The behavior of hot carriers in metal-halide perovskites (MHPs) present a
valuable foundation for understanding the details of carrier-phonon coupling in
the materials as well as the prospective development of highly efficient hot
carrier and carrier multiplication solar cells. Whilst the carrier population
dynamics during cooling have been intensely studied, the evolution of the hot
carrier properties, namely the hot carrier mobility, remain largely unexplored.
To address this, we introduce a novel ultrafast visible pump - infrared push -
terahertz probe spectroscopy (PPP-THz) to monitor the real-time conductivity
dynamics of cooling carriers in methylammonium lead iodide. We find a decrease
in mobility upon optically depositing energy into the carriers, which is
typical of band-transport. Surprisingly, the conductivity recovery dynamics are
incommensurate with the intraband relaxation measured by an analogous
experiment with an infrared probe (PPP- IR), and exhibit a negligible
dependence on the density of hot carriers. These results and the kinetic
modelling reveal the importance of highly-localized lattice heating on the
mobility of the hot electronic states. This collective polaron-lattice
phenomenon may contribute to the unusual photophysics observed in MHPs and
should be accounted for in devices that utilize hot carriers.