Phase-Sensitive Sum-Frequency Generation Measurements Using a Femtosecond Nonlinear Interferometer

Max Planck Institute for Polymer Research, Ackermannweg 10, 55128 Mainz, Germany
Laboratory for Water and Surface Studies, Chemistry Department, Tufts University, Medford, Massachusetts 02155, United States
§ Department of Physical Chemistry, University of Vienna, Währinger Str. 42, 1090 Wien, Austria
J. Phys. Chem. C, 2019, 123 (12), pp 7266–7270
DOI: 10.1021/acs.jpcc.9b00861
Publication Date (Web): March 6, 2019
Copyright © 2019 American Chemical Society
ACS AuthorChoice - This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.


Abstract Image

Phase-sensitive sum-frequency spectroscopy is a unique tool to interrogate the vibrational structure of interfaces. A precise understanding of the interfacial structure often relies on accurately determining the phase of χ(2), which has recently been demonstrated using a nonlinear interferometer in conjunction with a frequency-scanning picosecond laser system. Here, we implement nonlinear interferometry using a femtosecond laser system for broadband sum-frequency generation. The phase of the vibrational response from a self-assembled monolayer of octadecanethiol on gold is determined using the nonlinear femtosecond interferometer. The results are compared to those obtained using the more traditional heterodyne-detected phase measurements. Both methods give a similar phase spectrum and phase uncertainty. We also discuss the origin of the phase uncertainties and provide guidelines for further improvement.

The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.jpcc.9b00861.

  • Derivation of the phase change due to height change for heterodyne measurement and nonlinear interferometer (PDF)

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Article Views: 244 Times
Received 30 January 2019
Published online 6 March 2019
Published in print 28 March 2019
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