We report a theoretical framework for the study of the optimal control of multisurface molecular systems via a set of nondegenerate excitation fields. The resulting control equations in the strong response regime are presented in terms of both the Liouville-space density matrix dynamics and the Hilbert-space wave function evolution. We further derive a pair of eigenequations for the optimal pump-pump fields in the pure-state control of three-surface molecular systems in the weak response regime. The globally optimal pair of pump-pump fields in this case are identified. Application to the control of a rovibronic level on the final excited surface reveals a symmetry relation within the optimal pair of pump-pump fields in the weak response regime. For numerical demonstrations, we consider the control of the molecular system involving the initial ground the intermediate and the final surface. The target is chosen as an outgoing vibrational wave packet in the bound region of the final electronic state. The optimal control fields in both the strong and weak response regimes are calculated and further parameterized to fit simple experimentally realizable laser pulses.
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1 August 1998
Research Article|
August 01 1998
Optimal control of multisurface molecular systems Available to Purchase
Jixin Cheng;
Jixin Cheng
Department of Chemistry, Hong Kong University of Science and Technology, Kowloon, Hong Kong
Open Laboratory of Bond-Selective Chemistry, University of Science and Technology of China, Hefei, China
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Zhenwen Shen;
Zhenwen Shen
Department of Chemistry, Hong Kong University of Science and Technology, Kowloon, Hong Kong
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YiJing Yan
YiJing Yan
Department of Chemistry, Hong Kong University of Science and Technology, Kowloon, Hong Kong
Open Laboratory of Bond-Selective Chemistry, University of Science and Technology of China, Hefei, China
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Jixin Cheng
Department of Chemistry, Hong Kong University of Science and Technology, Kowloon, Hong Kong
Open Laboratory of Bond-Selective Chemistry, University of Science and Technology of China, Hefei, China
Zhenwen Shen
Department of Chemistry, Hong Kong University of Science and Technology, Kowloon, Hong Kong
YiJing Yan
Department of Chemistry, Hong Kong University of Science and Technology, Kowloon, Hong Kong
Open Laboratory of Bond-Selective Chemistry, University of Science and Technology of China, Hefei, China
J. Chem. Phys. 109, 1654–1662 (1998)
Article history
Received:
April 07 1998
Accepted:
April 22 1998
Citation
Jixin Cheng, Zhenwen Shen, YiJing Yan; Optimal control of multisurface molecular systems. J. Chem. Phys. 1 August 1998; 109 (5): 1654–1662. https://doi.org/10.1063/1.476740
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