arXiv:2503.15432cond-mat.mtrl-scics.LG2025-03被引 5

提出可精准验证的层状材料机器学习势,提升预测准确性十倍。

Accurate, transferable, and verifiable machine-learned interatomic potentials for layered materials

  • 分离层内与层间相互作用,提升模型精度
  • 能量和力预测准确率提升十倍,优于传统方法
  • 用一维超结构验证模型,适合多层材料研究

扭曲的层状范德华材料常表现出非扭曲结构中不存在的独特电子与光学性质。然而,由于大面积莫尔条纹畴的存在,原子结构预测极为困难。本文提出一种分割式机器学习势与数据集优化方法,将层内与层间相互作用解耦,使能量与力预测精度相比传统模型提升十倍。我们指出,传统机器学习势验证指标(能量误差、力误差)在莫尔结构中不充分,进而提出基于堆叠构型分布的物理驱动新指标,可整体比较大规模莫尔条纹域,而非仅依赖小周期胞的局部评估。最后,我们证明一维莫尔结构可作为高效替代系统,实现与第一性原理计算直接对比的实用验证流程。将该框架应用于HfS2/GaS双层体系,发现精确结构预测可直接带来可靠的电子性质预测。该模型无关方法可无缝集成各类层内/层间模型,实现从双层到复杂多层结构的计算可行且严格验证的弛豫模拟。

原文摘要 · Abstract (English)

Twisted layered van-der-Waals materials often exhibit unique electronic and optical properties absent in their non-twisted counterparts. Unfortunately, predicting such properties is hindered by the difficulty in determining the atomic structure in materials displaying large moiré domains. Here, we introduce a split machine-learned interatomic potential and dataset curation approach that separates intralayer and interlayer interactions and significantly improves model accuracy -- with a tenfold increase in energy and force prediction accuracy relative to conventional models. We further demonstrate that traditional MLIP validation metrics -- force and energy errors -- are inadequate for moiré structures and develop a more holistic, physically-motivated metric based on the distribution of stacking configurations. This metric effectively compares the entirety of large-scale moiré domains between two structures instead of relying on conventional measures evaluated on smaller commensurate cells. Finally, we establish that one-dimensional instead of two-dimensional moiré structures can serve as efficient surrogate systems for validating MLIPs, allowing for a practical model validation protocol against explicit DFT calculations. Applying our framework to HfS2/GaS bilayers reveals that accurate structural predictions directly translate into reliable electronic properties. Our model-agnostic approach integrates seamlessly with various intralayer and interlayer interaction models, enabling computationally tractable relaxation of moiré materials, from bilayer to complex multilayers, with rigorously validated accuracy.

机器学习势层状材料莫尔条纹结构预测

Thank you to arXiv for use of its open access interoperability. PaperDance 不是 arXiv 官方产品;中文卡片由大模型生成,请以原文为准。