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AIP conference proceedings

Laser control of non-stationary proton state in hydrogen-bonded system

Takahiro Yamaguchi

Published Jan 1, 2004• 0 citations
Publisher

Abstract

Stimulated Raman adiabatic passage method (STIRAP) is well known to be a very effective method for the efficient and selective transition between two molecular eigenstates in molecule. In this study, we generalize the STIRAP to be able to treat the transition to the non‐stationary state in the hydrogen bonded model system.
DOI
10.1063/1.1764307

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The effects of a background state, or states, on stimulated Raman adiabatic passage (STIRAP) processes are investigated. The study is based on a realistic model of the laser-assisted $\mathrm{HCN}\ensuremath{\rightarrow}\mathrm{HNC}$ isomerization process. While the high density of states in the energy regime above the isomerization barrier plays an important role, the strong variation of the transition dipole moments connecting these states with the localized HCN and HNC states is shown to be more significant in determining the success or failure of the STIRAP process. Therefore, care must be taken when proposing the use of STIRAP-based schemes to control molecular excitation especially when control is justified via few-level models.
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.
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.
We have studied the formation of ultracold RbSr molecules with laser pulses. After discussing the advantages of the Mott insulator phase for the control with pulses, we present two classes of strategies. The first class involves two electronic states. Two extensions of stimulated Raman adiabatic passage (STIRAP) for multilevel transitions are used: alternating STIRAP (A-STIRAP) and straddle STIRAP (S-STIRAP). Both transfer dynamics are modeled and compared. The second class of strategies involves only the electronic ground state and uses infrared (IR) and terahertz (THz) pulses. The molecular bond is first created by the application of a THz chirped pulse or $\ensuremath{\pi}$-pulse. Subsequently, the molecules are transferred to their rovibrational ground level using IR pulses. For this last step, different optimized pulse sequences that were obtained through optimal control techniques have been studied. The relative merits of these strategies in terms of efficiency and robustness are discussed with respect to the experimental feasibility based on present laser technologies.
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.