Effect of solvent on resonant CARS and CSRS: a possibility for separation of inhomogeneous width

Inhomogeneously broadened excitation profiles of CARS and CSRS are examined, using equations in the time representation. The effect of inhomogeneity reveals itself in different intensity distribution for CARS and CSRS and in different lineshapes/widths. The last circumstance can be used for the separation of homogeneous and inhomogeneous linewidths. A procedure is proposed which allows one to determine these linewidths, based on measured linewidths of the absorption and the excitation Lines of CARS and CSRS. It can be applied in cases of both static and dynamic inhomogeneneities and also at room temperature. The procedure enables one to determine very short relaxation times (of the other of femtoseconds) via stationary experiments. (C) 1997 John Wiley & Sons, Ltd.