Abstract
We propose and analyze theoretically the implementation of two pump pulses with orthogonal linear polarization for the separate measurement of an interaction induced response in liquids through the optically-heterodyne-detected optical-Kerr-effect. The key parameters controlling the specificity of the double-pulse excitation scenarios are the pulse duration, the delay between pulses and the relation between the pump pulses amplitudes. We use acetonitrile as an example to model the fifth-order optical response and consider some principles of the scenarios construction. We show that it is possible to adjust the excitation scenario in such a way that the intramolecular and orientational responses are removed from the detected signal. The theoretical analysis reveals that the double-pulse excitation technique can be useful for the selective spectroscopy of the interaction induced responses of the molecules in liquid.
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