Abstract
The ν1 (C–H) stretching mode of CHBr3 was investigated in the solvent CDBr3 at room temperature using three-colour femtosecond CARS and scanning multi-channel Raman difference spectroscopy (SMT-RDS). Small but measurable blue shifts (≤1 cm−1) of the isotropic part of the Raman scattering relative to the anisotropic component and upon isotopic dilution are the clear signatures of the Raman non-coincidence effect and isotopic lineshift, respectively. The experimental results are discussed in terms of theoretical models providing insight in the intermolecular coupling mechanisms. The measured shift ΔνID = 0.73 ± 0.02 cm−1 upon isotopic dilution is found to be dominated by the attractive interaction and is to be compared with the non-coincidence effect of ΔνNCE = 1.02 ± 0.05 cm−1 for the neat liquid. A 5% decrease in the dephasing rate 1/T2 and a similar change in the linewidth upon infinite dilution are observed and semi-quantitatively explained via repulsive intermolecular interaction in accordance with an estimate of the corresponding (small) wavenumber shift. Copyright © 2000 John Wiley & Sons, Ltd.
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