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Effect of disorder and polarization sequences on two-dimensional spectra of light-harvesting complexes

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Abstract

Two-dimensional electronic spectra (2DES) provide unique ways to track the energy transfer dynamics in light-harvesting complexes. The interpretation of the peaks and structures found in experimentally recorded 2DES is often not straightforward, since several processes are imaged simultaneously. The choice of specific pulse polarization sequences helps to disentangle the sometimes convoluted spectra, but brings along other disturbances. We show by detailed theoretical calculations how 2DES of the Fenna–Matthews–Olson complex are affected by rotational and conformational disorder of the chromophores.

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Acknowledgements

The work was supported by the German Research Foundation (DFG) grants KR 2889 and RE 1389 (“Realistic Simulations of Photoactive Systems on HPC Clusters with Many Core Processors”). We acknowledge compute time allocation by the North German Supercomputing Alliance (HLRN). M.R. has received funding from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant agreement No. 707636.

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Correspondence to Tobias Kramer.

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Kramer, T., Rodríguez, M. Effect of disorder and polarization sequences on two-dimensional spectra of light-harvesting complexes. Photosynth Res (2019). https://doi.org/10.1007/s11120-019-00699-6

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Keywords

  • Two-dimensional spectroscopy
  • Light-harvesting complex
  • FMO (Fenna–Matthews–Olson complex)