Bend Vibration of Surface Water Investigated by Heterodyne-Detected Sum Frequency Generation and Theoretical Study: Dominant Role of Quadrupole

Achintya Kundu, Shogo Tanaka, Tatsuya Ishiyama, Mohammed Ahmed, Ken Ichi Inoue, Satoshi Nihonyanagi, Hiromi Sawai, Shoichi Yamaguchi, Akihiro Morita, Tahei Tahara

Research output: Contribution to journalArticlepeer-review

35 Citations (Scopus)

Abstract

Heterodyne-detected vibrational sum frequency generation spectroscopy was applied to the water surface for measuring the imaginary part of second-order nonlinear susceptibility (Im χ(2)) spectrum in the bend frequency region for the first time. The observed Im χ(2) spectrum shows an overall positive band around 1650 cm-1, contradicting former theoretical predictions. We further found that the Im χ(2) spectrum of NaI aqueous solution exhibits an even larger positive band, which is apparently contrary to the flip-flop orientation of surface water. These unexpected observations are elucidated by calculating quadrupole contributions beyond the conventional dipole approximation. It is indicated that the Im χ(2) spectrum in the bend region has a large quadrupole contribution from the bulk water.

Original languageEnglish
Pages (from-to)2597-2601
Number of pages5
JournalJournal of Physical Chemistry Letters
Volume7
Issue number13
DOIs
Publication statusPublished - 2016 Jul 7
Externally publishedYes

ASJC Scopus subject areas

  • Materials Science(all)
  • Physical and Theoretical Chemistry

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