Förster resonance energy transfer, absorption and emission spectra in multichromophoric systems. III. Exact stochastic path integral evaluation
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Cao_Forster resonance.pdf
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664.77 KB
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Author(s)
Moix, Jeremy
Ma, Jian
Cao, Jianshu
Date Issued
March 2015
Journal
The Journal of Chemical Physics
Publisher
American Institute of Physics (AIP)
Citation
Moix, Jeremy M., Jian Ma, and Jianshu Cao. “Förster Resonance Energy Transfer, Absorption and Emission Spectra in Multichromophoric Systems. III. Exact Stochastic Path Integral Evaluation.” The Journal of Chemical Physics 142.9 (2015): 094108. © 2015 AIP Publishing LLC
Version
Final published version
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 Förster 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 (see Paper II) is the only perturbative method capable of generating uniformly reliable energy transfer rates and emission spectra across a broad range of system parameters.
MIT Department
Massachusetts Institute of Technology. Department of Chemistry
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Article is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.
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DOI of Published Version
https://doi.org/10.1063/1.4908601
