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Cho, Minhaeng
분자 분광학 및 동력학 연구단
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Discriminating Congested Vibrational Peaks of Condensed Organic Materials with Time- and Frequency-Resolved Coherent Anti-Stokes Raman Scattering Spectroscopy

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Title
Discriminating Congested Vibrational Peaks of Condensed Organic Materials with Time- and Frequency-Resolved Coherent Anti-Stokes Raman Scattering Spectroscopy
Author(s)
Choi, Dae Sik; Rhee, Hanju; Minhaeng Cho
Publication Date
2023-05
Journal
JOURNAL OF PHYSICAL CHEMISTRY B, v.127, no.17, pp.3958 - 3968
Publisher
AMER CHEMICAL SOC
Abstract
The spectral congestion of highly overlapping vibrational peaks of molecules in condensed phases is a persistent challenge in conventional linear vibrational spectroscopy, making it difficult to accurately determine the spectroscopic parameters. This study demonstrates the utility of time-and frequency-resolved coherent anti-Stokes Raman scattering (CARS) spectroscopy with a time-delayed picosecond probe pulse in resolving congested C-H stretching vibrational peaks of condensed organic matters. The results show that the overlapping vibrational peaks of polymeric films and oily liquids, which are not easily distinguishable in spontaneous Raman spectroscopy, can be separated in the time-resolved CARS (tr-CARS) spectra. To understand the physical basis of the enhanced spectral resolution, we examine the time series of CARS spectra obtained by varying the delay time between the pump and probe pulses. The global fit analysis indicates that the effective suppression of faster Raman free-induction-decay components and instantaneous nonresonant background signals contributes to improved spectral resolution. Additionally, the present study reveals that the CARS spectra at a sufficient probe delay time are highly sensitive to the incident and detection polarizations, further improving vibrational peak distinguishability through polarization-controlled tr-CARS.
URI
https://pr.ibs.re.kr/handle/8788114/13962
DOI
10.1021/acs.jpcb.3c00926
ISSN
1520-6106
Appears in Collections:
Center for Molecular Spectroscopy and Dynamics(분자 분광학 및 동력학 연구단) > 1. Journal Papers (저널논문)
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