Understanding Primary Charge Separation and Revealing Fermi's Golden Rule in the Heliobacterium Modesticaldum Reaction Center

Basit Öğe Kaydı
dc.authoridErtürk, Murat / 0000-0002-7039-1970
dc.authoridAksu, Hüseyin / 0000-0001-9463-3236
dc.contributor.authorErtürk, Murat
dc.contributor.authorGüneş, Zühra
dc.contributor.authorAksu, Hüseyin
dc.date.accessioned2025-05-29T02:57:50Z
dc.date.available2025-05-29T02:57:50Z
dc.date.issued2025
dc.departmentÇanakkale Onsekiz Mart Üniversitesi
dc.description.abstractWe investigate the spectroscopic properties and charge transfer (CT) processes in the homodimeric reaction center of Heliobacterium modesticaldum (HbRC), for which we report the first-principles calculation of Fermi's golden rule (FGR) for the first time in the literature. HbRC is the simplest known analogue to other photosystems and consists of the SPP molecule, the adjacent Acc, and key amino acid residues (His537 and Gln458), along with two water molecules. We identify intrapair CT processes within the SPP molecule, which acts as the donor for the simplified model used in this study. We also examine the SPP+Acc- CT processes, where we demonstrate, in agreement with experimental findings, symmetric hole-electron delocalization across both Acc monomers. The calculated forward CT states are lower in energy than the bright states, facilitating electron transfer through a downhill CT reaction pathway. To explore the influence of surrounding molecular pigments on the electronic structure and FGR rate, we use augmented models incorporating nonsymmetrized molecular orientations. Most FGR rates are found to be on the order of picoseconds (ps). All electronic parameters are derived using an optimally tuned screened range-separated hybrid functional within a polarizable continuum model (SRSH-PCM), considering different dielectric constants.
dc.description.sponsorshipT?rkiye Bilimsel ve Teknolojik Arastirma Kurumu [123Z591, TUBITAK 1001]; Scientific and Technological Research Council of Turkiye (TUBITAK); TUBITAK
dc.description.sponsorshipThis study was supported by the Scientific and Technological Research Council of Turkiye (TUBITAK) under Grant Number 123Z591 (TUBITAK 1001). Authors M.E. and H.A. thank TUBITAK for their support. The authors are thankful to Canakkale Onsekiz Mart University Faculty of Science for computing facilities and making the resources available to complete the reported research.
dc.identifier.doi10.1021/acs.jpcb.4c08385
dc.identifier.endpage4142
dc.identifier.issn1520-6106
dc.identifier.issn1520-5207
dc.identifier.issue17
dc.identifier.pmid40251736
dc.identifier.scopus2-s2.0-105004052702
dc.identifier.scopusqualityQ2
dc.identifier.startpage4133
dc.identifier.urihttps://doi.org/10.1021/acs.jpcb.4c08385
dc.identifier.urihttps://hdl.handle.net/20.500.12428/30193
dc.identifier.volume129
dc.identifier.wosWOS:001470688900001
dc.identifier.wosqualityQ3
dc.indekslendigikaynakWeb of Science
dc.indekslendigikaynakScopus
dc.indekslendigikaynakPubMed
dc.language.isoen
dc.publisherAmer Chemical Soc
dc.relation.ispartofJournal of Physical Chemistry B
dc.relation.publicationcategoryMakale - Uluslararası Hakemli Dergi - Kurum Öğretim Elemanı
dc.rightsinfo:eu-repo/semantics/closedAccess
dc.snmzKA_WOS_20250529
dc.subjectDensity-Functional Theory
dc.subjectTransfer States
dc.subjectRational Design
dc.subjectEnergy-Transfer
dc.subjectAb-Initio
dc.subjectBacteriochlorin
dc.subjectBenchmarking
dc.titleUnderstanding Primary Charge Separation and Revealing Fermi's Golden Rule in the Heliobacterium Modesticaldum Reaction Center
dc.typeArticle

Dosyalar

Orijinal paket
Listeleniyor 1 - 1 / 1
[ X ]
İsim:
Huseyin Aksu_Makale.pdf
Boyut:
4.14 MB
Biçim:
Adobe Portable Document Format
İndir

Koleksiyon

WoS İndeksli Yayınlar Koleksiyonu
Fizik Bölümü Koleksiyonu
PubMed İndeksli Yayınlar Koleksiyonu
Scopus İndeksli Yayınlar Koleksiyonu