Fundamental Studies of the Hydrogen-Atom Hydrogen-Molecule Exchange Reaction

斯坦福大学化学结构、动力学和机理（CSDM-A）项目资助了斯坦福大学Zare教授和他的研究生和博士后，他们通过控制碰撞能量和识别产物的详细状态来研究H + H2反应的动力学。该系统可以进行最精确的全量子力学和准经典轨迹计算，并与实验进行比较。本研究可以显著加深我们对该反应的理解，特别是对强红外激光场中几何相位效应和其他非绝热效应、矢量相关性以及势面变化的影响的理解。从这个简单反应中获得的知识可能适用于理解更复杂的反应。Zare和他的研究小组产生的氢原子具有足够的动能，可以超过H3系统的定义良好的锥形交叉点，在那里，Born-Oppenheimer近似预计会失效，这意味着相互作用发生在多个势能表面上。在另一个子项目中，通过使用强烈的非谐振红外激光场来操纵势能面，试图控制碰撞过程。这可以从实验上证明光子催化化学反应的可能性。

In this award, funded by the Chemical Structure, Dynamics and Mechanisms (CSDM-A) Program of the Division of Chemistry, Professor Zare of Stanford University and his graduate student and postdoc are investigating the dynamics of the H + H2 reaction by controlling the collision energies and by identifying the detailed states of the products. The most accurate full quantum mechanical and quasiclassical trajectory calculations can be done for this system to compare with experiments. This research may significantly deepen our understanding of this reaction, in particular, the geometric phase effect and other nonadiabatic effects, vector correlations, and the effects of a change in the potential surface in an intense infrared laser field. The knowledge obtained for this simple reaction may be applicable to understanding more complex reactions.Prof. Zare and his research group generates hydrogen atoms with sufficient kinetic energy to go above the well-defined conical intersection of the H3 system where the Born-Oppenheimer approximation is expected to break down, meaning the interactions take place on more than one potential energy surface. For another subproject, the potential energy surface is manipulated by using an intense off-resonant infrared laser field in an attempt to control the collision process. This may demonstrate experimentally the possibility of photon catalysis of a chemical reaction.