Partially-Bright Triplet Excitons in Perovskite Nanocrystals

Abstract: Advances in opto-electronics require the development of materials with novel and engineered characteristics. A class of materials that has garnered tremendous interest is metal-halide perovskites, stimulated by meteoric increases in photovoltaic efficiencies of perovskite solar cells. In addition, recent advances have applied perovskite nanocrystals (NCs) in light-emitting devices. It was discovered recently that, for cesium lead-halide perovskite NCs, their unusually efficient light-emission may be due to a unique excitonic fine-structure composed of three bright triplet states that minimally interact with a proximal dark singlet state. To study this fine-structure without isolating single NCs, we use multi-dimensional coherent spectroscopy at cryogenic temperatures to reveal coherences involving triplet states of a CsPbI$_3$ NC ensemble. Picosecond timescale dephasing times are measured for both triplet and inter-triplet coherences, from which we infer a unique exciton fine-structure level-ordering comprised of a dark state energetically positioned within the bright triplet manifold.