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Title: A new approach to vibrational sum frequency generation spectroscopy using near infrared pulse shaping

Abstract

In this work, we have developed a multipurpose vibrational sum frequency generation (vSFG) spectrometer that is uniquely capable of probing a broad range of chemical species, each requiring different experimental conditions, without optical realignment. Here, we take advantage of arbitrary near infrared (NIR) waveform generation using a 4f-pulse shaper equipped with a 2D spatial light modulator (SLM) to tailor upconversion pulses to meet sample dependent experimental requirements. This report details the experimental layout, details of the SLM calibration and implementation, and the intrinsic benefits/limitations of this new approach to vSFG spectroscopy. We have demonstrated the competency of this spectrometer by achieving an ~3-fold increase in spectral resolution compared to conventional spectrometers by probing the model dimethyl sulfoxide/air interface. We also show the ability to suppress nonresonant background contributions from electrode interfaces using time delayed asymmetric waveforms that are generated by the NIR pulse shaper. Lastly, it is expected that this advancement in instrumentation will broaden the types of samples researchers can readily study using nonlinear surface specific spectroscopies.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [3]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Knoxville Catholic High School, Knoxville, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1502551
Alternate Identifier(s):
OSTI ID: 1501957
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Review of Scientific Instruments
Additional Journal Information:
Journal Volume: 90; Journal Issue: 3; Journal ID: ISSN 0034-6748
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 47 OTHER INSTRUMENTATION

Citation Formats

Chowdhury, Azhad U., Watson, Brianna R., Ma, Ying-Zhong, Sacci, Robert L., Lutterman, Daniel A., Calhoun, Tessa R., and Doughty, Benjamin. A new approach to vibrational sum frequency generation spectroscopy using near infrared pulse shaping. United States: N. p., 2019. Web. doi:10.1063/1.5084971.
Chowdhury, Azhad U., Watson, Brianna R., Ma, Ying-Zhong, Sacci, Robert L., Lutterman, Daniel A., Calhoun, Tessa R., & Doughty, Benjamin. A new approach to vibrational sum frequency generation spectroscopy using near infrared pulse shaping. United States. doi:10.1063/1.5084971.
Chowdhury, Azhad U., Watson, Brianna R., Ma, Ying-Zhong, Sacci, Robert L., Lutterman, Daniel A., Calhoun, Tessa R., and Doughty, Benjamin. Fri . "A new approach to vibrational sum frequency generation spectroscopy using near infrared pulse shaping". United States. doi:10.1063/1.5084971. https://www.osti.gov/servlets/purl/1502551.
@article{osti_1502551,
title = {A new approach to vibrational sum frequency generation spectroscopy using near infrared pulse shaping},
author = {Chowdhury, Azhad U. and Watson, Brianna R. and Ma, Ying-Zhong and Sacci, Robert L. and Lutterman, Daniel A. and Calhoun, Tessa R. and Doughty, Benjamin},
abstractNote = {In this work, we have developed a multipurpose vibrational sum frequency generation (vSFG) spectrometer that is uniquely capable of probing a broad range of chemical species, each requiring different experimental conditions, without optical realignment. Here, we take advantage of arbitrary near infrared (NIR) waveform generation using a 4f-pulse shaper equipped with a 2D spatial light modulator (SLM) to tailor upconversion pulses to meet sample dependent experimental requirements. This report details the experimental layout, details of the SLM calibration and implementation, and the intrinsic benefits/limitations of this new approach to vSFG spectroscopy. We have demonstrated the competency of this spectrometer by achieving an ~3-fold increase in spectral resolution compared to conventional spectrometers by probing the model dimethyl sulfoxide/air interface. We also show the ability to suppress nonresonant background contributions from electrode interfaces using time delayed asymmetric waveforms that are generated by the NIR pulse shaper. Lastly, it is expected that this advancement in instrumentation will broaden the types of samples researchers can readily study using nonlinear surface specific spectroscopies.},
doi = {10.1063/1.5084971},
journal = {Review of Scientific Instruments},
number = 3,
volume = 90,
place = {United States},
year = {2019},
month = {3}
}

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