Navigating Order-(Dis)Order Family Trees via Group-Subgroup Transitions

Abstract

As closed-loop materials discovery systems scale to produce millions of candidate compounds, the credibility of the novelty they reward becomes a critical concern. Novelty is commonly assessed against databases of ordered crystal structures, in which atomic sites are fully occupied. Yet, a predicted ordered structure may simply correspond to a particular ordering of a known disordered phase, whose sites are occupied by multiple species in the statistical average structure; we refer to such a structure as an ordered child of a disordered parent. Here, we introduce order-(dis)order family trees, a symmetry-based framework that organizes ordered and disordered structures through group-subgroup relations and enables novelty to be explicitly evaluated. We develop a high-throughput family matching procedure, to identify possible disordered parents and symmetry-related ordered relatives for a given ordered structure. As validation, we test our framework on synthesis-facing case studies (A-Lab), where it correctly recovers existing disordered parents for the targeted ordered structures. Extending this family-tree-based benchmark to experimental structure databases (ICSD), computational datasets (MP-20, Alex-MP-20, and GNoME), and crystal generative models further reveals that many ordered structures that appear novel as individual entries are, in fact, better understood as members of experimentally known order-(dis)order family trees. We also show that this is particularly evident in symmetry-agnostic all-atom generative models, which more frequently produce ordered structures derived from known disordered parents, whereas symmetry-constrained models are 2-4x less prone to this behavior. Our results establish order-(dis)order family trees as a key requirement for achieving genuine novelty in data-driven materials discovery.