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arXiv:quant-ph/0403086 · The Journal of Chemical Physics

Measurement-assisted coherent control

Jiangbin Gong, Stuart A. Rice

Published May 10, 2004• 42 citations
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Abstract

Two advantageous roles of the influence of measurement on a system subject to coherent control are exposed using a five-level model system. In particular, a continuous measurement of the population in a branch state in the Kobrak-Rice extended stimulated Raman adiabatic passage scheme is shown to provide a powerful means for controlling the population transfer branching ratio between two degenerate target states. It is demonstrated that a measurement with a large strength may be used to completely shut off the yield of one target state and that the same measurement with a weak strength can dramatically enhance the robustness of the controlled branching ratio against dephasing.

DOI
10.1063/1.1735644

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Two advantageous roles of the influence of measurement on a system subject to coherent control are exposed using a five-level model system. In particular, a continuous measurement of the population in a branch state in the Kobrak-Rice extended stimulated Raman adiabatic passage scheme is shown to provide a powerful means for controlling the population transfer branching ratio between two degenerate target states. It is demonstrated that a measurement with a large strength may be used to completely shut off the yield of one target state and that the same measurement with a weak strength can dramatically enhance the robustness of the controlled branching ratio against dephasing.
A five-level four-pulse phase-sensitive extended stimulated Raman adiabatic passage scheme is proposed to realize complete control of the population transfer branching ratio between two degenerate target states. The control is achieved via a three-node null eigenstate that can be correlated with an arbitrary superposition of the target states. Our results suggest that complete suppression of the yield of one of two degenerate product states, and therefore absolute selectivity in photochemistry, is achievable and predictable, even without studying the properties of the unwanted product state beforehand.
A five-level four-pulse phase-sensitive extended stimulated Raman adiabatic passage scheme is proposed to realize complete control of the population transfer branching ratio between two degenerate target states. The control is achieved via a three-node null eigenstate that can be correlated with an arbitrary superposition of the target states. Our results suggest that complete suppression of the yield of one of two degenerate product states, and therefore absolute selectivity in photochemistry, is achievable and predictable, even without studying the properties of the unwanted product state beforehand.
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
Two-pulse selective photochemistry that exploits population transfer via adiabatic passage is considered for the case that there are degenerate product states with different lifetimes. As an example, a four-level model system with a complex symmetric Hamiltonian is constructed. Analytical and numerical studies of this model system demonstrate that extensive control over the product branching ratio can be achieved by detuning either the pump pulse or the Stokes pulse while maintaining negligible population in the intermediate state. This control approach represents a significant simplification of both the Kobrak-Rice extended stimulated Raman adiabatic passage scheme and the Chen-Shapiro-Brumer strong-field control scheme.
The effect of the collisions on the control of coherent population transfer in a closed inverse YYY-type four-level system driven by three laser fields is investigated with the stimulated Raman adiabatic passage technique. An arbitrary coherent superposition between the initial state and target state can be created either by varying the Rabi frequency of the control laser field or by tuning the one-photon detunings of the pump and Stokes laser fields. When the three laser fields with nearly equal peak Rabi frequencies are each tuned to resonance with the respective transitions, the low transfer efficiency due to the nonadiabatic coupling between two degenerate adiabatic states could be enhanced dramatically with the increase of the collision-induced coherence decay rates to the value nearly comparable to the Rabi frequency of the control field. The enhanced transfer efficiency results from the collision-controlled electromagnetically induced transparency in the $\ensuremath{\Lambda}$-type three-level subsystem and electromagnetically induced absorption in the ladder-type three-level subsystem of the four-level system.