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At least 73 records · Page 4

Off-Equilibrium Reactivity of Boron-Enriched Metal Diboride Surfaces in Electroreduction Conditions

Boron-based materials, featuring B-dependent reactivity and diverse phases, are emerging as promising catalyst systems. However, the catalytic mechanism on many borides remains poorly understood due to complex surface reconstructions under reaction conditions. Here, we investigate the MoB 2 surface in conditions of hydrogen evolution reaction in acidic media, using grand canonical global optimization, grand canonical density functional theory, ab initio molecular dynamics, free energy surface sampling, and an analytical model for electrochemical barrier evaluation. We propose a boron-enrichment strategy to tune the surface reactivity of the hexagonal face of MoB 2 . We reveal the dynamic nature of the B-enriched surface under H coverage and kinetic trapping of the system in the metastable regime with an extensive examination of the deactivation pathways. The metastable center B site on B-enriched surfaces, featuring buckled-up configuration and a usual relaxation effect, is found to be highly active toward HER via the Volmer–Heyrovsky mechanism. In conclusion, this work demonstrates how off-equilibrium behaviors can arise from the interplay between adsorbate coverage and surface reconstruction on a seemingly simple surface, and we present a theoretical framework and computational workflows to address these behaviors, along with other realistic complexities, in kinetics simulations.

Adsorption↗

Enhancing the activity of Pd ensembles on graphene by manipulating coordination environment

Atomic dispersion of metal catalysts on a substrate accounts for the increased atomic efficiency of single-atom catalysts (SACs) in various catalytic schemes compared to the nanoparticle counterparts. However, lacking neighboring metal sites has been shown to deteriorate the catalytic performance of SACs in a few industrially important reactions, such as dehalogenation, CO oxidation, and hydrogenation. Metal ensemble catalysts (M n ), an extended concept to SACs, have emerged as a promising alternative to overcome such limitation. Inspired by the fact that the performance of fully isolated SACs can be enhanced by tailoring their coordination environment (CE), we here evaluate whether the CE of M n can also be manipulated in order to enhance their catalytic activity. We synthesized a set of Pd ensembles (Pd n ) on doped graphene supports (Pd n /X-graphene where X = O, S, B, and N). We found that introducing S and N onto oxidized graphene modifies the first shell of Pd n converting Pd–O to Pd–S and Pd–N, respectively. Also, we further found that the B dopant significantly affected the electronic structure of Pd n by serving as an electron donor in the second shell. We examined the performance of Pd n /X-graphene toward selective reductive catalysis, such as bromate reduction, brominated organic hydrogenation, and aqueous-phase CO 2 reduction. We observed that Pd n /N-graphene exhibited superior performance by lowering the activation energy of the rate-limiting step, i.e., H 2 dissociation into atomic hydrogen. The results collectively suggest controlling the CE of SACs in an ensemble configuration is a viable strategy to optimize and enhance their catalytic performance.

36 MATERIALS SCIENCE↗

Optimizers for stabilizing likelihood-free inference

A growing number of applications in particle physics and beyond use neural networks as unbinned likelihood ratio estimators applied to real or simulated data. Precision requirements on the inference tasks demand a high-level of stability from these networks, which are affected by the stochastic nature of training. We show how physics concepts can be used to stabilize network training through a physics-inspired optimizer. In particular, the energy conserving descent (ECD) optimization framework uses classical Hamiltonian dynamics on the space of network parameters to reduce the dependence on the initial conditions while also stabilizing the result near the minimum of the loss function. We develop a version of this optimizer known as , which has few free hyperparameters with limited ranges guided by physical reasoning. We apply to representative likelihood-ratio estimation tasks in particle physics and find on average that it out-performs the widely used Adam optimizer. We expect that ECD will be a useful tool for wide array of data-limited problems, where it is computationally expensive to exhaustively optimize hyperparameters and mitigate fluctuations with ensembling.

Monte Carlo methods↗

A Semi-supervised Hybrid Machine Learning Framework for the Qualification of Resistance Spot Welds

• Industries requiring high structural integrity, including automotive, aerospace, and construction, place considerable significance on weld quality classification. • The inspection normally involves human expertise through predefined quality metrics that are subjective, error-prone, and time-intensive • The challenge to classification model development is the scarcity of labeled data and imbalanced distributions in the data that are labeled. • This work develops a new hybrid methodology that achieves clustering using KMeans++ together with supervised classification to overcome these challenges. • The ensemble-based classifiers were identified as optimal, with accuracy enhancements of up to 8% using the pseudo-labeled dataset. • The work provides practical insight into feature engineering and machine learning integration in industrial quality assurance applications.

Rogers, Jeremy K. [Savannah River National Laborat↗

STOCHASTIC OPTIMAL POWER FLOW FOR REAL-TIME MANAGEMENT OF DISTRIBUTED RENEWABLE GENERATION AND DEMAND RESPONSE (Final Report)

To meet the grand challenge of a sustainable energy future, there has been a surge of interest in renewable energy. Today, the uncertainty associated with renewable resources is handled by using operating reserves. The high penetration of renewable resources, however, introduces difficult-to-control dynamics and challenges for power system operation. Decision support tools are necessary at the bulk system operational level to recognize and efficiently utilize renewable resources and distributed demand response products in concert with traditional grid resources. It is envisaged that responsive load can potentially have very significant cost advantages over either spinning or non-spinning ramping reserve. Critical decisions are made during hour(s)-ahead and real-time power system operation regarding the commitment and dispatch of generators to ensure power delivery is both reliable and economic. These decisions are typically made by a security constrained optimal flow, which determines future generator commitments, dispatches, and ensures adequate reserves are available in the event of a contingency (unexpected outage) or if future system conditions deviate from forecasts. However, security has been always based on a pre-specified subset of contingency constraints whose enforcement does not guarantee security under all possible future possibilities while also giving little or no weight to the likelihood of each contingent event or the severity of its consequences. Existing tools, which are based exclusively on deterministic optimization models, do not yield optimal operational decisions to address these new challenges, in terms of both reliability and cost-effectiveness. This project has focused on developing a stochastic optimal power flow (SOPF) framework, which integrates renewable resource uncertainty, load uncertainty, distributed storage (DS), demand response (DR) products, in a holistic manner to address the uncertainty associated with ever-increasing renewable resources, along with the inclusion of distributed demand response products in future power systems. A proof-of-concept problem was created using the Pennsylvania-Jersey-Maryland (PJM) power system network. Synthetic wind generation was added to the system to simulate 50% wind penetration. A 1-hour test of SOPF operation indicated more than 6% operational cost savings. The project continued by adding the Midwestern Independent System Operator (MISO) as a partner, with focus shifting from SOPF to Stochastic Look-Ahead Unit Commitment (SLAC). Unlike PJM, MISO is faced with significant renewable energy resources within its footprint and is challenged with substantial uncertainty in its operations. The SLAC distinguishes itself from existing tools that operators use. At best, today’s tools solve two to three cases independently, where one or two system parameters, such as forecasted load level (e.g., a low, base, and high forecast), are varied and the resulting scenarios are analyzed independently. The stochastic-based optimization of SLAC leverages statistical information from an ensemble of potential operational scenarios and their respective likelihood. The SLAC output can be translated into valuable information to the operator such as suggested commitments, optimal scheduling and dispatch of resources, reserve requirements at both locational and zonal resolutions, ramping availability and requirements, availability of demand response including operational guidance concerning the near-term and real-time coordination between distributed energy resources, and utilization of distributed storage resources. The developed SOPF/SLAC tool, a stand-alone tool compatible with existing EMSs, will provide system operators with unprecedented visibility, flexibility and predictability to these resources and operational guidance concerning the real-time coordination between DERs and DR/DS products. The game changing and practical impact of this disruptive technology will be dramatic and will usher in a new era in the electric power industry, wherein green energy concepts are fully embraced, and electric power costs are lowered throughout the nation.

42 ENGINEERING↗

A machine learning approach targeting parameter estimation for plant functional type coexistence modeling using ELM-FATES (v2.0)

Tropical forest dynamics play a crucial role in the global carbon, water, and energy cycles. However, realistically simulating the dynamics of competition and coexistence between different plant functional types (PFTs) in tropical forests remains a significant challenge. This study aims to improve the modeling of PFT coexistence in the Functionally Assembled Terrestrial Ecosystem Simulator (FATES), a vegetation demography model implemented in the Energy Exascale Earth System Model (E3SM) land model (ELM), ELM-FATES. Specifically, we explore (1) whether plant trait relationships established from field measurements can constrain ELM-FATES simulations and (2) whether machine learning (ML)-based surrogate models can emulate the complex ELM-FATES model and optimize parameter selections to improve PFT coexistence modeling. We conducted three ensembles of ELM-FATES experiments at a tropical forest site near Manaus, Brazil. By comparing the ensemble experiments without (Exp-CTR) and with (Exp-OBS) consideration of observed trait relationships, we found that accounting for these relationships slightly improves the simulations of water, energy, and carbon variables when compared to observations but degrades the simulation of PFT coexistence. Using ML-based surrogate models trained on Exp-CTR, we optimized the trait parameters in ELM-FATES and conducted another ensemble of experiments (Exp-ML) with these optimized parameters. The proportion of PFT coexistence experiments significantly increased from 21 % in Exp-CTR to 73 % in Exp-ML. After filtering the experiments that allow for PFT coexistence to agree with observations (within 15 % tolerance), 33 % of the Exp-ML experiments were retained, which is a significant improvement compared to the 1.4 % in Exp-CTR. Exp-ML also accurately reproduces the annual means and seasonal variations in water, energy, and carbon fluxes and the field inventory of aboveground biomass. This study represents a reproducible method that utilizes machine learning to identify parameter values that improve model fidelity against observations and PFT coexistence in vegetation demography models for diverse ecosystems. Our study also suggests the need for new mechanisms to enhance the robust simulation of coexisting plants in ELM-FATES and has significant implications for modeling the response and feedbacks of ecosystem dynamics to climate change.

54 ENVIRONMENTAL SCIENCES↗

BEAST

The Bilinear Ensemble Actuation Synthesis Toolkit (BEAST) is a computational platform that optimizes time-varying control signals to achieve a specified transfer of states governed by bilinear ensemble systems in which model parameters are subject to uncertainty.

Zlotnik, anatoly↗

GMRES with embedded ensemble propagation for the efficient solution of parametric linear systems in uncertainty quantification of computational models

In a previous work, embedded ensemble propagation was proposed to improve the efficiency of sampling-based uncertainty quantification methods of computational models on emerging computational architectures. It consists of simultaneously evaluating the model for a subset of samples together, instead of evaluating them individually. A first approach introduced to solve parametric linear systems with ensemble propagation is ensemble reduction. In Krylov methods for example, this reduction consists in coupling the samples together using an inner product that sums the sample contributions. Ensemble reduction has the advantages of being able to use optimized implementations of BLAS functions and having a stopping criterion which involves only one scalar. However, the reduction potentially decreases the rate of convergence due to the gathering of the spectra of the samples. In this paper, we investigate a second approach: ensemble propagation without ensemble reduction in the case of GMRES. This second approach solves each sample simultaneously but independently to improve the convergence compared to ensemble reduction. This raises two new issues which are solved in this paper: the fact that optimized implementations of BLAS functions cannot be used anymore and that ensemble divergence, whereby individual samples within an ensemble must follow different code execution paths, can occur. We tackle those issues by implementing a high-performing ensemble GEMV and by using masks. The proposed ensemble GEMV leads to a similar cost per GMRES iteration for both approaches, i.e. with and without reduction. For illustration, we study the performances of the new linear solver in the context of a mesh tying problem. Furthermore, this example demonstrates improved ensemble propagation speed-up without reduction.

BLAS↗

Optimal Twirling Depth for Classical Shadows in the Presence of Noise

The classical shadows protocol is an efficient strategy for estimating properties of an unknown state p using a small number of state copies and measurements. In its original form, it involves twirling the state with unitaries from some ensemble and measuring the twirled state in a fixed basis. It was recently shown that for computing local properties, optimal sample complexity (copies of the state required) is remarkably achieved for unitaries drawn from shallow depth circuits composed of local entangling gates, as opposed to purely local (zero depth) or global twirling (infinite depth) ensembles. Here, we consider the sample complexity as a function of the depth of the circuit, in the presence of noise. We find that this noise has important implications for determining the optimal twirling ensemble. Under fairly general conditions, we (i) show that any single-site noise can be accounted for using a depolarizing noise channel with an appropriate damping parameter f, (ii) compute thresholds f th at which optimal twirling reduces to local twirling for Pauli operators, (iii) nth order Renyi entropies (n ≥2), and (iv) provide a meaningful upper bound t max on the optimal circuit depth for any finite noise strength f, which applies to observables and entanglement entropy measurements. In conclusion, these thresholds strongly constrain the search for optimal strategies to implement shadow tomography and are easily tailored to the experimental system at hand.

97 MATHEMATICS AND COMPUTING↗

Minimizing CGYRO HPC Communication Costs in Ensembles with XGYRO by Sharing the Collisional Constant Tensor Structure

First-principles fusion plasma simulations are both compute and memory intensive, and CGYRO is no exception. The use of many HPC nodes to fit the problem in the available memory thus results in significant communication overhead, which is hard to avoid for any single simulation. That said, most fusion studies are composed of ensembles of simulations, so we developed a new tool, named XGYRO, that executes a whole ensemble of CGYRO simulations as a single HPC job. By treating the ensemble as a unit, XGYRO can alter the global buffer distribution logic and apply optimizations that are not feasible on any single simulation, but only on the ensemble as a whole. The main saving comes from the sharing of the collisional constant tensor structure, since its values are typically identical between parameter-sweep simulations. This data structure dominates the memory consumption of CGYRO simulations, so distributing it among the whole ensemble results in drastic memory savings for each simulation, which in turn results in overall lower communication overhead.

CGYRO↗

Ensemble Learning Based Convex Approximation of Three-Phase Power Flow

Though the convex optimization has been widely used in power systems, it still cannot guarantee to yield a tight (accurate) solution to some problems. To mitigate this issue, this paper proposes an ensemble learning based convex approximation for alternating current (AC) power flow equations that differs from the existing convex relaxations. The proposed approach is based on three-phase quadratic power flow equations in rectangular coordinates. To develop this data-driven convex approximation of power flows, the polynomial regression (PR) is first deployed as a basic learner to fit convex relationships between the independent and dependent variables. Then, ensemble learning algorithms such as gradient boosting (GB) and bagging are introduced to combine learners to boost model performance. Based on the learned convex approximation of power flow, optimal power flow (OPF) is formulated as a convex quadratic programming problem. The simulation results on IEEE standard cases of both balanced and unbalanced systems show that, in the context of solving OPF, the proposed data-driven convex approximation outperforms the conventional semi-definite programming (SDP) relaxation in both accuracy and computational efficiency, especially in the cases that the conventional SDP relaxation fails

Convex approximation↗

Application-specific optimal model weighting of global climate models: A red tide example

Global climate models (GCMs) and Earth system models (ESMs) provide many climate services with environmental relevance. The High Resolution Model Inter-comparison Project (HighResMIP) of the Coupled Model Intercomparison Project Phase 6 (CMIP6) provides model runs of GCMs and ESMs to address regional phenomena. Developing a parsimonious ensemble of CMIP6 requires multiple ensemble methods such as independent-model subset selection, prescreening-based subset selection, and model weighting. The work presented here focuses on application-specific optimal model weighting, with prescreening-based subset selection. As such, independent ensemble members are categorized, selected, and weighted based on their ability to reproduce physically-interpretable features of interest that are problem-specific. We discuss the strengths and caveats of optimal model weighting using a case study of red tide prediction in the Gulf of Mexico along the West Florida Shelf. Red tide is a common name of specific harmful algal blooms that occur worldwide, causing adverse socioeconomic and environmental impacts. Our results indicate the importance of prescreening-based subset selection as optimal model weighting can underplay robust ensemble members by optimizing error cancellation. Prescreening-based subset selection also provides insights about the validity of the model weights. By illustrating the caveats of using non-representative models when optimal model weighting is used, the findings and discussion of this study are pertinent to many other climate services.

54 ENVIRONMENTAL SCIENCES↗

Evolving Ensembles of Spiking Neural Networks for Neuromorphic Systems

Evolutionary algorithms have been proposed as a solution to overcome many of the challenges associated with training spiking neural networks. While evolutionary optimization for spiking neural networks is very flexible, its performance has difficulty scaling to complex tasks and correspondingly complex network structures. Here we propose a method for evolving ensembles of spiking neural networks. By using ensemble learning, the flexibility of evolutionary optimization is fully preserved while scaling to more challenging tasks. We test the performance of the proposed method using handwritten digit classification. We investigate multiple strategies for constructing ensembles of spiking neural networks, and demonstrate that evolving ensembles of SNNs offers significant performance advantages over evolutionary optimization.

Elbrecht, Daniel↗

Resilience-based Recovery Scheduling of Transportation Network in Mixed Traffic Environment: A Deep-Ensemble-Assisted Active Learning Approach

Devising effective post-hazard recovery strategies is critical in enhancing the resilience of transportation networks (TNs). However, existing work does not consider the multiclass users’ travel behavior in network functionality quantification and the metaheuristic solution procedures often suffer from extensive computational burden due to the exploration need in large solution space and the expensive functionality quantification. Here, this study develops a bilevel decision-making framework for the resilience-based recovery scheduling of the TN in a mixed traffic environment with connected and autonomous vehicles (CAVs) and human-driven vehicles (HDVs). The lower level quantifies the TN's functionality over time considering different travel behavior of CAV and HDV users arisen from their different levels of information perception. The upper level presents a novel deep-ensemble-assisted active learning approach to balance optimization performance and computational cost. This framework can help decision makers better quantify the TN's functionality to support effective recovery scheduling of TN with different mixed traffic scenarios ranging from HDV-only to future CAV-dominant traffic. The optimization approach bears the potential to be extended to solving general large-scale network recovery scheduling problems effectively and efficiently. The proposed methodology is demonstrated using a real-world traffic network in Southern California under earthquake considering deterministic and stochastic repair durations.

42 ENGINEERING↗

Models, data, and scripts associated with “Prediction of Distributed River Sediment Respiration Rates using Community-Generated Data and Machine Learning”

This data package is associated with the publication “Prediction of Distributed River Sediment Respiration Rates using Community-Generated Data and Machine Learning’’ submitted to the Journal of Geophysical Research: Machine Learning and Computation (Scheibe et al. 2024). River sediment respiration observations are expensive and labor intensive to obtain and there is no physical model for predicting this quantity. The Worldwide Hydrobiogeochemisty Observation Network for Dynamic River Systems (WHONDRS) observational data set (Goldman et al.; 2020) is used to train machine learning (ML) models to predict respiration rates at unsampled sites. This repository archives training data, ML models, predictions, and model evaluation results for the purposes of reproducibility of the results in the associated manuscript and community reuse of the ML models trained in this project. One of the key challenges in this work was to find an optimum configuration for machine learning models to work with this feature-rich (i.e. 100+ possible input variables) data set. Here, we used a two-tiered approach to managing the analysis of this complex data set: 1) a stacked ensemble of ML models that can automatically optimize hyperparameters to accelerate the process of model selection and tuning and 2) feature permutation importance to iteratively select the most important features (i.e. inputs) to the ML models. The major elements of this ML workflow are modular, portable, open, and cloud-based, thus making this implementation a potential template for other applications. This data package is associated with the GitHub repository found at Please see the file level metadata (flmd; “sl-archive-whondrs_flmd.csv”) for a list of all files contained in this data package and descriptions for each. Please see the data dictionary (dd; “sl-archive-whondrs_dd.csv”) for a list of all column headers contained within comma separated value (csv) files in this data package and descriptions for each. The GitHub repository is organized into five top-level directories: (1) “input_data” holds the training data for the ML models; (2) “ml_models” holds machine learning models trained on the data in “input_data”; (3) “scripts” contains data preprocessing and postprocessing scripts and intermediate results specific to this data set that bookend the ML workflow; (4) “examples” contains the visualization of the results in this repository including plotting scripts for the manuscript (e.g., model evaluation, FPI results) and scripts for running predictions with the ML models (i.e., reusing the trained ML models); (5) “output_data” holds the overall results of the ML model on that branch. Each trained ML model resides on its own branch in the repository; this means that inputs and outputs can be different branch-to-branch. Furthermore, depending on the number of features used to train the ML models, the preprocessing and postprocessing scripts, and their intermediate results, can also be different branch-to-branch. The “main-*” branches are meant to be starting points (i.e. trunks) for each model branch (i.e. sprouts). Please see the Branch Navigation section in the top-level README.md in the GitHub repository for more details. There is also one hidden directory “.github/workflows”. This hidden directory contains information for how to run the ML workflow as an end-to-end automated GitHub Action but it is not needed for reusing the ML models archived here. Please the top-level README.md in the GitHub repository for more details on the automation.

13C↗

HAIMOS Ensemble Forecasts for Intra-day and Day- Ahead GHI, DNI and Ramps

The objective of this research is to develop a hybrid physics-based/data-driven forecast model to improve direct normal and global horizontal irradiance (DNI and GHI) prediction for horizons ranging from 1 to 72 hours. Project objectives also address key gaps in state-of-the-art solar forecasting: accurate probabilistic solar forecasts and the forecasting of large irradiance ramps (ramp onset and magnitude). The proposed model ensembles Numerical Weather Prediction (NWP) forecasts, determinist physics-based algorithms, and new-generation cloud cover products (high-resolution rapid refresh satellite images and Large Eddy Simulations). The result is the Hybrid Adaptive Input Model Objective Selection (HAIMOS) ensemble model. HAIMOS blends state of the art machine learning methodologies with physics-based models for cloud cover and cloud optical depth forecasts. The technical activities followed a two-pronged strategy. First, the preprocessing of data, the selection of inputs to the nonlinear approximators, the type of approximator and objective functions, and post-processing ensembling techniques included in HAIMOS were all optimized adaptively to find the best model for a specific goal (reduce DNI/GHI forecast error, improve the prediction of ramp onset, etc.). Second, a large effort was put in improving cloud identification and the forecast of cloud cover and cloud optical depth. To this end, new-generation cloud parametrization products were developed in this work. These include improved algorithms to assist in cloud identification, cloud classification and cloud parametrization from satellite images – three key factors in the accuracy of 1 to 6-hours irradiance forecasts and prediction of ramp onset. Furthermore, we also included cloud information extracted from high resolution rapid refresh satellite images (GOES-16) and Large Eddy Simulations (LES). LES was used to model the atmosphere in detail over locations of interest and produce cloud optical depth forecasts. Once these data streams were validated, they were used as input data to the HAIMOS forecast. The model was developed using data from several climatologically distinct locations with potential for high solar penetration. In the last year of the project, we conducted a validation campaign according to the guidelines stipulated by the Topic Area 1 project as described in the FOA. This effort brings, for the first time, proven machine-learning methodologies for generating state-of-the-art solar forecasts interweaved with detailed physics-based models for cloud detection, and cloud optical depth forecasts. HAIMOS will generate accurate irradiance probabilistic forecast to assist in reducing solar generation prediction error. Globally optimized solar forecast models are more likely to impact solar energy stakeholders. The goal of this project was to increase the state-of-the-art forecast skill from their present values of 10 to 35%. At the end of the project, we achieved between 30% and 50% forecast skill across a wide range of horizons for both GHI and DNI.

14 SOLAR ENERGY↗

Spin squeezing of macroscopic nuclear spin ensembles

Spin squeezing has been explored in atomic systems as a tool for quantum sensing, improving experimental sensitivity beyond the spin standard quantum limit for certain measurements. To optimize absolute metrological sensitivity, it is beneficial to consider macroscopic spin ensembles, such as nuclear spins in solids and liquids. Coupling a macroscopic spin ensemble to a parametrically-modulated resonant circuit can create collective spin squeezing by generating spin correlations mediated by the circuit. We analyze the squeezing dynamics in the presence of decoherence and finite spin polarization, showing that achieving 7 dB spin squeezing is feasible in several nuclear spin systems. The metrological benefit of squeezing a macroscopic spin ensemble lies in the suppression of technical noise sources in the spin detection system relative to the spin projection noise. This expands the experimental sensitivity bandwidth when searching for signals of unknown frequency and can improve the resonant signal-to-noise ratio. Squeezing macroscopic spin ensembles may prove to be a useful technique for fundamental physics experiments aimed at detecting spin interactions with oscillating background fields, such as ultralight dark matter. Published by the American Physical Society 2025

Boyers, Eric↗