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Title: Surface sum-frequency vibrational spectroscopy of nonpolar media

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [1];  [2]
  1. Fudan Univ., Shanghai (China)
  2. Fudan Univ., Shanghai (China); Univ. of California, Berkeley, CA (United States)

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.

Research Organization:
Univ. of California, Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC03-76SF00098
OSTI ID:
1348219
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 112, Issue 19; ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 27 works
Citation information provided by
Web of Science

References (27)

The air–liquid interface of benzene, toluene, m-xylene, and mesitylene: a sum frequency, Raman, and infrared spectroscopic study journal January 2003
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
Surface contribution versus bulk contribution in surface nonlinear optical spectroscopy journal March 1999
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
Surface properties probed by second-harmonic and sum-frequency generation journal February 1989
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
Molecular Bonding and Interactions at Aqueous Surfaces as Probed by Vibrational Sum Frequency Spectroscopy journal August 2002
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

Cited By (4)

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