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Coherent Nonlinear Spectroscopy with Multiple Mode-Locked Lasers

Cite this: J. Phys. Chem. Lett. 2021, 12, 42, 10284–10294
Publication Date (Web):October 15, 2021
https://doi.org/10.1021/acs.jpclett.1c01492
Copyright © 2021 American Chemical Society

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    Abstract

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    Coherent multidimensional spectroscopy has been widely used to study the structure and dynamics of chemical and biological systems. Each ultrashort pulse from a single mode-locked laser is split into multiple pulses by beam splitters. Their arrival times at a given molecular sample are controlled with mechanical time-delay generators for time-resolved measurements of molecular responses. Such nonlinear vibrational, electronic, or vibrational–electronic spectroscopy can now be carried out with multiple mode-locked lasers with highly stabilized repetition and sometimes carrier-envelope-offset frequencies. By precisely controlling the repetition frequencies of multiple mode-locked lasers, one can achieve automatic delay time scanning, known as asynchronous optical sampling, to investigate various relaxation processes associated with photochemical or photobiological phenomena at one sweep in time. In this Perspective, the current developments and applications of multiple mode-locked laser-based techniques to time-resolved nonlinear spectroscopy of chromophores in condensed phases are discussed. The author’s perspective on this approach is also presented.

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    Cited By

    This article is cited by 5 publications.

    1. Hyunmin Jang, Noh Soo Han, Gahyeon Kim, Kwang Seob Jeong, Tai Hyun Yoon, Minhaeng Cho. Unveiling Ultrafast Carrier Dynamics of Tellurium Microcrystals by Two-Color Asynchronous Sampling Infrared Transient Absorption Spectroscopy. The Journal of Physical Chemistry C 2024, 128 (1) , 268-278. https://doi.org/10.1021/acs.jpcc.3c06944
    2. Julian Lüttig, Stefan Mueller, Pavel Malý, Jacob J. Krich, Tobias Brixner. Higher-Order Multidimensional and Pump–Probe Spectroscopies. The Journal of Physical Chemistry Letters 2023, 14 (33) , 7556-7573. https://doi.org/10.1021/acs.jpclett.3c01694
    3. JunWoo Kim, Jonggu Jeon, Tai Hyun Yoon, Minhaeng Cho. Femtosecond multidimensional spectroscopy with multiple repetition-frequency-stabilized lasers: tutorial. Journal of the Optical Society of America B 2022, 39 (4) , 934. https://doi.org/10.1364/JOSAB.450875
    4. Noh Soo Han, JunWoo Kim, Tai Hyun Yoon, Minhaeng Cho. Time-resolved spectroscopy of thioflavin T solutions: Asynchronous optical sampling method with two frequency-upconverted mode-locked lasers. The Journal of Chemical Physics 2022, 156 (6) , 064201. https://doi.org/10.1063/5.0077756
    5. Vlastimil Fidler, Peter Kapusta. Fluorescence Kinetics and Time-Resolved Measurement. 2022https://doi.org/10.1007/4243_2022_31

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