Unraveling quantum coherences mediating primary charge transfer processes in photosystem II reaction center.

Autor: Jha A; Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo, 315211, P.R. China.; Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761, Hamburg, Germany.; Rosalind Franklin Institute, Harwell, Oxfordshire OX11 0QX, UK.; Department of Pharmacology, University of Oxford, Oxford OX1 3QT, UK., Zhang PP; Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo, 315211, P.R. China., Tiwari V; Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761, Hamburg, Germany.; Department of Chemistry, University of Hamburg, Martin-Luther-King Platz 6, 20146 Hamburg, Germany., Chen L; Zhejiang Laboratory, Hangzhou 311100, P.R. China., Thorwart M; I. Institut für Theoretische Physik, Universität Hamburg, Notkestr. 9, 22607 Hamburg, Germany.; The Hamburg Center for Ultrafast Imaging, Luruper Chaussee 149, 22761 Hamburg, Germany., Miller RJD; The Departments of Chemistry and Physics, University of Toronto, 80 St. George Street, Toronto, ON M5S 3H6, Canada., Duan HG; Department of Physics, School of Physical Science and Technology, Ningbo University, Ningbo, 315211, P.R. China.; Max Planck Institute for the Structure and Dynamics of Matter, Luruper Chaussee 149, 22761, Hamburg, Germany.; I. Institut für Theoretische Physik, Universität Hamburg, Notkestr. 9, 22607 Hamburg, Germany.; The Hamburg Center for Ultrafast Imaging, Luruper Chaussee 149, 22761 Hamburg, Germany.
Jazyk: angličtina
Zdroj: Science advances [Sci Adv] 2024 Mar 08; Vol. 10 (10), pp. eadk1312. Date of Electronic Publication: 2024 Mar 06.
DOI: 10.1126/sciadv.adk1312
Abstrakt: Photosystem II (PSII) reaction center (RC) is a unique complex that is capable of efficiently separating electronic charges across the membrane. The primary energy- and charge-transfer (CT) processes occur on comparable ultrafast timescales, which makes it extremely challenging to understand the fundamental mechanism responsible for the near-unity quantum efficiency of the transfer. Here, we elucidate the role of quantum coherences in the ultrafast energy and CT in the PSII RC by performing two-dimensional (2D) electronic spectroscopy at the cryogenic temperature of 20 kelvin, which captures the distinct underlying quantum coherences. Specifically, we uncover the electronic and vibrational coherences along with their lifetimes during the primary ultrafast processes of energy and CT. We construct an excitonic model that provides evidence for coherent energy and CT at low temperature in the 2D electronic spectra. The principles could provide valuable guidelines for creating artificial photosystems with exploitation of system-bath coupling and control of coherences to optimize the photon conversion efficiency to specific functions.
Databáze: MEDLINE