Hot-Hole Cooling Controls the Initial Ultrafast Relaxation in Methylammonium Lead Iodide Perovskite.

ABSTRACT: Understanding the initial ultrafast excited state dynamics of methylammonium lead iodide (MAPI) perovskite is of vital importance to enable its fullest utilisation in optoelectronic devices and the design of improved materials. Here we have combined advanced measurements of the ultrafast photoluminescence from MAPI films up to 0.6 eV above the relaxed excited state with cutting-edge advanced non-adiabatic quantum dynamics simulations, to provide a powerful unique insight into the earliest time behaviour in MAPI. Our joint experimental-theoretical approach highlights that the cooling of holes from deep in the valence band to the valence band edge is fast, occurring on a 100-500 fs timescale. Cooling of electrons from high in the conduction band to the conduction band edge, however, is much

SUBMITTER: Hedley GJ 

PROVIDER: S-EPMC5970208 | biostudies-literature | 2018 May

REPOSITORIES: biostudies-literature