Classical and Semiclassical Mechanics of Molecules

这项研究涉及分子束缚态和分子内动力学的经典和半经典理论。许多新的实验技术现在能够以前所未有的细节探索分子的高激发振动和振动-旋转态的性质，这种实验的解释对理论提出了严峻的挑战。本工作旨在通过统一处理高激发态的光谱和动力学来解决这些理论问题。多维系统半经典量子化的实用有效方法有待发展，这些方法和其他方法将被用于研究当前实验感兴趣的小分子的静力学和动力学。这一基础研究在理论和计算化学中的意义在于，它有助于详细了解能量在分子内流动的方式，以及这些细节的后果，从而知道化学反应中哪些键会断裂。

The proposed research is concerned with classical and semiclassical theories of molecular bound states and intramolecular dynamics. Many new experimental techniques are now able to probe the properties of highly excited molecular vibrational and vibration-rotation states in unprecedented detail, and the interpretation of such experiments poses severe challeges for theory. The present work aims to address these theoretical problems via unified treatment of the spectroscopy and dynamics of highly excited states. Practical and efficient methods for semiclassical quantization of multidimensional systems are to be developed, and these and other methods will be applied to studying the statics and dynamics of small molecules of current experimental interest. The significance of this basic research in Theoretical and Computational Chemistry lies in its contribution to a detailed understanding of the way in which energy flows within a molecule and the consequences of these details for knowing which bonds will break in a chemical reaction.