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Acta Physica Sinica

Lie algebraic approach to vibrational populations of diatomic molecules in infrared laser fields

Fang Liu, Jun Wang, Juan Zhao, Yan Xu, Meng Qing-Tian

Published Jan 1, 2011• 4 citations
Publisher

Abstract

In this paper, we study the vibrational populations of diatomic molecules in infrared fields using algebraic approach, and obtain the explicit analytical expression of the transition probability. The influences of frequency, intensity and pulse duration on the vibrational populations, which belong to, respectively, the ground state and the first excited state of vibration in NaCl and LiH molecular systems, are discussed.

DOI
10.7498/aps.60.040202

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In this paper, we study the vibrational populations of diatomic molecules in infrared fields using algebraic approach, and obtain the explicit analytical expression of the transition probability. The influences of frequency, intensity and pulse duration on the vibrational populations, which belong to, respectively, the ground state and the first excited state of vibration in NaCl and LiH molecular systems, are discussed.
Excitation of multilevel Rydberg states (atoms and diatomic molecules) is studied under an intense time-periodic perturbation that is instantaneously turned on and off. For a one-quantum excitation from a lower lying state, general expressions for the Laplace images of the population amplitudes of Rydberg states are obtained with regard to their decay characteristics. It is shown that the problem considered is reduced to the determination of the positions and widths of the energy levels of a quantum system in the field of monochromatic laser radiation of the same frequency and intensity as that in a pulse mode. To determine these quantities, an integral formulation is proposed for the eigenvalue problem for energies that is relatively simply solved with regard to the effect of the ionic core and its complex vibration-rotation structure on diatomic molecules. The specific features of the excitation of Rydberg states and the behavior of Rydberg wave packets are studied depending on the intensity and duration of laser radiation. A quantum phenomenon of rotational orientation of electron-excited diatomic molecules is considered.
A coherent control scheme for the population distribution in the vibrational states of nonpolar molecules is proposed. Our theoretical analysis and results of numerical simulations for the interaction of the hydrogen molecular ion in its electronic ground state with an infrared laser pulse reveal a selective two-photon transition between the vibrational states via a coupling with the first excited dissociative state. We demonstrate that for a given temporal intensity profile the population transfer between vibrational states, or a superposition of vibrational states, can be made complete for a single chirped pulse or a train of chirped pulses, which accounts for the accumulated phase difference due to the ac Stark effect. Effects of a spatial intensity (or focal) averaging are discussed.
We explore the possibility of using shaped infrared laser pulses to deexcite a homonuclear diatomic molecule from its highest vibrational state down to its ground vibrational state. The motivation for this study arises from the need to deexcite alkali metal dimers in a similar way so as to stabilize molecular Bose-Einstein condensates. We demonstrate that for the case of the H(2) molecule, where it is possible to evaluate all the necessary high accuracy ab initio data on the interaction of the molecule with an electric field, we are able to successfully design a sequence of infrared laser pulses to accomplish the desired deexcitation process in a highly efficient manner.
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The absolute laser phase dependence of the time-dependent populations of the molecular states, including the steady-state (long time) populations of the states, associated with the interaction of a molecule with a pulsed laser is investigated using illustrative two-level examples. One-photon transitions, including the effects of permanent dipoles, are discussed as a function of the pulse duration, intensity, and (absolute) laser phase, for selected laser frequencies. The effects of laser phase can be large, depending on the values of the pulse duration for a given frequency and intensity. The effects of permanent dipoles, relative to no permanent dipoles, are significant for large laser field strengths ε0. When the laser-molecule coupling parameter b=μ12ε0/E21⩾0.2, where μ12 and E21 are the transition dipole and energy difference between the ground and excited states, respectively, the dynamics of the pulse-molecule interaction are (strongly) phase dependent, independent of pulse duration, whereas the corresponding steady-state populations of the molecular states may or may not be phase-dependent depending on the pulse duration. Analytical rotating wave approximations for pulsed laser-molecule interactions are useful for interpreting the dynamics and the steady-state results as a function of field strength and pulse duration, including the effects of permanent dipole moments. The results reported in this paper are based on molecular parameters associated with an S0→S1 electronic transition in a dipolar molecule. However, they are presented in reduced form and therefore can be scaled to other regions of the electromagnetic spectrum. Short, intense pulses at or beyond the limits of current laser technology will often be required for the types of absolute laser phase effects of this paper to be appreciable for electronic excitations. The discussion, in the UV-VIS, also suffers from the use of a two-level model and from the requirement of field intensities that can be beyond the Keldysh limit. For other spectral regions, these absolute laser phase effects will be much more readily applicable.