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

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 strongl...

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Veröffentlicht in:Communications physics Jg. 3; H. 1
Hauptverfasser: Mewes, Lars, Wang, Mao, Ingle, Rebecca A., Börjesson, Karl, Chergui, Majed
Format: Journal Article
Sprache:Englisch
Veröffentlicht: London Nature Publishing Group UK 11.09.2020
Nature Publishing Group
Schlagworte:
639/624/1107/527
639/624/399/1098
639/638/440/94
639/638/440/949
639/766/400/2797
Bose-Einstein condensates
Broadband
cavities
chemistry
Coupling (molecular)
Energy harvesting
Excitation spectra
exciton-polaritons
Excitons
Fourier transforms
Fysik
Material properties
molecular-dynamics
Optical resonators
Physical Sciences
Physics
Physics and Astronomy
polariton dynamics
Polaritons
Quantum computing
Room temperature
Solar energy
Spectrum analysis
ISSN:2399-3650, 2399-3650
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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. Recent spectroscopic studies have elucidated light-matter interactions in exciton-polaritons at room temperature, yet their precise excited-state dynamics remain unclear. Here, broadband 2D Fourier transform spectroscopy reveals the relaxation between polaritonic states and the role of dark states.
AbstractList 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. Recent spectroscopic studies have elucidated light-matter interactions in exciton-polaritons at room temperature, yet their precise excited-state dynamics remain unclear. Here, broadband 2D Fourier transform spectroscopy reveals the relaxation between polaritonic states and the role of dark states.
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.
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. Recent spectroscopic studies have elucidated light-matter interactions in exciton-polaritons at room temperature, yet their precise excited-state dynamics remain unclear. Here, broadband 2D Fourier transform spectroscopy reveals the relaxation between polaritonic states and the role of dark states.
ArticleNumber 157
Author Chergui, Majed
Wang, Mao
Mewes, Lars
Ingle, Rebecca A.
Börjesson, Karl
Author_xml – sequence: 1
  givenname: Lars
  orcidid: 0000-0001-9269-1475
  surname: Mewes
  fullname: Mewes, Lars
  email: lars.mewes@tum.de
  organization: Laboratoire de Spectroscopie Ultrarapide and Lausanne Centre for Ultrafast Science, Institut des Sciences et Ingénierie Chimique, Ecole Polytechnique Fédérale de Lausanne, ISIC, Dynamische Spektroskopien, Fakultät für Chemie, Technische Universität München
– sequence: 2
  givenname: Mao
  orcidid: 0000-0002-0768-3452
  surname: Wang
  fullname: Wang, Mao
  organization: Department of Chemistry and Molecular Biology, University of Gothenburg
– sequence: 3
  givenname: Rebecca A.
  surname: Ingle
  fullname: Ingle, Rebecca A.
  organization: Laboratoire de Spectroscopie Ultrarapide and Lausanne Centre for Ultrafast Science, Institut des Sciences et Ingénierie Chimique, Ecole Polytechnique Fédérale de Lausanne, ISIC, Department of Chemistry, University College London
– sequence: 4
  givenname: Karl
  orcidid: 0000-0001-8533-201X
  surname: Börjesson
  fullname: Börjesson, Karl
  organization: Department of Chemistry and Molecular Biology, University of Gothenburg
– sequence: 5
  givenname: Majed
  orcidid: 0000-0002-4856-226X
  surname: Chergui
  fullname: Chergui, Majed
  email: majed.chergui@epfl.ch
  organization: Laboratoire de Spectroscopie Ultrarapide and Lausanne Centre for Ultrafast Science, Institut des Sciences et Ingénierie Chimique, Ecole Polytechnique Fédérale de Lausanne, ISIC
BackLink https://gup.ub.gu.se/publication/297873$$DView record from Swedish Publication Index (Göteborgs universitet)
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Snippet Coupling matter excitations to electromagnetic modes inside nano-scale optical resonators leads to the formation of hybrid light-matter states, so-called...
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SubjectTerms 639/624/1107/527
639/624/399/1098
639/638/440/94
639/638/440/949
639/766/400/2797
Bose-Einstein condensates
Broadband
cavities
chemistry
Coupling (molecular)
Energy harvesting
Excitation spectra
exciton-polaritons
Excitons
Fourier transforms
Fysik
Material properties
molecular-dynamics
Optical resonators
Physical Sciences
Physics
Physics and Astronomy
polariton dynamics
Polaritons
Quantum computing
Room temperature
Solar energy
Spectrum analysis
Title Energy relaxation pathways between light-matter states revealed by coherent two-dimensional spectroscopy
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