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Grant support

This study was supported by the Ministry of Education and Science of the Russian Federation (grant no. 14.Y26.31.0011). I. N. acknowledges the support from the Ministry of Higher Education, Research and Innovation of the French Republic and the University of Reims Champagne-Ardenne. The part of the work devoted to the microresonator development and adaptation was supported by the Russian Science Foundation (grant no. 21-79-30048). Y. R. acknowledges the support from the Basque Government (grant no. IT1164-19). We thank Vladimir Ushakov for the help with technical preparation of the manuscript.

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Lednev, MAuthor

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September 20, 2022
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Polariton-assisted manipulation of energy relaxation pathways: donor-acceptor role reversal in a tuneable microcavity

Publicated to:Chemical Science. 12 (38): 12794-12805 - 2021-10-14 12(38), DOI: 10.1039/d1sc02026a

Authors: Dovzhenko, Dmitriy; Lednev, Maksim; Mochalov, Konstantin; Vaskan, Ivan; Rakovich, Yury; Karaulov, Alexander; Nabiev, Igor;

Affiliations

Basque Fdn Sci, Ikerbasque, Bilbao 48009, Spain - Author
Moscow Inst Phys & Technol, Moscow 141701, Russia - Author
Natl Res Nucl Univ MEPhI, Moscow Engn Phys Inst, Moscow 115409, Russia - Author
Russian Acad Sci, Shemyakin Ovchinnikov Inst Bioorgan Chem, Moscow 117997, Russia - Author
Sechenov First Moscow State Med Univ, Sechenov Univ, Moscow 119146, Russia - Author
Univ Basque Country, Ctr Fis Mat MPC, CSIC UPV EHU, Donostia Int Phys Ctr,Polimems & Mat Avanzados Fi, Donostia San Sebastian 20018, Spain - Author
Univ Reims, Lab Rech Nanosci, LRN EA4682, F-51100 Reims, France - Author
Univ Southampton, Dept Phys & Astron, Southampton SO17 1BJ, Hants, England - Author
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Abstract

Resonant interaction between excitonic transitions of molecules and localized electromagnetic field allows the formation of hybrid light-matter polaritonic states. This hybridization of the light and the matter states has been shown to significantly alter the intrinsic properties of molecular ensembles placed inside the optical cavity. Here, we have observed strong coupling of excitonic transition in a pair of closely located organic dye molecules demonstrating an efficient donor-to-acceptor resonance energy transfer with the mode of a tuneable open-access cavity. Analysing the dependence of the relaxation pathways between energy states in this system on the cavity detuning, we have demonstrated that predominant strong coupling of the cavity photon to the exciton transition in the donor dye molecule can lead not only to an increase in the donor-acceptor energy transfer, but also to an energy shift large enough to cause inversion between the energy states of the acceptor and the mainly donor lower polariton energy state. Furthermore, we have shown that the polariton-assisted donor-acceptor chromophores' role reversal or "carnival effect" not only changes the relative energy levels of the donor-acceptor pair, but also makes it possible to manipulate the energy flow in the systems with resonant dipole-dipole interaction and direct energy transfer from the acceptor to the mainly donor lower polariton state. Our experimental data are the first confirmation of the theoretically predicted possibility of polariton-assisted energy transfer reversal in FRET systems, thus paving the way to new avenues in FRET-imaging, remote-controlled chemistry, and all-optical switching.

Keywords

DynamicsEmissionExcitonsOrganic-dyesResonance

Quality index

Bibliometric impact. Analysis of the contribution and dissemination channel

The work has been published in the journal Chemical Science 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, 2021, it was in position 25/179, thus managing to position itself as a Q1 (Primer Cuartil), in the category Chemistry, Multidisciplinary.

From a relative perspective, and based on the normalized impact indicator calculated from World Citations from Scopus Elsevier, it yields a value for the Field-Weighted Citation Impact from the Scopus agency: 1.45, which indicates that, compared to works in the same discipline and in the same year of publication, it ranks as a work cited above average. (source consulted: ESI Nov 14, 2024)

This information is reinforced by other indicators of the same type, which, although dynamic over time and dependent on the set of average global citations at the time of their calculation, consistently position the work at some point among the top 50% most cited in its field:

  • Field Citation Ratio (FCR) from Dimensions: 3.06 (source consulted: Dimensions Jul 2025)

Specifically, and according to different indexing agencies, this work has accumulated citations as of 2025-07-08, the following number of citations:

  • WoS: 12
  • Scopus: 16

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 2025-07-08:

  • The use, from an academic perspective evidenced by the Altmetric agency indicator referring to aggregations made by the personal bibliographic manager Mendeley, gives us a total of: 20.
  • 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: 23 (PlumX).

With a more dissemination-oriented intent and targeting more general audiences, we can observe other more global scores such as:

  • The Total Score from Altmetric: 17.25.
  • The number of mentions on the social network X (formerly Twitter): 1 (Altmetric).
  • The number of mentions in news outlets: 2 (Altmetric).

Leadership analysis of institutional authors

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