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Physical Review A

Stimulated Raman adiabatic passage in molecular electronic states

Chuan‐Cun Shu, Jie Yu, Kai‐Jun Yuan, Wenhui Hu, Jing Yang, Shu‐Lin Cong

Published Feb 17, 2009• 44 citations
Publisher

Abstract

We explore theoretically the rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) in molecular electronic states including both the rotational and the vibrational degrees of freedom, with the LiH molecule as an example. By using a pure rovibrational state as initial state, we find that, under the condition of two-photon resonance, an efficient rovibrational population transfer can be achieved via STIRAP in molecular electronic states and the desired target state can be selected by adjusting laser-pulse parameters. Besides the interested rovibrational states, however, some unwanted rovibrational states may affect population transfer process, especially while the two-photon detuning is taken into account. By inspecting the evolution process of wave packet, we can easily search these unwanted rovibrational states and study their influences. Moreover, the effect of rotational temperature on the population transfer process is discussed using thermal mixed state as initial state.

DOI
10.1103/physreva.79.023418

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Physical Review A•Sep 10, 2014•19 citations
We explore theoretically the rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) in molecular electronic states including both the rotational and the vibrational degrees of freedom, with the LiH molecule as an example. By using a pure rovibrational state as initial state, we find that, under the condition of two-photon resonance, an efficient rovibrational population transfer can be achieved via STIRAP in molecular electronic states and the desired target state can be selected by adjusting laser-pulse parameters. Besides the interested rovibrational states, however, some unwanted rovibrational states may affect population transfer process, especially while the two-photon detuning is taken into account. By inspecting the evolution process of wave packet, we can easily search these unwanted rovibrational states and study their influences. Moreover, the effect of rotational temperature on the population transfer process is discussed using thermal mixed state as initial state.
The rovibrational dynamics of stimulated Raman adiabatic passage (STIRAP) through permanent dipole moment transitions are investigated theoretically using a time-dependent quantum wave packet method for the ground electronic state of an HF molecule. The two basic STIRAP processes, $\ensuremath{\Lambda}$ and ladder systems, are simulated. The calculated results show that nearly 100100%100 of the population can be transferred to the target state. Besides the interested transitions, the pulses can induce other transitions which affect the dynamics of STIRAP. The final populations of the initial and target states depend on delay time.
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.
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.
We have developed a new type of stimulated Raman adiabatic passage (STIRAP) that is applicable to a degenerated reaction system. The direction of the photon polarization vector is the adiabatic parameter in the STIRAP. The molecular handedness of H2POSH, a preoriented phosphinotioic acid that has two stable configurations, L and R enantiomers, is used as a model system. The control of molecular handedness in both pure and mixed state cases are considered. In the case of a pure state, a STIRAP with a linearly polarized single laser allows an almost complete transfer from an L (R) enantiomer to the other by adiabatically changing its polarization direction. The adiabatic criterion for changing the polarization direction is clarified. In the case of a mixed state, a STIRAP with two linearly polarized laser pulses allows a selective preparation of pure enantiomers from its racemic mixture. In the low temperature limit, a five-level model reduces a three-level model by setting the direction of the polarization of the pump and Stokes pulses in such a way that only the forward transfer is allowed, while the reverse is forbidden. Furthermore, in the case of mixed state, relaxation effects originating from vibrational mode couplings are taken into account, and the influence of the population decay from intermediate states on the STIRAP is compared with that by a π-pulse approach.
Abstract The population transfer of a NaH molecule from the ground state X 1 Σ + to the target state A 1 Σ + via stimulated Raman adiabatic passage (STIRAP) is investigated. The results show that the intensity, delay time and detuning have a significant effect on population transfer. A large population transfer is observed with increased pump and Stokes intensity, especially when the pump and Stokes intensity match. Population transfer also depends on the delay time between the pump laser pulse and the Stokes laser pulse. The detuning of the two pulses influences the population transfer. Efficient population transfer can be realized under the resonant or two-photon resonant condition.
This paper begins with the premise that stimulated Raman adiabatic passage (STIRAP) from one state to another by coupling to an intermediate state necessarily requires some population of that intermediate state. The usual view of the process depends on having no population in the intermediate state, but a simple argument from the time-dependent Schr\"odinger equation shows that such adiabatic transfer cannot occur. From another perspective, removing the time dependence of the Hamiltonian by making the rotating frame transformation cancels the optical frequency oscillations but does not account for the envelopes of the pulses commonly used for STIRAP. By assuming a small but finite intermediate state amplitude ${\ensuremath{\varepsilon}}_{1}$ in the wave function, the propagator for the evolution between initial and final states is derived. Applying the propagator to the initial state produces a single compact formula for the final intermediate-state population that is readily evaluated for an arbitrary choice of laser pulse parameters. Several plots for various experimental conditions show that under the conditions normally used for STIRAP experiments the effects are typically a few percent or less, but in the end this effect puts an ultimate limit on total efficiency.