Hydrogen molecules in nanoscale confinement: A combined eigenstate-resolved/path integral study of the quantum translation-rotation dynamics, spectroscopy, and diffusion

纽约大学的Zlatko Bacic （PI）和Mark E. Tuckerman （co-PI）获得了化学部化学结构、动力学和机制项目的一项计算研究的支持，该研究旨在对不同主体材料（如笼形水合物、富勒烯和碳纳米管）的纳米级空腔内氢分子的量子动力学、光谱学和扩散进行基本理解和全面的理论描述。金属有机骨架（MOFs）。这将提供一个广泛的理论框架，以及定量预测，对于目前由世界各地的团体进行的这些系统的各种类型的光谱测量的规划，分析和解释是必不可少的。一系列强大的理论方法，从高维量子束缚态和散射方法到扩散蒙特卡罗和路径积分模拟，将被带到这些目标上。本研究的另一个目标是精确测定纳米受限氢（在某些情况下是H2O）与宿主材料的多维、各向异性和非调和相互作用势。要实现这一目标，需要结合复杂的量子动力学和从头算电子结构计算。本征态解析计算将由路径积分模拟补充，旨在阐明分子氢的能量学、自由能量学、空间分布和扩散的温度和浓度依赖性，特别是在大块笼形水合物和mof中。大规模使用氢作为清洁高效能源载体的一个主要障碍是开发安全经济的储存方法。在纳米多孔材料中吸收的一种可能性目前正受到广泛的研究。定量了解这种条件下氢分子的性质，以及表征氢与不同宿主环境的相互作用，对于合理设计储氢新介质的实验和理论工作至关重要。如果实现，开发高效储氢材料的挑战将对新兴能源技术产生巨大影响。这项研究将由纽约大学的研究生和本科生进行，包括那些传统上代表性不足的群体。此外，我们的实验合作者之一Stephen FitzGerald教授在Oberlin大学就读，他的学生将直接参与这个项目。

Zlatko Bacic (PI) and Mark E. Tuckerman (co-PI) of New York University are supported by an award from the Chemical Structures, Dynamics and Mechanisms program of the Chemistry Division for a computational study aimed at achieving a fundamental understanding and a comprehensive theoretical description of the quantum dynamics, spectroscopy, and diffusion of hydrogen molecules inside the nanoscale cavities of diverse host materials, such as clathrate hydrates, fullerenes and carbon nanotubes, and metal-organic frameworks (MOFs). This will provide a broad theoretical framework, as well as quantitative predictions, indispensable for the planning, analysis, and interpretation of various types of spectroscopic measurements of these systems presently carried out by groups around the world. An array of robust theoretical approaches, ranging from high-dimensional quantum bound state and scattering methods to diffusion Monte Carlo and path integral simulations, will be brought to bear on these objectives. Another goal of this proposal is the accurate determination of multidimensional, anisotropic and anharmonic interaction potentials of the nanoconfined hydrogen, and in certain cases H2O, with the host materials. Accomplishing this will involve the combination of sophisticated quantum dynamics and ab initio electronic structure calculations. The eigenstate-resolved calculations will be complemented by path integral simulations directed at elucidating the temperature and concentration dependence of the energetics, free-energetics, spatial distributions, and diffusion of molecular hydrogen, especially in bulk clathrate hydrates and MOFs. A major hurdle for the large-scale use of hydrogen as a clean and efficient energy carrier is developing ways to store it safely and economically. One possibility currently under intense investigation worldwide absorption in nanoporous materials. Quantitative understanding of the properties of molecular hydrogen under such conditions, and characterization of the interactions of hydrogen with various host environments is essential in joint experimental and theoretical efforts aimed at rational design of new media for hydrogen storage. If met, the challenge of developing efficient hydrogen-storage materials will have an enormous impact on emerging energy technologies. This research will be carried out by graduate and undergraduate students at NYU, including those from traditionally underrepresented groups. In addition, one of our experimental collaborators, Prof. Stephen FitzGerald, is at an undergraduate institution (Oberlin), and his students will be directly involved in the project.