Flexible approach to vibrational sum-frequency generation using shaped near-infrared light

Azhad U. Chowdhury; Fangjie Liu; Brianna R. Watson; Rana Ashkar; John Katsaras; C. Patrick Collier; Daniel A. Lutterman; Ying Zhong Ma; Tessa R. Calhoun; Benjamin Doughty

doi:10.1364/OL.43.002038

Flexible approach to vibrational sum-frequency generation using shaped near-infrared light

Azhad U. Chowdhury, Fangjie Liu, Brianna R. Watson, Rana Ashkar, John Katsaras, C. Patrick Collier, Daniel A. Lutterman, Ying Zhong Ma, Tessa R. Calhoun, Benjamin Doughty

Research output: Contribution to journal › Article › peer-review

35 Scopus citations

Abstract

We describe a new approach that expands the utility of vibrational sum-frequency generation (vSFG) spectroscopy using shaped near-infrared (NIR) laser pulses. We demonstrate that arbitrary pulse shapes can be specified to match experimental requirements without the need for changes to the optical alignment. In this way, narrowband NIR pulses as long as 5.75 ps are readily generated, with a spectral resolution of about 2.5 cm⁻¹, an improvement of approximately a factor of 3 compared to a typical vSFG system. Moreover, the utility of having complete control over the NIR pulse characteristics is demonstrated through nonresonant background suppression from a metallic substrate by generating an etalon waveform in the pulse shaper. The flexibility afforded by switching between arbitrary NIR waveforms at the sample position with the same instrument geometry expands the type of samples that can be studied without extensive modifications to existing apparatuses or large investments in specialty optics.

Original language	English
Pages (from-to)	2038-2041
Number of pages	4
Journal	Optics Letters
Volume	43
Issue number	9
DOIs	https://doi.org/10.1364/OL.43.002038
State	Published - May 1 2018

Funding

National Institute of General Medical Sciences (NIGMS) (NIGMS R15 GM119111); U.S. Department of Energy (DOE) (DE-AC05 00OR2275); Oak Ridge National Laboratory (ORNL). A. Chowdhury, F. Liu, R. Ashkar, J. Katsaras, C. Collier, D. Lutterman, Y.-Z. Ma, and B. Doughty were sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. T. Calhoun and B. Watson’s research was supported by the University of Tennessee, Knoxville, and the National Institutes of Health (NIH, NIGMS R15 GM119111). J. Katsaras is also supported through the Scientific User Facilities Division of the U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), under contract no. DE-AC05 00OR2275. Acknowledgment. A. Chowdhury, F. Liu, R. Ashkar, J. Katsaras, C. Collier, D. Lutterman, Y.-Z. Ma, and B. Doughty were sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. T. Calhoun and B. Watson’s research was supported by the University of Tennessee, Knoxville, and the National Institutes of Health (NIH, NIGMS R15 GM119111). J. Katsaras is also supported through the Scientific User Facilities Division of the U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES), under contract no. DE-AC05 00OR2275.

Funders	Funder number
Office of Basic Energy Sciences
National Institutes of Health
U.S. Department of Energy	DE-AC05 00OR2275
National Institute of General Medical Sciences	R15GM119111
Basic Energy Sciences
Oak Ridge National Laboratory
University of Tennessee

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title = "Flexible approach to vibrational sum-frequency generation using shaped near-infrared light",

abstract = "We describe a new approach that expands the utility of vibrational sum-frequency generation (vSFG) spectroscopy using shaped near-infrared (NIR) laser pulses. We demonstrate that arbitrary pulse shapes can be specified to match experimental requirements without the need for changes to the optical alignment. In this way, narrowband NIR pulses as long as 5.75 ps are readily generated, with a spectral resolution of about 2.5 cm−1, an improvement of approximately a factor of 3 compared to a typical vSFG system. Moreover, the utility of having complete control over the NIR pulse characteristics is demonstrated through nonresonant background suppression from a metallic substrate by generating an etalon waveform in the pulse shaper. The flexibility afforded by switching between arbitrary NIR waveforms at the sample position with the same instrument geometry expands the type of samples that can be studied without extensive modifications to existing apparatuses or large investments in specialty optics.",

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AU - Chowdhury, Azhad U.

AU - Liu, Fangjie

AU - Watson, Brianna R.

AU - Ashkar, Rana

AU - Katsaras, John

AU - Patrick Collier, C.

AU - Lutterman, Daniel A.

AU - Ma, Ying Zhong

AU - Calhoun, Tessa R.

AU - Doughty, Benjamin

PY - 2018/5/1

Y1 - 2018/5/1

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AB - We describe a new approach that expands the utility of vibrational sum-frequency generation (vSFG) spectroscopy using shaped near-infrared (NIR) laser pulses. We demonstrate that arbitrary pulse shapes can be specified to match experimental requirements without the need for changes to the optical alignment. In this way, narrowband NIR pulses as long as 5.75 ps are readily generated, with a spectral resolution of about 2.5 cm−1, an improvement of approximately a factor of 3 compared to a typical vSFG system. Moreover, the utility of having complete control over the NIR pulse characteristics is demonstrated through nonresonant background suppression from a metallic substrate by generating an etalon waveform in the pulse shaper. The flexibility afforded by switching between arbitrary NIR waveforms at the sample position with the same instrument geometry expands the type of samples that can be studied without extensive modifications to existing apparatuses or large investments in specialty optics.

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Flexible approach to vibrational sum-frequency generation using shaped near-infrared light

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