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Third-Order Optical Susceptibilities of Molecular and Polymeric Materials. Symmetry, Frequency, and Chromophore Structure Dependence as Probed by π-Electron Theory

Published online by Cambridge University Press:  26 February 2011

D. Li
Affiliation:
Department of Chemistry and Materials Research Center Northwestern University, Evanston, IL 60208
T. J. Marks
Affiliation:
Department of Chemistry and Materials Research Center Northwestern University, Evanston, IL 60208
M. A. Ratner
Affiliation:
Department of Chemistry and Materials Research Center Northwestern University, Evanston, IL 60208
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Abstract

Third-order optical susceptibilities (γijkl) can be efficiently analyzed for a variety of molecular structures employing perturbation theory and a PPP-SCF-SECI-DECI π-electron model Hamiltonian. The key, frequency tripling second hyperpolarizability γijkl(−3ω;ω,ω,ω) is calculated with full single and double CI. It is found that double excitations play a major role in third-order processes, and that γijkl, like the polarizability αij, is sensitive largely to the overall size (volume) of the π system, although charge transfer excitations may also contribute. The frequency dependence of v and correlations between γijkl and conjugation length are found for a series of trans polyenes.

Type
Research Article
Copyright
Copyright © Materials Research Society 1989

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Third-Order Optical Susceptibilities of Molecular and Polymeric Materials. Symmetry, Frequency, and Chromophore Structure Dependence as Probed by π-Electron Theory
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