Hoang Khang, Johannes M D
Department of Physics, North Dakota State University, Fargo, ND 58108, United States of America.
J Phys Condens Matter. 2018 Jul 25;30(29):293001. doi: 10.1088/1361-648X/aacb05.
Understanding the physics of structurally and chemically complex transition-metal oxide and polyanionic materials such as those used for battery electrodes is challenging, even at the level of pristine compounds. Yet these materials are also prone to and their properties and performance are strongly affected or even determined by crystallographic point defects. In this review, we highlight recent advances in the study of defects and doping in such materials using first-principles calculations. The emphasis is on describing a theoretical and computational approach that has the ability to predict defect landscapes under various synthesis conditions, provide guidelines for defect characterization and defect-controlled synthesis, uncover the mechanisms for electronic and ionic conduction and electrochemical extraction and (re-)insertion, and provide an understanding of the effects of doping. Though applied to battery materials here, the approach is general and applicable to any materials in which the defect physics plays a role or drives the properties of interest. Thus, this work is intended as an in-depth review of defect physics in particular classes of materials, but also as a methodological template for the understanding and design of complex functional materials.
理解结构和化学复杂的过渡金属氧化物及聚阴离子材料（如用于电池电极的材料）的物理性质具有挑战性，即使是在原始化合物层面。然而，这些材料也容易出现晶体学点缺陷，其性质和性能会受到强烈影响甚至由这些缺陷决定。在本综述中，我们重点介绍了使用第一性原理计算对这类材料中的缺陷和掺杂进行研究的最新进展。重点在于描述一种理论和计算方法，该方法能够预测各种合成条件下的缺陷态势，为缺陷表征和缺陷控制合成提供指导，揭示电子和离子传导以及电化学提取和（再）嵌入的机制，并理解掺杂的影响。尽管这里将该方法应用于电池材料，但它具有通用性，适用于任何缺陷物理起作用或驱动感兴趣性质的材料。因此，这项工作旨在对特定类别的材料中的缺陷物理进行深入综述，同时也作为理解和设计复杂功能材料的方法模板。
