mechanical vibration and so increase stability. This has led to an increase in mode hope free tuning range from ∼ 2 GHz to ∼8 as well as increased output power. Experimental Setup 60 Beam Splitting Cube 1/2 Wave Plate EOM ECDL Isolators 30dB Beam Splitting Cube Comb Light Polarizer Photodetector Fiber Coupler To Fabry Perot Figure 4.5: The controlling optics for the ECDL are shown. The output of the ECDL is first sent through a pair of optical isolators in order to prevent reflections from other optical elements entering the cavity which changes the feedback. A polarization dependent beam splitter is used to divide the beam between the beat note setup for stabilization and the interaction region. A wave plate is used to tune the power to both arms. The EOM in the interaction arm is used to stabilize the power to the chamber. The other arm is combined with light from the frequency comb in order to provide a beam note for the stabilization circuit. 4.1.3 Frequency Stabilization The beat note lock precisely controls the frequency of the diode laser by locking it to one mode of the comb. This is done by spatially overlapping the comb and diode light by combining them with a polarizing beam splitting cube. The ratio of the two beams can be adjusted using a polarizer after the cube to select a combination of the two beams. This combined light is then measured on a photodetector. Like the offset frequency lock, this signal is sent through a lowpass filter to remove unwanted frequencies from the signal. The lock frequency is chosen to be 200 MHz. It is then amplified and then mixed up with a 760 MHz signal from a synthesizer to 960 MHz. This signal is then sent through a tunable bandpass filter to further Experimental Setup 61 Output Mirror Current Controller Zero Order Diffraction Grating Diode Controller First Order Proportional Gain Collimation Lens rf Signal Generator 60 MHz High Voltage Amplifier Digital Phase Detector Loop Filter Divide by 16 Photodetector Counter Splitter Lowpass Filter Mixer Bandpass Filter rf Signal Generator 760 MHz Figure 4.6: The beat not of the heterodyned comb and diode light is detected using an amplified photodiode. This is then filtered and amplified before being mixed up to 960 MHz with the output of the synthesizer. This is sent through a divide by 16 before being sent to the feedback control. This is to increase the capture range as the effect of noise frequency noise on the diode will decreased through the mix up and division. This is sent through the controllable gain feedback which tunes the diode with both proportional gain current feedback and tunable PID gain from the loop filter which controls the grating. filter the signal and then the frequency is divided by sixteen. This again serves to increase the capture range of the lock. Here we use a divide by 16 instead of a divide by 8 as the frequency noise in the beat note is larger and so by dividing by 16 we increase the capture range which leads to a better lock. The signal is then mixed down with another synthesizer at 60 MHz to get our error signal. The error signal is then split and sent to the loop filter which controls the low frequency feedback as well as a current feedback for higher frequencies. The loop Experimental Setup 62 filter outputs to a high voltage amplifier which controls the piezo attached to the grating. This system stabilizes the frequency of the diode to one comb mode. To scan the frequency of the diode the repetition rate of the comb is scanned by changing the frequency of the synthesizer used in the repetition rate lock, this changes the frequency of the comb mode and so the diode. 4.1.4 Fabry-Perot Interferometer Fabry-Perot interferometers have many uses in both spectroscopy and other fields. A Fabry-Perot cavity in its simplest form is made up of a pair of parallel mirrors separated by a distance L. Coherent light will be transmitted through the cavity if its frequency is such that standing waves can be maintained inside the cavity. When the frequency of the light is not an integer multiple of the free spectral range of the cavity the light will destructively interfere and so not be transmitted. The power transmission of a Fabry-Perot cavity can be calculated using the phase difference acquired during the light traveling one cycle through the cavity. This calculation is performed in Ref. [32] and yields the Airy function T = 1+ [4r2 /(1 1 , − r2 )2 ] sin2 (δ/2) (4.1) where δ = 2kd is the phase shift acquired through one round trip through the cavity. The square bracketed term in Eq. 4.1 is called the coefficient of fitness, F which is dependent only on the reflectivity of the mirrors r. F = 4r2 , (1 − r2 )2 (4.2) As r varies from 0 to 1, F varies from 0 to infinity. Thus the transmission through the cavity given in Eq. 4.1 has a maximum when sin(δ/2) = 0 and min when sin(δ/2) = ±1. Thus the cavity will have a maximum when δ = m2π. For a planar cavity the wavelengths at which the cavity has maximum transmission are given by 2L = mλ. (4.3) Experimental Setup 63 In frequency space the separation of the transmission peaks is known as the free spectral range given by νF SR = c . 2L (4.4) Note that this means that the peak spacing is only a function of cavity length and so this allows Fabre-Perot cavities to act as an indicator or laser frequencies. Equation 4.4 assumes a planar cavity, this experiment uses a confocal cavity that has two curved mirror where the radius of curvature of the mirrors is equal to the cavity length.The free spectral range given by νF SR = c . 4L (4.5) The additional factor of 1/2 is because the round trip path of the light in a confocal cavity is twice as long as that of a planar cavity, shown in Fig. 4.7. The advantage of a confocal cavity is that for a given path length the confocal cavity is smaller and so more stabile. Similarly for a given cavity length a confocal cavity has twice the resolution of a planar cavity. Path length = 4L Path length = 2L L L Figure 4.7: Confocal and planar Fabry-Perot Cavities. The round trip path length for the confocal cavity is twice that of the planar cavity. The cavity in this experiment is constructed with a tube of length of 30 cm. The mirrors have radii of curvature equal to the length of the cavity. This gives a free spectral range of 250 MHz. Figure 4.8 shows the transmission of the Fabry-Perot cavity as a function of relative frequency. The spikes in transmission occur when the laser is a integer multiple of the free spectral range of the cavity. Fabry-Perot cavities are useful tools for characterization of the diode and its ability to scan over a frequency range. We cannot use it to give absolute frequency measurements of the diode laser but it is a good measure on overall stability Fabry-Perot Transmission (V) Experimental Setup 64 1.2 1.0 0.8 0.6 0.4 0.2 0 2 4 Frequency (GHz) 6 8 Figure 4.8: The transmission through the Fabry-Perot cavity is shown vs relative laser frequency. Each peak is separated by 250 MHz, the free spectral range of the cavity. This shows that the ECDL is single mode over an ∼ 8 GHz tuning range. and scanning range. If the peaks are clean with no noise it is an indicator that the laser is single mode. If the peak spacing changes that implies that there is nonlinearity in the piezo response. When characterizing the diode laser’s stability and tuning characteristics, the piezo attached to the grating on the diode laser is scanned with a 100 Hz triangle wave which modulates the frequency of the diode laser. Transmission through the Fabry-Perot cavity is then recorded with a photodetector. This has shown that we can get 8 GHz mode hope free tuning with the diode laser as shown in Fig. 4.8. This is a useful tool for insuring that the alignment of the ECDL cavity is robust over a large range. This is important for data collection stabilized to the comb, if the diode laser is not stabile then it will not be able to scan the transitions. 4.1.5 Optical Spectrum Analyser In order to set the ECDL to the appropriate wavelength we use an optical spectrum analyzer to calibrate the laser on a coarse scale. Diode laser light is split from the main beam and coupled into the OSA before entering the vacuum chamber. This analyzer is only accurate to ≈ .1 nm and exhibits a systematic offset. We normally observe transitions at 671.13 nm when the true wavelength is 670.94 nm. While Experimental Setup 65 this does not give a precise method of measuring the frequency it is a useful tool for rough calibrations that would be difficult otherwise. 4.1.6 Power Stabilization When scanning the frequency of the diode over the transitions there are power variations as the feedback and alignment changes. For any precision spectroscopy it is important to have consistent power incident on the atoms as the number of atoms stimulated is depended on the power. In order to solve this problem we use an electro-optic modulator to stabilize the beam power prior to the interaction region. Using a EOM to control the power is a better option then direct feedback to the laser as the EOM has no direct impact on the frequency stabilization of the laser while modulating the power with current would. Power Transmitted (mW) 2.5 2.0 1.5 1.0 -1.5 -1.0 -0.5 0.0 Monitor Voltage (V) 0.5 1.0 Figure 4.9: Response of Electro-optic modulator to applied electric field. The transmitted power is shown which follows a sin curve with applied voltage. The power can be cut to ∼ 30% of the maximum power. When locking the power signal we lock somewhere in the middle of EOM range shown in Fig. 4.9 using the offset on the high voltage amplifier, this way if the power pulls we have a fairly large stabilization range. The power signal is picked off from the probe laser directly before entering the chamber as shown in Fig. 4.10. The signal from the photodetector is sent to a loop filter where is is combined with a bias voltage. The bias is set to the negative of the DC voltage level of Fig. 4.9, Experimental Setup 66 this gives an error signal of around zero volts. The output of the loop filter is sent to a high voltage amplifier which goes to the EOM. To Interaction Region Fiber Coupler Fiber Coupler to OSA Polarizing Beam Splitting Cube 70:30 Splitter Photodetector Figure 4.10: The optics pictured are the post fiber coupled optics for the probe beam. These are used to generate a signal for the power stabilization which is directly before the interaction region. 4.1.7 Electro-Optic Modulators Electo-optic modulators consist of an electrooptic crystal with a refractive index which is sensitive to an applied electric field. Electro-optic modulators are used to tune the amplitude of an optical beam by introducing a phase shift between different components of the light. The change in index of refraction for a electrooptic crystal in an applied electric field is given by [33] ∆n = n30 r E , 2 (4.6) where E is is the applied electric field, n0 is the index of refraction without the presence of an electric field, and r is the component of the electro-optic tensor. The electro-optic tensor describes the crystals interaction with the electric field, typically r is very small. This effect introduces a phase shift in the light traveling Experimental Setup 67 Electooptical Crystal L x y Input Polarizer z DC Voltage Output Polarizer Figure 4.11: Diagram of an Electrooptic Modulator. Electrooptic Modulators use a crystal with indices of refraction that are dependent on the applied field. By changing the applied voltage the EOM induces a phase difference between the two paths which causes destructive interference and so amplitude modulation. The input and output polarizers are used to split and recombine the light from going through the crystal. through the crystal given by ∆φ = πn30 rV l , λ d (4.7) where V is the voltage applied across distance d in the crystal and l is the length of the crystal. A standard EOM is shown in Fig. 4.11, the main components are a pair of polarizers set 90◦ apart and an electro-optic crystal. When an electric field is applied to the electro-optic crystal acts as a variable wave plate. When a voltage is applied the electro-optic effect changes the index of refraction for the two crystal axis to a different degree, changing the optical path length of the two components of the light. This experiment uses a Conoptics 360-80 EOM, this is not designed for 671 nm light and so there is more loss in overall amplitude then a crystal designed for 671 nm light, however it works well enough for our application. Experimental Setup 4.2 68 Atomic Beam The most common atomic spectroscopy is done using a vapor cell. Here a sealed glass tube of the substance being investigated is heated and then probed with the excitation laser. These vapor cells are easy to use and do not require constant pumping to maintain vacuum. This makes them an easier solution then the atomic beam source for most experiments. The limitations with vapor cells is they have a large Doppler width meaning the transitions we are looking at will not be resolved. An additional limitation specific to lithium is that when heated it reacts and corrodes glass. Lithium Vapor Density 16 10 15 10 14 10 13 -3 Atomic Density [cm ] 10 12 10 11 10 10 10 9 10 8 10 7 10 6 10 450 500 550 600 650 700 750 800 850 900 950 Temperature [K] Figure 4.12: Atomic Denisty of Lithium as a function of Temperature. For this experiment the temperature of the oven is 400◦ C. This experiment uses an atomic beam source from a lithium oven. In order to create the beam we heat small pellets of lithium to ≈ 400◦ C. Heating the chamber this high gives a vapor pressure of ∼ 1013 atoms/cm3 as seen from the vapor pressure curve in Fig. 4.12. The oven was constructed using a 2 1/8” conflat nipple that was welded to a blank flange on one side and and a flange with a .5” hole on the other. This was welded Experimental Setup 69 instead of using standard copper gaskets as previous ovens had problems with leaking lithium after it corroded through the copper gasket. Threaded rods were then welded to both flanges in order to connect the oven to the vacuum chamber. The nozzle was not welded so that the lithium could be refilled. Threaded Rods to Attach to Vacuum Chamber Lithium Chamber Nozzle Heater Coils Figure 4.13: The lithium oven is constructed from 2 1/8” conflat nipple welded to a blank flange on one side and a flange with a half inch hole on the other. Threaded rods were then welded to the end to attach it to the vacuum chamber. A nozzle is attached to the hole on the other side. The oven is heated with tantalum heater wire wrapped in coils. The oven is heated using coiled tantalum heater wire. The wire is coiled and then placed in ceramic tubes to prevents shorting between the heaters and vacuum chamber. Originally the oven was set up to allow heating of both the chamber and the nozzle as a precaution against clogs. We have stopped using the nozzle heater and have not had any issues with clogging. The voltage to the heater is controlled by a Variac, normally in the 18-22 volt range. A thermocouple is connected to the outside of the oven which gives a ballpark reading for the temperature in the oven. One of the requirements for the atomic beam is that its width be as close to the natural line width of 6 MHz as possible. This is important as the spacing of the transitions we are looking at is such that we are limited in precision by the resolution of the peaks. If the line width of the atomic beam is large the peaks will not be resolved and so line shape modeling will be much more difficult. We tried many different nozzle designs attempting to collimate the beam before this setup. The previous nozzles all had large doppler widths and so were not sufficient for the level of precision requited in the measurement. The second method used to limit the effect of the doppler width and line asymmetries on the precision of our measurements is to reflect the probe beam back through the chamber parallel to the initial beam. This helps to symmetrize the Experimental Setup 70 peaks from any misalignment between the probe and atomic beams. This is done using a ThorLabs retroreflector prism that reflects the incoming beam 180◦ with part in 105 uncertainty. This is also useful for doppler-free saturated fluorescence spectroscopy. When the probe beam is tuned slightly off resonance it will excite two velocity classes at equal angles away from perpendicular. When the probe laser is the same frequency as the transition it will only excite the velocity class of atoms which are directly perpendicular to the probe beam. This means that there will be a dip at resonance as less atoms will be excited. This dip can be used to accurately find the centers in the case where the doppler width is large as so hides features. Collimation Plate Lithium Oven Probe Beam Figure 4.14: The atomic beam is collimated using a single channel nozzle on the lithium oven and then a collimation plate directly before the interaction region. This gives line widths of ∼ 16 MHz. Currently we are using a single channel nozzle attached to the oven and then a collimation plate bolted to the inside of the vacuum cube which houses the interaction region. This solution in has given line widths of ∼ 16 MHz. This is substantial improvement over the 120 MHz line widths that we had previously recorded, this is shown in Fig. 4.15 4.3 Vacuum System In order to precisely measure the transitions in lithium it is important that it is done at high vacuum. Like all alkali atoms, lithium is highly reactive and will Experimental Setup Amplitude (Scaled Voltage) 30x10 -3 71 Collimated Atomic Beam Original Atomic Beam 25 20 15 10 5 0 1450 1500 1550 1600 1650 Relative Frequency (MHz) 1700 1750 Figure 4.15: Data showing the narrowed width of the current atomic beam setup. The blue data was taken with the original setup and has line width of 120 MHz. The red data is taken with the improved setup which has a line width of 16 MHz. react in air. Also you cannot have an atomic beam in air as the atoms will collide with gas and disperse. The atomic beam and interaction region are housed in a 8” expanded spherical cube from Kimball Physics. Attached to this are are various nipples and bellows to connect the other components as shown in Fig. 4.16 and Fig. 4.18. Attached to the South side is a 4.50” nipple containing the oven and associated heaters and thermocouples. Opposite that is the ion pump used to pump down the system. Perpendicular to this are two adjustable bellows with AR coated windows on either side. The probe beam passes through from the east side and then is retro-reflected back through the interaction region using a corner cube. The chamber is kept at 10−9 Torr when the ovens are not on and gets to 10−7 Torr when running. All elements that are placed in the chamber are cleaned and baked prior to installation to minimize contamination of the chamber. Even with these precautions the chamber takes about 10 days to pump down after switching nozzles or other components. Experimental Setup 72 PMT with Filter Figure 4.16: The atomic beam and probe laser intersect in the center of the vacuum cube this houses a set of lenses used to magnify the fluorescence. The PMT is placed on the top of the cube and has a pass band filter at 670nm to filter the scattered light. 4.3.1 Interaction Region The fluorescence of the atoms is detected using a ET Enterprises 51mm photomultiplier tube (PMT). A 10 nm bandpass interference filter at 670 nm is placed in front the PMT to reduce ambient light entering the chamber. This is mounted at the top of the vacuum cube as to be perpendicular to both the atomic beam and probe laser. Inside the vacuum chamber a pair of 60 mm plano convex lenses are suspended above the interaction region as shown in Fig. 4.16. These serve Experimental Setup 73 Figure 4.17: Picture of the vacuum chamber and associated components. The over is visible on the right of the picture. The probe beam enters from the far side of the chamber and exits through the window in the foreground. to increase the detection efficiency by increasing the area of detection. The input windows are also attached to bellows such that any reflection from passing through the windows can be adjust away from the interaction region. This helps to reduce the scattered light level in the chamber. 4.3.2 Ion Pump This experiment uses an ion pump to maintain a pressure of 10−7 Torr while taking data with the ovens hot. In general ion pumps are able to achieve pressures of 10−11 Torr by ionizing the gas molecules and then catching them in the pump walls. Ion pumps consist of a set of charged anode rings and a grounded cathode plates and a set of strong magnets (Fig. 4.19). A strong magnetic field is applied through the center of the coils. As free electrons enter the anode rings they are trapped in the string magnetic field and begin to precess in the rings and as more electrons are trapped this creates an electron cloud. When stray gas molecules enter the pump there is now a high probability the will collide with a free electron and become a charged ion. This is then repelled by the anode to the neutral cathode plate where it trapped. Experimental Setup 74 Lithium Oven Atomic Beam Collimation Chopper Wheel Retroreflected, chopped Laser Light Corner Cube Ion Pump Figure 4.18: The vacuum setup with oven and ion pump is shown. The collimation plate is connect to the inside of the vacuum cube. The probe laser passes through the chamber and then is retroreflected back using a corner cube. When taking data with the lockin amplifier the chopper wheel is used to chop the retro beam. Ion pumps must be have a start pressure of 10−4 Torr or lower. We rough the system using a turbo-molecular pump backed by a mechanical pump. The ion pump used in this experiment is a Kurt J. Lesker LION ion pump. 4.3.3 Helmholtz Coils The presence of background fields in our interaction region must also be accounted for and trimmed out. This is done using a set of three Helmholtz coils in the northsouth, east-west, and up-down axis. The coils are much large then the interaction region and are outside the vaccum chamber. The advantage of this setup is the Experimental Setup 75 Vacuum Chamber Magnetic Field Magnet Magnet Anode Rings Cathodes Figure 4.19: The ion pump pumps by ionizing the gas and then accelerating the gas into the cathode plate where it reacts and is stuck. coils create a region of nearly uniform magnetic field with little gradient. This set up does not use exactly a helmhotz configuration which specifies that the coils should be seperated by the radius of the coils but it is close. This is restricted by our experimental setup in that the coils need to fit around the other components of the setup. This effect should be small, less the 1% change in total compensation field. We can find the field from these coils simply in terms of geometric descriptors and applied current. Starting from the on-axis field from a sing loop of wire. B(x) = µo IR2 (4.8) 3 2(R2 + x2 ) 2 Where x is the distance from the coil to the point and R is the radius of the coil. From this we can multiply by N for the number of turns in each coil and then substitute the distance between the coil and the interaciton region to find our field from the coils at the interaction region. B(x) = µo IR2 N 3 2(R2 + (− 2s )2 ) 2 + µo IR2 N 2(R2 + s 2 32 ) 2 , (4.9) Experimental Setup 76 Up Down East West North South Figure 4.20: Diagram of Helmholtz coils used to cancel the magnetic field in the center of the interaction region. Large diameter coils are used in order to have minimal gradients in the interaction region. Where s is the separation distance between the coils. Table 4.1 shows the conversion for all coils. Field North South East West Up Down Conversion 6.8 G/A 4.1 G/A 3.3 G/A Table 4.1: Conversion from applied current to magnetic field at interaction region. 4.4 Data Aquisition Data is recorded using a National Instruments PCI/MIO-16XE, 16 bit analog to digital converter. The data are recorded using LabView. The computer is connected to the synthesizer which the repetition rate is locked. To scan the Experimental Setup 77 frequency of the diode laser the computer steps the rep rate synthesizer which steps the frequency of frep and so the shifts frequency of the comb mode which the diode is locked to. LabView synchronizes the incoming data with the the scanned repetition rate. When scanning, the computer steps the synthesizer in 1 Hz increments and then averages for a set timescale. This is normally 500-1000 samples per channel when taking data. The scans increase over the range and then decrease back to the start value giving two scans for each run. The PMT signal, diode power, Fabry-Perot transmission, and beat note error signals for the offset frequency and diode beat note are recorded. 4.5 Collection Procedure The process of data collection requires the entire system to be stable for a period of a few hours. This has proved to be difficult because of the overall instability in the system. The diode laser and frequency comb are both highly sensitive to mechanical noise and well as changes in the conditions in the lab. The frequency comb oscillator must be kept extremely clean in order to maintain mode locked operation. Any condensation or dust on the crystal or mirrors results in a loss of power and so it will not mode lock. Both lasers are also temperature sensitive as changes in the ambient temperature change the cavity. This would not be an issue if the lab was reasonably stabile however we have recorded fluctuations of 15◦ F over the course of 24 hours. The first step in data collection is to adjust the wavelength of the diode laser to the frequency of the atomic transition. To find atoms the grating is modulated using a ±2 V triangle wave. The output of the PMT is viewed on an oscilloscope while changing the various parameters of the diode to tune the frequency. The grating is adjusted to get the approximate wavelength as measured by the OSA. The horizontal adjustment is used to tune the wavelength on the nm scale. The vertical adjustment is then used to adjust the feedback in order to increase the power as well as improve scanning response. The wavelength can also be adjusted using the temperature controller for the diode head. This is normally set around 19.2◦ C for the current Eagle Yard diode however this can operate in the range 18 − 22◦ C. By increasing the temperature the wavelength is increased but the power output decreases. Once we find the transitions we are interested in, we use the Fabry-Perot interferometer to make sure that the diode is scanning without Data and Analysis 78 mode hops and is stable for changes in the piezo. This is important as the locks become much less stabile if there are mode hops near the resonances. Once the offset frequency and repetition rate of the comb have been stabilized to the frequency standard, the beat note stabilizing the diode laser to the frequency comb must be found and stabilized. This is done by adjusting the specially overlap of the diode laser and comb light as well as adjusting the power of the comb such that it produces more light in the 670 nm region. Getting the f0 beat note and fb beat note to lockable levels is one of the continual challenges of the experiment as the comb tends produce more light in one frequency band but not the other. We have made improvements by increasing the sensitivity of the detection for both locks but this is still an area that would benefit from more work. If the beat notes are larger the system is more stable and the locks are less likely to jump, meaning data collection is more consistent. With diode laser locked to the frequency comb, data is collected by tuning the repetition rate of the frequency comb using the synthesizer. The repetition rate is scanned from an initial to final frequency and then back down to the initial frequency giving two data points for every frequency step. This scans the diode laser over the peaks and the PMT signal, repetition rate, power stabilization photodector, and Fabre-Perot signal are recorded. The increasing and decreasing scan provides a check for systematics such as lags in detection which might cause an offset. Chapter 5 Analysis and Results 5.1 Analysis The data recorded contain the fluorescence signal as a function of repetitional rate. To convert to absolute optical frequency we determine which transition we are observing by comparing the peak separation and relative amplitude to the known splittings. For each scan the f0 beat note frequency is recorded and from that and the repetition rate the mode number can be found. This then allows conversion to absolute frequency. The sign of f0 and fb are unknown and so this gives four possibilities for the frequency ν1 = nfrep + f0 + fb ν2 = nfrep + f0 − fb (5.1) ν3 = nfrep − f0 + fb ν4 = nfrep − f0 − fb . Here the sign of the offset frequency dependent on whether we see a sum or difference frequency of the doubled and normal light used to detect the offset frequency. The sign in the beat note for the diode laser stabilization is dependent on whether the diode laser is locked below or above one tooth of the frequency comb. We can compare this with the approximate frequency of the transition for the identified peaks to uniquely determine the mode number. With the scans converted to absolute frequency we then fit the transitions to a line shape model. For non saturated peaks the line shape can be modeled by a 79 Data and Analysis 80 combination of a Lorentzian and a Gaussian for each peak. This line shape is used because the atomic beam shape is given by a Gaussian distribution and the natural line width of the peak is a Lorentzian. This is not a perfect model but empirically it provides reasonable fits with unstructured residuals. The line shape model for a single transition is given by f (ν) = A fL γL2 /4 γL2 /4 + (ν − ν0 )2 +e − (ν−ν0 )2 2γ 2 G + B. (5.2) Here A is the overall amplitude of the peak, γL is the fractional lorentzian, γL is the width of the Lorentzian peak, γG is the width of the Gaussian peak, ν0 is the peak center, and B is an over offset used to fit the baseline. For spectra with multiple peaks we simply add more of the bracketed term and allow the amplitude and center frequency to vary for each peak. We keep the peak widths and fractional Lorentzian constant for multiple peaks as the width should not be dependent on transition only on the atomic beam an natural line width. Li7 D1 F = 2 -› 1 Li7 D1 F = 2 -› 2 50 Data 2012 Data 2013 Saturated Fluorescence Data 2015 Li7 D1 F = 1 -› 2 40 Li7 D1 F = 1 -› 1 x10 -3 30 20 10 0 800 1000 1200 1400 1600 1800 Figure 5.1: This plot shows the improvement in line shape due to the collimated beam. The red curve is the data from this work. The blue curve is data taken with the original atomic beam. The green is data taken using saturated fluorescence. The original plan for the measurement of these transitions was to use saturated fluorescence spectroscopy and so the broad line shape would not be a limiting factor. The full width at half max of the previous beam was 120 MHz and the current setup has a width of 16 MHz. Data and Analysis 81 This line shape model provides reasonable fits for peaks which are symmetric with no saturation. When there are asymmetries in the data we see clear structure in the residuals. This model also relies on the peaks being resolved as the line shape becomes more complicated when the peaks overlap. The atomic beam has bean narrowed yielding peaks with a full width at half maximum of ≈ 16 MHz meaning that all of the D1 lines are mostly resolved. The 6 Li hyperfine splitting in the excited state is 26 MHz meaning the tails of the peaks overlap however the peaks are resolved enough to easily get line shapes which accurately model the spectra. Figure 5.1 shows the line profile for data taken with a previous atomic beam. The blue curve is the initial atomic beam setup which gave line widths ∼ 120MHz. The broadness of the atomic beam resulted in many features of the spectra being hidden. This setup was initially designed to use saturated fluorescence spectroscopy which is not Doppler width dependent. The green curve shows the saturated fluorescence data that was taken in order to resolve the peaks. This was motivated by the idea that saturated fluorescence should result in Doppler width free features and resolve the transitions. This method was unsuccessful because the lines shape was not modeled with sufficient accuracy and crossover resonance complicated the line shape, see Ref. [34] for detailed analysis of this method. Figure 5.1 shows the data taken for this thesis with the new atomic beam in red. Here it is clear that the peaks are mostly resolved and the line width is ∼ 16 MHz. This is a large improvement over the previous data. Features such as the 6 Li D2 peak at the bottom of the 7 Li D1, F = 2 → 1 peak are now visible and can be accurately fit with the line shape given by Eq. (5.2). 5.2 Test of Frequency Standard This experiment uses a GPS steered SRS rubidium atomic clock as the frequency standard to reference the optical frequency comb. The atomic clock has very high stability in short term but will drift at longer time scales. To correct for this drift, the clock is steered to a GPS clock which on long time scales is very accurate. To measure the stability a frequency standard the most common technique is using an Allan deviation. Frequency standards tend to drift over long time scales, the Allen deviation compares successive sets of points in order to determine an Data and Analysis 82 3 GPS A 10 MHz Output vs SRS Rb Clock steered to GPS B Lucent Rb Clock vs SRS Rb Clock steered to GPS B Fractional Instability 2 -11 10 9 8 7 6 5 4 3 2 -12 10 0 1 10 2 10 3 10 10 Averaging Time (s) 4 10 Figure 5.2: Allan deviation comparing multiple frequency standards in the lab. The SRS atomic clock which is used as the frequency standard for the frequency comb has a accuracy when compared to the Lucent Clock of a part in 101 1 for the time scales that we collect data on resonance. This translates to a < 1 kHz uncertainty in the frequency standard. accuracy over long time periods. For a given frequency standard let ν(t) be the output of the frequency standard and νn be the ideal frequency. We can then define the fractional frequency as y(t) = ν(t) − νn . νn (5.3) The average fraction deviation for a given time interval from 0 to τ is then defined as the sum of y(t) over an interval. This can also defined as a continuously given by 1 x̄(t, ) = τ Z τ y(t)dt. (5.4) 0 Since y(t) is the derivative of x(t) we can write the nth average over some small time interval τ as ȳn = xn+1 − xn . τ (5.5) The Allen variance is then defined as [35] 1 1 σy2 (τ ) = h(ȳn+1 − ȳn )2 i = 2 h(xn+2 − 2xn+1 + xn )2 i. 2 2τ (5.6) Data and Analysis 83 This is result is normally presented as the Allen deviation given as the square root of the variance r q 1 σy (τ ) = σy2 (τ ) = h(xn+2 − 2xn+1 + xn )2 i. 2τ 2 (5.7) The Allen deviation is different from a standard deviation as it characterizes the stability by comparing the variance in a set of points as opposed to some fixed value. The SRS rubidium atomic clock in this experiment is compared to a second Lucent atomic clock as well as a GPS clock in Fig. 5.2. The stability in the SRS atomic clock steered by GPS gives an uncertainty of < 1 kHz when averaging for around 200 seconds. 5.3 Test of locks There are multiple checks for the quality of the locks. This is important as if the locks are not tight and consistent systematic shifts will be present in the data. The repetition rate lock is very consistent when counted and has very little frequency noise. The offset frequency and diode stabilization locks are less stabile as there is more frequency noise then on the repetition rate beat note. The lock error signals are recorded to give a indicator if they are have large frequency noise or if there are other issues such as consistent offsets. The first check of the locks is viewing the beat notes using an rf spectrum analyzer. When looking at the offset frequency the lock may appear to have frequency jitter if the beat note is not large enough. This will appear in the error signal as a large deviation from zero as the lock electronics correct. The other check is to look at the width of the beat note in frequency space. The narrower the beat note the tighter the lock, if the gain on the feedback is set to high the beat note will broaden and so have more frequency instability. A second check of the locks while collecting data is counting the beat notes using a precision frequency counter referenced to the atomic clock. The counter is accurate for rf frequencies on the hz scale. The beat notes for both the offset frequency and probe laser are counted, if the locks are good there is less then Data and Analysis 84 hz variation in counted frequency. These checks insure low uncertainty in the frequency stabilization of the probe laser. 5.4 Magnetic Field Evaluation The presence of Zeeman splitting from a non zero external magnetic field is an important systematic in this experiment. In order to achieve high accuracies in our measurement want to have as near to zero magnetic field as possible. The external field is mostly due to the Earth’s magnetic field. In order to compensate for this we use three Helmhotz coils which we use to zero the magnetic field in all three axis. We have made these coils about .5 meters in diameter to have as small a Residuals (mG) gradient as possible. We have used two methods to set zero field for the coils. The 0.4 0.0 -0.4 10 Magnetic Field (mG) 0 -10 -20 Fit Coefficients Background Field = -44.0 mG Slope = 1.4 G/A -30 -40 0 10 20 Current (mA) 30 40 Figure 5.3: Magnetic field at interaction region as a function of applied current through up down coils. Data is fit to a line to find zero field as well as calibration between applied current to coils and field at interaction region. first was using a flux gate magnetometer and zeroing the field in the interaction region before the chamber was in vacuum. This was done twice, a year apart with increased accuracy on the second iteration giving a residual magnetic field of 10 mG. The main source of uncertainty for these measurements is in the placement of the probe. In our first measurement we moved the probe one centimeter either direction in the axis of the field and saw a 30 mG shift in magnetic field. This gave us a very large uncertainty for the first measurement. We improved this in the second measurement to give an error of about 10 mG. These two measurements Data and Analysis 85 0.10 0.00 -0.10 -0.20 Coefficient values ± one standard deviation a =2.7313 ± 0.198 x0 =0.12379 ± 0.0187 b =16.681 ± 0.0568 19.0 Peak Width (MHz) 18.5 18.0 17.5 17.0 16.5 -0.6 -0.4 -0.2 0.0 Current (A) 0.2 0.4 0.6 Figure 5.4: Magnetic field at interaction region as a function of applied current through up down coils. Data is fit to a line to find zero field as well as calibration between applied current to coils and field at interaction region. agree with each other as shown in 5.1 which shows a stability in the system as these measurements were taken about a year apart. Axis Magnetic Field North-South 672.2 mG 35.4 mG East-West Up-Down 107 mG First Zero +- 30 mG 154 mA -8 mA 167 mA Second Zero +- 10 mG 127 mA -12 mA 157 mA Table 5.1: Magnetic Field Measured with flux gate magnetometer. The two measurements were taken a year apart. The uncertainty is from the probe position in the chamber. The second method used to evaluate the magnetic fields of our system was varying the magnetic field and then looking at the affect on line width of our transition. In this case the affect of non-zero magnetic field should appear as a broadening of our peak width. Our second method shows a clear increase in peak width with increased magnetic field in all three axis. Figure 5.4 shows an example of the correction for one axis of Data and Analysis 86 Field Minimum Using Meter (mA) Minimum from width data (mA) Up-down 157(10) 159 (8) 127(10) 124 (8) North-South -12(10) -7 (8) East-West Table 5.2: Zero magnetic field compensation current values for calibration using flux gate magnetometer and minimum based on broadening of spectral peaks. the field. This is fit to a parabola to find a minimum for each field. From this we are able to compare our two means of evaluating the magnetic field. This method is more precise the the probe method because when using the probe it is not certain that the probe is exactly where the atoms are interacting with the probe light. With the Helmholtz coils this effect should be small because the gradients in the center of the coils are near assumed to be near zero. The two methods agree for the value of the compensation current in order to have zero external field in all axes. 5.5 Evaluation of Probe Beam Alignment The alignment of the atomic beam with respect to the probe beam is extremely crucial for having symmetric line shapes such that the line shape models can accurately represent the data. This has been the most difficult systematic to address for several reasons. One of the issues in the alignment between the probe and atomic beam is that the sensitivity in the adjustment in the angle of the probe beam has less resolution than our ability to detect the misalignment. The angle of the probe beam is adjusted using the final mirror prior to the vacuum chamber. Originally we used a standard ThorLabs kinematic mirror mount with 1/4 − 80 threaded micrometers with a resolution of .1◦ . This mount had both stability issues and limited resolution. We changed to a Gimbal high stability mount which improved overall stability and gave slightly better resolution. This mount has a resolution of .02◦ . This spacing is still to large to accurately set the angle of the mirror to the level of detection. The first problem was finding a method to evaluate the symmetry of the peak in order to test the alignment. To do this we use a lock in amplifier with chop wheel to look at the contribution of the retro beam to the PMT signal. The probe beam 87 10 5 0 -5 -10 -15 x10 -3 Data and Analysis 1.6 Coefficient values ± 1 SD A1 =0.38491 ± 0.000832 C1 =666.01 ± 0.00061 WG =8.826 ± 0.00173 WL1 =27.068 ± 0.0501 FL =2.137 ± 0.0141 A2 =0.75853 ± 0.00304 C2 =666.31 ± 0.000652 WL2 =14.069 ± 0.0156 B =0.43338 ± 3.5e-005 M =0.0020008 ± 3.32e-006 Lockin PMT Data Fit Fit Residuals Lineshape Function Fluorescence Dip 1.4 1.2 1.0 0.8 0.6 620 640 660 680 700 720 Figure 5.5: This data is an example of the data used to align the probe laser with the atomic beam. The retro-reflected probe beam is chopped before the interaction region. This means we can use a locking amplifier to look at just the contribution of the retroreflected beam. This data is shown in red. If the probe beam is perpendicular to the atomic beam the saturation dip should be exactly symmetric in the line shape and the peak center for the line shape as well as the saturation dip should be the same. The data is fit in blue to a combination of the normally line shape composed of a Gaussian and Lorentzian (shown in black) minus the line shape for the saturation dip in green. is chopped after the vacuum chamber, before being reflected back into chamber shown in Fig. 4.18. The chopper wheel introduces some mechanical noise to the system and so was suspended from the unistrut such that it would not vibrate the optics table. The probe beam is operated in the saturation region such that the retro beam creates a dip at the center frequency because only one velocity class is excited when the laser is tuned on resonance (see Chapter 2). The dip is symmetric in the main peak when the probe and atomic beam are orthogonal. The center of the saturation peak and the main peaks should be the same if the two beams are orthogonal. Figure 5.5 shows one example of data taken with the lockin amplifier where the alignment is as close as possible given the resolution of the angle between Data and Analysis 88 0 x10 10-3 2 -3 4 -2 0.35 PMT Voltage (V) 0.30 0.25 0.20 Coefficient values ± 1 SD A1 =0.019708 \ ± 6.04e-005 C1 =573.88 ± 0.00255 WL =14.246 ± 0.0388 WG =7.7752 ± 0.00292 FL =7.7085 ± 0.204 A1S =0.094549 ± 0.00351 DS =0.12527 ± 0.00338 WLS =11.545 ± 0.0382 A2 =0.10669 ± 0.000146 C2 =665.83 ± 0.00194 A2S =0.66031 ± 0.0209 B =0.076665 ± 5.06e-006 M =0.0020027 ± 4.09e-005 0.15 0.10 560 580 600 620 640 660 Frequency (Hz - 446800000) 680 700 Figure 5.6: Example of the PMT combined PMT signal when collecting data for the alignment between the probe and atomic beam. The saturation dip is clear in the second peak but not present in the first peak because of the difference in saturation intensities for the two transitions. the beams. Here the dip is fairly centered in the PMT signal however there is still a visible offset between the saturation dip center and the line shape center. Ideally the saturation peak and line shape peak would have the center value, this would indicate that the probe beam and atomic beam are perpendicular to each other and there is no asymmetry in the line shape of the atomic beam. This data is fit to a Lorentzian plus a Gaussian for the main line shape, shown in black in Fig. 5.5 minus a Lorentzian for the saturation dip, shown in green. This is given by γL2 /4 f (ν) = A1 F L 2 γL /4 + (ν − ν1 )2 − +e (ν−ν1 )2 2γ 2 G − A2 2 γL2 /4 + B, 2 (γL2 /4 + (ν − ν2 )2 ) (5.8) where the first term is the line shape for the peak without the saturation dip and Data and Analysis 89 the second term is the lorentzian used to model the saturation dip. The center of the saturation dip is ν2 and the amplitude is given by A2 . A lorentzian is used for the saturation peak because the line shape does not depend on the velocity distribution of the atomic beam. Figure 5.6 shows the PMT signal for the combined beams. This is an example of how the saturation peak center changes for small changers in the beam alignment. This is as close to aligned as possible with the resolution in the mirror before the chamber. 5.5.1 Correction of Misalignment The misalignment in the probe beam with the atomic beam has been reduced as much as possible with the current setup and the alignment process outlined in the previous section. Unfortunately this still results in a shift in the data due to the misalignment. There are two ways to address this shift. The first is to correct aspects of the system in order to minimize the effect which will be addressed in the following section. The second is to correct for the shift when analyzing the data. When data are taken with both the probe beam and retro beam the recorded line shape is a combination of the contribution from both beams. If the power was equal in both beams then this would completely symmetrize the peak and remove any shift from the misalignment. Unfortunately because of the non-coated windows used for this data, the power in the retro beam is ≈ 60% of the incoming beam because of the losses to the windows. This makes fitting the line shape more difficult as it is the contribution of two non-symmetric peaks with different amplitudes. We can account for this asymmetry by using the line shape from data taken without the retro-reflected beam. This line shape is asymmetric because of either a asymmetric in the distribution of the atomic beam or a misalignment in the probe beam relative to the atomic beam. We can then fit this line shape using an interpolating function. This is used because the the peak cannot be fit it to a combination of a Lorentzian and a gaussian as used before as the asymmetries cause structure in the residuals. The contribution from the retro-reflected beam has this asymmetry mirrored because the propagation direction is reversed. In Data and Analysis 90 PMT Voltage (V) 0.05 — No RetroReflection Data — Retro-Reflection Data 0.04 0.03 0.02 0.01 620 640 660 680 700 720 Frequency (MHz - 446800000) Figure 5.7: Example of data used to fit the shift in from the misalignment between the probe beam and atomic beam. The Blue data is used as the base function for the interpolation function which is then used to fit the RetroReflection data. This is used to find a correction to the center frequency for the data taken with including the retro-reflected probe beam. order to fit the peak with contributions from both beams we start with line shape found from the peak from just one beam. This serves as a model for the line shape of the peak from both beams. Figure 5.7 shows the line shape model data in blue used for the interpolation. To fit the peak with with contributions from both beams the model line shape is mirrored over a center point and added to the line shape for single beam. This fit is given by L(ν) = A[Lm ((ν − δ) − ν0 ) + fR Lm (−(ν + δ) − ν0 )] + B (5.9) where Lm is the interpolated line shape from the non-retroreflection data, A is the overall applitude, fR is the fraction of the retroreflected beam, ν0 is the center frequency, δ is the mirror point, and B is a baseline offset. With this line shape model we can then fit the line shape of the data with both beams. With this method we were able to find fits which appear to have no structure to the residuals Data and Analysis 91 0.010 Residuals 0.0010 0.005 0.0005 50 100 150 -0.005 PMT Voltage (V) -0.0005 0.05 — Data — Interpolated Fit 0.04 0.03 0.02 0.01 620 640 660 680 700 Frequency (MHz - 446800000) Figure 5.8: Data shown is taken with contributions from both the probe beam and retro reflected probe beam. This is fit to the interpolated line shape for one beam that has been mirrored over a center value and multiplied by a relative amplitude to account for the contribution from both beams. This fit appears to have no structure to the residuals. as shown in Fig. 5.8. From this we can find the true frequency of the transition which is free of the shift present from the beam misalignment. When using this method the fractional retro contribution remains constant at .57 ± .02 for all fits. This agrees with the contribution expected as the loss in power due to the windows on the vacuum chamber is ≈ 40%. The peak center frequency is also independent of the frequency used as the mirror point. We also checked the fit by using different base fines to generate the line shape model. These fits were consistent between different base files in both retro beam contribution and center frequency. Applying this line shape model to our data we see that the scatter in center frequency is less then 100 kHz. We re fit the data using multiple different line shape model scans and then take the standard deviation of the center frequencies found with different models plus the statistical uncertainty in weighted mean of this data Data and Analysis 92 for our error. Using this method we find a center frequency of 446800666.439±.009 MHz for the 7 Li F = 1 → 2 transition. This gives our error bound for beam misalignment can be reduced to 9 kHz. The overall shift from the standard line shape model using a combination of a Lorentzian and a Gaussian is found to be -200 kHz. This correction is added to the optical frequencies presented. 5.6 AC Stark Measurement The expected AC Stark shift for the D1 is estimated in Section 2.6.1. For these data the intensity of the beam is 1.5 mW/cm2 , using this intensity we find that the upper bound in the uncertainty due to the AC Stark shift for each transition is given in Table 5.3. These uncertainties can be further limited by experimentally measuring the AC Stark shift and correcting for the shift to the optical frequencies. Transition 6 Li F = 1/2 → 1/2 F = 1/2 → 3/2 F = 3/2 → 1/2 F = 3/2 → 3/2 Expected Shift (kHz ± 10% -30 4 -15 15 7 Li F =1→1 F =1→2 F =2→1 F =2→2 -2 8 -5 5 Table 5.3: Estimated AC Stark shifts for beam intensity of 1.5 mW/cm2 . These values are a reasonable upper bound on the uncertainty due to the AC Stark shift. The effect is larger in 6 Li as the hyperfine splitting of the upper state is smaller and so the effect is stronger. 5.7 Isotope Shift and Hyperfine Structure Splitting The isotope shift is calculate by finding all of the D1 transition frequencies for 6 Li and 7 Li. Examples of the data used to find these optical frequencies are shown in Data and Analysis 93 Transition 6 Li D1 6 Li D1 cog 7 Li D1 6 Li D1 cog Fg 3/2 3/2 1/2 1/2 Fe 1/2 3/2 1/2 3/2 Frequency (MHz) 446 789 502.585 (27) 446 789 528.723(24) 446 789 731.834 (44) 446 789 756.973 (32) 446 789 596.093(42) 2 2 1 1 1 2 1 2 446 799 771.089 (12) 446 799 862.950(12) 446 800 574.507(17) 446 800 666.439(11) 446 800 129.800(26) Table 5.4: Optical Frequencies for the D1 transition infor 6 Li and 7 Li. Fig. 5.9, 5.10 and 5.11. These were fit using the line shape of a combination of a Lorentzian and Gaussian given by Eq. (5.8). Each scan is fit using a weighted fit where the weighting is given by the error in each point. By taking multiple scans of each transition and then averaging the data using a weighted mean we are able to further reduce our statistical uncertainty. We then correct for the misalignment between the atomic beam and probe laser as outlined above. This appears as a linear shift to all the peaks. The shift from the misalignment is subtracted from the optical frequencies of the peak centers. This systematic shift will not change the isotope shift measurement or fine structure measurement as it appears as a linear shift in all the data. The corrected optical frequencies given in Table 5.4. Systematic Statistical Beam Alignment Zeeman Effect Stark Shift Reference 7 Li D1 F = 1 → 2 6 Li F = 3/2 → 1/2 4 20 9 9 <1 <1 2 15 <1 <1 Total Uncertainty 11 27 Table 5.5: An example of the uncertainty budget for each center frequency. This is the error budget for 7 Li D1 F = 1 → 2. The errors are added in quadrature in order to get the total error in value. The data for the 7 Li transitions have a better signal to noise ratio then 6 Li because the peak amplitude is much smaller because the difference in natural abundance. The statistically biggest issue in these data is that the F = 1/2 → 1/2 peak is not resolved and has a much smaller amplitude and so the line shape model has higher Conclusions 94 uncertainty. For determining the isotope shift we will set the hyperfine splitting of the 6 Li F = 1/2 → F 0 equal to that determined from the 6 Li F = 3/2 → F 0 transition. This gives a hyperfine splitting of 26.138(35) and an corrected optical frequency for 6 Li F = 1/2 → 1/2 of 446 789 730.834(44). This value is used for the calculation of the isotope shift. Transition D1 Shift (MHz) Reference 10533.707(50) This Work 10533.763(9) Sansonetti [2] 10534.26(13) Walls [5] 10534.039(70) Noble [4] 10534.215(39) Das [3] Table 5.6: Isotope Shift Frequency for this work and previously published measurements. To calculate the isotope shift, the center of gravity for each transition must be calculated to find the overall D1 line for both isotopes. This is calculated by weighting the frequency of each transition by the degeneracy of the state. The optical frequencies used for this calculation are given in Table 5.4. An example of the error budget for two optical transitions is outline in Table 5.5. The uncertainty in the 6 Li transitions is significantly greater then the 7 Li. This is due to both the increased statistical uncertainty and larger AC Stark shift in 6 Li due to the smaller hyperfine splitting of the excited state. In calculating the isotope shift the uncertainty in the 6 Li center of gravity dominates the uncertainty in the isotope shift. We determined that the isotope shift for the D1 transition is 10533.707(50) MHz. This is within the combined uncertainty of the most recent measurement published by Sansonetti et al. [2] but does not agree with the other published values shown in Table 5.6. In order to resolve this discrepancy we need to further limit our systematic uncertainty. The hyperfine splitting measurements of both the ground state and excited state of the D1 transition are shown in Table 5.7. The ground state measurements agree with Sansonetti et al. [2] within the uncertainty in our measurement. It also agrees with the rf spectroscopy measurement by Beckmann [36] for 7 Li but not for 6 Li. The excite state measurements agree with the previous measurements within the combined uncertainty for each measurement except from Das et al [3]. These results would indicate that there is more work left in understanding the uncertainties present in the measurement, especially for 6 Li. Conclusions 95 Interval 7 Li 2s 2 S hfs Splitting (MHz) Reference 803.489(16) This Work 803.493(14) Sansonetti [2] 803.504 086 6(10) Beckmann [36] 6 Li 2s2 S hfs 228.250(35) 228.215(17) 228.205 261(3) This Work Sansonetti [2] Beckmann [36] 7 Li 2p2 P1/2 hfs 91.896(16) 91.887(9) 92.020(50) 92.047(6) This Work Sansonetti [2] Walls [5] Das [3] 6 Li 2p2 P hfs 26.138(35) 26.111(17) 26.079(46) 26.091(6) This Work Sansonetti [2] Walls [5] Das [3] Table 5.7: Hyperfine splitting for the D1 transition frequencies for 6 Li and 7 Li. Conclusions 96 x10 -6 Coefficient values ± one standard deviation A1 =0.0016551 ± 3.6e-05 A2 =0.0081582 ± 0.000183 C1 =1574.8 ± 0.0418 C2 =1666.6 ± 0.0129 WG =7.6771 ± 0.0805 WL =14.498 ± 0.121 FL =2.371 ± 0.0792 B =-0.00084804 ± 1.16e-05 600 400 200 0 -200 -400 -3 25x10 Li7 D1 F = 1 -› 2 Data Fit Residuals PMT Voltage (V) 20 15 10 5 Li7 D1 F = 1 -› 1 0 1550 1600 1650 Frequenecy (MHz - 446799000) 1700 Figure 5.9: Data for 7 Li D1 F = 1 → F 0 transitions. Peaks were fit to a combination of a Lorentzian and a Gaussian. Conclusions 97 x10 -3 Coefficient values ± one standard deviation A1 =0.053591 ± 0.000594 C1 =771.26 ± 0.01 A2 =0.0082337 ± 9.82e-05 C2 =803 ± 0.0392 A3 =0.052368 ± 0.000582 C3 =863.09 ± 0.0098 WG =7.949 ± 0.0374 WL =17.878 ± 0.105 FL =1.5505 ± 0.03 B =0.018799 ± 5.36e-05 2 1 0 -1 -2 0.14 Li7 D1 F = 2 -› 1 Data Fit Residuals Li7 D1 F = 2 -› 2 PMT Voltage (V) 0.12 0.10 0.08 Li6 D2 F = 1/2 -› 1/2, 3/2 0.06 0.04 750 800 Frequency (MHz - 446799000) 850 Figure 5.10: Data for 7 Li D1 F = 2 → F 0 transitions. Peaks were fit to a combination of a Lorentzian and a Gaussian. We see some structure to the residuals but they are mostly small variations. Coefficient values ± one standard deviation a1 =0.0095482 ± 0.000762 c1 =502.85 ± 0.038 a2 =0.011436 ± 0.000911 c2 =529.09 ± 0.0315 a3 =0.0012391 ± 0.000107 c3 =732.05 ± 0.27 a4 =0.0084791 ± 0.000679 c4 =757.11 ± 0.0402 wg =6.611 ± 0.0503 wl =26.11 ± 1.57 fl =0.88997 ± 0.152 b =0.040679 ± 1.87e-05 Conclusions 98 x10 -3 1.0 0.0 -1.0 Li6 D1 F = 3/2 -› 1/2 60x10 Li6 D1 F = 3/2 -› 3/2 -3 PMT Voltage (V) Li6 D1 F = 1/2 -› 3/2 55 Data Fit Residuals 50 Li6 D1 F = 1/2 -› 1/2 45 40 500 600 700 Frequency (MHz - 446800000) 800 Figure 5.11: Data taken on 6 Li D1 transitions. This transition has a much smaller amplitude then the 7 Li D1 transitions and so the signal to noise ratio is not a good as the 7 Li measurements. Each peak is fit to a combination of a Lorentzian and gaussian. Chapter 6 Conclusions The measurements of the D1 transition in the previous section show reasonable agreement with the previously published measurements. There is more work to be done to fully understand the uncertainties associated with the frequency measurements. With the measurement of the D1 complete we will move on to the D2 transitions. Most of the systematics associated with the D2 transitions are the same as those for the D1 transitions however there are other effects that were not present in the D1 lines. These include unresolved hyperfine structure as well as polarization effects outlined by Brown et al [1]. The hyperfine splitting of the D2 exited state is less the natural line width of lithium. When probing these transitions the peaks are not resolvable and so the line shape is complex. There is also interference effects dependent on the polarization of the probe laser relative to the detection. 6.1 Improvements to Apparatus In order to improve our error limit on the alignment between the probe beam and atomic beam we have replaced the input windows to the vacuum chamber which the probe beam travels through. If the retro reflected beam and probe beam have the same power then the contribution from both beams will be the same. Since the beams propagate from opposite directions this will symmetrize the spectral peaks. This will eliminate the asymmetry in the peak and put a lower error bound on the uncertainty. The windows that were used for the data in this work were 99 Conclusions 100 glass windows that reflects ≈ 20% of the laser light. Since the retro reflected probe beam travelled through the windows of the vacuum chamber twice before interacting with the atoms, the power in the retro-reflected beam was ≈ 60% of the input beam the spectral peaks. While we can correct for this using line shape models a truly symmetric peak would mean that our error bound would be lower. The amplitude of the beat notes for the the offset frequency of the comb and the diode laser stabilization are a consistent challenge in this experiment. While the frequency comb spans a frequency an optical octave, the power output per mode is not uniform over this range. Both the output of the Ti:Sapphire laser as well as the alignment of the micro-structure fiber effect the distribution of power through the output spectrum. This causes an constant compromise between tuning the alignment in order to get more power for the offset frequency beat note and the diode stabilization. To improve this we are working to improve the detection of both beat notes in order to make the power requirements lower. We are working on a new detection setup for the offset frequency using a Menlo Systems avalanche photodetector which is more sensitive the previous amplified photodetector. This should improve the detection of the beat note making it easier to stabilize. 6.2 AC Stark Measurement The only systematic that has not been fully evaluated for the D1 transition is the AC Stark shift. To measure this effect we will scan each transition with multiple powers as derived in Chapter 2 the shift will be greater for the 6 Li transitions. The shift should be linear with respect to power so can be extrapolated to zero. Measuring this effect will limit the uncertainty further then the estimation provided in the previous section. 6.3 Finalize Uncertainties In this work we have set an upper bound on all the uncertainties related to the measurement of the optical frequencies for the D1 transition. Several of these bounds can be improved with future work. The statistical error, particularly in the 6 Li data can be improved by taking more data to limit the uncertainty. Taking Conclusions 101 more data over the course of several weeks will also insure that the system is self consistent over long time periods. The new AR coated probe beam windows on the vacuum chamber should also provide a lower error on the uncertainty in the alignment between the probe laser and atomic beam. With these improvements we should be able to reduce the total uncertainty in the isotope shift measurement to less the 20 kHz from the 50 kHz uncertainty found in this data. Bibliography [1] Roger C. Brown, Saijun Wu, J. V. Porto, Craig J. Sansonetti, C. E. Simien, Samuel M. Brewer, Joseph N. Tan, and J. D. Gillaspy. Quantum interference and light polarization effects in unresolvable atomic lines: Application to a precise measurement of the 6,7 li d2 lines. Phys. Rev. A, 87:032504, Mar 2013. doi: 10.1103/PhysRevA.87.032504. URL http://link.aps.org/doi/ 10.1103/PhysRevA.87.032504. [2] Craig J. Sansonetti, C.E. C.E. Simien, J.D. Gillaspy, Joseph N. Tan, Samuel M. Brewer, Roger C. Brown, Saijun Wu, and J.V. Porto. Absolute frequency measurements of the lithium d lines: Precise determination of isotope shifts and fine-structure intervals. Physical Review Letters, 107(5), July 2011. [3] Dipankar Das and Vasant Natarajan. Absolute frequency measurement of the lithium d lines: Precise determination of isotope shifts and fine-structure intervals. Phys. Rev. A, 75:052508, May 2007. doi: 10.1103/PhysRevA.75. 052508. URL http://link.aps.org/doi/10.1103/PhysRevA.75.052508. [4] G. A. Noble, B. E. Schultz, H. Ming, and W. A. van Wijngaarden. Isotope shifts and fine structures of 6,7 Li d lines and determination of the relative nuclear charge radius. Phys. Rev. A, 74:012502, Jul 2006. doi: 10.1103/PhysRevA.74.012502. URL http://link.aps.org/doi/10.1103/ PhysRevA.74.012502. [5] J. Walls, R. Ashby, J.J. Clarke, B. Lu, and W.A. van Wijngaarden. Measurement of isotope shifts, fine and hyperfine structure splittings of the lithium d lines. The European Physics Journal D, 22, January 2003. [6] H. Orth, H. Ackermann, and E.W. Otten. Fine and hyperfine structure of the 22 p term of 7 li; determination of the nuclear quadrupole moment. Z. Physics A, 273, April 1975. 102 Conclusions 103 [7] Mariusz Puchalski and Krzysztof Pachucki. Quantum electrodynamics corrections to the 2p fine splitting in li. Phys. Rev. Lett., 113:073004, Aug 2014. doi: 10.1103/PhysRevLett.113.073004. URL http://link.aps.org/ doi/10.1103/PhysRevLett.113.073004. [8] Z.-C. Yan, W. Nörtershäuser, and G. W. F. Drake. High precision atomic theory for li and be+ : Qed shifts and isotope shifts. Phys. Rev. Lett., 100: 243002, Jun 2008. doi: 10.1103/PhysRevLett.100.243002. URL http:// link.aps.org/doi/10.1103/PhysRevLett.100.243002. [9] G. W. F. Drake and Zong-Chao Yan. Asymptotic-expansion method for the evaluation of correlated three-electron integrals, year = 1995. Physical Review A, 52(5), November . [10] Jacek Bieroń, Per Jönsson, and Charlotte Froese Fischer. Large-scale multiconfiguration dirac-fock calculations of the hyperfine-structure constants of the 2 s 2 s1/2 , 2 p 2 p1/2 , and 2 p 2 p3/2 states of lithium. Phys. Rev. A, 53:2181–2188, Apr 1996. doi: 10.1103/PhysRevA.53.2181. URL http: //link.aps.org/doi/10.1103/PhysRevA.53.2181. [11] M. Horbatsch and E. A. Hessels. Shifts from a distant neighboring resonance. Phys. Rev. A, 82:052519, Nov 2010. doi: 10.1103/PhysRevA.82.052519. URL http://link.aps.org/doi/10.1103/PhysRevA.82.052519. [12] Steven T. Cundiff and Jun Ye. Femtosecond optical frequency combs. Reviews of Modern Physics, 75, January 2003. [13] Christopher J. Foot. Atomic Physics. Oxford, 2005. [14] Gordan W. F. Drake, editor. Atomic,Molecular, and Optical Physics Handbook. American Institute of Physics, 1996. [15] J.J Sakuri. Modern Quantum Mechanics. Addison Wesley, 1985. [16] B.H. Brandon and C.J. Joachain. Physics of Atoms and Molecules. Longman, 1983. [17] David J. Griffiths. Introduction to Quantum Mechanics. Pearson, second edition, 2004. Conclusions 104 [18] P. A. M. Dirac. The quantum theory of the electron. Proceedings of the Royal Society of London. Series A, Containing Papers of a Mathematical and Physical Character, 117(778), Feb 1928. [19] Igor I. Sobelman. Atomic Spectra and Radiative Transitions. Springer, 1992. [20] David J. Griffiths. Introduction to Electrodynamics. Pearson, third edition, 1999. [21] Alan Corney. Atomic and Laser Spectroscopy. Oxford Science Publications, 1977. [22] Dmitry Budker, Derek Kimball, and David DeMille. Atomic Physics. Oxford, Berkeley, California, second edition, 2007. [23] Harold J. Metcalf and Peter van der Straten. Laser Cooling and Trapping. Springer, 1999. [24] W. Demtroder. Laser Spectroscopy. Springer, 2003. [25] T. M. Fortier, A. Bartels, and S. A. Diadems. Octave-spanning ti:sapphire laser with a repetition rate > 1 ghz for optical frequency measurements and comparisons. Optics Letters, 7, 2006. [26] David J. Jones, Scott A. Diddams, Jinendra K. Ranka, Andrew Stentz, Robert S. Windeler, John L. Hall, and Steven T. Cundiff. Carrier-envelope phase control of femtosecond mode-locked lasers and direct optical frequency synthesis. Science, 288(28), April 2000. [27] Albrecht Bartels. Gigahertz Femtosecond Lasers. Springer, 2005. [28] S. B. Bernfeld. Stabilization of a femtosecond laser frequency comb, 2009. [29] B. J. Eagleton, C Kerbage, P. S. Westbrook, R.S. Windeler, and A. Hale. Microstructured optical fiber devices. Optics Express, 9(13), December 2001. [30] J. Baron. Precision spectroscopy of atomic lithium with optical frequency comb, 2012. [31] Carl E. Wieman and Leo Hollberg. Using diode lasers for atomic physics. Review of Scientific Instruments, 62(1):1–20, January 1991. URL http:// link.aip.org/link/?RSI/62/1/1. Conclusions 105 [32] Frank L. Pedrotti, Leno S. Pedrotti, and Leno M. Pedrotti. Atomic Physics: an exploration through problems and solutions. Pearson, thrid edition, 2007. [33] Robert W. Boyd. Nonlinear Optics. Academic Press, 2003. [34] Michael E. Rowan. Doppler-free saturated fluorescence spectroscopy of lithium using a stabilized frequency comb, 2013. [35] W.J Riley. Handbook of Frequency Stability Analysis. NIST Special Publications, 2008. [36] A. Beckmann, K.D Boklen, and D Elke. Precision measurements of the nuclear magnetic dipole moments of 6 li, 7 li, 2 3na, 3 9k and 4 1k. Z. Physik, 270, November 1974.