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AIP conference proceedings

Control of cis-trans isomerization by stimulated Raman adiabatic passage method

Takahiro Yamaguchi

Published Jan 1, 2004• 1 citation
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 complete transfer between all‐trans and 11‐cis in the retinal.
DOI
10.1063/1.1764310

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We describe the exploitation of adiabatic transfer of population between selected states of a molecule as a means for the control of product selectivity in a branching unimolecular reaction. The particular procedures employed to achieve that adiabatic transfer of population depend on the character of the spectrum of states of the molecule; the ones we consider are either extensions of, or are illuminated by, the STIRAP method. The results of studies of efficient selective population of one of a pair of nearly degenerate states in the thiophosgene molecule, and of efficient promotion of the HCN → CNH isomerization reaction, are reported. In the former case the adiabatic population transfer is achieved by use of the Kobrak-Rice extended STIRAP method, while in the latter case it is achieved by use of consecutive STIRAP processes. In both cases the efficiency of selective population transfer is shown to be insensitive to radiative
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.
In this paper we extend the existing theory of stimulated Raman adiabatic passage (StiRAP) in three-level systems to examine the nature of selective photoexcitation using counterintuitively ordered pulses. Our goal is to develop a version of StiRAP that permits control of product selectivity in a chemical reaction. We analyze the case of selective excitation to one state in a pair of degenerate target states in a four-level system, and find that one cannot control the ratio of the populations in the two states in a resonant two-photon process. However, the extension of the system to include a fifth state and a third laser field makes selective excitation to one of the degenerate states possible. It is found that, subject to reasonable restrictions, one may accomplish complete population transfer to a single target state of a degenerate pair of states in a five-level system.
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 use a 28-level system consisting of the vibrational bend states of the HCN/HNC system as a model system for the investigation of population transfer across the isomerization barrier using counterintuitively ordered multiphoton (MP) laser pulses. This (m+n)-STIRAP (stimulated Raman-adiabatic passage) arrangement with m pump- and n Stokes-photons is found to be capable of driving HCN→HNC transition states selectively and in a robust manner, despite the presence of near-degenerate parallel processes of different photonicities. Employing Gaussian pulses with widths of 80 ps, the process of highest photonicity we demonstrate is (4+6)-STIRAP, and we investigate systematically the robustness against variations in pulse amplitudes and frequencies for all parallel processes with m=2 and 3, and n=1–6. We discuss the conditions under which selective population transfer is obtained. We also compare with (1+1)-STIRAP using overtone transitions to drive the same state-specific processes and conclude that the few-step sequential MP-STIRAP isomerization is a feasible alternative to the sequential (1+1)-STIRAP based method proposed by Kurkal and Rice [J. Phys. Chem. B 105, 6488 (2001)].