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At least 631 records · Page 35

A modeling comparison of deep greenhouse gas emissions reduction scenarios by 2030 in California

California aims to reduce greenhouse gas (GHG) emissions to 40% below 1990 levels by 2030. We compare six energy models that have played various roles in informing the state policymakers in setting climate policy goals and targets. These models adopt a range of modeling structures, including stock-turnover back-casting models, a least-cost optimization model, macroeconomic/macro-econometric models, and an electricity dispatch model. Results from these models provide useful insights in terms of the transformations in the energy system required, including efficiency improvements in cars, trucks, and buildings, electrification of end-uses, low- or zero-carbon electricity and fuels, aggressive adoptions of zero-emission vehicles (ZEVs), demand reduction, and large reductions of non-energy GHG emissions. Some of these studies also suggest that the direct economic costs can be fairly modest or even generate net savings, while the indirect macroeconomic benefits are large, as shifts in employment and capital investments could have higher economic returns than conventional energy expenditures. These models, however, often assume perfect markets, perfect competition, and zero transaction costs. They also do not provide specific policy guidance on how these transformative changes can be achieved. Greater emphasis on modeling uncertainty, consumer behaviors, heterogeneity of impacts, and spatial modeling would further enhance policymakers' ability to design more effective and targeted policies. Here, this paper presents an example of how policymakers, energy system modelers and stakeholders interact and work together to develop and evaluate long-term state climate policy targets. Lastly, even though this paper focuses on California, the process of dialogue and interactions, modeling results, and lessons learned can be generally adopted across different regions and scales.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Transuranium Sulfide via the Boron Chalcogen Mixture Method and Reversible Water Uptake in the NaCu T S 3 Family

The behavior of 5f electrons in soft ligand environments makes actinides, and especially transuranium chalcogenides, an intriguing class of materials for fundamental studies. Due to the affinity of actinides for oxygen, however, it is a challenge to synthesize actinide chalcogenides using non-metallic reagents. Using the Boron Chalcogen Mixture (BCM) method, we achieved the synthesis of the transuranium sulfide NaCuNpS 3 starting from the oxide reagent, NpO 2 . Via the same synthetic route, the isostructural composition of NaCuUS 3 was synthesized and the material contrasted with NaCuNpS 3 . Single crystals of the U-analog, NaCuUS 3 , were found to undergo an unexpected reversible hydration process to form NaCuUS 3 ·xH 2 O (x ≈ 1.5). Here, a large combination of techniques was used to fully characterize the structure, hydration process, and electronic structures, specifically a combination of single crystal, powder, high temperature powder X-ray diffraction, extended X-ray ab-sorption fine structure, infrared, and inductively coupled plasma spectroscopies, thermogravimetric analysis, and density functional theory calculations. The outcome of these analyses enabled us to determine the composition of NaCuUS 3 ·xH 2 O and obtain a structural model that demonstrated the retention of the local structure within the [CuUS 3 ] – layers throughout the hydration-dehydration process. Band structure, density of states, and Bader charge calculations for NaCuUS 3 , NaCu-US 3 ·xH 2 O, and NaCuNpS 3 along with X-ray absorption near edge structure, UV-vis-NIR and work function measurements on ACuUS 3 (A = Na, K, and Rb) and NaCuUS 3 ·xH 2 O samples were carried out to demonstrate that electronic properties arise from the [CuTS 3 ] – layers and show surprisingly little dependence on the interlayer distance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Uncertainty Quantification of Extratropical Forest Biomass in CMIP5 Models over the Northern Hemisphere

Abstract Simplified representations of processes influencing forest biomass in Earth system models (ESMs) contribute to large uncertainty in projections. We evaluate forest biomass from eight ESMs outputs archived in the Coupled Model Intercomparison Project Phase 5 (CMIP5) using the biomass data synthesized from radar remote sensing and ground-based observations across northern extratropical latitudes. ESMs exhibit large biases in the forest distribution, forest fraction, and mass of carbon pools that contribute to uncertainty in forest total biomass (biases range from −20 Pg C to 135 Pg C). Forest total biomass is primarily positively correlated with precipitation variations, with surface temperature becoming equally important at higher latitudes, in both simulations and observations. Relatively small differences in forest biomass between the pre-industrial period and the contemporary period indicate uncertainties in forest biomass were introduced in the pre-industrial model equilibration (spin-up), suggesting parametric or structural model differences are a larger source of uncertainty than differences in transient responses. Our findings emphasize the importance of improved (1) models of carbon allocation to biomass compartments, (2) distribution of vegetation types in models, and (3) reproduction of pre-industrial vegetation conditions, in order to reduce the uncertainty in forest biomass simulated by ESMs.

54 ENVIRONMENTAL SCIENCES↗

Atomically thin interlayer phase from first principles enables defect-free incommensurate SnO2/CdTe interface

Advancing optoelectronic and emerging technologies increasingly requires control and design of interfaces between dissimilar materials. However, incommensurate interfaces are notoriously defective and rarely benefit from first-principles predictions, because no explicit atomic-structure models exist. Here, we adopt a bulk crystal structure prediction method to the interface geometry and apply it to SnO2/CdTe heterojunctions without and with the addition of CdCl2, a ubiquitous and beneficial, but abstruse processing step in CdTe photovoltaics. Whereas the direct SnO2/CdTe interface is highly defective, we discover a unique two-dimensional CdCl2 interphase, unrelated to the respective bulk structure. It facilitates a seamless transition from the rutile to zincblende lattices and removes defect-states from the interface bandgap. Implementing the predicted interface electronic structure in device simulations, we demonstrate the theoretical feasibility of bufferless oxide-CdTe heterojunction solar cells approaching the Shockley–Queisser limit. Our results highlight the broader potential of designing atomically thin interlayers to enable defect-free incommensurate interfaces.

14 SOLAR ENERGY↗

Influence of interstitial Mn on local structure and magnetism in Mn 1 + δ Sb

We report x-ray total scattering and pair distribution function (PDF) studies of the structural relaxation around interstitial manganese (Mn i ) in ferromagnetic Mn 1+δ Sb (0.03 ≤ δ ≤ 0.23) alloys, guided by density functional theory (DFT). Refinements to the experimental PDF using a crystallographically constrained structural model indicate an expansion in the equatorial plane of the Mn i Sb 5 trigonal bipyramidal site, which introduces significant positional disorder in addition to the nominally random occupation of interstitial voids. Observation of a weak diffuse signal near the symmetry-forbidden (001) reflection position is indicative of correlated disorder from the clustering of Mn i . Density functional relaxation of supercells approximating the δ = 0.08, 0.15, and 0.23 compositions provides improved models that accurately describe the short-range structural distortions captured in the PDFs. Furthermore, such structural relaxation increases the DFT calculated moment on Mn i , which aligns antiparallel to the primary Mn moments, but leads to insubstantial changes in the average Mn and Sb moments and moments of Mn and Sb proximal to interstitials, thus providing a more accurate description of the observed bulk magnetic properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Small Molecule Evaluator

Using machine learning to score potential drug candidates may offer an advantage over traditional imprecise scoring functions because the parameters and model structure can be learned from the data. However, models may lack interpretability, are often overfit to the data, and are not generalizable to drug targets and chemotypes not in the training data. Benchmark datasets are prone to artificial enrichment and analogue bias due to the overrepresentation of certain scaffolds in experimentally determined active sets. Datasets can be evaluated using spatial statistics to quantify the dataset topology and better understand potential biases. Dataset clumping comprises a combination of self-similarity of actives and separation from decoys in chemical space and is associated with overoptimistic virtual screening results. This code explores methods of quantifying potential biases and examines some common benchmark datasets.

Ellingson, Sally↗

Molecular Dynamics-based Simulations of Bulk/Interfacial Structures and Diffusion Behaviors in Nuclear Waste Glasses

This NEUP Project aimed to generate accurate atomic structural models of nuclear waste glasses by using large-scale molecular dynamics-based computer simulations and to use these models to investigate self-diffusion behaviors, interfacial structures, and hydrated gel structures formed during dissolution of these glasses. The goal was to obtain realistic and accurate short and medium range structures of these complex oxide glasses, to provide a mechanistic understanding of the dissolution behaviors, and to generate reliable information with predictive power in designing nuclear waste glasses for long-term geological storage. Looking back of the research accomplishments of this project, most of the scientific goals initially proposed have been achieved through intensive research in the three and a half year period of the project. This project has also generated a wealth of scientific data and vibrant discussions with various groups through collaborations within and outside of this project. Throughout the project one book chapter and 14 peer reviewed journal publications have been generated (including one under review) and 16 presentations (including 8 invited talks) have been made to disseminate the results of this project in national and international conference. Furthermore, this project has trained several outstanding graduate students and young researchers for future workforce in nuclear related field, especially on nuclear waste immobilization. One postdoc and four PhD students have been fully or partially supported through the project with intensive training in the field material science and engineering with expertise on glass science and nuclear waste disposal

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Physics-Informed Machine Learning Model for Ceramic Matrix Composite Creep

A physics-informed recurrent neural network (RNN) based surrogate model is developed to emulate the nonlinear, time-dependent constitutive behavior of ceramic matrix composites (CMCs) driven by matrix damage and constituent creep at the microscale. Physics-informed constraints are introduced into the surrogate model through regularization to ground the prediction in physics and improve its predictive capabilities. Training data is generated using the high-fidelity generalized method of cells (HFGMC) approach which calls appropriate creep and damage models for each of the constituents. This coupling permits simulating the nonlinear behavior of CMCs based on constituent response at the microscale along with microstructural features such as fiber and porosity volume fraction and fiber radius. The microscale repeating unit cell is loaded under creep fatigue conditions to replicate the material loading experienced in a turbine engine. Therefore, the RNN-based surrogate model is tasked with predicting, as a function of variable input stress sequence, temperature, and microstructural features, the resulting strain history response while satisfying physical constraints related to creep rate, isochoric inelastic deformation, and strain energy density. The trained surrogate model is shown to effectively match the strain history over quantified distributions of microstructural features and relevant loading regimes and temperatures. Neural network based surrogate models can offer efficient alternatives to running computationally intensive multiscale material models to simulate the nonlinear response of large structural models. Therefore, the presented work provides evidence towards the feasibility of developing, training, and running such models for CMCs with complex microstructures, nonlinear time-dependent material response, and under non-monotonic loading conditions.

ceramic matrix composites↗

Earth System Reanalysis in Support of Climate Model Improvements

Recent climate model developments, established through increased model resolution, have led to substantial improvements in model simulations of the time-evolving, coupled Earth system and its subcomponents. However, regardless of resolution, climate models will always produce climate features and variability that differ from the real world and will be prone to biases. This is due to many remaining uncertainties, such as in parametric and structural model uncertainty, in the initial conditions prescribed, and in the prescribed (scenario) forcing which varies on decadal to centennial timescales. Further model improvements are expected to arise specifically from improved representation of physical processes realized through model-data fusion. This will create an unprecedented opportunity to better exploit a large array of Earth observations, from in situ measurements to weather radars and satellite observations, as the resolved scales of the models approach those of the observations. For this, climate DA will be the central tool to bring models and observations into consistency, by improving initial conditions, inferring uncertain model parameters and structure, and quantifying uncertainty. Generally, there will be advantages and complementarities of adjoint-based smoother approaches, ensemble-based filter approaches, or new ML-inspired approaches. Yet, the ever-increasing model resolution will present growing challenges arising from computational cost, calling for new ways of performing data assimilation and model optimization. Using the complementarity in a hybrid approach, blending tools and concepts from variational, ensemble and ML methods might be what is required in the future. In this context ML could be important to handle non-linear responses, and to better approximate non-Gaussian distributions.

54 ENVIRONMENTAL SCIENCES↗

Connections Between Mean North Pacific Circulation and Western US Precipitation Extremes in a Warming Climate

Abstract Extreme precipitation has widespread impacts over the western US (WUS), which are expected to be exacerbated in the future given thermodynamically driven increases in atmospheric moisture and shifts in atmospheric circulation patterns. However, internal climate variability complicates how these factors affect future projections of precipitation changes. In this study, we investigate late 21st‐century changes in mean‐state responses over the North Pacific Ocean and associated WUS precipitation extremes using the Multi‐Model Large Ensemble Archive, which is a recent and valuable resource to disentangle the effects of model structural differences from internal variability. We found that inter‐model differences in precipitation extremes over the WUS are large: from south to north (here, from California to Washington), models show different levels of increases for both the frequency and intensity of heavy precipitation. In general, the Pacific Northwest sees a more consistent signal than California. We show that wet‐season mean circulation influences extreme precipitation, by using a decomposition of the relative contributions of thermodynamic (atmospheric humidity) and dynamic (large‐scale circulation) driven changes. The thermodynamic contribution dominates, however, the dynamic contribution varies with latitude and differs substantially between model ensembles. Inter‐model differences affect the spread in not only the magnitude, but also the sign of the dynamic contribution. This implies that mean circulation changes contribute to uncertainty in quantifying the regional structure of concentrated moisture flux and future extreme events. This result highlights the need to more accurately constrain projected North Pacific coupled circulation changes to narrow the spread in projections of future precipitation extremes.

54 ENVIRONMENTAL SCIENCES↗

Three-dimensional structure of a flavivirus dumbbell RNA reveals molecular details of an RNA regulator of replication

Abstract Mosquito-borne flaviviruses (MBFVs) including dengue, West Nile, yellow fever, and Zika viruses have an RNA genome encoding one open reading frame flanked by 5′ and 3′ untranslated regions (UTRs). The 3′ UTRs of MBFVs contain regions of high sequence conservation in structured RNA elements known as dumbbells (DBs). DBs regulate translation and replication of the viral RNA genome, functions proposed to depend on the formation of an RNA pseudoknot. To understand how DB structure provides this function, we solved the x-ray crystal structure of the Donggang virus DB to 2.1Å resolution and used structural modeling to reveal the details of its three-dimensional fold. The structure confirmed the predicted pseudoknot and molecular modeling revealed how conserved sequences form a four-way junction that appears to stabilize the pseudoknot. Single-molecule FRET suggests that the DB pseudoknot is a stable element that can regulate the switch between translation and replication during the viral lifecycle by modulating long-range RNA conformational changes.

Akiyama, Benjamin M.↗

Magnetic-Field-Driven Electron Dynamics in Graphene

Graphene exhibits unique optoelectronic properties originating from the band structure at the Dirac points. It is an ideal model structure to study the electronic and optical properties under the influence of the applied magnetic field. In graphene, electric field, laser pulse, and voltage can create electron dynamics which is influenced by momentum dispersion. However, computational modeling of momentum-influenced electron dynamics under the applied magnetic field remains challenging. In this work, we perform computational modeling of the photoexcited electron dynamics achieved in graphene under an applied magnetic field. Our results show that magnetic field leads to local deviation from momentum conservation for charge carriers. With the increasing magnetic field, the delocalization of electron probability distribution increases and forms a cyclotron-like trajectory. Our work facilitates understanding of momentum resolved magnetic field effect on non-equilibrium properties of graphene, which is critical for optoelectronic and photovoltaic applications.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Structure and aggregation in model tetramethylurea solutions

The structure of model aqueous tetramethylurea (TMU) solutions is investigated employing large-scale (32 000, 64 000 particles) molecular dynamics simulations. Results are reported for TMU mole fractions, X{sub t}, ranging from infinite dilution up to 0.07, and for two temperatures, 300 and 330 K. Two existing force fields for TMU-water solutions are considered. These are the GROMOS 53A6 united-atom TMU model combined with SPC/E water [TMU(GROMOS-UA)/W(SPC/E)], and the more frequently employed AMBER03 all-atom force field for TMU combined with the TIP3P water model [TMU(AMBER-AA)/W(TIP3P)]. It is shown that TMU has a tendency towards aggregation for both models considered, but the tendency is significantly stronger for the [TMU(AMBER-AA)/W(TIP3P)] force field. For this model signs of aggregation are detected at X{sub t} = 0.005, aggregation is a well established feature of the solution at X{sub t} = 0.02, and the aggregates increase further in size with increasing concentration. This is in agreement with at least some experimental studies, which report signals of aggregation in the low concentration regime. The TMU aggregates exhibit little structure and are simply loosely ordered, TMU-rich regions of solution. The [TMU(GROMOS-UA)/W(SPC/E)] model shows strong signs of aggregation only at higher concentrations (X{sub t} ≳ 0.04), and the aggregates appear more loosely ordered, and less well-defined than those occurring in the [TMU(AMBER-AA)/W(TIP3P)] system. For both models, TMU aggregation increases when the temperature is increased from 300 to 330 K, consistent with an underlying entropy driven, hydrophobic interaction mechanism. At X{sub t} = 0.07, the extra-molecular correlation length expected for microheterogeneous solutions has become comparable with the size of the simulation cell for both models considered, indicating that even the systems simulated here are sufficiently large only at low concentrations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Art and Science of the Cellular Mesoscale

Experimental information from microscopy, structural biology, and bioinformatics may be integrated to build structural models of entire cells with molecular detail. This integrative modeling is challenging in several ways: the intrinsic complexity of biology results in models with many closely packed and heterogeneous components; the wealth of available experimental data is scattered among multiple resources and must be gathered, reconciled, and curated; and computational infrastructure is only now gaining the capability of modeling and visualizing systems of this complexity. We present recent efforts to address these challenges, both with artistic approaches to depicting the cellular mesoscale, and development and application of methods to build quantitative models.

59 BASIC BIOLOGICAL SCIENCES↗

A quantitative assessment of the model form error of friction models across different interface representations for jointed structures

Hysteretic models are widely used to model frictional interactions in joints to recreate experimental behavior. However, it is unclear which models are best suited for fitting or predicting the responses of structures. Here, the present study evaluates 26 friction model/interface representation combinations to quantify the model form error. A Quasi-Static Modal Analysis approach (termed Rayleigh Quotient Nonlinear Modal Analysis) is adopted to calculate the nonlinear system response, and a Multi-Objective Optimization is solved to fit experimental data of the first mode of the Brake-Reuß Beam. Optimized parameters from the first mode are applied to the second and third bending modes to quantify the predictive ability of the models. Formulations for both tracing full hysteresis loops and recreating hysteresis loops from a single loading curve (Masing assumptions) are considered. Smoothly varying models applied to a five patch representation showed the highest flexibility (for fitting mode 1) and good predictive potential (for modes 2 and 3). For a second formulation, which uses 152 frictional elements to represent the interface, the physically motivated spring in series with a Coulomb slip model (elastic dry friction) has high error for fitting mode 1 and performs near the middle for predicting higher modes. For both interface representation, the best fit models are not the most physical, but rather the ones with the most parameters (as expected); however, the more physical models perform somewhat better for predicting the higher modes.

42 ENGINEERING↗

On the Nanoscale Structure of K x Fe 2-y Ch 2 (Ch = S, Se): A Neutron Pair Distribution Function View

Comparative exploration of the nanometer-scale atomic structure of K x Fe 2-y Ch 2 (Ch = S, Se) was performed using neutron total scattering-based atomic pair distribution function (PDF) analysis of 5 K powder diffraction data in relation to physical properties. Whereas K x Fe 2-y Se 2 is a superconductor with a transition temperature of about 32 K, the isostructural sulphide analogue is not, which instead displays a spin glass semiconducting behavior at low temperatures. The PDF analysis explores phase separated and disordered structural models as candidate descriptors of the low temperature data. For both materials, the nanoscale structure is well described by the iron (Fe)-vacancy-disordered K 2 Fe 5-y Ch 5 (I4/m) model containing excess Fe. An equally good description of the data is achieved by using a phase separated model comprised of I4/m vacancy-ordered and I4/mmm components. The I4/mmm component appears as a minority phase in the structure of both K x Fe 2-y Se 2 and K x Fe 2-y S 2 , and with similar contribution, implying that the phase ratio is not a decisive factor influencing the lack of superconductivity in the latter. Comparison of structural parameters of the Fe-vacancy-disordered model indicates that the replacement of selenium (Se) by sulphur (S) results in an appreciable reduction in the Fe-Ch interatomic distances and anion heights, while simultaneously increasing the irregularity of FeCh 4 tetrahedra, suggesting the more significant influence of these factors. Finally, structural features are also compared to the non-intercalated FeSe and FeS parent phases, providing further information for the discussion about the influence of the lattice degrees of freedom on the observed properties in layered iron chalcogenides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Thermodynamic nature of vitrification in a 1D model of a structural glass former

We propose a new spin-glass model with no positional quenched disorder which is regarded as a coarse-grained model of a structural glass-former. The model is analyzed in the 1D case when the number N of states of a primary cell is large. For N → ∞, the model exhibits a sharp freezing transition of the thermodynamic origin. It is shown both analytically and numerically that the glass transition is accompanied by a significant growth of a static length scale ξ pointing to the structural (equilibrium) nature of dynamical slowdown effects in supercooled liquids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Purification and Characterization of Protein Nanotubes Assembled from a Single Bacterial Microcompartment Shell Subunit

Bacterial microcompartments (BMCs) are apparently icosahedral proteinaceous organelles that are bioinformatically identified in an increasing number of bacterial species. BMCs are delimited by a protein shell composed predominantly of hexameric (BMC-H) subunits that tile into the facets of the BMC shell. Here we report a new biomaterial composed of the single BMC-H protein encoded in the BMC locus of Mycobacterium smegmatis; the function of this type of BMC is unknown. When expressed in Escherichia coli, this BMC-H protein, RmmH, self-assembles into nanotubes, densely packed in the cytoplasmic space. These are the first BMC nanotubes to be purified from cells intact and characterized. Here, we also show formation of the nanotubes initiated from free RmmH hexamers in vitro. Based on the dimensions of the nanotubes and modeling of the RmmH hexamer, we propose two possible structural models. BMC nanotubes offer a new spatial architecture both in vivo and in vitro, composed of a single protein that may be genetically or chemically modified and for use as tubular scaffolding.

36 MATERIALS SCIENCE↗