Forster resonance energy transfer, absorption and emission spectra in multichromophoric systems: III. Exact stochastic path integral evaluation

Abstract

A numerically exact path integral treatment of the absorption and emission spectra of open quantum systems is presented that requires only the straightforward solution of a stochastic differential equation. The approach converges rapidly enabling the calculation of spectra of large excitonic systems across the complete range of system parameters and for arbitrary bath spectral densities. With the numerically exact absorption and emission operators one can also immediately compute energy transfer rates using the multi-chromophoric Forster resonant energy transfer formalism. Benchmark calculations on the emission spectra of two level systems are presented demonstrating the efficacy of the stochastic approach. This is followed by calculations of the energy transfer rates between two weakly coupled dimer systems as a function of temperature and system-bath coupling strength. It is shown that the recently developed hybrid cumulant expansion is the only perturbative method capable of generating uniformly reliable energy transfer rates and spectra across a broad range of system parameters.

20 pages, 4 figures

References in corpus (4)

• Dynamics of quantum dissipation systems interacting with bosonic canonical bath: Hierarchical equations of motion approach
• Decoherence of Excitons in Multichromophore Systems: Thermal Line Broadening and Destruction of Superradiant Emission
• Non-Markovian quantum state diffusion for absorption spectra of molecular aggregates
• Förster resonance energy transfer, absorption and emission spectra in multichromophoric systems: I. Cumulant expansions

Cited by in corpus (7)

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• Simulation of absorption spectra of molecular aggregates: a Hierarchy of Stochastic Pure States approach
• Accuracy of approximate methods for the calculation of absorption-type linear spectra with a complex system-bath coupling
• Emission spectral non-Markovianity in qubit-cavity systems in the ultrastrong coupling regime
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