Journal
CHEMISTRY-AN ASIAN JOURNAL
Volume 15, Issue 13, Pages 1996-2004Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/asia.202000467
Keywords
Light-harvesting complexes; Excitation energy transfer; Multidimensional spectroscopy; HEOM-PMA
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Funding
- Singapore Ministry of Education Academic Research Fund [Tier 2 MOE2015-T2-1-039, Tier 1 RG15/18]
- Hungarian National Research, Development and Innovation Fund [NN-124904, 2018-1.2.1-NKP-2018-00009]
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We simulated two-dimensional electronic spectra (2DES) of the chlorophyll a manifold of light-harvesting complex II (LHCII) at various temperatures (77, 110, 150, 190, 230, 273, and 293 K) using the hierarchical equations of the motion-phase matching approach. We confirm the main excitation energy transfer pathways assignments within the chlorophyll a manifold of LHCII measured in a recent work (J. Phys. Chem. B 2019, 123, 6765-6775). The calculated transfer rates are also in general agreement with the measured rates. We also provided theoretical confirmation for the experimental assignments, as uphill and downhill energy transfer processes, of 2D spectral features that were reported in recent experimental reports. These temperature-dependent features were also ascertained to follow the detailed-balance principle.
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