CAREER: Coupled Electron-Proton Dynamics at Photocatalytic Interfaces

有了这个职业奖，化学系的化学结构，动力学和机制（CSDM-A）计划资助南加州大学的Jahan Dawlaty教授和他的博士后，研究生和本科生同事进行实验研究，旨在了解质子和电子的运动是如何在界面处的光催化反应中耦合的。 在这些反应中，质子和电子运动的耦合被认为有助于使这些反应更容易发生。 光催化反应在生物学（光合作用）和化学工程（太阳能燃料的生产）等不同领域都很重要。 从事该项目的博士后，研究生和本科生将接受最先进的激光和光学科学，光谱学以及复杂实验设计方面的培训，同时研究具有重大现实影响的重要化学问题。 从事该项目的年轻研究人员将接受激光科学和现代光谱方法方面的优秀技术培训，为现代科学劳动力做好准备。 在这个CAREER奖的教育目标下，Dawlaty教授将建立简单的物理模型来说明重要的物理化学原理。Jahan Dawlaty教授和他的研究小组将使用超快激光技术来研究质子耦合电子转移的界面化学。 他将使用光谱技术来测量光催化过程中电子和质子的同步运动。 在该奖项支持的实验中，Dawlaty的小组将研究：（1）无定形氧化锰表面;（2）赤铁矿表面和（3）硅功能化表面。 这些反应将使用各种表面敏感光谱方法进行探测，包括二维电子振动相关光谱。从拟议的工作，一个新的理解表面氧化还原反应，其中质子是免费的波恩-奥本海默近似有望出现。从长远来看，这项工作旨在指导具有光可控质子活性的界面的设计，这是一个新概念，有可能揭示多电子和多质子表面氧化还原反应的机理细节。

With this CAREER award, the Chemical Structure, Dynamics and Mechanisms (CSDM-A) Program of the Division of Chemistry is funding Professor Jahan Dawlaty of the University of Southern California and his post-doctoral, graduate and undergraduate student colleagues to conduct experimental studies aimed at understanding how the motions of protons and electrons are coupled in photocatalytic reactions at interfaces. The coupling of proton and electron motion in these reactions is believed to help to make these reactions take place more readily. Photocatalytic reactions are important in realms as diverse as biology (photosynthesis) and chemical engineering (production of solar fuels). Post-doctoral, graduate and undergraduate students working on this project will receive training in state-of-the-art laser and optical science, spectroscopy, and the design of complex experiments, while working on important chemical problems with significant real-world impact. The young researchers working on this project will receive excellent technical training in laser science and modern spectroscopic methods which will prepare them for the modern scientific workforce. Under the educational aims of this CAREER award, Prof. Dawlaty will build simple physical models to illustrate important physical chemical principles.Prof. Jahan Dawlaty and his research group will use ultrafast laser techniques to study the interfacial chemistry of proton-coupled electron transfer. He will use spectroscopic techniques to measure the synchronous motion of electrons and protons during photocatalytic events. In the experiments supported with this award Dawlaty's group will study: (1) amorphous manganese oxide surfaces; (2) hematite surfaces and (3) and silicon functionalized surfaces. The reactions will be probed using a variety of surface-sensitive spectroscopic methods, including two-dimensional electronic-vibrational correlation spectroscopy. From the proposed work, a new understanding of surface redox reactions, where protons are free from the Born-Oppenheimer approximation is expected to emerge. In the longer term, the work is aimed at guiding the design of interfaces with light-controllable proton activity is a new concept that has potential to unravel the mechanistic details of multi-electron and multi-proton surface redox reactions.