General model for the description of the third-order optical nonlinearitiesin conjugated systems: Application to the all-trans Β-carotene molecule

D. Beljonne, J. Cornil, Z. Shuai, J. Brédas, F. Rohlfing, D. Bradley

Research output: Contribution to journalArticlepeer-review

67 Scopus citations

Abstract

On the basis of an extended configuration-interaction description of the lowest singlet excited states, we investigate the third-order nonlinear optical response of the Β-carotene molecule by means of the sum-over-states approach. We first uncover the nature of the electronic states contributing primarily to the cubic molecular polarizabilities. From this starting point, we apply a simplified model to evaluate the frequency-dependent third-harmonic generation (THG) and electroabsorption (EA) spectra; the vibronic structure of the spectra is described by taking into account Franck-Condon factors calculated in a displaced oscillator model. For both the THG and EA processes, we obtain good agreement between the theoretical simulations and the experimental data, which underlines the general character of our model.

Original languageEnglish (US)
Pages (from-to)1505-1516
Number of pages12
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume55
Issue number3
DOIs
StatePublished - Jan 1 1997
Externally publishedYes

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

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