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Physical Review A

Thermal-average effects on photoassociation with a slowly-turned-on and rapidly-turned-off laser pulse

Yong‐Chang Han, Jinwei Hu, Binbin Wang

Published Oct 15, 2018• 11 citations
Publisher

Abstract

We investigate theoretically the photoassociation (PA) of two $\mathrm{Cs}$ atoms using a slowly-turned-on and rapidly-turned-off (STRT) laser pulse at the temperature of $54\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{K}$ by taking the thermal average of the initial continuum states into account. For comparison, the PA probabilities under the action of the STRT and typical Gauss-type pulses are calculated, respectively. The rising and falling times of the STRT pulse are set to be ${\ensuremath{\tau}}_{r}=10$ ps and ${\ensuremath{\tau}}_{f}=0.2$ ps, and the two Gauss-type pulses are set to be ${\ensuremath{\tau}}_{r}={\ensuremath{\tau}}_{f}=10$ ps and ${\ensuremath{\tau}}_{r}={\ensuremath{\tau}}_{f}=5.1$ ps, respectively. Compared to the calculation considering a single initial continuum state (non-thermal-average calculations), the PA probabilities with the consideration of the thermal average are reduced to different extents according to different laser pulses. The PA process induced by the STRT pulse is more robust than that by the two Gauss-type pulses. For the STRT pulse, the PA probability is reduced by roughly 30%, while for the two Gauss-type pulses, it is reduced by roughly 97% and 64%, respectively. Because of the larger bandwidth and the asymmetric time profile of the STRT pulse, the PA probability induced by this pulse is related to both the off-resonant and the near-resonant transitions in a much broader phase space formed by the initial continuum states and the final vibrational states. Consequently, the thermal average of the initial continuum states has relatively smaller influence on the PA probability induced by the STRT pulse. By changing the pulse shape of the standard Gaussian to the ${\mathrm{sin}}^{2}$ and the Lorentz ones, the STRT pulse still results in the highest PA probability and is the most robust to the thermal average.

DOI
10.1103/physreva.98.043420

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We investigate theoretically the photoassociation (PA) of two Cs\mathrm{Cs}Cs atoms using a slowly-turned-on and rapidly-turned-off (STRT) laser pulse at the temperature of 54\ensuremathμK54\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{K}54\ensuremathμK by taking the thermal average of the initial continuum states into account. For comparison, the PA probabilities under the action of the STRT and typical Gauss-type pulses are calculated, respectively. The rising and falling times of the STRT pulse are set to be \ensuremathτr=10{\ensuremath{\tau}}_{r}=10\ensuremathτr​=10 ps and \ensuremathτf=0.2{\ensuremath{\tau}}_{f}=0.2\ensuremathτf​=0.2 ps, and the two Gauss-type pulses are set to be \ensuremathτr=\ensuremathτf=10{\ensuremath{\tau}}_{r}={\ensuremath{\tau}}_{f}=10\ensuremathτr​=\ensuremathτf​=10 ps and \ensuremathτr=\ensuremathτf=5.1{\ensuremath{\tau}}_{r}={\ensuremath{\tau}}_{f}=5.1\ensuremathτr​=\ensuremathτf​=5.1 ps, respectively. Compared to the calculation considering a single initial continuum state (non-thermal-average calculations), the PA probabilities with the consideration of the thermal average are reduced to different extents according to different laser pulses. The PA process induced by the STRT pulse is more robust than that by the two Gauss-type pulses. For the STRT pulse, the PA probability is reduced by roughly 30%, while for the two Gauss-type pulses, it is reduced by roughly 97% and 64%, respectively. Because of the larger bandwidth and the asymmetric time profile of the STRT pulse, the PA probability induced by this pulse is related to both the off-resonant and the near-resonant transitions in a much broader phase space formed by the initial continuum states and the final vibrational states. Consequently, the thermal average of the initial continuum states has relatively smaller influence on the PA probability induced by the STRT pulse. By changing the pulse shape of the standard Gaussian to the sin2{\mathrm{sin}}^{2}sin2 and the Lorentz ones, the STRT pulse still results in the highest PA probability and is the most robust to the thermal average.
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We present a theoretical scheme used for investigating the formation of ultracold molecules via photoassociation with a slowly-turned-on and rapidly-turned-off (STRT) laser pulse, with Cs2{}_{2}2​ as an example. As compared with an unshaped laser pulse, this kind of shaped laser pulse has a prominent advantage by which we can prevent the associated molecules from returning to the initial scattering state. Numerical calculations show that an efficient photoassociation can be realized with the STRT laser pulse, which is available in the current experiment as an optical tool.
The photoassociation (PA) dynamics implemented by a train of asymmetric slowly turned-on and rapidly turned-off (STRT) laser pulses is investigated theoretically with Cs2{}_{2}2​ as an example. A higher PA efficiency is achieved by optimizing the parameters of the STRT pulse train. The PA reaction goes partly beyond the scope of the PA window. Numerical calculations show that an efficient population accumulation in the PA process can be realized with the STRT laser-pulse train which is available in the current experiment based on laser mode-lock and shaping technology.
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By taking the femtosecond two-photon photoassociation (PA) of magnesium atoms as an example, we propose a method to calculate the thermally averaged population, which is transferred from the ground X1Σg+ state to the target (1)1Πg state, based on the solution of full-dimensional time-dependent Schrödinger equation. In this method, named as method A, we use thermal-random-phase wavefunctions with the random phases expanded in both the vibrational and rotational degrees of freedom to model the thermal ensemble of the initial eigenstates. This method is compared with the other two methods (B and C) at different temperatures. Method B is also based on thermal-random-phase wavefunctions, except that the random-phase expansion is merely used for the vibrational degree of freedom. Method C is based on the independent propagation of every initial eigenstate, instead of the thermal-random-phase wavefunctions. Taking the (1)1Πg state as the target state, it is found that although these three methods can present the same population on the (1)1Πg state, the computation efficiency of method A increases dramatically with the increase in temperature. With this efficient method A, we find that the PA process at 1000 K can also induce rotational coherence, i.e., the molecular field-free alignment in the excited electronic states.
Photoassociation is a possible route for the formation of chemical bonds. In this process, the binding of colliding atoms can be induced by means of a laser field. Photoassociation has been studied in the ultracold regime and also with temperatures well above millikelvins in the thermal energy domain, which is a situation commonly encountered in the laboratory. A photoassociation mechanism can be envisioned based on the use of infrared pulses to drive a transition from free colliding atoms on the electronic ground state to form a molecule directly on that state. This work takes a step in this direction, investigating the laser-pulse-driven formation of heteronuclear diatomic molecules in a thermal gas of atoms including rotational effects. Based on the assumption of full system controllability, the maximum possible photoassociation yield is deduced. The photoassociation probability is calculated as a function of the laser parameters for different temperatures. Additionally, the photoassociation yield induced by subpicosecond pulses of a priori fixed shape is compared to the maximum possible yield.