High-Throughput Prediction of Thermodynamic Stabilities of Dopant-Defect Clusters at Misfit Dislocations in Perovskite Oxide Heterostructures
High-Throughput Prediction of Thermodynamic Stabilities of Dopant-Defect Clusters at Misfit Dislocations in Perovskite Oxide Heterostructures
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DOI：
10.1021/acs.jpcc.3c02367
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发表时间：
2023-08
期刊：
影响因子：
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通讯作者：
Chloe Marzano;P. Dholabhai
中科院分区：
文献类型：
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作者：
Chloe Marzano;P. Dholabhai
复合氧化物异质结构和薄膜已经成为具有广泛应用前景的候选材料，其中通过连接两种不同的氧化物形成的界面在单个组分中不存在的新颖性能中发挥了核心作用。这两种氧化物之间的晶格失配会导致失配位错的形成，这往往会影响重要的材料性质。在氧化物中，掺杂是一种改善性能的策略，其中异价掺杂会导致氧空位缺陷的形成。在低温下，这些掺杂剂和缺陷通常形成稳定的团簇。在半粘性钙钛矿氧化物异质结构中，这种团簇在失配位错处的稳定性，虽然还没有被很好地理解，但预计会影响界面管理的性质。在这里，我们报道了原子模拟阐明了失配位错对SrTiO_3/BaZrO_3异质结中掺杂缺陷团簇稳定性的影响。考虑了具有不同失配位错结构的SRO-BaO、SRO-ZrO2、BaO-TiO2四种界面。对失配位错附近的275,610个掺杂缺陷团簇的热力学稳定性进行了高通量计算。给定界面位错结构和相应的原子层化学对几何多样性团簇的热力学稳定性起着基础性的作用。与相干阶地相比，失配位错线和交叉处的团簇稳定性明显不同。这些结果为理解钙钛矿型氧化物异质结构的功能提供了原子尺度的视角，揭示了掺杂、点缺陷和扩展缺陷之间的复杂相互作用。
Complex oxide heterostructures and thin films have emerged as promising candidates for diverse applications, wherein interfaces formed by joining two different oxides play a central role in novel properties that are not present in the individual components. Lattice mismatch between the two oxides leads to the formation of misfit dislocations, which often influence vital material properties. In oxides, doping is used as a strategy to improve properties, wherein inclusion of aliovalent dopants leads to formation of oxygen vacancy defects. At low temperatures, these dopants and defects often form stable clusters. In semicoherent perovskite oxide heterostructures, the stability of such clusters at misfit dislocations, while not well understood, is anticipated to impact interface-governed properties. Herein, we report atomistic simulations elucidating the influence of misfit dislocations on the stability of dopant-defect clusters in SrTiO3/BaZrO3heterostructures. SrO–BaO, SrO–ZrO2, BaO–TiO2, and ZrO2–TiO2interfaces having dissimilar misfit dislocation structures were considered. High-throughput computing was implemented to predict the thermodynamic stabilities of 275,610 dopant-defect clusters in the vicinity of misfit dislocations. The misfit dislocation structure of the given interface and corresponding atomic layer chemistry play a fundamental role in influencing the thermodynamic stability of geometrically diverse clusters. A stark difference in cluster stability is observed at misfit dislocation lines and intersections as compared to the coherent terraces. These results offer an atomic scale perspective of the complex interplay between dopants, point defects, and extended defects, which is necessary to comprehend the functionalities of the perovskite oxide heterostructures.