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Title: Orientations of nonlocal vibrational modes from combined experimental and theoretical sum frequency spectroscopy

Abstract

Inferring molecular orientations from vibrational sum frequency generation (SFG) spectra is challenging in polarization combinations that result in low signal intensities, or when the local point group symmetry approximation fails. While combining experiments with density functional theory (DFT) could overcome this problem, the scope of the combined method has yet to be established. Here, we assess its feasibility of determining the distributions of molecular orientations for one monobasic ester, two epoxides and three alcohols at the vapor/fused silica interface. We find that molecular orientations of nonlocal vibrational modes cannot be determined using polarization-resolved SFG measurements alone.

Authors:
; ORCiD logo; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1378004
Report Number(s):
PNNL-SA-122921
Journal ID: ISSN 0009-2614; 49672; 49291; KP1704020
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Chemical Physics Letters; Journal Volume: 683; Journal Issue: C
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Environmental Molecular Sciences Laboratory

Citation Formats

Chase, Hilary M., Chen, Shunli, Fu, Li, Upshur, Mary Alice, Rudshteyn, Benjamin, Thomson, Regan J., Wang, Hong-Fei, Batista, Victor S., and Geiger, Franz M. Orientations of nonlocal vibrational modes from combined experimental and theoretical sum frequency spectroscopy. United States: N. p., 2017. Web. doi:10.1016/j.cplett.2017.01.015.
Chase, Hilary M., Chen, Shunli, Fu, Li, Upshur, Mary Alice, Rudshteyn, Benjamin, Thomson, Regan J., Wang, Hong-Fei, Batista, Victor S., & Geiger, Franz M. Orientations of nonlocal vibrational modes from combined experimental and theoretical sum frequency spectroscopy. United States. doi:10.1016/j.cplett.2017.01.015.
Chase, Hilary M., Chen, Shunli, Fu, Li, Upshur, Mary Alice, Rudshteyn, Benjamin, Thomson, Regan J., Wang, Hong-Fei, Batista, Victor S., and Geiger, Franz M. Fri . "Orientations of nonlocal vibrational modes from combined experimental and theoretical sum frequency spectroscopy". United States. doi:10.1016/j.cplett.2017.01.015.
@article{osti_1378004,
title = {Orientations of nonlocal vibrational modes from combined experimental and theoretical sum frequency spectroscopy},
author = {Chase, Hilary M. and Chen, Shunli and Fu, Li and Upshur, Mary Alice and Rudshteyn, Benjamin and Thomson, Regan J. and Wang, Hong-Fei and Batista, Victor S. and Geiger, Franz M.},
abstractNote = {Inferring molecular orientations from vibrational sum frequency generation (SFG) spectra is challenging in polarization combinations that result in low signal intensities, or when the local point group symmetry approximation fails. While combining experiments with density functional theory (DFT) could overcome this problem, the scope of the combined method has yet to be established. Here, we assess its feasibility of determining the distributions of molecular orientations for one monobasic ester, two epoxides and three alcohols at the vapor/fused silica interface. We find that molecular orientations of nonlocal vibrational modes cannot be determined using polarization-resolved SFG measurements alone.},
doi = {10.1016/j.cplett.2017.01.015},
journal = {Chemical Physics Letters},
number = C,
volume = 683,
place = {United States},
year = {Fri Sep 01 00:00:00 EDT 2017},
month = {Fri Sep 01 00:00:00 EDT 2017}
}