Mechanisms of sum frequency generation from liquid benzene: Symmetry breaking at interface and bulk contribution

Tatsuya Kawaguchi, Kazuya Shiratori, Yuki Henmi, Tatsuya Ishiyama, Akihiro Morita

Research output: Contribution to journalArticlepeer-review

32 Citations (Scopus)

Abstract

Liquid benzene emits a significant sum frequency generation (SFG) signal of C-H stretching vibration, though it is composed of centrosymmetric molecules. The present paper theoretically elucidates the SFG spectrum from liquid benzene by considering two mechanisms, symmetry breaking at the interface and bulk contribution. Molecular dynamics and quantum chemical calculations reproduced the observed SFG spectrum and revealed that the two mechanisms are equally significant in the SFG spectrum of liquid benzene. At the interface, the SFG signal arises from local C-H stretching modes via the mixing of IR active and Raman active modes. The local modes are readily induced by the anisotropic environment at the interface. The observed SFG signal should also involve significant amount of quadrupole contribution, which is attributed to the IR active mode of the bulk liquid.

Original languageEnglish
Pages (from-to)13169-13182
Number of pages14
JournalJournal of Physical Chemistry C
Volume116
Issue number24
DOIs
Publication statusPublished - 2012 Jun 21

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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