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At least 361 records · Page 20

Non-autoregressive time-series methods for stable parametric reduced-order models

Advection-dominated dynamical systems, characterized by partial differential equations, are found in applications ranging from weather forecasting to engineering design where accuracy and robustness are crucial. There has been significant interest in the use of techniques borrowed from machine learning to reduce the computational expense and/or improve the accuracy of predictions for these systems. These rely on the identification of a basis that reduces the dimensionality of the problem and the subsequent use of time series and sequential learning methods to forecast the evolution of the reduced state. Often, however, machine-learned predictions after reduced-basis projection are plagued by issues of stability stemming from incomplete capture of multiscale processes as well as due to error growth for long forecast durations. To address these issues, we have developed a non-autoregressive time series approach for predicting linear reduced-basis time histories of forward models. In particular, we demonstrate that non-autoregressive counterparts of sequential learning methods such as long short-term memory (LSTM) considerably improve the stability of machine-learned reduced-order models. Further, we evaluate our approach on the inviscid shallow water equations and show that a non-autoregressive variant of the standard LSTM approach that is bidirectional in the principal component directions obtains the best accuracy for recreating the nonlinear dynamics of partial observations. Moreover-and critical for many applications of these surrogates-inference times are reduced by three orders of magnitude using our approach, compared with both the equation-based Galerkin projection method and the standard LSTM approach.

97 MATHEMATICS AND COMPUTING↗

Protein Molecular Dynamics Simulations with Approximate QM: What Can We Learn?

Classical force fields are essential for computer simulations of proteins and are typically parameterized to reproduce secondary and tertiary structure of isolated proteins. However, while protein-protein interactions are ubiquitous in nature, they are not considered in parameterization efforts and are far less understood than isolated proteins. A better characterization of intermolecular interactions is widely recognized as a key to revolutionizing drug and therapeutic developments with high-throughput computational screening. Urgently needed is a critical assessment of the performance of modern protein force fields against first-principles electronic structure methods and experiments. In a daring step toward this goal, we here describe a comparison of peptide folding dynamics as predicted by a molecular mechanics force field on the one hand and by an approximate electronic structure quantum mechanical (QM) method based on density-functional tight-binding (DFTB) on the other. We further compare the dynamics from straightforward DFTB simulations with a near-linear scaling version of DFTB for massively parallel computation based on the fragment molecular orbital (FMO-DFTB) method. We illustrate differences between the phenomenology of the folding dynamics from these three methods for a small model peptide, as well as charge polarization and dynamic fluctuations, point out possible correlations and implications for force field developers, and discuss the lessons learned that might become applicable to future predictive high-throughput computer screening for personalized neoantigen cancer therapy.

Irle, Stephan↗

A Secure Learning Control Strategy via Dynamic Camouflaging for Unknown Dynamical Systems under Attacks

This paper presents a secure reinforcement learning (RL) based control method for unknown linear time-invariant cyber-physical systems (CPSs) that are subjected to compositional attacks such as eavesdropping and covert attack. We consider the attack scenario where the attacker learns about the dynamic model during the exploration phase of the learning conducted by the designer to learn a linear quadratic regulator (LQR), and thereafter, use such information to conduct a covert attack on the dynamic system, which we refer to as doubly learning-based control and attack (DLCA) framework. We propose a dynamic camouflaging based attack-resilient reinforcement learning (ARRL) algorithm which can learn the desired optimal controller for the dynamic system, and at the same time, can inject sufficient misinformation in the estimation of system dynamics by the attacker. The algorithm is accompanied by theoretical guarantees and extensive numerical experiments on a consensus multi-agent system and on a benchmark power grid model.

Mukherjee, Sayak↗

Dynamic Tensile Response of a Fe–49Co–2V Alloy at Various Strain Rates and Temperatures

Soft ferromagnetic alloys are often utilized in electromagnetic applications due to their desirable magnetic properties. In support of these applications, the ferromagnetic alloys are also required to bear mechanical load under various loading and environmental conditions. In this study, a Fe–49Co–2V alloy was dynamically characterized in tension with a Kolsky tension bar and a Drop–Hopkinson bar at various strain rates and temperatures. Dynamic tensile stress–strain curves of the Fe–49Co–2V alloy were obtained at strain rates ranging from 40 to 230 s -1 and temperatures from - 100 to 100 °C. All dynamic tensile stress–strain curves exhibited an initial linear elastic response to an upper yield followed by Lüders band response and then a nearly linear work-hardening behavior. The yield strength of this material was found to be sensitive to both strain rate and temperature, whereas the hardening rate was independent of strain rate or temperature. The Fe–49Co–2V alloy exhibited a feature of brittle fracture in tension under dynamic loading with no necking being observed.

36 MATERIALS SCIENCE↗

Midfidelity model verification for a point-absorbing wave energy converter with linear power take-off

In the preliminary design stage of a wave energy converter (WEC), researchers need fast and reliable simulation tools. High-fidelity numerical models are usually employed to study the wave-structure interaction, but the computational cost is demanding. As an alternative, midfidelity models can provide simulations in the order of real time. In this study, we operate Uppsala University’s WEC in a relatively mild sea state and model it using WEC-Sim. The model is verified based on OpenFOAM simulations. To analyze the ability of the midfidelity model to capture WEC dynamics, we investigate the system separately with 1, 2, and 3 degrees of freedom. We examine the contribution of viscous phenomena, and study both linear and weakly nonlinear solutions provided by WEC-Sim. Our results indicate that the viscous effects can be neglected in heave and surge motion, but not for pitch. We also find that the weakly nonlinear WEC-Sim solution successfully agrees with the computational fluid dynamics, whereas the linear solution could suggest misleading results.

16 TIDAL AND WAVE POWER↗

Dynamical quantum phase transitions in interacting atomic interferometers

Particle-wave duality has allowed physicists to establish atomic interferometers as celebrated complements to their optical counterparts in a broad range of quantum devices. In particular, interactions give rise to multiparticle correlations unavailable in linear interferometers. Here, we show that interactions lead to dynamical quantum phase transitions (DQPTs) between NOON states in an atomic interferometer. These transition points result from zeros of the Loschmidt echo, which approach the real axis of the complex time plane in the large-particle-number limit, and signify pair condensates, another type of exotic quantum states featured with prevailing two-body correlations. Such DQPTs thus provide us with a new angle to understand many-body states emergent from quantum nonequilibrium dynamics. Further, our work also suggests interacting atomic interferometers as a new tool for creating highly entangled states to beat the standard quantum limit.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Dynamics of McMillan mappings I. McMillan multipoles

In this article, we consider two dynamical systems: the McMillan sextupole and octupole integrable mappings, originally proposed by Edwin McMillan. Both represent the simplest symmetric McMillan maps, characterized by a single intrinsic parameter. While these systems find numerous applications across various domains of mathematics and physics, some of their dynamical properties remain unexplored. We aim to bridge this gap by providing a comprehensive description of all stable trajectories, including the parametrization of invariant curves, Poincaré rotation numbers, and canonical action–angle variables. In the second part, we establish connections between these maps and general chaotic maps in standard form. Our investigation reveals that the McMillan sextupole and octupole serve as first-order approximations of the dynamics around the fixed point, akin to the linear map and quadratic invariant (known as the Courant–Snyder invariant in accelerator physics), which represents zeroth-order approximations (referred to as linearization). Furthermore, we propose a novel formalism for nonlinear Twiss parameters, which accounts for the dependence of rotation number on amplitude. This stands in contrast to conventional betatron phase advance used in accelerator physics, which remains independent of amplitude. Notably, in the context of accelerator physics, this new formalism demonstrates its capability in predicting dynamical aperture around low-order resonances for flat beams, a critical aspect in beam injection/extraction scenarios.

43 PARTICLE ACCELERATORS↗

A Framework for Closed-Loop Optimization of an Automated Mechanical Serial-Sectioning System via Run-to-Run Control as Applied to a Robo-Met.3D

Optimization of automated data collection is gaining increased interest for the purposes of enabling closed-loop self-correcting systems that inherently maximize operational efficiencies and reduce waste. Many data collection systems have several variables which influence data accuracy or consistency and which can require frequent user interaction to be monitored and maintained. Operating upon a Robo-MET.3D™ automated mechanical serial-sectioning system, a run-to-run control algorithm has been developed to accelerate data collection and reduce data inconsistency. Here, using historical data amassed over a decade of experiments, a linear regression model of the deterministic system dynamics is created and used to employ a run-to-run control algorithm that optimizes selected system inputs to reduce operator intervention and increase efficacy while reducing variance of system output.

42 ENGINEERING↗

Extrapolation of thermal conductivity in non-equilibrium molecular dynamics simulations to bulk scale

Predictions of the bulk scale thermal conductivity of solids using non-equilibrium molecular dynamics (MD) simulations have relied on the linear extrapolation of the thermal resistivity versus the reciprocal of the system length in the simulations. Several studies have reported deviation of the extrapolation from linearity near the micro-scale, raising a concern of its applicability to large systems. To investigate this issue, present work conducted extensive MD simulations of silicon with two different potentials (EDIP and Tersoff-II) for unprecedented length scales up to 10.3 μm and simulation times up to 530 ns. For large systems ≥0.35 μm in size the non-linearity of the extrapolation of the reciprocal of the thermal conductivity is mostly due to ignoring the dependence of the thermal conductivity on temperature. To account for such dependence, the present analysis fixes the temperature range for determining the gradient for calculating the thermal conductivity values. However, short systems ≤0.23 μm in size show significant non-linearity in the calculated thermal conductivity values using a temperature window of 500 ± 10 K from the simulations results with the EDIP potential. Since these system sizes are shorter than the mean phonon free path in EDIP (~0.22 μm), the nonlinearity may be attributed to phonon transport. For the MD simulations with the Tersoff-II potential there is no significant non-linearity in the calculated thermal conductivity values for systems ranging in size from 0.05 to 5.4 μm.

42 ENGINEERING↗

A heat flux sensor leveraging the transverse Seebeck effect in elemental antimony

Certain configurations of anisotropic single crystal materials can generate a thermoelectric voltage orthogonal to an induced temperature gradient. This phenomenon is known as the Transverse Seebeck Effect (TSE) and can be leveraged to fabricate simple and robust heat flux sensors. Only a small number of materials have been considered as TSE-based transducers and, among these, few have been developed into sensors with ruggedization against chemical and mechanical degradation. Here, we report on the fabrication and characterization of a rugged TSE-based heat flux sensor using prismatic antimony single crystals. The heat flux sensor was tested under static and dynamic heating scenarios. The sensor has a linear responsivity of 16.8 µV/(W/cm2) to heat fluxes spanning more than two orders of magnitude and a time constant of 4.4 s. The sensor’s response to localized heating, probed with a laser scanning technique, validated that the transduction mechanism is primarily the TSE by ruling out a sizable contribution from the conventional Seebeck effect. Finite element analysis corroborated that components used in the sensor package are the primary determinants of the time constant and the decrement of the responsivity from its theoretical maximum. Design principles that may be applied to elicit a faster transient response or higher responsivity are proposed. Furthermore, the results establish single crystal antimony as a promising transducer material for heat flux measurement systems and demonstrate potential effects of ruggedization on sensor performance.

36 MATERIALS SCIENCE↗

Destabilization of binary mixing layer in supercritical conditions

Compressible mixing layer instabilities are of importance to a wide range of environmental and industrial applications. Past studies have focused on either ideal-gas or real-fluid thermodynamic regimes of single-species mixing layers. However, mixing layers of binary mixtures at supercritical conditions, commonly encountered in fuel injection systems, introduce additional complexities due to the added compositional degree-of-freedom. Moreover, the effect of strong variations in thermodynamic response functions across the Widom line on the binary mixing layer stability remains poorly understood. Thus, the objective of this study is to examine the coupling between the hydrodynamic instability and the real-fluid thermodynamics across the Widom line and its effects on the overall binary mixing layer dynamics. To this end, we develop a linear stability analysis of the full binary-species compressible transport equations coupled with the PC-SAFT equation of state. Analysis shows the existence of a novel instability mechanism that arises from juxtapositioning of the Widom-line transition and the hydrodynamic inflection point. This novel thermodynamically induced instability mechanism has the net effect of destabilizing the binary mixing layer at lowering supercritical conditions towards the critical pressure point. This is in contrast to previous stability analyses of supercritical single-species mixing layers, where increasing pressure destabilizes the flow due to its effect on reducing the density stratification. The discovered thermodynamically induced instability mechanism of binary mixing flows highlights the need for an extension of classical instability criteria to incorporate the effect of strong variations in the thermodynamic response functions across the Widom line on mixing layer instability.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Machine-Learned Force Field for Molecular Dynamics Simulations of Nonequilibrium Ammonia Synthesis on Iron Catalysts

Ammonia (NH 3 ) is one of the most important industrial chemicals. The conventional NH 3 synthesis method-the Haber–Bosch process-converts atmospheric nitrogen (N 2 ) into NH 3 using H 2 with an iron (Fe) catalyst. However, this process requires high pressures (100–200 atm) and temperatures (700–800 K) near thermal equilibrium. Recently, Fe-based nanocatalysts have been reported to produce promising NH 3 yields under atmospheric pressures and temperature-modulated nonequilibrium conditions. Understanding the mechanism of nonequilibrium catalysis with programmed temperature variation could help to optimize this fully electrified and less energy-intensive process. Although reactive molecular dynamics (RMD) simulations can be a useful tool to model nonequilibrium catalytic processes, they require the development of accurate force fields (i.e., interatomic potentials). Here, we present a machine-learned (ML) force field within the Deep Potential MD (DPMD) framework, trained using periodic density functional theory (DFT) calculations, to model NH 3 synthesis on Fe catalysts with various surface adsorbates such as *N, *H, *N 2 , *H 2 , *NH, *NH 2 , and *NH 3 . Here, we generated the DFT data from static models of elementary reactions on the most stable (110) surface of body-centered cubic Fe, which then were augmented by data from constant number of particles–volume–temperature (NVT) DFT-MD trajectories at various temperatures. Finally, we utilized the fully optimized ML force field to investigate reaction dynamics at an Fe(110) surface at linearly increasing temperatures using NVT-DPMD simulations. Our simulations indicate that pulsed temperature ramping could prove favorable for NH3 synthesis. For example, we conducted ramping under multiple sets of conditions: (i) from 900 to 1200 K over periods of 0.1–0.3 ns for Fe surfaces precovered with N or NH along with H; and (ii) from 300 to 600 K over 0.1–0.3 ns for Fe surfaces precovered with NH 3 . While our simulations so far are limited to short time scales (very rapid heating), these observations shed light on the mechanism of the high NH 3 synthesis rate achieved in a novel temperature-modulated nonequilibrium catalytic reactor using pulsed heating and cooling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Exact-Factorization-Based Surface Hopping without Velocity Adjustment

While surface hopping has emerged as a powerful method for simulating non-adiabatic dynamics in large molecules, the ad hoc nature of the necessary velocity adjustments and decoherence corrections in the algorithm somewhat reduces its reliability. Here we propose a new scheme that eliminates these aspects by combining the nuclear equation from the quantum-trajectory surface-hopping approach with the electronic equation derived from the exact-factorization approach. Furthermore, the resulting method, denoted QTSH-XF, yields a surface-hopping method on firmer ground than previous and is shown to successfully capture dynamics in Tully models and in a linear vibronic coupling model of the photoexcited uracil cation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dielectric-Engineered Monolayer MoS 2 Memtransistors for Brain-Inspired Computing with High Recognition Accuracy

Two-dimensional transition metal dichalcogenides (2D-TMDs)-based memtransistors have emerged as promising candidates for neuromorphic hardware due to their exceptional ability to emulate synaptic behavior. However, many existing 2D-TMDs memtransistors rely on polycrystalline channels with grain boundaries or defects introduced through postgrowth treatments, raising concerns about material integrity and the preservation of intrinsic properties. Here, in this work, we demonstrate a monocrystalline monolayer MoS 2 memtransistor fabricated on a silicon nitride (SiN X ) substrate, achieving a large resistive switching ratio of 10 4 , a dynamic range exceeding 90, along with highly linear and symmetric weight updates, minimal cycle-to-cycle variability, and low device-to-device variability. These attributes are critical for enabling high-performance neuromorphic hardware. Based on experimental data, we further show that these artificial synapses enable a recognition accuracy of more than 97% on the MNIST handwritten digits data set. Our findings present a straightforward approach to realizing 2D-TMDs memtransistors through dielectric engineering, offering a promising platform for next-generation neuromorphic computing systems.

2D TMDs↗

Viscosity in water from first-principles and deep-neural-network simulations

Abstract We report on an extensive study of the viscosity of liquid water at near-ambient conditions, performed within the Green-Kubo theory of linear response and equilibrium ab initio molecular dynamics (AIMD), based on density-functional theory (DFT). In order to cope with the long simulation times necessary to achieve an acceptable statistical accuracy, our ab initio approach is enhanced with deep-neural-network potentials (NNP). This approach is first validated against AIMD results, obtained by using the Perdew–Burke–Ernzerhof (PBE) exchange-correlation functional and paying careful attention to crucial, yet often overlooked, aspects of the statistical data analysis. Then, we train a second NNP to a dataset generated from the Strongly Constrained and Appropriately Normed (SCAN) functional. Once the error resulting from the imperfect prediction of the melting line is offset by referring the simulated temperature to the theoretical melting one, our SCAN predictions of the shear viscosity of water are in very good agreement with experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dual nature of magnetism driven by momentum dependent f-d Kondo hybridization

The intricate nature of magnetism in uranium-based Kondo lattices is a consequence of correlations between U-5 f and conduction electrons. Previously, the source of magnetism has been ascribed to either Mott physics or Ruderman-Kittel-Kasuya-Yosida interaction, both of which are not fully applicable to uranium-based Kondo lattices. Using linearized quasiparticle self-consistent GW plus dynamical mean-field theory, we demonstrate a crossover from incoherent to coherent f - d Kondo cloud in the paramagnetic phase of UTe 2 , USbTe and USbSe. As the transition occurs, we observe an augmented f - d coherence and Pauli-like magnetic susceptibility, with a substantial frozen magnetic moment of U-5 f persisting. We show that momentum dependent f - d hybridization is responsible for the magnetic moments arising from the renormalized f electrons’ van Hove singularity. Our findings provide a perspective to explain the dual nature of magnetism and the long-range magnetic ordering induced by pressure in UTe 2 .

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Excess Density as a Descriptor for Electrolyte Solvent Design

Electrolytes mediate interactions between the cathode and anode and determine performance characteristics of batteries. Mixtures of multiple solvents are often used in electrolytes to achieve desired properties, such as viscosity, dielectric constant, boiling point, and melting point. Conventionally, multi-component electrolyte properties are approximated with linear mixing, but in practice, significant deviations are observed. Excess quantities can provide insights into the molecular behavior of the mixture and could form the basis for designing high-performance electrolytes. Here we investigate the excess density of commonly used Li-ion battery solvents such as cyclic carbonates, linear carbonates, ethers, and nitriles with molecular dynamics simulations. We additionally investigate electrolytes consisting of these solvents and a salt. The results smoothly vary with mole percent and are fit to permutation-invariant Redlich-Kister polynomials. Mixtures of similar solvents, such as cyclic-cyclic carbonate mixtures, tend to have excess properties that are lower in magnitude compared to mixtures of dissimilar substances, such as carbonate-nitrile mixtures. We perform experimental testing using our automated test stand, Clio, to provide validation to the observed simulation trends. We quantify the structure similarity using SOAP fingerprints to create a descriptor for excess density, enabling the design of electrolyte properties. To a first approximation, this will allow us to estimate the deviation of a mixture from ideal behavior based solely upon the structural dissimilarity of the components.

74 ATOMIC AND MOLECULAR PHYSICS↗

Transition metal dichalcogenide monolayers in an ultrashort optical pulse: Femtosecond currents and anisotropic electron dynamics

We theoretically study the interaction of an ultrafast intense linearly polarized optical pulse with monolayers of transition metal dichalcogenides (TMDCs). Such a strong pulse redistributes electrons between the bands and generates femtosecond currents during the pulse. Due to the large bandwidth of the incident pulse, this process is completely an off-resonant. While in TMDCs, the time-reversal symmetry is conserved, the inversion symmetry is broken, and these monolayers have axial symmetry along the armchair direction but not along with the zigzag one. The pulse, polarized along with asymmetric directions of TMDC monolayer, generates both longitudinal, i.e., along the direction of polarization, and transverse, i.e., in the perpendicular direction, currents. Such currents result in charge transfer through the system. Finally, we study different TMDC materials and show how the femtosecond transport in TMDC monolayers depend on their parameters, such as lattice constant and bandgap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗