建立计算与实验的量化评估体系,提升高熵合金相稳定性预测可信度。
High-throughput validation of phase formability and simulation accuracy of Cantor alloys
- 构建置信度指标,量化计算与实验在相变行为上的吻合度。
- 在约1000℃下验证了大量FeNiMnCr合金,发现高锰区面心/体心相预测偏差显著。
- 为机器学习模型优化提供实证依据,适合材料高通量设计研究者。
高通量方法加速复杂体系如高熵合金的新材料发现,其相稳定性覆盖广阔的成分空间。密度泛函理论(DFT)和相图计算(CALPHAD)可辅助筛选成分与温度依赖的相形成能力。然而,计算预测与实验验证的整合仍具挑战。本文引入定量置信度指标,评估基于DFT或CALPHAD训练的机器学习模型对实验数据的拟合程度。实验数据通过高通量原位同步辐射X射线衍射获取,针对成分多样的FeNiMnCr合金库从室温加热至约1000 °C。采用温度无关相分类或考虑温度依赖相形成概率的模型,评估预测与观测相态的一致性。该方法揭示了计算与实验整体一致性较高的区域,同时识别出高锰区面心立方(FCC)与体心立方(BCC)相预测的关键偏差,为未来模型改进提供方向。
原文摘要 · Abstract (English)
High-throughput methods enable accelerated discovery of novel materials in complex systems such as high-entropy alloys, which exhibit intricate phase stability across vast compositional spaces. Computational approaches, including Density Functional Theory (DFT) and calculation of phase diagrams (CALPHAD), facilitate screening of phase formability as a function of composition and temperature. However, the integration of computational predictions with experimental validation remains challenging in high-throughput studies. In this work, we introduce a quantitative confidence metric to assess the agreement between predictions and experimental observations, providing a quantitative measure of the confidence of machine learning models trained on either DFT or CALPHAD input in accounting for experimental evidence. The experimental dataset was generated via high-throughput in-situ synchrotron X-ray diffraction on compositionally varied FeNiMnCr alloy libraries, heated from room temperature to ~1000 °C. Agreement between the observed and predicted phases was evaluated using either temperature-independent phase classification or a model that incorporates a temperature-dependent probability of phase formation. This integrated approach demonstrates where strong overall agreement between computation and experiment exists, while also identifying key discrepancies, particularly in FCC/BCC predictions at Mn-rich regions to inform future model refinement.
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