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MO: Fachverband Molekülphysik

MO 3: Electronic I

MO 3.2: Talk

Monday, March 14, 2022, 17:00–17:15, MO-H5

Simulation of Two-Dimensional Electronic Spectra of molecular aggregates: a Hierarchy of Stochastic Pure State approach — •Lipeng Chen¹, Doran I.G. Bennett², and Alexander Eisfeld¹ — ¹Max Planck Institute for the Physics of Complex Systems, Nöthnitzer Str 38, Dresden, Germany — ²Department of Chemistry, Southern Methodist University, PO Box 750314, Dallas, TX, USA

Modern techniques of time-resolved nonlinear optical spectroscopy have expanded our understanding of the photophysics of molecular aggregates, which is of particular importance for unravelling excitonic relaxation and dephasing processes in both artificial materials and photosynthetic complexes. In particular, two dimensional electronic spectroscopy has become a powerful technique to probe molecular excitons in the visible region and reveal couplings and relaxation pathways. We develop a new methodology for simulating two dimensional electronic spectra of molecular aggregates with strong coupling of electronic excitation to a structured environment by combining the stochastic hierarchy of pure states (HOPS) method with the nonlinear response function formalism. In our approach, the third-order response functions are evaluated by employing a novel propagation scheme where the combined ket and bra states are propagated in an augmented electronic Hilbert space. The new approach shows fast convergence properties with respect to the number of stochastic trajectories, providing a promising technique for numerical calculation of two dimensional spectra of large molecular aggregates.