A Spectroscopic Journey through Time and Space in Complex Electronic Materials

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This proposal leverages 15 years of NSERC Discovery funded research on ultrafast laser spectroscopy of nanoscale materials. Here, we will take our state/resolved pump/probe (SRPP) spectroscopic approach and expand it into a unified approach for time resolved spectroscopy. We have developed a suite of three high-performance ultrafast spectroscopy tools - Two-Dimensional Electronic (2DE) spectroscopy, time-resolved photoluminescence (t-PL) spectroscopy, and our SRPP spectroscopy. These three forms of time-resolved electronic spectroscopy will be applied towards unraveling electronic processes in complex materials over four orders of magnitude in time and three orders of magnitude in space. The objective of this program is to apply some of the most sophisticated spectroscopic tools in existence to three classes of materials that are at the global center of nanoscale materials science. We will focus first on CdSe Semiconductor Quantum dots as they form a model system for the development of new spectroscopies and the examination of exotic dynamics based upon their relative maturity and our historic expertise. We will then extend the studies to the newest and most compelling materials in the global stage now - lead halide perovskites. We will begin with perovskite nanocrystals which we have begun to synthesize. These materials represent the global leading edge for the basic science of new materials and for the application of these ideas to new technologies in optoelectronics. In the long term we will move towards thin films of perovskites and transition metal dichalchogenides. These two dimensional materials offer interesting anisotropies that we are uniquely poised to probe with our one of a kind collinear 2DE spectrometer with polarization control.