A Spectroscopic Journey through Time and Space in Complex Electronic Materials

该提案利用了15年的NSERC Discovery资助的纳米材料超快激光光谱学研究。在这里，我们将采取我们的状态/分辨泵浦/探测（SRPP）光谱方法，并将其扩展为时间分辨光谱的统一方法。我们已经开发了一套三个高性能的超快光谱工具二维电子（2DE）光谱，时间分辨光致发光（t-PL）光谱，和我们的SRPP光谱。这三种形式的时间分辨电子光谱将被应用于解开复杂材料中的电子过程，时间上超过四个数量级，空间上超过三个数量级。** 该计划的目标是将现有的一些最复杂的光谱工具应用于处于纳米材料科学全球中心的三类材料。我们将首先关注CdSe半导体量子点，因为它们形成了一个模型系统，用于开发新的光谱学和基于其相对成熟度和我们的历史专业知识的外来动力学检查。然后，我们将研究扩展到全球舞台上最新和最引人注目的材料，现在是铅卤化物钙钛矿。我们将开始与钙钛矿纳米晶体，我们已经开始合成。这些材料代表了新材料基础科学以及将这些想法应用于光电子新技术的全球领先优势。从长远来看，我们将转向钙钛矿和过渡金属二硫属化物的薄膜。这些二维材料提供了有趣的各向异性，我们独特地准备用我们的一种具有偏振控制的共线2DE光谱仪进行探测。 *****

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. *****