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At least 271 records · Page 15

Locally purified maximally mixed states at scale: Entanglement pruning and symmetries

Locally Purified Density Operators (LPDOs) are state-of-the-art tensor network ansatze candidates that efficiently represent mixed quantum states at scale. However, given their non-uniqueness, their representational complexity is generally sub-optimal in practical computations. Here, in this work we perform a comprehensive numerical and analytical analysis and resolve this issue in the experimentally relevant limit where noise depolarizes the density operator into a maximally mixed state. To resolve the sub-optimality issue, we analyze two numerical tools, one analytic method, and detail the relations between them. The numerical tools used are fidelity-preserving truncations and isometric gauge transformations leveraging Riemannian optimizations over entropic objective functions. In addition, by invoking the injectivity and symmetry constraints of the maximally mixed LPDO, we also present analytical closed-form expressions for the disentangler and discuss their relation to numerical optimizers. Further, away from the maximally mixed state, our simulations highlight how the truncation threshold smoothly interpolate, as a function of depolarization, between established matrix product results and our new results. Our work shows how, by minimizing the resources required to represent key states of practical interest in experiment, the efficiency of tensor network algorithms can be substantially increased. This paves the path for uncovering tensor network’s fundamental scalability limits and latent potential in representing the wide locus of mixed quantum states that are accessible on near-term quantum devices.

Gangapuram, Amit Jamadagni [Oak Ridge National Lab↗

VOTCA: multiscale frameworks for quantum and classical simulations in soft matter

Many physical phenomena in liquids and soft matter are multiscale by nature and can involve processes with quantum and classical degrees of freedom occurring over a vast range of length- and timescales. Examples range from structure formation processes of complex polymers or even polymer blends (Svaneborg & Everaers, 2023) on the classical side to charge and energy transport and conversion processes (Lee et al., 2019) involving explicit electronic and, therefore, quantum information. The Versatile Object-oriented Toolkit for Coarse-graining Applications (VOTCA) provides multiscale frameworks built on a comprehensive set of methods for the development of classical coarse-grained potentials (VOTCA-CSG) as well as state-of-the art excited state electronic structure methods based on density-functional and many-body Green’s function theories, coupled in mixed quantum-classical models and used in kinetic network models (VOTCA-XTP).

97 MATHEMATICS AND COMPUTING↗

Computational Power of Random Quantum Circuits in Arbitrary Geometries

Empirical evidence for a gap between the computational powers of classical and quantum computers has been provided by experiments that sample the output distributions of two-dimensional quantum circuits. Many attempts to close this gap have utilized classical simulations based on tensor network techniques, and their limitations shed light on the improvements to quantum hardware required to frustrate classical simulability. In particular, quantum computers having in excess of approximately 50 qubits are primarily vulnerable to classical simulation due to restrictions on their gate fidelity and their connectivity, the latter determining how many gates are required (and, therefore, how much infidelity is suffered) in generating highly entangled states. Here, we describe recent hardware upgrades to Quantinuum’s H2 quantum computer, enabling it to operate on up to 56 qubits with arbitrary connectivity and 99.843(5)% two-qubit gate fidelity. We define a class of circuits with random geometries that become hard to classically simulate in very low depth and implement them utilizing the flexible connectivity of H2. A careful analysis demonstrating the fast saturation of classical simulation complexity with depth indicates that H2 can yield data well beyond the reach of state-of-the art classical simulation methods at unprecedented fidelities. We find that the considerable difficulty of classically simulating H2 is likely limited only by qubit number, demonstrating the promise and scalability of the quantum charge-coupled device architecture as continued progress is made toward building larger machines. Published by the American Physical Society 2025

DeCross, M.↗

Alternating and Gaussian Fermionic Isometric Tensor Network States

Isometric tensor networks in two dimensions enable efficient and accurate study of quantum many-body states, yet the effect of the isometric restriction on the represented quantum states is not fully understood. We address this question in two main contributions. First, we introduce an improved variant of isometric tensor network states (isoTNS) in two dimensions, where the isometric arrows on the columns of the network alternate between pointing upward and downward; hence the name alternating isometric tensor network states. Second, we introduce a numerical tool—the isometric Gaussian fermionic TNS (isoGfTNS)—that incorporates isometric constraints into the framework of Gaussian fermionic tensor network states. We demonstrate in numerous ways that alternating isoTNSs represent many-body ground states of two-dimensional quantum systems significantly better than the original isoTNSs. First, we show that the entanglement in an isoTNS is mediated along the isometric arrows and that alternating isoTNSs mediate entanglement more efficiently than conventional isoTNSs. Second, alternating isoTNSs correspond to a deeper, and thus more representative, sequential-circuit construction of depth 𝒪⁢(𝐿𝑥 ⋅𝐿𝑦) compared to the original isoTNSs of depth 𝒪⁢(𝐿𝑥 +𝐿𝑦). Third, using the Gaussian framework and gradient-based energy minimization, we provide numerical evidence of better bond-dimension scaling and variational energy of alternating isoGfTNSs for ground states of various free-fermionic models, including the Fermi surface, the band insulator, and the 𝑝𝑥 +𝑖⁢𝑝𝑦 mean-field superconductor. Finally, benchmarking on the transverse-field Ising model, we demonstrate that an alternating isoTNS provides substantially improved performance and stability relative to the original isoTNS for the ground-state search algorithm in interacting systems.

Wu, Yantao [Chinese Academy of Sciences, Beijing (↗

Sign Problem in Tensor-Network Contraction

We investigate how the computational difficulty of contracting tensor networks depends on the sign structure of the tensor entries. Using results from computational complexity, we observe that the approximate contraction of tensor networks with only positive entries has lower computational complexity as compared to tensor networks with general real or complex entries. This raises the question of how this transition in computational complexity manifests itself in the hardness of different tensor-network-contraction schemes. We pursue this question by studying random tensor networks with varying bias toward positive entries. First, we consider contraction via Monte Carlo sampling and find that the transition from hard to easy occurs when the tensor entries become predominantly positive; this can be understood as a tensor-network manifestation of the well-known negative-sign problem in quantum Monte Carlo. Second, we analyze the commonly used contraction based on boundary tensor networks. The performance of this scheme is governed by the number of correlations in contiguous parts of the tensor network (which by analogy can be thought of as entanglement). Remarkably, we find that the transition from hard to easy—i.e., from a volume-law to a boundary-law scaling of entanglement—already occurs for a slight bias of the tensor entries toward a positive mean, scaling inversely with the bond dimension D , and thus the problem becomes easy the earlier the larger D occurs. This is in contrast both to expectations and to the behavior found in Monte Carlo contraction, where the hardness at fixed bias increases with the bond dimension. To provide insight into this early breakdown of computational hardness and the accompanying entanglement transition, we construct an effective classical statistical-mechanical model that predicts a transition at a bias of the tensor entries of 1 / D , confirming our observations. We conclude by investigating the computational difficulty of computing expectation values of tensor-network wave functions (projected entangled-pair states, PEPSs) and find that in this setting, the complexity of entanglement-based contraction always remains low. We explain this by providing a local transformation that maps PEPS expectation values to a positive-valued tensor network. This not only provides insight into the origin of the observed boundary-law entanglement scaling but also suggests new approaches toward PEPS contraction based on positive decompositions. Published by the American Physical Society 2025

Chen, Jielun (ORCID:0000000178411545)↗

Learning thermodynamic master equations for open quantum systems

The characterization of Hamiltonians and other components of open quantum dynamical systems plays a crucial role in quantum computing and other applications. Scientific machine learning techniques have been applied to this problem in a variety of ways, including by modeling with deep neural networks. However, the majority of mathematical models describing open quantum systems are linear, and the natural nonlinearities in learnable models have not been incorporated using physical principles. We present a data-driven model for open quantum systems that includes learnable, thermodynamically consistent terms. The trained model is interpretable, as it directly estimates the system Hamiltonian and linear components of coupling to the environment. We validate the model on synthetic two and three-level data, as well as experimental two-level data collected from a quantum device at Lawrence Livermore National Laboratory.

Mathematics and Computing↗

Hot Chips and Hot Interconnects for High End Computing Systems

I will discuss several processors: 1. The Cray proprietary processor used in the Cray X1; 2. The IBM Power 3 and Power 4 used in an IBM SP 3 and IBM SP 4 systems; 3. The Intel Itanium and Xeon, used in the SGI Altix systems and clusters respectively; 4. IBM System-on-a-Chip used in IBM BlueGene/L; 5. HP Alpha EV68 processor used in DOE ASCI Q cluster; 6. SPARC64 V processor, which is used in the Fujitsu PRIMEPOWER HPC2500; 7. An NEC proprietary processor, which is used in NEC SX-6/7; 8. Power 4+ processor, which is used in Hitachi SR11000; 9. NEC proprietary processor, which is used in Earth Simulator. The IBM POWER5 and Red Storm Computing Systems will also be discussed. The architectures of these processors will first be presented, followed by interconnection networks and a description of high-end computer systems based on these processors and networks. The performance of various hardware/programming model combinations will then be compared, based on latest NAS Parallel Benchmark results (MPI, OpenMP/HPF and hybrid (MPI + OpenMP). The tutorial will conclude with a discussion of general trends in the field of high performance computing, (quantum computing, DNA computing, cellular engineering, and neural networks).

Saini, Subhash↗

Identification of Solid-Electrolyte Interphase Species by Joint Characterization of Li-Ion Battery Chemistry by Mass Spectrometry and Electrochemical Reaction Networks

The formation and stability of the solid-electrolyte interphase (SEI) play central roles in determining the long-term performance and safety of modern electrochemical energy storage systems. Despite decades of research, the SEI’s heterogeneous, dynamic, and multiphase nature has defied comprehensive molecular-level characterization, creating a critical knowledge gap that limits rational battery design. In this work, we introduce a computational−experimental framework that integrates high-throughput quantum chemistry calculations, data-driven electrochemical reaction networks (eCRNs), stochastic algorithms, and laser desorption/ionization Fourier transform ion cyclotron resonance mass spectrometry (LDI-FTICR-MS) to unravel SEI formation in carbonatebased electrolytes without imposing predefined mechanisms. We constructed the most comprehensive eCRN to date, spanning over 10,000 species and 209 million reactions. Through stochastic network analysis, we successfully recovered 27 species that were previously reported in the literature and predicted 28 novel SEI species nearly doubling our scientific knowledge in this area. Each new species was rigorously confirmed through advanced mass spectral analysis of its distinct molecular and isotopic signatures. We kinetically refined the formation pathways for a select set of both previously reported and novel SEI products, revealing kinetically feasible elementary reaction mechanisms with activation barriers below 1 eV. This computational−experimental approach deepens our molecular-level understanding of SEI chemistry by resolving which species form and through which decomposition mechanisms they emerge. Such knowledge provides the foundation necessary to connect electrolyte composition to the resulting SEI components, a critical step toward a more informed electrolyte development in next-generation lithium-based batteries.

25 ENERGY STORAGE↗

S U ( 2 ) principal chiral model with tensor renormalization group on a cubic lattice

We study the continuous phase transition and thermodynamic observables in the three-dimensional Euclidean S U ( 2 ) principal chiral field model with the triad tensor renormalization group and the anisotropic tensor renormalization group methods. Using these methods, we find results that are consistent with previous Monte Carlo estimates and the predicted renormalization group scaling of the magnetization close to criticality. These results bring us one step closer to studying finite-density quantum chromodynamics in four dimensions using tensor network methods. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Towards a real-time computation of timelike hadronic vacuum polarization and light-by-light scattering: Schwinger Model tests

Hadronic vacuum polarization (HVP) and light-by-light scattering (HLBL) are crucial for evaluating the Standard Model predictions concerning the muon’s anomalous magnetic moment. However, direct first-principle lattice gauge theory-based calculations of these observables in the timelike region remain challenging. Discrepancies persist between lattice quantum chromodynamics (QCD) calculations in the spacelike region and dispersive approaches relying on experimental data parametrization from the timelike region. Here, we introduce a methodology employing 1+1-dimensional quantum electrodynamics (QED), i.e. the Schwinger Model, to investigate the HVP and HLBL. To that end, we use both tensor network techniques, specifically matrix product states, and classical emulators of digital quantum computers. Demonstrating feasibility in a simplified model, our approach sets the stage for future endeavors leveraging digital quantum computers.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Beyond-classical computation in quantum simulation

Quantum computers hold the promise of solving certain problems that lie beyond the reach of conventional computers. However, establishing this capability, especially for impactful and meaningful problems, remains a central challenge. Here, we show that superconducting quantum annealing processors can rapidly generate samples in close agreement with solutions of the Schrödinger equation. We demonstrate area-law scaling of entanglement in the model quench dynamics of two-, three-, and infinite-dimensional spin glasses, supporting the observed stretched-exponential scaling of effort for matrix-product-state approaches. We show that several leading approximate methods based on tensor networks and neural networks cannot achieve the same accuracy as the quantum annealer within a reasonable time frame. Thus, quantum annealers can answer questions of practical importance that may remain out of reach for classical computation.

King, Andrew D. [D-Wave Quantum Inc., Burnaby, BC ↗

Probing celestial energy and charge correlations through real-time quantum simulations: Insights from the Schwinger model

Motivated by recent developments in the application of light-ray operators (LROs) in high energy physics, we propose a new strategy to study correlation functions of LROs through real-time quantum simulations. We argue that quantum simulators provide an ideal laboratory to explore the properties LROs in lower-dimensional quantum field theories. This is exemplified in the 1 + 1 -d Schwinger model, employing tensor network methods, focusing on the calculation of energy and charge correlators. Despite some challenges in extracting the necessary correlation functions from the lattice, the methodology used can be extended to real quantum devices. Published by the American Physical Society 2025

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Entanglement engineering of optomechanical systems by reinforcement learning

Entanglement is fundamental to quantum information science and technology, yet controlling and manipulating entanglement—so-called entanglement engineering—for arbitrary quantum systems remains a formidable challenge. There are two difficulties: the fragility of quantum entanglement and its experimental characterization. We develop a model-free deep reinforcement-learning (RL) approach to entanglement engineering, in which feedback control together with weak continuous measurement and partial state observation is exploited to generate and maintain desired entanglement. We employ quantum optomechanical systems with linear or nonlinear photon–phonon interactions to demonstrate the workings of our machine-learning-based entanglement engineering protocol. In particular, the RL agent sequentially interacts with one or multiple parallel quantum optomechanical environments, collects trajectories, and updates the policy to maximize the accumulated reward to create and stabilize quantum entanglement over an arbitrary amount of time. The machine-learning-based model-free control principle is applicable to the entanglement engineering of experimental quantum systems in general.

97 MATHEMATICS AND COMPUTING↗

NoRA: A Tensor Network Ansatz for Volume-Law Entangled Equilibrium States of Highly Connected Hamiltonians

Motivated by the ground state structure of quantum models with all-to-all interactions such as mean-field quantum spin glass models and the Sachdev-Ye-Kitaev (SYK) model, we propose a tensor network architecture which can accomodate volume law entanglement and a large ground state degeneracy. We call this architecture the non-local renormalization ansatz (NoRA) because it can be viewed as a generalization of MERA, DMERA, and branching MERA networks with the constraints of spatial locality removed. We argue that the architecture is potentially expressive enough to capture the entanglement and complexity of the ground space of the SYK model, thus making it a suitable variational ansatz, but we leave a detailed study of SYK to future work. We further explore the architecture in the special case in which the tensors are random Clifford gates. Here the architecture can be viewed as the encoding map of a random stabilizer code. We introduce a family of codes inspired by the SYK model which can be chosen to have constant rate and linear distance at the cost of some high weight stabilizers. We also comment on potential similarities between this code family and the approximate code formed from the SYK ground space.

Physics↗

Real-Time Detection of Charge Jumps in Superconducting Qubits with a Convolutional Neural Network

Ionizing radiation from cosmic rays and gammas can induce discontinuous jumps in the environmental charge of superconducting qubits (charge jumps), causing correlated errors that challenge fault-tolerant quantum computing while simultaneously providing a detection signature for quantum sensing applications. Current detection methods operate offline, introducing latency incompatible with in-the-loop qubit control. In this paper, an online detector of charge jumps for superconducting qubits, based on a dilated causal convolutional neural network (DCCNN) designed for in-the-loop deployment on the Quantum Instrumentation Control Kit (QICK) platform, is presented. The network is trained on synthetic Ramsey tomography scans generated from qubit templates measured at the Northwestern Experimental Underground Site (NEXUS) at Fermilab, and translated to FPGA firmware via hls4ml with ap_fixed$\langle 16,6 \rangle$ quantization, reaching a per-inference latency of $6.19 μ$s on the Zynq UltraScale+ RFSoC ZCU216. At this operating point the DCCNN matches the detection efficiency of the established offline $χ^2$ algorithm ($0.843 \pm 0.022$ vs. $0.866 \pm 0.020$ on $|Δq| \in [0.1, 0.5] e$ at matched false-positive rate), while requiring no per-qubit hyperparameter tuning. This shifts charge-jump detection from a post-hoc diagnostic to a control-loop primitive, enabling adaptive protocols that respond to radiation-induced events in situ, with applications to quantum-computing error mitigation and to the use of superconducting qubits as particle detectors.

Gaytan-Villarreal, Daniel [Carnegie Mellon U.]↗

Simultaneous prediction of structural properties in epitaxially–grown GaN with quantum and conventional multi–output learning algorithms

Hundreds of GaN thin film crystal plasma–assisted molecular beam epitaxy synthesis experiment records spanning two decades were organized into a dataset correlating the growth experiment design parameters with discrete, binary determinations of crystallinity and surface morphology. Conventional data science techniques as well as both quantum and classical multi–output supervised machine learning algorithms were implemented to investigate the relationships between the operating parameter data and the structural figures of merit. Correlation coefficients, decision tree nodes, p–values, and SHAP values all support substrate temperature and gallium effusion cell conditions as being statistically significant for simultaneously influencing GaN crystallinity and surface morphology. Here, a conventional deep neural network learned best from the data, followed by a quantum–classical hybrid gradient boosting algorithm. When combined with calculations of uncertainty intervals based on VennAbers predictors, machine learning predictions of both structural properties show good agreement with results reported in published experimental literature.

36 MATERIALS SCIENCE↗

Efficient simulation of low-temperature physics in one-dimensional gapless systems

Here, we discuss the computational efficiency of the finite-temperature simulation with minimally entangled typical thermal states (METTS). To argue that METTS can be efficiently represented as matrix product states, we present an analytic upper bound for the average entanglement Rényi entropy of METTS for a Rényi index 0 < q ≤ 1. In particular, for one-dimensional (1D) gapless systems described by conformal field theories, the upper bound scales as O⁡(cN 0 ⁢log⁡β) where c is the central charge and N is the system size. Furthermore, we numerically find that the average Rényi entropy exhibits a universal behavior characterized by the central charge and is roughly given by half of the analytic upper bound. Based on these results, we show that METTS can provide a speedup compared to employing the purification method to analyze thermal equilibrium states at low temperatures in 1D gapless systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

HydraGNN_Predictive_GFM_2026 - Ensemble of predictive graph foundation models for atomistic materials modeling

This release contains data and parameters of HydraGNN-based graph foundation models trained as a result of the work published in the pre-print "Exascale Multi-Task Graph Foundation Models for Imbalanced, Multi-Fidelity Atomistic Data" by M. Lupo Pasini et al. (https://arxiv.org/abs/2604.15380). We jointly train on 16 open first-principles datasets (544+ million structures covering 85+ elements) using a multi-task architecture with per-dataset heads and a scalable ADIOS2/DDStore data pipeline. On Frontier, we execute six large-scale DeepHyper hyperparameter optimization campaigns in FP64 and promote the top-performing message-passing models to sustained 2,048-node training, yielding a PaiNN-based lead model. The version of HydraGNN used to generate the outputs provided in this release is HydraGNN v5.0 (https://github.com/ORNL/HydraGNN/releases/tag/v5.0) The list of datasets used for the training of the graph foundation model is the following: 1) Alexandria [1] 2) ANI1x [2] 3) MPTrj [3] 4) Open Catalyst 2020 (OC20) [4] 5) Open Catalyst 2022 (OC22) [5] 6) Open Catalyst 2025 (OC25) [6] 7) Open Direct ir Capture 2023 (ODAC23) [7] 8) Open Materials 2024 (OMat24) [8] 9) Open Molecules 2025 (OMol25) [9] 10) OMol25-neutral (subset of OMol25 that contains only molecules with zero total charge) 11) OMol25-non-neutral (subset of OMol25 that contains only molecules with non-zero total charge) 12) Open Polymers 2026 (OPoly2026) [10] 13) Nabla2DFT [11] 14) QCML [12] 15) QM7X [reference 13] 16) transition1x [14] Dataset references: [1] J. Schmidt et al., “A dataset of 175k stable and metastable materials calculated with the PBEsol and SCAN functionals,” Scientific Data, vol. 9, p. 64, 2022. [2] J. S. Smith et al., “The ANI-1ccx and ANI-1x data sets, coupled-cluster and density functional theory properties for molecules,” Scientific Data, vol. 7, p. 134, 2020. [Online]. Available: https: //www.nature.com/articles/s41597-020-0473-z [3] A. Jain et al., “Commentary: The Materials Project: A materials genome approach to accelerating materials innovation,” APL Materials, vol. 1, no. 1, p. 011002, 07 2013. [Online]. Available: https://doi.org/10.1063/1.4812323 [4] L. Chanussot et al., “Open catalyst 2020 (oc20) dataset and community challenges,” ACS Catalysis, vol. 11, no. 10, pp. 6059–6072, 2021. [Online]. Available: https://doi.org/10.1021/acscatal.0c04525 [5] K. Tran et al., “Open catalyst 2022 (oc22) dataset and challenges for oxidation electrocatalysts,” ACS Catalysis, vol. 13, no. 5, pp. 3066–3084, 2023. [Online]. Available: https://doi.org/10.1021/acscatal.2c05426 [6] S. J. Sahoo et al., “The open catalyst 2025 (oc25) dataset and models for solid-liquid interfaces,” arXiv preprint arXiv:2509.17862, 2025. [Online]. Available: https://arxiv.org/abs/2509.17862 [7] A. Sriram et al., “The open DAC 2023 dataset and challenges for sorbent discovery in direct air capture,” ACS Central Science, vol. 10, no. 5, pp. 923–941, 2024. [8] L. Barroso-Luque et al., “Open materials 2024 (omat24) inorganic materials dataset and models,” 2024. [Online]. Available: https://arxiv.org/abs/2410.12771 [9] D. S. Levine et al., “The open molecules 2025 (OMol25) dataset, evaluations, and models,” 2025. [Online]. Available: https://arxiv.org/abs/2505.08762 [10] D. S. Levine et al., The open polymers 2026 (OPoly26) dataset and evaluations,” arXiv preprint arXiv:2512.23117, 2025. [Online]. Available: https://arxiv.org/abs/2512.23117 [11] K. Khrabrov et al., “Nabla2dft: A universal quantum chemistry dataset of drug-like molecules and a benchmark for neural network potentials,” in NeurIPS 2024 Datasets and Benchmarks Track, 2024. [Online]. Available: https://openreview.net/forum?id=ElUrNM9U8c [12] S. Ganscha et al., “The QCML dataset, quantum chemistry reference data from 33.5M DFT and 14.7B semi-empirical calculations,” Scientific Data, vol. 12, p. 406, 2025. [13] J. Hoja et al., “QM7-X, a comprehensive dataset of quantum-mechanical properties spanning the chemical space of small organic molecules,” Scientific Data, vol. 8, p. 43, 2021. [Online]. Available: https://www.nature.com/articles/s41597-021-00812-2 [14] M. Schreiner et al., “Transition1x - a dataset for building generalizable reactive machine learning potentials,” Scientific Data, vol. 9, p. 779, 2022. The folder "datasets_ADIOS2_format" contains the set of pre-processed datasets in Adaptable I/O System (ADIOS) format (https://www.exascaleproject.org/research-project/adios/) that have been used for the development and training of GFMs in this work. The "datasets_ADIOS2_format" directory contains 2 sub-directories, one for the version "v1" of the datasets and one for the version "v2" of the datasets. The version "v1" of the datasets provides values of the total energy as they are extracted from the original data as it was released by the respective institutions. The version "v2" of the datasets provides values of the energy that have been realigned. The realignment was performed by training a linear regression model that predicts the total energy as a function of the chemical composition of the atomistic structure, and then subtract such prediction from the original value of the total energy. Both folders "v1" and "v2" contain 16 sub-directories, each corresponding to an ADIOS2-formatted dataset The folder "DeepHyper-results" contains the configurational files and model's parameters for all the 186 HPO trials that were successfully completed by the scalable hyperparameter optimization (HPO) runs on Frontier. The content of the folder "DeepHyper-results" I structured as follows: 1) task-list.txt: list of mpnn name, jobid, and deephyper task id 2) gfm_${MPNN}_${JOBID}_0.${TASKID}: run directory with checkpoint files 3) gfm_${MPNN}: deephyper summary directory (*.csv) for each specific MPNN type 4) deephyper-experiment-${JOBID}: output and error logs for each job The file "deephyper-sorted.csv" contains the details of each HydraGNN model built and tested by HPO, obtained by merging the (*.csv) filed from each HPO run executed. Out of all the HPO trials, we selected 10 to continue the training of the respective HydraGNN models. Due to limited computational budget available in the LRN070 allocation we could not complete the training till convergence for all these 10 selected models. The folder "models" contains multiple sub-folders, one per each HydraGNN model trained. Each model sub-folder contains the parameters of each HydraGNN model, with multiple checkpoint-restarts. The list of sub-folders are as follows: 1) multidataset_hpo-BEST1-fp64 2) multidataset_hpo-BEST2-fp64 3) multidataset_hpo-BEST3-fp64 4) multidataset_hpo-BEST4-fp64 5) multidataset_hpo-BEST5-fp64 6) multidataset_hpo-BEST6-fp64 7) multidataset_hpo-BEST7-fp64 8) multidataset_hpo-BEST8-fp64 9) multidataset_hpo-BEST9-fp64 10) multidataset_hpo-BEST10-fp64 Within each one of these folders, additional auxiliary log files are provided with descriptions about how the training proceeded. The lead PaiNN-model is contained inside "multidataset_hpo-BEST6-fp64". The file "mlp_branch_weights" contains the parameters of the multi-layer perceptron (MLP) used to reconcile the predictions of the 16 output decoding heads of the HydragNN architectures. The MLP takes in input the chemical composition of the atomistic structure and predicts averaging weights to linearly mix the predictions of each output decoding head toward consolidating them into a single one. The folder "1.1billion-structure-inference" contains 1.1 billion atomistic structures randomly generated. Each structures is associated with energy and forces predicted with the lead-PaiNN model combined with the MLP model for reconciliation of the multi-branch predictions generated by the 16 output decoding heads. The folder "1.1billion-structure-inference" contains 9,300 (*.tar.gz) subdirectories, one per Frontier compute node used to execute the inference at exascale. Once uncompressed, each (*.tar.gz) subdirectory contains an ADIOS2 (*.bp) file container, where each atomistic structure is stored as a PyTorch-Geometric Data object. The file "export_dataset_environment_variables.sh" contains the environment variables that need to be set before running the HydraGNN code to reproduce the results provided in this dataset release. The code that can be used to load the ADIOS2 files, load HydraGNN models, and run inference is available at: https://github.com/ORNL/HydraGNN/releases/tag/v5.0

36 MATERIALS SCIENCE↗