The ultrafast dynamics of liquid CBrCl3 studied with optical Kerr effect and Raman scattering

Author: Huang Tzer-Hsiang   Hsu Chia-Chen   Wei Tai-Huei   Chen Michael Jiunn   Tse Wan-Sun   Chiang Hai-Pang   Kuo Chie-Tong   Chang Springfield   Gu Xi-Jia  

Publisher: Taylor & Francis Ltd

ISSN: 1362-3028

Source: Molecular Physics, Vol.96, Iss.3, 1999-02, pp. : 389-396

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Abstract

The ultrafast inter- and intramolecular dynamics of liquid CBrCl are studied with a femtosecond laser in a pump/probe optical Kerr experiment. The prompt part of the observed Kerr signal is found to comprise not just electronic response but also coherent coupling. As reported in the literature, the weak and delayed part of the signal is attributed to three kinds of intermolecular dynamics: diffusive reorientation, polarizability distortion, and molecular libration with decay times, respectively, of 2ps, 500fs, and 190fs. Included in the delayed Kerr signal are long lasting oscillations which are ascribed to quantum interference involving four normal vibrations of the molecule. By a careful fitting of both the time domain (Kerr) and frequency domain (Raman) data with existing theories the four vibrations are identified as upsilon2 = 422cm-1, upsilon3 = 246cm-1, upsilon5 = 295cm-1, and upsilon6 = 191cm-1, with dephasing times, 1.1ps, 1.7ps, 1ps, and 1ps, respectively.