Collaborative Research: Fluid Polyamorphism: Theory, Experiment and Simulation

合作研究：流体多晶现象：理论、实验和模拟

• 批准号: 1856506
• 负责人: Jeffery Yarger
• 金额: $ 26.82万
• 依托单位: Arizona State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2019
• 资助国家: 美国
• 起止时间: 2019-08-01 至 2023-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1856506&HistoricalAwards=false
• 关键词: Collaborative; Research; Fluid; Polyamorphism; Theory

This project, funded by the Chemical Structure, Dynamics and Mechanisms-A (CSDM-A) program of the Chemistry Division, supports a collaboration between scientists and engineers at the University of Maryland at College Park, Arizona State University, Boston University, and Princeton University. The collaborative team employs theoretical, computational, and experimental methods to investigate the different types of molecular structures that can occur in liquids. The molecules within a liquid, while not as ordered as they would be in a solid crystal, may still form distinguishable types of structures. This phenomenon, known as polyamorphism, has been predicted to occur in water at sub-freezing temperatures and high pressures. The team is employing experimental techniques such as calorimetry (to measure the flow of heat into and out of samples as they undergo phase changes), infrared spectroscopy (to characterize the molecular vibrations in the system), and computational tools (molecular dynamics simulations) to characterize polyamorphic phases in water and other liquids. In addition to gaining fundamental insights into the nature of matter, the results of this investigation may have impacts in fields such as glass technology, cryobiology, and atmospheric science. The graduate students involved in this project are gaining experience in both experimental and computational chemistry, They benefit from personnel exchanges among the different participating institutions. The broader impacts of the project may include development of computer hardware based on silicon alternatives, better pharmaceutical formulations, new routes to low-temperature tissue preservation, computational models for high school students, and more accurate weather predictions based on an improved understanding of cloud microphysics.This project involves the development and verification of a generic thermodynamic approach to describe polyamorphism in single-component substances. The unifying concept is that of equilibrium interconversion between competing molecular or supramolecular structures. Simulations involve studies of chirality-driven, liquid-liquid phase separations, critical behaviors and finite-size scaling under deeply supercooled conditions, and the interplay between crystallization, fluid phase separation, and fluid structural relaxation. Calorimetry, optical microscopy, dynamic light scattering, infrared and Raman spectroscopies, and transmission electron microscopy provide complementary experimental characterization on polyamorphic systems, including non-crystallizing aqueous solutions. The two-state thermodynamic formalism provides a unifying theoretical perspective. The broader impacts of the project may include development of computer hardware based on silicon alternatives, better pharmaceutical formulations, new routes to low-temperature tissue preservation, computational models for high school students, and more accurate weather prediction through improved understanding of cloud microphysics.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.

该项目由化学部的化学结构、动力学和机理-A（CSDM-A）项目资助，支持马里兰州大学帕克分校、亚利桑那州立大学州立大学和普林斯顿大学的科学家和工程师之间的合作。该合作团队采用理论、计算和实验方法来研究液体中可能出现的不同类型的分子结构。液体中的分子虽然不像固体晶体中那样有序，但仍然可以形成可区分的结构类型。 这种现象被称为多晶现象，预计会在冰点以下的温度和高压下发生。 该团队正在使用实验技术，如量热法（测量样品发生相变时流入和流出的热量），红外光谱（表征系统中的分子振动）和计算工具（分子动力学模拟）来表征水和其他液体中的多晶相。 除了获得对物质性质的基本见解外，这项研究的结果可能会对玻璃技术，低温生物学和大气科学等领域产生影响。 参与该项目的研究生正在获得实验和计算化学方面的经验，他们受益于不同参与机构之间的人员交流。 该项目的更广泛影响可能包括基于硅替代品的计算机硬件的开发，更好的药物配方，低温组织保存的新途径，高中生的计算模型，和更准确的天气预报的基础上提高云微物理学的理解。这个项目涉及到一个通用的热力学方法的发展和验证，以描述多晶在单一的，组成物质。统一的概念是竞争分子或超分子结构之间的平衡相互转化。模拟涉及手性驱动的研究，液-液相分离，临界行为和有限尺寸缩放深度过冷条件下，结晶，流体相分离和流体结构松弛之间的相互作用。量热法，光学显微镜，动态光散射，红外和拉曼光谱，和透射电子显微镜提供互补的实验表征多晶系统，包括非结晶水溶液。双态热力学形式主义提供了一个统一的理论视角。该项目的更广泛影响可能包括基于硅替代品的计算机硬件的开发，更好的药物配方，低温组织保存的新途径，高中生的计算模型，该奖项反映了NSF的法定使命，并通过使用基金会的智力价值进行评估而被认为值得支持和更广泛的影响审查标准。

项目成果

The Structure of Liquid and Glassy Carbamazepine

液体和玻璃状卡马西平的结构

• DOI: 10.3390/qubs6040031
• 发表时间: 2022
• 期刊: Quantum Beam Science
• 影响因子: 1.4
• 作者: Benmore, Chris J.;Edwards, Angela;Alderman, Oliver L.;Cherry, Brian R.;Smith, Pamela;Smith, Daniel;Byrn, Stephen;Weber, Richard;Yarger, Jeffery L.
• 通讯作者: Yarger, Jeffery L.

A High Energy X-ray Diffraction Study of Amorphous Indomethacin

• DOI: 10.1016/j.xphs.2021.12.003
• 发表时间: 2022-03-04
• 期刊: JOURNAL OF PHARMACEUTICAL SCIENCES
• 影响因子: 3.8
• 作者: Benmore, C. J.;Benmore, S. R.;Weber, J. K. R.
• 通讯作者: Weber, J. K. R.