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At least 37 records · Page 2

Investigating Tropical Versus Extratropical Influences on the Southern Hemisphere Tropical Edge in the Unified Model

Abstract Since the late 1970s, observations have shown a widening of the tropical Hadley cell (HC) circulation. State‐of‐the‐art climate models reproduce the general trend along with a projected continuous expansion. Discrepancies in expansion rates of observation‐ and model‐based studies have been attributed to differences in applied methods, natural variability and model shortcomings. Furthermore, the driving influence of tropical or extratropical processes on these changes is not well understood. All of this highlights the dynamical mechanisms and the region of origin controlling the tropical width are still insufficiently understood. Here we examine the influence of systematic model biases of the atmosphere‐only Unified Model (UM) onto the simulation of the Southern Hemisphere (SH) tropical edge. We utilize nudged experiments with prescribed sea surface temperatures, where potential temperature and horizontal winds are relaxed back to ERA‐Interim reanalysis for a 20‐year period in selected regions. Correcting model biases in the tropics and extratropics separately allows us to dissect the dominant remote impacts of present model errors onto the SH tropical edge simulation. The experiments are applied to established tropical width metrics ranging from near‐surface to upper‐level metrics capturing the poleward flank of the HC. We find both regions work remotely to reduce errors in the UM fields and location of the tropical edge. Surprisingly, correcting the extratropical biases, south of 45°S, more consistently improves the tropical width across the metrics and seasons than nudging the tropics (10°N–10°S). These findings demonstrate the substantial role of extratropical influences in locating the SH tropical edge.

54 ENVIRONMENTAL SCIENCES↗

Diffusion behavior of lanthanide fission products in bcc Fe cladding: A first-principles study

Fuel-cladding chemical interaction poses significant challenges in nuclear reactors, where fission products generated from nuclear fuel interact with Fe-based cladding materials, potentially compromising their structural integrity. This study investigates the diffusion behavior of lanthanide fission products, Lanthanum (La), Cerium (Ce), Praseodymium (Pr), and Neodymium (Nd), within body-centered cubic (bcc) Fe cladding using the density functional theory, nudged elastic band method, and self-consistent mean field theory. Our results reveal significant vacancy binding energies, particularly with the 1st and 2nd nearest neighbors, which diminish beyond the 5th nearest neighbor, with La exhibiting the strongest binding affinity, followed by Nd, Ce, and Pr. The nudged elastic band calculations indicate significant high barriers for the dissociation of 1st nearest neighbor vacancy-solute pairs for all fission products. The tracer diffusion coefficients of these fission products were derived in an Arrhenius form, with a magnetic correction that accounts for the high-temperature paramagnetic state. The significant trapping effect of vacancies caused by a very dilute concentration of fission products reduces vacancy mobility, potentially leading to modifications in point defect supersaturation, void nucleation, and swelling under irradiation. These represent critical challenges for irradiated cladding materials. The tracer diffusion coefficients indicate that Nd diffuses the fastest, followed by La, Ce, and Pr. Furthermore, this study provides essential insights for understanding fission product transport in cladding materials and informs future design strategies to mitigate fuel-cladding chemical interaction, ultimately enhancing nuclear reactor safety and performance.

Diffusion↗

On the Regionality of Moist Kelvin Waves and the MJO: The Critical Role of the Background Zonal Flow

Abstract A global model with superparameterized physics is used to shed light on the observed regionality of convectively coupled Kelvin waves and the Madden‐Julian Oscillation (MJO). A series of aquaplanet simulations over zonally uniform sea‐surface temperatures is performed, in which the axisymmetric structure of the background zonal flow is altered through nudging, while maintaining a quasi‐fixed rainfall climatology. Results show that nudging at the equator to match profiles typical of the Indo‐Pacific or eastern Pacific sectors yields eastward‐moving tropical rain spectra typical of those sectors. Two different mechanistic pathways are identified as being responsible for this mean‐flow dependence, in addition to Doppler shifting effects. The first is through shifts of the Rossby wave critical line in the subtropical upper troposphere that affect the lateral forcing of Kelvin‐mode circulations at the equator by eastward and equatorward‐propagating eddies impinging on the tropics from higher latitudes. The second is through changes in the strength of the mean cyclonic shear in the lower tropical troposphere that affect the degree to which intraseasonal fluctuations in Kelvin‐mode zonal winds modulate the activity of higher‐frequency equatorial Rossby‐type eddies. In cases where the mean low‐level cyclonic shear is enhanced, the strength of this modulation, referred to as “shear‐induced eddy modulation” or SIEM, is also seen to be enhanced, such that MJO‐like modes of variability are rendered either unstable or near neutral, depending on the strength of the shear.

Tulich, S. N.↗

Disentangling the chemistry and transport impacts of the quasi-biennial oscillation on stratospheric ozone

The quasi-biennial oscillation (QBO) in tropical winds perturbs stratospheric ozone throughout much of the atmosphere via changes in transport of ozone and other trace gases, as well as via temperature changes, both of which alter ozone chemistry. Attributing these causes of QBO–ozone variability may provide insights into model-to-model differences that contribute to ozone simulation. Here we develop a novel metric of steady-state ozone (SSO) to separate these effects: SSO calculates the local steady-state response of ozone due to the changes in temperature, chemical species, and overhead ozone column; the response due to circulation change is presumed when SSO shows no response. It is applied to the nudged Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2) with interactive ozone chemistry to demonstrate its validity. The E3SMv2 simulations nudged to reanalysis data produced reasonable wind and ozone patterns, especially in the tropics. Consistent with previous studies, we find clear demarcations with pressure. Ozone perturbations in the upper stratosphere (<6 hPa) are predicted by temperature changes; those between 6 and 20 hPa are predicted by NO y changes, and those in the lower stratosphere show no temperature or NO y response and are presumably driven by circulation changes. These results are important for diagnosing model-to-model discrepancy in QBO–ozone response and enhancing the reliability of ozone projections.

Xie, Jinbo [Lawrence Livermore National Laboratory↗

Energetics of the nucleation and glide of disconnection modes in symmetric tilt grain boundaries

Grain boundaries (GBs) evolve by the nucleation and glide of disconnections, which are dislocations with a step character. In this work, motivated by recent success in predicting GB properties such as the shear coupling factor and mobility from the intrinsic properties of disconnections, we develop a systematic method to calculate the energy barriers for the nucleation and glide of individual disconnection modes under arbitrary driving forces and a quasi-2D setting. This method combines tools from bicrystallography to enumerate disconnection modes and the Nudged elastic band (NEB) method to calculate their energetics, yielding minimum energy paths and atomistic mechanisms for the nucleation and glide of each disconnection mode. We apply the method to accurately predict shear coupling factors of $[001]$ symmetric tilt grain boundaries in Cu. Particular attention is paid to the boundaries where the dislocation-based disconnection nucleation model produces incorrect nucleation barriers. We demonstrate that the method can accurately compute energy barriers and predict shear-coupling factors in the low-temperature regime. For certain disconnection modes in which the assumptions underlying our method do not hold, we report upper bounds on the energy barriers for disconnection nucleation and glide. In addition, the NEB trajectories reveal interesting phenomena such as the dissociation of a higher energy mode into lower energy modes, and in some cases, shear coupling being mediated by partial disconnections, wherein the GB structure temporarily changes to a metastable state before reverting back to its original structure. Graphical abstract

36 MATERIALS SCIENCE↗

Atomistic determination of Peierls barriers of dislocation glide in nickel

The Peierls barrier measures the lattice resistance to dislocation glide in crystalline solids. We use the nudged elastic band (NEB) method to calculate the Peierls barriers for screw and edge dislocation glide in a face-centered cubic (FCC) metal of Ni. The minimum energy paths (MEPs) across single or sequential Peierls barriers are determined under shear loading. The NEB results show the decreasing Peierls barrier with increasing shear stress, giving the Peierls stress at which the Peierls barrier vanishes. The effects of boundary condition and system size on Peierls barriers are studied by comparing strain- and stress-controlled NEB results. Furthermore, the free-end NEB methods are applied to determine MEPs with improved computational efficiency. The NEB results are also used to evaluate the energetic driving force of dislocation glide, which is consistent with that determined from the Peach-Koehler force. The accuracy of the present NEB results based on an empirical interatomic potential is assessed by comparison with a machine-learning potential. This work demonstrates the robust and efficient quantification of Peierls barriers to dislocation glide in an FCC metal, and it lays a solid foundation for the atomistic determination of Peierls barriers in compositionally complex alloys with the FCC structure in future studies.

42 ENGINEERING↗

Revealing the Defect‐Driven Ferroelectric Mechanisms of Aluminum Nitride

Wurtzite III-nitride compounds are CMOS-compatible with widespread industrial interest to exercise ferroelectricity, despite their polar structure being highly resistant to polarization reversal. Here, we induce and tune ferroelectric properties in w-AlN via direct-write ion-beam processing, using nanoscale patterned defect engineering as a post-growth alternative to conventional cation substitution. Nanometric piezoresponse spectroscopy of the focused He + beam patterned defect concentrations in ferroelectric Al 0.92 B 0.08 N measures a localized 10x enhancement in effective piezoresponse and 40% reduction in switching barrier. The irradiation-induced point defects convert piezoelectric AlN into a ferroelectric system with site-saturated nucleation and raise the dielectric susceptibility, switched polarization, and effective piezoelectric coefficient. Enhanced defect-lattice interactions in AlN increase carrier conduction and phonon scattering loss but preserve long-range crystallinity. Here, based on atomistic analysis of nudged elastic band density functional theory calculations and reactive force field simulations, both nitrogen vacancies and defect complexes disrupt bond ordering, facilitating a line-by-line low-barrier switching of pristine AlN.

36 MATERIALS SCIENCE↗

Water‐mediated Decomposition Pathways of ε‐Hexanitrohexaazaisowurtzitane

The dominant initial decomposition mechanism of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (HNIW) is understood from the literature to be the N─NO 2 bond scission unimolecular mechanism. Here we have found a water-mediated HONO release initial decomposition mechanism energetically competitive with the N─NO 2 bond scission mechanism modeled using ab initio nudged elastic band simulations. The activation energy of the water-mediated HONO mechanism was calculated to be 138.9 kJ/mol with the Perdew, Burke, and Ernzerhof (PBE) functional (177.8 with PBE0), while the double NO 2 release mechanism is 171.9 kJ/mol (203.3 with PBE0). Branching secondary, tertiary, and quaternary decomposition steps were also discovered including oxidation of HONO or H 2 O causing ring-opening that leads to C─N bond breaking and N 2 O or NO release. The reaction rate of HONO oxidation is much faster than HONO release, making the HONO concentration low. The Helmholtz free energy barrier of the double NO 2 release mechanism is lower than the water-mediated HONO release above 438 K (165°C) due to the vibrational contribution to the free energy. This helps explain why the literature reports more NO 2 release at higher temperatures. The present study reveals a physical mechanism for how water can catalyze the decomposition of HNIW at low enough temperatures, and reveals secondary, tertiary, and quaternary reaction mechanisms leading to NO x release. In conclusion, as water is realistically always present, the reported barriers are important for building kinetic models needed to ensure the safety and reliability of HNIW.

Steele, Brad A. [Lawrence Livermore National Labor↗

Long-term single-column model intercomparison of diurnal cycle of precipitation over midlatitude and tropical land

General Circulation Models (GCMs) have for decades exhibited difficulties in modelling the diurnal cycle of precipitation (DCP). This issue can be related to inappropriate representation of the processes controlling sub-diurnal phenomena like convection. In this study, 11 single-column versions of GCMs are used to investigate the interactions between convection and environmental conditions, processes that control nocturnal convections, and the transition from shallow to deep convection on a diurnal time-scale. Long-term simulations are performed over two continental land sites: the Southern Great Plains (SGP) in the USA for 12 summer months from 2004 to 2015 and the Manacapuru site at the central Amazon (MAO) in Brazil for two full years from 2014 to 2015. The analysis is done on two regimes: afternoon convective regime and nocturnal precipitation regime. Most models produce afternoon precipitation too early, likely due to the missing transition of shallow-to-deep convection in these models. At SGP, the unified convection schemes better simulate the onset time of precipitation. At MAO, models produce the heating peak in a much lower level compared with observation, indicating too shallow convection in the models. For nocturnal precipitation, models that produce most of nocturnal precipitation all allow convection to be triggered above the boundary layer. This indicates the importance of model capability to detect elevated convection for simulating nocturnal precipitation. Sensitivity studies indicate that (a) nudging environmental variables towards observations has a minor impact on DCP, (b) unified treatment of shallow and deep convection and the capability to capture mid-level convection can help models better capture DCP, and (c) the interactions of the atmosphere with other components in the climate system (e.g. land) are also important for DCP simulations in coupled models. Finally, these results provide long-term statistical insights on which physical processes are essential in climate models to simulate DCP.

54 ENVIRONMENTAL SCIENCES↗

Atmospheric teleconnection associated with the Atlantic multidecadal variability in summer: assessment of the CESM1 model

Observational analysis shows that the Atlantic multidecadal variability (AMV) is associated with climate variability in the Northern Hemisphere through a zonal atmospheric teleconnection extending from the North Atlantic Ocean and propagating eastward around the Northern Hemisphere. Here, we studied the fidelity of model simulations in reproducing the observed summer AMV and the associated impacts on the mid-latitude climate by analysing simulations using the National Centre for Atmospheric Research Community Earth System Model Version 1 (CESM1), including CESM1 North Atlantic idealized and pacemaker simulations, CESM1 large ensemble twentieth century uninitialized simulations and large ensemble initialized CESM1 decadal predictions. To further compare the fidelity of CESM1, we also analysed large ensemble simulations from three other models. Our results suggest that the uninitialized large ensemble simulations from all models can produce an AMV time evolution and its regional climate impacts similar to the observations to certain degree. By initializing the observed oceanic condition in decadal prediction simulations, the simulated AMV and its regional impacts are closer to the observed ones than those in uninitialized ensemble simulations. In addition, the pacemaker simulations that nudged the time-evolving observed North Atlantic sea surface temperature anomalies produce spatiotemporal characteristics of the AMV and AMV climate impacts closer to the observed ones than the uninitialized simulations. We conclude that although coupled models can produce AMV and its regional impacts similar to observed, proper initialization and bias correction of the sea surface temperature spatial and temporal structure can improve this capability.

Initialization↗

Adsorption and Surface Diffusion of Metals on α-Al2O3 for Advanced Manufacturing Applications

Abstract The adsorption and diffusion of Mo and Nb adatoms on the $$\alpha$$ α -Al 2 O 3 (0001) surface were explored using density functional theory-based methods. Adsorption energies of Mo and Nb adatoms at minima sites on the surface were determined. Mo and Nb adatoms prefer to adsorb to the same locations on the surface, and larger adsorption energies calculated for Nb compared to Mo indicate that Nb adatom-surface interactions are stronger than Mo. Using minima adsorption sites as initial and final locations for surface diffusion, energy barriers for diffusion were calculated using the nudged elastic band method. Overall, Mo and Nb follow roughly the same diffusion paths. The diffusion pre-factors for Mo and Nb are similar; however, Mo diffusion has a lower energy barrier and thus a larger diffusion coefficient compared with Nb. These results provide insight into the role of surface diffusion of Mo and Nb adatoms during advanced manufacturing processes.

Biaggne, Austin (ORCID:0000000328074960)↗

Atomistic modeling of surface and grain boundary dislocation nucleation in FCC metals

Dislocation nucleation plays a critical role in the plastic deformation of crystalline materials. However, it is challenging to predict the active mode and associated rate of dislocation nucleation under typical experimental loading conditions through molecular dynamics simulation due to timescale limitations. In this report we use the free-end nudged elastic band method to determine the activation energies and activation volumes of dislocation nucleation in four typical face-centered cubic metals of Au, Al, Cu and Ni. We focus on the representative processes of surface and grain boundary dislocation nucleation. The atomistically determined activation volumes of these dislocation nucleation processes are larger than 10b3 (with b being the Burgers vector length) under typical experimental loading conditions. These results are compared with experimentally measured activation volumes in ultrafine-grained and nanocrystalline metals, thereby providing mechanistic insight into their rate-controlling deformation mechanisms.

36 MATERIALS SCIENCE↗

An automated cluster surface scanning method for exploring reaction paths on metal-cluster surfaces

Metal-cluster surfaces present a wide variety of unique coordination environments. This complexity makes it difficult to manually probe the surface reactivity of such clusters. Here, we present a simple and automated method to systematically discover reaction pathways on cluster surfaces, based on the automated cluster surface scanning (ACSS) technique for mapping out potential energy surfaces. We showcase our method on 55-atom icosahedral Cu and Ag clusters, where we determine the activation energies of four elementary steps common in heterogeneous catalysis – hydrogen recombination (H* + H* → H 2 * + *), oxygen recombination (O* + O* → O 2 * + *), water formation (OH* + H* → H 2 O* + *), and CO oxidation (CO* + O* → CO 2 * + *) – with density functional theory calculations (DFT-PBE + D3). We show that the ACSS method requires significantly less human effort than the established manually performed climbing-image nudged elastic band (MP + CI-NEB) technique and locates transition states with comparable accuracy (root-mean-squared error of 0.10 eV) and similar computational cost. Rigorous sampling of the potential energy surface with the ACSS method allows one to locate all lowest-energy reaction pathways obtained via the MP+CI-NEB approach, as well as alternative pathways that one may have missed with the MP+CI-NEB approach due to the many possible pathways available on these clusters. The accuracy and efficiency afforded by the ACSS method could enable high-throughput exploration of the diverse reactivity of metal clusters.

36 MATERIALS SCIENCE↗

Hydrogen Localization and Cluster Formation in α-Zr from First-Principles Investigations

We report alpha-zirconium (α-Zr) is a hydrogen atom host material used in nuclear energy and semiconducting applications due to Zr's excellent properties such as corrosion resistance, low thermal neutrons cross-section, and thermodynamically favorable interstitial sequestering of H atoms. Herein we use density functional theory simulations to systematically analyze the initial stages of H insertion in the Zr matrix, and determine optimal hydrogen localization, distribution, and clustering tendencies from a thermodynamics and kinetics perspective. Our results suggest that H occupation of tetrahedral sites is strongly favored, consistent with previous experimental and theoretical studies. Further, a cooperative effect in H localization is shown where H atoms favor clustering. The H pair is found to be the most stable by occupying tetrahedral sites with pairs at second nearest-neighbor positions (TTn2). Among the four H atom clusters, the most favorable configuration has two TTn2 pairs forming "box " or "zig-zag" shaped-cluster with the pairs separated by 3.03 or 3.25 Å, respectively. Nudged elastic band simulations suggest that the formation of TTn2 is facile and is limited by the small diffusion barrier of the monomer of less than 0.1 eV. Further, the formation routes for the 4H atom clusters are also presented. The current study can serve as a foundation to systematically model H atom clustering in metals and alloys.

36 MATERIALS SCIENCE↗

Ensemble variational Fokker-Planck methods for data assimilation

Particle flow filters solve Bayesian inference problems by smoothly transforming a set of particles into samples from the posterior distribution. Particles move in state space under the flow of an McKean-Vlasov-Itˆo process. This work introduces the Variational Fokker-Planck (VFP) framework for data assimilation, a general approach that includes previously known particle flow filters as special cases. The McKean-Vlasov-Itˆo process that transforms particles is defined via an optimal drift that depends on the selected diffusion term. It is established that the underlying probability density - sampled by the ensemble of particles - converges to the Bayesian posterior probability density. For a finite number of particles the optimal drift contains a regularization term that nudges particles toward becoming independent random variables. Based on this analysis, we derive computationally-feasible approximate regularization approaches that penalize the mutual information between pairs of particles, and avoid particle collapse. Moreover, the diffusion plays a role akin to a particle rejuvenation approach that aims to alleviate particle collapse. The VFP framework is very flexible. Different assumptions on prior and intermediate probability distributions can be used to implement the optimal drift, and localization and covariance shrinkage can be applied to alleviate the curse of dimensionality. A robust implicit-explicit method is discussed for the efficient integration of stiff McKean- Vlasov-Itˆo processes. Here, the effectiveness of the VFP framework is demonstrated on three progressively more challenging test problems, namely the Lorenz ’63, Lorenz ’96 and the quasi-geostrophic equations.

97 MATHEMATICS AND COMPUTING↗

Density functional theory calculations of the thermodynamic and kinetic properties of point defects in β -U

Density functional theory (DFT) calculations of the thermodynamic and kinetic properties of point defects in the β phase of uranium are reported. Defect energies and entropies were calculated using 2 x 2 x 2 supercells and the Generalized Gradient Approximation (GGA) of Perdew-Burke-Ernzerhof (PBE) for the exchange-correlation potential. Due to computational cost, calculations of the vibrational properties governing entropies were performed by only displacing atoms within (roughly) the 3rd or 4th nearest neighbor shell of the defect, which implicitly assumes that atoms beyond this distance are unaffected by the defect. Migration barriers were estimated by nudged elastic band (NEB) calculations. The low symmetry of the β-U phase (the unit cell is tetragonal and contains 30 atoms) results in many point defect configurations and even more migration pathways. A connectivity map, starting from the most stable point defects, was developed in order to identify the rate-limiting step controlling the net diffusion rate in each crystallographic direction. The uranium self-diffusivity tensor was calculated by combining the defect formation energies, entropies, migration barriers and attempt frequencies. The fastest diffusion rate was determined to be a vacancy mechanism in the z crystallographic direction. The predicted uranium self-diffusivity for this mechanism agrees well with available experimental data. Finally, the diffusion mechanisms and rates identified in this study will inform fuel performance models of swelling and gas evolution.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

The impact of chemistry on anion migration in bixbyite-structured lanthanide oxides

This manuscript describes atomistic calculations of oxygen vacancy and interstitial migration in bixbyite structured lanthanide oxides. We examine two types of compounds, one in which only one type of lanthanide cation is present and a second class in which two lanthanides are present in a 3:1 ratio as dictated by the symmetry of the bixbyite crystal structure. Using temperature accelerated dynamics and the nudged elastic band method, we quantify the role of chemistry on the energy barriers for the most important pathways for both vacancy and interstitial migration. We then analyze the impact of these variations on the overall diffusivity of each defect, quantifying the contribution of each pathway using the theory of kinosons. We find that vacancy mobility can vary by as much as three orders of magnitude through changes in chemistry at 500 K. Changes in interstitial mobility are more modest but can still vary by an order of magnitude. This points to the ability to tune the mass transport characteristics of these compounds through appropriate choices in chemistry. We have also included supplementary information containing the atomic structures of the relevant pathways.

36 MATERIALS SCIENCE↗

Li + Diffusion in Amorphous and Crystalline Al 2 O 3 for Battery Electrode Coatings

Al 2 O 3 is often applied protectively to lithium-ion battery anode and cathode materials to inhibit surface degradation, suppress dendrite formation, and relieve mechanical stresses. Given the very high intrinsic band gap and diffusion barrier of the material, the mechanism that allows Li diffusion through these coatings is not well understood, and widely varying laboratory results indicate that there may be dependencies on morphology and stoichiometry. Using nudged elastic band calculations and ab initio molecular dynamics, we perform a systematic investigation across Al 2 O 3 structures, both crystalline and amorphous, and at various concentrations of Li + to uncover the optimal parameters for maximally diffusive coatings. We find a correlation between the low proximity of Li + to Al 3+ and the low Li + migration barrier. Although barriers are the lowest in the highly diffusive one-dimensional channels of crystalline θ-Al 2 O 3 , the system is structurally delicate and subject to detrimental distortion as the Li + content is increased. The α-Al 2 O 3 lattice is, conversely, highly stable against distortion at all Li + concentrations but disadvantageous for Li + migration. In amorphous systems, unscreened Li + –Li + Coulomb repulsion and pre-emptive occupation of “trapping sites” combine to lower the energy barriers as a function of increasing concentration. One of our most important findings is that Al-deficient materials can sharply increase Li + movement, and we predict that an amorphous material with a combination of high Li + concentration and Al deficiency would enable highly Li + -conductive protective coatings for electrodes.

25 ENERGY STORAGE↗