发表机构
Hong Kong University of Science and Technology; IAS Center for AI for Scientific Discoveries; Department of Chemical and Biological Engineering（香港科技大学; IAS科学发现人工智能中心; 化学工程与生物工程系）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究利用自主智能体发现8条无机结构合理性规则（PRIS），可高效筛选晶体结构，其合成评分（PSS）能减少DFT验证工作量，还可解释晶体相关问题，推动晶体诊断筛选发展。
AI 中文摘要
晶体生成器和使用工具的智能体提出候选晶体结构的速度快于密度泛函理论（DFT）能量、声子计算或实验对这些结构的评估速度，因此，判断哪些候选结构值得开展昂贵评估成为了瓶颈，然而大多数筛选仅测试原子重叠，未给出失败的化学原因。本研究中，智能体生成、测试并主动否定了200万条候选定律，最终得到8条无机结构合理性规则（PRIS）。这些规则编码了5种机制：短程排斥、离子接触与堆积、静电平衡、键价守恒以及晶体学位点复杂性。实验结构满足本研究的规则集的比例为82%至99%，但同时满足鲍林规则2至5的比例仅为6.5%。最严格的规则集可检测出87.9%的受损晶体结构，而距离截断法仅能检测1.6%至3.2%。PRIS合理性与可合成性呈线性相关，因此基于PRIS的合成评分（PSS）可解释性地筛选出83.7%的难合成结构，同时保留80.7%的实验结构。在属性约束的逆设计运行中，PRIS和PSS可将DFT验证队列最多减少67.3%，并保留99.2%的DFT验证后体积模量达到设计目标的候选结构。除筛选外，PRIS还解释了GNoME为何富含罕见的低对称结构，并揭示了伪造晶体报告中的错误元素分配如何隐藏在看似合理的坐标之后。PRIS将筛选从“通过/不通过”的判定转变为给出失败的化学原因，表明自主智能体可通过主动否定发现指导计算与实验的物理化学定律。
英文摘要
Crystal generators and tool-using agents propose structures faster than density functional theory (DFT) energy and phonon calculations or experiments can assess them. Deciding which candidates merit expensive assessment is therefore the bottleneck, yet most screens test little beyond atomic overlap and give no chemical reason for failure. Here, our agents generate, test and actively refute two million candidate laws, leaving eight Plausibility Rules for Inorganic Structures (PRIS). These laws encode five mechanisms: short-range repulsion, ionic contact and packing, electrostatic balance, bond-valence conservation and crystallographic site complexity. Experimental structures satisfy our law sets at 82--99%, but satisfy Pauling's rules 2--5 together at only 6.5%. The strictest set detects 87.9% of damaged crystal structures, whereas distance cutoffs detect only 1.6--3.2%. PRIS plausibility is linearly correlated with synthesizability, so the PRIS-derived synthesis score (PSS) explainably screens 83.7% of hard-to-synthesize structures while retaining 80.7% of experimental structures. In a property-conditioned inverse-design run, PRIS and PSS can reduce the DFT validation queue by up to 67.3% and keep 99.2% of the candidates whose DFT-validated bulk moduli reach the design target. Beyond screening, PRIS explains why GNoME remains enriched in rare low-symmetry structures and reveals how wrong-element assignments in falsified crystal reports hide behind plausible coordinates. PRIS moves screening from a pass-or-fail verdict to a chemical reason for failure, showing that autonomous agents can discover, by active refutation, physicochemical laws that guide calculations and experiments.
