发表机构
Institute of Artificial Intelligence, Hefei Comprehensive National Science Center; University of Science and Technology of China; Laboratory of Quantum Information; Hefei National Laboratory（合肥人工智能研究院，合肥综合性国家科学中心; 中国科学技术大学; 量子信息实验室; 合肥国家实验室）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过机器学习原子模拟揭示界面取向和晶体学匹配可控制HfO2多晶型相稳定性，并降低相变势垒，为稳定亚稳相提供新策略。
AI 中文摘要
HfO$_2$表现出丰富的多晶型现象，不同相之间的竞争支撑着其许多功能特性。然而，仅凭体相自由能关系无法解释混合相边界处的相选择，在混合相边界处，界面取向和结构连续性约束了集体重排。在此，我们利用机器学习原子模拟和以Hf为中心的局域相分类方案，证明了晶体学界面匹配会改变相竞争和可及的转变路径。在300至1800 K的3 ns模拟中，M(100)/T(100)界面始终保持为M/T混合物。M/PO、M/AO和PO/AO界面在高达900 K时保持两相共存，而所有T/PO界面均变为PO主导。在1800 K时，所有非M界面均变为T主导，而含M界面则保持单斜相多数。微移弹性带计算揭示了通过界面态的较低势垒路径。对于M(100)$\rightarrow$T(100)，长胞（$\sim$12 nm）中的界面介导路径产生的势垒为136.03 meV/f.u.，比短胞（$\sim$3 nm）中的直接路径低29.2%。这一差异与短胞中不存在的顺序相前沿运动有关。这些结果将相边界确定为相稳定性和转变的积极参与者，并确立了界面取向和晶体学匹配作为稳定亚稳多晶型和引导HfO$_2$中相转变的变量。
英文摘要
HfO$_2$ exhibits rich polymorphism, and competition among different phases underpins many of its functional properties. Yet bulk free-energy relations alone cannot explain phase selection at mixed-phase boundaries, where interface orientation and structural continuity constrain collective rearrangements. Here, using machine-learning atomistic simulations and a Hf-centered local phase classification scheme, we show that crystallographic interface matching redirects phase competition and accessible transformation pathways. The M(100)/T(100) interface remains pinned as an M/T mixture throughout 3 ns simulations from 300 to 1800 K. M/PO, M/AO, and PO/AO interfaces retain two-phase coexistence up to 900 K, whereas all T/PO interfaces become PO-dominant. At 1800 K, all non-M interfaces become T-dominant, while M-containing interfaces retain a monoclinic majority. Nudged elastic band calculations reveal lower-barrier routes through interface states. For M(100)$\rightarrow$T(100), the interface-mediated route in a long cell ($\sim$12 nm) yields a barrier of 136.03 meV/f.u., 29.2 % lower than the direct route in a short cell ($\sim$3 nm). This difference is associated with sequential phase-front motion absent from the short cell. These results identify phase boundaries as active participants in phase stability and transformation and establish interface orientation and crystallographic matching as variables for stabilizing metastable polymorphs and directing phase conversion in HfO$_2$.
DOI：10.1038/s41524-026-02353-x
