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At least 145 records · Page 8

AI and extreme scale computing to learn and infer the physics of higher order gravitational wave modes of quasi-circular, spinning, non-precessing black hole mergers

We use artificial intelligence (AI) to learn and infer the physics of higher order gravitational wave modes of quasi-circular, spinning, non precessing binary black hole mergers. We trained AI models using 14 million waveforms, produced with the surrogate model NRHybSur3dq8, that include modes up to $\ell$ ≤ 4 and (5,5), except for (4,0) and (4,1), that describe binaries with mass-ratios $\textit{q}$ ≤ 8, individual spins $s^z_{\{1,2\}} \in$[–0.8,0.8], and inclination angle $θ \in$ [0,π]. Our probabilistic AI surrogates can accurately constrain the mass-ratio, individual spins, effective spin, and inclination angle of numerical relativity waveforms that describe such signal manifold. We compared the predictions of our AI models with Gaussian process regression, random forest, k-nearest neighbors, and linear regression, and with traditional Bayesian inference methods through the PyCBC Inference toolkit, finding that AI outperforms all these approaches in terms of accuracy, and are between three to four orders of magnitude faster than traditional Bayesian inference methods. Our AI surrogates were trained within 3.4 hours using distributed training on 1,536 NVIDIA V100 GPUs in the Summit supercomputer.

79 ASTRONOMY AND ASTROPHYSICS↗

A novel approach for large-scale wind energy potential assessment

Increasing wind energy generation is central to grid decarbonization, yet methods to estimate wind energy potential are not standardized, leading to inconsistencies and even skewed results. This study aims to improve the fidelity of wind energy potential estimates through an approach that integrates geospatial analysis and machine learning (i.e., Gaussian process regression). We demonstrate this approach to assess the spatial distribution of wind energy capacity potential in the Contiguous United States (CONUS). We find that the capacity-based power density ranges from 1.70 MW/km2 (25th percentile) to 3.88 MW/km2 (75th percentile) for existing wind farms in the CONUS. The value is lower in agricultural areas (2.73 ± 0.02 MW/km2, mean ± 95 % confidence interval) and higher in other land cover types (3.30 ± 0.03 MW/km2). Notably, advancements in turbine manufacturing could reduce power density in areas with lower wind speeds by adopting low specific-power turbines, but improve power density in areas with higher wind speeds (>8.35 m/s at 120m above the ground), highlighting opportunities for repowering existing wind farms. Wind energy potential is shaped by wind resource quality and is regionally characterized by land cover and physical conditions, revealing significant capacity potential in the Great Plains and Upper Texas. The results indicate that areas previously identified as hot spots using existing approaches (e.g., the west of the Rocky Mountains) may have a limited capacity potential due to low wind resource quality. Improvements in methodology and capacity potential estimates in this study could serve as a new basis for future energy systems analysis and planning.

Dai, Tao↗

Polymers for Extreme Conditions Designed Using Syntax-Directed Variational Autoencoders

We report the design/discovery of new materials is highly nontrivial owing to the near-infinite possibilities of material candidates and multiple required property/performance objectives. Thus, machine learning tools are now commonly employed to virtually screen material candidates with desired properties by learning a theoretical mapping from material-to-property space, referred to as the forward problem. However, this approach is inefficient and severely constrained by the candidates that the human imagination can conceive. Thus, in this work on polymers, we tackle the materials discovery challenge by solving the inverse problem: directly generating candidates that satisfy desired property/performance objectives. We utilize syntax-directed variational autoencoders (VAE) in tandem with Gaussian process regression (GPR) models to discover polymers expected to be robust under three extreme conditions: (1) high temperatures, (2) high electric field, and (3) high temperature and high electric field, useful for critical structural, electrical, and energy storage applications. This approach to learn from and augment) human ingenuity is general and can be extended to discover polymers with other targeted properties and performance measures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Direct Deoxygenation of Phenol over Fe-Based Bimetallic Surfaces Using On-the-Fly Surrogate Models

We present an accelerated nudged elastic band (NEB) study of phenol direct deoxygenation (DDO) on Fe-based bimetallic surfaces using a recently developed Gaussian process regression (GPR) calculator. Our test calculations demonstrate that the GPR calculator achieves up to 3 times speedup compared to conventional density functional theory calculations while maintaining high accuracy, with energy barrier errors below 0.015 eV. Using GPR-NEB, we systematically examine the DDO mechanism on pure Fe(110) and surfaces modified with Co and Ni in both top and subsurface layers. Our results show that subsurface Co and Ni substitutions preserve favorable thermodynamics and kinetics for both C–O bond cleavage and C–H bond formation, comparable to those on the pure Fe(110) surface. In contrast, top-layer substitutions generally increase the C–O bond cleavage barrier, render the step endothermic, and result in significantly higher reverse reaction rates, making DDO unfavorable on these surfaces. This work demonstrates the effectiveness of GRR-accelerated transition state searches for complex surface reactions and provides insights into rational design of bimetallic catalysts for selective deoxygenation.

Aromatic compounds↗

Prediction of O and OH Adsorption on Transition Metal Oxide Surfaces from Bulk Descriptors

In the search for stable and active catalysts, density functional theory and machine learning (ML) based models can accelerate the screening of materials. While stability is conveniently addressed on the bulk level of computation, the modelling of catalytic activity requires expensive surface simulations. Here, in this work, we develop models for the surface adsorption energy of O and OH intermediates across a consistent and extensive dataset of pure transition metal oxide surfaces. We show that adsorption energies across metal oxidation states of +2 to +6 are well captured from the metal-oxygen bond strength extracted from the bulk level calculation. Specifically, we calculate the integrated crystal orbital Hamiltonian population (ICOHP) of the metal-oxygen bond in the bulk oxide and employ a simple normalization scheme to obtain a strong correlation with adsorption energetics. By combining our ICOHP descriptor with non DFT features in a Gaussian Process regression (GPR) model, we achieve high model accuracy with mean absolute errors of 0.166 and 0.219 eV for OH and O adsorption, respectively. By targeting the O-OH adsorption energy difference with our GPR model, we predict the the oxygen evolution reaction (OER) activity from bulk descriptors only. Furthermore, we utilize the strong correlation between the COHP and metal oxygen bond lengths to rapidly predict adsorption energetics and catalytic activity from the optimized bulk geometry. Our approach can enable an efficient search for active catalysts by eliminating the need for surface calculations in the initial screening phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Chemical Robotics Enabled Exploration of Stability in Multicomponent Lead Halide Perovskites via Machine Learning

Metal halide perovskites have attracted immense interest as a promising material for a variety of optoelectronic and sensing applications. However, issues regarding long-term stability have emerged as the key bottleneck for commercialization. Here, we develop an automated experimental workflow based on combinatorial synthesis and rapid throughput characterization to explore long-term stability of these materials in ambient conditions. We apply it to four model perovskite systems: MA x FA y Cs 1–x–y PbBr 3 , MA x FA y Cs 1–x–y PbI 3 , Cs x FA y MA 1–x–y Pb(Br x+y I 1–x–y ) 3 , and Cs x MA y FA 1–x–y Pb(I x+y Br 1–x–y ) 3 . Non-negative matrix factorization and Gaussian process regression are used to interpolate the photoluminescent behavior of the phase diagram. This interpolative regression analysis helps to distinguish mixtures that form solid solutions from those that segregate into multiple materials, pointing out the most stable regions of the phase diagram. Here, we find stability dependence on composition to be nonuniform within the composition space, suggesting the presence of potential preferential compositional regions. This proposed workflow is universal and can be applied to other solution-processable materials.

36 MATERIALS SCIENCE↗

Machine learning-assisted crystal engineering of a zeolite

Abstract It is shown that Machine Learning (ML) algorithms can usefully capture the effect of crystallization composition and conditions (inputs) on key microstructural characteristics (outputs) of faujasite type zeolites (structure types FAU, EMT, and their intergrowths), which are widely used zeolite catalysts and adsorbents. The utility of ML (in particular, Geometric Harmonics) toward learning input-output relationships of interest is demonstrated, and a comparison with Neural Networks and Gaussian Process Regression, as alternative approaches, is provided. Through ML, synthesis conditions were identified to enhance the Si/Al ratio of high purity FAU zeolite to the hitherto highest level (i.e., Si/Al = 3.5) achieved via direct (not seeded), and organic structure-directing-agent-free synthesis from sodium aluminosilicate sols. The analysis of the ML algorithms’ results offers the insight that reduced Na 2 O content is key to formulating FAU materials with high Si/Al ratio. An acid catalyst prepared by partial ion exchange of the high-Si/Al-ratio FAU (Si/Al = 3.5) exhibits improved proton reactivity (as well as specific activity, per unit mass of catalyst) in propane cracking and dehydrogenation compared to the catalyst prepared from the previously reported highest Si/Al ratio (Si/Al = 2.8).

36 MATERIALS SCIENCE↗

On-the-fly active learning of interpretable Bayesian force fields for atomistic rare events

Abstract Machine learned force fields typically require manual construction of training sets consisting of thousands of first principles calculations, which can result in low training efficiency and unpredictable errors when applied to structures not represented in the training set of the model. This severely limits the practical application of these models in systems with dynamics governed by important rare events, such as chemical reactions and diffusion. We present an adaptive Bayesian inference method for automating the training of interpretable, low-dimensional, and multi-element interatomic force fields using structures drawn on the fly from molecular dynamics simulations. Within an active learning framework, the internal uncertainty of a Gaussian process regression model is used to decide whether to accept the model prediction or to perform a first principles calculation to augment the training set of the model. The method is applied to a range of single- and multi-element systems and shown to achieve a favorable balance of accuracy and computational efficiency, while requiring a minimal amount of ab initio training data. We provide a fully open-source implementation of our method, as well as a procedure to map trained models to computationally efficient tabulated force fields.

36 MATERIALS SCIENCE↗

Autonomous scanning probe microscopy investigations over WS2 and Au{111}

Abstract Individual atomic defects in 2D materials impact their macroscopic functionality. Correlating the interplay is challenging, however, intelligent hyperspectral scanning tunneling spectroscopy (STS) mapping provides a feasible solution to this technically difficult and time consuming problem. Here, dense spectroscopic volume is collected autonomously via Gaussian process regression, where convolutional neural networks are used in tandem for spectral identification. Acquired data enable defect segmentation, and a workflow is provided for machine-driven decision making during experimentation with capability for user customization. We provide a means towards autonomous experimentation for the benefit of both enhanced reproducibility and user-accessibility. Hyperspectral investigations on WS 2 sulfur vacancy sites are explored, which is combined with local density of states confirmation on the Au{111} herringbone reconstruction. Chalcogen vacancies, pristine WS 2 , Au face-centered cubic, and Au hexagonal close-packed regions are examined and detected by machine learning methods to demonstrate the potential of artificial intelligence for hyperspectral STS mapping.

36 MATERIALS SCIENCE↗

Probing multi-dimensional composition spaces in search of strong metallic alloys

Refractory complex concentrated alloys (RCCA) offer exceptionally high-temperature strength compared to pure metals and dilute alloys, but predictive theory for RCCA design is lacking. We present large-scale molecular Dynamics (MD) simulations of crystal plasticity to explore alloy compositions for maximum mechanical strength, focusing on Fe-Ta-W and Nb-Ta-Mo-W alloy families modeled with Embedded Atom Model (EAM) and Spectral Neighbor Analysis Potentials (SNAP). To efficiently guide the search for strong alloy compositions, we employ iterative optimization using Gaussian process regression. Many simulated RCCA compositions exhibit pronounced cocktail strengthening, with strengths surpassing their strongest constituent metal, tungsten. Contrary to expectations, the highest strength is found on binary edges of the RCCA composition space. Detailed analyses of atomistic simulations reveal that, similar to pure BCC metals, plastic response in RCCA is primarily governed by screw dislocations. However, at large strains, dislocation multiplication and interactions (Taylor hardening) become the dominant mechanisms contributing to RCCA strength.

Materials science↗

Unveiling the effect of composition on nuclear waste immobilization glasses’ durability by nonparametric machine learning

Abstract Ensuring the long-term chemical durability of glasses is critical for nuclear waste immobilization operations. Durable glasses usually undergo qualification for disposal based on their response to standardized tests such as the product consistency test or the vapor hydration test (VHT). The VHT uses elevated temperature and water vapor to accelerate glass alteration and the formation of secondary phases. Understanding the relationship between glass composition and VHT response is of fundamental and practical interest. However, this relationship is complex, non-linear, and sometimes fairly variable, posing challenges in identifying the distinct effect of individual oxides on VHT response. Here, we leverage a dataset comprising 654 Hanford low-activity waste (LAW) glasses across a wide compositional envelope and employ various machine learning techniques to explore this relationship. We find that Gaussian process regression (GPR), a nonparametric regression method, yields the highest predictive accuracy. By utilizing the trained model, we discern the influence of each oxide on the glasses’ VHT response. Moreover, we discuss the trade-off between underfitting and overfitting for extrapolating the material performance in the context of sparse and heterogeneous datasets.

36 MATERIALS SCIENCE↗

Advances in Kriging-Based Autonomous X-Ray Scattering Experiments

Autonomous experimentation is an emerging paradigm for scientific discovery, wherein measurement instruments are augmented with decision-making algorithms, allowing them to autonomously explore parameter spaces of interest. We have recently demonstrated a generalized approach to autonomous experimental control, based on generating a surrogate model to interpolate experimental data, and a corresponding uncertainty model, which are computed using a Gaussian process regression known as ordinary Kriging (OK). We demonstrated the successful application of this method to exploring materials science problems using x-ray scattering measurements at a synchrotron beamline. Here, we report several improvements to this methodology that overcome limitations of traditional Kriging methods. The variogram underlying OK is global and thus insensitive to local data variation. We augment the Kriging variance with model-based measures, for instance providing local sensitivity by including the gradient of the surrogate model. As with most statistical regression methods, OK minimizes the number of measurements required to achieve a particular model quality. However, in practice this may not be the most stringent experimental constraint; e.g. the goal may instead be to minimize experiment duration or material usage. We define an adaptive cost function, allowing the autonomous method to balance information gain against measured experimental cost. We provide synthetic and experimental demonstrations, validating that this improved algorithm yields more efficient autonomous data collection.

36 MATERIALS SCIENCE↗

Uncertainty quantification for Bayesian active learning in rupture life prediction of ferritic steels

Abstract Three probabilistic methodologies are developed for predicting the long-term creep rupture life of 9–12 wt%Cr ferritic-martensitic steels using their chemical and processing parameters. The framework developed in this research strives to simultaneously make efficient inference along with associated risk, i.e., the uncertainty of estimation. The study highlights the limitations of applying probabilistic machine learning to model creep life and provides suggestions as to how this might be alleviated to make an efficient and accurate model with the evaluation of epistemic uncertainty of each prediction. Based on extensive experimentation, Gaussian Process Regression yielded more accurate inference ( $$Pearson\;correlation\;coefficent> 0.95$$ P e a r s o n c o r r e l a t i o n c o e f f i c e n t > 0.95 for the holdout test set) in addition to meaningful uncertainty estimate (i.e., coverage ranges from 94 to 98% for the test set) as compared to quantile regression and natural gradient boosting algorithm. Furthermore, the possibility of an active learning framework to iteratively explore the material space intelligently was demonstrated by simulating the experimental data collection process. This framework can be subsequently deployed to improve model performance or to explore new alloy domains with minimal experimental effort.

20 FOSSIL-FUELED POWER PLANTS↗

Predictive machine learning approaches for the microstructural behavior of multiphase zirconium alloys

Abstract Zirconium alloys are widely used in harsh environments characterized by high temperatures, corrosivity, and radiation exposure. These alloys, which have a hexagonal closed packed (h.c.p.) structure thermo-mechanically degrade, when exposed to severe operating environments due to hydride formation. These hydrides have a different crystalline structure, than the matrix, which results in a multiphase alloy. To accurately model these materials at the relevant physical scale, it is necessary to fully characterize them based on a microstructural fingerprint, which is defined here as a combination of features that include hydride geometry, parent and hydride texture and crystalline structure of these multiphase alloys. Hence, this investigation will develop a reduced order modeling approach, where this microstructural fingerprint is used to predict critical fracture stress levels that are physically consistent with microstructural deformation and fracture modes. Machine Learning (ML) methodologies based on Gaussian Process Regression, random forests, and multilayer perceptrons (MLP) were used to predict material fracture critical stress states. MLPs, or neural networks, had the highest accuracy on held-out test sets across three predetermined strain levels of interest. Hydride orientation, grain orientation or texture, and hydride volume fraction had the greatest effect on critical fracture stress levels and had partial dependencies that were highly significant, and in comparison hydride length and hydride spacing have less effects on fracture stresses. Furthermore, these models were also used accurately predicted material response to nominal applied strains as a function of the microstructural fingerprint.

36 MATERIALS SCIENCE↗

Transfer learning of memory kernels for transferable coarse-graining of polymer dynamics

The present work concerns the transferability of coarse-grained (CG) modeling in reproducing the dynamic properties of the reference atomistic systems across a range of parameters. In particular, we focus on implicit-solvent CG modeling of polymer solutions. The CG model is based on the generalized Langevin equation, where the memory kernel plays the critical role in determining the dynamics in all time scales. Thus, we propose methods for transfer learning of memory kernels. The key ingredient of our methods is Gaussian process regression. By integration with the model order reduction via proper orthogonal decomposition and the active learning technique, the transfer learning can be practically efficient and requires minimum training data. Through two example polymer solution systems, we demonstrate the accuracy and efficiency of the proposed transfer learning methods in the construction of transferable memory kernels. The transferability allows for out-of-sample predictions, even in the extrapolated domain of parameters. Built on the transferable memory kernels, the CG models can reproduce the dynamic properties of polymers in all time scales at different thermodynamic conditions (such as temperature and solvent viscosity) and for different systems with varying concentrations and lengths of polymers.

Ma, Zhan↗

Machine learning-assisted ultrafast flash sintering of high-performance and flexible silver–selenide thermoelectric devices

Flexible thermoelectric generators (TEGs) have shown immense potential for serving as a power source for wearable electronics and the Internet of Things. A key challenge preventing large-scale application of TEGs lies in the lack of a high-throughput processing method, which can sinter thermoelectric (TE) materials rapidly while maintaining their high thermoelectric properties. Herein, we integrate high-throughput experimentation and Bayesian optimization (BO) to accelerate the discovery of the optimum sintering conditions of silver–selenide TE films using an ultrafast intense pulsed light (flash) sintering technique. Due to the nature of the high-dimensional optimization problem of flash sintering processes, a Gaussian process regression (GPR) machine learning model is established to rapidly recommend the optimum flash sintering variables based on Bayesian expected improvement. For the first time, an ultrahigh-power factor flexible TE film (a power factor of 2205 μW m -1 K -2 with a zT of 1.1 at 300 K) is demonstrated with a sintering time less than 1.0 second, which is several orders of magnitude shorter than that of conventional thermal sintering techniques. Further, the films also show excellent flexibility with 92% retention of the power factor (PF) after 10 3 bending cycles with a 5 mm bending radius. In addition, a wearable thermoelectric generator based on the flash-sintered films generates a very competitive power density of 0.5 mW cm -2 at a temperature difference of 10 K. This work not only shows the tremendous potential of high-performance and flexible silver–selenide TEGs but also demonstrates a machine learning-assisted flash sintering strategy that could be used for ultrafast, high-throughput and scalable processing of functional materials for a broad range of energy and electronic applications.

25 ENERGY STORAGE↗

Machine learning inversion from small-angle scattering for charged polymers

We develop Monte Carlo simulations for uniformly charged polymers and a machine learning algorithm to interpret the intra-polymer structure factor of the charged polymer system, which can be obtained from small-angle scattering experiments. The polymer is modeled as a chain of fixed-length bonds, where the connected bonds are subject to bending energy, and there is also a screened Coulomb potential for charge interaction between all joints. The bending energy is determined by the intrinsic bending stiffness, and the charge interaction depends on the interaction strength and screening length. All three contribute to the stiffness of the polymer chain and lead to longer and larger polymer conformations. The screening length also introduces a second length scale for the polymer besides the bending persistence length. To obtain the inverse mapping from the structure factor to these polymer conformation and energy-related parameters, we generate a large data set of structure factors by running simulations for a wide range of polymer energy parameters. We use principal component analysis to investigate the intra-polymer structure factors and determine the feasibility of the inversion using the nearest neighbor distance. We employ Gaussian process regression to achieve the inverse mapping and extract the characteristic parameters of polymers from the structure factor with low relative error.

36 MATERIALS SCIENCE↗

Machine learning-assisted profiling of a kinked ladder polymer structure using scattering

Ladder polymers consisting of fused rings in the backbone have very limited conformational freedom, which results in very different properties from traditional linear polymers. However, accurately determining their size and chain conformations from solution scattering remains a challenge. Their chain conformations of kinked ladder polymers are largely governed by the structures and relative orientations or configurations of the repeat units, unlike conventional polymer chains whose bending angles between repeat units follow a unimodal Gaussian distribution. Meanwhile, traditional scattering models for polymer chains do not account for these unique structural features. This work introduces a novel approach that integrates machine learning with Monte Carlo simulations to construct a model that can describe the geometry of a type of kinked CANAL ladder polymers. We first develop a Monte Carlo simulation model for sampling the configuration space of CANAL ladder polymers, where each repeat unit is modeled as a biaxial segment. Then, we establish a machine learning-assisted scattering analysis framework based on Gaussian Process Regression. Finally, we conduct small-angle neutron scattering experiments on a CANAL ladder polymer solution to apply our approach. Our method uncovers structural features of such ladder polymers that conventional methods fail to capture.

Ding, Lijie [Oak Ridge National Laboratory (ORNL),↗