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Energy relaxation pathways between light-matter states revealed by coherent two-dimensional spectroscopy

Mewes, L; Wang, M; Ingle, RA; Borjesson, K; Chergui, M; (2020) Energy relaxation pathways between light-matter states revealed by coherent two-dimensional spectroscopy. Communications Physics , 3 , Article 157. 10.1038/s42005-020-00424-z. Green open access

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Abstract

Coupling matter excitations to electromagnetic modes inside nano-scale optical resonators leads to the formation of hybrid light-matter states, so-called polaritons, allowing the controlled manipulation of material properties. Here, we investigate the photo-induced dynamics of a prototypical strongly-coupled molecular exciton-microcavity system using broadband two-dimensional Fourier transform spectroscopy and unravel the mechanistic details of its ultrafast photo-induced dynamics. We find evidence for a direct energy relaxation pathway from the upper to the lower polariton state that initially bypasses the excitonic manifold of states, which is often assumed to act as an intermediate energy reservoir, under certain experimental conditions. This observation provides new insight into polariton photophysics and could potentially aid the development of applications that rely on controlling the energy relaxation mechanism, such as in solar energy harvesting, manipulating chemical reactivity, the creation of Bose–Einstein condensates and quantum computing.

Type: Article
Title: Energy relaxation pathways between light-matter states revealed by coherent two-dimensional spectroscopy
Open access status: An open access version is available from UCL Discovery
DOI: 10.1038/s42005-020-00424-z
Publisher version: https://doi.org/10.1038/s42005-020-00424-z
Language: English
Additional information: 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/.
Keywords: Chemical physics, Excited states, Nanocavities, Polaritons, Optical spectroscopy
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10116942
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