Hierarchical Equations of Motion Simulation of Temperature-Dependent Two-Dimensional Electronic Spectroscopy of the Chlorophyll a Manifold in LHCII

Leng, Xuan and Do, Thanh Nhut and Akhtar, Parveen and Nguyen, Hoang Long and Lambrev, Petar H. (2020) Hierarchical Equations of Motion Simulation of Temperature-Dependent Two-Dimensional Electronic Spectroscopy of the Chlorophyll a Manifold in LHCII. CHEMISTRY - AN ASIAN JOURNAL, 15 (13). pp. 1996-2004. ISSN 1861-4728 (print); 1861-471X (online)

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Abstract

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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