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Acta Physica Sinica

Population transfer of HF molecules in the ground electronic state through multiphoton transition

Rong Wang, Jun-Ling Xiu, Niu Ying-Yu

Published Jan 1, 2013• 2 citations
Publisher

Abstract

The multiphoton transition is investigated theoretically by using wave packet method for the ground electronic state of HF molecule. A laser field composed of two overlapping infrared pulses is used in our model, and the ratio of their frequencies is 1:2. States |4,0> and |4,2> are chosen as target states. Calculated results show that the population can be transferred to different target states as the corresponding resonant frequency is chosen. The probability of the population transfer can be controlled by the initial phase difference of the two pulses. When the initial phase difference is of an odd number of π/2, the probability of population transfer reaches the maximal value. When the initial phase difference is of an even number of π/2, the probability of population transfer reaches the minimum value. In comparison with the state |4,2>, the initial phase difference has a stronger in fluence on the population of the state |4,0>.

DOI
10.7498/aps.62.093301

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The multiphoton transition is investigated theoretically by using wave packet method for the ground electronic state of HF molecule. A laser field composed of two overlapping infrared pulses is used in our model, and the ratio of their frequencies is 1:2. States |4,0> and |4,2> are chosen as target states. Calculated results show that the population can be transferred to different target states as the corresponding resonant frequency is chosen. The probability of the population transfer can be controlled by the initial phase difference of the two pulses. When the initial phase difference is of an odd number of π/2, the probability of population transfer reaches the maximal value. When the initial phase difference is of an even number of π/2, the probability of population transfer reaches the minimum value. In comparison with the state |4,2>, the initial phase difference has a stronger in fluence on the population of the state |4,0>.
A time-dependent quantum wave-packet method is employed to investigate the rovibrational dynamics of population transfer in the ground electronic state controlled by two-color ($\ensuremath{\omega}+2\ensuremath{\omega}$) pulses analogous to coherently control the processes of ionization and dissociation. The population can be transferred to three target states, $|4,1\ensuremath{\rangle},\phantom{\rule{0.16em}{0ex}}|0,1\ensuremath{\rangle}$, and $|4,0\ensuremath{\rangle}$, at the same time through the ladder $\ensuremath{\Lambda}$ and multiphoton transitions. With the variation of the relative phase between $\ensuremath{\omega}$ and $2\ensuremath{\omega}$ pulses, the population distributions show oscillation behavior with a period of $\ensuremath{\pi}$. The population variation with relative phase depends on the size of the electric field asymmetry. The probabilities transferred to different target states can be controlled by varying the pulse amplitudes.
The processes of population transfer in the ground electronic state of HCl molecule through the three transition schemes are investigated by numerically solving the time-dependent Schrödinger equation. Two harmonic pulses are employed to induce population transfer and the relative phase of the two pulses can control the final population distributions. In the ladder transition scheme, the variation range of the target population with the relative phase is nearly 100% which is larger than that in the multi-photon transition scheme. It is more efficient for the mixed transition scheme to control population transfer between the initial and target states by using the relative phase. Comparing with the multi-photon and ladder schemes, the transition probability of the target population is more sensitive to the two pulse amplitudes in the mixed transition scheme.
Rovibrational population transfer is controlled by a two-overlapping- pulse scheme in which the frequency ratio of the two pulses is 1:3. The calculated results show that nearly 100% of the population can be transferred from initial state |0,0to target state |3,1. The probability of population transfer can be controlled by pulse phase. When 1 =1.68 , the two pulses can be increased mutually and the probability of population transfer is also increased. When 1 =0.64 , the two pulses can be offset mutually and the probability of population transfer is reduced. The intensity of the second pulse has a significant effect on the population transfer.
The population transfer of stimulated Raman adiabatic passage (STIRAP) is investigated using a time-dependent quantum wave packet method. The population is transferred from an initial state to a target state through the interaction of the external laser field with the permanent dipole moment and the transition dipole moment. The laser field is composed of an infrared pulse and a near ultraviolet pulse. The two pulses with small detunings are more efficient to achieve the STIRAP transition. The process of STIRAP is sensitive to the detunings of the two pulses. When the two detunings are the same in a Λ transition or the positive detuning of the pump pulse is equal to the negative detuning of the Stokes pulse in a ladder transition, the final population in the intermediate state can be eliminated and the target population is increased.
Efficient population transfer by adiabatically chirping through a multiphoton resonance in microwave driven and kicked Rydberg atoms has recently been reported both experimentally and theoretically. Here we report on our simulations in which we have exploited this mechanism to vibrationally excite a diatomic molecule up to |ν = 4, J from the ground state by chirping through a four-photon resonance condition. This is an efficient means of population transfer, which is an alternative to the ladder climbing scheme requiring chirping through a sequence of states in the correct order. We discuss and compare one-dimensional quantum and classical models where there is no rotational degree of freedom. This comparison suggests that for the lowest laser intensity we consider, the process is classically forbidden and the transition occurs through tunnelling. We show that for larger peak intensities, the transfer can be looked upon as a classical transition in phase space, similar to that observed in the atomic case. We extend our simulations to fully three-dimensional quantum calculations and investigate the effect of coupling between different rotational pathways. We finally discuss the effect of thermal averaging over the initial J-states using a temperature for which the first few rotational levels inside the ν = 0 manifold are populated.
The rovibrational dynamics of an extended ladder stimulated Raman adiabatic passage (STIRAP) system through permanent dipole moment transitions is investigated theoretically using the time-dependent quantum-wave-packet method for the ground electronic state of the HF molecule. The calculated results show that nearly 100% of the population can be transferred to the target state through (1+2), (1+3), and (2+2) STIRAP schemes. By choosing a suitable excitation pathway, the effects of the background states on the final population of the target state can be removed. For the multiphoton STIRAP process, the one-photon overtone pump scheme is more efficient than the two-photon pump scheme in controlling the population transfer to the target state.