Antioxidative Triplet Excitation Energy Transfer in Bacterial Reaction Center Using a Screened Range Separated Hybrid Functional

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dc.contributor.authorBegam, Khadiza
dc.contributor.authorAksu, Huseyin
dc.contributor.authorDunietz, Barry D.
dc.date.accessioned2025-01-27T20:51:50Z
dc.date.available2025-01-27T20:51:50Z
dc.date.issued2024
dc.departmentÇanakkale Onsekiz Mart Üniversitesi
dc.description.abstractExcess energy absorbed by photosystems (PSs) can result in photoinduced oxidative damage. Transfer of such energy within the core pigments of the reaction center in the form of triplet excitation is important in regulating and preserving the functionality of PSs. In the bacterial reaction center (BRC), the special pair (P) is understood to act as the electron donor in a photoinduced charge transfer process, triggering the charge separation process through the photoactive branch A pigments that experience a higher polarizing environment. At this work, triplet excitation energy transfer (TEET) in BRC is studied using a computational perspective to gain insights into the roles of the dielectric environment and interpigment orientations. We find in agreement with experimental observations that TEET proceeds through branch B. The TEET process toward branch B pigment is found to be significantly faster than the hypothetical process proceeding through branch A pigments with ps and ms time scales, respectively. Our calculations find that conformational differences play a major role in this branch asymmetry in TEET, where the dielectric environment asymmetry plays only a secondary role in directing the TEET to proceed through branch B. We also address TEET processes asserting the role of carotenoid as the final triplet energy acceptor and in a mutant form, where the branch pigments adjacent to P are replaced by bacteriopheophytins. The necessary electronic excitation energies and electronic state couplings are calculated by the recently developed polarization-consistent framework combining a screened range-separated hybrid functional and a polarizable continuum mode. The polarization-consistent potential energy surfaces are used to parametrize the quantum mechanical approach, implementing Fermi's golden rule expression of the TEET rate calculations.
dc.description.sponsorshipTrkiye Bilimsel ve Teknolojik Arastirma Kurumu; Kent State University, College of Arts and Sciences Computing Cluster [123Z591]; TUBITAK 1001
dc.description.sponsorshipWe are grateful for the generous resource allocations at the Ohio Supercomputer Center and the Kent State University, College of Arts and Sciences Computing Cluster. H.A. is grateful for support from TUBITAK 1001, project number 123Z591. K.B. thanks Srijana Bhandari for her help and support.
dc.identifier.doi10.1021/acs.jpcb.3c08501
dc.identifier.endpage4324
dc.identifier.issn1520-6106
dc.identifier.issn1520-5207
dc.identifier.issue18
dc.identifier.pmid38687467
dc.identifier.scopus2-s2.0-85192183541
dc.identifier.scopusqualityQ2
dc.identifier.startpage4315
dc.identifier.urihttps://doi.org/10.1021/acs.jpcb.3c08501
dc.identifier.urihttps://hdl.handle.net/20.500.12428/25538
dc.identifier.volume128
dc.identifier.wosWOS:001227795500001
dc.identifier.wosqualityN/A
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.indekslendigikaynakPubMed
dc.language.isoen
dc.publisherAmer Chemical Soc
dc.relation.ispartofJournal of Physical Chemistry B
dc.relation.publicationcategoryinfo:eu-repo/semantics/openAccess
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.snmzKA_WoS_20250125
dc.subjectPhotosynthetic Reaction-Center
dc.subjectLight-Harvesting Complex
dc.subjectSinglet Oxygen Production
dc.subjectCharge-Transfer
dc.subjectRhodobacter-Sphaeroides
dc.subjectElectron-Transfer
dc.subjectPhotosystem-Ii
dc.subjectSpecial Pair
dc.subjectCarotenoids
dc.subjectMechanism
dc.titleAntioxidative Triplet Excitation Energy Transfer in Bacterial Reaction Center Using a Screened Range Separated Hybrid Functional
dc.typeArticle

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