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Chinese Physics Letters

Rovibrational Formation of Ultracold NaH Molecules Induced by an Ultrashort Laser Pulse

Qianzhen Su, Yu Jie, Niu Ying-Yu, Shu‐Lin Cong

Published Sep 1, 2010• 5 citations
Publisher

Abstract

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.

DOI
10.1088/0256-307x/27/9/093401

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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 formation of NaH molecules in the lowest rovibrational level of the ground electronic state is investigated using a pump-dump photoassociation (PA) scheme. In short-range region, two colliding atoms Na and H are efficiently associated into the NaH molecule in the rovibrational |0,0〉 state of the ground electronic state via the intermediately rovibrational |10,1〉 state of the excited electronic state. The changes of populations with the electric field amplitudes, frequency detunings, dump pulse duration and delay time between two laser pulses are calculated and discussed. The PA probability reaches 0.623 with a high state-selectivity.
Photoassociation of ultracold atoms with pulsed laser light is shown to lead to alignment of the product molecules along the excitation laser polarization axis. We theoretically investigate pulsed two-photon photoassociation of 87Rb^{87}\mathrm{Rb}87Rb atoms into a specific weakly bound level of the $a{\phantom{\rule{0.16em}{0ex}}}^{3}{\mathrm{\ensuremath{\Sigma}}}_{u}^{+}$ metastable electronic state and find both stationary and time-dependent field-free alignment. Although a transform-limited pulse yields significant alignment, a frequency-chirped pulse dramatically enhances the ultracold molecular formation rate at the cost of a slight decrease in the alignment. Employing multiple pulses synchronized with the vibrational and rotational periods leads to coherent enhancement of both population and alignment of the target state. Inclusion of the rotational degree of freedom in the model gives rise to processes with multiple quantum paths, which lead to quantum effects such as interference and coherence revivals.
The formation of ultracold Cs 2 molecules via photoassociation (PA) with a spectral π-jump laser pulse is theoretically investigated by solving the time-dependent Schrödinger equation using the mapped Fourier grid method. Numerical calculations show that the population distributions of associated molecules mainly result from the off-resonant excitation of the π-jump laser pulse. Compared with the transform-limited pulse, an efficient population accumulation in the PA process is achieved with the π-jump pulse. An oscillation pattern appears in the population on the vibrational levels of the state owing to the action of the post-half-pulse in the π-jump pulse. The PA efficiency is related to the Rabi angle of the laser pulse. A π-jump pulse can be used to enhance more effectively the PA efficiency than a transform-limited pulse with the same Rabi angle.
Alkali-metal hydride molecules have large dipole moments in their ground electronic states. We explore the possibility of forming such molecules from a mixture of the ultracold atomic gases, employing a one-photon stimulated radiative association process. Using accurate molecular potential-energy curves and dipole moments, we have calculated the rate coefficients for populating each of the vibrational levels of the $X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}^{+}$ states of LiH and NaH. We have found that significant molecule formation rates into the upper vibrational levels can be realized with laser intensities and atomic densities that are easily attainable experimentally. We examine the spontaneous emission cascade which takes place from these upper vibrational levels on a time scale of milliseconds, and calculate the resulting rotational populations in v=0v=0v=0. We show that photon emission in the cascade process does not contribute to trap loss and that a large population of molecules in v=0v=0v=0 can be achieved.
We investigate theoretically the formation of ultracold Cs2 molecules via photoassociation (PA) with three kinds of pulses (the Gaussian pulse, the asymmetric shaped laser pulse SL1 with a large rising time and a small falling time and the asymmetric shaped laser pulse SL2 with a small rising time and a large falling time). For the three kinds of pulses, the final population on vibrational levels from v′ = 120 to 175 of the excited state displays a regular oscillation change with pulse width and interaction strength, and a high PA efficiency can be achieved with optimised parameters. The PA efficiency in the excited state steered by the SL1-pulse (SL2-pulse) train with optimised parameters which is composed of four SL1 (SL2) pulses is 1.74 times as much as that by the single SL1 (SL2) pulse due to the population accumulation effect. Moreover, a dump laser is employed to transfer the excited molecules from the excited state to the vibrational level v″ = 12 of the ground state to obtain stable molecules.
The formation of diatomic molecules with rotational and vibrational coherence is demonstrated experimentally in free-to-bound two-photon femtosecond photoassociation of hot atoms. In a thermal gas at a temperature of 1000 K, pairs of magnesium atoms, colliding in their electronic ground state, are excited into coherent superpositions of bound rovibrational levels in an electronically excited state. The rovibrational coherence is probed by a time-delayed third photon, resulting in quantum beats in the UV fluorescence. A comprehensive theoretical model based on ab initio calculations rationalizes the generation of coherence by Franck-Condon filtering of collision energies and partial waves, quantifying it in terms of an increase in quantum purity of the thermal ensemble. Our results open the way to coherent control of a binary reaction.