Probing dynamics in perovskite nanocrystals with quantum confinement and doping

半导体钙钛矿自2014年在光伏薄膜中取得巨大的初步表现以来，迅速出现在材料科学领域。这些钙钛矿是目前科学领域最热门的材料之一，因为它们在光电应用和新物理方面具有前景。在这个提议中，我们将首次遵循整个生命周期，从最初的极化子形成，到激子形成，到激子热化，再到新的钙钛矿纳米晶体中的激子发射，使用一套三种最先进的光谱，由一个独一无二的超快光谱实验室实现。利用二维电子光谱（2DE）、状态分辨泵浦/探针（SRPP）光谱和时间分辨光致发光（t-PL）光谱这三种工具，我们将监测一套新型钙钛矿体系中电子激发的动力学诞生、量子动力学演化和热力学消亡的各个方面。在我们对块状钙钛矿纳米晶体的初步研究之后，我们将与Dong Hee Son （Texas A&M）合作，探索他们最新的钙钛矿，包括量子点钙钛矿和原子掺杂钙钛矿。这项工作的影响将是对几十年来最新和最引人注目的光电材料中结构-功能关系的理解。我们的竞争优势是我们拥有世界领先的超快激光光谱设备和我们在量子点超快激子动力学方面15年的专业知识。我们与DH Son集团建立了一个高知名度的国际合作伙伴关系，这将使我们的团队能够发现级科学，并学习新的材料系统。这项合作将加强加拿大的国际研究网络，为加拿大研究人员带来新科学，并为HQP提供增值培训。

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.