Please use this identifier to cite or link to this item: https://hdl.handle.net/10356/155597
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dc.contributor.authorNguyen, Hoang Longen_US
dc.contributor.authorDo, Thanh Nhuten_US
dc.contributor.authorAkhtar, Parveenen_US
dc.contributor.authorJansen, Thomas L. C.en_US
dc.contributor.authorKnoester, Jasperen_US
dc.contributor.authorWang, Wendaen_US
dc.contributor.authorShen, Jian-Renen_US
dc.contributor.authorLambrev, Petar H.en_US
dc.contributor.authorTan, Howe-Siangen_US
dc.date.accessioned2022-03-14T08:18:30Z-
dc.date.available2022-03-14T08:18:30Z-
dc.date.issued2021-
dc.identifier.citationNguyen, H. L., Do, T. N., Akhtar, P., Jansen, T. L. C., Knoester, J., Wang, W., Shen, J., Lambrev, P. H. & Tan, H. (2021). An exciton dynamics model of Bryopsis corticulans light-harvesting complex II. Journal of Physical Chemistry B, 125(4), 1134-1143. https://dx.doi.org/10.1021/acs.jpcb.0c10634en_US
dc.identifier.issn1520-6106en_US
dc.identifier.urihttps://hdl.handle.net/10356/155597-
dc.description.abstractBryopsis corticulans is a marine green macroalga adapted to the intertidal environment. It possesses siphonaxanthin-binding light-harvesting complexes of photosystem II (LHCII) with spectroscopic properties markedly different from the LHCII in plants. By applying a phenomenological fitting procedure to the two-dimensional electronic spectra of the LHCII from B. corticulans measured at 77 K, we can extract information about the excitonic states and energy-transfer processes. The fitting method results in well-converged parameters, including excitonic energy levels with their respective transition dipole moments, spectral widths, energy-transfer rates, and coupling properties. The 2D spectra simulated from the fitted parameters concur very well with the experimental data, showing the robustness of the fitting method. An excitonic energy-transfer scheme can be constructed from the fitting parameters. It shows the rapid energy transfer from chlorophylls (Chls) b to a at subpicosecond time scales and a long-lived state in the Chl b region at around 659 nm. Three weakly connected terminal states are resolved at 671, 675, and 677 nm. The lowest state is higher in energy than that in plant LHCII, which is probably because of the fewer number of Chls a in a B. corticulans LHCII monomer. Modeling based on existing Hamiltonians for the plant LHCII structure with two Chls a switched to Chls b suggests several possible Chl a-b replacements in comparison with those of plant LHCII. The adaptive changes result in a slower energy equilibration in the complex, revealed by the longer relaxation times of several exciton states compared to those of plant LHCII. The strength of our phenomenological fitting method for obtaining excitonic energy levels and energy-transfer network is put to the test in systems such as B. corticulans LHCII, where prior knowledge on exact assignment and spatial locations of pigments are lacking.en_US
dc.description.sponsorshipMinistry of Education (MOE)en_US
dc.language.isoenen_US
dc.relationRG2/19en_US
dc.relationRG15/18en_US
dc.relation.ispartofJournal of Physical Chemistry Ben_US
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry B, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcb.0c10634.en_US
dc.subjectScience::Chemistryen_US
dc.titleAn exciton dynamics model of Bryopsis corticulans light-harvesting complex IIen_US
dc.typeJournal Articleen
dc.contributor.schoolSchool of Physical and Mathematical Sciencesen_US
dc.identifier.doi10.1021/acs.jpcb.0c10634-
dc.description.versionSubmitted/Accepted versionen_US
dc.identifier.pmid33478222-
dc.identifier.scopus2-s2.0-85100272403-
dc.identifier.issue4en_US
dc.identifier.volume125en_US
dc.identifier.spage1134en_US
dc.identifier.epage1143en_US
dc.subject.keywordsFlowen_US
dc.subject.keywordsEnergy Transferen_US
dc.description.acknowledgementH.-S.T acknowledges support from the Singapore Ministry of Education Academic Research Fund (Tier 1 RG2/19 and Tier 1 RG15/18). P.H.L. acknowledges grants from the National Research, Development and Innovation Fund (Grants NN124904 and 2018-1.2.1-NKP-2018-00009). This work was also supported by a Strategic Priority Research Program (XDB17030100) of China, a Key Research Project for Frontier Science (QYZDY-SSW-SMC003) from the Chinese Academy of Sciences (CAS), China, and a bilateral project between CAS and the Hungary Academy of Sciences.en_US
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