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      Selective manipulation of electronically excited states through strong light–matter interactions

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      Nature Communications
      Nature Publishing Group UK

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          Abstract

          Strong coupling between light and matter leads to the spontaneous formation of hybrid light–matter states, having different energies than the uncoupled states. This opens up for new ways of modifying the energy landscape of molecules without changing their atoms or structure. Heavy metal-free organic light emitting diodes (OLED) use reversed intersystem crossing (RISC) to harvest light from excited triplet states. This is a slow process, thus increasing the rate of RISC could potentially enhance OLED performance. Here we demonstrate selective coupling of the excited singlet state of Erythrosine B without perturbing the energy level of a nearby triplet state. The coupling reduces the triplet–singlet energy gap, leading to a four-time enhancement of the triplet decay rate, most likely due to an enhanced rate of RISC. Furthermore, we anticipate that strong coupling can be used to create energy-inverted molecular systems having a singlet ground and lowest excited state.

          Abstract

          Manipulating energy levels in molecules could allow applications such as improving organic LEDs. Here, the authors show evidence that reversed intersystem crossing can be enhanced in Erythrosine B coupled to a cavity by selectively manipulating the energy of the singlet state.

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          Single-molecule strong coupling at room temperature in plasmonic nanocavities

          Emitters placed in an optical cavity experience an environment that changes their coupling to light. In the weak-coupling regime light extraction is enhanced, but more profound effects emerge in the single-molecule strong-coupling regime where mixed light-matter states form1,2. Individual two-level emitters in such cavities become non-linear for single photons, forming key building blocks for quantum information systems as well as ultra-low power switches and lasers3–6. Such cavity quantum electrodynamics has until now been the preserve of low temperatures and complex fabrication, severely compromising their use5,7,8. Here, by scaling the cavity volume below 40 nm3 and using host-guest chemistry to align 1-10 protectively-isolated methylene-blue molecules, we reach the strong-coupling regime at room temperature and in ambient conditions. Dispersion curves from >50 plasmonic nanocavities display characteristic anticrossings, with Rabi frequencies of 300 meV for 10 molecules decreasing to 90 meV for single molecules, matching quantitative models. Statistical analysis of vibrational spectroscopy time-series and dark-field scattering spectra provide evidence of single-molecule strong coupling. This dressing of molecules with light can modify photochemistry, opening up the exploration of complex natural processes such as photosynthesis9 and pathways towards manipulation of chemical bonds10.
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            Exciton-polariton Bose-Einstein condensation

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              Room-temperature polariton lasing in an organic single-crystal microcavity

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                Author and article information

                Contributors
                karl.borjesson@gu.se
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                11 June 2018
                11 June 2018
                2018
                : 9
                : 2273
                Affiliations
                ISNI 0000 0000 9919 9582, GRID grid.8761.8, Department of Chemistry and Molecular Biology, , University of Gothenburg, ; Kemigården 4, 412 96 Gothenburg, Sweden
                Article
                4736
                10.1038/s41467-018-04736-1
                5995866
                29891958
                b09e4ef8-fb9b-4dbd-a84c-0826d429396c
                © The Author(s) 2018

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

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                : 13 March 2018
                : 18 May 2018
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