Unraveling the excitonics of light emission from metal-halide perovskite quantum dots

Abstract

Metal halide semicondictor perovskites have been under intense investigation for their promise in light absorptive applications like photovoltaics. They have more recently experienced interest for their promise in light emissive applications. A key aspect of perovskites is their glassy, ionic lattice that exhibits dynamical disorder. One possible result of this dynamical disorder is their strong coupling between electronic and lattice degrees of freedom which may confer remarkable properties for light emission such as defect tolerance. How does the system, comprised of excitons, couple to the bath, comprised of lattice modes? How does this system-bath interaction give rise to novel light emissive properties and how do these properties give insight into the nature of these materials? We review recent work from this group in which time-resolved photoluminescence spectroscopy is used to reveal such insights. Based upon a fast time resolution of 3 ps, energy resolution, and temperature dependence, a wide variety of insights are gleaned. These insights include: lattice contributions to the emission linewidths, multiexciton formation, hot carrier cooling, excitonic fine structure, single dot superradiance, and a breakdown of the Condon approximation, all due to complex structural dynamics in these materials.