Quantum-chemical investigation of second-order nonlinear optical chromophores: Comparison of strong nitrile-based acceptor end groups and role of auxiliary donors and acceptors

A. Leclercq, E. Zojer, S. H. Jang, S. Barlow, V. Geskin, A. K.Y. Jen, S. R. Marder, J. L. Bŕdas

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33 Scopus citations

Abstract

We report a detailed quantum-chemical investigation of donor-acceptor substituted dipolar nonlinear optical chromophores incorporating the 4-(dimethylamino)phenyl donor end group and a variety of strong heterocyclic acceptor end groups, including tricyanofurans and tricyanopyrroles. In particular, we study the variation of the molecular second-order polarizability (Β) with the acceptor end group and when inserting auxiliary donors (thiophene) and acceptors (thiazole) into the π bridge. Both finite-field calculations (in the context of local contributions) and sum-over-states calculations were carried out in order to probe the relationship between Β and the chemical structure of the various chromophores. The trends obtained with these two methods are fully consistent. The large Β values (up to 700× 10-30 esu) as well as the observed tunability of the optical absorption maximum (λmax) make the chromophores investigated here interesting candidates for use in electro-optic applications at telecommunications wavelengths.

Original languageEnglish (US)
Article number044510
JournalJournal of Chemical Physics
Volume124
Issue number4
DOIs
StatePublished - 2006
Externally publishedYes

ASJC Scopus subject areas

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

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