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At least 37 records · Page 2

Hydrodynamic instabilities and heat transfer characteristics in the duct flow of a fluid in the supercritical thermodynamic regime

The behavior of fluids at supercritical thermodynamic conditions is inherently complex due to large variations in thermodynamic and transport properties. Recent numerical and experimental investigations illustrate ongoing interest for these fluids, especially supercritical CO 2 and supercritical water, for a variety of applications. For example, supercritical water reactors (SCWR) operate in this extreme condition of high-pressure and temperature, resulting in highly dynamic flow fields and unexpected heat transfer regimes. The potential heat transfer benefits in this regime are directly associated with the extreme variations in thermodynamic and transport properties, which occur at, and above, the critical point. This work characterizes the hydrodynamic instabilities that arise for fluids at supercritical thermodynamic conditions when buoyancy forces are significant. Two specific configurations are considered, a natural convection cavity flow, and a mixed convection, heated, horizontal channel flow. Natural convection flow in a cavity is a classical configuration with expected behavior below the critical point. This configuration aids in characterizing the effect of the variable properties in the supercritical thermodynamic regime. Further, limited studies in the existing literature have been conducted for low-Reynolds and intermediate-Rayleigh numbers, mixed-convection channel flows for supercritical water, which is the focus of the channel flow configuration. To investigate the thermally driven hydrodynamic instabilities in this regime, a high-order fully-implicit numerical method is used. Such strong variations in thermophysical properties (in particular, density) are difficult to simulate and an altogether compressible framework is needed. Therefore, the compressible Navier-Stokes equations are solved without any additional assumptions. The fully implicit, high-order in space and time, reconstructed discontinuous Galerkin method as implemented within the multi-physics code called ALE3D (Arbitrary Lagrangian and Eulerian in 2D and 3D), developed at Lawrence Livermore National Laboratory (LLNL), is used. This fully implicit, L-stable method accurately captures the compressible nature of the ow in the limit of very low Mach number. It has been widely accepted that above the critical point, only one phase is observed. However, recent research has indicated the existence of the distinct gas-like and liquid-like regions separated by the Widom line, the locus of the maxima of the specific heat. Along the Widom line, density decreases 6-fold, viscosity drops by a factor of 2, while specific heat spikes by an order of magnitude. These variations, specifically in density and viscosity, produce a thick pseudo-interface and flow dynamics behavior akin to film boiling. A pseudo-film at the heated wall of the cavity and the horizontal channel is observed where buoyancy forces induce mixing through the specific configurations. Further the local Rayleigh and Richardson numbers provide maps of the flow field and the buoyancy forces driving the microscopic mixing. In the first chapter, I describe a background of supercritical fluid and the various applications. The second chapter focuses on the mathematical model and numerical method used for simulations, where a description of the equation of state for supercritical water is described. The third chapter focuses on the natural convection cavity with a heated bottom wall. In this cavity a gas-like and a liquid-like flow within the supercritical thermodynamic regime are observed. The fourth chapter focuses on a forced convection, horizontal channel, distinguishing between the gas-like, liquid-like, and mixed flow regimes. Mixed convection flow, with the addition of gravitational forces in the horizontal channel show the influence of variable properties on the hydrodynamic development, heat transfer, and rising instabilities. The last chapter of this research focuses on characterizing the unstable hydrodynamics through time-averaging processes and analysis of the movement of energy through the developing plumes.

42 ENGINEERING↗

Condensed Phase Water Molecular Multipole Moments from Deep Neural Network Models Trained on Ab Initio Simulation Data

Ionic solvation phenomena in liquids involve intense interactions in the inner solvation shell. For interactions beyond the first shell, the ion–solvent interaction energies result from the sum of many smaller-magnitude contributions that can still include polarization effects. Deep neural network (DNN) methods have recently found wide application in developing efficient molecular models that maintain near-quantum accuracy. In this work, we extend the DeePMD-kit code to produce accurate molecular multipole moments in the bulk and near interfaces. The new method is validated by comparing the DNN moments with those generated by ab initio simulations. The moments are used to compute the electrostatic potential at the center of a molecular-sized hydrophobic cavity in water. The results show that the fields produced by the DNN models are in quantitative agreement with the AIMD-derived values. These efficient methods will open the door to more accurate solvation models for large solutes such as proteins.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stochastic equilibrium Raman spectroscopy (STERS)

In this manuscript, we propose a new method for cavity- and surface-enhanced Raman spectroscopy (SERS) with improved temporal resolution in the measurement of stochastic Raman spectral fluctuations. Our approach combines Fourier spectroscopy and photon correlation to decouple the integration time from the temporal resolution. Using statistical optics Monte Carlo simulations, we establish the relationship between time resolution and Raman signal strength, revealing that typical Raman spectral fluctuations, commensurate with molecular conformational dynamics, can theoretically be resolved on micro- to millisecond timescales. The method can further extract average single-molecule dynamics from small sub-ensembles, thereby potentially mitigating challenges in achieving strictly single-molecule isolation on SERS substrates.

Cobb-Bruno, Colburn [University of California, Ber↗

Spray Mechanism of Contained-Electrospray Ionization

Analytical characteristics of contained electrospray ionization (ESI) are summarized in terms of its potential to modify the analyte solution during the stages of droplet formation to provide opportunities to generate native versus denatured biomolecular gas-phase ions, without the need for bulk-phase analyte modifications. The real-time modification of the charged microdroplets occurs in a cavity that is included in the outlet of the contained-ESI ion source. Close examination of the inside of the cavity using a high-speed camera revealed the formation of discrete droplets as well as thin liquid films in the droplets wake. When operated at 20 psi N2 pressure, the droplets were observed to move at an average speed of 8 mm/s providing ~1 s mixing time in a 10 mm cavity length. Evidence is provided for the presence of highly reactive charged droplets based on myoglobin charge state distribution, apo-myoglobin contents, and ion mobility drift time profiles under different spray conditions. Mechanistic insights for the capture of vapor-phase reagents and droplet dynamics as influenced by different operational modes are also described.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Case studies of the time-dependent potential energy surface for dynamics in cavities

Here, the exact time-dependent potential energy surface driving the nuclear dynamics was recently shown to be a useful tool to understand and interpret the coupling of nuclei, electrons, and photons in cavity settings. Here, we provide a detailed analysis of its structure for exactly solvable systems that model two phenomena: cavity-induced suppression of proton-coupled electron-transfer and its dependence on the initial state, and cavity-induced electronic excitation. We demonstrate the inadequacy of simply using a weighted average of polaritonic surfaces to determine the dynamics. Such a weighted average misses a crucial term that redistributes energy between the nuclear and the polaritonic systems, and this term can in fact become a predominant term in determining the nuclear dynamics when several polaritonic surfaces are involved. Evolving an ensemble of classical trajectories on the exact potential energy surface reproduces the nuclear wavepacket quite accurately, while evolving on the weighted polaritonic surface fails after a short period of time. The implications and prospects for application of mixed quantum-classical methods based on this surface are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Improved natural convection heat transfer correlations for reactor cavity cooling systems of high-temperature gas-cooled reactors: From computational fluid dynamics to Pronghorn

The Reactor Cavity Cooling System (RCCS) is a common reactor safety system in High Temperature Gas Cooled Reactors (HTGR) that removes heat from the Reactor Pressure Vessel (RPV) by radiation ($\sim 80\%$) and natural convection ($\sim 20\%$). For simulation of accident scenarios of HTGRs, intermediate fidelity and system codes models must be employed for limiting the models' execution time. While accurate quantification of the radiative heat transfer is available in these models, quantification of natural convection must rely on correlations of questionable accuracy for the Nusselt number. Commonly used correlations are based in experiments performed at low Rayleigh numbers and/or using isothermal walls in simplified geometries. Here, this work improves on the accuracy of natural convection heat transfer correlations in support for HTGR designs. These correlations include both local and average Nusselt numbers as a function of the global Rayleigh number, the local Rayleigh number, and the temperature profile at the hot wall of the RCCS. In the absence of dedicated experiments and the difficulty of performing high-fidelity simulations at realistic Rayleigh numbers, the data to fit the correlations are generated with Computational Fluid Dynamics (CFD) using Reynolds Averaged Navier-Stokes (RANS) models. First, a careful selection of the RANS turbulence model is performed by comparing the results obtained with different RANS turbulence models against high fidelity simulations of natural convection at $Ra \ 1 \times 10^{11}$ in a rectangular cavity. Next, the selected model is used to perform simulations of an HTGR cavity at different high Rayleigh numbers $\in [6.1 \times 10^{11},2.9 \times 10^{13}]$ to encompass several HTGR designs, assuming an isothermal RPV wall. The results obtained are used to fit a correlation for the average and space-varying Nusselt number as a function of the global and local Rayleigh numbers via a sparsity-promoting least-squares method. The selected RANS model is then used to perform simulations of a PBMR 400 HTGR cavity with the temperature profiles at the RPV wall obtained during a PLOFC transient. We use the results obtained to fit a temperature-dependent correction to the space-varying Nusselt number with the sparsity-promoting least-squares method. The results obtained in this work, enable system-level codes, such as Pronghorn, to perform higher-fidelity simulations of the heat exchange process in the RCCS while still maintaining a low computational cost.

42 ENGINEERING↗

Imposing strong correlated energy spread on relativistic bunches with transverse deflecting cavities

We demonstrate a novel scheme for imposing or removing large energy chirp on relativistic electron bunches. This method relies on the transverse-to-longitudinal mixing accomplished with a set of transverse deflecting cavities. The working principles of the new concept are explained using the first-order matrix formalism in the approximation of the linear single-particle dynamics. The scheme demonstrates versatility regarding the average beam energy and, hence, positioning along the accelerator beam line. The performance of the scheme is numerically investigated with the elegant particle-tracking code. It is shown that the associated nonlinear effects causing emittance deterioration for the extreme quantities of the total energy spread can be effectively compensated by optimization of the Twiss parameters while relying on the eigenemittance analysis. The impact of the longitudinal space charge effects on the beam dynamics in the proposed scheme is also investigated.

43 PARTICLE ACCELERATORS↗

Structure and dynamics of hydrodynamically interacting finite-size Brownian particles in a spherical cavity: Spheres and cylinders

The structure and dynamics of confined suspensions of particles of arbitrary shape are of interest in multiple disciplines from biology to engineering. Theoretical studies are often limited by the complexity of long-range particle-particle and particle-wall forces, including many-body fluctuating hydrodynamic interactions. Here, we report a computational study on the diffusion of spherical and cylindrical particles confined in a spherical cavity. We rely on an immersed-boundary general geometry Ewald-like method to capture lubrication and long-range hydrodynamics and include appropriate non-slip conditions at the confining walls. A Chebyshev polynomial approximation is used to satisfy the fluctuation-dissipation theorem for the Brownian suspension. We explore how lubrication, long-range hydrodynamics, particle volume fraction, and shape affect the equilibrium structure and the diffusion of the particles. It is found that once the particle volume fraction is greater than 10%, the particles start to form layered aggregates that greatly influence particle dynamics. Hydrodynamic interactions strongly influence the particle diffusion by inducing spatially dependent short-time diffusion coefficients, stronger wall effects on the particle diffusion toward the walls, and a sub-diffusive regime-caused by crowding-in the long-time particle mobility. The level of asymmetry of the cylindrical particles considered here is enough to induce an orientational order in the layered structure, decreasing the diffusion rate and facilitating a transition to the crowded mobility regime at low particle concentrations. Our results offer fundamental insights into the diffusion and distribution of globular and fibrillar proteins inside cells.

36 MATERIALS SCIENCE↗

Probing Non-Equilibrium Pair-Breaking and Quasiparticle Dynamics in Nb Superconducting Resonators Under Magnetic Fields

We conducted a comprehensive study of the non-equilibrium dynamics of Cooper pair breaking, quasiparticle (QP) generation, and relaxation in niobium (Nb) cut from superconducting radio-frequency (SRF) cavities, as well as various Nb resonator films from transmon qubits. Using ultrafast pump–probe spectroscopy, we were able to isolate the superconducting coherence and pair-breaking responses. Our results reveal both similarities and notable differences in the temperature- and magnetic-field-dependent dynamics of the SRF cavity and thin-film resonator samples. Moreover, femtosecond-resolved QP generation and relaxation under an applied magnetic field reveals a clear correlation between non-equilibrium QPs and the quality factor of resonators fabricated by using different deposition methods, such as DC sputtering and high-power impulse magnetron sputtering. These findings highlight the pivotal influence of fabrication techniques on the coherence and performance of Nb-based quantum devices, which are vital for applications in superconducting qubits and high-energy superconducting radio-frequency applications.

43 PARTICLE ACCELERATORS↗

Probing the ultrafast gain and refractive index dynamics of a VECSEL

Typically, strong gain saturation and gain dynamics play a crucial role in semiconductor laser mode-locking. While there have been several investigations of the ultrafast gain dynamics in vertical-external-cavity surface-emitting lasers (VECSELs), little is known about the associated refractive index changes. Yet, such refractive index changes do not only have a profound impact on the pulse formation process leading to self-phase modulation, which needs to be compensated by dispersion, but they are also of particular relevance for assessing the feasibility of Kerr-lens mode-locking of VECSELs. Here, we measure both refractive index as well as gain dynamics of a VECSEL chip using the ultrafast beam deflection method. We find that, in contrast to the gain dynamics, the refractive index dynamics is dominated by an instantaneous (100 fs) and a very slow component (100 ps). The time-resolved measurement of nonlinear refraction allows us to predict a pulse-length dependent, effective nonlinear refractive index n 2,eff , which is shown to be negative and on the order of 10 -16 m 2 =W for short pulse lengths (100 fs). It becomes positive for large excitation fluences and large pulse lengths (few ps). These results agree with some previous reports of self-mode-locked VECSELs for which the cavity design and pulse properties determine sign and strength of the nonlinear refractive index when assuming Kerr-lens mode-locking.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Fluid-driven fractures in granular media: Insights from numerical investigations

We investigate the mechanisms of opening-mode fracture initiation in granular media. The study is based on a simulation of grain-scale fluid-grain interactions through a coupled numerical approach in which the discrete element method is used to solve for the mechanics of a solid granular medium, and computational fluid dynamics is used to model fluid flow and drag forces. In this work, we present benchmark problems with analytical solutions and validate this numerical model against experiments on a viscous-drag-driven cavity in the literature. Additional simulation results show fracture initiation mechanisms in a random granular packing subjected to constant boundary stresses and to fluid injection with a localized source. The dimensionless variable $F_s/F_{sk}$ (ratio of seepage force $F_s$ and skeletal force $F_{sk}$) incorporates the impacts of physical properties and injection parameters including fluid viscosity, injection velocity, grain size, and effective stresses, and it has been used as a criterion separating regimes of fluid invasion and drag-driven fracture opening. Our simulation results show that $F_s/F_{sk}$ in combination with $τ_1$ (ratio of diffusion time from hydromechanical coupling and injection time) serves as a prediction of fracture opening within granular packing. We suggest a simple criterion ($F_s/F_{sk}$ > 1 or $τ_1$ > 0.17) that is valid for various types of granular media and injection conditions to determine if fracture opening will occur. Among other applications, this study is useful to predict the initiation and propagation of fractures in natural sediments.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Adaptive machine learning for time-varying systems: low dimensional latent space tuning

Machine learning (ML) tools such as encoder-decoder convolutional neural networks (CNN) can represent incredibly complex nonlinear functions which map between combinations of images and scalars. For example, CNNs can be used to map combinations of accelerator parameters and images which are 2D projections of the 6D phase space distributions of charged particle beams as they are transported between various particle accelerator locations. Despite their strengths, applying ML to time-varying systems, or systems with shifting distributions, is an open problem, especially for large systems for which collecting new data for re-training is impractical or interrupts operations. Particle accelerators are one example of large time-varying systems for which collecting detailed training data requires lengthy dedicated beam measurements which may no longer be available during regular operations. We present a novel method of adaptive ML for time-varying systems. Our approach is to map very high (N ≈ 100k) dimensional inputs (a combination of scalar parameters and images) into the low dimensional (N ≈ 2) latent space at the output of the encoder section of an encoder-decoder CNN. We then actively tune the low dimensional latent space-based representation of complex system dynamics by the addition of an adaptively tuned feedback vector directly before the decoder sections builds back up to our image-based high-dimensional phase space density representations. This method allows us to learn correlations within and to quickly tune the characteristics of incredibly large parameter space systems and to track their evolution in real time based on feedback without massive new data sets for re-training. We demonstrate that our method can accurately predict and track the phase space of charged particle beams at various locations in a particle accelerator by adaptively adjusting in real-time while the unknown input beam distribution of the accelerator is changing in shape, charge, and offset and while the RF system of the accelerator itself is also changing in an unpredictable way. For FACET-II we demonstrate that such an approach has the potential to use transverse deflecting cavity and energy spread spectrum beam measurements to accurately predict 2D projections of the 6D phase space of the electron beam at the plasma wakefield acceleration interaction point where such diagnostics are unavailable.

47 OTHER INSTRUMENTATION↗

Realistic simulations of spin squeezing and cooperative coupling effects in large ensembles of interacting two-level systems

We describe an efficient numerical method for simulating the dynamics of interacting spin ensembles in the presence of dephasing and decay. The method builds on the discrete truncated Wigner approximation for isolated systems, which combines the mean-field dynamics of a spin ensemble with a Monte Carlo sampling of discrete initial spin values to account for quantum correlations. Here we show how this approach can be generalized for dissipative spin systems by replacing the deterministic mean-field evolution by a stochastic process, which describes the decay of coherences and populations while preserving the length of each spin. We demonstrate the application of this technique for simulating nonclassical spin-squeezing effects or the dynamics and steady states of cavity QED models with 10 5 interacting two-level systems. This opens up the possibility to perform accurate real-scale simulations of a diverse range of experiments in quantum optics or with solid-state spin ensembles under realistic laboratory conditions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Machine Learning for Anomaly Detection in Neural Network Security and SRF Cavities

This dissertation explores the development and deployment of machine learning approaches to address critical challenges in anomaly detection across two distinct domains: neural network security in federated learning settings and cavity behavior analysis in particle accelerator operations at Jefferson Lab in Newport News, Virginia. Anomaly detection identifies deviations from expected patterns, safeguarding systems in cybersecurity, industry, and research against malicious activities and failures. This dissertation demonstrates how our machine learning approaches enhance detection accuracy and efficiency in both neural network security and industrial applications. First, we investigate vulnerabilities in deep neural networks deployed in federated learning. Although federated learning preserves user privacy by training models locally, it remains vulnerable to backdoor attacks, in which malicious participants embed hidden triggers that induce targeted misbehavior. We propose a self-supervised contrastive learning framework to detect and mitigate such backdoor attacks. In our experiments, this method achieves higher detection accuracy and lower false positive rates than existing defenses, while operating without access to local model updates or original training data and thus preserving the privacy guarantees of the federated setting. Second, we address the operational reliability of superconducting radio-frequency (SRF) cavities at the Continuous Electron Beam Accelerator Facility (CEBAF). Our research leverages an unsupervised learning approach, combined with Principal Component Analysis (PCA) and k-means clustering, to identify anomalous behaviors in SRF cavities. Our method detects subtle anomalous behavior by analyzing SRF signal data. This knowledge allows for the early detection and resolution of potential faults, significantly improving the efficiency and reliability of operations. Third, we extend these insights to time-series anomaly detection more broadly. We design a contrastive-learning based model tailored to increasingly dynamic environments and academic research. This model improves detection accuracy in settings that require real-time monitoring and predictive maintenance. Our research underscores the broader applicability and impact of advanced machine learning techniques in anomaly detection. By extracting meaningful patterns from complex data, machine learning can significantly enhance security in distributed neural networks and improve the efficiency of particle accelerator operations. This dissertation serves as a stepping stone for future investigations into the vast possibilities of anomaly detection, inspiring further exploration and development of machine learning techniques in this field.

Ferguson, Hal [Old Dominion University]↗

Polariton Control of Molecular Charge Transfer in Perylene Diimide Semiconductors

We report the modulation of molecular charge transfer in a bay-substituted perylene diimide derivative embedded in a planar distributed Bragg reflector microcavity. Angle-resolved reflectance spectra confirm the formation of upper and lower polaritons with clear Rabi splitting, indicating strong coupling between the cavity mode and molecular excitons. Using broadband transient absorption spectroscopy, we compare the ultrafast dynamics of cavity and non-cavity films. While excited-state absorption and stimulated emission pathways remain largely unchanged, kinetic modeling reveals a moderate increase in the charge transfer rate and yield under strong coupling. This enhancement is attributed to a reduction in the effective driving force via the formation of the lower polariton, placing the system deeper into the Marcus inverted regime. Our results demonstrate a promising non-chemical method leveraging cavity quantum electrodynamics to modulate charge separation processes in molecular semiconductors.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Simulating and Optimizing Quantum State Transport

The goal of this project was to produce an accurate simulator of the “pitch and catch” process of sending quantum states between SRF cavities, and to find a method for optimizing the control pumps. We developed a program in C++ to integrate the equations of motion with high speed and precision, and used this as a basis for finding an optimal control function to maximize the state transfer efficiency. To demonstrate this we have shown an example of an optimal drive function and the resulting system dynamics, as well as a heat map of the cost function for a range of drive amplitudes.

Weston, Jacob↗

Extremum seeking for optimal control problems with unknown time-varying systems and unknown objective functions

We consider the problem of optimal feedback control of an unknown, noisy, time-varying, dynamic system that is initialized repeatedly. Examples include a robotic manipulator which must perform the same motion, such as assisting a human, repeatedly and accelerating cavities in particle accelerators which are turned on for a fraction of a second with given initial conditions and vary slowly due to temperature fluctuations. In this paper, we present an approach that applies to systems of practical interest. The method presented here is model independent; does not require knowledge of the objective function; is robust to measurement noise; is applicable for any set of initial conditions; is applicable to simultaneously controlling an arbitrary number of parameters; and may be implemented with a broad range of continuous or discontinuous functions such as sine or square waves. For systems with convex cost functions we prove that our algorithm will produce controllers that approach the minimal cost. For linear systems we reproduce the cost minimizing linear quadratic regulator optimal controller that could have been designed analytically had the system and cost function been known. We demonstrate the effectiveness of the algorithm with simulation studies of noisy and time-varying systems.

42 ENGINEERING↗

Summary Report Of The FY25 Computational Fluid Dynamics Verification And Validation Exercises In The Advanced Reactor Technologies - Gas-cooled Reactor Program

Verification and Validation (V&V) of numerical tools is critical for ensuring reasonable predictions during design, safety analysis, and licensing. Recent work in the Advanced Reactor Technologies - Gas-cooled Reactor (ART-GCR) program has focused on V&V of common Computational Fluid Dynamics (CFD) tools that are used within the Untied States. This report presents an update on these CFD V&V activities. These Generation IV Forum (GIF) Very High Temperature Reactor (VHTR) Computational Methods, Validation, and Benchmarking (CMVB) is an international organization dedicated to the verification and validation of High Temperature Gas-Cooled Reactor (HTGR) simulation tools. Participation in the CMVB provides additional value to the V&V activities, as it allows for access to a wider range of data, and provides valuable benchmarking exercises. Three HTGR phenomena are targeted: Reactor Cavity Cooling System (RCCS) performance, core bypass flow, and lower plenum mixing. Simulations of the University of Wisconsin-Madison (UW-Madison) RCCS facilities are performed with Reynolds Averaged Navier-Stokes (RANS) in StarCCM+. Results are compared for both forced and natural convection conditions, with both exhibiting good agreement with experimental measurements. The Idaho National Laboratory (INL) matched index of refraction (MIR) and Korean Atomic Energy Research Institute (KAERI) bypass flow expeirments are used to validation CFD predictions of bypass flow. Simulations are performed with RANS in StarCCM+ and with Large Eddy Simulation (LES) in NekRS. Finally, preliminary simulations of the Institute of Nuclear and New Energy Technology (INET) lower plenum mixing facilities are presented. Initial work has developed models with LES, RANS, and porous media models. These preliminary models are presented and compared to each other to gauge differences in predictions with each of the three methods.

and Benchmarking (CMVB)↗