Published June 7, 2015 | Version v1
Journal article

Molecular dynamics study of two-dimensional sum frequency generation spectra at vapor/water interface

  • 1. Department of Applied Chemistry, Graduate School of Science and Engineering, University of Toyama, Toyama 930-8555 (Japan)
  • 2. Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan and Elements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto University, Kyoto 615-8520 (Japan)
  • 3. Molecular Spectroscopy Laboratory, RIKEN and Ultrafast Spectroscopy Research Team, RIKEN Center for Advanced Photonics (RAP), 2-1 Hirosawa, Wako 351-0198 (Japan)

Description

Two-dimensional heterodyne-detected vibrational sum frequency generation (2D HD-VSFG) spectra at vapor/water interface were studied by molecular dynamics (MD) simulation with a classical flexible and nonpolarizable model. The present model well describes the spectral diffusion of 2D infrared spectrum of bulk water as well as 2D HD-VSFG at the interface. The effect of isotopic dilution on the 2D HD-VSFG was elucidated by comparing the normal (H2O) water and HOD water. We further performed decomposition analysis of 2D HD-VSFG into the hydrogen-bonding and the dangling (or free) OH vibrations, and thereby disentangled the different spectral responses and spectral diffusion in the 2D HD-VSFG. The present MD simulation demonstrated the role of anharmonic coupling between these modes on the cross peak in the 2D HD-VSFG spectrum

Additional details

Identifiers

Publishing Information

Journal Title
Journal of Chemical Physics
Journal Volume
142
Journal Issue
21
Journal Page Range
p. 212407-212407.13
ISSN
0021-9606
CODEN
JCPSA6

Optional Information

Notes
(c) 2015 AIP Publishing LLC