Nonlinear Optical Studies of Condensed Phase Dynamics

凝聚相动力学的非线性光学研究

• 批准号: 0706468
• 负责人: Graham Fleming
• 金额: $ 74.4万
• 依托单位: University of California-Berkeley
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2007
• 资助国家: 美国
• 起止时间: 2007-06-01 至 2011-05-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0706468&HistoricalAwards=false
• 关键词: Nonlinear; Optical; Studies; Condensed; Phase

Graham Fleming of the University of California-Berkeley is supported by the Experimental Physical Chemistry Program to carry out nonlinear optical studies of condensed phase dynamics. New methods to extend two-dimensional (2D) spectroscopic methods into the optical region will be developed, allowing 2D electronic spectroscopy with femtosecond time resolution. This technique, along with the simpler two-color photon echo peak shift technique, will enable the determination of electronic couplings and pathways of relaxation, reveal quantum aspects of ultrafast dynamics, and may enable electronic and spatial structure of molecular complexes to be directly connected. In addition, the nature and geometry of conical intersection seams, thought to control the products of many if not most ultrafast photochemical processes, can be accessed with 2D and combined visible/infrared spectroscopic experiments. The experimental technique involves the generation of independently tunable femtosecond light pulses and Fourier transform photon echo spectroscopy to record the full field of the third-order nonlinear response. Outcomes are expected to influence the understanding and design of molecular complexes and nanostructures for optoelectronic applications. Two-dimensional spectroscopic methods have proved extraordinarily powerful in nuclear magnetic resonance (NMR) spectroscopy, and have become an area of active development in the infrared spectral region for studying how molecules vibrate. The research supported here moves these techniques into the visible light region, creating new opportunities for the understanding of important chemical systems. As a result, critical information is expected to be provided for the design of highly efficient light harvesting devices for solar energy conversion, and the applications of single walled carbon nanotubes in opto-electronic devices. The studies of photochemical reactions are anticipated to influence the use of light-driven chemistry to produce high-value chemicals. This project as well will contribute to the US scientific infrastructure by providing state-of-the-art research training to young scientists at the undergraduate, graduate, and postdoctoral levels.

加州大学伯克利分校的Graham Fleming在实验物理化学项目的支持下进行了凝聚态动力学的非线性光学研究。将开发将二维（2D）光谱方法扩展到光学区域的新方法，使二维电子光谱具有飞秒时间分辨率。该技术与更简单的双色光子回波峰移技术一起，将能够确定电子耦合和弛豫途径，揭示超快动力学的量子方面，并可能使分子复合物的电子和空间结构直接连接。此外，锥形相交接缝的性质和几何形状，被认为可以控制许多（如果不是大多数）超快光化学过程的产物，可以通过二维和组合可见/红外光谱实验来访问。实验技术包括产生可独立调谐的飞秒光脉冲和傅立叶变换光子回波光谱来记录三阶非线性响应的全场。研究结果有望影响光电子应用中分子复合物和纳米结构的理解和设计。二维光谱方法在核磁共振波谱学中已经被证明是非常强大的，并且已经成为红外光谱区研究分子振动的一个积极发展的领域。这里支持的研究将这些技术转移到可见光区域，为理解重要的化学系统创造了新的机会。研究结果有望为设计高效的太阳能转换光收集装置以及单壁碳纳米管在光电器件中的应用提供重要信息。预计光化学反应的研究将影响光驱动化学生产高价值化学品的使用。该项目还将通过为本科生、研究生和博士后水平的年轻科学家提供最先进的研究培训，为美国的科学基础设施做出贡献。