A Spectroscopic Journey through Time and Space in Complex Electronic Materials

该提案利用了NSERC发现资助的纳米级材料超快激光光谱研究的15年。在这里，我们将把我们的状态/分辨泵浦/探针（SRPP）光谱方法扩展为统一的时间分辨光谱方法。我们开发了一套三种高性能超快光谱工具，包括二维电子（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能谱将应用于在时间上四个数量级和空间上三个数量级的复杂材料中展开电子过程。******该计划的目标是将一些最复杂的光谱工具应用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，并基于它们的相对成熟度和我们的历史专业知识来检查外来动力学。然后，我们将把研究扩展到目前全球舞台上最新和最引人注目的材料——卤化钙钛矿。我们将从已经开始合成的钙钛矿纳米晶体开始。这些材料代表了新材料基础科学以及这些思想在光电子新技术中的应用的全球领先优势。从长远来看，我们将朝着钙钛矿和过渡金属二硫族化物薄膜的方向发展。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带偏振控制的共线2DE光谱仪来探测。＊＊＊＊＊

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. *****