Efficient Intraband Hot Carrier Relaxation in the Perovskite Semiconductor Cs1-xRbxSnI3 Mediated by Strong Electron-Phonon Coupling

The dynamic increase in terahertz photoconductivity resulting from energetic intraband relaxation was used to track the formation of highly mobile charges in thin films of the tin iodide perovskite Cs1-xRbxSnI3, with x = 0 and 0.1. Energy relaxation times were found to be around 500 fs, comparable to those in the prototypical inorganic semiconductor GaAs. At low excess energies, the efficient intraband energy relaxation in the lowest conduction and valence bands of Cs1-xRbxSnI3 can be understood within the context of the Frohlich electron-phonon interaction, with a strong coupling strength. For higher excess energies, the photoconductivity rise time lengthens in accordance with carrier injection into multiple bands, identified by quantitative first-principles bandstructure calculations and photoluminescence spectroscopy. The findings contribute to the development of design rules for photovoltaic devices capable of extracting hot carriers from perovskite semiconductors.