Discriminating Congested Vibrational Peaks of Condensed Organic Materials with Time- and Frequency-Resolved Coherent Anti-Stokes Raman Scattering Spectroscopy

被引:6
作者
Choi, Dae Sik [1 ,2 ]
Rhee, Hanju [3 ]
Cho, Minhaeng [4 ,5 ]
机构
[1] Korea Inst Ind Technol KITECH, Technol Human Resource Support SMEs Ctr, Cheonan 31056, South Korea
[2] Uniotech, R&D Ctr, Daejeon 34013, South Korea
[3] Korea Basic Sci Inst, Seoul Ctr, Seoul 02841, South Korea
[4] Inst Basic Sci IBS, Ctr Mol Spect & Dynam, Seoul 02841, South Korea
[5] Korea Univ, Dept Chem, Seoul 02841, South Korea
关键词
POLARIZATION-SENSITIVE CARS; FS-CARS; MICROSCOPY; GENERATION; BAND; SUPPRESSION; MOLECULES; DYNAMICS; STATE;
D O I
10.1021/acs.jpcb.3c00926
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:3958 / 3968
页数:11
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