arXiv:2604.02524cond-mat.mtrl-scics.LG2026-04

构建高温卤化物数据集,提升机器学习势函数在电池电解质中的可靠性。

AQVolt26: High-Temperature r$^2$SCAN Halide Dataset for Universal ML Potentials and Solid-State Batteries

  • 基于高温构型采样生成32万条r²SCAN计算数据。
  • 通用模型在高温畸变下能量预测失效,需针对性数据增强。
  • 近平衡弛豫数据对极端应变不友好,仅适合作为补充任务数据。

高安全性、高能量密度电池的需求推动了卤化物固态电解质的研究,其具有更高的离子迁移率、电化学稳定性及界面可变形性。加速发现依赖于大规模分子动力学模拟,这得益于基于基础数据集训练的通用机器学习原子间势。然而,卤化物的动态柔顺性对通用模型在高温高畸变条件下的可靠性构成严峻考验。本文提出AQVolt26,包含322,656条锂卤化物的r²SCAN单点计算数据,覆盖约5K温度下的~5,000种构型。结果表明,基础数据集能提供稳定的卤化物化学基线并良好传递局部力,但高温畸变下的绝对能量预测性能下降。通过与AQVolt26联合训练可解决此盲区。同时,引入Materials Project弛豫数据虽提升近平衡性能,却降低极端应变鲁棒性,且未改善高温力场精度。研究证实,针对特定领域进行构型采样对可靠筛选卤化物电解质至关重要。此外,尽管基础模型提供稳健基础,但在动态软性固态体系中,必须结合高温目标数据才能有效。最后,近平衡弛豫数据更适合作为任务特异性补充,而非普适增益。

原文摘要 · Abstract (English)

The demand for safe, high-energy-density batteries has spotlighted halide solid-state electrolytes, which offer the potential for enhanced ionic mobility, electrochemical stability, and interfacial deformability. Accelerating their discovery requires extensive molecular dynamics, which has been increasingly enabled by universal machine learning interatomic potentials trained on foundational datasets. However, the dynamic softness of halides poses a stringent test of whether general-purpose models can reliably replace first-principles calculations under the highly distorted, elevated-temperature regimes necessary to probe ion transport. Here, we present AQVolt26, a dataset of 322,656 r$^2$SCAN single-point calculations for lithium halides, generated via high-temperature configurational sampling across $\sim$5K structures. We demonstrate that foundational datasets provide a strong baseline for stable halide chemistries and transfer local forces well, however absolute energy predictions degrade in distorted higher-temperature regimes. Co-training with AQVolt26 resolves this blind spot. Furthermore, incorporating Materials Project relaxation data improves near-equilibrium performance but degrades extreme-strain robustness without enhancing high-temperature force accuracy. These results demonstrate that domain-specific configurational sampling is essential for the reliable dynamic screening of halide electrolytes. Furthermore, our findings suggest that while foundational models provide a robust base, they are most effective for dynamically soft solid-state chemistries when augmented with targeted, high-temperature data. Finally, we show that near-equilibrium relaxation data serves as a task-specific complement rather than a universally beneficial addition.

机器学习势固态电池高温数据卤化物电解质

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