1. Untargeted effects in organic exciton-polariton transient spectroscopy: A cautionary tale
- Author
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Andrew J. Musser, Lizhi Gai, Akshay Rao, Zhen Shen, Scott Renken, David G. Lidzey, Raj Pandya, Kyriacos Georgiou, and Rahul Jayaprakash
- Subjects
Physics ,Chemical Physics (physics.chem-ph) ,Exciton ,General Physics and Astronomy ,Physics::Optics ,FOS: Physical sciences ,02 engineering and technology ,021001 nanoscience & nanotechnology ,01 natural sciences ,Potential energy ,Photoexcitation ,Coupling (physics) ,Chemical physics ,Physics - Chemical Physics ,0103 physical sciences ,Ultrafast laser spectroscopy ,Polariton ,Transient (oscillation) ,Physical and Theoretical Chemistry ,010306 general physics ,0210 nano-technology ,Transient spectroscopy ,Physics - Optics ,Optics (physics.optics) - Abstract
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.
- Published
- 2021