Ultrafast nonequilibrium dynamics of strongly coupled resonances in the intrinsic cavity of WS_{2} nanotubes

Abstract

Strong coupling of electric transition dipoles with optical or plasmonic resonators modifies their light-matter interaction and, therefore, their optical spectra. Semiconducting WS_{2} nanotubes intrinsically provide the dipoles through their excitonic resonances, and the optical cavity via their cylindrical shape. We investigate the nonequilibrium light-matter interaction in WS_{2} nanotubes in the time domain using femtosecond transient extinction spectroscopy. We develop a phenomenological coupled oscillator model with time-dependent parameters to describe the transient extinction spectra, allowing us to extract the underlying nonequilibrium electron dynamics. We find that the exciton and trion resonances shift due to many-body effects of the photogenerated charge carriers and their population dynamics on the femto- and picosecond timescale. Our results show that the time-dependent phenomenological model quantitatively reproduces the nonequilibrium optical response of strongly coupled systems.