期刊
JOURNAL OF CHEMICAL PHYSICS
卷 155, 期 15, 页码 -出版社
AIP Publishing
DOI: 10.1063/5.0063173
关键词
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资金
- Engineering and Physical Sciences Research Council, UK [EP/M025330/1]
- EPSRC
- Winton Program for the Physics of Sustainability
- European Research Council (ERC) under the European Union's Horizon 2020 research and innovation programme [758826]
- EPSRC [EP/M025330/1] Funding Source: UKRI
Strong light-matter coupling to form exciton- and vibropolaritons can alter the fundamental properties of organic materials, with potential applications in catalysis and electronic devices. Optical complexity makes polaritonic systems prone to misleading optical signatures, necessitating high-time-resolution measurements for unique characterization of coherent polariton dynamics.
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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