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At least 613 records · Page 34

Probing the electrolyte/electrode interface with vibrational sum frequency generation spectroscopy: A review

Over the past decades, Lithium-ion batteries have seen extensive improvements, and as a result are now the primary choice in many applications for their power, energy, and durability. In recent years, battery cost has reduced by orders of magnitude through adoption of new materials and processes. Despite these advances, interfaces in these battery systems are yet to be fully understood. This is seen as a major limitation to further increase cycle life, calendar life, abuse tolerance, and performances. A major obstacle is a lack of comprehensive understanding of the complex dynamic chemical processes occurring at the electrolyte/electrode interface. In this context, vibrational sum frequency generation (vSFG) spectroscopy possesses the unique capability of probing a molecularly thin interfacial layer to obtain molecular-level information through nonlinear optical interaction. Probing the molecular level processes at the interfaces using such a versatile technique would be a game changer in the advancement of current battery research knowledge. This review article summarizes recent vSFG studies on the electrolyte/electrode interface of various electrode materials and nonaqueous electrolytes for LIBs and discusses future research perspectives. Finally, overall, this focused review highlights the advantages and versatility of vSFG that can be used to further advance present-day battery research.

25 ENERGY STORAGE↗

The magnetohydrodynamics of current sheets

Examples of current sheets are summarized and their formation is described. A universal phenomenon in cosmic plasmas is the creation of sheets off intense current near X-type neutral points (where the magnetic field vanishes). These sheets are important as sites where the magnetic-field energy is converted efficiently into heat and bulk kinetic energy and where particles can be accelerated to high energies. Examples include disruptions in laboratory tokamaks, substorms in the earth's magnetosphere, and flares on the sun. The basic behavior of a one-dimensional sheet is presented, together with an account of the linear tearing-mode instability that can cause the field lines in such a sheet to reconnect. Such reconnection may develop in different ways: it may arise from a spontaneous instability or it may be driven, either from outside by motions or locally by a resistivity enhancement. Various processes are described that may occur during the nonlinear development of tearing, along with the many numerical and laboratory experiments that are aiding our understanding of this intriguing cosmical process.

Priest, E. R.↗

Acoustic fatigue life prediction for nonlinear structures with multiple resonant modes

An efficient method is presented for estimating the high-cycle fatigue lives of complex nonlinear structures. The procedure is based on an application of the method of equivalent linearization to construct a time-domain representation of the stress or strain response of a nonlinear structure. Fatigue estimates are obtained by processing the time-domain signal, and it is a simple matter to incorporate any damage accumulation model desired in the procedure. The method may also be applied to a wide range of complex nonlinear systems. Comparisons are presented of estimated fatigue lives for a nonlinear beam with random excitation obtained using the approximate method and using a conventional numerical simulation. The two techniques are found to give nearly identical results regardless of the level of nonlinearity. The number of calculations required in the approximate method is nearly the same as in a linear system and is not significantly affected by the type and level of nonlinearity in the structure.

Sun, J. Q.↗

Nonlinear Spectral Mixture Modeling of Lunar Multispectral: Implications for Lateral Transport

Linear and nonlinear spectral mixture models applied to Clementine multispectral images of the Moon result in roughly similar spatial distributions of endmember abundances. However, there are important differences in the absolute values of the predicted abundances. The magnitude of these differences and the implications for understanding geological processes are investigated across a geologic contact between mare and highland in the Grimaldi Basin on the western nearside of the Moon. Vertical and lateral mass transport due to impact cratering has redistributed mare and highland materials across the contact, creating a gradient in composition. Solutions to linear and nonlinear spectral mixture models for identical spectral endmembers of mare, highland, and fresh crater materials are compared across this simple geologic contact in the Grimaldi Basin. Profiles of mare abundance across the contact are extracted and compared quantitatively. Profiles from the linear mixture models indicate that the geologic contact has an average mare abundance of 60%, and the compositional boundary is asymmetric with more mare transported onto the highland side of the contact than highland onto the mare side of the contact. In contrast the nonlinear abundance profiles indicate that the geologic contact has an average mare abundance of 50%, and the compositional boundary is remarkably symmetric. Given the expectation that materials will be intimately mixed on the surface of the Moon, and that the asymmetries implied by the linear model are not consistent with our understanding of lunar surface processes, the nonlinear spectral mixture model is preferred and should be applied whenever quantitative abundance information is required. The remarkable symmetry in the compositional gradients across this contact indicate that lateral mass transport dominates over vertical transport at this boundary.

Mustard, John F.↗

Ultrafast electron dynamics of graphene quantum dots: High harmonic generation

We study theoretically nonlinear optical properties of graphene quantum dots placed in a field of a short and strong linearly polarized optical pulse. We address the problem of high harmonic generation in quantum dots and how such nonlinear effect is affected by dephasing processes in a quantum dot. The dephasing makes the ultrafast electron dynamics more irreversible with a large residual population of the excited quantum dot levels. In relation to the high-harmonic spectrum, with increasing the dephasing time, the intensities of the low-frequency harmonics increase while the cutoff energy decreases. The dependence of the cutoff energy on the amplitude of the optical pulse is also sensitive to the frequency of the pulse. When the frequency of the optical pulse is much less than the quantum dot band gap, this dependence is almost linear, but when the frequency of the pulse is comparable to the band gap, the cutoff energy shows saturation behavior at large field amplitude, >0.4 V/Å.

36 MATERIALS SCIENCE↗

Multiple Degradation Mechanisms in Reinforced Concrete Structures, Modeling and Risk Analysis

The overarching goal of this project is to complement ongoing Department of Energy (DOE) Light Water Reactor Sustainability (LWRS)-funded Grizzly concrete modeling development efforts by providing improved multi-physics models for incorporation into the Grizzly and BlackBear codes. Objectives of this work identified at the outset of this project include: 1. Coupling between mechanical damage and transport processes. The mechanical damage will be characterized by nonlinear mechanical constitutive models appropriate for concrete used in nuclear power plants (NPPs). 2. Improved representation of the coupling among the transport process, building on the current moisture and thermal transport models in Grizzly. The parameters for coupling among heat and mass transport in the multi-physics model will be experimentally determined. 3. Coupling among different scale levels of concrete constituents, fine and coarse aggregates, cement paste, hydration products, and pore structure. 4. Probabilistic analysis of the random nature of the heterogeneous concrete structure and the environmental factors (ambient temperature and humidity) and their multiple effects on concrete deterioration. 5. Benchmark verification, validation and uncertainty quantification of the thermo-hygro- chemo-mechanical (THCM) concrete formulation. The end goal of this work was to provide a comprehensive and robust simulation capability that can be applied at the engineering scale for analysis of realistic deterioration scenarios in NPP concrete structures.

36 MATERIALS SCIENCE↗

The effects on the ionosphere of inertia in the high latitude neutral thermosphere

High-latitude ionospheric currents, plasma temperatures, densities, and composition are all affected by the time-dependent response of the neutral thermosphere to ion drag and Joule heating through a variety of complex feedback processes. These processes can best be studied numerically using the appropriate nonlinear numerical modeling techniques in conjunction with experimental case studies. In particular, the basic physics of these processes can be understood using a model, and these concepts can then be applied to more complex realistic situations by developing the appropriate simulations of real events. Finally, these model results can be compared with satellite-derived data from the thermosphere. We used numerical simulations from the National Center of Atmospheric Research Thermosphere/Ionosphere General Circulation Model (NCAR TIGCM) and data from the Dynamic Explorer 2 (DE 2) satellite to study the time-dependent effects of the inertia of the neutral thermosphere on ionospheric currents, plasma temperatures, densities, and composition. One particular case of these inertial effects is the so-called 'fly-wheel effect'. This effect occurs when the neutral gas, that has been spun-up by the large ionospheric winds associated with a geomagnetic storm, moves faster than the ions in the period after the end of the main phase of the storm. In these circumstances, the neutral gas can drag the ions along with them. It is this last effect, which is described in the next section, that we have studied under this grant.

Burns, Alan↗

Physics informed deep neural network embedded in a chemical transport model for the Amazon rainforest

Secondary organic aerosols (SOA) are fine particles in the atmosphere, which interact with clouds, radiation and affect the Earth’s energy budget. SOA formation involves chemistry in gas phase, aqueous aerosols, and clouds. Simulating these chemical processes involve solving a stiff set of differential equations, which are computationally expensive steps for three-dimensional chemical transport models. Deep neural networks (DNNs) are universal function approximators that could be used to represent the complex nonlinear changes in aerosol physical and chemical processes; however, key challenges such as generalizability to extended time periods, preservation of mass balance, simulating sparse model outputs, and maintaining physical constraints have limited their use in atmospheric chemistry. Here, we develop an approach of using a physics-informed DNN that overcomes previous such challenges and demonstrates its applicability for the chemical formation processes of isoprene epoxydiol SOA (IEPOX-SOA) over the Amazon rainforest. The DNN is trained with data generated by simulating IEPOX-SOA over the entire atmospheric column, using the Weather Research and Forecasting Model coupled with Chemistry (WRF-Chem). The trained DNN is then embedded within WRF-Chem to replace the computationally expensive default solver of IEPOX-SOA formation. The trained DNN predictions generalizes well with the default model simulation of the IEPOX-SOA mass concentrations and its size distribution (20 size bins) over several days of simulations in both dry and wet seasons. The embedded DNN reduces the computational expense of WRF-Chem by a factor of 2. Our approach shows promise in terms of application to other computationally expensive chemistry solvers in climate models.

54 ENVIRONMENTAL SCIENCES↗

Experimental Performance of a Nonlinear Control Strategy to Regulate Temperature of a High-Temperature Solar Reactor

Abstract Despite the significant potential of solar thermochemical process technology for storing solar energy as solid-state solar fuel, several challenges have made its industrial application difficult. It is important to note that solar energy has a transient nature that causes instability and reduces process efficiency. Therefore, it is crucial to implement a robust control system to regulate the process temperature and tackle the shortage of incoming solar energy during cloudy weather. In our previous works, different model-based control strategies were developed namely a proportional integral derivative controller (PID) with gain scheduling and adaptive model predictive control (MPC). These methods were tested numerically to regulate the temperature inside a high-temperature tubular solar reactor. In this work, the proposed control strategies were experimentally tested under various operation conditions. The controllers were challenged to track different setpoints (500 °C, 1000 °C, and 1450 °C) with different amounts of gas/particle flowrates. Additionally, the flow controller was tested to regulate the reactor temperature under a cloudy weather scenario. The ultimate goal was to produce 5 kg of reduced solar fuel magnesium manganese oxide (MgMn2O4) successfully, and the controllers were able to track the required process temperature and reject disturbances despite the system's strong nonlinearity. The experimental results showed a maximum error in the temperature setpoint of less than 0.5% (6 °C), and the MPC controller demonstrated superior performance in reducing the control effort and rejecting disturbances.

Energy & Fuels↗

Higher-Order Spectral Analysis of a Nonlinear Pitch and Plunge Apparatus

Simulated aeroelastic responses of a nonlinear pitch and plunge apparatus are analyzed using various statistical signal processing techniques including higher-order spectral methods. A MATLAB version of the Nonlinear Aeroelastic Testbed Apparatus (NATA) at the Texas A&M University is used to generate various aeroelastic response data including limit cycle oscillations (LCO). Traditional and higher-order spectral (HOS) methods are applied to the simulated aeroelastic responses. Higher-order spectral methods are used to identify critical signatures that indicate the transition from linear to nonlinear (LCO) aeroelastic behavior.

Silva, Walter A.↗

Relative contributions of discrete and continuum absorption to the photodissociation of vibrationally excited O2 (v = 12-20)

In order to test the proposal that photodissociation of highly vibrationally excited O2 in the Schumann-Runge (SR) band is a source of upper stratospheric ozone, cross sections for the band and continuum absorption are calculated. Calculated maximum SR cross sections are in the 1-2 x 10 to the -18th sq cm range, with the O2(B) state contributing 2-3 orders of magnitude greater absorption than the 1 3Pi(u) state. For v-double prime = 12, it is shown that the SR band and continuum cross sections merge smoothly at 250 nm. It is shown that numerous processes, the most important of which is nonlinear photoabsorption, ultimately lead to the prediction that narrow laser line absorption in the 248-nm region should generate comparable O atom yields whether absorption is into the bands or the continuum. In the atmosphere, SR band absorption is the dominant process.

Saxon, R. P.↗

Interannual fires as a source for subarctic summer decadal climate variability mediated by permafrost thawing

Climate model simulations run under the Coupled Model Intercomparison Project Phase 6 (CMIP6) use an inhomogeneous biomass burning aerosol (BBA) emission dataset, which exhibits pronounced interannual variability from 1997–2014 due to the infusion of satellite data. Using the Community Earth System Model version 2 Large Ensemble (CESM2-LE) with original and smoothed CMIP6 BBA forcings, we show that the CMIP6 data inhomogeneity causes spurious decadal subarctic land warming. During years with reduced aerosol concentrations, increased solar radiation can trigger abrupt subarctic permafrost thawing, increased soil water drainage, upper soil drying, and subsequent surface warming. This slow process, which is further amplified by nonlinear cloud-aerosol interactions, cannot be completely offset during years of increased aerosol fluxes, thereby reddening surface temperature spectra in response to large-amplitude interannual aerosol forcing. More generally, our CESM2 experiments identify a pathway for generating decadal variability in high latitudes, involving interannual shortwave forcing and slow nonlinear soil responses.

54 ENVIRONMENTAL SCIENCES↗

Use of computer vision for analysis of image datasets from high temperature plasma experiments

Great strides have been made in improving the quality of x-ray radiographs in high energy density plasma experiments, enabled in part by innovations in engineering and manufacturing of integrated circuits and materials. As a consequence, the radiographs of today are filled with a great deal of detail, but few of these features are extracted in a systematic way. Analysis techniques familiar to plasma physicists tend toward brittle 1D lineout or Fourier transform type analyses. The techniques applied to process our data have not kept pace with improvements in the quality of our data. Fortunately, the field of computer vision has a wealth of tools to offer, which have been widely used in industrial imaging and, more recently, adopted in biological imaging. We demonstrate the application of computer vision techniques to the analysis of x-ray radiographs from high energy density plasma experiments, as well as give a brief tutorial on the computer vision techniques themselves. These tools robustly extract 2D contours of shocks, boundaries of inhomogeneities, and secondary flows, thereby allowing for increased automation of analysis, as well as direct and quantitative comparisons with simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Potential vorticity transport in weakly and strongly magnetized plasmas

Tangled magnetic fields, often coexisting with an ordered mean field, have a major impact on turbulence and momentum transport in many plasmas, including those found in the solar tachocline and magnetic confinement devices. We present a novel mean field theory of potential vorticity mixing in β-plane magnetohydrodynamic (MHD) and drift wave turbulence. Our results show that mean square stochastic fields strongly reduce Reynolds stress coherence. This decoherence of potential vorticity flux due to stochastic field scattering leads to suppression of momentum transport and zonal flow formation. A simple calculation suggests that the breaking of the shear-eddy tilting feedback loop by stochastic fields is the key underlying physics mechanism. Furthermore, a dimensionless parameter that quantifies the increment in power threshold is identified and used to assess the impact of stochastic field on the L-H transition. We discuss a model of stochastic fields as a resisto-elastic network.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

An eigenvalue-based method for computing the relaxed pressure in compressible multiphase flow with N phases

The modeling of compressible multiphase flows is a decades-old area of study with many applications across various fields. Many of these application areas use stiff pressure relaxation. This process involves the solution of a nonlinear system with N + 1 equations and N + 1 unknowns, where N is the number of phases. The resolution of this system with general equations of state (EOSs) is difficult. Furthermore, nonlinear systems can admit multiple solutions, and current solution methods do not address this possibility. Very recently, a thermodynamic relaxation method was introduced, which effectively maps a relatively simple predictor equation of state onto a more complex target equation of state. In this context, the target EOSs are the chosen EOSs for the thermodynamic model. Furthermore, this thermodynamic relaxation has the benefit of simplifying the stiff pressure relaxation system of equations. In this article, we show this system reduces to a polynomial of degree N, which can be recast as an eigenvalue problem through the use of the associated companion matrix. We show that although this eigenvalue method is generally less efficient than Newton–Raphson iteration, it does not suffer from convergence issues and finds all N roots of the polynomial. Hence, the method provides a fail-safe for root-finding iterative methods and a way to address the issue of multiple solutions to the nonlinear system of equations in stiff pressure relaxation.

Eigenvalue algorithm↗

Nonlinear optical control of chiral charge pumping in a topological Weyl semimetal

Solids with topologically robust electronic states exhibit unusual electronic and optical properties that do not exist in other materials. A particularly interesting example is chiral charge pumping, the so-called chiral anomaly, in recently discovered topological Weyl semimetals, where simultaneous application of parallel DC electric and magnetic fields creates an imbalance in the number of carriers of opposite topological charge (chirality). Here, using time-resolved terahertz measurements on the Weyl semimetal TaAs in a magnetic field, we optically interrogate the chiral anomaly by dynamically pumping the chiral charges and monitoring their subsequent relaxation of the nonequilibrium state. Theory based on Boltzmann transport shows that the observed effects originate from an optical nonlinearity in the chiral charge pumping process. Our measurements reveal that the nonequilibrium chiral excitation relaxation time is much greater than 1 ns. The observation of terahertz-controlled chiral carriers with long coherence times and topological protection suggests the application of Weyl semimetals for quantum optoelectronic technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Enhancing EV Motor Design Through Knowledge-Based AI and Hierarchical Fuzzy Logic Model

This work presents a novel approach to optimizing electric vehicle motor design through the integration of Knowledge-Based Artificial Intelligence (KB-AI) and Hierarchical Fuzzy Logic. Traditional motor design processes are time-intensive, relying heavily on iterative simulations and domain-specific expertise. These processes are further complicated by the nonlinear relationships between key design parameters. The proposed framework addresses these challenges by systematically encoding expert knowledge from scientific literature into a fuzzy logic system, allowing for the efficient handling of complex design variables. The hierarchical fuzzy logic model reduces computational complexity by decomposing the nonlinear relationships into manageable rule sets while maintaining design accuracy. The proposed methodology was applied to the design of a 100 kW motor, yielding optimal values for key parameters. This resulted in a compact motor design with a volume of 2.2 liters, showcasing the framework’s ability to deliver high-performance, application-specific motor configurations.

Kumar, Praveen [ORNL] (ORCID:0000000291877857)↗

Pupil movements to light and accommodative stimulation - A comparative study.

Isolation and definition of specific response components in pupil reflexes through comparison of the dynamic features of light-induced and accommodation-induced pupil movements. A quantitative analysis of the behavior of the complex nonlinear pupil responses reveals the presence of two independent nonlinear characteristics: a range-dependent gain and a direction dependence or movement asymmetry. These nonlinear properties are attributed to motor processes because they are observable in pupil responses to both light and accommodation stimuli. The possible mechanisms and consequences of these pupil response characteristics are quantitatively defined and discussed.

Semmlow, J.↗