用主动拒绝机制,用极少真实数据训练出更可靠的分子力场模型。
Active rejection enables reliable generalization of universal machine-learning interatomic potentials

- 通过多教师投票和不确定性判断,筛选可信预测并拒绝不可靠结构。
- 仅用0.2%真实数据生成289万条高质量伪标签,性能超越基准模型。
- 适合需要高精度、高鲁棒性分子模拟的材料科学家和工程师。
通用机器学习原子间势(uMLIPs)兼具量子力学精度与大规模分子动力学效率,但高精度计算如r²SCAN的成本限制了训练数据规模。现有模型虽平均表现良好,却无法保证每个结构的预测可靠性。本文提出自适应多教师路由(ATR),将高保真数据构建转化为结构级不确定性决策问题。利用仅0.2%候选结构的真实r²SCAN标签,ATR校准多个预训练uMLIP教师,结合结构描述符、教师身份及教师间分歧,评估每对结构-教师的可靠性。选择高置信度预测用于伪标签生成,并拒绝无足够可靠教师的结构。最终生成289万条可追溯的r²SCAN级伪标签用于预训练。在保留的r²SCAN结构和MP-r²SCAN基准上,基于ATR数据训练的轻量级CHGNet始终优于基线与非路由对照组。有限温度分子动力学表明,ATR在多种材料体系中提升了动态鲁棒性,使模拟轨迹稳定运行,而基线模型出现灾难性结构坍塌。结果证明,主动拒绝是构建可扩展、高可靠性的高保真uMLIP数据系统的有效机制。
原文摘要 · Abstract (English)
Universal machine learning interatomic potentials (uMLIPs) bridge quantum-mechanical accuracy and large-scale molecular dynamics, but the cost of high-accuracy calculations such as r$^2$SCAN limits training to datasets that remain small relative to the open materials space. Strong average benchmark performance also does not guarantee reliable energy--force predictions for every structure. We propose Adaptive Multi-Teacher Routing (ATR), which reformulates high-fidelity data construction as a structure-wise decision problem under uncertainty. Using a small set of real r$^2$SCAN labels, ATR calibrates multiple pretrained uMLIP teachers and combines structural descriptors, teacher identity, and inter-teacher disagreement to estimate the reliability of each structure--teacher pair. It selects high-confidence predictions for pseudo-label generation and rejects structures for which no teacher is sufficiently reliable. With real r$^2$SCAN labels for only 0.2\% of candidate structures, ATR distils 2.89 million traceable r$^2$SCAN-level pseudo-labels for pretraining. On held-out r$^2$SCAN structures and the MP-r$^2$SCAN benchmark, a lightweight CHGNet trained on the ATR-generated dataset consistently outperforms the baseline and non-routed controls. Finite-temperature molecular dynamics further shows that ATR improves dynamical robustness across multiple material systems, maintaining stable trajectories where baseline simulations undergo catastrophic structural collapse. These results establish active rejection as an effective mechanism for converting multiple pretrained uMLIPs into a scalable and reliable data-construction system for high-fidelity uMLIPs.
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