Theoretical investigation of the origin of the large non-linear optical response in acceptor-substituted carotenoids

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

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

Correlated semiempirical quantum-chemical calculations are performed to rationalize the origin of the large first- (α), second- (β), and third- (γ) order molecular polarizabilities found in carotenoid-like molecules capped at a single end by an acceptor group. The ground state polarization in the apocarotenal H(-CH double bond CH-)10CH double bond C(CN)2, is made to vary via the application of an external homogeneous electric field. The important structural characteristics found for this long polymethine are (i) the relative instability of the cyanine-like (equal-bond length) structures and (ii) the double-step evolution of the dipole moment caused by the transfer of a first and then a second electron towards the acceptor end of the molecule as the electric field increases in the range 107-108 V/cm. The abruptness of these steps results in very large values of the molecular polarizabilities. The longitudinal components of the molecular polarizabilities are analyzed as a function of the bond-order alternation (BOA) parameter.

Original languageEnglish (US)
Pages (from-to)263-267
Number of pages5
JournalSynthetic Metals
Volume116
Issue number1-3
DOIs
StatePublished - Jan 1 2001

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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