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


ABSTRACT: 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 ?(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.

SUBMITTER: Sun S 

PROVIDER: S-EPMC6443213 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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

Sun Shumei S   Bisson Patrick J PJ   Bonn Mischa M   Shultz Mary Jane MJ   Backus Ellen H G EHG  

The journal of physical chemistry. C, Nanomaterials and interfaces 20190306 12


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<sup>(2)</sup>, 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  ...[more]

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