Oxide Perovskites for Thermally Enhanced Solar Energy Conversion

以下研究建议旨在提供一个基本的理解，如何掺杂剂和缺陷（包括无关的能量和结构无序）可以修改主族金属氧化物钙钛矿，如缺氧BaSnO 3-x，具有光学活性价ns2孤对态的电子结构和电荷传输特性。该项目提供了基础能源材料理论，先进的光谱表征和设备演示的特殊组合。该项目的主要目标之一是解决目前对工程金属氧化物半导体中电荷传输的理解中的某些争议，这些争议通常偏离适用于经典晶体吸收材料的典型带状模型。以相对高的浓度（1 - 10mol%）将特定的掺杂剂和/或缺陷添加到氧化物钙钛矿中可以导致增加的峰值电荷载流子迁移率、适度的载流子浓度（通过补偿），并且错误地产生具有相对强的光学跃迁的中间带隙状态。这种工程工艺有可能大大提高氧化物半导体的光电性能。将使用最先进的实验和理论方法相结合，包括先进的化学沉积和器件制造，深入的材料表征，光电化学/催化分析，以及能量和时间依赖光谱。这项研究的一个独特的方面是表征温度依赖性的载流子动力学提供了一个准确的mechanisticunderstanding热激活电荷输运在氧化物材料考虑动态无序模型.随后，Weim将展示太阳能热集成如何作为一种创新策略，以提高基于氧化物的光催化和光伏（PV）系统的性能，使高效的太阳能转换高达10%。

The following research proposal is aimed at providing a fundamental understanding of how dopants and defects (including theirrespective energetic and structural disorder) can modify the electronic structure and charge transport properties of main group metaloxide perovskites, such as oxygen-deficient BaSnO3-x, which possess optically active valent ns2 lone pair states. This project offers anexceptional combination of fundament energy materials theory, advanced spectroscopic characterization, and devicedemonstrations. One of the main goals of the project is to resolve certain controversies in the current understanding of chargetransport in engineered metal oxide semiconductors, which often deviate from the typical band-like models applied to classicalcrystalline absorber materials. Adding specific dopants and/or defects into oxide perovskites, at relatively high concentrations (1-10mol %) can lead to increased peak charge carrier mobilities, moderate carrier concentrations (via compensation), and simultaneouslygenerate mid-band gap states with relatively strong optical transitions. This engineering process has the potential to substantiallyenhance the optoelectronic performance of the oxide semiconductors. A combination of state-of-the-art experimental andtheoretical approaches will be used, including advanced chemical deposition and device fabrication, in-depth materialscharacterization, photo-electrochemical/catalytic analysis, and energy and time dependant spectroscopy. A unique aspect of thisresearch is the characterization of temperature-dependent charge carrier dynamics to provide an accurate mechanisticunderstanding of thermally activated charge transport in oxide materials by considering dynamic disorder models. Subsequently, weaim to demonstrate how solar thermal integration can act as an innovative strategy to enhance the performance of oxide basedphotocatalytic and photovoltaic (PV) systems for efficient solar energy conversion up to 10%.