arXiv subjects

Eszter Varga-Umbrich

Publications and source records attributed to Eszter Varga-Umbrich.

5 recordsLinked to original sources

arXiv2026

Fine-tuning MLIP foundation models: strategies for accuracy and transferability

Adapting machine-learned interatomic potential (MLIP) foundation models to specialised tasks through fine-tuning is an increasingly important practice, yet systematic guidance on when and how to fine-tune is currently limited. We evaluate seven fine-tuning strategies -- naive full-parameter updates, two layer-freezing variants, Low-Rank Adaptation (LoRA), multihead replay, pseudolabelled replay, and replay combined with LoRA -- across five chemically diverse benchmarks (aqueous NaCl, ice polymorphs, S$_\mathrm{N}$2 reactions, SPICE biomolecules, and lithium electrolytes), three generations of foundation models, and training sets spanning five orders of magnitude. To support this evaluation we implement three capabilities in the MACE codebase: LoRA adapted for equivariant message-passing architectures, including both scalar and equivariant linear layers; pseudolabelled replay, which decouples the replay data source from the original pretraining corpus; and model-aware atomic reference energy (E0) reestimation for fine-tuning workflows. We find that foundation model quality, correct E0 initialisation, and well-chosen hyperparameters are prerequisites whose impact routinely exceeds that of the fine-tuning strategy itself. Once these prerequisites are met, most strategies achieve strong target-task accuracy, consistently surpassing models trained from scratch. The practical distinction depends on deployment scope: naive fine-tuning offers the best convergence for single-system applications, while multihead replay -- with either original or pseudolabelled data -- is the only approach tested that consistently preserves out-of-distribution robustness, maintaining both pretraining-distribution accuracy for broader deployment and many-body short-range repulsion.

physics.chem-ph↗

arXiv2026

Machine Learning Interatomic Potentials: Advancing Open-Source Software for Efficient and Scalable Molecular Simulation

Machine learning interatomic potentials (MLIPs) enable atomistic simulations with near ab initio accuracy at significantly reduced computational cost, but their broader adoption is often limited by fragmented tooling, limited scalability, and inflexible software design. We present mlip v2, a new generation of the mlip library that advances efficient and scalable molecular simulation through a unified and extensible framework. The new release features a targeted API redesign with improved modularity and control, enabling flexible customization of training, data processing, and simulation workflows. It further integrates a new high-performance backend for equivariant operations, e3j, significantly accelerating model inference and simulations. In addition, the framework introduces a range of entirely new capabilities, including the eSEN architecture with a Mixture-of-Experts formulation for scalable training on large and diverse datasets, improved handling of electrostatics through more physically grounded charge modeling and long-range interaction treatment, and advanced simulation features such as NPT ensembles and nudged elastic band methods. Together, these extensions significantly broaden the scope of MLIP applications, enabling efficient modeling of complex, reactive, and out-of-equilibrium systems, and bridging the gap between ML research and practical molecular simulation applications. The library is available on GitHub and on PyPI under the Apache license 2.0.

physics.chem-ph↗

arXiv2026

Pretrained Model Representations as Acquisition Signals for Active Learning of MLIPs

Training machine learning interatomic potentials (MLIPs) for reactive chemistry is often bottlenecked by the high cost of quantum chemical labels and the scarcity of transition state configurations in candidate pools. Active learning (AL) can mitigate these costs, but its effectiveness hinges on the acquisition rule. We investigate whether the latent space of a pretrained MLIP already contains the information necessary for effective acquisition, eliminating the need for auxiliary uncertainty heads, Bayesian training and fine-tuning, or committee ensembles. We introduce two acquisition signals derived directly from a pretrained MACE potential: a finite-width neural tangent kernel (NTK) and an activation kernel built from hidden latent space features. On reactive-chemistry benchmarks, both kernels consistently outperform fixed-descriptor baselines, committee disagreement, and random acquisition, reducing the data required to reach performance targets by an average of 38% for energy error and 28% for force error. We further show that the pretrained model induces similarity spaces that preserve chemically meaningful structure and provide more reliable residual uncertainty estimates than randomly initialised or fixed-descriptor-based kernels. Our results suggest that pretraining aligns latent-space geometry with model error, yielding a practical and sufficient acquisition signal for reactive MLIP fine-tuning.

cs.LG↗

arXiv2026

Force-Aware Neural Tangent Kernels for Scalable and Robust Active Learning of MLIPs

Active learning for machine-learning interatomic potentials (MLIPs) must address several challenges to be practical: scaling to large candidate pools, leveraging energy-force supervision, and maintaining robustness when candidate pools are biased relative to the target distribution. In this work, we jointly address these challenges. We first introduce a linearly scaling acquisition framework based on chunked feature-space posterior-variance shortlisting. By avoiding materialisation of the candidate and train set kernels, this approach enables screening of ~200k structures within hours and applies broadly to acquisition strategies that score candidates based on molecular similarity metrics. We then extend the Neural Tangent Kernel (NTK) to a force-aware setting via mixed parameter-coordinate derivatives, yielding a force NTK and a joint energy-force NTK that provide natural similarity metrics for vector-field prediction. We demonstrate the effectiveness of the joint energy-force NTK on the OC20 dataset, where force-aware acquisition is crucial: it achieves the lowest energy and force MAE and RMSE across all metrics and distribution splits. Across T1x, PMechDB, and RGD benchmarks, our force NTK methods remain competitive with established baselines while being significantly more efficient than committee-based approaches. Under a controlled candidate-pool shift case study on T1x, acquisition based on pretrained MLIP embeddings and NTKs remains robust, whereas committee-based methods exhibit higher variance. Overall, these results show that a single pretrained MLIP can enable scalable, force-aware, and distribution-robust active learning for foundation-model fine-tuning.

cs.LG↗

arXiv2025

A foundation model for atomistic materials chemistry

Atomistic simulations of matter, especially those that leverage first-principles (ab initio) electronic structure theory, provide a microscopic view of the world, underpinning much of our understanding of chemistry and materials science. Over the last decade or so, machine-learned force fields have transformed atomistic modeling by enabling simulations of ab initio quality over unprecedented time and length scales. However, early ML force fields have largely been limited by: (i) the substantial computational and human effort of developing and validating potentials for each particular system of interest; and (ii) a general lack of transferability from one chemical system to the next. Here we show that it is possible to create a general-purpose atomistic ML model, trained on a public dataset of moderate size, that is capable of running stable molecular dynamics for a wide range of molecules and materials. We demonstrate the power of the MACE-MP-0 model - and its qualitative and at times quantitative accuracy - on a diverse set of problems in the physical sciences, including properties of solids, liquids, gases, chemical reactions, interfaces and even the dynamics of a small protein. The model can be applied out of the box as a starting or "foundation" model for any atomistic system of interest and, when desired, can be fine-tuned on just a handful of application-specific data points to reach ab initio accuracy. Establishing that a stable force-field model can cover almost all materials changes atomistic modeling in a fundamental way: experienced users get reliable results much faster, and beginners face a lower barrier to entry. Foundation models thus represent a step towards democratising the revolution in atomic-scale modeling that has been brought about by ML force fields.

physics.chem-ph↗