Strong light–matter coupling to form exciton– and vibropolaritons is increasingly touted as a powerful tool to alter the fundamental properties of organic materials. It is proposed that these states and their facile tunability can be used to rewrite molecular potential energy landscapes and redirect photophysical pathways, with applications from catalysis to electronic devices. Crucial to their photophysical properties is the exchange of energy between coherent, bright polaritons and incoherent dark states. One of the most potent tools to explore this interplay is transient absorption/reflectance spectroscopy. Previous studies have revealed unexpectedly long lifetimes of the coherent polariton states, for which there is no theoretical explanation. Applying these transient methods to a series of strong-coupled organic microcavities, we recover similar long-lived spectral effects. Based on transfer-matrix modeling of the transient experiment, we find that virtually the entire photoresponse results from photoexcitation effects other than the generation of polariton states. Our results suggest that the complex optical properties of polaritonic systems make them especially prone to misleading optical signatures and that more challenging high-time-resolution measurements on high-quality microcavities are necessary to uniquely distinguish the coherent polariton dynamics.
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21 October 2021
Research Article|
October 15 2021
Untargeted effects in organic exciton–polariton transient spectroscopy: A cautionary tale
Special Collection:
2021 JCP Emerging Investigators Special Collection
Scott Renken;
Scott Renken
1
Department of Chemistry and Chemical Biology, Cornell University
, Ithaca, New York 14853, USA
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Raj Pandya
;
Raj Pandya
2
Cavendish Laboratory, University of Cambridge
, JJ Thomson Avenue, CB3 0HE Cambridge, United Kingdom
3
Laboratoire Kastler Brossel, École Normale Superiéure-Université PSL, CNRS, Sorbonne Université, College de France
, Paris 75005, France
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Kyriacos Georgiou
;
Kyriacos Georgiou
4
Department of Physics and Astronomy, University of Sheffield
, Sheffield, United Kingdom
5
Department of Physics, University of Cyprus
, P.O. Box 20537, Nicosia 1678, Cyprus
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Rahul Jayaprakash
;
Rahul Jayaprakash
4
Department of Physics and Astronomy, University of Sheffield
, Sheffield, United Kingdom
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Lizhi Gai;
Lizhi Gai
6
Key Laboratory of Organosilicon Chemistry and Material Technology, Ministry of Education, Hangzhou Normal University
, Hangzhou 311121, China
7
State Key Laboratory of Coordination and Chemistry, School of Chemistry and Chemical Engineering, Nanjing University
, Nanjing 210046, China
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Zhen Shen
;
Zhen Shen
7
State Key Laboratory of Coordination and Chemistry, School of Chemistry and Chemical Engineering, Nanjing University
, Nanjing 210046, China
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David G. Lidzey
;
David G. Lidzey
4
Department of Physics and Astronomy, University of Sheffield
, Sheffield, United Kingdom
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Akshay Rao
;
Akshay Rao
2
Cavendish Laboratory, University of Cambridge
, JJ Thomson Avenue, CB3 0HE Cambridge, United Kingdom
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Andrew J. Musser
Andrew J. Musser
a)
1
Department of Chemistry and Chemical Biology, Cornell University
, Ithaca, New York 14853, USA
a)Author to whom correspondence should be addressed: ajm557@cornell.edu
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a)Author to whom correspondence should be addressed: ajm557@cornell.edu
Note: This paper is part of the 2021 JCP Emerging Investigators Special Collection.
J. Chem. Phys. 155, 154701 (2021)
Article history
Received:
July 12 2021
Accepted:
September 29 2021
Citation
Scott Renken, Raj Pandya, Kyriacos Georgiou, Rahul Jayaprakash, Lizhi Gai, Zhen Shen, David G. Lidzey, Akshay Rao, Andrew J. Musser; Untargeted effects in organic exciton–polariton transient spectroscopy: A cautionary tale. J. Chem. Phys. 21 October 2021; 155 (15): 154701. https://doi.org/10.1063/5.0063173
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