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Chinese Physics B

Theoretical simulation of the photoassociation process for NaCs

Chang-Zhe Zhang, Bin Zheng, Jun Wang, Qingtian Meng

Published Feb 1, 2013• 6 citations
Publisher

Abstract

We investigate the two-step association process of NaCs using the time-dependent wave packet method. Ground state atoms can be photoassociated to the low vibrational levels of the ground state for an NaCs molecule by the two-step association. The time-dependent Schrödinger equation of the association process is solved within a three-state model and the wave packet is propagated with the “split operator-Fourier transform" scheme and the rotating-wave approximation (RWA). The vibrational population distribution of the ground state can be obtained by projecting the wave packet to every vibrational level of the ground state. The results not only show that for NaCs achievement of photoassociation production is accompanied by the photodissociation of the higher vibrational molecules, but also show that the vibrational distribution in lower vibrational levels of the ground state changes with the laser parameters.

DOI
10.1088/1674-1056/22/2/023401

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We investigate the two-step association process of NaCs using the time-dependent wave packet method. Ground state atoms can be photoassociated to the low vibrational levels of the ground state for an NaCs molecule by the two-step association. The time-dependent Schrödinger equation of the association process is solved within a three-state model and the wave packet is propagated with the “split operator-Fourier transform" scheme and the rotating-wave approximation (RWA). The vibrational population distribution of the ground state can be obtained by projecting the wave packet to every vibrational level of the ground state. The results not only show that for NaCs achievement of photoassociation production is accompanied by the photodissociation of the higher vibrational molecules, but also show that the vibrational distribution in lower vibrational levels of the ground state changes with the laser parameters.
This paper presents calculation results for the photoassociation of a NaK molecule with a two-color modulated laser and gives a detailed analysis about them. For the two-step photoassociation process in intense fields, the effect of two-color modulated laser parameters, such as relative phase, envelope period, and laser intensity, on the population of the molecular electronic state can be obtained by solving the time-dependent Schrödinger equation through the quantum wave packet method. The numerical simulation shows not only that the influence of laser parameters on the vibrational distribution presents some regularity, but also that a higher population in the ground electronic state can be realized through adjusting these laser parameters.
This paper aims at studying the time-dependent effects involved in the photoassociation reaction for a sample of cold alkali-metal atoms, within a two-channel model where the vibrational motion in the excited state is coupled by laser light to the continuum state describing two colliding atoms in the lowest triplet electronic state $(a{}^{3}{\ensuremath{\Sigma}}_{u}^{+}).$ Both photodissociation and photoassociation processes are considered at a time scale shorter than the radiative lifetime, so that spontaneous emission does not have to be considered. The characteristic times are then the vibrational period in the excited state, which for alkali-metal dimers can be estimated of the order of a few hundreds of picoseconds, and the Rabi period, depending upon the laser intensity. Numerical calculations using wave-packet propagation are performed for the coupling of the vibrational motion in the Cs21g(6s+6p3/2){\mathrm{Cs}}_{2}{1}_{g}{(6s+6p}_{3/2})Cs2​1g​(6s+6p3/2​) and ${a}^{3}{\ensuremath{\Sigma}}_{u}^{+}(6s+6s)$ channels by a cw laser slightly red detuned relative to the D2{\mathrm{D}}_{2}D2​ resonance line. The results show Rabi oscillations in the populations of the two channels during time intervals when the vibrational motion is stopped at the outer turning point. At intensities of $\ensuremath{\approx}250\mathrm{kW}{\mathrm{cm}}^{\ensuremath{-}2},$ a new characteristic time appears, a factor of 2 larger than the classical vibrational period, which corresponds to vibrational motion in the upper adiabatic potential created by the coupling. Such an effect modifies the scattering length for collisions in the lower state, and it clearly opens a possibility of control by tuning the laser intensity.
The formation of the NaH molecule from unaligned ultracold atoms via photoassociation (PA) is theoretically investigated by numerically solving the time-dependent Schrödinger equation including the vibrational and rotational degrees of freedom. The PA processes via one- and two-photon excitations are described. The calculated results show that the associated molecule can be prepared to a desired rovibrational state of the ground electronic state for NaH. Compared with the one-photon association probability, the two-photon association probability is obviously enhanced.
The laser-induced vibrational state-selectivity of product HF in photoassociation reaction H+F→HF is theoretically investigated by using the time-dependent quantum wave packet method. The population transfer process from the continuum state down to the bound vibrational states can be controlled by the driving laser. The effects of laser pulse parameters and the initial momentum of the two collision atoms on the vibrational population of the product HF are discussed in detail. Photodissociation accompanied with the photoassociation process is also described.
The photoassociation of alkali metal molecules (Rb2, Cs2, and RbCs) at short range is investigated in theory. Based on ab initio calculations to rationalize Franck–Condon filtering, the target states of photoassociation have been obtained. They correspond to vibrational transition levels from excited state (Rb2: v′{v}{\kern 1pt} 'v′ = 17–21, Cs2: v′{v}{\kern 1pt} 'v′ = 21–25, and RbCs: v′{v}{\kern 1pt} 'v′ = 18–22) to ground state. By using quantum wave-packet dynamic methods, the yields with time evaluation of the selected states are calculated interacting with a resonant laser pulse. Using gaussian pulse leads to the yield of Rb2 up to 82% at 860 fs. After a laser pulse, the positive chirp promotes the yield of vibrational states to increase, but the negative chirp inhibits it. That is to say, by changing the laser parameters and pulse shapes, it is much easier to control the photochemical process along desired direction. For photoassociation of alkali-metal dimers, homonuclear molecules have a better response to laser pulse than heteronuclear molecules. The efficiency of photochemical reaction of homonuclear molecules is much better and the photoassociative yield is much higher. Those conditions will provide an important reference and suggest a scheme for a feasible photoassociation for further experimental and theoretical research.
We demonstrate that a photoassociation resonance detuned less than a wave number below the Cs 62P3/26 {}^{2}{P}_{3/2}62P3/2​ atomic line can be used to create a deeply bound molecular sample of ultracold polar NaCs. We assign $1 {}^{1}{\ensuremath{\Sigma}}^{+}$ (v=4,5,6,11,19v=4,5,6,11,19v=4,5,6,11,19) vibrational levels utilizing a pulsed depletion spectroscopic method (scanning  700~700 700 cm${}^{\ensuremath{-}1}$ at a time) in which we observe the $1 {}^{1}{\ensuremath{\Sigma}}^{+}\ensuremath{\rightarrow}2 {}^{1}{\ensuremath{\Sigma}}^{+}\ensuremath{-}1 {}^{3}\ensuremath{\Pi}$ vibrational progression. These data are compared with results from a hot-molecule collision-enhanced laser-induced fluorescence experiment and shown to be in good agreement. This technique is a powerful tool to experimentally determine the population distribution in any ultracold molecular system.