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A variational method for the calculation of dynamic polarizabilities and two-photon transition moments - The dressed molecule approachThe solution of the time-dependent Schroedinger equation of the molecule + radiation field system is analyzed. A quantized radiation field is used. The relationship between the oscillatory wave function and the dressed state wave function is established, the oscillatory wave function being the solution if the radiation field is turned on at t = 0 and the dressed state being the stationary solution satisfying the boundary condition only if the field is present at t = negative infinity. In general, the oscillatory wave function can be expressed using a complete set of dressed states. However, in the presence of a nonresonant radiation field, the system is well represented by a single dressed state. Molecular properties such as dynamic polarizabilities and two-photon transition moments can be deduced from the dressed state wave function instead of the oscillatory wave function as in previous methods. Because of its stationary character, the dressed state is more amenable to approximate calculations. A CI method is developed for this purpose. The CI matrix is simple in form and can be readily constructed using existing computer codes. The present method can also be adapted to calculate other optical properties.
Document ID
19850032102
Acquisition Source
Legacy CDMS
Document Type
Reprint (Version printed in journal)
External Source(s)
Authors
Huo, W. M.
(NASA Ames Research Center Moffett Field, CA; Notre Dame, University, Notre Dame, IN, United States)
Date Acquired
August 12, 2013
Publication Date
October 15, 1984
Publication Information
Publication: Journal of Chemical Physics
Volume: 81
ISSN: 0021-9606
Subject Category
Atomic And Molecular Physics
Accession Number
85A14253
Distribution Limits
Public
Copyright
Other

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