Optimal control approach to suppression of radiationless transitions

Maxim Sukharev; Tamar Seideman

doi:10.1103/PhysRevLett.93.093004

Optimal control approach to suppression of radiationless transitions

Maxim Sukharev^*, Tamar Seideman

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

44 Scopus citations

Abstract

A general approach for eliminating radiationless transitions (RT) in polyatomic molecules is proposed. The approach is a combination of optimal control theory and electronically localized eigenstates of strongly vibronically coupled systems, to populate a superposition state that is immune to nonradiative decay. It is found that in the spectra of systems undergoing RT, the transition of the spectrum from regular to irregular at the interaction energy is a general phenomenon. The results show that most eigenstates are of strongly mixed character, above the intersection energy, but eigenstates of essentially pure character are found at all energies above E_c.

Original language	English (US)
Article number	093004
Pages (from-to)	093004-1-093004-4
Journal	Physical review letters
Volume	93
Issue number	9
DOIs	https://doi.org/10.1103/PhysRevLett.93.093004
State	Published - Aug 27 2004

Funding

We gratefully acknowledge the National Energy Research Scientific Computing Center, supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC03-76SF00098, for computational resources.

ASJC Scopus subject areas

General Physics and Astronomy

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10.1103/PhysRevLett.93.093004

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AU - Seideman, Tamar

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N2 - A general approach for eliminating radiationless transitions (RT) in polyatomic molecules is proposed. The approach is a combination of optimal control theory and electronically localized eigenstates of strongly vibronically coupled systems, to populate a superposition state that is immune to nonradiative decay. It is found that in the spectra of systems undergoing RT, the transition of the spectrum from regular to irregular at the interaction energy is a general phenomenon. The results show that most eigenstates are of strongly mixed character, above the intersection energy, but eigenstates of essentially pure character are found at all energies above Ec.

AB - A general approach for eliminating radiationless transitions (RT) in polyatomic molecules is proposed. The approach is a combination of optimal control theory and electronically localized eigenstates of strongly vibronically coupled systems, to populate a superposition state that is immune to nonradiative decay. It is found that in the spectra of systems undergoing RT, the transition of the spectrum from regular to irregular at the interaction energy is a general phenomenon. The results show that most eigenstates are of strongly mixed character, above the intersection energy, but eigenstates of essentially pure character are found at all energies above Ec.

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Optimal control approach to suppression of radiationless transitions

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