Chemical Dynamics at Solid Surfaces

耶鲁大学的John Tully教授得到了理论和计算化学项目的支持，研究固体表面的化学动力学。 这项研究的目的是推进原子的理解在固体表面的动力学过程。 新的理论被开发，方法论被计算地实现。重点是模拟表面的光化学过程是由电子激发介导的。重点是理解振动隧穿和零点运动如何影响这些过程。 开发了用于加速与非平衡化学反应相关的罕见事件的模拟的方法。这些计算依赖于密度泛函理论和传统的量子化学方法的使用。原子的运动和反应可以平稳地发展，但也可能涉及与电子跃迁和光的吸收或发射相关的不连续过程。这样的过程可能无法用经典势来建模，需要理解电子和振动过程，以及描述电子之间的相互作用，振动自由度和光的能力。 这种相互作用与催化活性、材料加工、生物物理学和光化学密切相关。 了解这种相互作用也是相关的问题，如古代文物的材料的无损评估。一个旨在包括本科生在这样的努力计划是包括在这项研究计划。

Professor John Tully, of Yale University, is supported by the Theoretical and Computational Chemistry program to study chemical dynamics at solid surfaces. The objective of this research is to advance the atomistic understanding of dynamical processes at solid surfaces. New theories are developed and methodologies are implemented computationally. The focus is on the simulation of those photochemical processes at surfaces that are mediated by electronic excitations. There is an emphasis on understanding how vibrational tunneling and zero point motion affect such processes. Methods for accelerating the simulation of rare events associated with non-equilbrium chemical reactions are developed. These calculations rely on the use of density functional theory and conventional quantum chemistry methods.Atomistic motions and reactions can evolve smoothly but may also involve discontinuous processes that are associated with electronic transitions and absorption or emission of light. Such processes may not be modeled with classical potentials and require an understanding of both electronic and vibrational processes as well as the ability to describe interactions between electrons, vibrational degrees of freedom, and light. Such interactions are strongly relevant to catalytic activity, materials processing, biophysics and photochemistry. Understanding of such interactions is also relevant to the problem of nondestructive evaluation of materials such as ancient artifacts. A program aimed at including undergraduates in such endeavors is included in this research initiative.