arXiv subjects

Kevin K. Huguenin-Dumittan

Publications and source records attributed to Kevin K. Huguenin-Dumittan.

6 recordsLinked to original sources

arXiv2026

Overcoming the limitations of body-ordered potentials for atomistic machine learning

Machine-learning interatomic potentials have become indispensable tools in atomistic simulations. The most popular models rely heavily on physical priors, such as locality, smoothness and symmetry, that are assumed to improve the accuracy and transferability of the trained models. However, recent evidence suggests that, in the data-rich regime, unconstrained models that learn symmetry from the data can achieve very competitive accuracy and computational efficiency, without sacrificing stability and generalization power. Many equivariant symmetric architectures historically rely on the assumption that the interatomic potential can be approximated well by a convergentcluster expansion, i.e., a decomposition in terms associated to atomic pairs, triplets, quadruplets, and higher-order tuples. We describe an architecture that incorporates locality, smoothness, and symmetry priors, but that -- thanks to a computationally efficient tensor product formulation -- does not assume low-order truncation of the body-ordered series.

physics.chem-ph↗

arXiv2025

Fast and flexible long-range models for atomistic machine learning

Most atomistic machine learning (ML) models rely on a locality ansatz, and decompose the energy into a sum of short-ranged, atom-centered contributions. This leads to clear limitations when trying to describe problems that are dominated by long-range physical effects - most notably electrostatics. Many approaches have been proposed to overcome these limitations, but efforts to make them efficient and widely available are hampered by the need to incorporate an ad hoc implementation of methods to treat long-range interactions. We develop a framework aiming to bring some of the established algorithms to evaluate non-bonded interactions - including Ewald summation, classical particle-mesh Ewald (PME), and particle-particle/particle-mesh (P3M) Ewald - into atomistic ML. We provide a reference implementation for pyTorch as well as an experimental one for JAX. Beyond Coulomb and more general long-range potentials, we introduce purified descriptors which disregard the immediate neighborhood of each atom, and are more suitable for general long-ranged ML applications. Our implementations are fast, feature-rich, and modular: They provide an accurate evaluation of physical long-range forces that can be used in the construction of (semi)empirical baseline potentials; they exploit the availability of automatic differentiation to seamlessly combine long-range models with conventional, local ML schemes; and they are sufficiently flexible to implement more complex architectures that use physical interactions as building blocks. We benchmark and demonstrate our torch-pme and jax-pme libraries to perform molecular dynamics simulations, to train ML potentials, and to evaluate long-range equivariant descriptors of atomic structures.

physics.chem-ph↗

arXiv2025

Adaptive energy reference for machine-learning models of the electronic density of states

The electronic density of states (DOS) provides information regarding the distribution of electronic energy levels in a material, and can be used to approximate its optical and electronic properties and therefore guide computational material design. Given its usefulness and relative simplicity, it has been one of the first electronic properties used as target for machine-learning approaches going beyond interatomic potentials. A subtle but important point, well-appreciated in the condensed matter community but usually overlooked in the construction of data-driven models, is that for bulk configurations the absolute energy reference of single-particle energy levels is ill-defined. Only energy differences matter, and quantities derived from the DOS are typically independent on the absolute alignment. We introduce an adaptive scheme that optimizes the energy reference of each structure as part of the training process, and show that it consistently improves the quality of ML models compared to traditional choices of energy reference, for different classes of materials and different model architectures. On a practical level, we trace the improved performance to the ability of this self-aligning scheme to match the most prominent features in the DOS. More broadly, we believe that this work highlights the importance of incorporating insights into the nature of the physical target into the definition of the architecture and of the appropriate figures of merit for machine-learning models, that translate in better transferability and overall performance.

cond-mat.mtrl-sci↗

arXiv2024

Expanding Density-Correlation Machine Learning Representations for Anisotropic Coarse-Grained Particles

Physics-based, atom-centered machine learning (ML) representations have been instrumental to the effective integration of ML within the atomistic simulation community. Many of these representations build off the idea of atoms as having spherical, or isotropic, interactions. In many communities, there is often a need to represent groups of atoms, either to increase the computational efficiency of simulation via coarse-graining or to understand molecular influences on system behavior. In such cases, atom-centered representations will have limited utility, as groups of atoms may not be well-approximated as spheres. In this work, we extend the popular Smooth Overlap of Atomic Positions (SOAP) ML representation for systems consisting of non-spherical anisotropic particles or clusters of atoms. We show the power of this anisotropic extension of SOAP, which we deem \AniSOAP, in accurately characterizing liquid crystal systems and predicting the energetics of Gay-Berne ellipsoids and coarse-grained benzene crystals. With our study of these prototypical anisotropic systems, we derive fundamental insights into how molecular shape influences mesoscale behavior and explain how to reincorporate important atom-atom interactions typically not captured by coarse-grained models. Moving forward, we propose \AniSOAP as a flexible, unified framework for coarse-graining in complex, multiscale simulation.

physics.comp-ph↗

arXiv2023

Completeness of Atomic Structure Representations

In this paper, we address the challenge of obtaining a comprehensive and symmetric representation of point particle groups, such as atoms in a molecule, which is crucial in physics and theoretical chemistry. The problem has become even more important with the widespread adoption of machine-learning techniques in science, as it underpins the capacity of models to accurately reproduce physical relationships while being consistent with fundamental symmetries and conservation laws. However, some of the descriptors that are commonly used to represent point clouds -- most notably those based on discretized correlations of the neighbor density, that underpin most of the existing ML models of matter at the atomic scale -- are unable to distinguish between special arrangements of particles in three dimensions. This makes it impossible to machine learn their properties. Atom-density correlations are provably complete in the limit in which they simultaneously describe the mutual relationship between all atoms, which is impractical. We present a novel approach to construct descriptors of \emph{finite} correlations based on the relative arrangement of particle triplets, which can be employed to create symmetry-adapted models with universal approximation capabilities, which have the resolution of the neighbor discretization as the sole convergence parameter. Our strategy is demonstrated on a class of atomic arrangements that are specifically built to defy a broad class of conventional symmetric descriptors, showcasing its potential for addressing their limitations.

physics.chem-ph↗

arXiv2023

Physics-inspired Equivariant Descriptors of Non-bonded Interactions

One essential ingredient in many machine learning (ML) based methods for atomistic modeling of materials and molecules is the use of locality. While allowing better system-size scaling, this systematically neglects long-range (LR) effects, such as electrostatics or dispersion interaction. We present an extension of the long distance equivariant (LODE) framework that can handle diverse LR interactions in a consistent way, and seamlessly integrates with preexisting methods by building new sets of atom centered features. We provide a direct physical interpretation of these using the multipole expansion, which allows for simpler and more efficient implementations. The framework is applied to simple toy systems as proof of concept, and a heterogeneous set of molecular dimers to push the method to its limits. By generalizing LODE to arbitrary asymptotic behaviors, we provide a coherent approach to treat arbitrary two- and many-body non-bonded interactions in the data-driven modeling of matter.

physics.chem-ph↗