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Updated: Aug 28, 2025

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids
Published on: May 27, 2020
Calculating nonlinear response functions for multidimensional electronic spectroscopy using dyadic non-Markovian
Lipeng Chen1, Doran I G Bennett2, Alexander Eisfeld1
1Max Planck Institute for the Physics of Complex Systems, Nöthnitzer Str. 38, Dresden, Germany.
Abstract:
We present a methodology for simulating multidimensional electronic spectra of molecular aggregates with coupling of electronic excitation to a structured environment using the stochastic non-Markovian quantum state diffusion (NMQSD) method in combination with perturbation theory for the response functions. A crucial aspect of our approach is that we propagate the NMQSD equation in a doubled system Hilbert space but with the same noise. We demonstrate that our approach shows fast convergence with respect to the number of stochastic trajectories, providing a promising technique for numerical calculation of two-dimensional electronic spectra of large molecular aggregates.
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