Nonlinear optical processes in conjugated polymers: configuration interaction description of linear polyenes and VEH/SOS evaluation of polyarylene vinylenes

Zhigang Shuai, D. Beljonne, Jean-Luc Bredas*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

4 Scopus citations

Abstract

We have used a Multi-Reference Determinant (MRD) Configuration Interaction (CI) approach, including double excitations within a Pariser-Parr-Pople Hamiltonian, to investigate linear polyenes containing from four to sixteen carbons. We have calculated the low-lying excited states, the two-photon absorption spectrum, and the Third Harmonic Generation response. We have analyzed the length dependence of the static third-order susceptibility, χ(3): an indication of saturation behavior has been found. Focusing our attention on the two-photon resonance peak present in the free-electron laser THG measurements on polyacetylene, we conclude that the experimental data can be explained within a strongly correlated electron model. The Valence Effective Hamiltonian (VEH) method has been extended to calculate nonlinear optical coefficients and has been applied to investigate the static and dynamic third-order polarizabilities in poly(p-phenylene vinylene) and poly(thienylene vinylene). The relation between aromaticity and hyperpolarizability is discussed.

Original languageEnglish (US)
Pages (from-to)123-133
Number of pages11
JournalSynthetic Metals
Volume51
Issue number1-3
DOIs
StatePublished - Sep 1 1992

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics
  • Mechanics of Materials
  • Mechanical Engineering
  • Metals and Alloys
  • Materials Chemistry

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