摘要：SummaryThe long-standing performance-stability contradiction issue of high energy density materials (HEDMs) is of extremely complex and multi-parameter nature. Herein, machine learning was employed to handle 28 feature descriptors and 5 properties of detonation and stability of 153 HEDMs, wherein all 21,648 data used were obtained through high-throughput crystal-level quantum mechanics calculations on supercomputers. Among five models, namely, extreme gradient boosting regression tree (XGBoost), adaptive boosting, random forest, multi-layer perceptron, and kernel ridge regression, were respectively trained and evaluated by stratified sampling and 5-fold cross-validation method. Among them, XGBoost model produced the best scoring metrics in predicting the detonation velocity, detonation pressure, heat of explosion, decomposition temperature, and lattice energy of HEDMs, and XGBoost predictions agreed best with the 1,383 experimental data collected from massive literatures. Feature importance analysis was conducted to obtain data-driven insight into the causality of the performance-stability contradiction and delivered the optimal range of key features for more efficient rational design of advanced HEDMs.Graphical abstractDisplay OmittedHighlights•Crystal-level quantum mechanics calculations of 21,648 physicochemical data of 153 HEDMs•Machine learning of detonation and stability of HEDMs and experimental validation•Data-driven insight into the causality of performance-stability contradiction•Optimal range of key features for rational design of advanced HEDMsComputational Materials Science; Computational Method in Materials Science; Energy Materials; Materials Design
