Collaborative Research: Spectroscopy and Chemistry of Open-Shell Atoms in Solid Hydrogen Matrices

怀俄明大学的David Anderson教授和田纳西大学的Robert Hinde教授在实验物理化学部的支持下，合作研究了以开壳原子为替代杂质的低温分子氢固体的红外光谱和化学。通过实验(Anderson)和第一性原理模拟(Hinde)的结合，该项目的目标是使用红外光谱来量化氢、溶剂？扰乱了开壳原子的电子结构。大多数化学都是在溶剂存在的情况下进行的，这些基础研究的目的是了解溶剂效应是如何在简单的原子自由基与分子氢反应中表现出来的。这将通过首先开发一个理论框架来实现，该框架用于理解固体氢中捕获的氯原子(Cl)在溶剂中引起的电子结构扰动。在这些卤素原子研究中获得的知识将被应用于氧原子(O)掺杂的固体氢，以研究O原子与分子氢的典型燃烧反应的溶剂扰动。这项研究的目的是发展光谱分析，使掺入原子自由基的固体氢可以作为一种新的反应介质来研究凝聚相中的低温化学细节。冻结分子氢是一种独特的结晶固体，由于氢分子在氢气冻结的低温(T13.8K)下具有明显的量子力学效应，因此被区分为量子固体。这些对量子固体中化学反应的研究将直接影响我们对低温化学反应中的量子力学效应的理解，以及利用光控制化学反应路径的能力，并有可能为高重量储存和清洁生产分子氢提供变革性的见解。这项研究也将为本科生和研究生的研究经验和培训提供丰富的载体。

Professors David Anderson of the University of Wyoming and Robert Hinde of the University of Tennessee are supported by the Experimental Physical Chemistry Division for a collaborative investigation of the infrared (IR) spectroscopy and chemistry of cryogenic molecular hydrogen solids containing open-shell atoms as substitutional impurities. Through a combination of experiment (Anderson) and first principles simulations (Hinde) the project goal is to use the IR spectroscopy to quantify how the presence of the hydrogen ?solvent? perturbs the electronic structure of the open-shell atom. Most chemistry occurs in the presence of a solvent and these fundamental studies are aimed at understanding how solvent effects are manifested in simple atomic radical reactions with molecular hydrogen. This will be accomplished by first developing a theoretical framework for understanding the solvent-induced perturbation of the electronic structure of chlorine atoms (Cl) trapped in solid hydrogen. The knowledge gained in these halogen atom studies will then be applied to oxygen atom (O) doped solid hydrogen to study solvent perturbations of the prototypical combustion reaction of O-atoms with molecular hydrogen. The goal of this research is to develop the spectroscopic analysis such that solid hydrogen doped with atomic radicals can be used as a new reaction medium to study the details of low temperature chemistry in a condensed phase. Frozen molecular hydrogen is a unique crystalline solid that is distinguished as a quantum solid due to pronounced quantum mechanical effects of the hydrogen molecule at the low temperatures at which hydrogen freezes (T13.8 K). These studies of chemical reactions in a quantum solid will have direct impact on our understanding of quantum mechanical effects in low temperature chemical reactions, the ability to use light to control chemical reaction pathways, and potentially provide transformative insight into both high gravimetric storage and clean production of molecular hydrogen. This research will also provide a rich vehicle for undergraduate and graduate research experience and training.