发表机构
National University of Singapore; University of Birmingham; University of Houston; Texas Center for Superconductivity; University College London（新加坡国立大学; 伯明翰大学; 休斯顿大学; 德克萨斯超导中心; 伦敦大学学院）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
研究针对多元化合物表面建模的非物理表面能问题，开发SALAMI软件包生成低能slab模型，通过调控配位环境优化Li₃PS₄和ZnSb₂O₆的表面能，缩小Wulff形状体积约20%，明确了精准控制配位环境的必要性。
AI 中文摘要
在对多元化合物的表面进行建模时，常规解理面常穿过键合强烈的多面体，导致非物理的表面能。本文介绍了SALAMI（Symmetric Atomic Layers for Arbitrary Multinary Interfaces，适用于任意多元界面的对称原子层），这是一款用于生成多元化合物的对称、电中性、无偶极矩且低能的 slab（ slab模型）的Python软件包。SALAMI执行组合搜索，选择性移除表面原子并生成保留最优配位环境的波纹状终止结构。我们将该工作流应用于两种典型结构中所有对称不等价的晶面取向（Miller指数≤2）：固态电解质Li₃PS₄和透明导电氧化物ZnSb₂O₆。密度泛函理论计算表明，Li₃PS₄必须保留所有PS₄单元才能达到最低表面能；对于ZnSb₂O₆，低能表面通过表面Sb原子的部分低配位实现，从体相SbO₆转变为SbO₅或SbO₄，具体取决于表面取向。与无约束配位生成的表面模型相比，应用约束以实现最优局部配位环境可显著降低表面能，使预测的Wulff形状体积缩小约20%。本研究表明，精准控制局部配位环境对于准确预测多元化合物的表面能量学是必要的。
英文摘要
When modeling surfaces of multinary compounds, conventional cleavage planes often cut through strongly bonded polyhedra, resulting in unphysical surface energies. Here, we introduce SALAMI (Symmetric Atomic Layers for Arbitrary Multinary Interfaces), a Python package that generates symmetric, charge-neutral, dipole-free, and low-energy slab models for multinary compounds. SALAMI performs combinatorial searches to selectively remove surface atoms and generate corrugated terminations that preserve optimal coordination environments. We applied this workflow to all symmetrically inequivalent crystallographic orientations with Miller indices up to 2 for two prototypical structures: the solid-state electrolyte Li3PS4 and the transparent conducting oxide ZnSb2O6. Density functional theory calculations reveal that Li3PS4 must preserve all PS4 units to achieve the minimum surface energy. For ZnSb2O6, low-energy surfaces are achieved by partial undercoordination of surface Sb atoms to SbO5 or SbO4 from the bulk SbO6, depending on the surface orientations. Compared to surface models generated with unconstrained coordination, applying constraints to achieve optimal local coordination environments significantly lowers surface energies, shrinking the volume of the predicted Wulff shape by approximately 20%. Our results demonstrate that meticulous control of local coordination environments is necessary for accurately predicting the surface energetics of multinary compounds.
Comments27 pages, 8 figures, 2 tables; Supplementary information included as appendices; Open-source software repository: https://github.com/caneparesearch/salami
