First Principles Quantum Molecular Dynamics: Density Matrix Theory and Computational Aspects

佛罗里达大学的大卫米查是由理论和计算化学计划的支持，以追求密度矩阵方法的第一原理量子动力学的分子相互作用。 新的技术将联合收割机时间相关的哈特里-福克理论与程函方法的核运动。 计算算法将被开发来计算电子状态的人口，自旋轨道再耦合，和状态到状态的横截面的时间演化。 应用包括飞秒动力学和光谱的电子重排在气相碰撞和固体表面。 该理论旨在提供新的见解，概念和预测计算工具来处理分子中碰撞诱导和光诱导的电子跃迁。它的计算实现产生电子势能，它们的耦合，和过渡偶极子的动力学现象的研究。 它将有助于解释最近的新实验，涉及飞秒化学，瞬态物种的受激发射，和溶剂化物种的光谱。

David Micha of the University of Florida is supported by the Theoretical and Computational Chemistry Program to pursue density matrix approaches to first principle quantum dynamics of molecular interactions. New techniques will combine time-dependent Hartree-Fock theory with eikonal methods for nuclear motion. Computational algorithms will be developed to calculate time-evolution of electronic state populations, spin-orbit recoupling, and state-to-state cross sections. Applications include femtosecond dynamics and spectra of electronic rearrangement in gas-phase collisions and at solid surfaces. This theory aims to provide new insight, concepts, and predictive computational tools to deal with collision-induced and photoinduced electronic transitions in molecules. Its computational implementation generates electronic potential energies, their couplings, and transition dipoles for studies of dynamical phenomena. It will aid in the interpretation of recent novel experiments involving femtosecond chemistry, stimulated emission of transient species, and spectroscopy of solvated species.