Mechanisms of blueshifts in organic polariton condensates
Mechanisms of blueshifts in organic polariton condensates
Bose-Einstein condensates of exciton-polaritons in inorganic semiconductor microcavities are known to possess strong interparticle interactions attributed to their excitonic component. The interactions play a crucial role in the nonlinear dynamics of such systems and can be witnessed as the energy blueshifts of polariton states. However, the localised nature of Frenkel excitons in strongly coupled organic microcavities precludes interparticle Coulomb exchange-interactions that change mechanisms of the nonlinearity and blueshifts accordingly. In this report, we unravel the origins of blueshifts in organic polariton condensates. We examine the possible contributions: intracavity optical Kerr-effect, gain-induced frequency-pulling, polariton interactions and effects related to saturation of optical transitions for weakly- and strongly-coupled molecules. We conclude that blueshifts in organic polariton condensates arise from the interplay of the saturation effects and intermolecular energy migration. Our model predicts the commonly observed step-like increase of both the emission energy and degree of linear polarization at the polariton condensation threshold.
Yagafarov, Timur
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Sannikov, Denis
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Zasedatelev, Anton
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Georgiou, Kyriacos
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Baranikov, Anton
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Kyriienko, Oleksandr
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Shelykh, Ivan
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Gai, Lizhi
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Shen, Zhen
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Lidzey, David
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Lagoudakis, Pavlos
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22 January 2020
Yagafarov, Timur
278060d1-9097-458b-93b4-058a7300a7bf
Sannikov, Denis
12dc6676-a9e5-417c-b451-27108cc221b5
Zasedatelev, Anton
b8f8265a-58a1-48c8-abf5-68e4e6ef8f70
Georgiou, Kyriacos
c93188ef-80fb-4b7c-9069-99b606d26211
Baranikov, Anton
c4e6ac0f-3475-42cb-8cfc-499282990a6b
Kyriienko, Oleksandr
7c3771ad-119f-4968-8285-81212337fdc4
Shelykh, Ivan
36ca7136-8728-4eb1-9e1c-2fbb0e7b0304
Gai, Lizhi
649e01f8-7ab7-4a01-9b98-33f3efbbdd17
Shen, Zhen
29a8d242-3a43-4a4e-a53b-f359182c7708
Lidzey, David
4c1f0189-29db-482f-896b-b90f28909baf
Lagoudakis, Pavlos
ea50c228-f006-4edf-8459-60015d961bbf
Yagafarov, Timur, Sannikov, Denis, Zasedatelev, Anton, Georgiou, Kyriacos, Baranikov, Anton, Kyriienko, Oleksandr, Shelykh, Ivan, Gai, Lizhi, Shen, Zhen, Lidzey, David and Lagoudakis, Pavlos
(2020)
Mechanisms of blueshifts in organic polariton condensates.
Communications Physics, 3 (1), [18].
(doi:10.1038/s42005-019-0278-6).
Abstract
Bose-Einstein condensates of exciton-polaritons in inorganic semiconductor microcavities are known to possess strong interparticle interactions attributed to their excitonic component. The interactions play a crucial role in the nonlinear dynamics of such systems and can be witnessed as the energy blueshifts of polariton states. However, the localised nature of Frenkel excitons in strongly coupled organic microcavities precludes interparticle Coulomb exchange-interactions that change mechanisms of the nonlinearity and blueshifts accordingly. In this report, we unravel the origins of blueshifts in organic polariton condensates. We examine the possible contributions: intracavity optical Kerr-effect, gain-induced frequency-pulling, polariton interactions and effects related to saturation of optical transitions for weakly- and strongly-coupled molecules. We conclude that blueshifts in organic polariton condensates arise from the interplay of the saturation effects and intermolecular energy migration. Our model predicts the commonly observed step-like increase of both the emission energy and degree of linear polarization at the polariton condensation threshold.
Text
s42005-019-0278-6
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Accepted/In Press date: 17 December 2019
Published date: 22 January 2020
Additional Information:
Funding Information:
We thank Professor Nikolay Gippius for helpful discussions. A.Z. and A.B. acknowledge financial support from the Russian Scientific Foundation (RSF) grant No. 18-72-00227. O.K. and I.S. acknowledge support from the Government of the Russian Federation (projects 14.Y26.31.0015 and 3.2614.2017/4.6) and ITMO Fellowship Program. We also acknowledge partial funding from the UK EPSRC via Programme Grant “Hybrid Polaritonics” EP/M025330/1.
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© 2020, The Author(s).
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Local EPrints ID: 438419
URI: http://eprints.soton.ac.uk/id/eprint/438419
ISSN: 2399-3650
PURE UUID: 8d05850b-5e91-49d4-b8fa-1107bc8aacae
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Date deposited: 09 Mar 2020 17:33
Last modified: 16 Mar 2024 06:49
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Contributors
Author:
Timur Yagafarov
Author:
Denis Sannikov
Author:
Kyriacos Georgiou
Author:
Anton Baranikov
Author:
Oleksandr Kyriienko
Author:
Ivan Shelykh
Author:
Lizhi Gai
Author:
Zhen Shen
Author:
David Lidzey
Author:
Pavlos Lagoudakis
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