Autor: |
Liu Z; Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo 315211, P. R. China., Zhang P; Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo 315211, P. R. China., Mei C; Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo 315211, P. R. China., Liang XT; Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo 315211, P. R. China., Jha A; Rosalind Franklin Institute, Harwell Campus, OX11 0QX Didcot, U.K.; Department of Pharmacology, University of Oxford, OX1 3QT Oxford, U.K., Duan HG; Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo 315211, P. R. China. |
Abstrakt: |
Chirality plays a pivotal role across scientific disciplines with profound implications spanning light-matter interactions, molecular recognition, and natural evolutionary processes. This study delves into the active influence of molecular chirality on exciton energy transfer within photosynthetic protein complexes, focusing on the Fenna-Matthews-Olson (FMO) complex. Employing two-dimensional circular dichroism (2DCD) spectroscopy, we investigate the transient chiral dynamics of excitons during energy transfer processes within the FMO complex. Our approach, incorporating pulse information into population dynamics based on the third-order response function, facilitates the calculation of 2DCD spectra and dynamics. This enables the extraction of chiral contributions to excitonic energy transfer and the examination of electronic wave functions. We demonstrate that 2DCD spectra offer excitation energies that are better resolved than those from conventional two-dimensional electronic spectroscopy. These findings deepen our understanding of exciton energy transfer mechanisms in natural photosynthesis, emphasizing the potential of 2DCD spectroscopy as a powerful tool for unraveling the chiral contribution to exciton dynamics. |