skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Surface sum-frequency vibrational spectroscopy of nonpolar media

Abstract

Sum-frequency generation spectroscopy is surface specific only if the bulk contribution to the signal is negligible. Negligible bulk contribution is, however, not necessarily true, even for media with inversion symmetry. The inevitable challenge is to find the surface spectrum in the presence of bulk contribution, part of which has been believed to be inseparable from the surface contribution. Here, we show that, for nonpolar media, it is possible to separately deduce surface and bulk spectra from combined phase-sensitive sum-frequency vibrational spectroscopic measurements in reflection and transmission. Finally, the study of benzene interfaces is presented as an example.

Authors:
 [1];  [1];  [2]
  1. Fudan Univ., Shanghai (China)
  2. Fudan Univ., Shanghai (China); Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Univ. of California, Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1348219
Grant/Contract Number:  
AC03-76SF00098
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 112; Journal Issue: 19; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; nonpolar media; sum-frequency spectroscopy; surface structure; bulk contribution; electric-quadrupole contribution

Citation Formats

Sun, Shumei, Tian, Chuanshan, and Shen, Y. Ron. Surface sum-frequency vibrational spectroscopy of nonpolar media. United States: N. p., 2015. Web. doi:10.1073/pnas.1505438112.
Sun, Shumei, Tian, Chuanshan, & Shen, Y. Ron. Surface sum-frequency vibrational spectroscopy of nonpolar media. United States. https://doi.org/10.1073/pnas.1505438112
Sun, Shumei, Tian, Chuanshan, and Shen, Y. Ron. 2015. "Surface sum-frequency vibrational spectroscopy of nonpolar media". United States. https://doi.org/10.1073/pnas.1505438112. https://www.osti.gov/servlets/purl/1348219.
@article{osti_1348219,
title = {Surface sum-frequency vibrational spectroscopy of nonpolar media},
author = {Sun, Shumei and Tian, Chuanshan and Shen, Y. Ron},
abstractNote = {Sum-frequency generation spectroscopy is surface specific only if the bulk contribution to the signal is negligible. Negligible bulk contribution is, however, not necessarily true, even for media with inversion symmetry. The inevitable challenge is to find the surface spectrum in the presence of bulk contribution, part of which has been believed to be inseparable from the surface contribution. Here, we show that, for nonpolar media, it is possible to separately deduce surface and bulk spectra from combined phase-sensitive sum-frequency vibrational spectroscopic measurements in reflection and transmission. Finally, the study of benzene interfaces is presented as an example.},
doi = {10.1073/pnas.1505438112},
url = {https://www.osti.gov/biblio/1348219}, journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {0027-8424},
number = 19,
volume = 112,
place = {United States},
year = {Mon Apr 27 00:00:00 EDT 2015},
month = {Mon Apr 27 00:00:00 EDT 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 27 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Phase-Sensitive Sum-Frequency Spectroscopy
journal, April 2013


Ambiguities in surface nonlinear spectroscopy calculations
journal, November 2011


Fundamental difficulty in the use of second-harmonic generation as a strictly surface probe
journal, June 1987


Separation Problems in Optical Spectroscopies
journal, January 2004


Optical Second-Harmonic Generation in Reflection from Media with Inversion Symmetry
journal, October 1968


Optical Second Harmonic Generation at Interfaces
journal, October 1989


Optical Second-Harmonic Generation in Reflection from Media with Inversion Symmetry
journal, February 1969


Strong bulk magnetic dipole induced second-harmonic generation from C 60
journal, November 1993


Optical Second Harmonic Generation At Interfaces
journal, January 1989


Evaluation of Surface vs Bulk Contributions in Sum-Frequency Vibrational Spectroscopy Using Reflection and Transmission Geometries
journal, April 2000


Phase-Sensitive Sum-Frequency Vibrational Spectroscopy and Its Application to Studies of Interfacial Alkyl Chains
journal, August 2007


Mechanisms of Sum Frequency Generation from Liquid Benzene: Symmetry Breaking at Interface and Bulk Contribution
journal, June 2012


Nonlinear optical studies of the pure liquid/vapor interface: Vibrational spectra and polar ordering
journal, February 1991


Vibrational Sum Frequency Generation by the Quadrupolar Mechanism at the Nonpolar Benzene/Air Interface
journal, May 2013


Theory of Quadrupole Contributions from Interface and Bulk in Second-Order Optical Processes
journal, October 2012


Bulk versus surface contributions in nonlinear optics of isotropic centrosymmetric media
journal, December 2005


Electric quadrupole contribution to the nonresonant background of sum frequency generation at air/liquid interfaces
journal, May 2011


Bulk contribution from isotropic media in surface sum-frequency generation
journal, November 2002


Liquid Interfaces Probed by Second-Harmonic and Sum-Frequency Spectroscopy
journal, January 1996


Sum-frequency generation spectroscopy of interfaces
journal, March 2005


Surface nonlinear optics [Invited]
journal, January 2011


Nonlinear Optical Properties of Solids: Energy Considerations
journal, May 1963


Bulk contribution in surface second-harmonic generation
journal, October 1988


Works referencing / citing this record:

How surface-specific is 2nd-order non-linear spectroscopy?
journal, December 2019


Quadrupolar mechanism for vibrational sum frequency generation at air/liquid interfaces: Theory and experiment
journal, August 2019


Symmetry-breaking-induced nonlinear optics at a microcavity surface
journal, November 2018


Phase reference in phase-sensitive sum-frequency vibrational spectroscopy
journal, June 2016