M. Monti, K.D.G.I. Jayawardena, E. Butler-Caddle, R.M.I. Bandara, J.M. Woolley, M. Staniforth, S.R.P. Silva and J. Lloyd-Hughes
Phys. Rev. B 102 245204 (Dec 2020) [ pdf ] [ ref ]

The electron-phonon interaction controls the intrinsic mobility of charges in metal halide perovskites, and determines the rate at which carriers lose energy. Here, the carrier mobility and cooling dynamics were directly examined using a combination of ultrafast transient absorption spectroscopy and optical pump, THz probe spectroscopy, in perovskites with different lead and tin content, and for a range of carrier densities. Significantly, the carrier mobility in the “hot phonon bottleneck” regime, where the LO phonon bath keeps carriers warm, was found to be similar to the mobility of cold carriers. A model was developed that provides a quantitative description of the experimental carrier cooling dynamics, including electron-phonon coupling, phonon-phonon coupling and the Auger mechanism. In the Pb and Sn alloy the duration of the hot carrier regime was extended as a result of the slower decay of optical phonons. The findings offer an intuitive link between macroscopic properties and the underlying microscopic energy transfer processes, and suggest new routes to control the carrier cooling process in metal halide perovskites to optimize optoelectronic devices.