Nonlinear optical response in acceptor-substituted carotenoids: a theoretical study

M. Yu Balakina*, J. Li, V. M. Geskin, S. R. Marder, Jean-Luc Bredas

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

31 Scopus citations

Abstract

Presented is a theoretical study of the structure and molecular polarizabilities for a set of carotenoid-like molecules. The degree of ground-state polarization is varied by application of an external homogeneous electric field along the long axis of the chromophore. The dipole moment of the apocarotenal molecules evolves stepwise with field, which results in very large values of the first- (α), second- (β), and third-order (γ) molecular polarizabilities. The latter have been evaluated through the sum-over-states expression at the correlated level; simplified three-state and four-term models for β and γ, respectively, have been analyzed in detail. The evolution of the dipole moment μ (and thus the molecular polarizabilities α, α, and γ) can be described adequately as a function of the bond-order alternation structural parameter; the derivative relations among μ, α, α, and γ as a function of bond-order alternation are shown to hold.

Original languageEnglish (US)
Pages (from-to)9598-9609
Number of pages12
JournalJournal of Chemical Physics
Volume113
Issue number21
DOIs
StatePublished - Dec 1 2000

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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