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Keith T Butler

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Open access Aug 2026

A multi-scale mixture of experts model for cross-size structural prediction of Cu nanoparticles

Predicting structures and energetics of metallic nanoparticles across wide size ranges remains challenging because the balance of interaction scales changes rapidly with system size. We introduce a multi-scale Mixture-of-Experts (MoE) architecture for Cu clusters and nanoparticles that explicitly separates short-, medium-, and long-range interactions using three specialised machine-learning interatomic potential experts combined through a learnable size-conditioned gating network. The resulting MoE aggregates per-atom energies into a single conservative potential, ensuring forces are obtained as energy gradients and enabling stable molecular dynamics. Across mixed cluster-nanoparticle test sets, the MoE improves accuracy relative to both an off-the-shelf foundation potential and a finetuned single-expert baseline. Stress tests show that force errors remain comparatively stable across cluster sizes and that the model retains robust energetics under morphology out-of-distribution shifts quantified using a structural outlier score based on similarity measures. The learned gating weights further provide an interpretable, size-dependent decomposition of interaction scales. Finally, validation against linear-scaling density functional theory using the ONETEP code, together with finite-temperature molecular dynamics tests, demonstrates consistent energetics, stable force behaviour, and well-behaved dynamical trajectories, supporting the use of the model for efficient structural optimisation and configurational sampling across nanoparticle sizes.

Yunyu Zhang, Keith T Butler, C. Richard A. Catlow · 0 citations
Preprint Aug 2026

Building atomistic models of heterointerfaces with optimal transport

Heterogeneous interfaces underpin technologies from microelectronics to energy conversion and storage, but their configurational complexity precludes exhaustive first-principles screening of interface registries. Although data-driven approaches can alleviate this burden, they remain limited by sparse interface datasets. Here, we introduce an energy-independent workflow that represents coherent interfaces as attributed graphs, quantifies their similarity to parent bulk environments using the fused Gromov-Wasserstein (FGW) distance, and couples this metric with Bayesian optimization over the in-plane registry space. We assess the approach for KI/NaCl, GaP/GaAs and GaN/$\mathrm{Al_{2}O_{3}}$ interfaces spanning ionic, covalent and mixed-bonding regimes, using hierarchical validation with MACE and density functional theory (DFT). Comparison with single-point energy landscapes shows that the FGW distance captures registry-dependent periodicity, while interfaces exhibit deviations between structural and energetic extrema, reflecting additional chemistry-specific contributions. Furthermore, FGW distances show an overall association with relaxed energies. Under limited screening budgets, FGW-guided registry selection consistently outperforms random search and is more robust across interface systems than selection guided by pretrained MACE energies. The workflow converts the qualitative notion of bulk-like continuity into a quantitative prescreening criterion, enabling efficient registry exploration and providing physically informed candidate structures for materials discovery workflows.

Yuxuan Tang, Keith T Butler · 0 citations