Short-Range Effects in the Special Pair of Photosystem II Reaction Centers: The Nonconservative Nature of Circular Dichroism

Felix G. Gemeinhardt*, Yigal Lahav, Igor Schapiro, Dror Noy, Frank Müh, Dominik Lindorfer, Thomas Renger*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

Photosystem II reaction centers extract electrons from water, providing the basis of oxygenic life on earth. Among the light-sensitive pigments of the reaction center, a central chlorophyll a dimer, known as the special pair, so far has escaped a complete theoretical characterization of its excited state properties. The close proximity of the special pair pigments gives rise to short-range effects that comprise a coupling between local and charge transfer (CT) excited states as well as other intermolecular quantum effects. Using a multiscale simulation and a diabatization technique, we show that the coupling to CT states is responsible for 45% of the excitonic coupling in the special pair. The other short-range effects cause a nonconservative nature of the circular dichroism spectrum of the reaction center by effectively rotating the electric transition dipole moments of the special pair pigments inverting and strongly enhancing their intrinsic rotational strength.

Original languageAmerican English
Pages (from-to)11758-11767
Number of pages10
JournalJournal of Physical Chemistry Letters
Volume14
Issue number51
DOIs
StatePublished - 28 Dec 2023

Bibliographical note

Publisher Copyright:
© 2023 The Authors. Published by American Chemical Society.

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