Structure-property relationships for three-photon absorption in stilbene-based dipolar and quadrupolar chromophores

Lingyun Zhu*, Yuanping Yi, Zhigang Shuai, Jean Luc Brédas, David Beljonne, Egbert Zojer

*Corresponding author for this work

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19 Scopus citations

Abstract

Based on essential-state models for three-photon absorption (3PA), we have investigated the structure-property relationships for stilbene-based dipolar and quadrupolar chromophores. The emphasis lies on the evolution of the 3PA cross section with the degree of ground-state polarization. For dipolar systems, we find a dominant role played by Δμ, which expresses the change in dipole moment between the ground state and the 3PA active excited state. Thus, the strategies usually applied to maximize the second-order polarizability β are also applicable to optimize the 3PA cross section. For quadrupolar systems, the 3PA response is dominated by contributions from channels including various low-lying two-photon allowed states, which limits the applicability of essential-state models. Optimization strategies can be proposed but vary for different ranges of ground-state polarization.

Original languageEnglish (US)
Article number044101
JournalJournal of Chemical Physics
Volume125
Issue number4
DOIs
StatePublished - 2006

ASJC Scopus subject areas

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

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