Npj Comput. Mater.: 数据驱动—助益复杂材料全局优化和科学分析

海归学者发起的公益学术平台

分享信息，整合资源

交流学术，偶尔风月

来自中国南京信息工程大学的张磊教授及其团队成员，基于机器学习和材料计算，科学地评估了卤化物钙钛矿的稳定性。在这项研究中，他们系统地研究了在不同表面上功能的多分子修饰的CH₃NH₃PbI₃膜的水性光电化学稳定性，发现了一种有效的多分子钙钛矿材料体系“calcein + PbBr₂ + DMSO +CH₃NH₃PbI₃”，具有出色的液态水环境光电稳定性（相同水环境下光生电流是CH₃NH₃PbI₃薄膜输出的103倍)和92.5%的水稳定性。随后，通过遗传算法和极端随机树的Shapley分析来检测分子修饰钙钛矿材料的实验水性光电化学性质，以提供机器解释和解耦分子贡献，强调这些兼容分子的协同效应及其亲水/亲脂性对目标输出的重要性。DFT计算表明，该多分子全局优化体系存在大量氢键和阴离子··π表面相互作用以稳定其界面结构。除了预测高水稳定性的钙钛矿体系外，该研究团队还优化了光电化学、机器学习和DFT模型总体数据驱动工作流程用于评估卤化物钙钛矿稳定性。

Figure 1 Post-hoc DFT calculation (atomic and electronic structures)

Figure 2 Fabrication details, classification method and molecular variables.

Figure 3 Feature analysis via SHAP.

Figure 4 Overall workflow of this study.

Data-driven optimization and machine learning analysis of compatible molecules for halide perovskite material 

Shaojun Wang, Yiru Huang, Wenguang Hu & Lei Zhang

Optoelectronic stability of halide perovskite material in hostile conditions such as water is rather limited, preventing them from further industrial deployment. Here, we optimize and perform machine learning analysis on CH₃NH₃PbI₃materials with additives, solvents and post-treatment molecules using combined experimental and data-driven methods. A champion system consisting of a compatible tertiary molecular combination ‘calcein+PbBr₂ + DMSO’ active at diverse surfaces is identified, delivering a large aqueous photoelectrochemical (PEC) photocurrent of 10^-5 A/cm² and an improved aqueous stability of 92.5%. Subsequently, machine interpretation is provided to decouple the multi-molecule contributions with the assistance of genetic programming (GP) and extra-trees (ET) machine learning models, highlighting the intricate molecular features for the target outputs. The posthoc density functional theory (DFT) calculation suggests the presence of multiple hydrogen bond and anion··π surface interactions to stabilize the interfacial structures. The present ‘PEC + GP + ET + DFT’ approach is suggested to be an effective approach to design and comprehensively evaluate moleculemodified materials.