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Chin. Sci. Bull. DOI 10.1007/s11434-014-0448-6 csb.scichina.com www.springer.com/scp Article Atomic & Molecular Physics Laser intensity induced transparency in atom-molecular transition process Jie Ma • Yuqing Li • Jizhou Wu • Liantuan Xiao Suotang Jia • Received: 8 January 2014 / Accepted: 17 April 2014 Ó Science China Press and Springer-Verlag Berlin Heidelberg 2014 Abstract We propose a new transparency mechanism, which is based on photoassociation (PA) laser intensity induced transitional frequency shift for ultracold cesium molecules formed in PA scheme. The PA laser intensity is supposed to change before the atom-molecule resonance. Thus, a remarkable transparent effect for PA laser is expected to appear in the vicinity of original resonant transitional line, where the variation of PA laser intensity induces the shift of the excited molecular levels. The mechanism is different from electromagnetically induced transparency effect and interesting for further research on the scattering length for cesium atomic condensate. Keywords Atom-molecular transition Ultracold Cesium molecules Laser induced frequency shift Laser intensity induced transparency 1 Introduction The atom-molecule system involved in the photoassociation (PA) process provides a spectacular platform that enables the physicists implementing various applications on high sensitive and high resolution measurements [1–3], which are essential for investigating the long-range molecular dipole-dipole interaction [4–6], atom-molecule collision [7, 8] and quantum information processing [9, 10], storage [11] and quantum simulation [12, 13]. Especially, J. Ma (&) Y. Li J. Wu L. Xiao S. Jia State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Laser Spectroscopy, College of Physics and Electronics Engineering, Shanxi University, Taiyuan 030006, China e-mail: [email protected] molecular dimmers populated in the ground state can be obtained by spontaneous decay from the optical excited molecule formed during single-color PA experiment [14]. Furthermore, the deeply bound ground state molecules can be produced by two-color PA through optical coupling with stimulated Raman transition [15, 16]. In the experimental and theoretical study of two-color PA spectroscopy, there was an interesting effect, i.e. the Autler–Townes splitting of the excited molecular level induced by the Raman laser, which was observed firstly from the signal of atom-loss in the PA progress in optically trapped 6Li MOT [17]. Importantly, the trapped cold atoms did not lose at the resonant position of the transitional line. The Electromagnetically Induced Transparency (EIT) [18] has been well known as a superposition of the long-lived system eigenstates decoupled from the light field [11]. The atom-molecule dark state was also observed in a Rb Bose–Einstein condensate by two-color PA [19]. So far, EIT has been demonstrated to extend to Doppler broadened molecular gas by using two photon transition related to a V-type molecular system in a vapor cell for sodium molecules [20]. The frequency shift of resonant transitional positions from atomic scattering states to molecular excited state is a significant finding. The frequency shifts in 7Li quantum degenerate gas [21] and Na Bose–Einstein condensate [22] were analyzed by semi-analytical channel scattering theory [23]. A more precise measurement for the shifts of the rovibrational level was developed in ultracold metastable 4 He atoms [24], in which the s-wave scattering length was determined. Recently, the high sensitive determination of PA laser-induced frequency shifts for ultralcold cesium molecules had been reported by employing a frequency shifter technique [25]. In the photoassociation process, a pair of cold alkali atoms, mainly at large inter-atomic distance, resonantly 123 Chin. Sci. Bull. absorbs a photon whose frequency red-detuned from the s?p atomic transition. Thus, a molecule with short lifetime is obtained mainly populated in a high-lying rovibrational level in the electronic excited state. In this paper, we theoretically present that a transparency would occur in the vicinity of the absolute resonance line by changing the PA laser intensity, as the PA laser frequency detuned to the atom-molecule resonant transitional line. We show that the variation of PA laser intensity induces a shift for the excited molecular levels, and consequently, the PA laser beam is not absorbed by the atoms with the resonant transitional frequency, but absorbs at a special red or blue detuning from the original resonant transitional frequency. We define this effect as an ‘‘artificial transparency’’, which occurs due to the manipulation of the PA laser intensity. 2 The semi-analytic line-shape formula In order to intuitively describe the interaction between the scattering atoms and laser field, a line-shape formula is deduced. The line-shape formulas had been suggested previously for single- [26] and two-color [27] PA spectra using atomic scattering theory. A general formula shows that the trap loss probability clearly separates laser intensity and detuning from the overlap integrals of molecular wave functions [23]. Correspondingly, laser-induced energy shift and line broadening are contained in this simplified line-shape formula (1), which is derived from the scattering matrix element of K rate coefficient, jsj2 ¼ cC ½E ðD þ E1 Þ2 þ cþC 2 2 ; ð1Þ where c and C means spontaneous radiation rate and stimulated rate, respectively; E is excited molecular energy, D is the detuning from the resonant transitional line, and E1 is laser induced energy shift for the excited molecular level. In the experiment, laser induced frequency shift of the atom-molecule resonant transitional line stems from the laser induced coupling between the atomic scattering state and the bound molecular state. The energy shifts show a linear dependence on laser intensity [25]. For the Cesium molecular case, the slopes for different vibrational levels and rotational progressions are listed in Table 1. Thus a simple function of energy shift versus PA laser intensity can be written as: E1 ¼ aI þ b; ð2Þ where a is the slope for the linear variation of energy shift versus PA laser intensity, b is the intercept, I is the PA laser intensity. 123 Table 1 The rate of laser induced frequency shift and molecular energy without perturbation v J Bound energy (cm-1) Slope (a) 4 4 11,661.954 -0.08396 11 4 11,672.943 -0.13676 17 4 11,681.337 -0.1531 17 3 11,681.326 -0.1207 17 2 11,681.317 -0.21958 3 Cesium atom-molecule system case In order to demonstrate the laser intensity induced transparency, a specific frequency was chosen, at which the PA laser intensity was set to 300 W/cm2, such that the resonant frequency is not influenced by the variation of PA laser intensity. The binding energy of excited molecule for different vibrational and rovibrational levels was listed in Ref. [28]. As PA laser intensity changed before the frequency detuned to the atom-molecule resonant transitional line, the transparency of PA laser thus occur in the PA process. In the experiment, a square wave pulse signal can be used to modulate the acoustic-optical modulator (AOM) through thus the PA laser intensity can be varied from I1 = 345 W/cm2 to I2 = 255 W/cm2. The start point of changing PA laser intensity is set corresponding to the original atommolecule resonant line, for example, *300 W/cm2. The binding energy level (v = 17, J = 2) of excited cesium molecular (6S1/2 ? 6P3/2) 0g state is chosen for the analysis. The new resonant lines will red and blue shifted for –10 and ?10 MHz from the original transitional frequency corresponding to a PA laser intensity of *300 W/cm2. This is calculated by Eq. (2) of PA laser-induced frequency shift. The atomic loss signal emerges as the frequency of PA laser detuned to the atom-molecule resonant transitional line where no modulation is applied. The PA laser intensity is kept to *300 W/cm2, and simultaneously, a direct current signal with a constant voltage is imported into the ‘‘Mod in’’ port of the AOM. The PA photon will be resonantly absorbed to bind two colliding atoms and form an excited molecule. As the PA laser red detuned from the original resonant transitional line, the PA laser intensity is changed to I1 = 345 W/cm2. And the laser intensity is averted to I2 = 255 W/cm2 immediately as the PA laser blue detuned from the transitional line. As a result, the excited molecular level will red shift for 10 MHz comparing with the original resonant line and blue shifted for 10 MHz, respectively just as Fig. 1 shown. The jdi state is the scattering state for two colliding ground atoms, and jbi is the excited molecular level. The jbi state would shift to jai or jci by changing the PA laser intensity between I1 = Chin. Sci. Bull. a AOM PA laser d Fig. 1 (Color online) PA laser intensity induced excited molecular energy shift schemes: The output power of PA laser will be varied between two different values by using a square wave signal to modulate AOM. Thus, the excited molecular energy shifts with different detunings (the two solid lines) to original resonant frequency (dash line) were obtained 345 W/cm2 and I2 = 255 W/cm2, corresponding to the red or blue detuning of the original resonant level jbi. As the PA laser frequency is scanned over a very large range, the number of the trapped atoms decreases obviously at the frequency detuned for ; 10 MHz from the original resonant transitional line, thus the fluorescence spectra of the atoms presents a transparency at the original resonant transitional position in the single color PA process, i.e. atoms do not lose by absorbing the photons from the PA laser. mainly determined by both c and C for a certain excited molecular state. According to the result of Ref. [29], the trap-loss probability reaches maximum amplitude and keeps invariable as increasing the PA laser intensity since the saturation intensity. This means that the value of C keeps invariable as the PA laser intensity reaches the saturation intensity. In order to avoid the influence from the variation of C, we define the resonant transitional frequency where PA laser intensity is *300 W/cm2 as the original atom-molecule resonant transitional line. This PA laser intensity is high enough to achieve the saturation effect in the PA process, and therefore the value of C is regarded as a constant and equals to c [29]. The trap-loss probability in PA process is demonstrated in Fig. 2 for different PA laser intensity. The new resonant position is obtained by changing the laser intensity and locates at the red and blue detuning to the original resonant transitional line with –10 and ?10 MHz respectively. This results from the variation of PA laser intensity induced shift of original resonant transitional frequency. Note that the PA laser intensity is large enough so that the saturation effect could be observed and thus enabled us simply employing a parameter for stimulated rate. For cesium molecule, we can obtain C & c & 10.4 MHz. Figure 3 shows the transparency occurring on the original resonant transitional line. The PA laser will be transparent in atom-molecule system when no loss signal emerges and PA laser is not absorbed by the colliding Scattering probability (a.u.) c b 4 Results and analyses According to the scattering theory [23], the stimulated rate of the trapped cold atoms in the PA process, namely C, is a function of the PA laser intensity I, 4p2 I jh/jf0 ij2 d2 ; c ð3Þ where u and f0 are the wavefunctions for bound excited molecular state and initial free atomic scattering state in PA process, respectively. d is the atom-molecule dipole matrix element and regarded as a constant. On the other hand, the spontaneous decay rate c is only determined by the coupling between the bound excited molecular state u and the ultimate atomic state f1, c ¼ 2pjh/jf1 ij2 V 2 ; ð4Þ where V is the artificial coupling element between the bound excited molecular state and the ultimate free atomic state. C increases with the PA laser intensity I, while c is almost a constant. When C equals to c, the saturation effect of PA occurs. The saturation intensity of PA laser Is is Dispersive index (a.u.) C¼ 0.04 (a) 0.03 0.02 0.01 0.00 (b) 0.0005 0.0000 –0.0005 –100 –80 –60 –40 –20 0 20 40 60 80 100 Detuning (MHz) Fig. 2 (Color online) a Solid line: the trap-loss probability as a function of the detuning to the resonant line with I = 390 W/cm2; dash line: the trap-loss probability corresponds to I = 345 W/cm2; dotted line: the trap-loss probability corresponds to I = 300 W/cm2. b The corresponding dispersive curves for curves in a 123 Chin. Sci. Bull. 0.02 new different resonant transitional lines are anticipated locating on both sides of the original resonant transitional line. The transparency of PA laser would emerge at the position of the original resonance line when the PA laser intensity varies before the original resonant transitional line. 0.01 5 Conclusions Dispersive index (a.u.) Scattering probability (a.u.) 0.04 (a) 0.03 (b) 0.0005 0.0000 –0.0005 –100 –80 –60 –40 –20 0 20 40 60 80 100 Detuning (MHz) Fig. 3 (Color online) PA laser intensity induced transparency. a Dash line: The trap-loss probability as a function of the detuning to the resonant line with I = 345 W/cm2; solid line: The trap-loss probability corresponds to I = 390 W/cm2 before the original resonance line and then I = 300 W/cm2, and reflects transparency effect by changing PA laser intensity; b the dispersive curves corresponds to graph (a) atoms in PA experiment. In addition, in Fig. 3b, a very steep dispersive signal indicates that the transparency for PA laser appears near the original resonant transitional line. The transparency of PA laser in an atom-molecular system is proposed by changing the PA laser intensity. The mechanism resulted in the transparency of PA laser is different from the EIT effect in the atomic system, which required a strong coupling laser and a weak probing laser, and involved in a coherent effect due to the dark quantum superposition state. We analyze this effect by using the semi-analytical coupling scattering theory, and the artificial potential is introduced to derive line-shape formula containing laser intensity induced energy shift. The artificial channel accounts phenomenologically for trap-loss processes in PA experiment, the energy shift is responsible for phase shifts due to the interaction between other channels [23]. According to the experimental result [25], we choose the excited molecular level (v = 17, J = 2) which has a very large rate for variation of frequency shift versus PA laser intensity, and thus obtain more frequency shifts data by changing PA laser intensity. For comparison, we present the curve of trap-loss probability in PA process and its dispersive curve with different laser intensities. The two 123 In conclusion, a new transparency mechanism is proposed, which is based on PA laser intensity induced transitional frequency shift for cesium molecules. This work is crucial for investigating the problem of the phase shift between the colliding scattering atomic pair and the rate of PA. The theoretical results shown in Fig. 3 are similar as the line shape of EIT effect or Coupled-Resonator-Induced Transparency (CRIT) effect [30]. The result we presented can be analyzed by trap-loss probability of PA process. The selfinduced transparency for the PA laser intensity is a different and interesting mechanism comparing with EIT and CRIT. The current atom-molecular system resorts to only one laser and does not involve in any coherent effects in the process. Further more, the location of the transparency can be controlled by modifying the PA laser intensity and thus the position of the resonant transitional lines can be easily relocated. Acknowledgments This work was supported by the National Basic Research Program of China (2012CB921603), the National High Technology Research and Development Program of China (2011AA010801), the Program for Changjiang Scholars and Innovative Research Team in University (IRT13076), the International Science and Technology Cooperation Program of China (2011DFA12490), the National Natural Science Foundation of China (NSFC) (61378014, 61308023 and 10934004), the NSFC Project for Excellent Research Team (61121064), the Specialized Research Fund for the Doctoral Program of Higher Education of China (20131401120012) and the Natural Science Foundation (NSF) for Young Scientists of Shanxi Province (2013021005-1). References 1. 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