The polarization dependence of vibrational coupling signals seen in femtosecond stimulated Raman spectroscopy (FSRS) is investigated. Changing the polarization of a pulse used to impulsively excite coherent low frequency chlorine bending motion in CDCl3 has a dramatic effect on the line shape of vibrational sidebands which arise from the anharmonic coupling of the pumped modes at 262 and 365 cm(-1) with the higher frequency symmetric stretching mode at 652 cm(-1). The asymmetric bend sideband (652+262 cm(-1)) changes sign and magnitude as the impulsive pulse polarization is rotated relative to the Raman pulses, while the symmetric bend sideband (652+365 cm(-1)) is relatively polarization independent. These experiments demonstrate the ability of FSRS to obtain time-resolved information on not only the vibrational coupling strength but also the symmetry of anharmonically coupled modes. (C) 2007 American Institute of Physics.
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