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Multidimensional Spectral Fingerprints of a New Family of Coherent Analytical Spectroscopies

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    Multidimensional Spectral Fingerprints of a New Family of Coherent Analytical Spectroscopies
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    Department of Chemistry, University of Wisconsin-Madison, Madison, Wisconsin 53706, United States
    *E-mail: [email protected]
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    Analytical Chemistry

    Cite this: Anal. Chem. 2017, 89, 24, 13182–13189
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    https://doi.org/10.1021/acs.analchem.7b02917
    Published November 14, 2017
    Copyright © 2017 American Chemical Society
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    Abstract

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    Triply resonant sum frequency (TRSF) and doubly vibrationally enhanced (DOVE) spectroscopies are examples of a recently developed family of coherent multidimensional spectroscopies (CMDS) that are analogous to multidimensional NMR and current analytical spectroscopies. CMDS methods are particularly promising for analytical applications because their inherent selectivity makes them applicable to complex samples. Like NMR, they are based on creating quantum mechanical superposition states that are fully coherent and lack intermediate quantum state populations that cause quenching or other relaxation effects. Instead of the nuclear spin states of NMR, their multidimensional spectral fingerprints result from creating quantum mechanical mixtures of vibrational and electronic states. Vibrational states provide spectral selectivity, and electronic states provide large signal enhancements. This paper presents the first electronically resonant DOVE spectra and demonstrates the capabilities for analytical chemistry applications by comparing electronically resonant TRSF and DOVE spectra with each other and with infrared absorption and resonance Raman spectra using a Styryl 9 M dye as a model system. The methods each use two infrared absorption transitions and a resonant Raman transition to create a coherent output beam, but they differ in how they access the vibrational and electronic states and the frequency of their output signal. Just as FTIR, UV–vis, Raman, and resonance Raman are complementary methods, TRSF and DOVE methods are complementary to coherent Raman methods such as coherent anti-Stokes Raman spectroscopy (CARS).

    Copyright © 2017 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.analchem.7b02917.

    • Details on the experimental methods and their corrections for beam pointing and position, temporal and spatial overlap, and phase matching changes during spectral scanning of the excitation frequencies (PDF)

    • Software requirements, recommendations, and instructions for use (PDF)

    • Original data for the FTIR, Raman, and TRSF 2D spectra as well as the Python code used to graph the spectra (ZIP)

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    This article is cited by 8 publications.

    1. Maxim F. Gelin, Lipeng Chen, Wolfgang Domcke. Equation-of-Motion Methods for the Calculation of Femtosecond Time-Resolved 4-Wave-Mixing and N-Wave-Mixing Signals. Chemical Reviews 2022, 122 (24) , 17339-17396. https://doi.org/10.1021/acs.chemrev.2c00329
    2. John C. Wright. Schrödinger Cat State Spectroscopy—A New Frontier for Analytical Chemistry. Analytical Chemistry 2020, 92 (13) , 8638-8643. https://doi.org/10.1021/acs.analchem.0c01662
    3. Jonathan D. Handali, Kyle F. Sunden, Blaise J. Thompson, Nathan A. Neff-Mallon, Emily M. Kaufman, Thomas C. Brunold, John C. Wright. Three Dimensional Triply Resonant Sum Frequency Spectroscopy Revealing Vibronic Coupling in Cobalamins: Toward a Probe of Reaction Coordinates. The Journal of Physical Chemistry A 2018, 122 (46) , 9031-9042. https://doi.org/10.1021/acs.jpca.8b07678
    4. Thresa A. Wells, Victoria J. Barber, Muhire H. Kwizera, Patience Mukashyaka, Peter C. Chen. Nonparametric High-Resolution Coherent 3D Spectroscopy as a Simple and Rapid Method for Obtaining Excited-State Rotational Constants. The Journal of Physical Chemistry A 2018, 122 (44) , 8794-8801. https://doi.org/10.1021/acs.jpca.8b08640
    5. Darien J. Morrow, Daniel D. Kohler, Yuzhou Zhao, Song Jin, John C. Wright. Triple sum frequency pump-probe spectroscopy of transition metal dichalcogenides. Physical Review B 2019, 100 (23) https://doi.org/10.1103/PhysRevB.100.235303
    6. Blaise Thompson, Kyle Sunden, Darien Morrow, Daniel Kohler, John Wright. WrightTools: a Python package for multidimensional spectroscopy. Journal of Open Source Software 2019, 4 (33) , 1141. https://doi.org/10.21105/joss.01141
    7. Darien J. Morrow, Daniel D. Kohler, Kyle J. Czech, John C. Wright. Communication: Multidimensional triple sum-frequency spectroscopy of MoS2 and comparisons with absorption and second harmonic generation spectroscopies. The Journal of Chemical Physics 2018, 149 (9) https://doi.org/10.1063/1.5047802
    8. Jonathan D. Handali, Kyle F. Sunden, Emily M. Kaufman, John C. Wright. Interference and phase mismatch effects in coherent triple sum frequency spectroscopy. Chemical Physics 2018, 512 , 13-19. https://doi.org/10.1016/j.chemphys.2018.05.023
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    Analytical Chemistry

    Cite this: Anal. Chem. 2017, 89, 24, 13182–13189
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.analchem.7b02917
    Published November 14, 2017
    Copyright © 2017 American Chemical Society
    Request reuse permissions

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