Chemical Dynamics at Solid Surfaces

固体表面的化学动力学

• 批准号: 0075744
• 负责人: John Tully
• 金额: $ 45.83万
• 依托单位: Yale University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2000
• 资助国家: 美国
• 起止时间: 2000-08-01 至 2003-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0075744&HistoricalAwards=false
• 关键词: Chemical; Dynamics; Solid; Surfaces

John Tully of Yale University is supported by the Theoretical and Computational Chemistry Program for research that focuses on the atomic-level understanding of dynamical processes at solid surfaces. New theoretical and computational tools will be created and used to study specific chemical problems in three areas. First, dynamics at metal surfaces will be explored to enable prediction of the contribution of electron-hole pair transitions to adsorbate energy transfer. Methods for computing the relative intensities of vibrational modes and approximate propensity rules in scanning tunneling microscopy (STM) will be developed. Second, mixed quantum-classical dynamics will be developed with the goal of extending conventional molecular dynamics simulations to practical applications involving electronic transitions and/or quantum nuclear motion. Finally, ab initio methods for computing energies and lifetimes of adsorbate excited states at semiconductor and metal surfaces will be developed and tested, then extended to calculating energies and widths of adsorbate-ion resonance states and excited states. Understanding molecule and electron behavior on solid surfaces is important for gaining insights needed to drive innovations in technologically important areas such as semiconductor processing. Outcomes from this research are expected to impact a variety of important chemical applications, including the determination of molecular identity from observed topographical features in STM, and the understanding of multi-dimensional processes such as those involved in electrochemistry, condensed phase dynamics, and enzyme reactions.

耶鲁大学的John Tully得到了理论和计算化学项目的支持，其研究重点是对固体表面动力学过程的原子级理解。 新的理论和计算工具将被创建并用于研究三个领域的特定化学问题。 首先，在金属表面的动力学将被探索，使预测的电子-空穴对跃迁的吸附质能量转移的贡献。 将发展计算扫描隧道显微镜（STM）中振动模式的相对强度和近似倾向规则的方法。 第二，将开发混合量子-经典动力学，目标是将传统的分子动力学模拟扩展到涉及电子跃迁和/或量子核运动的实际应用。 最后，从头计算方法计算的能量和寿命的吸附物激发态在半导体和金属表面将开发和测试，然后扩展到计算能量和宽度的吸附离子共振态和激发态。 了解固体表面上的分子和电子行为对于获得推动半导体加工等重要技术领域创新所需的洞察力非常重要。 这项研究的结果预计将影响各种重要的化学应用，包括从STM中观察到的地形特征确定分子身份，以及了解多维过程，如电化学，凝聚相动力学和酶反应中涉及的过程。