Neutral supercells for charged impurities by explicit acceptor/donor compensation - defects in diamond

To investigate charged defects in gapped materials by first-principles calculations, they must be charged by either adding/removing electrons or compensating donors/acceptors. The former approach is more common, but it is not without drawbacks. We tested the latter method for a collection of model systems consisting of charge-compensated point defects in diamond (NV/SiV-centers, substitutional nitrogen/phosphorous/oxygen/sulfur donors, and substitutional boron/beryllium acceptors), comparing the geometrical and electronic properties of the compensated defect pairs with those of the individual defects in charged supercells. We find that the charging by explicit donors/acceptors works well and can be advantageous if properly designed, although interpretation of the results can be challenging. In this archive, we share the final optimized geometries of all studied structural models (in CIF format).

为通过第一性原理计算（first-principles calculations）研究带隙材料（gapped materials）中的带电缺陷（charged defects），可通过两种方式对缺陷进行带电处理：一是添加/移除电子，二是补偿施主（donor）/受主（acceptor）。前者更为常用，但并非不存在局限性。我们针对一系列由金刚石（diamond）中电荷补偿点缺陷构成的模型体系——包括NV/SiV中心、替位式氮/磷/氧/硫施主，以及替位式硼/铍受主——测试了后者方法，并将补偿缺陷对的几何与电子性质，与带电超胞（supercells）中单个缺陷的对应性质进行了对比。我们发现，通过显性施主/受主进行带电处理的方法效果良好，若设计得当还可具备优势，尽管对结果的解读可能存在一定难度。在本数据档案中，我们共享了所有研究结构模型的最终优化几何构型，格式为CIF（CIF format）。