Made to order? Structural order and disorder in solid materials on the mesoscale

如何量化结晶固体和非晶固体之间的有序度？结构周期性的变化会对材料的物理性质和反应性产生巨大的影响，它可以为许多地成因和生物成因材料的物质形成途径提供有价值的见解。然而，对非玻璃固体的无序性研究还很不充分。如果我们能在不同的长度尺度上量化有序，那么材料中的这种无序能告诉我们它是如何形成或演变的吗？我们是否也可以利用这些知识来调整材料生产，使其达到特定的无序程度，从而控制物理性质？这些知识缺口激发了我的研究计划，寻求无序固体材料的合成、结构和物理性质之间的变革联系。定义和量化固体材料中的无序有可能从根本上改变我们对周围原子水平世界的看法。我的研究项目是高度原创和创新的，它旨在开发策略，以新的方式使用常见的光谱工具来解决这一未被充分研究的现象。在这项为期五年的研究中，我所关注的从红外光谱中提取结晶度信息的研究将会有一些现成的受众。我们最近在方解石红外光谱分析方面的突破受到了研究矿物中碳封存的同事的密切关注。我们还将利用我们的结果开发基于结构紊乱的光谱诊断工具，这将导致考古挖掘策略的范式转变。因此，这项拟议研究的环境和人类利益应用对一个非常广泛的社区具有及时的影响和重要性。

How can one quantify degrees of order between crystalline solids and their amorphous counterparts? Changes to structural periodicity can have a dramatic influence on a material's physical properties and reactivity, and it can offer valuable insights into material formation pathways in many geogenic and biogenic materials. Nevertheless, disorder in non-glassy solids is extremely understudied. If we can quantify order at different length scales, can the kind of disorder in a material tell us how it formed or evolved over time? Can we also use this knowledge to tailor material production toward a specified degree of disorder, thereby controlling physical properties? These knowledge gaps inspire my research program that seeks transformative links between the synthesis, structure and physical properties of disordered solid materials. Defining and quantifying disorder in solid materials has the potential to radically change how we think about the atomic-level world around us. My research program is highly original and innovative in the way it is designed to develop strategies for using common spectroscopic tools in new ways to address this understudied phenomenon. During the five-year term of this proposed research, my focused studies to extract crystallinity information from infrared spectra will have several ready audiences. Our recent breakthroughs with calcite infrared spectral analyses are followed closely by colleagues who study carbon sequestration in minerals. We will also use our results to develop spectroscopic diagnostic tools, based on structural disorder, that are leading to a paradigm shift for archaeological excavation strategies. Thus, the environmental and human-interest applications of this proposed research have timely impact and importance to a very broad community.