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

怀俄明大学的大卫·安德森教授和田纳西大学的罗伯特·欣德教授在实验物理化学部门的支持下，对含有开壳原子作为取代杂质的低温氢固体分子的红外光谱和化学进行了合作研究。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的存在如何？扰乱开壳层原子的电子结构。大多数化学反应都是在溶剂的存在下进行的，这些基础研究的目的是了解溶剂效应是如何在与氢分子的简单原子自由基反应中表现出来的。这将通过首先发展一个理论框架来理解被困在固体氢中的氯原子（Cl）的溶剂诱导的电子结构的扰动来完成。在这些卤素原子研究中获得的知识将随后应用于氧原子(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。本研究的目的是发展光谱分析，使掺杂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态低温化学的细节。冷冻氢分子是一种独特的结晶固体，由于氢分子在低温下（T13.8 K）冻结时的量子力学效应，它被区分为量子固体。这些关于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，利用光控制化学反应途径的能力，并有可能为高重力储存和分子氢的清洁生产提供革命性的见解。这项研究也将为本科生和研究生的研究经验和训练提供丰富的载体。

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.