We introduce ACEpotentials.jl, a Julia-language software package that constructs interatomic potentials from quantum mechanical reference data using the Atomic Cluster Expansion [R. Drautz, Phys. Rev. B 99, 014104 (2019)]. As the latter provides a complete description of atomic environments, including invariance to overall translation and rotation as well as permutation of like atoms, the resulting potentials are systematically improvable and data efficient. Furthermore, the descriptor’s expressiveness enables use of a linear model, facilitating rapid evaluation and straightforward application of Bayesian techniques for active learning. We summarize the capabilities of ACEpotentials.jl and demonstrate its strengths (simplicity, interpretability, robustness, performance) on a selection of prototypical atomistic modelling workflows.

Langevin dynamics is a versatile stochastic model used in biology, chemistry, engineering, physics and computer science. Traditionally, in thermal equilibrium, one assumes (i) the forces are given as the gradient of a potential and (ii) a fluctuation-dissipation relation holds between stochastic and dissipative forces; these assumptions ensure that the system samples a prescribed invariant Gibbs-Boltzmann distribution for a specified target temperature. In this article, we relax these assumptions, incorporating variable friction and temperature parameters and allowing nonconservative force fields, for which the form of the stationary state is typically not known a priori. We examine theoretical issues such as stability of the steady state and ergodic properties, as well as practical aspects such as the design of numerical methods for stochastic particle models. Applications to nonequilibrium systems with thermal gradients and active particles are discussed.

Adaptive Langevin dynamics is a method for sampling the Boltzmann--Gibbs distribution at prescribed temperature in cases where the potential gradient is subject to stochastic perturbation of unknow...

Summary: Classification with high-dimensional data is of widespread interest and often involves dealing with imbalanced data. Bayesian classification approaches are hampered by the fact that current Markov chain Monte Carlo algorithms for posterior computation become inefficient as the number $p$ of predictors or the number $n$ of subjects to classify gets large, because of the increasing computational time per step and worsening mixing rates. One strategy is to employ a gradient-based sampler to improve mixing while using data subsamples to reduce the per-step computational complexity. However, the usual subsampling breaks down when applied to imbalanced data. Instead, we generalize piecewise-deterministic Markov chain Monte Carlo algorithms to include importance-weighted and mini-batch subsampling. These maintain the correct stationary distribution with arbitrarily small subsamples and substantially outperform current competitors. We provide theoretical support for the proposed approach and demonstrate its performance gains in simulated data examples and an application to cancer data.

Dynamics of coarse-grained particle systems derived via the Mori–Zwanzig projection formalism commonly take the form of a (generalized) Langevin equation with configuration-dependent friction tensor and diffusion coefficient matrix. In this article, we introduce a class of equivariant representations of tensor-valued functions based on the Atomic Cluster Expansion framework that allows for efficient learning of such configuration-dependent friction tensors from data. Besides satisfying the correct equivariance properties with respect to the Euclidean group E(3), the resulting heat bath models satisfy a fluctuation-dissipation relation. We demonstrate the capabilities of the model approach by fitting a model of configuration-dependent tensorial electronic friction calculated from first principles that arises during reactive molecular dynamics at metal surfaces.