Effects of third-order susceptibility in sum frequency generation spectra: A molecular dynamics study in liquid water

Tatsuya Joutsuka, Tomonori Hirano, Michiel Sprik, Akihiro Morita

Research output: Contribution to journalArticle

31 Citations (Scopus)

Abstract

When sum frequency generation (SFG) spectroscopy is applied to charged solid/liquid interfaces, the observed SFG signals include both the second-order and third-order polarizations. The latter is called the χ(3) effect, which mainly includes induced molecular orientation by electric fields at charged interfaces. We theoretically evaluate the χ(3) effect on the SFG spectroscopy of liquid water using molecular dynamics (MD) simulations. The MD simulations enable us to definitely calculate the χ(3) susceptibility as a bulk property, and thereby separating it from the usual χ(2) effect shown in the SFG spectra. The calculated results of χ(3) for liquid water are fairly consistent with the experimental estimates. The present finding is utilized to analyze the spectral change of SFG at the air/water interface under electric fields and at the charged silica/water interface. The present analysis of the spectral changes allows for distinguishing the intrinsic change of the interface structure and the χ(3) effect from bulk liquid.

Original languageEnglish
Pages (from-to)3040-3053
Number of pages14
JournalPhysical Chemistry Chemical Physics
Volume20
Issue number5
DOIs
Publication statusPublished - 2018 Feb 7

ASJC Scopus subject areas

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

Fingerprint Dive into the research topics of 'Effects of third-order susceptibility in sum frequency generation spectra: A molecular dynamics study in liquid water'. Together they form a unique fingerprint.

  • Cite this