Parahydrogen Matrix Isolation Infrared Spectroscopy and Kinetics

仲氢基质分离红外光谱和动力学

• 批准号: 2101719
• 负责人: David Anderson
• 金额: $ 50万
• 依托单位: University of Wyoming
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-06-01 至 2025-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2101719&HistoricalAwards=false
• 关键词: Parahydrogen; Matrix; Isolation; Infrared; Spectroscopy

With support from the Chemical Structure, Dynamics, and Mechanisms-A (CSDM-A) Program in the Division of Chemistry, Professor David T. Anderson and his group at the University of Wyoming are using extremely cold crystals made from molecular hydrogen as a reaction vessel to investigate chemistry at low temperatures. The first thrust of the research project examines the diffusion and reactivity of hydrogen atoms. At extremely low temperatures (-457°F), hydrogen atoms are better described as matter waves instead of particles, which has a major impact on how they diffuse through the crystal and react chemically with other species. Chemistry is transformed under these low-temperature conditions into the fully quantum mechanical regime where unexpected chemical behavior can be discovered. The second thrust of the work involves experimental studies of nuclear spin states in polyatomic molecules that undergo rapid cooling, photochemistry, or chemical reactions. Nuclear spin refers to the internal state of an atom, and sometimes has an orientation. Certain molecules, like water, come in two different forms, one where the two hydrogen atoms have their nuclear spins aligned in the same direction, and the other with the two hydrogen atom spins aligned in opposite directions. These different nuclear spin isomers of water have different magnetic properties. The research team led by Professor Anderson is examining to what extent nuclear spin is conserved during various physical and chemical processes, with the goal of learning how to use nuclear spin to control chemical reactions and to enhance magnetic imaging techniques. This experimental work uses a custom-designed cryogenic apparatus to synthesize cryocrystals of para-hydrogen (a specific nuclear spin isomer of molecular hydrogen) doped with parts per million concentrations of chemical impurities at temperatures in the 1.5 to 5 K range. Hydrogen atoms are created in situ using a variety of ultraviolet light sources and the ensuing reaction kinetics are measured using high-resolution Fourier-transform infrared spectroscopy. Professor Anderson and his group utilize a liquid helium cryostat to achieve such low temperatures and have built a dedicated helium recovery system to recycle the spent helium gas to minimize supply costs. The students working with Professor Anderson gain experience using sophisticated methods in experimental physical chemistry that probe the physical and chemical properties of quantum materials, materials whose properties are dominated by the laws of quantum mechanics. The involvement of students in the research has a significant impact by training future scientists in the techniques of low-temperature chemistry and the quantum-mechanical manipulation of matter.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在化学系化学结构、动力学和机理 A (CSDM-A) 项目的支持下，怀俄明大学 David T. Anderson 教授和他的团队正在使用由分子氢制成的极冷晶体作为反应该研究项目的第一个重点是研究氢原子在极低温度（-457°F）下的扩散和反应性，氢原子最好被描述为物质波而不是粒子。重大影响研究它们如何在晶体中扩散并与其他物质发生化学反应，在这些低温条件下化学转化为完全量子力学状态，可以发现意想不到的化学行为。在经历快速冷却、光化学或化学反应的多原子分子中，核自旋是指原子的内部状态，有时具有方向性，某些分子（例如水）有两种不同的形式，其中两个氢原子具有方向。它们的核自旋排列在安德森教授领导的研究小组正在研究核自旋在各种物理和化学过程中的守恒程度。过程，目的是学习如何使用核自旋来控制化学反应并增强磁成像技术。这项实验工作使用定制设计的低温装置来合成仲氢（分子氢的一种特定核自旋异构体）的低温晶体。掺杂在 1.5 至 5 K 范围内的温度下，使用各种紫外光源原位产生百万分之一的化学杂质浓度，并使用高分辨率傅里叶变换红外光谱仪测量随后的反应动力学。他的团队利用液氦低温恒温器来实现如此低的温度，并建立了专用的氦气回收系统来回收废氦气，以最大限度地降低供应成本。与安德森教授合作的学生获得了经验。使用实验物理化学中的复杂方法来探测量子材料的物理和化学性质，这些材料的性质受量子力学定律支配，学生参与研究对于培训未来的科学家具有重大影响。 -温度化学和物质的量子力学操纵。该奖项反映了 NSF 的法定使命，并且通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

Infrared Spectroscopic Studies of Oxygen Atom Quantum Diffusion in Solid Parahydrogen

固体仲氢中氧原子量子扩散的红外光谱研究

• DOI: 10.1021/acs.jpca.3c00266
• 发表时间: 2023
• 期刊: The Journal of Physical Chemistry A
• 作者: Muddasser, Ibrahim;Nguyen, Anh H.;Strom, Aaron I.;Hardee, Aaron M.;Pluid, Bryan G.;Anderson, David T.
• 通讯作者: Anderson, David T.