Strong coupling of a confined optical field to the excitonic or vibronic transitions of a molecular material results in the formation of new hybrid states called polaritons. Such effects have been extensively studied in Fabry–Pèrot microcavity structures where an organic material is placed between two highly reflective mirrors. Recently, theoretical and experimental evidence has suggested that strong coupling can be used to modify chemical reactivity as well as molecular photophysical functionalities. However, the geometry of conventional microcavity structures limits the ability of molecules “encapsulated” in a cavity to interact with their local environment. Here, we fabricate mirrorless organic membranes that utilize the refractive index contrast between the organic active material and its surrounding medium to confine an optical field with Q-factor values up to 33. Using angle-resolved white light reflectivity measurements, we confirm that our structures operate in the strong coupling regime, with Rabi-splitting energies between 60 and 80 meV in the different structures studied. The experimental results are matched by transfer matrix and coupled oscillator models that simulate the various polariton states of the free standing membranes. Our work demonstrates that mechanically flexible and easy-to-fabricate free standing membranes can support strong light–matter coupling, making such simple and versatile structures highly promising for a range of polariton applications.
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21 December 2023
Research Article|
December 19 2023
Strong coupling in mechanically flexible free-standing organic membranes
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2023 JCP Emerging Investigators Special Collection
Kyriacos Georgiou
;
Kyriacos Georgiou
a)
(Conceptualization, Data curation, Formal analysis, Funding acquisition, Supervision, Writing – original draft, Writing – review & editing)
1
Department of Physics, Laboratory of Ultrafast Science, University of Cyprus
, Nicosia 1678, Cyprus
a)Author to whom correspondence should be addressed: [email protected]
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Modestos Athanasiou
;
Modestos Athanasiou
(Data curation, Formal analysis)
2
Department of Physics, Experimental Condensed Matter Physics Laboratory, University of Cyprus
, Nicosia 1678, Cyprus
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Rahul Jayaprakash
;
Rahul Jayaprakash
(Software)
3
Department of Physics and Astronomy, University of Sheffield
, Hicks Building, Hounsfield Road, Sheffield S3 7RH, United Kingdom
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David G. Lidzey
;
David G. Lidzey
(Writing – original draft, Writing – review & editing)
3
Department of Physics and Astronomy, University of Sheffield
, Hicks Building, Hounsfield Road, Sheffield S3 7RH, United Kingdom
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Grigorios Itskos
;
Grigorios Itskos
(Funding acquisition, Writing – original draft, Writing – review & editing)
2
Department of Physics, Experimental Condensed Matter Physics Laboratory, University of Cyprus
, Nicosia 1678, Cyprus
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Andreas Othonos
Andreas Othonos
(Funding acquisition, Writing – original draft, Writing – review & editing)
1
Department of Physics, Laboratory of Ultrafast Science, University of Cyprus
, Nicosia 1678, Cyprus
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Kyriacos Georgiou
1,a)
Modestos Athanasiou
2
Rahul Jayaprakash
3
David G. Lidzey
3
Grigorios Itskos
2
Andreas Othonos
1
1
Department of Physics, Laboratory of Ultrafast Science, University of Cyprus
, Nicosia 1678, Cyprus
2
Department of Physics, Experimental Condensed Matter Physics Laboratory, University of Cyprus
, Nicosia 1678, Cyprus
3
Department of Physics and Astronomy, University of Sheffield
, Hicks Building, Hounsfield Road, Sheffield S3 7RH, United Kingdom
a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 159, 234303 (2023)
Article history
Received:
September 26 2023
Accepted:
November 22 2023
Citation
Kyriacos Georgiou, Modestos Athanasiou, Rahul Jayaprakash, David G. Lidzey, Grigorios Itskos, Andreas Othonos; Strong coupling in mechanically flexible free-standing organic membranes. J. Chem. Phys. 21 December 2023; 159 (23): 234303. https://doi.org/10.1063/5.0178144
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