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dc.contributor.authorDo, Thanh Nhuten_US
dc.contributor.authorHuerta-Viga, Adrianaen_US
dc.contributor.authorAkhtar, Parveenen_US
dc.contributor.authorNguyen, Hoang Longen_US
dc.contributor.authorNowakowski, Paweł J.en_US
dc.contributor.authorMuhammad Faisal Khyasudeenen_US
dc.contributor.authorLambrev, Petar H.en_US
dc.contributor.authorTan, Howe-Siangen_US
dc.identifier.citationDo, T. N., Huerta-Viga, A., Akhtar, P., Nguyen, H. L., Nowakowski, P. J., Khyasudeen, M. F., . . . Tan, H.-S. (2019). Revealing the excitation energy transfer network of Light-Harvesting Complex II by a phenomenological analysis of two-dimensional electronic spectra at 77 K. The Journal of Chemical Physics, 151(20), 205101-. doi:10.1063/1.5125744en_US
dc.description.abstractEnergy equilibration in light-harvesting antenna systems normally occurs before energy is transferred to a reaction center. The equilibration mechanism is a characteristic of the excitation energy transfer (EET) network of the antenna. Characterizing this network is crucial in understanding the first step of photosynthesis. We present our phenomenology-based analysis procedure and results in obtaining the excitonic energy levels, spectral linewidths, and transfer-rate matrix of Light-Harvesting Complex II directly from its 2D electronic spectra recorded at 77 K with waiting times between 100 fs to 100 ps. Due to the restriction of the models and complexity of the system, a unique EET network cannot be constructed. Nevertheless, a recurring pattern of energy transfer with very similar overall time scales between spectral components (excitons) is consistently obtained. The models identify a "bottleneck" state in the 664-668 nm region although with a relatively shorter lifetime (∼4-6 ps) of this state compared to previous studies. The model also determines three terminal exciton states at 675, 677-678, and 680-681 nm that are weakly coupled to each other. The excitation energy equilibration between the three termini is found to be independent of the initial excitation conditions, which is a crucial design for the light-harvesting complexes to ensure the energy flow under different light conditions and avoid excitation trapping. We proposed two EET schemes with tentative pigment assignments based on the interpretation of the modeling results together with previous structure-based calculations and spectroscopic observables.en_US
dc.relation.ispartofThe Journal of Chemical Physicsen_US
dc.rights© 2019 Author(s). All rights reserved. This paper was published by AIP Publishing in The Journal of Chemical Physics and is made available with permission of Author(s).en_US
dc.titleRevealing the excitation energy transfer network of Light-Harvesting Complex II by a phenomenological analysis of two-dimensional electronic spectra at 77 Ken_US
dc.typeJournal Articleen
dc.contributor.schoolSchool of Physical and Mathematical Sciencesen_US
dc.description.versionPublished versionen_US
dc.subject.keywordsSpectral Linewidthsen_US
dc.description.acknowledgementThe authors acknowledge support from the Hungarian Ministry of Innovation and Technology, National Research, Development and Innovation Office (Grant Nos. NN-124904 and 2018-1.2.1-NKP-2018-00009 to P.H.L.) and the Singapore Ministry of Education, Academic Research Fund (Tier 2 Grant No. MOE2015-T2-1-039 and Tier 1 Grant No. RG15/18 to H.-S.T.). The ELI-ALPS Project (No. GINOP-2.3.6-15-2015-00001) is supported by the European Union and co-financed by the European Regional Development Fund.en_US
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