Calculating non-linear response functions for multi-dimensional electronic spectroscopy using dyadic non-Markovian quantum state diffusion

Abstract

We present a methodology for simulating multi-dimensional 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 spectra of large molecular aggregates.

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• Coherent Nonlinear Optical Response for High-Intensity Excitation
• Simulating Non-Markovian Dynamics in Multidimensional Electronic Spectroscopy via Quantum Algorithm
• Giant atoms coupled to waveguide: Continuous coupling and multiple excitations
• Extracting Coupling-Mode Spectral Densities with Two-Dimensional Electronic Spectroscopy
• Uniform process tensor approach for the calculation of multi-time correlation functions of non-Markovian open systems