English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT
 
 
DownloadE-Mail
  Excitation landscape of the CP43 photosynthetic antenna complex from multiscale simulations

Bhattacharjee, S., Arra, S., Daidone, I., & Pantazis, D. A. (2024). Excitation landscape of the CP43 photosynthetic antenna complex from multiscale simulations. Chemical Science. doi:10.1039/D3SC06714A.

Item is

Files

show Files

Locators

show

Creators

show
hide
 Creators:
Bhattacharjee, Sinjini1, Author           
Arra, Srilatha2, Author
Daidone, Isabella2, Author
Pantazis, Dimitrios A.3, Author           
Affiliations:
1Research Department Neese, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541710              
2Department of Physical and Chemical Sciences, University of L'Aquila , Via Vetoio (Coppito 1), 67010 L'Aquila, Italy, ou_persistent22              
3Research Group Pantazis, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541711              

Content

show
hide
Free keywords: -
 Abstract: Photosystem II (PSII), the principal enzyme of oxygenic photosynthesis, contains two integral light harvesting proteins (CP43 and CP47) that bind chlorophylls and carotenoids. The two intrinsic antennae play crucial roles in excitation energy transfer and photoprotection. CP43 interacts most closely with the reaction center of PSII, specifically with the branch of the reaction center (D1) that is responsible for primary charge separation and electron transfer. Deciphering the function of CP43 requires detailed atomic-level insights into the properties of the embedded pigments. To advance this goal, we employ a range of multiscale computational approaches to determine the site energies and excitonic profile of CP43 chlorophylls, using large all-atom models of a membrane-bound PSII monomer. In addition to time-dependent density functional theory (TD-DFT) used in the context of a quantum-mechanics/molecular-mechanics setup (QM/MM), we present a thorough analysis using the perturbed matrix method (PMM), which enables us to utilize information from long-timescale molecular dynamics simulations of native PSII-complexed CP43. The excited state energetics and excitonic couplings have both similarities and differences compared with previous experimental fits and theoretical calculations. Both static TD-DFT and dynamic PMM results indicate a layered distribution of site energies and reveal specific groups of chlorophylls that have shared contributions to low-energy excitations. Importantly, the contribution to the lowest energy exciton does not arise from the same chlorophylls at each system configuration, but rather changes as a function of conformational dynamics. An unexpected finding is the identification of a low-energy charge-transfer excited state within CP43 that involves a lumenal (C2) and the central (C10) chlorophyll of the complex. The results provide a refined basis for structure-based interpretation of spectroscopic observations and for further deciphering excitation energy transfer in oxygenic photosynthesis.

Details

show
hide
Language(s): eng - English
 Dates: 2023-12-142024-04-09
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/D3SC06714A
 Degree: -

Event

show

Legal Case

show

Project information

show

Source 1

show
hide
Title: Chemical Science
  Abbreviation : Chem. Sci.
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: Cambridge, UK : Royal Society of Chemistry
Pages: - Volume / Issue: - Sequence Number: - Start / End Page: - Identifier: ISSN: 2041-6520
CoNE: https://pure.mpg.de/cone/journals/resource/2041-6520