Redox-active oxides find use in many applications, including catalysts, photovoltaic devices, self-cleaning glasses, chemical sensors and electronic components. Their utility derives from their unique ability to access multiple metal-charge states within a finite energy window. However, this property also confounds our ability to study reducible oxides, because it leads to structural, compositional and electronic complexities that elude simplistic models of materials structure and function. Oxygen vacancies play a critical role in shaping the functional properties of such oxides; most notably, they lead to mobile-charge imbalances that impact surface processes at substantial distances from the originating defect. Atomistic simulations are inherently equipped to illuminate these phenomena at a fundamental level; however, reducible oxides pose great challenges, owing to the high level of electron correlation needed to correctly describe them. Understanding how defects form, couple, propagate, agglomerate or repel each other and influence the surface properties of reducible oxides is only now coming into the grasp of modern theory and simulation capabilities. This knowledge is also key to discovering and controlling emergent materials properties with tunable multifunctionalities at the nanometre scale and beyond.

氧化还原活性氧化物可用于许多领域，包括催化剂，光伏设备，自清洁玻璃，化学传感器和电子组件。它们的实用性源于其在有限的能量窗口内访问多种金属电荷状态的独特能力。但是，这种性质也混淆了我们研究可还原氧化物的能力，因为它导致结构，组成和电子复杂性，而使材料结构和功能的简化模型无法实现。氧空位在塑造此类氧化物的功能特性方面起着至关重要的作用。最值得注意的是，它们导致移动电荷不平衡，从而在距原始缺陷很大距离的地方影响表面处理。固有的原子模拟可以从根本上阐明这些现象。然而，由于正确描述它们需要高水平的电子相关性，因此可还原的氧化物提出了巨大的挑战。了解缺陷如何相互形成，耦合，传播，凝聚或排斥并影响可还原氧化物的表面性能，才刚刚成为现代理论和仿真能力的掌握。这些知识也是发现和控制具有纳米级及以上可调多功能功能的新兴材料特性的关键。