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• W4229082488 abstract "Strong light–matter coupling results in eigenstates called polaritons which share the properties of both light and matter and provide a useful way to engineer electronic energies and behaviors. In this work, we study nearly monochiral (6,5) semiconducting carbon nanotubes (CNTs) in a Fabry–Pérot microcavity. Light–matter coupling leads to the formation of three bands of bright polariton states (upper, middle, and lower─resulting from coupling to the bright S11 CNT exciton and the X1 phonon sideband of the K-momentum dark exciton state). The structure also supports many exciton-like subradiant states at the bright S11 and X1 energies. Here, ultrafast transient reflection spectroscopy is used to study the dynamics and spectral signatures of excited subradiant-state polariton populations and the pathways by which they are populated. After a pump pulse, the excited subradiant-state population is revealed by (i) spectral signatures with relaxation times (∼5 ps) similar to those of CNT S11 band gap excitons outside of the cavity and (ii) a Rabi contraction of the lower polariton energy, whose magnitude quantifies the excited subradiant-state population. Data show that, following the excitation of the upper polariton (UP), the excited subradiant-state population is maximized at a sample position with a detuning of 118 meV, light–matter coupling of 336 meV, and UP transition energy of 1.52 eV. The excited subradiant-state population is reduced for other detunings. The X1 Hopfield coefficient of the UP also peaks at the same energy, revealing UP to X1 scattering as a potentially efficient relaxation pathway. These results will be important for understanding and controlling energy relaxation and transport in future CNT polariton devices." @default.
• W4229082488 created "2022-05-08" @default.
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• W4229082488 date "2022-05-06" @default.
• W4229082488 modified "2023-09-23" @default.
• W4229082488 title "Population of Subradiant States in Carbon Nanotube Microcavities in the Ultrastrong Light–Matter Coupling Regime" @default.
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• W4229082488 doi "https://doi.org/10.1021/acs.jpcc.2c02076" @default.
• W4229082488 hasPublicationYear "2022" @default.
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