arXiv subjects

Laurence I. Midgley

Publications and source records attributed to Laurence I. Midgley.

6 recordsLinked to original sources

arXiv2026

DFT Accuracy on Crystal Structure Prediction with Machine Learning Interatomic Potentials

We present an evaluation of CSP-MACE-Å, a machine learning interatomic potential intended to replace DFT in crystal structure prediction (CSP). We decompose the total energy into separate intramolecular and intermolecular components. For the intramolecular component, we adopt the MACE-POLAR architecture and train it on the OMol25 dataset. The intermolecular component combines three terms: an intermolecular contribution from the MACE-POLAR model, a long-range dispersion term with the functional form of the XDM correction, and a learned delta model trained to reproduce B86bPBE-XDM intermolecular energies. The learned delta model is trained on residual intermolecular targets derived from 50,000 B86bPBE-XDM calculations on molecular crystal structures. On an evaluation set composed of 19 compounds, including a salt, selected from AstraZeneca's previous CSP publications, CSP-MACE-Å achieves performance comparable to PBE DFT with the Neumann-Perrin dispersion correction. On a second evaluation set composed of 28 compounds, including cocrystals and salts, collated from the seven CSP blind tests, CSP-MACE-Å achieves performance close to B86bPBE-XDM DFT. In both evaluation sets, reranking with harmonic free energies substantially improves performance relative to ranking by energy alone. Across our evaluation suite, CSP-MACE-Å is shown to outperform the MACE-POLAR-1 and UMA-OMC foundation models. Lastly, on a set of five compounds, CSP-MACE-Å is shown to capture temperature-dependent trends in the relative stability of polymorphs through estimation of the free energy under the harmonic approximation. By running multiple orders of magnitude faster than DFT, CSP-MACE-Å enables energy and free energy evaluation of far more candidate structures, providing greater confidence when derisking solid forms.

physics.chem-ph↗

arXiv2025

Efficient and Unbiased Sampling from Boltzmann Distributions via Variance-Tuned Diffusion Models

Score-based diffusion models (SBDMs) are powerful amortized samplers for Boltzmann distributions; however, imperfect score estimates bias downstream Monte Carlo estimates. Classical importance sampling (IS) can correct this bias, but computing exact likelihoods requires solving the probability-flow ordinary differential equation (PF-ODE), a procedure that is prohibitively costly and scales poorly with dimensionality. We introduce Variance-Tuned Diffusion Importance Sampling (VT-DIS), a lightweight post-training method that adapts the per-step noise covariance of a pretrained SBDM by minimizing the $α$-divergence ($α=2$) between its forward diffusion and reverse denoising trajectories. VT-DIS assigns a single trajectory-wise importance weight to the joint forward-reverse process, yielding unbiased expectation estimates at test time with negligible overhead compared to standard sampling. On the DW-4, LJ-13, and alanine-dipeptide benchmarks, VT-DIS achieves effective sample sizes of approximately 80 %, 35 %, and 3.5 %, respectively, while using only a fraction of the computational budget required by vanilla diffusion + IS or PF-ODE-based IS.

cs.LG↗

arXiv2024

Efficient and Unbiased Sampling of Boltzmann Distributions via Consistency Models

Diffusion models have shown promising potential for advancing Boltzmann Generators. However, two critical challenges persist: (1) inherent errors in samples due to model imperfections, and (2) the requirement of hundreds of functional evaluations (NFEs) to achieve high-quality samples. While existing solutions like importance sampling and distillation address these issues separately, they are often incompatible, as most distillation models lack the necessary density information for importance sampling. This paper introduces a novel sampling method that effectively combines Consistency Models (CMs) with importance sampling. We evaluate our approach on both synthetic energy functions and equivariant n-body particle systems. Our method produces unbiased samples using only 6-25 NFEs while achieving a comparable Effective Sample Size (ESS) to Denoising Diffusion Probabilistic Models (DDPMs) that require approximately 100 NFEs.

cs.LG↗

arXiv2024

Jumanji: a Diverse Suite of Scalable Reinforcement Learning Environments in JAX

Open-source reinforcement learning (RL) environments have played a crucial role in driving progress in the development of AI algorithms. In modern RL research, there is a need for simulated environments that are performant, scalable, and modular to enable their utilization in a wider range of potential real-world applications. Therefore, we present Jumanji, a suite of diverse RL environments specifically designed to be fast, flexible, and scalable. Jumanji provides a suite of environments focusing on combinatorial problems frequently encountered in industry, as well as challenging general decision-making tasks. By leveraging the efficiency of JAX and hardware accelerators like GPUs and TPUs, Jumanji enables rapid iteration of research ideas and large-scale experimentation, ultimately empowering more capable agents. Unlike existing RL environment suites, Jumanji is highly customizable, allowing users to tailor the initial state distribution and problem complexity to their needs. Furthermore, we provide actor-critic baselines for each environment, accompanied by preliminary findings on scaling and generalization scenarios. Jumanji aims to set a new standard for speed, adaptability, and scalability of RL environments.

cs.LG↗

arXiv2024

SE(3) Equivariant Augmented Coupling Flows

Coupling normalizing flows allow for fast sampling and density evaluation, making them the tool of choice for probabilistic modeling of physical systems. However, the standard coupling architecture precludes endowing flows that operate on the Cartesian coordinates of atoms with the SE(3) and permutation invariances of physical systems. This work proposes a coupling flow that preserves SE(3) and permutation equivariance by performing coordinate splits along additional augmented dimensions. At each layer, the flow maps atoms' positions into learned SE(3) invariant bases, where we apply standard flow transformations, such as monotonic rational-quadratic splines, before returning to the original basis. Crucially, our flow preserves fast sampling and density evaluation, and may be used to produce unbiased estimates of expectations with respect to the target distribution via importance sampling. When trained on the DW4, LJ13, and QM9-positional datasets, our flow is competitive with equivariant continuous normalizing flows and diffusion models, while allowing sampling more than an order of magnitude faster. Moreover, to the best of our knowledge, we are the first to learn the full Boltzmann distribution of alanine dipeptide by only modeling the Cartesian positions of its atoms. Lastly, we demonstrate that our flow can be trained to approximately sample from the Boltzmann distribution of the DW4 and LJ13 particle systems using only their energy functions.

cs.LG↗

arXiv2022

Synthesis of separation processes with reinforcement learning

This paper shows the implementation of reinforcement learning (RL) in commercial flowsheet simulator software (Aspen Plus V12) for designing and optimising a distillation sequence. The aim of the SAC agent was to separate a hydrocarbon mixture in its individual components by utilising distillation. While doing so it tries to maximise the profit produced by the distillation sequence. All actions of the agent were set by the SAC agent in Python and communicated in Aspen Plus via an API. Here the distillation column was simulated by use of the build-in RADFRAC column. With this a connection was established for data transfer between Python and Aspen and the agent succeeded to show learning behaviour, while increasing profit. Although results were generated, the use of Aspen was slow (190 hours) and Aspen was found unsuitable for parallelisation. This makes that Aspen is incompatible for solving RL problems. Code and thesis are available at https://github.com/lollcat/Aspen-RL

cs.LG↗