搜索

x
中国物理学会期刊

面向软晶格筛选的立方钙钛矿体模量可解释性描述符研究

CSTR: 32037.14.aps.74.20250652

Descriptors for the interpretability of cubic perovskite bulk modulus oriented towards soft lattice screening

CSTR: 32037.14.aps.74.20250652
PDF
HTML
导出引用
  • 近年来, 软晶格被认为是钙钛矿材料实现缺陷容忍性的主要物理来源, 体模量则作为晶格“软硬度”的关键衡量指标. 本文针对立方钙钛矿体系, 基于SISSO (sure independence screening and sparsifying operator)与VS-SISSO (集成迭代变量选择机制的SISSO框架)方法, 构建了两类低维、物理可解释性强的体模量预测模型. 首先, 基于共价半径、熔点和体积等结构和热力学特征构建的热-结构耦合描述符模型, 在测试集上实现了均方根误差RMSE = 7.41 GPa, 决定系数R2 = 97.8% 的良好预测性能; 进一步引入电负性、原子价态与未配对电子数等电子层级特征后, 构建了电子-热-结构三重耦合描述符模型, 预测精度显著提升, 在测试集上RMSE降至5.34 GPa, R2提升至98.35%. 基于该模型, 本文对超过10000个卤族和硫族立方钙钛矿进行高通量预测, 筛选出约170种体模量位于10—20 GPa区间、与Pb-I钙钛矿相近的候选体系. 研究结果为软晶格机制在无铅体系中的适用性提供了初步支持, 并为高通量筛选具缺陷容忍潜力的稳定无铅钙钛矿材料提供了理论依据与数据支撑. 本文数据集可在https://doi.org/10.57760/sciencedb.j00213.00161中访问获取.

     

    In recent years, soft lattices have been considered a primary physical origin of defect tolerance in lead-halide perovskite materials, with bulk modulus serving as a key indicator of lattice “softness”. This work focuses on cubic perovskites and constructing a dataset of bulk moduli for 213 compounds based on density functional theory (DFT) calculations. A total of 138 features are compiled, including 132 statistical features extracted using the Matminer toolkit and 6 manually selected elemental descriptors. Four conventional machine learning regression models (RF, SVR, KRR, and EXR) are employed for prediction. Of them, the SVR model shows the best performance, achieving a test-set Root Mean Square Error (RMSE) of 7.35 GPa and Coefficient of Determination (R2) of 97.86%. Feature importance analysis reveals that thermodynamic-structural features such as melting point, covalent radius, and atomic volume play dominant roles in determining bulk modulus. Based on the 12 most important features, a thermodynamic-structural coupling descriptor is constructed using the SISSO method, yielding a test-set RMSE of 7.41 GPa and R2 of 97.80%. The resulting descriptor indicates that the bulk modulus is proportional to melting point and inversely proportional to atomic volume. Furthermore, the VS-SISSO method combined with a random subset selection and iterative variable screening strategy is used, enabling the selection of electronic-level features such as electronegativity, valence state, and number of unpaired electrons. The resulting electronic-thermodynamic-structural coupling descriptor further improves the prediction accuracy, reaching an RMSE of 5.34 GPa and R2 of 98.35% on the test set. Notably, due to the difference in valence states, this model effectively distinguishes between the bulk moduli of chalcogen-based (divalent) and halogen-based (monovalent) perovskites. Based on this model, high-throughput screening is performed on over 10000 cubic chalcogenides and halide perovskites, and approximately 170 lead-free candidates with bulk moduli in the range of 10–20 GPa are identified, which are comparable to Pb-I perovskites. These results provide preliminary evidence for supporting the applicability of the soft-lattice mechanism in lead-free systems and offer theoretical guidance and data support for the high-throughput discovery of stable, defect-tolerant, lead-free perovskite materials. All the data presented in this paper are openly available at https://doi.org/10.57760/sciencedb. j00213.00161.

     

    目录

    /

    返回文章
    返回