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At least 901 records · Page 50

Implications of reduced-complexity aerosol thermodynamics on organic aerosol mass concentration and composition over North America

Atmospheric organic aerosol (OA) mass concentrations can be affected by water uptake through its impact on the gas–particle partitioning of semi-volatile compounds. Current chemical transport models (CTMs) neglect this process. We have implemented the Binary Activity Thermodynamics model coupled to a volatility basis set partitioning scheme in the GEOS-Chem CTM, providing an efficient reduced-complexity OA model that predicts relative-humidity-dependent mixing and partitioning thermodynamics, while limiting the impact on computational efficiency. We provide a quantitative assessment of this water-sensitive OA treatment, focusing on a subdomain over North America. The updated OA scheme predicts a spatiotemporal mean enhancement in surface-level OA mass concentration of 145 % for January 2019 and 76 % for July 2019 compared to GEOS-Chem's most advanced OA scheme. The temporal mean surface-level OA organic mass concentration can increase by up to ∼590 % for January 2019 and ∼280 % for July 2019, with the greatest enhancements occurring over the ocean. The updated OA scheme also quantifies the OA-associated water content. The simulations show how different OA precursors and related OA surrogates contribute and respond to water uptake, including that due to changes in temperature and relative humidity over the diurnal cycle in selected winter and summer months. These results are independent of future CTM improvements involving updates to chemical reaction schemes and emission inventories. Our water-sensitive OA scheme allows for a better representation of the seasonal and regional variations in OA mass concentration in CTMs.

54 ENVIRONMENTAL SCIENCES↗

A reinterpretation of the electronic spectrum of pyrrole: A quantum dynamics study

The first band in the electronic spectrum of pyrrole is calculated from wavepacket propagations performed using the MCTDH method. To do so, two model Hamiltonians are constructed to describe seven low-lying excited electronic states of pyrrole. These Hamiltonians are based on the vibronic coupling model, and are parameterised via fitting to extensive CASPT2 and EOM-CCSD calculations. A detailed analysis of the structure of pyrrole's electronic spectrum in the range 5.5 to 6.5 eV is made. The role of intensity borrowing from transitions to ππ{sup *} states by lower-lying 3s and 3p Rydberg states is assessed, and reassignments of much of the spectrum are subsequently made which indicate that most of the states in the spectrum are predominantly Rydberg in character. The resulting conclusions drawn serve to highlight the limitations of assignments based on the matching of calculated vertical excitation energies and the positions of peak maxima observed in electronic spectra.

74 ATOMIC AND MOLECULAR PHYSICS↗

Plasma-catalyst modeling for materials selection: challenges and opportunities in nitrogen oxidation

Reliable kinetic models are essential to rationalize observations and to guide the selection of appropriate plasma-catalyst combinations. Kinetic models coupling plasma- and heterogeneous-catalytic-chemistries, however, are primitive. Here, we combine reduced plasma chemistries and density functional theory parameterized surface reactions to model NO formation from N2 oxidation, an alternative nitrogen fixation process. We first show plasma excited species can enhance turnover frequencies of both Pt and Au. The enhancing potential is a function of plasma species and their densities. We then compare NO production between plasma/Pt and plasma/Au with an integral reactor model and explore the dependence of NO production as a function of plasma conditions, reactor configurations and chemical compositions. Plasma/Pt generates more NO than plasma/Au under most thermal and plasma parametric conditions. Plasma/Au outperforms plasma/Pt under high plasma excitations at low temperatures. Furthermore, these results highlight that selection of plasma-catalyst combinations should consider the properties of plasmas, materials and the coupling of the two.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Mean-Field Ring Polymer Rates Using a Population Dividing Surface

Mean-field Ring Polymer Molecular Dynamics (MF-RPMD) offers a computationally efficient method for the simulation of reaction rates in multi-level systems. Previous work has established that, to model a nonadiabatic state-to-state reaction accurately, the dividing surface must be chosen to explicitly sample kinked ring polymer configurations where at least one bead is in a different electronic state than the others. Building on this, we introduce a population difference coordinate and a kink-constrained dividing surface, and we test the accuracy of the resulting mean-field rate theory on a series of bilinear coupling model systems. Here, we demonstrate that this new MF-RPMD rate approach is efficient to implement and quantitatively accurate for models over a wide range of driving forces, coupling strengths, and temperatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Simulation of hardened cement degradation and estimation of uncertainty in predicted failure times with peridynamics

Modeling the degradation of cement-based infrastructure due to aqueous environmental conditions continues to be a challenge. In order to develop a capability to predict concrete infrastructure failure due to chemical degradation, here we created a chemomechanical model of the effects of long-term water exposure on cement paste. The model couples the mechanical static equilibrium balance with reactive–diffusive transport and incorporates fracture and failure via peridynamics (a meshless simulation method). The model includes fundamental aspects of degradation of ordinary Portland cement (OPC) paste, including the observed softening, reduced toughness, and shrinkage of the cement paste, and increased reactivity and transport with water induced degradation. This version of the model focuses on the first stage of cement paste decalcification, the dissolution of portlandite. Given unknowns in the cement paste degradation process and the cost of uncertainty quantification (UQ), we adopt a minimally complex model in two dimensions (2D) in order to perform sensitivity analysis and UQ. We calibrate the model to existing experimental data using simulations of common tests such as flexure, compression and diffusion. Then we calculate the global sensitivity and uncertainty of predicted failure times based on variation of eleven unique and fundamental material properties. We observed particularly strong sensitivities to the diffusion coefficient, the reaction rate, and the shrinkage with degradation. Also, the predicted time of first fracture is highly correlated with the time to total failure in compression, which implies fracture can indicate impending degradation induced failure; however, the distributions of the two events overlap so the lead time may be minimal. Extension of the model to include the multiple reactions that describe complete degradation, viscous relaxation, post-peak load mechanisms, and to three dimensions to explore the interactions of complex fracture patterns evoked by more realistic geometry is straightforward and ongoing.

36 MATERIALS SCIENCE↗

The Roles of Tidal Marshes in the Estuarine Biochemical Processes: A Numerical Modeling Study

Observations suggest that the existence of tidal marsh can alter the oxygen and nutrient dynamics in adjacent water bodies, but assessing the impacts of large tidal marshes on an estuary is challenging. In this study, we use a modeling approach to investigate the roles of tidal marshes on the estuarine biochemical processes. The marsh model, which simulates the ecological functions of marshes at seasonal and annual time-scales, is embedded inside an unstructured-grid three-dimensional hydrodynamic and eutrophication model (SCHISM-ICM). This modeling system simulates the growth and metabolism of the tidal marshes and links biological processes to nutrient dynamics in the water column and sediment. This model dynamically simulates nutrient recycling and physical transport of the materials between marshes and open water through wetting-drying processes. This coupled model system is validated and successfully applied to the York River Estuary. Model results suggest that tidal marshes influence the local diurnal dissolved oxygen (DO) cycle by exporting dissolved organic carbon and high sediment oxygen demand in the marsh system through the tidal exchange. The high deposition rates of organics and diurnal DO cycle enhance the sediment release of phosphorus. On the other hand, marshes tend to decrease dissolved inorganic nitrogen in the water column by settling particulate nutrients and enhancing the denitrification process. The study demonstrates that tidal marshes exert substantial impacts on the estuarine biochemical processes. The developed tidal marsh model enhances eutrophication modeling and advances the understanding of the feedback effects between marsh biogeochemistry and estuarine eutrophication processes on a systemic scale.

54 ENVIRONMENTAL SCIENCES↗

Impacts of climate change on subannual hydropower generation: a multi-model assessment of the United States federal hydropower plant

Abstract Hydropower is a low-carbon emission renewable energy source that provides competitive and flexible electricity generation and is essential to the evolving power grid in the context of decarbonization. Assessing hydropower availability in a changing climate is technically challenging because there is a lack of consensus in the modeling representation of key dynamics across scales and processes. Focusing on 132 US federal hydropower plants, in this study we evaluate the compounded impact of climate and reservoir-hydropower models’ structural uncertainties on monthly hydropower projections. In particular, instead of relying on one single regression-based hydropower model, we introduce another conceptual reservoir operations-hydropower model in the assessment framework. This multi-model assessment approach allows us to partition uncertainties associated with both climate and hydropower models for better clarity. Results suggest that while at least 70% of the uncertainties at the annual scale and 50% at the seasonal scale can be attributed to the choice of climate models, up to 50% of seasonal variability can be attributed to the choice of hydropower models, particularly in regions over the western US where the reservoir storage is substantial. The analysis identifies regions where multi-model assessments are needed and presents a novel approach to partition uncertainties in hydropower projections. Another outcome includes an updated evaluation of Coupled Model Intercomparison Project Phase 5 (CMIP5)-based federal hydropower projection, at the monthly scale and with a larger ensemble, which can provide a baseline for understanding future assessments based on CMIP6 and beyond.

54 ENVIRONMENTAL SCIENCES↗

Phase-field model for diffusion-induced grain boundary migration: An application to battery electrodes

Diffusion-induced grain boundary migration is a phenomenon in which a grain boundary moves in response to the driving forces generated by diffusing solute species. For example, diffusing solute species change the atomic volume in the host material, either by filling a vacancy with a misfitting solute atom or by expanding host lattices through interstitial diffusion. These volume changes are inhomogeneous and are stored as elastic energy in the material that drives grain boundaries. In this paper, we introduce our previously developed Cahn-Hilliard–phase-field-crystal model (CH-PFC) as a computational tool to investigate diffusion-induced grain boundary migration in crystalline materials. This multiscale phase-field model couples the composition field of a diffusing species with the crystallographic texture of a host material. We apply the CH-PFC model to battery electrodes and investigate whether interstitial solute diffusion induces grain growth in FePO 4 /LiFePO 4 electrodes. To this end, we compute grain growth in 60 FePO 4 electrodes by conducting two parallel trials: In the first trial, we cycle the electrode and calculate diffusion-induced grain growth. In the second trial, we do not cycle the electrode and calculate curvature-driven grain growth. We find a statistically significant grain growth in the cycled electrodes and negligible grain growth in the noncycled electrodes. Altogether, we show that the CH-PFC model not only predicts electrode microstructures as a function of the Li composition, but also predicts the crystallographic features of an electrode during battery operation.

36 MATERIALS SCIENCE↗

Dynamic Multi-Sensor Multi-Mission Optimal Planning Tool

Remote sensing systems have firmly established a role in providing immense value to commercial industry, scientific exploration, and national security. Continued maturation of sensing technology has reduced the cost of deploying highly-capable sensors while at the same time increased reliance on the information these sensors can provide. The demand for time on these sensors is unlikely to diminish. Coordination of next-generation sensor systems, larger constellations of satellites, unmanned aerial vehicles, ground telescopes, etc. is prohibitively complex for existing heuristics-based scheduling techniques. The project was a two-year collaboration spanning multiple Sandia centers and included a partnership with Texas A&M University. We have developed algorithms and software for collection scheduling, remote sensor field-of-view pointing models, and bandwidth-constrained prioritization of sensor data. Our approach followed best practices from the operations research and computational geometry communities. These models provide several advantages over state of the art techniques. In particular, our approach is more flexible compared to heuristics that tightly couple models and solution techniques. First, our mixed-integer linear models afford a rigorous analysis so that sensor planners can quantitatively describe a schedule relative to the best possible. Optimal or near-optimal schedules can be produced with commercial solvers in operational run-times. These models can be modified and extended to incorporate different scheduling and resource constraints and objective function definitions. Further, we have extended these models to proactively schedule sensors under weather and ad hoc collection uncertainty. This approach stands in contrast to existing deterministic schedulers which assume a single future weather or ad hoc collection scenario. The field-of-view pointing algorithm produces a mosaic with the fewest number of images required to fully cover a region of interest. The bandwidth-constrained algorithms find the highest priority information that can be transmitted. All of these are based on mixed-integer linear programs so that, in the future, collection scheduling, field-of-view, and bandwidth prioritization can be combined into a single problem. Experiments conducted using the developed models, commercial solvers, and benchmark datasets have demonstrated that proactively scheduling against uncertainty regularly and significantly outperforms deterministic schedulers.

47 OTHER INSTRUMENTATION↗

Identification of key parameters controlling demographically structured vegetation dynamics in a land surface model: CLM4.5(FATES)

Vegetation plays an important role in regulating global carbon cycles and is a key component of the Earth system models (ESMs) that aim to project Earth's future climate. In the last decade, the vegetation component within ESMs has witnessed great progress from simple “big-leaf” approaches to demographically structured approaches, which have a better representation of plant size, canopy structure, and disturbances. These demographically structured vegetation models typically have a large number of input parameters, and sensitivity analysis is needed to quantify the impact of each parameter on the model outputs for a better understanding of model behavior. In this study, we conducted a comprehensive sensitivity analysis to diagnose the Community Land Model coupled to the Functionally Assembled Terrestrial Simulator, or CLM4.5(FATES). Specifically, we quantified the first- and second-order sensitivities of the model parameters to outputs that represent simulated growth and mortality as well as carbon fluxes and stocks for a tropical site with an extent of 1 x 1°. While the photosynthetic capacity parameter (V c,max25 )is found to be important for simulated carbon stocks and fluxes, we also show the importance of carbon storage and allometry parameters, which determine survival and growth strategies within the model. The parameter sensitivity changes with different sizes of trees and climate conditions. The results of this study highlight the importance of understanding the dynamics of the next generation of demographically enabled vegetation models within ESMs to improve model parameterization and structure for better model fidelity.

54 ENVIRONMENTAL SCIENCES↗

A Hamiltonian fluid-kinetic model for a two-species non-neutral plasma

A model for describing the dynamics of a pure electron plasma in the presence of a population of massive charged particles is presented. The model couples the fluid dynamics of the pure electron plasma with the dynamics of the massive particle population, the latter being treated kinetically. The model is shown to possess a noncanonical Hamiltonian structure and to preserve invariants analogous to those of the two-dimensional (2D) Euler equation for an incompressible inviscid fluid, and of the Vlasov equation. The Hamiltonian structure of the model is used to derive a set of stability conditions for rotating coherent structures of the two-species system, in the case of negatively charged massive particles. According to these conditions, stability is attained if both the equilibrium distribution function of the kinetic species and the equilibrium density of the electron fluid are monotonically decreasing functions of the corresponding single-particle energies in the rotating frame. For radially confined equilibria near the axis, the stability condition corresponds to the existence of a finite interval of rotation frequencies for the reference frame, with the upper bound determined by the presence of the kinetic population.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Urgent need for warming experiments in tropical forests

Abstract Although tropical forests account for only a fraction of the planet's terrestrial surface, they exchange more carbon dioxide with the atmosphere than any other biome on Earth, and thus play a disproportionate role in the global climate. In the next 20 years, the tropics will experience unprecedented warming, yet there is exceedingly high uncertainty about their potential responses to this imminent climatic change. Here, we prioritize research approaches given both funding and logistical constraints in order to resolve major uncertainties about how tropical forests function and also to improve predictive capacity of earth system models. We investigate overall model uncertainty of tropical latitudes and explore the scientific benefits and inevitable trade‐offs inherent in large‐scale manipulative field experiments. With a Coupled Model Intercomparison Project Phase 5 analysis, we found that model variability in projected net ecosystem production was nearly 3 times greater in the tropics than for any other latitude. Through a review of the most current literature, we concluded that manipulative warming experiments are vital to accurately predict future tropical forest carbon balance, and we further recommend the establishment of a network of comparable studies spanning gradients of precipitation, edaphic qualities, plant types, and/or land use change. We provide arguments for long‐term, single‐factor warming experiments that incorporate warming of the most biogeochemically active ecosystem components (i.e. leaves, roots, soil microbes). Hypothesis testing of underlying mechanisms should be a priority, along with improving model parameterization and constraints. No single tropical forest is representative of all tropical forests; therefore logistical feasibility should be the most important consideration for locating large‐scale manipulative experiments. Above all, we advocate for multi‐faceted research programs, and we offer arguments for what we consider the most powerful and urgent way forward in order to improve our understanding of tropical forest responses to climate change.

Cavaleri, Molly A.↗

On the Correspondence between Mean Forecast Errors and Climate Errors in CMIP5 Models

The present study examines the correspondence between short- and long-term systematic errors in five atmospheric models by comparing the 16 five-day hindcast ensembles from the Transpose Atmospheric Model Intercomparison Project II (Transpose-AMIP II) for July–August 2009 (short term) to the climate simulations from phase 5 of the Coupled Model Intercomparison Project (CMIP5) and AMIP for the June–August mean conditions of the years of 1979–2008 (long term). Because the short-term hindcasts were conducted with identical climate models used in the CMIP5/AMIP simulations, one can diagnose over what time scale systematic errors in these climate simulations develop, thus yielding insights into their origin through a seamless modeling approach. The analysis suggests that most systematic errors of precipitation, clouds, and radiation processes in the long-term climate runs are present by day 5 in ensemble average hindcasts in all models. Errors typically saturate after few days of hindcasts with amplitudes comparable to the climate errors, and the impacts of initial conditions on the simulated ensemble mean errors are relatively small. This robust bias correspondence suggests that these systematic errors across different models likely are initiated by model parameterizations since the atmospheric large-scale states remain close to observations in the first 2–3 days. However, biases associated with model physics can have impacts on the large-scale states by day 5, such as zonal winds, 2-m temperature, and sea level pressure, and the analysis further indicates a good correspondence between short- and long-term biases for these large-scale states. Therefore, improving individual model parameterizations in the hindcast mode could lead to the improvement of most climate models in simulating their climate mean state and potentially their future projections.

54 ENVIRONMENTAL SCIENCES↗

Influence of Lake Ice Biases in Reanalysis Data on Downscaled Climate Simulations over the Great Lakes Region

This data package contains observation-based and model-simulated datasets (all provided in NetCDF format) for evaluating how wintertime lake-ice representation affects regional weather and climate over the Laurentian Great Lakes (freshwater lake ecosystem) during the high–ice-cover winter of 2009. The observational component includes: (1) Stage IV gridded precipitation at 4 km, hourly resolution for January–February 2009 over the Great Lakes region (radar–gauge multisensor precipitation analyses); (2) Great Lakes Surface Environmental Analysis (GLSEA) satellite-derived lake-ice coverage at 1.3 km, daily resolution for the 2009 winter months, providing ice coverage over Lakes Superior, Michigan, Huron, Erie, and Ontario; and (3) in situ measurements at the Standard Rock site on Lake Superior from the Great Lakes Evaporation Network (GLEN) at hourly resolution, including near-surface atmospheric variables and sensible and latent heat fluxes (air–lake exchange) at a fixed point location. The modeling component provides corresponding fields from two simulations, both archived at 4 km, hourly resolution: a standalone Weather Research Forecasting model (WRF) run driven by the European Centre for Medium-Range Weather Forecasts (ECMWF) Reanalysis 5 (ERA5), and a two-way coupled model using WRF and the Finite Volume Community Ocean Model (WRF-FVCOM, a 3-D hydrodynamic lake model). These outputs include variables relevant to air–lake interaction and lake-effect processes (e.g., near-surface temperature, humidity, wind, precipitation, and surface turbulent fluxes), enabling direct comparison with the observational datasets. Users can analyze and visualize these NetCDF files with common tools such as Python (e.g., xarray, netCDF4, numpy, pandas), NCO/CDO, Panoply, or ncview; NetCDF variables can also be converted to other formats (e.g., CSV, GeoTIFF) using these utilities.

EARTH SCIENCE > ATMOSPHERE > ATMOSPHERIC TEMPERATU↗

Source attribution of black carbon and its direct radiative forcing in China

Abstract. The source attributions for mass concentration, haze formation, transport and direct radiative forcing of black carbon (BC) in various regions of China are quantified in this study using the Community Earth System Model (CESM) with a source-tagging technique. Anthropogenic emissions are from the Community Emissions Data System that is newly developed for the Coupled Model Intercomparison Project Phase 6 (CMIP6). Over north China where the air quality is often poor, about 90 % of near-surface BC concentration is contributed by local emissions. Overall, 35 % of BC concentration over south China in winter can be attributed to emissions from north China, and 19 % comes from sources outside China in spring. For other regions in China, BC is largely contributed from nonlocal sources. We further investigated potential factors that contribute to the poor air quality in China. During polluted days, a net inflow of BC transported from nonlocal source regions associated with anomalous winds plays an important role in increasing local BC concentrations. BC-containing particles emitted from East Asia can also be transported across the Pacific. Our model results show that emissions from inside and outside China are equally important for the BC outflow from East Asia, while emissions from China account for 8 % of BC concentration and 29 % in column burden in the western United States in spring. Radiative forcing estimates show that 65 % of the annual mean BC direct radiative forcing (2.2 W m−2) in China results from local emissions, and the remaining 35 % is contributed by emissions outside of China. Efficiency analysis shows that a reduction in BC emissions over eastern China could have a greater benefit for the regional air quality in China, especially in the winter haze season.

54 ENVIRONMENTAL SCIENCES↗

New Multi-group Transport Neutronics (PHISICS) Capabilities for RELAP5-3D and its Application to Phase I of the OECD/NEA MHTGR-350 MW Benchmark

PHISICS is a neutronics code system currently under development at the Idaho National Laboratory (INL). Its goal is to provide state of the art simulation capability to reactor designers. The different modules for PHISICS currently under development are a nodal and semi-structured transport core solver (INSTANT), a depletion module (MRTAU) and a cross section interpolation (MIXER) module. The INSTANT module is the most developed of the mentioned above. Basic functionalities are ready to use, but the code is still in continuous development to extend its capabilities. This paper reports on the effort of coupling the nodal kinetics code package PHISICS (INSTANT/MRTAU/MIXER) to the thermal hydraulics system code RELAP5-3D, to enable full core and system modeling. This will enable the possibility to model coupled (thermal-hydraulics and neutronics) problems with more options for 3D neutron kinetics, compared to the existing diffusion theory neutron kinetics module in RELAP5-3D (NESTLE). In the second part of the paper, an overview of the OECD/NEA MHTGR-350 MW benchmark is given. This benchmark has been approved by the OECD, and is based on the General Atomics 350 MW Modular High Temperature Gas Reactor (MHTGR) design. The benchmark includes coupled neutronics thermal hydraulics exercises that require more capabilities than RELAP5-3D with NESTLE offers. Therefore, the MHTGR benchmark makes extensive use of the new PHISICS/RELAP5-3D coupling capabilities. The paper presents the preliminary results of the three steady state exercises specified in Phase I of the benchmark using PHISICS/RELAP5-3D.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Higher order statistics of curvature perturbations in IFF model and its Planck constraints

We compute the power spectrum P{sub ζ} and non-linear parameters f{sub NL} and τ{sub NL} of the curvature perturbation induced during inflation by the electromagnetic fields in the kinetic coupling model (IFF model). By using the observational result of P{sub ζ},f{sub NL} and τ{sub NL} reported by the Planck collaboration, we study the constraint on the model comprehensively. Interestingly, if the single slow-rolling inflaton is responsible for the observed P{sub ζ}, the constraint from τ{sub NL} is most stringent. We also find a general relationship between f{sub NL} and τ{sub NL} generated in this model. Even if f{sub NL} ∼ O(1), a detectable τ{sub NL} can be produced.

79 ASTRONOMY AND ASTROPHYSICS↗

Responses of East Asian Summer Monsoon to Natural and Anthropogenic Forcings in the 17 Latest CMIP5 Models

In this study, we examined the responses of East Asian Summer Monsoon (EASM) to natural (solar variability and volcanic aerosols) and anthropogenic (greenhouse gasses and aerosols) forcings simulated in the 17 latest Coupled Model Intercomparison Program phase 5 (CMIP5) models with 105 realizations. The observed weakening trend of low-level EASM circulation during 1958-2001 is partly reproduced under all-forcing runs. A comparison of separate forcing experiments reveals that the aerosol-forcing plays a primary role in driving the weakened low-level monsoon circulation. The preferential cooling over continental East Asia caused by aerosol affects the monsoon circulation through reducing the land-sea thermal contrast and results in higher sea level pressure over northern China. In the upper-level, both natural-forcing and aerosol-forcing contribute to the observed southward shift of East Asian subtropical jet through changing the meridional temperature gradient.

anthropogenic forcings↗