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Phys. Chem. Chem. Phys., 2020, 22, 25720--25729.pdf 5096.01 Mb

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This work was supported by the Dutch Research Council (NWO) via a Vici grant to R. C. RvG acknowledges the financial support offered to him via the BioInspired Solar Energy Program of the Canadian Institute For Advanced Research (CIFAR). V. I. N. was supported by the Russian Foundation for Basic Research (Grant No. 18-04-00105). E. R. was supported by the European Research Council (Starting Grant number 805524, BioInspired_H2), and by the CERCA Program/Generalitat de Catalunya.

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Romero, ElisabetAuthor

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December 7, 2020
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Complete mapping of energy transfer pathways in the plant light-harvesting complex Lhca4

Publicated to:Physical Chemistry Chemical Physics. 22 (44): 25720-25729 - 2020-11-28 22(44), DOI: 10.1039/d0cp03351k

Authors: Tros, M; Novoderezhkin, VI; Croce, R; van Grondelle, R; Romero, E

Affiliations

Barcelona Inst Sci & Technol BIST, Inst Chem Res Catalonia ICIQ, Avinguda Dels Paisos Catalans 16, Tarragona 43007, Spain - Author
LaserLaB Amsterdam, Boelelaan 1081, NL-1081 HV Amsterdam, Netherlands - Author
Moscow MV Lomonosov State Univ, AN Belozersky Inst Physicochem Biol, Moscow 119992, Russia - Author
Vrije Univ Amsterdam, Dept Biophys, Fac Sci, Boelelaan 1081, NL-1081 HV Amsterdam, Netherlands - Author

Abstract

The Lhca4 antenna complex of plant Photosystem I (PSI) is characterized by extremely red-shifted and broadened absorption and emission bands from its low-energy chlorophylls (Chls). The mixing of a charge-transfer (CT) state with the excited state manifold causing these so-called red forms results in highly complicated multi-component excited energy transfer (EET) kinetics within the complex. The two-dimensional electronic spectroscopy experiments presented here reveal that EET towards the CT state occurs on three timescales: fast from the red Chls (within 1 ps), slower (5-7 ps) from the stromal side Chls, and very slow (100-200 ps) from a newly discovered 690 nm luminal trap. The excellent agreement between the experimental data with the previously presented Redfield-Forster exciton model of Lhca4 strongly supports the equilibration scheme of the bulk excitations with the dynamically localized CT on the stromal side. Thus, a complete picture of the energy transfer pathways leading to the population of the CT final trap within the whole Lhca4 complex is presented. In view of the environmental sensitivity of the CT contribution to the Lhca4 energy landscape, we speculate that one role of the CT states is to regulate the EET from the peripheral antenna to the PSI core.

Keywords

Absorption and emissionsAntennaAntennasCharge transferCharge transfer stateCharge-transfer statesComplete mappingsDynamicsEnergy transferEnvironmental sensitivitiesExcited statesExcitonFar-redFormsKineticsLight harvesting complexesLow-energy chlorophyllsPhotosynthesisPhotosystem-iPlant photosystemPlants (botany)ProteinsRed shiftSpectroscopic propertiesTwo-dimensional electronic spectroscopies

Quality index

Bibliometric impact. Analysis of the contribution and dissemination channel

The work has been published in the journal Physical Chemistry Chemical Physics due to its progression and the good impact it has achieved in recent years, according to the agency WoS (JCR), it has become a reference in its field. In the year of publication of the work, 2020, it was in position 8/37, thus managing to position itself as a Q1 (Primer Cuartil), in the category Physics, Atomic, Molecular & Chemical.

Independientemente del impacto esperado determinado por el canal de difusión, es importante destacar el impacto real observado de la propia aportación.

Según las diferentes agencias de indexación, el número de citas acumuladas por esta publicación hasta la fecha 2025-08-13:

  • Google Scholar: 6
  • WoS: 6

Impact and social visibility

From the perspective of influence or social adoption, and based on metrics associated with mentions and interactions provided by agencies specializing in calculating the so-called "Alternative or Social Metrics," we can highlight as of 2025-08-13:

  • The use of this contribution in bookmarks, code forks, additions to favorite lists for recurrent reading, as well as general views, indicates that someone is using the publication as a basis for their current work. This may be a notable indicator of future more formal and academic citations. This claim is supported by the result of the "Capture" indicator, which yields a total of: 20 (PlumX).

It is essential to present evidence supporting full alignment with institutional principles and guidelines on Open Science and the Conservation and Dissemination of Intellectual Heritage. A clear example of this is:

  • The work has been submitted to a journal whose editorial policy allows open Open Access publication.
  • Assignment of a Handle/URN as an identifier within the deposit in the Institutional Repository: http://hdl.handle.net/2072/378124

Leadership analysis of institutional authors

This work has been carried out with international collaboration, specifically with researchers from: Netherlands; Russia.

There is a significant leadership presence as some of the institution’s authors appear as the first or last signer, detailed as follows: Last Author (Romero Mesa, Elisabet).