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At least 1,387 records · Page 77

Low‐dimensional manifold learning for uncertainty quantification in complex multi‐scale stochastic systems

Broadly speaking, the goals of the project are to develop techniques to use manifold learning to develop reduced‐order and surrogate models for "hyper‐reduction" of very high‐dimensional complex multi‐scale systems. This is being achieved by employing a newly proposed form of manifold projection and learning that leverages recent advancements in computational geometry and data‐driven modeling. In particular, we are applying a manifold projection technique to project the solutions of very high‐dimensional systems onto the so‐called Grassmannmanifold, a Reimannian manifold comprised of orthonormal matrices. We then apply data‐driven machine learning techniques to classify the solutions on the manifold (e.g. clustering techniques) according to their proximity on the manifold and leverage a further nonlinear dimension reduction to organize the structured data on the manifold. Finally, we are developing novel techniques that enable us to directly interpolate the hyper‐reduced data such that we can predict the solution of the complex, high‐ dimensional system without need to call the full expensive computational model. Given their adherence to the underlying structure of the solution of the physical system, it is expected that these approximate solutions will be sufficiently constrained so as to (approximately) adhere to physical principles.

97 MATHEMATICS AND COMPUTING↗

A User-Friendly GUI Tool for Automated Microstructural Analysis of Fiber-Reinforced Composites and Porous Structures

Understanding and quantifying microstructural features such as fiber orientation and porosity is critical for predicting the mechanical behavior and performance of fiber-reinforced polymer composites. Traditional manual analysis is time-consuming, subjective, and unsuitable for high-throughput datasets. We present a graphical user interface (GUI) application that automates the analysis of microscopy images to extract key microstructural metrics, including fiber orientation tensors, fiber orientation distribution, porosity and pore size distribution. The app integrates multiple image segmentation techniques including global and local thresholding, clustering, and region-based approaches, offering flexibility for different types of image qualities and features. Users can load microstructural images, select regions of interest and segmentation techniques tailored to their image dataset. It also addresses a critical challenge in fiber orientation analysis: the ambiguities caused by touching, overlapping, or partially cut fibers. It supports autorun examples for standardized workflows, enabling reproducible analysis and facilitating training and benchmarking. This tool significantly reduces manual intervention, enhances consistency, and accelerates data generation for structure–property modeling, process optimization, and digital materials research. The tool is intended for use by materials scientists, engineers, and researchers engaged in composite characterization, quality control, and machine learning-based microstructural studies.

Chawla, Komal [ORNL] (ORCID:0000000190327565)↗

Prediction of Dielectric Constant in Series of Polymers by Quantitative Structure-Property Relationship (QSPR)

This work is devoted to the investigation of dielectric permittivity which is influenced by electronic, ionic, and dipolar polarization mechanisms, contributing to the material’s capacity to store electrical energy. In this study, an extended dataset of 86 polymers was analyzed, and two quantitative structure–property relationship (QSPR) models were developed to predict dielectric permittivity. From an initial set of 1273 descriptors, the most relevant ones were selected using a genetic algorithm, and machine learning models were built using the Gradient Boosting Regressor (GBR). In contrast to Multiple Linear Regression (MLR)- and Partial Least Squares (PLS)-based models, the gradient boosting models excel in handling nonlinear relationships and multicollinearity, iteratively optimizing decision trees to improve accuracy without overfitting. The developed GBR models showed high R2 coefficients of 0.938 and 0.822, for the training and test sets, respectively. An Accumulated Local Effect (ALE) technique was applied to assess the relationship between the selected descriptors—eight for the GB_A model and six for the GB_B model, and their impact on target property. ALE analysis revealed that descriptors such as TDB09m had a strong positive effect on permittivity, while MLOGP2 showed a negative effect. These results highlight the effectiveness of the GBR approach in predicting the dielectric properties of polymers, offering improved accuracy and interpretability.

Ascencio-Medina, Estefania↗

Using feature importance as an exploratory data analysis tool on Earth system models

Abstract. Machine learning (ML) models are commonly used to generate predictions, but these models can also support the discovery of new science. Generating accurate predictions necessitates that a model captures the structure of the underlying data. If the structure is properly extracted, ML could be a useful exploratory and evidential tool. In this paper, we present a case study that demonstrates the use of ML for exploratory data analysis (EDA) in the climate space. We apply the ML explainability method of spatiotemporal zeroed feature importance (stZFI) to understand how climate-variable associations evolve over space and time. Our analyses focus on data from ensembles of Earth system models (ESMs) which provide data on different climate states and conditions. We elect to work with ESM ensembles since they allow us to compare feature importance across alternative scenarios not available with observed data. The ensembles also account for natural variability so that we can distinguish between signal and noise due to natural climate variability when computing feature importance. The use of perturbed initial condition ensembles introduces variability mimicking the natural variability in the atmosphere; thus the signals emerging using feature importance (FI) can be evaluated against the natural variability in the climate system. For our analyses, we consider the 1991 volcanic eruption of Mount Pinatubo, which was a large stratospheric aerosol injection. We explore the climate pathway associated with the eruption from aerosols to radiation to temperature at both the near-surface and stratospheric levels. In addition to applying the method to data generated from two different ESMs, we apply stZFI to reanalysis data to compare the associations identified by stZFI. We show how stZFI tracks the importance of aerosol optical depth over time on forecasting temperatures. This case study illustrates usefulness of an ML tool (stZFI) for EDA on a well-studied climate exemplar.

Ries, Daniel (ORCID:0000000250294647)↗

Machine Learning Approaches for Nuclear Material Accounting Data from Irradiation and Reprocessing

We are currently exploring data analysis methods for their ability to strengthen the synthesis and evaluation of information generated within domestic and international safeguard regimes. Safeguard data typically includes rich heterogenous datasets amenable to advanced data analytics methods, such as machine learning. We have converted transactional data containing both numerical and categorical attributes from a domestic nuclear material control and accountability (NMC&A) system into a low-dimensional numerical structure via linear principal component analysis. This data representation allows for global structure discovery via cluster analysis, which can characterize the typical behavior of each of the primary types of transaction events. Furthermore, the structure of the top principal components captures the “typical behavior” of the data and is thus amenable to anomaly detection through statistical hypothesis testing. We explored this capability by generating erroneous permutations of the data and computing the Q-residual quantity increase associated with the information loss when these data are projected into the low-dimensional principal component analysis space representative of typical transactions.Future work will focus on identifying data transformations (e.g., graph networks) that more closely align with the inherent structure of these transactions to explain more salient information and disambiguate the underlying nuclear process—in this case, irradiation and reprocessing—from artifacts of NMC&A system transactional record keeping data.

Drescher, Adam↗

Harnessing the power of ab initio calculations, distributed computing and machine learning to efficiently locate extreme molecules for use in carbon-based solar cells (Final Technical Report)

The use of high-throughput virtual screening (HTVS) tools is a powerful tool to expedite the materials discovery of commercially relevant materials. In previous years, our group has developed a molecular discovery platform to generate libraries in order to obtain suitable candidates for different applications, starting from the Harvard Clean Energy Project. This platform is suitable to test in-silico on traditional supercomputing clusters and shared resources, for example, in the IBM World Community Grid. In this project, we used the molecular discovery platform to create and screen a library of candidates of organic photovoltaic (OPVs) molecules. Based on a set of candidates created with combinations of molecular moieties, we were able to filter, by conformation stability, the energy of electronic orbitals and approximated power conversion efficiencies (PCE). To improve the predictions of orbital energies calculated and the PCEs, we used Gaussian Process regression and two sets of molecules. These sets correspond to electronic structure calculations of a higher level of theory and experimental PCE values, respectively. Finally, we selected a subset of the best candidates (molecules with a PCE higher than 10%) to understand its absorbance properties with TD-DFT. This project has demonstrated the capabilities of our molecular discovery platform for HTVS. Finally, machine learning can help us to introduce more complex effects included in bulk conditions and computational intensive calculations on models.

14 SOLAR ENERGY↗

Efficient Multiscale Optoelectronic Prediction for Conjugated Polymers

Conjugated polymers represent a high-potential material class due to the tunability of their optoelectronic properties via straightforward processing protocols. However, to in silico tailor these optoelectronic properties, one must compute the conformationally dependent electronic structure over mesoscopic length and time scales. This task represents a challenging multiscale computational problem in which quantum chemistry and atomistic or coarse-grained molecular dynamics must be integrated. Recently, we introduced a methodology, called electronic coarse graining (ECG), that utilizes artificial neural networks to compute ab initio quality electronic structures using only the reduced degrees of freedom of coarse-grained models. Here, we adapt ECG to variable-molecular weight conjugated oligomers by casting the problem in the framework of sequence detection. A machine-learning (ML) architecture employing one-dimensional convolutional neural networks and long short-term memory networks is utilized to compute ground-state orbital energies, charge density distributions, and optical spectra solely from the coarse-grained model's configurational degrees of freedom. Robust molecular weight transferability for ECG is established via a A-ML approach that leverages model electronic Hamiltonians for ground and excited-state property determination. The accuracy and transferability of the ECG methodology opens the door for scalable optoelectronic property prediction in conjugated polymers directly from coarse-grained degrees of freedom.

36 MATERIALS SCIENCE↗

Classification of octet AB-type binary compounds using dynamical charges: A materials informatics perspective

The role of dynamical (or Born effective) charges in classification of octet AB-type binary compounds between four-fold (zincblende/wurtzite crystal structures) and six-fold (rocksalt crystal structure) coordinated systems is discussed. We show that the difference in the dynamical charges of the fourfold and sixfold coordinated structures, in combination with Harrison’s polarity, serves as an excellent feature to classify the coordination of 82 sp–bonded binary octet compounds. We use a support vector machine classifier to estimate the average classification accuracy and the associated variance in our model where a decision boundary is learned in a supervised manner. Lastly, we compare the out-of-sample classification accuracy achieved by our feature pair with those reported previously.

36 MATERIALS SCIENCE↗

Machine Learning for Prediction of Thermodynamic Descriptors

Our objective is to apply machine learning (ML) algorithms for the prediction of molecular catalysis descriptors from geometric properties derived from experimental crystallographic databases. Catalysis is often considered a “low-data” discipline that is poorly suited for ML methods. An exception is the extensive structural information that is available for molecular catalysts through the Cambridge Structural Database (CSD), which contains atomically precise molecular structures from X-ray diffraction analysis for >600K metal complexes. As a proof-of-principle, we targeted the prediction of hydricity, a thermodynamic property that provides understanding and control of catalytic hydride transfer. We built a training set composed of ~100 molecular complexes with a known hydricity and structural information from the CSD. This data set was converted into a machine-readable format using the smooth overlap of atomic positions (SOAP) representation and further labeled with simple electronic descriptors for the metal centers. Multiple different neural networks were trained on this data set, and the accuracy of the hydricity predictions ranged from < 2 kcal/mol to 20 kcal/mol. The accuracy of each model was highly sensitive to which compounds were in the train versus test set, underscoring the challenges associated with small and chemically diverse data sets. Finally, to further augment the data set, we attempted to experimentally measure several new hydricity values, however these experiments were unsuccessful due to undesired chemical reactivity of the selected complexes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Enhancing gene regulatory network inference through data integration with markov random fields

Here, a gene regulatory network links transcription factors to their target genes and represents a map of transcriptional regulation. Much progress has been made in deciphering gene regulatory networks computationally. However, gene regulatory network inference for most eukaryotic organisms remain challenging. To improve the accuracy of gene regulatory network inference and facilitate candidate selection for experimentation, we developed an algorithm called GRACE (Gene Regulatory network inference ACcuracy Enhancement). GRACE exploits biological a priori and heterogeneous data integration to generate high- confidence network predictions for eukaryotic organisms using Markov Random Fields in a semi-supervised fashion. GRACE uses a novel optimization scheme to integrate regulatory evidence and biological relevance. It is particularly suited for model learning with sparse regulatory gold standard data. We show GRACE’s potential to produce high confidence regulatory networks compared to state of the art approaches using Drosophila melanogaster and Arabidopsis thaliana data. In an A. thaliana developmental gene regulatory network, GRACE recovers cell cycle related regulatory mechanisms and further hypothesizes several novel regulatory links, including a putative control mechanism of vascular structure formation due to modifications in cell proliferation.

59 BASIC BIOLOGICAL SCIENCES↗

Large-Scale Materials Modeling at Quantum Accuracy: Ab Initio Simulations of Quasicrystals and Interacting Extended Defects in Metallic Alloys

Ab initio electronic-structure has remained dichotomous between achievable accuracy and length-scale. Quantum many-body (QMB) methods realize quantum accuracy but fail to scale. Density functional theory (DFT) scales favorably but remains far from quantum accuracy. We present a framework that breaks this dichotomy by use of three interconnected modules: (i) invDFT: a methodological advance in inverse DFT linking QMB methods to DFT; (ii) MLXC: a machine-learned density functional trained with invDFT data, commensurate with quantum accuracy; (iii) DFT-FE-MLXC: an adaptive higher-order spectral finite-element (FE) based DFT implementation that integrates MLXC with efficient solver strategies and HPC innovations in FE-specific dense linear algebra, mixed-precision algorithms, and asynchronous compute-communication. Furthermore, we demonstrate a paradigm shift in DFT that not only provides an accuracy commensurate with QMB methods in ground-state energies, but also attains an unprecedented performance of 659.7 PFLOPS (43.1% peak FP64 performance) on 619,124 electrons using 8,000 GPU nodes of Frontier supercomputer.

density functional theory↗

Correlated dynamic disorder, octahedral tilts, and acoustic phonon softening in CsSnBr 3 and CsPbBr 3

Metal halide perovskites (MHPs) have emerged as highly promising materials for optoelectronic applications, with all-inorganic MHPs presenting enhanced stability compared to their hybrid counterparts. Here, in this study, we investigate the atomic dynamics and structural fluctuations in single crystals of CsSnBr⁢ 3 and CsPbBr⁢ 3 through systematic inelastic neutron scattering (INS) measurements as a function of temperature. Our experiments are compared with first-principle simulations, augmented with large-scale molecular dynamics modeling, based on machine-learned neural network potentials. Through both INS and simulations, we find quasi-elastic diffuse rods in reciprocal space in both compounds, originating from fluctuating planar domains featuring correlated tilts of Br octahedron. The diffuse rods exhibit a slow, overdamped dynamic process, modulated across 𝑸 space, reflecting the strong lattice anharmonicity of the inorganic framework. We do not find evidence for dynamic off-centering of the Sn 2+ ions besides phonon vibrations at the center of the Br octahedron. These results offer valuable insights into the unusual anharmonic atomic dynamics and intricate correlated structural distortions in MHPs, which will be critical for rationalizing and further tailoring their thermal and optoelectronic properties.

36 MATERIALS SCIENCE↗

Fusion of Multiple Models for Improving Gross Primary Production Estimation With Eddy Covariance Data Based on Machine Learning

Abstract Terrestrial gross primary production (GPP) represents the magnitude of CO 2 uptake through vegetation photosynthesis, and is a key variable for carbon cycles between the biosphere and atmosphere. Light use efficiency (LUE) models have been widely used to estimate GPP for its physiological mechanisms and availability of data acquisition and implementation, yet each individual GPP model has exhibited large uncertainties due to input errors and model structure, and further studies of systematic validation, comparison, and fusion of those models with eddy covariance (EC) site data across diverse ecosystem types are still needed in order to further improve GPP estimation. We here compared and fused five GPP models (VPM, EC‐LUE, GOL‐PEM, CHJ, and C‐Fix) across eight ecosystems based on FLUXNET2015 data set using the ensemble methods of Bayesian Model Averaging (BMA), Support Vector Machine (SVM), and Random Forest (RF) separately. Our results showed that for individual models, EC‐LUE gave a better performance to capture interannual variability of GPP than other models, followed by VPM and GLO‐PEM, while CHJ and C‐Fix were more limited in their estimation performance. We found RF and SVM were superior to BMA on merging individual models at various plant functional types (PFTs) and at the scale of individual sites. On the basis of individual models, the fusion methods of BMA, SVM, and RF were examined by a five‐fold cross validation for each ecosystem type, and each method successfully improved the average accuracy of estimation by 8%, 18%, and 19%, respectively.

Environmental Sciences & Ecology↗

Graphical Gaussian Process Regression Model for Aqueous Solvation Free Energy Prediction of Organic Molecules in Redox Flow Battery

The solvation free energy of organic molecules is a critical parameter in determining emergent properties such as solubility, liquid-phase equilibrium constants, and pKa and redox potentials in an organic redox flow battery. In this work, we present a machine learning (ML) model that can learn and predict the aqueous solvation free energy of an organic molecule using Gaussian process regression method based on a new molecular graph kernel. To investigate the performance of the ML model on electrostatic interaction, the nonpolar interaction contribution of solvent and the conformational entropy of solute in solvation free energy, three data sets with implicit or explicit water solvent models, and contribution of conformational entropy of solute are tested. We demonstrate that our ML model can predict the solvation free energy of molecules at chemical accuracy with a mean absolute error of less than 1 kcal/mol for subsets of the QM9 dataset and the Freesolv database. To solve the general data scarcity problem for a graph-based ML model, we propose a dimension reduction algorithm based on the distance between molecular graphs, which can be used to examine the diversity of the molecular data set. It provides a promising way to build a minimum training set to improve prediction for certain test sets where the space of molecular structures is predetermined.

25 ENERGY STORAGE↗

A multiscale multi-permeability poroplasticity model linked by recursive homogenizations and deep learning

Many geological materials, such as shale, mudstone, carbonate rock, limestone and rock salt are multi-porosity porous media in which pores of different scales may co-exist in the host matrix. When fractures propagate in these multi-porosity materials, these pores may enlarge and coalesce and therefore change the magnitude and the principal directions of the effective permeability tensors. The pore-fluid inside the cracks and the pores of host matrix may interact and exchange fluid mass, but the difference in hydraulic properties of these pores often means that a single homogenized effective permeability tensor field is insufficient to characterize the evolving hydraulic properties of these materials at smaller time scale. Furthermore, the complexity of the hydro-mechanical coupling process and the induced mechanical and hydraulic anisotropy originated from the micro-fracture and plasticity at grain scale also makes it difficult to propose, implement and validate separated macroscopic constitutive laws for numerical simulations. Here this article presents a hybrid data-driven method designed to capture the multiscale hydro-mechanical coupling effect of porous media with pores of various different sizes. At each scale, data-driven models generated from supervised machine learning are hybridized with classical constitutive laws in a directed graph that represents the numerical models. By using sub-scale simulations to generate database to train material models, an offline homogenization procedure is used to replace the up-scaling procedure to generate cohesive laws for localized physical discontinuities at both grain and specimen scales. Through a proper homogenization procedure that preserves spatial length scales, the proposed method enables field-scale simulations to gather insights from meso-scale and grain-scale micro-structural attributes. This method is proven to be much more computationally efficient than the classical DEM–FEM or FEM2 approach while at the same time more robust and flexible than the classical surrogate modeling approach. Due to the usage of bridging-scale technique, the proposed model may provide multiple opportunities to incorporate different types of simulations and experimental data across different length scales for machine learning. Numerical issues will also be discussed.

42 ENGINEERING↗

Machine-Learning Functional Zonation Approach for Characterizing Terrestrial–Aquatic Interfaces: Application to Lake Erie

Ecosystems at coastal terrestrial–aquatic interfaces play a significant role in global biogeochemical cycles. In this study, we aimed to characterize coastal wetlands with particular focus on the co-variability between plant dynamics, topography, soil, and other environmental factors. We proposed a functional zonation approach based on machine learning clustering to identify the spatial regions, i.e., zones that capture these co-varied properties. This approach was applied to publicly available datasets along Lake Erie, in the Great Lakes Region. We investigated the heterogeneity of coastal ecosystem structures as a function of along-shore distance and transverse distance, based on the spatial data layers, including topography, wetland vegetation cover, and the time series of Landsat’s enhanced vegetation index (EVI) between 1990 and 2020. Results showed that the topographic metrics (elevation and slope), soil texture, and plant productivity influence the spatial distribution of wetland land-covers (emergent and phragmites). These results highlight a natural organization along the transverse axis, where the elevation and the EVI increase further away from the coastline. In addition, the clustering analysis allowed us to identify regions with distinct environmental characteristics, as well as the ones that are more sensitive to interannual lake-level variations.

47 OTHER INSTRUMENTATION↗

Multistage nucleation pathway in LiF molten salt mirrors the crystal–melt interface structure

Despite over a century of studies, fundamental questions remain about the processes governing crystal nucleation from melts or solutions. Research over the past three decades has presented mounting evidence for kinetic pathways of crystal nucleation that are more complex than envisioned by the simplest forms of classical theory. Such observations have been presented for colloidal and elemental systems with covalent and metallic bonding. Despite the technological and geochemical importance of molten salts, similar studies for these ionically bonded systems are currently lacking. Here we develop a machine learning interatomic potential for a model ionic system: LiF. The potential features quantum-level accuracy for both liquid and multiple solid polymorphs over wide temperature and pressure ranges and accurately reproduces experimentally measured properties. Thanks to the efficiency of the potential, which enables microsecond-scale molecular dynamics simulations, induction times for nucleation of LiF solids from their melts are computed over a range of undercoolings. With the aid of a set of robust local order parameters established here, the simulations reveal that homogeneous crystal nucleation in undercooled melts preferentially initiates from liquid regions showing slow dynamics and high bond orientational order simultaneously, and the second-shell order of both precritical nuclei and the surface of postcritical nuclei is dominated by hexagonal close packing and body-centered cubic local structure, even though the nucleus core is dominated by face-centered cubic structure corresponding to the stable rocksalt crystal structure. Finally, we establish a connection between the crystallization pathway and the equilibrium crystal-melt interface structure.

Applied Physical Sciences↗

Characterization data of an (AlFeNiTiVZr) 1-x Cr x multi-principal element alloy continuous composition spread library

The data provided in this article is related to the research article entitled “Phase stabilization and oxidation of a continuous composition spread multi-principal element (AlFeNiTiVZr) 1-x Cr x alloy”. This data article describes the high-throughput synthesis and characterization processes of an (AlFeNiTiVZr) 1-x Cr x alloy system. Continuous composition spread (CCS) thin-film libraries were synthesized by co-depositing an AlFeNiTiVZr metal alloy target and Cr target via magnetron sputtering. Post-processing was performed on the sample libraries with a vacuum anneal at 873 K and an air anneal at 873 K. Compositional data was determined via WDS in order to verify parameters provided by an in-house sputter model. Crystallographic data was captured via synchrotron diffraction and diffractograms were compared as a function of the change in Cr concentration. These measurements were taken in order to observe phase behavior after oxidation throughout the composition library. Furthermore, vibrational spectrographic data is provided of the oxidized library to show surface speciation along the composition gradient of the alloy system. The structural and oxidative behavior of the (AlFeNiTiVZr) 1-x Cr x alloy can be analysed using the data provided in this article. Additionally, this characterization dataset can be utilized in machine learning algorithms for determining important features and parameters for future hypothesis generation of functional multi-principal element alloys (MPEAs).

36 MATERIALS SCIENCE↗