Ultrafast Dynamics of Electronic Excited States: Photocatalysis and Photomagnetism

电子激发态的超快动力学：光催化和光磁性

• 批准号: 1300239
• 负责人: Kevin Kubarych
• 金额: $ 42万
• 依托单位: Regents of the University of Michigan - Ann Arbor
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-10-01 至 2016-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1300239&HistoricalAwards=false
• 关键词: Ultrafast; Dynamics; Electronic; Excited; States

In this project funded by the Chemical Structure, Dynamics, and Mechanisms Program-A (CSDM-A) and the Chemical Instrumentation Program of Division of Chemistry, Professor Kevin J. Kubarych of the University of Michigan and his graduate and undergraduate students are addressing the fundamental relationships between structure, dynamics and function in molecules that, powered by light, are poised to dramatically reshape approaches to transforming carbon dioxide and to storing information. In both classes of system, photocatalysts for reduction of carbon dioxide, and photomagnets, the key chemical starting point involves molecules that have absorbed light, carrying out their initial functional steps in excited electronic states. Using novel experimental techniques based on ultrafast two-dimensional infrared (2D-IR) spectroscopy and related methods, Professor Kubarych and his group will obtain the level of detailed dynamical information on the active excited states that is presently only possible on ground state molecules. By employing novel pulse sequences that combine different spectral ranges such as the visible and infrared, including multiple laser sources permitting access to timescales ranging from femtoseconds to seconds, Professor Kubarych's team will be able to disentangle complex photocycles and identify transient intermediate species using the powerful resolution of 2D-IR spectroscopy. With the addition of low-temperature capabilities, the group will gain access to the cooperative ultrafast dynamics of photoswitchable magnetic molecules and materials, which they will examine using novel hybrid electronic/vibrational spectroscopy methods. The long term goal of this research project is to address the clear societal need to develop new approaches for energy conversion, storage, as well as the removal of greenhouse gases. Results of this project will guide development of new chemical systems as well as macromolecular constructs by elucidating the fundamental design principles. Professor Kubarych will leverage the widespread interest in energy, technology, and climate change to appeal to the next generation of women and minority scientists by developing hands-on demonstrations of dye-sensitized solar cells for middle and high school students in the southeast Michigan area. To dramatically broaden his reach, he will produce videos and a web resource describing basic challenges in solar energy conversion, highlighting the role of physical chemistry in the development of new solutions.

In this project funded by the Chemical Structure, Dynamics, and Mechanisms Program-A (CSDM-A) and the Chemical Instrumentation Program of Division of Chemistry, Professor Kevin J. Kubarych of the University of Michigan and his graduate and undergraduate students are addressing the fundamental relationships between structure, dynamics and function in molecules that, powered by light, are poised to dramatically reshape approaches to transforming carbon dioxide and to存储信息。在这两类系统中，用于还原二氧化碳和光磁体的光催化剂，关键的化学起点涉及吸收光吸收光的分子，在激发电子状态下执行其初始功能步骤。 Kubarych教授及其小组使用基于超快二维红外（2D-IR）光谱和相关方法的新型实验技术，将获得有关主动激发态的详细动力学信息的水平，目前仅在基态分子上才有可能。通过采用结合不同频谱范围（例如可见光和红外线）的新型脉冲序列，包括多个激光源，允许访问从飞秒到几秒钟的时间表，Kubarych教授的团队将能够使用2D-IR光谱镜的强大分辨率识别复杂的复杂光型并识别瞬时中介物种。随着添加低温功能，该组将访问可拍摄的磁分子和材料的合作超快动力学，他们将使用新型混合电子/振动光谱法检查它们。该研究项目的长期目标是满足开发能源转化，存储以及去除温室气体的新方法的明确社会需求。该项目的结果将通过阐明基本设计原理来指导新的化学系统以及大分子结构的开发。 Kubarych教授将通过为密歇根州东南部地区的中学和高中生开发动手演示，利用对能源，技术和气候变化的广泛兴趣吸引下一代妇女和少数民族科学家。为了极大地扩大自己的影响力，他将制作视频和网络资源，描述太阳能转化的基本挑战，强调物理化学在新解决方案开发中的作用。