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The slow-light effect: An experimental study of light propagation through rubidium vapour Mark Zentile Department of Physics, Durham University, South Road, Durham, DH1 3LE, UK (Dated: June 28, 2012) This report presents a study of the slow-light effect in a 2 mm long cell containing thermal rubidium vapour. The model for the electric susceptibility previously developed in our group has been used, along with a Fourier analysis, to model the pulse propagation and is then compared with experiment. Two experimental methods were used where the results show agreement. Advantages and disadvantages of the different techniques are discussed along with further improvements that could be made. Measurements of absolute absorption have also been carried out to verify the electric susceptibility theory, which was then used to verify that the presence of buffer gas contained within one particular experimental cell cannot be considered negligible. A discussion of the future outlook of our project is also presented. CONTENTS I. Introduction A. Motivation for smaller cells II. Theory A. The phase shift and absorption from the electric susceptibility B. Equation for the electric susceptibility C. Absolute absorption D. Optical Pulse Propagation 1. Narrowband approximation III. Experiments A. Absolute Absorption 1. Experimental Method 2. Results 3. Discussion 4. Conclusion B. Slow-light 1. Experimental Method 2. Results 3. Discussion 4. Conclusion I. 1 2 3 3 3 4 4 4 5 5 6 7 7 9 9 9 10 11 11 IV. Future Outlook 12 A. Tunable laser lock using the Faraday effect in high magnetic fields 12 B. Optical Switch 13 Acknowledgements 13 A. Fitting with simulated annealing 13 B. Laser locking by polarisation spectroscopy 14 C. A Monte-Carlo method for theoretical photon counted pulses 14 References 15 INTRODUCTION The interaction of light with atoms or molecules in thermal vapours has become of great interest. The electric susceptibility of the vapour is essential in characterising this interaction, and once known can be used to quantitatively predict a wide variety of physical phenomena. The aim of this report is to present an experimental study of the slow-light effect in a 2 mm long rubidium vapour cell. This report shows how the model for the electric susceptibility, which has previously been developed in the slowlight project, has been applied for this purpose. There has been much interest in recent years on the phenomenon of slow-light [1, 2]. It is characterised by the situation where the light pulse velocity is much less than that of continuous-wave light, and is realised in systems where there is a large derivative of the refractive index with frequency of light. Slow-light increases the amount of time a light pulse spends in the medium, and so can greatly increase the atom-light interaction. This means that processes, such as all optical switching [3], image rotation [4] and an optical delay line [5] can be realised in experimental set-ups of modest length. A slow light medium can also increase the sensitivity of interferometers [6, 7]. When combined with the Faraday effect [8], a slow light pulse placed off resonance can act as a sensitive atomic probe [9]. Electromagnetically induced transparency (EIT) [10] is often used to create large pulse delays [11, 12] due to the extremely (spectrally) narrow transparent features that can be achieved. However, one drawback of this is that it requires pulses with low bandwidth to avoid distortion, which corresponds to relatively long (of the order of a microsecond) pulses. For communication purposes, shorter pulses means more information can be sent in any given time. However, slow light using EIT gives the ability to store light [13], by switching the pump beam off while the pulse is in the medium, giving the possibility of quantum memory [14]. For the Slowlight project in AtMol we use < 800 ps pulse widths. Knowledge of the electric susceptibility, χ, of the 2 atomic vapour is essential in understanding and performing experiments in pulse propagation. A spectroscopic measurement is all that is required to determine quantities such as pulse delays (dispersion can be calculated from absorption [15, 16]). However, a model of χ allows experiments to be modelled and optimised before being built. Also, it allows many phenomena other than pulse propagation to be investigated, of which some have been investigated in the slowlight project. One is quantitative spectroscopy [17–20], which is essential in characterising the properties of atomic or molecular transitions, and has applications in measuring the Boltzmann constant [21– 23] and molecular fingerprinting [24], amongst many others. Another phenomenon investigated is that of Faraday rotation [20, 25], which can be used to make an optical isolator [26], dichroic beam splitter [27] or filter [28] and a laser frequency locking signal [29], to name but a few. The excellent agreement between experiment and theory already seen in references [17–20, 25] gives us confidence in our model. Due to equipment constraints, the vapour cell that was used for most of the experimental data in this report contained an unknown quantity of an unknown species of buffer gas. Our model currently does not include the effects of broadening and shifts due to buffer gasses, and although it should be relatively simple to incorporate empirically [30], it will still be very difficult to identify the buffer gas species and pressure. However, A study of the slow light effect should not be hindered by the presence of the buffer gas, because as previously mentioned, spectroscopic measurement can provide all the information about pulse delay times. However, using this cell for future experiments may be difficult since a good theory prediction might be hard to achieve. This is why measurements of absolute absorption have been done to see if the buffer gas can be considered significant. All our experiments are done with rubidium vapour, rather than any other choice of atom or molecule, for three reasons. The first is that our theoretical model for χ is based on alkali metal atoms, due to relative simplicity of a hydrogen-like system with a quantum defect [31]. The second is vapour pressure. Heating a 2 mm vapour cell from room temperature to around 200◦ C allows us to go from an optically thin medium to an optically thick one, giving us a full range of control of this experimental parameter. We have found that it is relatively simple to heat the vapour cell to this range of temperatures using ceramic resistors. This contrasts to sodium and potassium, where temperatures need to be ∼ 100◦ C and ∼ 300◦ C hotter respectively to achieve the same vapour pressure [32], which creates more of an experimental challenge. The third reason is that Rubidium D1 and D2 transitions are resonant at ∼ 795 nm and ∼ 780 nm respectively, where there exist relatively cheap diode lasers that are convenient to work with. A. Motivation for smaller cells The absorption of continuous-wave monochromatic light by a medium of length L is given by the well known Beer-Lambert law [33]: I = I0 exp (−αL) (1) where I is intensity after the medium, I0 is the initial intensity and α is the absorption coefficient. Interesting physical phenomena such as Rydberg blockade [34], the cooperative Lamb shift [35, 36] and saturated opacity [37], can be seen at large atom number densities. This means that α will be large (see section II C) and so using conventional cell lengths of a few centimetres the medium becomes optically thick. This means that a probe beam cannot be used to extract information about the sample. The solution to this is to make L much smaller hence making the exponential of the product −αL nonnegligible. Another reason to work with a small cell, and is of particular interest for the future outlook of our project, is the realisation of an optical switch [3, 38] using side pumping (see section IV B). To access the same volume of the dense atomic vapour for two crossed beams, a thin cell is required (see Fig. 1). FIG. 1. Schematic of an optical switch using a dense atomic vapour with two crossed beams. The side beam is resonant and so is fully attenuated at a short depth. For maximum anisotropy of the ground state atoms, and hence maximum efficiency, there should be as much overlap of the path of the pump and probe beams as possible. Another reason to work with smaller cells is to create light and compact instruments [26, 39–41], that allow mobile devices to be constructed. 3 II. A. THEORY B. The phase shift and absorption from the electric susceptibility For a particular transition, labelled j, we can write χj as [17] The electric susceptibility, χ, of an atomic vapour characterizes both its absorptive and dispersive properties. We can see this by writing χ (a function of angular frequency ω) in terms of the relative permittivity [42], r ≡ = 1 + χ, (2) 0 where is the permittivity in the medium. In the electric dipole approximation (magnetic response of the medium is negligible at optical frequencies), the refractive index, n is simply given by the square root of r [42]. The definition of the refractive index is the ratio of the speed of light in vacuum to the phase velocity in the medium. With this it is easy to show nω0 k = nk0 = , (3) c where k is the wave number in the medium, k0 is the wave number of the incident light before entering the medium, ω0 is the angular frequency of the incident light and c is the speed of light in a vacuum. Now, using the equation of a plane wave, at depth z in the medium and at time t [42], we see that ~ = E~0 exp (i [kz − ω0 t]) , E ~ = E~0 exp (−nI k0 z) exp (i [nR k0 z − ω0 t]) , E (4) where n is allowed to be complex and is decomposed into its real (nR ) and imaginary parts (nI ). Using the binomial expansion and noting that χ is small for atomic vapours (at densities we can achieve experimentally) we get χ (5) n≈1+ , 2 χR nR ≈ 1 + , (6) 2 χR nI ≈ . (7) 2 This gives us the result h i ~ = E~0 exp − χI k0 z exp i k0 z − ω0 t + χR k0 z , E 2 2 (8) where we can immediately identify a phase shift of χR k0 z. (9) ∆φ = 2 Now using the relation [43] n0 c ~ 2 I= |E| , 2 (10) (valid for harmonic fields) and equation (1) we can also identify the absorption coefficient, α = k0 χI . Equation for the electric susceptibility (11) χj (∆j ) = c2j d2 N sj (∆j ) , h̄0 (12) where cj is the transition strength factor, d is the reduced dipole matrix element, N is the number density, h̄ is the reduced Planck constant, 0 is the vacuum permittivity, sj (∆j ) is the line-shape of the transition. ∆j is the angular detuning defined as ∆j ≡ ωL − ωj , where ωL is the laser angular frequency and ωj is the natural angular frequency of the transition. The total value of χ is given by summing over all contributions P from individual electric dipole transitions, χ (∆) = j χj (∆), and is a function of the detuning around a defined global linecentre. For this report we have chosen, for convenience, to use the weighted average of the transition frequencies in the hyperfine manifold. In this report we use the D1 transition (52 S1/2 → 52 P1/2 ) and define the line-centre to be (2π × 377 107 407.299 MHz). Transition frequencies at a given magnetic field are calculated using methods given in [20]. The line-shape factor sj (∆j ) is obtained by a convolution between the (complex) line-shape factor in the absence of Doppler broadening with a normalised Gaussian distribution [17]. The line-shape factor in the absence of Doppler broadening contains broadening due to natural line width, Γ0 , and collisional broadening, Γcol . In a rubidium vapour cell, Γ0 is effectively equal for all hyperfine transitions and magnetic sub-levels to the accuracy that we can measure. For the D1 transition, the experimentally determined value of Γ0 = 2π × (5.746 ± 0.008) MHz [44] is used. For a rubidium vapour cell without buffer gas Γcol has only a contribution from self-broadening and can be calculated using the treatment given in [19]. However, due to the presence of an unknown buffer gas at an unknown pressure, the total Lorentzian line-width, Γtot = Γ0 + Γcol , is allowed to float when fitting to data. The collisional broadening parameter is again approximated to be equal for all hyperfine transitions and their magnetic sub-levels, as well as isotopes. Also, there should exist a frequency shift due to energy level changes in collisions, but this has not been taken into account. No deviation from the validity of these approximations [45] has been seen in vicinity of experimental conditions available to us [19], however this has not been tested in the presence of buffer gas. All these considerations leave a line-shape factor equal for all transitions, with the only difference being the obvious shift in frequency due to the hyperfine interaction. The overall rubidium atomic vapour number density, N , is given by an equation in [32]. It should be noted that N is strongly temperature dependent. The fractions of this number density that are either of the naturally abundant isotopes 85 Rb or 87 Rb area expected to be given by 4 the abundance in the metal reservoir. The atoms are assumed to be evenly distributed among the ground state energy levels. This is justified as the Boltzmann factor [46] is very close to one for the two ground states, while being negligible when considering a thermal excitation to either P-state. A weak probe beam must be used so as to not pump the atoms into the dark ground state [47]. C. Absolute absorption Recalling the Beer-Lambert law given in equation (1), we now define the transmission T ≡ I = exp (−α(∆, T )L) I0 (13) which can be seen as simply normalising the input intensity to one. This is convenient because it retains all the relevant information and means measurements with different initial intensity can be easily compared. Equation (11) gives the absorption coefficient which is a function of ∆ and temperature, T . Each individual χI,j has the form of a Voigt profile [48], arising from a convolution between the Lorentzian line shape due to homogeneous broadening mechanisms (full width at half maximum given by Γtot ) and a Gaussian due to the MaxwellBoltzmann distribution of velocities at a given temperature. When comparing theoretical and experimental spectra, several variables can be extracted from the data by numerical fitting. If using a vapour cell containing rubidium that is not at its natural abundance, the ratio between the isotopes 85 Rb and 87 Rb will need to be determined for the cell and can be extracted from fits. This only needs to be done once and then the fraction can be kept as a constant for future fits. The temperature of the vapour often needs to be extracted from a fit because the spectrum is a strong function of temperature and cannot be measured precisely or accurately enough with our current equipment constraints. The Lorentzian width is fully determined by the temperature of the cell, but as mentioned earlier, due to the presence of an unknown buffer gas this also needs to be fitted. When a magnetic field B is applied, its value can be extracted from a fit. No effort is made to shield the vapour cells from the background field, but it has been seen that assuming it to be zero is a valid approximation for measurements of absolute absorption [17]. Issues can arise when fitting with many parameters, or the initial guesses to those parameters are poor. Appendix A describes these issues and how they are dealt with. D. and absorptive properties. We have seen earlier how to extract the phase shift and absorption of monochromatic continuous-wave light from the electric susceptibility. Pulses are characterised by a sharp change in intensity with time and are clearly not monochromatic continuous-wave light. The technique for dealing with this is to write the pulse as a superposition of continuouswave light of different frequencies, we can then find the phase shift and absorption of each component. To do this, we first use equation (10) to relate the intensity the initial pulse (as a function of time), with the magnitude of its electric field. Given this initial electric field (E(z = 0, t)), we perform a Fourier transform to find the electric field in terms of angular frequency, Optical Pulse Propagation To determine how an optical pulse propagates through a medium we need to know the medium’s dispersive 1 E (z = 0, ω) = √ 2π Z∞ E(z = 0, t) exp(−iωt)dt. (14) −∞ To find the electric field at an a arbitrary depth z, we then need to multiply by this result by exp(ik(ω)z) (see equations (3) to (7)). Setting z = L gives us the pulse angular frequency profile at the exit of the medium. We can then use the reverse Fourier transform to construct the electric field as a function of time at z = L, 1 E (z = L, t) = √ 2π Z∞ E(z = L, ω) exp(iωt)dω. (15) −∞ Now we can again use equation (10) to reconstruct the intensity pulse. The pulse propagation modelled in this report relies on equation (12) to provide k(ω). This equation gives the electric susceptibility as derived from the steady state solutions to the optical Bloch equations [43]. The pulses of light we use for our experiments have a full width at half maximum (FWHM) of < 800 ps, far less than the lifetime of the excited states. However, equation (12) is still valid for our pulses as long as we remain in the weak probe regime. The pulse is considered weak if its effect on the atomic ensemble is negligible, and so time derivatives on the density matrix [49] should be correspondingly negligible. 1. Narrowband approximation The previous treatment is all that is required to model pulse propagation but does not give a great deal of insight. In this section we make two approximations that aid in understanding. We start by making the approximation that our pulses are Gaussian in shape, which is not too bad an assumption when compared with measurements of the initial pulse profile. The range of frequencies that encompass ∼ 99% of the pulse is defined as the ‘bandwidth’ and the peak frequency is known as the carrier frequency. We then make the ‘narrowband approximation’, which essentially means that the change in 5 absorption and dispersion is small across the pulse bandwidth. With these approximations, the peak of the pulse travels at the ‘group velocity’ [43], which we label vg . We now define the group refractive index ng ≡ c/vg which is given by the following equation [50]: dnR (ω) dω (16) Using this equation and our model for the electric susceptibility we can calculate ng for an alkali metal atomic vapour. Fig. 2 shows the result of this for a 2 mm long vapour cell containing rubidium in its natural abundance. Notice that there are regions where ng is negative, which corresponds to the pulse peak exiting the medium before it has entered. These parts of the curve are regions where the narrowband approximation breaks down or the pulse is fully absorbed. However around these regions, ‘fast- ng,( ×103 ) nR Transmission 1.0 0.8 0.6 0.4 0.2 0.0 1.008 1.004 1.000 0.996 0.992 4 2 0 2 4 6 8 8 6 4 2 0 2 Detuning (GHz) 4 6 8 FIG. 2. Theoretical plots of transmission, the refractive index for a continuous-wave beam (real part) and the group refractive index against detuning. The the colours correspond to different cell temperatures as follows: red = 80◦ C, green = 100◦ C, blue = 120◦ C, cyan = 140◦ C, yellow = 160◦ C and purple = 180◦ C. The regions with the largest magnitude of the group refractive index are regions of high absorption. The grey highlighted region shows the bandwidth of the initial pulse used for the experiment, with a carrier detuning of 300 MHz. light’ pulses can be seen. Fig. 3 shows the result after solving the discrete form of equation 15 numerically [51] for a pulse with a carrier frequency that is resonant while the medium is not optically thick. The peak of the pulse after the medium arrives before a reference pulse travelling at the speed of light in vacuum. One thing to note is that the pulse seen after traversing the medium is completely enveloped by the reference pulse on the leading edge. This predicts that no more photons will arrive at the detector at a given time then would have been the case for the reference pulse. The topics of causality, energy transfer and signal velocities in a fast-light medium are currently an area of much interest with much debate. This is beyond the scope of this report. 0.8 Normalised Intensity ng (ω) = nR (ω) + ω 1.0 0.6 0.4 0.2 0.0 2.0 1.5 1.0 0.5 0.0 0.5 Time (ns) 1.0 1.5 2.0 FIG. 3. Graph showing intensity against time for a reference pulse travelling through vacuum (larger red curve) and the pulse seen after traversing the medium (smaller blue curve). The vertical dashed line crosses the blue curve at its peak. We can see that the peak of the pulse traversing the medium arrives before a pulse travelling through vacuum. The medium is modelled as atomic rubidium vapour in its natural abundance at 80◦ C in a 2 mm long vapour cell while the carrier frequency is set to -1.5 GHZ (resonant with the 85 Rb Fg = 3 → Fe = 2, 3 Doppler broadened transition). Parameters have been chosen such that an experiment could be performed in the future to verify this prediction. In this report we present experiments where the slowlight effect is manifest. To clearly present the effect we need to work in a region where the group refractive index does not change vastly over the pulse bandwidth while maintaining a relatively high value. Also the transmission should be high so that the output pulse is clearly visible. Using Fig. 2 we have identified a region corresponding to the pulse bandwidth centred at 300 MHz (shown as the grey shaded region), which best fits these criteria. III. A. EXPERIMENTS Absolute Absorption The aim of these experiments were to see if the presence of buffer gas in the 2 mm long 87 Rb vapour cell has a considerable effect on transmission spectra. If experimental spectra agree with theoretical fits, we can confidently say that expected shifts due to the buffer gas are negligible. Collisional broadening, however, can be accounted for by fitting the Lorentzian width (because collisions should be homogeneous), and so are not expected to be to be an issue. 6 Experimental Method Fig. 4 shows a schematic of the experimental apparatus used. A Toptica DL 100 external cavity diode laser (ECDL) is used to produce the a coherent light beam. The frequency of the laser beam is scanned around the D1 line-centre (377 107 407.299 MHz). The beam passes through a 50:50 beam splitter (BS) where a fraction of the light passes through a Fabry-Pérot etalon (FPE) and onto a photo-detector (PD). The remaining light is incident on a polarising beam splitter (PBS) where a fraction of the light passes through and is then attenuated by a neutral density filter (ND) before passing through the experimental cell. The light reflected at the PBS is used to perform sub-Doppler hyperfine pumping spectroscopy [52]. Linearly polarised light performs hyperfine pumping on the reference cell, before being attenuated by an ND and passing though a quarter wave-plate (λ/4). The beam is then reflected back to be counter propagating to itself, passing again through the λ/4, ND and reference cell. The double pass through the λ/4 causes a π/2 rotation in the linear polarisation, ensuring the light is now transmitted through the PBS and onto a PD. The experimental cell is contained in an oven which allows a laser beam to travel through. Outside the oven is an aluminium magnet holder which holds two permanent magnets on either side of the oven. The magnets allow the laser beam to pass through the centre of them, and are placed such that they create a magnetic field (B) parallel to the laser beam. The magnets can be removed from the holder when no magnetic field is required. The light after the experimental cell is then incident onto another PD. The signals from all the PDs are measured simultaneously on an oscilloscope. Using the method outlined in [17], the FPE signal and sub-Doppler spectroscopy signal are used to recalibrate the time axis of the oscilloscope into a frequency axis. nal gives a peak at fixed intervals in frequency, which allows the scan to be made linear in frequency. The frequency axis is then calibrated using the peaks of the sub-Doppler signal as reference points, where the values of the transitions are taken from [53] and the crossovers are taken to be half way in between the transition values. If we apply this procedure to the sub-Doppler signal 2.5 Intesnity (Arbitrary Units) 1. 2.0 1.5 1.0 0.5 0.00 5 10 15 Time (Arbitrary units) 20 FIG. 5. Example of data raw data from the FPE signal (blue) and sub-Doppler spectroscopy (red). The time axis is converted to a frequency axis by first linearising the data using the FPE signal, and then using the sub-Doppler signal is to calibrate the axis. itself, we can extract a rough estimate of the accuracy of the frequency calibration and linearisation on resonance. Fig. 6 shows the result of doing this. Freq. Diff. (MHz) 4.4 Intensity (Arbitrary units) 4.2 4.0 6 4 2 0 2 4 64 2 0 2 4 6 3.8 3.6 3.4 3.2 3.0 2.8 4 FIG. 4. Diagram of the experimental apparatus used for spectroscopy. The oven and magnet holder are not shown. Fig. 5 shows an example of the both the FPE signal and the sub-Doppler spectroscopy signal. The FPE sig- 2 0 2 Detuning (GHz) 4 6 FIG. 6. Graph of the sub-Doppler spectroscopy signal where the intensity is plotted against the calibrated frequency. The vertical lines correspond to known values for the transition frequencies and crossovers. The inset shows the difference between the peak positions and vertical lines. The difference is less than 6 MHz for all peaks. 7 2. Results Fig. 7 shows the transmission through a 75 mm cell containing rubidium in its natural abundance [55]. A least squares fit was done to extract the temperature of (20.70 ± 0.13) o C, which was the only free parameter. The uncertainty on this value was taken as the difference on the temperatures extracted from fits when the rubidium ratio was changed by ±0.01 (the uncertainty in the rubidium ratio). At this temperature self broadening is negligible [19] and so the Lorentzian width can be taken to be just the natural line-width. Excellent agreement is seen between theory and experiment, as shown by the residuals. Fig. 8 shows a plot of transmission against detuning for a 2 mm long cell containing (98.20 ± 0.09%) 87 Rb. The temperature, Lorentzian width and ratio of 87 Rb to 85 Rb were extracted from fits to five separate spectra taken in quick succession (less than 20 seconds). Notice that the Lorentzian width is far higher than would be expected for a cell containing just rubidium at this temperature. The likely cause is buffer gas. This particular spectrum was used to calculate the ratio of rubidium isotopes because the 87 Rb and 85 Rb absorption peaks are both visible but not optically thick. This meant that the fit to the ratio should be most sensitive and hence most accurate. The ratio extracted from this fit was used to fix the value for all calculations using this cell. In Fig 9 a spectrum taken at high temperature is shown. All the rubidium transition features have almost completely merged, giving a broad region of high absorption. 1.00 Transmission 0.95 0.90 0.85 0.80 0.75 0.70 0.4 0.2 0.0 0.2 0.4 Residuals ( ×100) The PD output voltage is linear with intensity, but the background intensity varies with frequency due to the laser scan and reflections in the set-up. The background can be quantified by finding known regions in the absorption spectrum where the absorption should be negligible and fitting a polynomial to those areas. This works well for spectra which have relatively narrow features which correspond to low temperatures. However, at high temperatures there may not be any region negligible absorption in the scan range. For a 2 mm cell this problem can be solved by taking a ‘background’ spectrum when the cell is at room temperature, where the absorption is negligible. After the data was normalised and frequency calibrated, the data was fitted to theory using either a Marquardt-Levenberg (ML) algorithm [54] or a simulated annealing (SA) algorithm, or often both (see appendix A). Five spectra were taken and the quoted fit parameters are the mean given with the standard error. A thermocouple measurement was taken along with each spectrum to ensure the temperature does not vary much over the length of time taken to obtain five spectra (usually around 20 seconds). The thermocouple measurement was not used to give the temperature of the vapour, this was always extracted from the fit. 6 5 4 3 2 1 0 1 2 Detuning (GHz) 3 4 5 6 FIG. 7. Graph of the transmission against detuning in a 75 mm long cell containing rubidium in its natural abundance (72.17% 85 Rb & 27.83% 87 Rb) [55]. The black curve shows the experimental data while the red curve shows the theoretical result after a least squares fit to the temperature using an ML algorithm. Five spectra were taken (only one shown), each of which were fitted to theory using the ML algorithm. The temperature was found to be (20.70±0.13) o C. The statistical variation in the five fits was very small and so the uncertainty quoted was found using the functional approach [54], varying the rubidium ratio by ±0.01. The bottom graph plots the residuals of the data and theory curves in the top graph. The result of fits to a spectrum taken at high magnetic field are shown in Fig. 10. Two techniques were used to fit the data. The first involved taking spectra with the magnets removed and fitting for temperature and Lorentzian width only (magnetic field set to zero). The magnets were then placed into the holder, and then the spectra seen in Fig. 10 were taken and fitted to magnetic field only. The other technique involved fitting the spectrum for magnetic field, temperature and Lorentzian width using an SA algorithm followed by an ML algorithm. We can see that the value of the Lorentzian width extracted via the two methods strongly disagree. 3. Discussion Fig. 7 showed, as expected, that a long cell with no buffer gas gives an excellent agreement between theory and experiment. Also the value of the temperature extracted from the fit is in agreement with the thermocouple measurement. This agrees with the work in [17] and gives us confidence in the theory for the electric susceptibility for rubidium vapour at low temperatures and no buffer gas. The measurement of the ratio of the rubidium isotopes was taken from a fit to the spectra shown in Fig. 8. This measurement should be insensitive to shifts and broadening due to buffer gas, because it is sensitive only to the amplitude of the peaks (a strong function of number den- 1.0 0.8 0.8 Transmission 1.0 0.6 0.4 0.6 0.4 0.2 0.0 6 4 2 0 2 4 610 0.0 3 2 1 0 1 2 310 8 6 4 2 0 2 4 Detuning (GHz) 6 8 10 FIG. 8. 98.20% Rb87 cell in the presence of buffer gas. The black curve shows the experimental data while the red curve shows the theoretical result after fitting the temperature and Lorentzian width with the ML algorithm. Five spectra were taken (only one shown), each fitted to theory with the SA algorithm to find the global minimum in parameter space. Each of the five spectra were then fitted to theory using the ML algorithm using the SA fit results as the input parameters. The temperature was found to be (90.17 ± 0.10) o C, the Lorentzian width was Γtot = 2π × (165 ± 1) MHz and the fraction of 87 Rb was found to be (98.20 ± 0.09)%. The uncertainties quoted are the statistical fluctuation in the five measurements. The bottom graph plots the residuals of the data and theory curves in the top graph. sity). Furthermore, the measurement should be insensitive to the overall value of the number density (and hence temperature) because only the ratio of number densities of the two rubidium isotopes is measured. For these reasons, the value of the ratio extracted from this measurement is trusted and was fixed for all subsequent fits. The overall fit to theory seen in Fig. 8 and Fig. 9 is reasonably good, as seen by the residuals. However, the values of the temperature extracted from the fits disagreed with thermocouple measurements. The thermocouple measurement for the spectrum shown in Fig. 8 was ∼ 40◦ C higher than the fit, and it was ∼ 30◦ C higher for the spectrum shown in Fig. 9. The accuracy of the thermocouple was therefore brought into question. The thermocouple calibration was checked using boiling water and was found to agree with the defined value of 100◦ C. The fit to the spectra in the long rubidium cell (Fig. 7) was in agreement with the thermocouple measurement when both were at ambient room temperature. Therefore, within the range of 20◦ C to 100◦ C, we expect the thermocouple to be accurate. This rules out the thermocouple accuracy as the cause of the discrepancy, at least for the lower temperature spectrum. One possible explanation for the discrepancy may be that the thermocouple tip was placed in the cell heater at a place that was hotter than that of the cell. Another explanation is Residuals ( ×100) 0.2 Residuals ( ×100) Transmission 8 8 6 4 2 0 2 4 Detuning (GHz) 6 8 10 FIG. 9. 98.2% 87 Rb cell in the presence of buffer gas. The black curve shows the experimental data while the red curve shows the theoretical result after fitting the temperature and Lorentzian width with the ML algorithm. Five spectra were taken (only one shown), each fitted to theory with the ML algorithm. A fit using SA was used on each spectrum to ensure that the fit parameters are in the global minimum. The temperature was found to be (182.1 ± 0.4)o C, while the Lorentzian width was Γtot = 2π × (170 ± 4) MHz. The uncertainties quoted are the statistical fluctuation in the five measurements. The bottom graph plots the residuals of the data and theory curves in the top graph. that the formula, giving the number density at a given temperature [32], is invalid for this particular cell. Buffer gas pressures in the cell may be high, causing a smaller rubidium number density for a given temperature. Also if the cell is deficient in rubidium, that will also cause a smaller number density at a given temperature. If there is a smaller number density for a given temperature, fits to theory will show a lower temperature than they should (because number density is a stronger function of temperature than the Doppler width). This may then cause the Lorentzian width to be fitted larger than it should, to compensate for the small theoretical Doppler width. Of the two methods used to fit the spectra taken at high magnetic field, the one using a spectrum with the magnets removed to measure the temperature and Lorentzian width should be more reliable. However, we expect the global minimum in parameter space to correspond to accurate values of the parameters if the theory is valid. However, the Lorentzian widths disagree. One explanation for the disagreement may be that the shifts due to the buffer gas may be compensated by an increase in Lorentzian width, for an optically thick medium when the magnetic field is set to zero. However, when the magnetic field is on and the spectrum no longer is optically thick, the fit to the magnetic field should be able to account for shifts better than an increase in Lorentzian width and so the Lorentzian width will be seen to be smaller. 9 B. 1.0 Transmission 0.8 Slow-light The following section shows the experiments that were done to demonstrate the slow-light effect and to test the theory developed to account for it. A variety of methods were used, the results of which are discussed and will be used to improve future experiments. 0.6 0.4 0.2 Residuals ( ×100) 0.0 4 2 0 2 4 10 1. 8 6 4 2 0 2 4 Detuning (GHz) 6 8 10 FIG. 10. 98.2% Rb87 cell in the presence of buffer gas. The black curve shows the experimental data while the red curve shows the theoretical result after fitting the magnetic field with the ML algorithm. Five spectra were taken (only one shown) and the magnetic field was found to be (895 ± 6) Gauss. Fits to five spectra with the magnets removed gave the values of the temperature (110.94 ± 0.02)o C and Lorentzian width 2π × (127.7 ± 0.3) MHz. An SA fit of the temperature, Lorentzian width and magnetic field showed that fit given by the red curve is not in the global minimum. The blue curve is a ML fit of the data after ensuring the fit is within the global minimum, giving the magnetic field as (904.8 ± 0.6) Gauss, temperature as (110.136 ± 0.014)o C and Lorentzian width as 2π×(91.8±0.4) MHz. The uncertainties quoted are the statistical fluctuation in the five measurements. The bottom graph plots the residuals, with like colours corresponding the theoretical curves in the top graph. Normalised RMS deviation of red (blue) curve to data = 1.5(1.2)%. 4. Conclusion We have seen that while our theoretical fits can account for the vast majority of the structure of the spectrum in our rubidium cell with buffer gas, an excellent agreement is not obtained. Good fits are obtained, but the values of the extracted parameters cannot be fully trusted. This means the buffer gas cannot be considered negligible because our theory (in its current form) cannot account fully for the spectrum due to shifts and the difference in the number density at a given temperature. This cell may not be suitable for future experiments because theoretical models that help design experiments, may not be valid for this cell. However, this cell can still be used for simple pulse propagation experiments, because we can characterise the absorptive and dispersive properties of the medium using a spectroscopic measurement. This is done by simply allowing our model to fit to the data such that a good agreement is obtained, while acknowledging that the parameters are more phenomenological. A dispersion curve can then be generated from theory. Experimental Method Fig. 11 shows a schematic of the apparatus used for the experiment. A Toptica DL 100 laser is used to generate continuous wave light. The beam passes through a high extinction, Glan-Thompson polarisation beam splitter (PBS) linearly polarising the beam. The beam then enters a Pockels cell [56], which rotates the plane of polarisation when a large voltage is applied to the Pockels cell. The beam is then incident on another high extinction, Glan-Thompson PBS which is crossed with respect to the first PBS. The Pockels cell is attached to a voltage supply which can rapidly switch a large voltage. The crossed PBSs with the Pockels cell create a pulse of light when the plane of polarisation is rapidly rotated. The light pulse is then attenuated by a neutral density filter (ND) before entering the experimental cell. The experimental cell is placed in an oven that is used to heat the cell and change the vapour pressure. After traversing the cell the pulse is then incident on either a fast photo-diode detector (FPD) or an avalanche photo-diode detector (APD). The signal from the FPD or APD is then recorded on a fast oscilloscope (∼ 160 ps rise time). The avalanche photo-diode has an extremely fast response time (< 50 ps quoted from the manufacturer) and works as part of a photon counting module. This means it needs many repetitions to accumulate a pulse profile. The FPD on the other hand gives a profile over one shot, but has insufficient resolution to accurately characterise the pulse. The FIG. 11. A schematic of the experimental apparatus. The oven is not shown. Also not shown is a third PBS placed just before the cell with a FPD measuring the output of the side arm. input pulse shape is important to characterise accurately for an accurate theoretical prediction. The FPD can be used to experimentally measure pulse delays, but are not 10 accurate enough for an excellent agreement with theory. The APD can be used to gain a much higher resolution but many repetitions need to be measured to accumulate a pulse profile. The input pulse was characterised using the APD because of the better time response. However, it was noticed that the output from the FPD is not exactly the same with each repetition. The time when the pulse arrives after the trigger of the oscilloscope changes, and also the peak height of the pulse changes. Fig. 12 shows a plot of the peak voltage (proportional to peak pulse intensity) against the arrival time of the peak. This ‘jitter’ will have the affect of broadening the pulse as measured by the photon counters. To quantify this effect a Mont-Carlo algorithm [57] reproducing this distribution was used to model the jitter and found that the broadening was negligible (< 20 ps increase in the FWHM, see appendix C). Therefore, the input pulse profile obtained by counting over many repetitions was taken as the initial pulse on all occasions. 2. Results Fig.13 shows experimental plots of slow-light pulses. The pulses were measured using a FPD, and show qualitatively that pulses of light can be significantly slowed with respect to a reference pulse. 0.5075 0.5050 Peak voltage measured (V) a phenomenological function in order to smooth it. To measure a reference pulse, the laser was tuned far off resonance and the pulse profile was formed after counting for the same amount of time. A third PBS placed before the ND and the experimental cell (not shown in Fig. 11) was used with a FPD to measure any change in laser power when moving the frequency far off resonance. This change in laser power was then factored out during analysis. A measurement of absolute absorption (like that in section II C) was taken soon after the pulse data was taken. This transmission spectrum was then fitted to theory to extract χ for the atomic vapour. This χ was then used to create a theoretical output pulse profile using the off resonance pulse as the initial pulse. 0.5025 0.5000 0.4975 0.4950 0.4925 0.4900 50.00 50.05 50.10 50.15 50.20 50.25 50.30 50.35 50.40 Time of peak pulse after trigger (ns) FIG. 12. Graph of the peak voltage output of the FPD against time after the trigger of the oscilloscope, when a pulse is incident on the FPD. There are 2011 points, each taken in quick succession through the vapour cell when off resonance and at room temperature. The distribution is consistent with a Gaussian in voltage and time, with standard deviations measured as approximately 3 mV and 50 ps respectively. When forming a pulse profile via photon counting over many repetitions, a long time-scale of the order of an hour was needed to gain a very good profile. However, when measuring the output pulse on or near resonance in a hot medium, this time-scale is enough to see the laser shift frequency by a noticeable amount. To minimise laser drift over the counting period the laser should be locked. When using the 98.2% 87 Rb cell the laser was locked using polarisation spectroscopy to the 85 Rb Fg = 3 → Fe = 2 transition (see appendix B). However, when using the cell with rubidium at its natural abundance, this method of laser locking was unsuitable. To compromise, a short counting time of around 10 minutes was used to give a pulse profile, that was then fitted to FIG. 13. Graph of intensity against time for slow-light pulses in a 2 mm long cell containing rubidium vapour at its natural abundance. The black curve is the pulse measured using a FPD when the cell was at room temperature and optically thin, and was assumed to have a negligible time delay. The room temperature of 22◦ C was measured with a thermocouple. The other curves are pulse profiles measured using a FPD at temperatures (shown next to the respective curve) that were extracted from fits to transmission spectra. These temperature values were extracted from fits to absorption spectra. The carrier detuning was approximately 300 MHz. The laser was not locked. Fig. 14 shows the result from measurements of pulses after traversing the 98.2% 87 Rb cell. A FPD was used for the measurements and the laser was frequency locked. The theoretical predication in Fig. 14 was the result of solving equation (15) numerically for a reference pulse approximated to be a Gaussian FWHM of 900 ps. We 11 can see that the pulse is largely absorbed, with not much delay. FIG. 14. Graph of normalised intensity against time for pulses after traversing a 2 mm long cell containing rubidium of which 98.2% is 87 Rb. The cell also contained buffer gas. The solid blue curve is the pulse measured using a FPD when the cell was at room temperature and was assumed to have negligible delay or absorption. The solid pink curve was measured when using a FPD when the cell was heated. The laser was locked using polarisation spectroscopy to the 85 Rb Fg = 3 → Fe = 2 transition (≈ −1500 MHz detuning). The red dashed curve is the theoretical prediction when a Gaussian with a FWHM of 900 ps is taken as the reference pulse. Fig.15 shows a delayed pulse as measured using an APD as part of a photon counting module. The pulse was measured by building up a profile over 11 minutes and 30 seconds and then fitting a phenomenological curve to the profiles. The carrier wave detuning of the pulse was approximately 300 MHz and the reference pulse was taken to be the pulse profile when the carrier wave was far off resonance. This reference pulse, along with a measurement of absolute absorption to extract χ, allowed the theoretical curve to be produced. 3. Discussion In Fig.13, it is shown that by increasing the cell temperature it is possible to get large time delays, where the pulse can be delayed by more than the pulse width. A rough calculation shows that group refractive indices of ∼ 400 and ∼ 1000 are seen for the two hottest temperatures. The FPD detectors do not have a very good time resolution but they are sufficient to see the rough time delay. In regions where the absorption is large, the absorption and dispersion often change rapidly with frequency. Frequency locking the laser is therefore advantageous when performing experiments in these frequency regions. The results in Fig.14 were taken when the laser was locked. A FPD was used and so the laser would not have drifted much over the course of the experiment, but the advan- FIG. 15. Graph of intensity against time for a pulse of light on and off resonance with the atomic vapour. The intensity axis is normalised to the peak hight of the solid blue curve. The blue markers show the count number (normalised) from the APD, within a bin width of 20 ps, for a far off-resonance (∼15 GHz) pulse measured over many repetitions for 11 minutes and 30 seconds. The red markers show the count number (normalised) from the APD, within a bin width of 20 ps, for a pulse carrier detuning of ≈ 300 MHz measured over the same amount of time as the off-resonance pulse. The solid blue and red curves are phenomenological fits to the blue and red markers respectively. The time axis is zeroed at the peak of the solid blue curve. The black dashed curve is a theoretical prediction for the delayed pulse when taking the solid blue curve to be the reference. The experimental cell was 2 mm long containing rubidium in its natural abundance and was at a temperature measured to be 137.6◦ C. tage here for laser locking was that it also provides a more accurate measure of the frequency. Fig.14 shows reasonable agreement between theory and experiment, but hindered by not being able to measure the pulses accurately enough with the FPD. An improvement can be made to the data made in this graph by using the photon counters Fig.15 shows the result of using the photon counting method and achieves a good agreement. The discrepancy between theory and experiment may be due to the fact that the profile of the measured pulses were lacking in precision due to the relatively short counting time. Also the laser was not locked which may have meant that the value taken as the carrier frequency was not very accurate. A tunable laser lock would therefore improve this experiment (see section IV A). 4. Conclusion Reasonable agreement between experiment and theory has been observed. We have seen that APDs are preferred over FPDs because of their better time resolution. We have also seen that locking the laser may improve 12 IV. A. FUTURE OUTLOOK Tunable laser lock using the Faraday effect in high magnetic fields 1 Ix − Iy = cos (2φ) exp − α+ + α− L I0 2 FIG. 16. Schematic of the proposed apparatus that can be used for a laser lock. This arrangement is similar to that in Fig.4 with the addition of a half-wave plate (λ/2) to rotate the initial plane of polarisation, and a PBS after the cell with two photo-diodes used to detect the beam on each arm of the PBS. These two photo-diodes can be used as part of a differencing detector to get a Faraday signal. The experimental cell will be a 1 mm long micro-fabricated cell placed within a permanent magnet (not shown) that produces a high magnetic field. the beam is separated into horizontally polarised (Ix ) and vertically polarised (Iy ) components. These components are then measured on separate photo-detectors (PD). By tuning the experimental parameters of magnetic field, temperature and angle of the plane of polarisation of the initial light (θ0 ), we can find a vast number of (17) where φ is the angle of the plane of polarised light with respect to the x-axis after the cell, and α+ and α− are the absorption coefficients for light driving σ + and σ − transitions respectively. The rotation angle is given by the phase shift of the two circularly polarized components of the beam which can be found using our model for χ in the circular basis. Also, α+ and α− can be given by our model. Using our model we can now change experimental parameters to find locking points. Fig.17 is one example of this where a locking point at a detuning of 300 MHz was found. (Ix −Iy )/I0 In order to improve the photon counting method for generating a pulse profile, it will be necessary to frequency lock the laser. Taking inspiration from reference [29] we can use a Faraday signal to lock the frequency of our laser. If we use a micro-fabricated 1 mm long cell placed within a permanent magnet, magnetic fields of up to around 0.6 T are achievable [26]. By changing the depth of the cell in the magnet, we can tune the magnetic field. Fig.16 gives a schematic of the apparatus that can be used to generate the laser locking signal. The schematic is very similar to that in Fig.4. After the cell locking points (zero crossings) over a range of about 50 GHz. To give an example of this, we first choose our Faraday signal to be (Ix −Iy )/I0 (this is one of the Stoke’s parameters [20]). This Faraday signal can then be given by the following equation (taken from [20]), Transmission the accuracy of the experiment. Future experiments will benefit from using a tunable laser lock along with the APDs to get the most reliable experimental data. We have also seen that using the room temperature cell to characterise the reference pulse may be unreliable due to reflection effects changing with temperature. Moving the laser frequency off resonance, whilst accounting for any changes in laser intensity, may therefore give better results. 1.0 0.8 0.6 0.4 0.2 0.0 1.0 0.8 0.6 0.4 0.2 0.0 0.2 0.4 0.6-10 -8 -6 -4 -2 0 2 4 Detuning (GHz) 6 8 10 FIG. 17. Theoretical transmission and (Ix − Iy )/I0 against detuning. Shown with the vertical dashed line is a zero crossing which can be used as a locking point. The experimental cell was modelled as 1 mm long, containing 99% 87 Rb. The following experimental parameters were chosen: B = 2142 Gauss, θ0 = 2π/5 and T = 150◦ C In general the signals obtained, like that in Fig.17, do not have very sharp zero crossings and so may be less precise than other locking schemes. For the type of pulse propagation experiments shown in this report, less locking precision is needed when away from a resonant feature, for which this method may be suitable. However, when on-resonance, we need a higher precision due to the rapidly changing absorption and dispersion. For this we can use a laser lock based on polarization spectroscopy (see appendix B). 13 B. Optical Switch One possible future outlook for our project will be to create an optical switch based on the controlled Faraday rotation of a pulse [25]. To cause a Faraday rotation of the polarisation of linear polarised light, we need to cause a phase shift between the two circular components of the light. This is can be done using a thermal atomic ensemble in two different ways (shown in Fig.18). One way is to use a magnetic field to cause one of the σ transitions to be more resonant than the other. The other way is to use optical pumping to make the populations of the magnetic sub-levels uneven. Using optical pumping we FIG. 19. Diagram of the optical switch (adapted from a figure made by Lee Weller). The initial polarisation vector of the probe pulse (FARADAY ) is rotated by both the presence of an applied magnetic field (B) and the pump beam. A change in the angle of the polarisation of the pump beam (PUMP ) changes strength of the component of light driving either σ or π transitions. FIG. 18. Simplified energy level diagram showing 2 ground state magnetic sub-levels and one excited state level. An anisotropy in the strength of coupling to the probe beam is achieved in two different ways. (a): A larger fraction of the atoms are in one ground state rather than the other, causing a stronger coupling of the ensemble to the probe beam for the transition with more atoms. (b): A magnetic field lifts the degeneracy in the magnetic sub-levels causing one to be shifted further from resonance while the other is shifted towards resonance. can change the amount of Faraday rotation of the probe beam. If we can change the polarization by π/2, light can be made to switch between orthogonal polarisation channels by use of a PBS after the cell. This would create an optical switch. Optical pumping alone is difficult to create the required rotation, but it was shown in [25] that combining this with a magnetic field makes this possible. A counter-propagating pump and probe beam was used as the arrangement in [25]. Our intention is to use these principles, and create an optical switch for pulsed light that is pumped using a beam that accesses the medium orthogonal to the direction of the probe beam. This way the medium can be more uniformly pumped over the volume that the pump and probe cross, and also the pump and probe both address the same atoms across a wide range of velocity classes. This should increase the performance of the optical switch. At present, the idea is to have the probe pulse on the D1 line and the pump on the D2 . ACKNOWLEDGEMENTS The work in this report was carried out in collaboration with Lee Weller, Charles Adams and Ifan Hughes. Appendix A: Fitting with simulated annealing Fitting many parameters at once can create issues with finding the best fit parameters. When fitting theory to experimental data some sort of cost function (a measure of how much the fit deviates from the data) is employed, and is minimised to find the best value of the parameters. The cost function lives in a space with the same number of dimensions as parameters, and is often impractical (or even impossible) to completely explore it within its allowed bounds. Therefore, a simple and fast method is to make a guess of the parameters and then vary the parameters, only allowing changes that decrease the cost function and finish when each step is no longer reducing the cost function very much. This method is called ‘hill climbing’ (from the situation where the cost function is defined with the different sign convention). There are many hill climbing algorithms of which the Marquardt-Levenberg method (ML) [54] is the one we use. The problem with the hill climbing method is that there is a real danger of falling into a local minimum and not finding the best overall parameters. This problem is sometimes caused by parameters compensating for each other, and with more parameters, there can be many more local minima. Fig. 20 shows an example of how fitting using a hill climbing algorithm can get stuck in a local minimum. Two fits to experimental transmission spectra were done using the ML algorithm but with different starting guesses to the three parameters. After calculating the root-mean-square deviation of the fits to the data, we can clearly see that one fit is better than the other. The difference between some of the fit parameters is far larger than the uncertainty in the fit parameters (as given by the Hessian matrix used in a ML fit [54]). This means 14 that the worse fitting one must have been the result of fitting in a local minimum. 1.0 Transmission 0.8 0.6 tial energy. An example of this is silicon dioxide which forms glass when rapidly cooled. Annealing is analogous to our problem, where the positions of the particles are the many parameters and the internal energy of the system is the cost function. In its simplest form the simulated annealing algorithm takes the following steps: 0.4 1. Make initial guesses for the parameters and evaluate the cost function (F1 ) 0.2 2. Change these parameters and evaluate the cost function again (F2 ) Residuals ( ×100) 0.0 4 2 0 2 4 6 810 3. If F2 < F1 accept these new parameters. 8 6 4 2 0 2 4 Detuning (GHz) 6 8 10 FIG. 20. Graph of transmission against detuning for a 2 mm long vapour cell, containing 98.2% 87 Rb. The red and blue curves are ML least-square fits to theory with different starting guesses for the parameters. The starting parameters for the red (blue) curve were: B = 800(600) Gauss, T = 131(120)◦ C, Γtot /2π = 120(100) MHz. The final values for the red (blue) curve were: B = 861(858) Gauss, T = 93.0(92.8)◦ C, Γtot /2π = 262(314) MHz. The normalised RMS deviation of the red (blue) curve to data was 1.96(2.30)%. The best method to get around this problem is by engineering the situation such that only one parameter need be fitted at any one time. For example, if we want to take data that we will later want to fit the temperature and magnetic field to, we should first take a spectrum with no applied field and then quickly apply the field and take the data. This way the two spectra should have been taken at the same temperature (assuming the vapour cell is not rapidly changing in temperature). This way the first spectrum can be used to extract the temperature when the magnetic field is fixed at zero, and then we can fit the magnetic field to the second spectrum while fixing the temperature. Fitting as few parameters as possible is always important, but due to the presence of buffer gas in the experimental cell, a fit to just one parameter is not possible. The Lorentzian width is needs to be fitted along with the temperature. This means a new algorithm needs to be employed, one that will find the global minimum with a high number of parameters and potentially bad initial guesses for the parameters. For this purpose a fitting code using ‘simulated annealing’ [58] has been developed. Simulated annealing uses the Metropolis algorithm [59] to emulate the remarkable observation that when a substance is cooled to a crystalline solid slowly, it always finds the state of minimum energy. The crystalline form is one of low energy, but if the substance is rapidly cooled it may form an amorphous solid of higher internal poten- 4. If F2 > F1 accept these new parameters with probability exp[(F1 −F2 )/kT ], where k is a scaling factor (like Boltzmann’s constant) and T is ‘temperature’ parameter. 5. Reduce T and repeat the procedure until the system is ‘cold’, i.e T is very small. The initial value of T and k need to be chosen appropriately along with a slow method of decreasing T . The method that was used for decreasing T was setting the new T value to T /(1+βT ), where β is a sufficiently small number [60]. After applying the simulated annealing algorithm to the data in Fig. 20, it was found that in fact both the ML fits were not in the global minimum, with both having vast overestimations of the Lorentzian width. Appendix B: Laser locking by polarisation spectroscopy Polarization spectroscopy [61, 62] was used to frequency lock the laser when taking the data shown in Fig. 14. Shown in Fig. 21 is the locking signal. We can see that the difference between the locking signal, and the accepted value of -1.497657 GHz [53] for the transition, is of the order of 10 MHz. Over time the height of this signal may vary (due to batteries running low on the detector). Therefore, the laser will be locked anywhere between the peak and trough of the signal, without jumping to another zero crossing. The distance between the peak and trough is approximately 20 MHz while the frequency calibration is accurate to approximately 5 MHz. We can therefore say that when locking to this signal, the laser detuning was −1.50+0.01 −0.02 GHz from the defined global line-centre. Appendix C: A Monte-Carlo method for theoretical photon counted pulses Pulses were measured using the photon counting method have shown FWHM values of as low as 750 ps. When using a FPD the pulse shape is not accurately represented but it is assumed that it reacts the same for each pulse. This assumption would mean that the measured peak arrival times should correspond directly to 15 malised to a peak hight of one. This result was then be plotted on top of the initial pulse that would theoretically be seen over just one shot (by a perfect FPD), shown in Fig. 22. The graph shows four curves, two are for a theoretical reference pulse and two are for a delayed pulse after traversing a medium with the same conditions as for the experiment shown in Fig. 14. The two curves for each pulse show the result for just one shot and the result of the Monte-Carlo code respectively. The two curves lie almost on top of each other, where the broadening is only just visible. By inspection it is possible to see that the broadening is less than 20 ps which is smaller than exper- Intesnity (Arbitrary Units) 0.2 0.1 0.0 0.1 0.2 0.3 1.56 1.54 1.52 1.50 Frequency (GHz) 1.48 1.0 1.46 0.9 FIG. 21. Graph of the polarisation spectroscopy signal in the region if the 85 Rb Fg = 3 → Fe = 2 transition. The vertical dashed line shows the transition detuning of -1.497657 GHz. the actual pulse peak arrival times. The ‘jitter’ observed in Fig. 12 shows pulses arrived at different times over a range of approximately 300 ps, which intuitively would seem like the photon counted pulse may just be the result of a much thinner pulse broadened significantly by photon counting over many repetitions. A Monte-Carlo method to simulate this was therefore used to try to infer the original width of the pulse. The Monte-Carlo computer code works by first reproducing the sort of distribution seen in Fig. 12. The code takes into account any possible linear trend in the data by fitting a line of best fit to the distribution. Fig. 12 clearly does not have much of a linear trend, but a linear trend has been seen in other measurements of the Jitter. The 2-D distribution is then recreated by modelling the 1-D distributions in time and distance from the line of best fit as Gaussian. Once the distribution is recreated, pulses were modelled for the points in the distribution. 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