Theoretical investigation of molecule-intense laser interactions using quantum chemical approaches

使用量子化学方法对分子强激光相互作用进行理论研究

• 批准号: 0855676
• 负责人: Xi Chu
• 金额: $ 18万
• 依托单位: University of Montana
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2009
• 资助国家: 美国
• 起止时间: 2009-09-01 至 2013-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0855676&HistoricalAwards=false
• 关键词: Theoretical; investigation; molecule; intense; laser

AbstractThis award is funded under the American Recovery and Reinvestment Act of 2009 (Public Law 111-5).Ultra-fast intense lasers can be developed into powerful tools for imaging electronic structures, probing ultra-fast dynamics, and controlling the electron population and molecular fragmentation. So far proof-of-principle experiments for these applications have been demonstrated for only a small number of molecules. Theoretical understanding of the intense laser-molecule interaction is crucial for the generalization of these applications and it has been limited to over-simplified models. This work explores quantum chemical (QC) methods for two important types of such interactions: multiphoton ionization and high harmonic generation. To properly treat them, the involvement of highly excited electronic states and many-electron effects have to be addressed. This is beyond conventional applications of the QC methods that treat only ground or low-lying excited states. A series of benchmark calculations will be performed to validate the methods and to identify the physics that dominates these processes. Possible improvement of the methods at theoretical level will be in collaboration with two European theoretical chemists. This project will have an impact in both strong field molecular physics and theoretical chemistry. It will help the development of new tools to study chemical reactions with state of the art lasers. In addition, it will also be integrated into the undergraduate physical chemistry education in the University of Montana. Junior year students will have their first experience with computational chemistry to enhance their understanding of electronic structure and matter-radiation field interactions.

摘要这一奖项是根据2009年的《美国回收与再投资法》（公法111-5）资助的。可以将激烈的激光发展为功能强大的工具，用于成像电子结构，探测超快速的动力学以及控制电子种群和分子碎片。到目前为止，仅针对少数分子证明了针对这些应用的原则实验。对强烈激光分子相互作用的理论理解对于这些应用的概括至关重要，并且它仅限于过度简化的模型。这项工作探讨了两种重要类型的这种相互作用的量子化学方法（QC）方法：多光子电离和高谐波产生。为了正确处理它们，必须解决高度激发的电子状态和许多电子效应的参与。这超出了QC方法的常规应用，该方法仅处理地面或低洼的激发态。将进行一系列基准计算以验证方法并确定主导这些过程的物理学。理论层面的方法可能会与两位欧洲理论化学家合作改善。该项目将对强场分子物理学和理论化学产生影响。它将有助于开发新工具，以使用最先进的激光研究化学反应。此外，它还将纳入蒙大拿大学的本科生化学教育。大三学生将首先拥有计算化学的经验，以增强他们对电子结构和物质辐射场相互作用的理解。