发表机构
Chimie ParisTech, PSL University; Shanghai University（巴黎高等化学学院，巴黎文理研究大学; 上海大学）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究提出量子谱热力学框架与主动学习工作流，以密度泛函精度探索770万高熵陶瓷构型，揭示声子自能效应稳定相并发现约12%溶质阈值，实现高温刚度与低热导率组合。
AI 中文摘要
理解多组分固体的相稳定性并导航广阔的组分空间，仍是固态化学中的核心挑战。在此，我们开发了一个量子谱热力学框架，将相互作用诱导的声子谱展宽与自由能联系起来，并辅以不确定性引导的主动学习工作流，以密度泛函理论精度探索770万个高熵陶瓷构型，实现了10^5倍的加速。我们表明，由化学无序产生的声子自能效应为热力学稳定化提供了超越理想构型熵的内在振动贡献，补偿了不利的混合焓并抑制了相分离。在整个化学空间中，我们揭示了一个稳健的约12原子百分比溶质阈值，将强化与软化区域分开，这与金属-碳反键态的填充相关。化学无序还进一步实现了高温机械刚度与低热导率的异常组合，以及反常的温度依赖性晶格热输运。这项工作为将多体相互作用与热力学和相稳定性联系起来建立了量子谱基础，同时为探索以前无法触及的多组分化学空间提供了一个可扩展的框架。
英文摘要
Understanding phase stability and navigating vast compositional spaces in multicomponent solids remain central challenges in solid-state chemistry. Here, we develop a quantum spectral thermodynamic framework connecting interaction-induced phonon spectral broadening to free energy, alongside an uncertainty-guided active-learning workflow that explores 7.7 million high-entropy ceramic configurations at density-functional-theory fidelity, achieving a $10^5$-fold acceleration. We show that phonon self-energy effects arising from chemical disorder provide an intrinsic vibrational contribution to thermodynamic stabilization beyond ideal configurational entropy, compensating unfavorable mixing enthalpies and suppressing phase separation. Across the chemical space, we uncover a robust ~12 at.% solute threshold separating strengthening and softening regimes, associated with the filling of metal-carbon antibonding states. Chemical disorder further enables an unusual combination of high-temperature mechanical stiffness and low thermal conductivity, together with anomalous temperature-dependent lattice heat transport. This work establishes a quantum spectral foundation for connecting many-body interactions to thermodynamics and phase stability, while providing a scalable framework for exploring previously inaccessible multicomponent chemical spaces.
