Premium
Hierarchical Equations of Motion Simulation of Temperature‐Dependent Two‐Dimensional Electronic Spectroscopy of the Chlorophyll a Manifold in LHCII
Author(s) -
Leng Xuan,
Do Thanh Nhut,
Akhtar Parveen,
Nguyen Hoang Long,
Lambrev Petar H.,
Tan HoweSiang
Publication year - 2020
Publication title -
chemistry – an asian journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.18
H-Index - 106
eISSN - 1861-471X
pISSN - 1861-4728
DOI - 10.1002/asia.202000467
Subject(s) - work (physics) , manifold (fluid mechanics) , excitation , spectroscopy , chlorophyll a , chemistry , light harvesting complex , molecular physics , physics , chemical physics , computational physics , analytical chemistry (journal) , photosynthesis , thermodynamics , photosystem ii , quantum mechanics , chromatography , engineering , mechanical engineering , biochemistry
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.