Electric Field-Induced Quenching of MAPbI3 Photoluminescence in PeLED Architecture.

Photoluminescence (PL) measurements are a widely used technique for the investigation of perovskite-based materials and devices. Although electric field-induced PL quenching provides additional useful information, this phenomenon is quite complex and not yet clearly understood. Here, we address the PL quenching of methylammonium lead iodide (MAPbI3) perovskite in a light-emitting diode (PeLED) architecture. We distinguish two quenching mechanisms: (a) indirect quenching by slow irreversible or partially reversible material changes that occur gradually under the applied light and electric field and (b) direct quenching by the influence of the electric field on the charge carrier densities, their spatial distributions, and radiative recombination rates. Direct quenching, observed under the abrupt application of negative voltage, causes a decrease of the PL intensity. However, the PL intensity then partially recovers within tens of milliseconds as mobile ions screen the internal electric field. The screening time increases to hundreds of seconds at low temperatures, indicating activation energies for ion motion of about 80 meV. On the other hand, ultrafast time-resolved PL measurements revealed two main phases of direct quenching: an instantaneous reduction in the radiative carrier recombination rate, which we attribute to the electron and hole displacement within individual perovskite grains, followed by a second phase lasting hundreds of picoseconds, which is due to the charge carrier extraction and spatial separation of electron and hole "clouds" within the entire perovskite layer thickness.