Theory of Transient, Collision-Induced Changes in Molecular Dipoles and Polarizabilities

凯瑟琳亨特博士得到了理论研究所的资助。 和计算化学程序来研究的理论 瞬时的，碰撞引起的分子偶极子的变化， 极化率 这些研究将帮助光谱学家 亚皮秒流体分子间动力学探测 这反过来将有助于他们阐明溶质-溶剂 对化学反应至关重要。 亨特博士的理论工作将有助于确定 碰撞引起的分子偶极的变化， 极化率需要提取动力学信息， 观察线条形状。 对于相互作用的分子， 电荷重叠，她计划使用新的 发展了极化率密度理论， 分子内极化率分布与强迫重叠 阻尼，以及色散，更高的多极感应，和 局部电场的不均匀性 她将开发 计算非局部响应张量的有效方法， 包括非线性极化率。 她会找到 这些张量的物理近似，并执行 计算碰撞引起的重要性质 光谱学上 她计划治疗非累加性的 通过改进的密度泛函交换极化 方法或交换微扰理论。 从头算 计算也将进行分子与 明显的重叠。

Dr. Katherine Hunt is supported by a grant from the Theoretical and Computational Chemistry Program to study the theory of transient, collision-induced changes in molecular dipoles and polarizabilities. These studies will help spectroscopists to probe intermolecular dynamics of fluids on subpicosecond time scales which in turn will help them to elucidate solute-solvent interactions critically important to chemical reactions. Dr. Hunt's theoretical work will help to determine transient, collision-induced changes in molecular dipoles and polarizabilities needed to extract dynamical information from observed line shapes. For interacting molecules with slight charge overlap, she plans to perform calculations using a newly developed polarizability density theory which accounts for the intramolecular distribution of polarizability and for overlap damping, as well as dispersion, higher-multipole induction, and nonuniformity in the local electric field. She will develop efficient methods for computing nonlocal response tensors, including nonlinear susceptibilities. She will find physically-based approximations to these tensors, and carry out calculations of collision-induced properties that are important spectroscopically. She plans to treat nonadditive exchange-polarization via a modified density-functional approach or exchange-perturbation theory. Ab initio calculations will also be carried out for molecules with appreciable overlap.