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Transient third-order optical nonlinearity of organic molecules

Transient third-order nonlinearity is induced by electronic resonances of excited molecules. Intensity of a signal, which is generated due to transient nonlinear susceptibility, strongly depends on a relaxation pathway and rate of high excited molecular electronic states, and on molecular dynamics in a low-lying excited state. Experimental and theoretical data, concerning a transient susceptibility dependence on dynamics of excited polyatomic organic molecules (ultrafast dephasing and depopulation processes, orientation anisotropy, time-dependence of transient absorption spectrum), are discussed. Obtained results demonstrate a high sensitivity of transient third order susceptibility to dynamics of excited molecules.