Probing dynamics in perovskite nanocrystals with quantum confinement and doping

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Semiconductor perovskites have rapidly emerged onto the materials science scene since their tremendous initial performance in photovoltaic films in 2014. These perovskites are among the hottest materials in science now for their promise in optoelectronic applications and their new physics. In this proposal we will for the first time follow the full Life Cycle spanning birth of an excitation from initial polaron formation, to exciton formation, to exciton thermalization, to excitonic emission in new perovskite nanocrystals using a suite of three state-of-the-art spectroscopies, made uniquely possible by a one-of-a-kind ultrafast spectroscopy lab. With these three tools of two dimensional electronic spectroscopy (2DE), state-resolved pump/probe (SRPP) spectroscopy, and time-resolved photoluminescence (t-PL) spectroscopy we will monitor all aspects of the dynamical birth, quantum-kinetic evolution, and thermodynamic death of an electronic excitation in a set of novel perovskite system. Following our initial work on bulk perovskite nanocrystals, we will collaborate with Dong Hee Son (Texas A&M) to probe their newest perovskites including quantum dot perovskites and atomically doped perovskites. The impact of this work will be an understanding of structure-function relationships in the newest and most compelling of optoelectronic materials in decades. Our competitive advantage is our world leading ultrafast laser spectroscopy facilities and our prior 15 years expertise in ultrafast exciton dynamics in quantum dots. With the DH Son group we establish a high profile international partnership that will enable discovery grade science and for our group to learn new materials systems. This collaboration will strengthen Canadian international research networks and bring new science to Canadian researchers and provide value added training to HQP.