materials simulation teams

Abstract: We introduce machine learning models that accurately predict the electron density, the central variable of density functional theory. They are built on Transformer-inspired architectures, which require little computation per parameter and can therefore be enlarged at low cost. The proposed models, SwinUNETR-V2 and its attention-free counterpart NeXtUNETR, achieve state-of-the-art accuracy on QM9, with normalized mean absolute errors in the density averaging 0.075% and 0.046%, respectively. The predicted densities are accurate enough to bypass the self-consistent iteration: a single Kohn-Sham step reproduces the self-consistent electronic structure. For NeXtUNETR, the median errors are 0.036 meV in the total energy, 0.65 meV/angstrom in the forces and 1.8 meV in the HOMO-LUMO gap. The forces not only recover the self-consistent minima in geometry optimization but also successfully drive ab initio molecular dynamics. Fine-tuned on small datasets, both networks also transfer accurately to systems containing elements absent from QM9 or larger than its molecules.

Abstract: Rotationally equivariant architectures improve the physical fidelity of machine-learned (ML) universal materials models based on graph neural networks (GNNs). However, their scalability is limited by the use of non-trivial, high-precision tensor operations during both training and inference. Adopting the reduced-precision formats of matrix multiplication units (MMUs), e.g., FP8 instead of FP32, provides massive increases in throughput, up to 30x (60x) on NVIDIA Hopper (Blackwell) GPUs, but may lead to drastic loss of accuracy. Here, we introduce tailored 'emulated' low-precision operations under the integer Ozaki scheme to accelerate the 'SO(2)-equivariant' processing layers of GNNs, which dominate the runtime of (1) many state-of-the-art ML interatomic potentials (MLIPs) and (2) most universal ML Hamiltonian (MLH) models. Our framework, FlashSO(2), outperforms TF32, the most accurate native low-precision MMU format, in throughput, accuracy, and memory footprint at once. At the SO(2) layer level, it reaches 40x (7x) the throughput of MALOQ's (UMA's) reference implementation, an MLH (MLIP) model, sustaining up to 236 (232) effective Tflop/s on an NVIDIA GH200, 3.5x the FP32 peak. At the model level, FlashSO(2) helps train MALOQ 3.9x faster than its pure-FP32 version while reducing peak memory by 58% at no loss in accuracy. In molecular dynamics simulations with UMA, the speedup factor is 3.3x, and the peak memory is reduced by 51%. FlashSO(2) thus pushes the speed-accuracy Pareto frontier of equivariant materials models beyond the native low-precision formats and substantially lowers the resources required to exploit their scaling laws.

Abstract: Simulating molecular excited-state processes requires resolving electronic and nuclear dynamics, but the cost of direct quantum-chemical calculations limits accessible system sizes and timescales. Machine-learning models can extend these simulations, yet they often need to be tailored to specific molecular systems and scientific objectives. Building and deploying such models requires coordinated decisions across conformational sampling, quantum-chemical labelling, model training, validation and dynamics. Here we introduce Paired agents for Unified Learning and Simulation of Excited States (PULSES), a multi-agent system that automates this workflow within expert-approved boundaries. A human expert and planner define the scientific objective, methods and decision boundaries, while an orchestrator coordinates domain agents and artifact-specific scientific assurance during execution. We evaluate PULSES on 15 computational chemistry tasks and demonstrate end-to-end applications to perylene exciton Hamiltonians, solvent-dependent biphenyl relaxation, and excited-state proton transfer in 10-hydroxybenzo[h]quinoline. These results demonstrate traceable, expert-bounded construction and deployment of specialized excited-state models, while retaining scientific validation as a requirement rather than assuming that successful execution establishes correctness.

Abstract: Collective ordering in correlated electron systems emerges from microscopic dynamics, yet the evolution of observable textures need not admit a closed, memoryless description. We introduce a graph-recurrent neural network (GRNN) framework that learns such emergent dynamics directly from trajectories without specifying microscopic equations of motion. The framework integrates gated recurrent memory with graph message passing: local hidden states encode information beyond the instantaneous observables, while spatial coupling allows this information to propagate between sites. The observable and hidden fields evolve jointly through a shared local rule, providing a scalable representation of dynamics with spatial interactions and temporal memory. We demonstrate this framework on the emergent dynamics of charge-density-wave order in the semiclassical Holstein model, successfully reproducing temporal and spatial correlations and dynamical scaling during domain coarsening. By learning finite-time evolution directly, the GRNN offers a route to efficient, data-driven descriptions of collective dynamics with unresolved microscopic degrees of freedom.

Abstract: Residual stress remains in an object even in the absence of external forces or thermal pressure, which, in turn, may cause significant plastic deformations. In case the residual stress creates unwanted effects on the material and so is undesirable, an efficient solution is necessary to track and eliminate this stress. Smoothed Particle Hydrodynamics has been extensively used in solid mechanics simulations and the inherent colour-field generation approach is a promising tracker for the residual stress. In this paper, we propose a way to use the colour-field approach for eliminating the residual stress and prevent the undesirable premature failure of solid objects.

Abstract: Accurate atomistic simulations of materials under electric fields require long-range electrostatics and electrical-response modeling at length scales beyond the reach of conventional first-principles methods. Yet these capabilities remain difficult to reconcile with the scalability of machine-learning interatomic potentials (MLIPs). Strictly local models enable efficient spatial parallelization but neglect long-range interactions, whereas existing electrostatic extensions introduce global dependencies that hinder distributed computation. Here, we overcome this limitation by analytically separating the long-range electrostatic forces and Born effective charges (BECs) into a global electrostatics calculation and strictly local derivatives of learned latent charges. This formulation preserves the spatial decomposability of equivariant MLIPs while enabling distributed evaluation of energies, forces, stresses, and BECs across different boundary conditions. Implemented as DPA4C-LR on the \texttt{nvalchemi} platform, the framework scales to 5.2 million atoms on four GPUs at approximately twice the computational cost of its short-range backbone. Trained on energies and forces, DPA4C-LR accurately infers BECs and reproduces the field-dependent infrared spectra of water. We further demonstrate its capabilities by recovering the characteristic slim polarization hysteresis of relaxor \ce{Pb(Mg_{1/3}Nb_{2/3})O3}, which is obscured by finite-size effects in smaller simulations; predicting a room-temperature field-driven ionic conductivity of $6.8 \pm 0.7$~mS/cm in amorphous \ce{Li_{0.9}NbO_{0.9}Cl_{4.1}}; and modeling interfacial thermal transport across Si/diamond interfaces with slab-corrected electrostatics. By combining long-range physics, electrical-response inference, and distributed computation, this framework extends predictive atomistic modeling toward device-relevant length scales.

Abstract: Accurate electronic band structures are essential for predicting material properties, but high-fidelity calculations are computationally demanding. We introduce O-kRystal, a dual-space orbital-learning framework that uses a lower-cost Perdew-Burke-Ernzerhof (PBE) calculation as both an energy baseline and a source of structured orbital information. Combining PBE band energies with real- and reciprocal-space orbital matrices, O-kRystal predicts higher-level corrections for individual electronic states as a function of crystal momentum and spin. For states within 5 eV of the band-edge midpoint, it predicts Heyd-Scuseria-Ernzerhof (HSE06) band energies with a mean absolute error of $0.171 \pm 0.009$ eV across nearly 6,000 three-dimensional materials spanning insulating, metallic, magnetic, and nonmagnetic systems. On a separate benchmark of six strongly correlated materials, it reduces the corresponding PBE band-energy MAE by 68.7% and resolves orbital-dependent changes in the relative placement of transition-metal d and ligand p states. Despite training only at high-symmetry points, it maintains comparable accuracy at unseen points along band paths and reconstructs HSE06 densities of states from dense Brillouin-zone predictions. Finally, training O-kRystal on $G_0W_0$ quasiparticle energies for two-dimensional materials demonstrates its applicability across levels of theory and the potential of orbital learning for higher-fidelity, momentum-resolved electronic-structure prediction beyond density functional theory.

Abstract: Automated materials discovery requires evaluating large pools of candidate configurations, with density functional theory (DFT) as a major throughput bottleneck. Pretrained machine-learned interatomic potentials (MLIPs) approximate DFT cheaply, but their errors vary by orders of magnitude across configurations, making it difficult to decide when to trust the MLIP predictions and when to fall back to DFT. We frame this decision as a risk-controlled selection problem and solve it within a conformal risk control (CRC) framework. Each configuration is mapped from atomic numbers and Cartesian coordinates to a fixed geometric descriptor, which a lightweight predictor uses to estimate an MLIP-DFT disagreement score in energy, average force, and maximum force. CRC then calibrates this score into a selection threshold for DFT labeling such that the MLIP error on the unselected configurations, which keep their MLIP labels, stays below a user-chosen fraction $α$ of the expected error. Under an identical guarantee across eight dataset-MLIP pairs, our predictor routes 7% and 14% fewer configurations to DFT at $α=0.3$ than committee baselines. Because committee disagreement overlooks errors the MLIPs share, our gains are largest when the DFT labels and MLIP training data differ in DFT functional and basis set, and narrow when the two agree. Without model access, the structure-only predictor also ranks errors as well as the target MLIP's latent representation and outperforms widely used descriptors such as Smooth Overlap of Atomic Positions (SOAP) and Atom-Centered Symmetry Functions (ACSF).

Abstract: We introduce STRUCTURES-P, a machine-learned all-electron orbital-free density functional for periodic CHNO systems. Electrostatics are evaluated analytically in an atom-centered Gaussian basis, while an equivariant network learns the kinetic and exchange-correlation energy from energies and gradients of non-ground-state densities. Minimizing the functional from a superposition of atomic densities recovers the Kohn-Sham ground state: on held-out crystals, the density error falls from 6.7% to 0.4% of the electron count and the energy error reaches 0.25 mHa per atom, half that of a same-architecture interatomic potential. A single functional can be trained for both isolated molecules and periodic systems, and the model generalizes to larger unit cells. It largely preserves relative-energy rankings and reproduces convex-hull vertices on the tested H-N composition slice. Together, these results demonstrate the viability of machine-learned all-electron orbital-free DFT for variational density optimization and energy evaluation in fixed-geometry solids.

Abstract: Predicting thermally activated diffusion and defect evolution with event-driven models requires identifying atomic rearrangement mechanisms and their activation barriers. Discovering the associated saddle points is a major computational bottleneck: multiple rearrangements may originate from one metastable state, while costly local searches can fail or repeatedly converge to the same saddle. To address this challenge, we introduce ASPIRE (Atomistic Saddle-Point Inference with Refinement for Events), a framework that predicts a set of saddle candidates from a single initial atomic environment and refines them through Dimer searches on the original interatomic potential. The framework's equivariant set predictor, Ev-Quiformer, integrates (i) geometry-conditioned scalar-vector event slots for generating multiple saddle-point proposals and (ii) a decoder that maps each slot to a full atomic displacement field by combining atom, slot, and anchor-relative vectors with invariant coefficients. We also contribute two datasets: (i) BCCFE4VACAV-4000, comprising 4,000 four-vacancy body-centered cubic iron configurations and 65,450 reference events grouped by initial state for set supervision and post-refinement evaluation; and (ii) BCCFE-1TO4VAC, comprising 5,372 configurations with one to four vacancies each. Theoretically, we establish conditions for proposal equivariance. Experimentally, ASPIRE achieves 77.20% reference-event coverage on this benchmark, compared with 75.73% for a conventional Dimer baseline, while requiring approximately half as many Dimer force evaluations. In a timing evaluation on 50 configurations, ASPIRE reduces wall time per configuration from 478.8 s to 176.3 s under the stated hardware settings.

Abstract: A holographic superconductor whose scalar mass depends on the gauge field strength, $M(\Fsq)$, reproduces a superconducting dome for a suitable $M$, and recovering that $M$ from a given dome has so far taken days for a single training run. We propose a new way of training this model, with which an inversion takes from about ten minutes to an hour. Training needs the gradient of the condition that fixes the critical temperature, which the earlier method obtains by finite differences, repeating the bulk integrations for every training parameter. Here that condition is obtained, without any fit, from two integrations started at the horizon and at the boundary, and its derivative with respect to $M$ is an integral over the same two solutions, so the gradient needs no integration of its own. We use the speed to study the part of $M$ that a dome cannot determine, on the interval between the value $\Fsq$ takes at the horizon for the lowest doping and $\Fsq=0$, at which $M$ is the scalar mass $M(0)$ that fixes the dimension of the dual operator. We hold the scalar mass at several values, which we call pinned masses, retrain everything else at each, and find that the reconstructions agree wherever the horizons of the dome reach, including the minima of $M$, and differ only on that interval. A rule that keeps the reconstruction with the simplest closed form recovers both the scalar mass and the mass function of a test dome. On Gaussian and double-Gaussian domes and on the measured phase diagrams of YBa$_{2}$Cu$_{3}$O$_{y}$ and 2M-WS$_{2}$, however, the pinned mass it keeps rests on ties or on narrow margins, so for these targets the scalar mass is left open. The dome thus constrains $M$ where its horizons reach, and fixing the dimension of the dual operator needs a second observable.

Abstract: Magneto-active elastomers, as a class of smart materials, exhibit strongly coupled magnetic and mechanical behavior at finite strains. Considering variations in microstructure, material properties, and geometry can lead to computationally expensive analyses. Building on the finite operator learning (FOL) framework, this study develops a data-free, physics-informed operator-learning framework for families of coupled finite-strain magneto-mechanical boundary-value problems. The governing magnetostatic and mechanical equations are enforced through finite-element weak-form residuals, allowing the neural operators to be trained without labeled finite-element solution data. The main contribution of this study is the development of a weak-form staggered neural operator (WSNO) framework for strongly coupled magneto-mechanical saddle-point problems. Separate magnetic and mechanical neural operators are trained alternately using a staggered optimization strategy, while their physical coupling is retained through the constitutive relations and residual evaluations. The resulting framework learns mappings from parameterized material and geometric descriptions to the corresponding coupled magnetic and mechanical solution fields. The proposed framework is investigated across several settings, including heterogeneous random-inclusion microstructures, varying magnetic phase contrast, area-fraction-dependent geometries, strongly out-of-distribution material morphologies, and three-dimensional geometry-parametric problems. In addition, the learned operator is combined with a neural-initialized Newton strategy, in which the nonlinear finite-element solver is initialized using the neural prediction. The results demonstrate that the proposed operator-learning framework can accurately capture coupled magneto-mechanical responses across a broad range of parametric problem settings.

Abstract: Sampling from Boltzmann distributions of molecular systems is an inference problem that has seen significant recent developments fuelled by advances in neural density estimation. We develop a novel sampling algorithm, Neural Transport Nested Sampling (NTNS), which combines the classical strengths of nested sampling with modern neural flow-based methods. NTNS uses a flow matching velocity as the drift in a Metropolis--Hastings corrected Langevin kernel inside a nested sampling outer loop, requiring only evaluations of the target energy function and providing scalable estimation of the full partition function of high-dimensional particle systems. We benchmark NTNS on challenging molecular sampling benchmarks, scaling up to Lennard--Jones clusters of 55 interacting particles, where it reduces both interatomic distance and energy Wasserstein errors to reference MCMC by over an order of magnitude relative to the strongest neural baselines at lower wall-clock cost. To our knowledge, NTNS is also the first neural sampler to return a calibrated, temperature resolved partition function estimate at this scale, recovering the phase structure across temperature from a single run.

Abstract: In scientific machine learning, $Δ$-learning trains models on residual errors relative to physical baselines, assuming that more accurate baselines with smaller residual scales inherently improve downstream performance. Here, we demonstrate that residual scale alone is an insufficient heuristic for learnability. Evaluating molecular graph neural networks on total energy targets, we show that complex local descriptor baselines can yield small residual targets that are disproportionately rough within architecture-informed proxy spaces and harder to learn relative to their scale. Conversely, semi-empirical baseline reduces both scale and normalized roughness, improving in-domain and out-of-domain prediction. We introduce scale-normalized graph Dirichlet roughness ($D_{\text{IQR}}$) as a pre-training diagnostic for residual learnability and establish baseline complementarity as a core target-design principle, elevating target space formulation alongside model architecture as a key axis for scientific machine learning.

Abstract: Machine learning interatomic potentials (MLIPs) learn the mapping from atomic positions to potential energy. The forces, the negative gradient of this energy, drive molecular dynamics and are readily obtained using automatic differentiation. Higher-order derivatives, most notably the Hessian, describe collective motion and allow the direct prediction of experimental observables, but are considered computationally inaccessible for large systems. We suggest a solution: in physical systems, interactions decay with distance, and most MLIPs build on this locality through message passing up to a finite receptive field. This implies both sparsity of higher-order derivatives and their decay with distance. This structure can be exploited using automatic sparse differentiation (ASD). We explain how to compute the sparsity pattern for MLIP derivatives and demonstrate that, for multiple foundation MLIPs, ASD computes full Hessians of large porous materials exactly, but with modest speedups at best. The larger gains come from truncated ASD: discarding small, but nonzero, Hessian entries between distant atoms yields order-of-magnitude speedups with negligible impact on predicted observables.

Abstract: Studying the dynamical behavior of a system often depends on characterizing how it transitions between long-lived states. Because such transitions are rare, observing them usually requires specialized enhanced sampling techniques. Transition Path Sampling (TPS) is a well-established method for generating reactive trajectories, which is simple to implement and does not require the definition of a preconceived reaction coordinate. However, its efficiency is limited by its sequential nature and the resulting correlations between sampled paths. Previous work addressed this limitation by combining TPS with a sampling scheme based on conditioned Boltzmann Generators, a generative machine learning model capable of sampling a given target probability distribution. This approach produces uncorrelated transition paths but relies on an accurate reaction coordinate, which is rarely known in advance. Building on recent advances in committor learning, specifically on the Artificial Intelligence for Molecular Mechanism Discovery (AIMMD) method, in this work we introduce GenAIMMD, an iterative algorithm that actively and self-consistently learns the ideal reaction coordinate (the committor) and trains a conditioned Boltzmann Generator to sample from arbitrary bias windows along it. GenAIMMD thereby provides a correlation-free and fully parallelizable path sampling scheme that does not require prior knowledge of the system's transition mechanism. We apply GenAIMMD to a two-dimensional toy model and a higher-dimensional polymer system. In both cases, GenAIMMD succeeds in training the Boltzmann Generator and learning the committor. Benchmark results show a substantial increase in performance compared to standard TPS.

Abstract: Kohn-Sham density functional theory (DFT) remains the workhorse of ab initio materials simulation, yet cubic computational and quadratic memory scaling have confined calculations to a few hundred to thousands of atoms, spanning only nanometers, far below experimentally relevant length scales. We introduce XLSDFT, a linear-scaling DFT framework based on divide-and-conquer decomposition of the one-particle density matrix and Chebyshev-filtered subspace iteration, achieving linear computational and memory scaling while retaining DFT accuracy. Deployed on the LineShine exascale supercomputer, XLSDFT reduces computational complexity by orders of magnitude, enabling unprecedented DFT scale: a 200-million-atom silicon crystal, twentyfold beyond the prior record. Our implementation achieves 96.6% weak-scaling efficiency and sustained 157.9 Pflop/s (FP64) for a 100-million-atom scaling study. We further simulate an 11-million-atom all-solid-state battery interface of unprecedented complexity, 1,000 times beyond prior DFT for such systems, revealing how lithium metal reacts with the solid electrolyte at atomic resolution, in quantitative agreement with spectroscopy experiments.

Abstract: Universal machine-learning interatomic potentials (u-MLIPs) aim to generalize across diverse configurations. Benchmarks enable reproducible evaluation but may not expose failures outside their predefined scope. Here, we show that physics-informed search can complement benchmark-based evaluation by uncovering hidden failure modes. We introduce MLIP Detective, an agentic framework for active failure mode discovery. Starting from benchmark evidence, MLIP Detective generates falsifiable, physics-informed failure hypotheses, screens them with inexpensive simulations, and escalates only the most suspicious cases to human experts together with proposed verification protocols. Without issue-specific prompting, MLIP Detective identified and characterized a systematic anomaly in MACE-MPA-0: the model predicted some relaxed adsorbate-surface systems involving O- or F-containing adsorbates to be higher in energy than their corresponding separated fragments. Using cross-model comparisons, MLIP Detective further inferred a likely training-data origin for the anomaly, consistent with recent reports.

Abstract: Foundation models for ground states in spin-1/2 systems are a promising method for problems ranging from quantum chemistry to identifying new phase diagrams. Nearly all such models are currently pure-states that condition on the Hamiltonian's parameters, whose Monte Carlo samples give energy estimates according to the variational principle. In this contribution, we show that this representation is topologically obstructed. For any gapped Hamiltonian family whose ground-state bundle is non-trivial, every continuous normalized state-vector model has zero fidelity with the ground state at some parameter value in the Hamiltonian family. For that value, the energy is at least one spectral gap, $Δ$, with an $O(Δ)$ gap in an open-neighbourhood of that point. We show that this is a sufficient no-go also in the case of degenerate ground-state manifolds, time dynamics, and periodic systems with mixed space-time topology, demonstrating these obstructions on one- and two-qubit systems. We discuss how this causes a spike in the fidelity susceptibility, giving a numerical signature of a phase-transition where there is none. We then show that operator-valued models canonically avoid these obstructions and preserve topological information, implying a structural necessity in representation for foundation neural quantum states.