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At least 127 records · Page 7

Numerical Simulation of Vibrational Sum Frequency Generation Intensity for Non-Centrosymmetric Domains Interspersed in an Amorphous Matrix: A Case Study for Cellulose in Plant Cell Wall

Vibrational sum frequency generation (SFG) spectroscopy can specifically probe molecular species non-centrosymmetrically arranged in a centrosymmetric or isotropic medium. This capability has been extensively utilized to detect and study molecular species present at the two-dimensional (2D) interface at which the centrosymmetry or isotropy of bulk phases is naturally broken. The same principle has been demonstrated to be very effective for the selective detection of non-centrosymmetric crystalline nanodomains interspersed in three-dimensional (3D) amorphous phases. However, the full spectral interpretation of SFG features has been difficult due to the complexity associated with the theoretical calculation of SFG responses of such 3D systems. This paper describes a numerical method to predict the relative SFG intensities of non-centrosymmetric nanodomains in 3D systems as functions of their size and concentration as well as their assembly patterns, i.e., the distributions of tilt, azimuth, and rotation angles with respect to the lab coordinate. We applied the developed method to predict changes in the CH and OH stretch modes characteristic to crystalline cellulose microfibrils distributed with various orders, which are relevant to plant cell wall structures. As a result, the same algorithm can also be applied to any SFG-active nanodomains interspersed in 3D amorphous matrices.

36 MATERIALS SCIENCE↗

Data-Driven Learning for the Mori--Zwanzig Formalism: A Generalization of the Koopman Learning Framework

A theoretical framework which unifies the conventional Mori--Zwanzig formalism and the approximate Koopman learning of deterministic dynamical systems from noiseless observation is presented. In this framework, the Mori--Zwanzig formalism, developed in statistical mechanics to tackle the hard problem of construction of reduced-order dynamics for high-dimensional dynamical systems, can be considered as a natural generalization of the Koopman description of the dynamical system. We next show that, similar to the approximate Koopman learning methods, data-driven methods can be developed for the Mori--Zwanzig formalism with Mori's linear projection operator. We have developed two algorithms to extract the key operators, the Markov and the memory kernel, using time series of a reduced set of observables in a dynamical system. We have adopted the Lorenz `96 system as a test problem and solved for the above operators. These operators exhibit complex behaviors, which are unlikely to be captured by traditional modeling approaches in Mori--Zwanzig analysis. The nontrivial generalized fluctuation-dissipation relationship, which relates the memory kernel with the two-time correlation statistics of the orthogonal dynamics, was numerically verified as a validation of the solved operators. Here we present numerical evidence that the generalized Langevin equation, a key construct in the Mori--Zwanzig formalism, is more advantageous in predicting the evolution of the reduced set of observables than the conventional approximate Koopman operators.

97 MATHEMATICS AND COMPUTING↗

Resilient Operation of Networked Community Microgrids with High Solar Penetration

This project, funded by the US Department of Energy’s Solar Energy Technologies Office (SETO), focused on the operation of microgrids as a coordinated network. The primary objective, which was successfully achieved, was to develop both control strategies and hardware solutions to support the resilient and efficient operation of networked microgrids with high solar penetration. The work was structured around the following four main tasks: • Development of distributed and scalable optimization algorithms for AC-coupled networked microgrids. • Design and implementation of a novel DC interconnection hardware to enable precise power exchange between microgrids. • Laboratory operational validation of the developed technologies using 480 V testbeds and commercially available hardware. • Field operational validation of the complete solution in Adjuntas, Puerto Rico, interconnecting two kW-scale, split-phase microgrids of Casa Pueblo’s microgrids. This project addressed multiple technical challenges across the domains of optimization, control, hardware interconnection, and protection. One of its key contributions was delivering tangible, real-world solutions for networking microgrids. In contrast to purely theoretical or simulation-based work, this project included full-scale hardware operational validation both in the lab and in the field. The work conducted as part of this project—in collaboration with the University of Puerto Rico; the University of Tennessee, Knoxville; the University of Central Florida; and Casa Pueblo—has advanced the state of the art in networked microgrids. Key contributions include the development of distributed control strategies, practical solutions for real-world implementation challenges, and the introduction of a novel DC interlink approach for microgrid interconnection. The project featured both laboratory and field validation using commercial off-the-shelf components. The field deployment successfully validated that a group of microgrids can operate in a coordinated manner, enabling precise power flow between systems and mutual support during extreme events. This project resulted in 15 journal publications and 15 conference papers; 5 graduate students and 15 undergraduate students were supported. The codes of distributed optimization and forecasting were made open-source through OSTI.gov for distributed optimization and forecasting. All the publications are available in the ORNL-hosted project landing page. The DC interlink with state-of-charge balancing control was operationally validated in Adjuntas by interconnecting two real-world, 240 V split-phase microgrids. To the best knowledge of the team, this represents the first operational validation of AC microgrids interconnected via DC-interlinks. As a culmination of this project, a follow-on grant was awarded to support the technology transfer of the distributed optimization framework to a commercial microgrid controller, Stellar Edge, developed by the California-based company New Sun Road.

14 SOLAR ENERGY↗

Generalized master equation for particle transport in binary random media with renewal statistics

Particle transport in binary stochastic mixtures is classically modeled assuming Markovian or exponential mixing statistics but in many applications material memory invalidates the Markov assumption. For non-Markovian mixing characterized by alternating renewal processes, a transport-theoretic framework is presented that provides an exact description of transport in nonscattering random binary media with general non-exponential statistics. Our approach is to Markovianize the problem by augmenting the {material type, particle flux} state space with the age or distance from the last interface. A Chapman-Kolmogorov equation is formulated for the joint probability density of the material type, particle flux, and age, and subsequently reduced to a generalized Master equation (GME) in differential form. This constitutes the primary result of this work. A state-updating Monte Carlo algorithm consistent with the GME is developed and benchmarked against analytical solutions for multiple chord-length laws. For purely absorbing renewal statistical media, the GME reproduces analytical benchmarks for the equilibrium age distribution, interior mean/variance of material-conditioned fluxes, and boundary transmittance. Simulations further demonstrate that a Markov (exponential) approximation of non-exponential statistics can introduce large errors in transmittance and interior flux profiles. Lastly, the reintroduction of memory due to scattering is briefly addressed through heuristic considerations.

Fluctuations & noise↗

Toward Mixed Analog-Digital Quantum Signal Processing: Quantum AD/DA Conversion and the Fourier Transform

Signal processing stands as a pillar of classical computation and modern information technology, applicable to both analog and digital signals. Recently, advancements in quantum information science have suggested that quantum signal processing (QSP) can enable more powerful signal processing capabilities. However, the developments in QSP have primarily leveraged digital quantum resources, such as discrete-variable (DV) systems like qubits, rather than analog quantum resources, such as continuous-variable (CV) systems like quantum oscillators. Consequently, there remains a gap in understanding how signal processing can be performed on hybrid CV-DV quantum computers. Here we address this gap by developing a new paradigm of mixed analog-digital QSP. We demonstrate the utility of this paradigm by showcasing how it naturally enables analog-digital conversion of quantum signals—specifically, the transfer of states between DV and CV quantum systems. We then show that such quantum analog-digital conversion enables new implementations of quantum algorithms on CV-DV hardware. This is exemplified by realizing the quantum Fourier transform of a state encoded on qubits via the free-evolution of a quantum oscillator, albeit with a runtime exponential in the number of qubits due to information theoretic arguments. Collectively, this work marks a significant step forward in hybrid CV-DV quantum computation, providing a foundation for scalable analog-digital signal processing on quantum processors.

42 ENGINEERING↗

Randomized Algorithms for Linear Solvers

Recently, randomized algorithms in numerical linear algebra, specifically those centered around random sketching, have gained traction in primarily theoretical research due to their potential to significantly reduce problem dimensionality at the cost of an O(1) multiplicative distortion factor. It has been assumed that this sketching can be done efficiently, but thorough investigation into how precisely to do it has been neglected. Moreover, the theory-based community has argued for sketching’s ability to reduce computational cost via complexity analysis, but has not researched how it affects the stability of the algorithms. At Sandia, efficient linear solvers that scale well on modern HPC architectures while maintaining stability are imperative for practical applications. In this LDRD, we developed a random sketching strategy that is substantially faster than existing ones, and demonstrate its superior performance in practice on a NVIDIA H100 GPU. Moreover, we show how this can be used to significantly outperform existing linear least squares solvers while improving the solver’s stability as well. Additionally, we demonstrate how this sketching strategy can be used to make a fast, stable QR factorization that can subsequently be used in s-step and block Krylov solvers. Finally, we incorporate a sketching-based block orthogonalization scheme into s-step GMRES, which is stable and faster than existing approaches on the Perlmutter supercomputer.

97 MATHEMATICS AND COMPUTING↗

Scalable Implicit Solvers with Dynamic Mesh Adaptation for a Relativistic Drift-Kinetic Fokker–Planck–Boltzmann Model

In this work we consider a relativistic drift-kinetic model for runaway electrons along with a Fokker–Planck operator for small-angle Coulomb collisions, a radiation damping operator, and a secondary knock-on (Boltzmann) collision source. Here, we develop a new scalable fully implicit solver utilizing finite volume and conservative finite difference schemes and dynamic mesh adaptivity. A new data management framework in the PETSc library based on the p4est library is developed to enable simulations with dynamic adaptive mesh refinement (AMR), distributed memory parallelization, and dynamic load balancing of computational work. This framework and the runaway electron solver building on the framework are able to dynamically capture both bulk Maxwellian at the low-energy region and a runaway tail at the high-energy region. To effectively capture features via the AMR algorithm, a new AMR indicator prediction strategy is proposed that is performed alongside the implicit time evolution of the solution. This strategy is complemented by the introduction of computationally cheap feature-based AMR indicators that are analyzed theoretically. Numerical results quantify the advantages of the prediction strategy in better capturing features compared with nonpredictive strategies; and we demonstrate trade-offs regarding computational costs. The robustness with respect to model parameters, algorithmic scalability, and parallel scalability are demonstrated through several benchmark problems including manufactured solutions and solutions of different physics models. We focus on demonstrating the advantages of using implicit time stepping and AMR for runaway electron simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Dynamic mode decomposition with core sketch

With the increase in collected data volumes, either from experimental measurements or high fidelity simulations, there is an ever-growing need to develop computationally efficient tools to process, analyze, and interpret these datasets. Modal analysis techniques have gained great interest due to their ability to identify patterns in the data and extract valuable information about the system being considered. Dynamic mode decomposition (DMD) relies on elements of the Koopman approximation theory to compute a set of modes, each associated with a fixed oscillation frequency and a decay/growth rate. Extracting these details from large datasets can be computationally expensive due to the need to implement singular value decomposition of the input data matrix. Sketching algorithms have become popular in numerical linear algebra where statistical theoretic approaches are utilized to reduce the cost of major operations. A sketch of a matrix is another matrix, which is significantly smaller, but still sufficiently approximates the original system. We put forth an efficient DMD framework, SketchyDMD, based on a core sketching algorithm that captures information about the range and corange (their mutual relationship) of input data. The proposed sketching-based framework can accelerate various portions of the DMD routines, compared to classical methods that operate directly on the raw input data. We conduct numerical experiments using the spherical shallow water equations as a prototypical model in the context of geophysical flows. In conclusion, we show that the proposed SketchyDMD is superior to existing randomized DMD methods that are based on capturing only the range of the input data.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Hydrogen density mapping in biomolecular crystals through dynamic nuclear polarization

Many fundamental biological processes, including those in photosynthetic reaction centers and enzyme active sites, involve charge and energy transfer, bond cleavage, protonation and hydrogen bonding. Because H atoms play such central roles in these reactions, accurately determining their positions is essential. Yet, conventional X-ray crystallography primarily resolves the heavy atoms in biological structures and provides limited insight into hydrogen, even at atomic resolution. Neutron macromolecular crystallography (NMC) overcomes this limitation by offering exceptional sensitivity to hydrogen and deuterium. Here, we present a theoretical framework for the development of dynamic nuclear polarization NMC (DNP-NMC) techniques, which exploit the alignment of neutron and proton nuclear spins to enhance and tune the hydrogen signal contribution. The DNP-NMC approach advances the resolution of H atoms within biomolecular crystals, whether bound to protein residues or present in solvent. The method establishes key relationships for the coherent structure factor of polarized neutron scattering from hydrogenous matter. It theoretically achieves full accuracy in phase reconstruction and offers a path to improve neutron structure determination, achieving accuracies exceeding ≳80% by incorporating titration states. Using a variant of the hybrid input/output phase-retrieval algorithm, it allows recovery of the hydrogen density with ≳90% phase accuracy. In conclusion, we further discuss sources of experimental uncertainty for the upcoming DNP-enabled, quasi-Laue IMAGINE-X experiment at Oak Ridge National Laboratory's High Flux Isotope Reactor.

dynamic nuclear polarization↗

Lithium Metal Battery Quality Control via Transformer–CNN Segmentation

Lithium metal battery (LMB) has the potential to be the next-generation battery system because of its high theoretical energy density. However, defects known as dendrites are formed by heterogeneous lithium (Li) plating, which hinders the development and utilization of LMBs. Non-destructive techniques to observe the dendrite morphology often use X-ray computed tomography (XCT) to provide cross-sectional views. To retrieve three-dimensional structures inside a battery, image segmentation becomes essential to quantitatively analyze XCT images. This work proposes a new semantic segmentation approach using a transformer-based neural network called TransforCNN that is capable of segmenting out dendrites from XCT data. In addition, we compare the performance of the proposed TransforCNN with three other algorithms, U-Net, Y-Net, and E-Net, consisting of an ensemble network model for XCT analysis. Our results show the advantages of using TransforCNN when evaluating over-segmentation metrics, such as mean intersection over union (mIoU) and mean Dice similarity coefficient (mDSC), as well as through several qualitatively comparative visualizations.

Quenum, Jerome (ORCID:0000000271265853)↗

Advanced fuel fusion, phase space engineering, and structure-preserving geometric algorithms

Non-thermal advanced fuel fusion trades the requirement of a large amount of recirculating tritium in the system for that of large recirculating power. Phase space engineering technologies utilizing externally injected electromagnetic fields can be applied to meet the challenge of maintaining non-thermal particle distributions at a reasonable cost. The physical processes of the phase space engineering are studied from a theoretical and algorithmic perspective. It is emphasized that the operational space of phase space engineering is limited by the underpinning symplectic dynamics of charged particles. The phase space incompressibility according to the Liouville theorem is just one of many constraints, and Gromov's non-squeezing theorem determines the minimum footprint of the charged particles on every conjugate phase space plane. In this sense and level of sophistication, the mathematical abstraction of phase space engineering is symplectic topology. To simulate the processes of phase space engineering, such as the Maxwell demon and electromagnetic energy extraction, and to accurately calculate the minimum footprints of charged particles, recently developed structure-preserving geometric algorithms can be used. The family of algorithms conserves exactly, on discretized spacetime, symplecticity and thus incompressibility, non-squeezability, and symplectic capacities. The algorithms apply to the dynamics of charged particles under the influence of external electromagnetic fields as well as the charged particle–electromagnetic field system governed by the Vlasov–Maxwell equations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Quantum computing and preconditioners for hydrological linear systems

Modeling hydrological fracture networks is a hallmark challenge in computational earth sciences. Accurately predicting critical features of fracture systems, e.g. percolation, can require solving large linear systems far beyond current or future high performance capabilities. Quantum computers can theoretically bypass the memory and speed constraints faced by classical approaches, however several technical issues must first be addressed. Chief amongst these difficulties is that such systems are often ill-conditioned, i.e. small changes in the system can produce large changes in the solution, which can slow down the performance of linear solving algorithms. We test several existing quantum techniques to improve the condition number, but find they are insufficient. We then introduce the inverse Laplacian preconditioner, which improves the scaling of the condition number of the system from O(N) to O($\sqrt{N}$) and admits a quantum implementation. These results are a critical first step in developing a quantum solver for fracture systems, both advancing the state of hydrological modeling and providing a novel real-world application for quantum linear systems algorithms.

97 MATHEMATICS AND COMPUTING↗

An Efficient Bayesian Approach to Learning Droplet Collision Kernels: Proof of Concept Using “Cloudy,” a New n -Moment Bulk Microphysics Scheme

The small-scale microphysical processes governing the formation of precipitation particles cannot be resolved explicitly by cloud resolving and climate models. Instead, they are represented by microphysics schemes that are based on a combination of theoretical knowledge, statistical assumptions, and fitting to data (“tuning”). Historically, tuning was done in an ad hoc fashion, leading to parameter choices that are not explainable or repeatable. Recent work has treated it as an inverse problem that can be solved by Bayesian inference. The posterior distribution of the parameters given the data—the solution of Bayesian inference—is found through computationally expensive sampling methods, which require over $\mathcal{O}$(10 5 ) evaluations of the forward model; this is prohibitive for many models. We present a proof of concept of Bayesian learning applied to a new bulk microphysics scheme named “Cloudy,” using the recently developed Calibrate-Emulate-Sample (CES) algorithm. Cloudy models collision-coalescence and collisional breakup of cloud droplets with an adjustable number of prognostic moments and with easily modifiable assumptions for the cloud droplet mass distribution and the collision kernel. The CES algorithm uses machine learning tools to accelerate Bayesian inference by reducing the number of forward evaluations needed to $\mathcal{O}$(10 2 ). It also exhibits a smoothing effect when forward evaluations are polluted by noise. In a suite of perfect-model experiments, we show that CES enables computationally efficient Bayesian inference of parameters in Cloudy from noisy observations of moments of the droplet mass distribution. In an additional imperfect-model experiment, a collision kernel parameter is successfully learned from output generated by a Lagrangian particle-based microphysics model.

54 ENVIRONMENTAL SCIENCES↗

A Multireference Approach to Electron and Electron–Nuclear Dynamics in Nanomaterials (Final Report)

Many important chemical and physical phenomena involve dynamics on large number of electronic states. Thus, there is a critical need to develop methods to simulate dynamics in dense manifolds of states. Towards this end, we have: a) developed the multiple cloning in dense manifolds of states (MCDMS) method, which is capable of accurately modeling the quantum mechanical coherence between populations on a large number of electronic states, b) implemented MCDMS into the free, open-source PySpawn software package, c) developed graphics processing unit-accelerated algorithms modeling electron dynamics in light fields via Floquet time-dependent configuration interaction (F-TDCI), and d) critically compared different orbital bases in order to achieve an accurate and efficient F-TDCI expansion. This grant ended in August 2020, when our group moved to from Michigan State University to Stony Brook University, where this project continues under grant number DE-SC0021643.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Online data-enabled predictive control

We develop an online data-enabled predictive (ODeePC) control method for optimal control of unknown systems, building on the recently proposed DeePC (Coulson et al., 2019). Our proposed ODeePC method leverages a primal-dual algorithm with real-time measurement feedback to iteratively compute the corresponding real-time optimal control policy as system conditions change. The proposed ODeePC conceptual-wise resembles standard adaptive system identification and model predictive control (MPC), but it provides a new alternative for the standard methods. ODeePC is enabled by computationally efficient methods that exploit the special structure of the Hankel matrices in the context of DeePC with Fast Fourier Transform (FFT) and primal-dual algorithm We provide theoretical guarantees regarding the asymptotic behavior of ODeePC, and we demonstrate its performance through numerical examples.

97 MATHEMATICS AND COMPUTING↗

Path-Integrated Stereo X-Ray Digital Image Correlation: Resolving the Violation of Conservation of Intensity

In this study, x-ray imaging addresses many challenges with visible light imaging in extreme environments, where optical diagnostics such as digital image correlation (DIC) and particle image velocimetry (PIV) suffer biases from index of refraction changes and/or cannot penetrate visibly occluded objects. However, conservation of intensity—the fundamental principle of optical image correlation algorithms—may be violated if ancillary components in the X-ray path besides the surface or fluid of interest move during the test. The test series treated in this work sought to characterize the safe use of fiber-epoxy composites in aerospace and aviation industries during fire accident scenarios. Stereo X-ray DIC was employed to measure test unit deformation in an extreme thermal environment involving a visibly occluded test unit, incident surface heating to temperatures above 600°C, and flames and soot from combusting epoxy decomposition gasses. The objective of the current work is to evaluate two solutions to resolve the violation of conservation of intensity that resulted from both the test unit and the thermal chamber deforming during the test. The first solution recovered conservation of intensity by pre-processing the path-integrated X-ray images to isolate the DIC pattern of the test unit from the thermal chamber components. These images were then correlated with standard, optical DIC software. The second solution, called Path-Integrated Digital Image Correlation (PI-DIC), modified the fundamental matching criterion of DIC to account for multiple, independently-moving components contributing to the final image intensity. The PI-DIC algorithm was extended from a 2D framework to a stereo framework and implemented in a custom DIC software. Both solutions accurately measured the cylindrical shape of the undeformed test unit, recovering radii values of R = 76.20±0.12 mm compared to the theoretical radius of R theor = 76.20 mm. During the test, the test unit bulged asymmetrically as decomposition gasses pressurized the interior and eventually burned in a localized jet. Both solutions measured the heterogeneous radius of this bulge, which reached a maximum of approximately R = 91 mm, with a discrepancy of 2–3% between the two solutions. Two solutions that resolve the violation of conservation of intensity for path-integrated X-ray images were developed. Both were successfully employed in a stereo X-ray DIC configuration to measure deformation of an aluminum-skinned, fiber-epoxy composite test unit in a fire accident scenario.

47 OTHER INSTRUMENTATION↗

A Fundamentally New Coupled Approach to Contact Mechanics via the Dirichlet‐Neumann Schwarz Alternating Method

Contact phenomena are crucial for understanding the behavior of mechanical systems. However, existing computational approaches for simulating mechanical contact often face numerical challenges, such as inaccurate physical predictions, energy conservation errors, and unwanted oscillations. Here, we introduce an alternative technique for simulating dynamic contact based on the non‐overlapping Schwarz alternating method, originally developed for domain decomposition. In multibody contact scenarios, this method treats each body as a separate, non‐overlapping domain and prevents interpenetration using an alternating Dirichlet–Neumann iterative process. This approach has a strong theoretical foundation, eliminates the need for contact constraints, and offers flexibility, making it ideal for multiscale and multiphysics applications. We conducted a numerical comparison between the Schwarz method and traditional methods, such as the Lagrange multiplier and penalty methods, focusing on a benchmark impact problem. Our results indicate that the Schwarz alternating method outperforms traditional methods in several key areas: it provides more accurate predictions for various measurable quantities and demonstrates exceptional energy conservation capabilities. To address unwanted oscillations in contact velocities and forces, we explored various algorithms and stabilization techniques, ultimately opting for the naïve‐stabilized Newmark scheme for its simplicity and effectiveness. Additionally, we validated the efficiency of the Schwarz method in a three‐dimensional impact problem, highlighting its inherent capacity to accommodate different mesh topologies, time‐integration schemes, and time steps for each interacting body.

Schwarz alternating method↗

Modeling noise in global Mølmer-Sørensen interactions applied to quantum approximate optimization

Many-qubit Mølmer-Sørensen (MS) interactions applied to trapped ions offer unique capabilities for quantum information processing, with applications including quantum simulation and the quantum approximate optimization algorithm (QAOA). Here, we develop a physical model to describe many-qubit MS interactions under four sources of experimental noise: vibrational mode frequency fluctuations, laser power fluctuations, thermal initial vibrational states, and state preparation and measurement errors. The model parametrizes these errors from simple experimental measurements, without free parameters. Herein, we validate the model in comparison with experiments that implement sequences of MS interactions on two 171 Yb + ions. The model shows reasonable agreement after several MS interactions as quantified by the reduced chi-squared statistic $χ^{2}_{red}$≈2. As an application we examine MaxCut QAOA experiments on three and six ions. The experimental performance is quantified by approximation ratios that are 91% and 83% of the optimal theoretical values. Our model predicts $0.93^{+0.03}_{-0.02}$ and $0.95^{+0.04}_{-0.03}$, respectively, with disagreement in the latter value attributable to secondary noise sources beyond those considered in our analysis. With realistic experimental improvements to reduce measurement error and radial trap frequency variations, the model achieves approximation ratios that are 99% of the optimal. Incorporating these improvements into future experiments is expected to reveal new aspects of noise for future modeling and experimental improvements.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗