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Simultaneous measurements of global vibrational spectra and dephasing times of molecular vibrational modes by broadband time-resolved coherent anti-Stokes Raman scattering spectrography
Authors:Yin Jun  Yu Ling-Yao  Liu Xing  Wan Hui  Lin Zi-Yang and Niu Han-Ben
Affiliation:Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province, Institute of Optoelectronics, Shenzhen University, Shenzhen 518060, China
Abstract:In broadband coherent anti-Stokes Raman scattering (CARS) spectroscopy with supercontinuum (SC), the simultaneously detectable spectral coverage is limited by the spectral continuity and the simultaneity of various spectral components of SC in an enough bandwidth. By numerical simulations, the optimal experimental conditions for improving the SC are obtained. The broadband time-resolved CARS spectrography based on the SC with required temporal and spectral distributions is realised. The global molecular vibrational spectrum with well suppressed nonresonant background noise can be obtained in a single measurement. At the same time, the measurements of dephasing times of various molecular vibrational modes can be conveniently achieved from intensities of a sequence of time-resolved CARS signals. It will be more helpful to provide a complete picture of molecular vibrations, and to exhibit a potential to understand not only both the solvent dynamics and the solute-solvent interactions, but also the mechanisms of chemical reactions in the fields of biology, chemistry and material science.
Keywords:coherent anti-Stokes Raman scattering  photonic crystal fibre  supercontinuum  molecular vibrational spectrum  dephasing time  time-resolved measurement
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