Probing the dynamics of excitons requires nonlinear spectroscopy in general, for which significant progress has been made over the past two decades.  As yet, there remains much progress needed in theoretical interpretation of the various spectroscopic signals and in understanding their implications.  In particular, the interplay of quantum coherence and non-Markovian environmental relaxation on the spatio-temporal dynamics of excitons and the best strategy to characterize key spectroscopic observables for such observables remain unclear.  Furthermore, quantitative description of the effects of the disorder and time dependent fluctuations are missing in many of current theoretical formulations being used for the interpretation of experimental data. This talk presents two complementary formulations that can clarify these issues through explicit incorporation of the open system dynamics framework into the experimental set up of well-known time resolved nonlinear spectroscopies of exciton dynamics.  One is a direct two-pulse generalization of the conventional line shape theory and the other is the response function formalism of four-wave mixing spectroscopy.  Results of these formulations indicate existence of various cross terms that can complicate experimental interpretation, but accurate calculation of which can assist developing unambiguous consensus for well-defined experimental protocols for probing general time resolved dynamics of excitons in complex environments.

Open system dynamics formulations of the time-resolved nonlinear spectroscopy of excitons

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