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DOE OSTI2020

Summertime Post-Cold-Frontal Marine Stratocumulus Transition Processes over the Eastern North Atlantic

Abstract Marine boundary layer (MBL) cloud morphology associated with two summertime cold fronts over the eastern North Atlantic (ENA) is investigated using high-resolution simulations from the Weather Research and Forecasting (WRF) Model and observations from the Atmospheric Radiation Measurement (ARM) ENA Climate Research Facility. Lagrangian trajectories are used to study the evolution of post-cold-frontal MBL clouds from solid stratocumulus to broken cumulus. Clouds within specified domains in the vicinity of transitions are classified according to their degree of decoupling, and cloud-base and cloud-top breakup processes are evaluated. The Lagrangian derivative of the surface latent heat flux is found to be strongly correlated with that of the cloud fraction at cloud base in the simulations. Cloud-top entrainment instability (CTEI) is shown to operate only in the decoupled MBL. A new indicator of inversion strength at cloud top that employs the vertical gradients of equivalent potential temperature and saturation equivalent potential temperature, which can be computed directly from soundings, is proposed as an alternative to CTEI. Overall, results suggest that the deepening–warming hypothesis suggested by Bretherton and Wyant explains many of the characteristics of the summertime postfrontal MBL evolution of cloud structure over the ENA, thereby widening the phase space over which the hypothesis may be applied. A subset of the deepening–warming hypothesis involving warming initially dominating over moistening is proposed. It is postulated that changes in climate change–induced modifications in cold-frontal structure over the ENA may be accompanied by coincident changes in the location and timing of MBL cloud transitions in the post-cold-frontal environment.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2023

Techno-economic Analysis of the Cryogenic Flux Capacitor Compared to Other forms of Hydrogen Production and Storage

The Cryogenic Flux Capacitor (CFC) is a cold, dense energy storage core that is being studied in the cryo-compressed, about 300 bar and 80K, region of gaseous hydrogen (GH2) storage and liquid hydrogen (LH2) region near the normal boiling point. The hydrogens storage is improved by physically bonding the molecules within the nanoscale pores of the aerogel composite blanket material. The process of bonding or debonding is governed by principles of physical adsorption (physisorption) and thermodynamics. The large surface area afforded by the nanoporous aerogel (~1,000 m2/g) allows its storage performance to easily exceed capacities of high-pressure GH2 storage for an equivalent volume. With the integrated aerogel, subscale tests have shown that storage is increased by about 49% over a simple tank filled with GH2 at the same operating temperature and pressure. For LH2 conditions, the CFC is shown to operate at equivalent densities. For the techno-economic analysis (TEA), the source of hydrogen is compared between onsite steam methane reforming (SMR) and onsite solar photovoltaic (PV) panels providing power to electrolyzers to produce GH2. The TEA compares pure hydrogen burning in a combined cycle gas turbine (CCGT) to hydrogen fuel cells with an overall net power output of 650 MW. The SMR system uses natural gas as an input and includes a carbon capture and storage (CCS) system. The levelized cost of electricity is developed based on the capital cost and operating cost of the systems. Sensitivities are discussed around the cost of natural gas, ranging from 1.93 USD per MMBTU to 6.75 USD per MMBTU, and carbon dioxide disposal, ranging from 7 USD per tonne to 10 USD per tonne. For comparison to the conventional CCGT baseline, a baseload scenario is adopted with 85% capacity factor. The results of the study show that onsite hydrogen generation from SMR is about 1 to 3 USD per kg over the life of the plant and the PV hydrogen production produces at 4 to 5 USD per kg. The cost of storage for CFC is compared to other systems, including high-pressure GH2 and atmospheric LH2. The system is shown to provide the lowest costs for all these options at the grid scale, due to its higher capacity than high-pressure GH2 and ability to operate at 80K, receiving refrigeration from liquid nitrogen systems reducing capital and operating costs when compared LH2 storage systems. SMR is competitive with CCGT at the gas prices, both of which have lower LCOE than the PV system. When accounting for variability in gas prices, the PV and electrolyzer system is less sensitive to these changes and provides the lowest LCOE across the whole range.

08 HYDROGEN↗

DOE OSTI2022

Surface chemistry on a polarizable surface: Coupling of CO with KTaO 3 (001)

Polarizable materials attract attention in catalysis because they have a free parameter for tuning chemical reactivity. Their surfaces entangle the dielectric polarization with surface polarity, excess charge, and orbital hybridization. How this affects individual adsorbed molecules is shown for the incipient ferroelectric perovskite KTaO 3 . This intrinsically polar material cleaves along (001) into KO- and TaO 2 -terminated surface domains. At TaO 2 terraces, the polarity-compensating excess electrons form a two-dimensional electron gas and can also localize by coupling to ferroelectric distortions. TaO 2 terraces host two distinct types of CO molecules, adsorbed at equivalent lattice sites but charged differently as seen in atomic force microscopy/scanning tunneling microscopy. Temperature-programmed desorption shows substantially stronger binding of the charged CO; in density functional theory calculations, the excess charge favors a bipolaronic configuration coupled to the CO. These results pinpoint how adsorption states couple to ferroelectric polarization.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Severe Dirac Mass Gap Suppression in Sb 2 Te 3 -Based Quantum Anomalous Hall Materials

The quantum anomalous Hall (QAH) effect appears in ferromagnetic topological insulators (FMTIs) when a Dirac mass gap opens in the spectrum of the topological surface states (SSs). Unaccountably, although the mean mass gap can exceed 28 meV (or ~320 K), the QAH effect is frequently only detectable at temperatures below 1 K. Using atomic-resolution Landau level spectroscopic imaging, we compare the electronic structure of the archetypal FMTI Cr 0.08 (Bi 0.1 Sb 0.9 ) 1.92 Te 3 to that of its nonmagnetic parent (Bi 0.1 Sb 0.9 ) 2 Te 3 , to explore the cause. In (Bi 0.1 Sb 0.9 ) 2 Te 3 , we find spatially random variations of the Dirac energy. Statistically equivalent Dirac energy variations are detected in Cr 0.08 (Bi 0.1 Sb 0.9 ) 1.92 Te 3 with concurrent but uncorrelated Dirac mass gap disorder. Additionally, these two classes of SS electronic disorder conspire to drastically suppress the minimum mass gap to below 100 μeV for nanoscale regions separated by <1 μm. This fundamentally limits the fully quantized anomalous Hall effect in Sb 2 Te 3 -based FMTI materials to very low temperatures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Experimental measurement of the rapid mixing of fuel and air in a multi-element diffusion (Hencken) burner

Flat flame burners are valuable tools for studying complex combustion phenomena like particle synthesis due to the well-controlled and well-behaved initial and boundary conditions. In this study, the methane/air flame temperature and tracer density profiles of a multi-element diffusion burner equipped with a central tube were characterized using krypton (Kr) x-ray fluorescence at the Advanced Photon Source at Argonne National Laboratory. The experiments were performed using a fuel-to-oxygen equivalence ratio of 0.8 and 3.3% Kr by volume was added to the reactant gases. One- and two-dimensional scans of non-combusting (i.e., cold flow) and combusting conditions, both with and without flow through the central tube were performed. Spatially-resolved Kr number density profiles were obtained at different planar locations and heights above the surface of the burner. The results show rapid mixing occurred near the exit-plane of the burner and increased spatial uniformity was achieved from 0.1 mm to 0.5 mm above the surface of the burner. Further, the data also showed the impact of the central tube flow on the main methane/air flame, including evidence of the central tube flow mixing with the main flow. Flame temperatures were calculated from the fluorescence measurements at various heights above the burner surface and were in good agreement with model predictions for a burner stabilized flame. These high-fidelity measurements provide accurate baseline data that are particularly valuable for understanding the effects of fuel and air mixing on downstream phenomena, such as the formation of condensed-phase products.

42 ENGINEERING↗

DOE OSTI2026

Evapotranspiration partitioning estimates from 8 methods from 47 NEON sites, 2019-2021

This dataset provides daily estimates of evapotranspiration (ET) and the transpiration-to-evapotranspiration ratio (T/ET) across 47 terrestrial National Ecological Observatory Network (NEON) sites spanning diverse environmental and biome conditions in the United States across three years of data (2019-2021). Daily ET is reported in both energy units (MJ m⁻² day⁻¹) and equivalent water depth (mm day⁻¹), assuming a constant latent heat of vaporization of 2.45 MJ/kg. The primary method uses a hybrid recurrent neural network–Penman–Monteith framework (RNN-PM), which integrates physically based surface energy balance constraints with data-driven learning to partition ET into transpiration and evaporation components. Model inputs include in situ meteorological observations (air temperature, vapor pressure deficit, wind speed, and radiation) combined with satellite-derived land surface temperature, leaf area index, and soil moisture. For benchmarking and uncertainty assessment, T/ET estimates from seven additional models are included: Priestley-Taylor Jet Propulsion Laboratory (PT-JPL), Penman-Monteith (P-M), Two-Source Energy Balance (TSEB), Support Vector Regression (SVR), and Categorical Boosting (CatBoost), among others—spanning empirical, machine-learning, and process-based approaches (see methods section or linked publication for detailed descriptions). Data Package Contents: The dataset a csv files containing daily ET and T/ET estimates for each site and model, along with associated metadata files these variables. Data can be accessed using common spreadsheet software (e.g., Microsoft Excel, LibreOffice) or programming environments such as R or Python. Together, these data support cross-site comparisons of ecosystem water use, evaluation of ET partitioning methods, and development of improved land–atmosphere exchange models.

EARTH SCIENCE > ATMOSPHERE↗

DOE OSTI2023

A novel method for quantifying irradiation damage in nuclear graphite using Raman spectroscopy

Raman spectroscopy has long been used in studying irradiation damage in carbon/graphite materials. It is however unclear if the measurements from different types of materials are directly comparable. Further, decoupling the contribution from irradiation temperature and fluence to the total damage in nuclear graphite possessing irradiation damage gradient is currently not readily feasible as it requires a complete set of test reactor irradiation experiments over the relevant temperature and fluence range. A novel methodology has therefore been proposed and developed to quantify total irradiation damage evolution at crystal level based on graphite Raman G-band position shift. Specifically, G-band positions derived from a large number of spectra collected from the fractured surface of microfine-grained POCO ZXF-5Q graphite possessing proton irradiation damage gradient were plotted with open literature Raman data on HOPG, BEPO (AXGP graphite), PCEA and IG-110 graphite as a function of dpa. The total damage level within 2σ beam radius in this POCO graphite was estimated to be equivalent to ~2–5 dpa at ~350–370 °C. Derived G-band positions were then mapped to the three-stage amorphization trajectory model indicating beam centre area has entered the second stage, i.e., transitioning from nanocrystalline graphite into amorphous carbon. G-band position relative shift (ΔG) curve with a ‘turn-around’ peak as a function of total damage can be used for in-service lifetime prediction. Importantly, the developed methodology has the potential to ‘unify’ total damage levels across different grades of nuclear graphite caused by ion, neutron and proton irradiation at different temperatures.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

Low temperature hydrogen plasma permeation in palladium and its alloys for fuel recycling in fusion systems

Superpermeation of hydrogen isotopes through metal foils is a critical component for efficient fuel recycling in fusion power systems. In that context hydrogen permeation through foils of palladium and its alloys with silver and copper was studied at low temperature (60 - 200°C) under plasma exposure. These alloys differ significantly in both bulk and surface properties, and comparisons can provide mechanistic insights. Here, permeation was observed only during plasma operation, confirming the negligible contribution of molecular hydrogen to the observed flux. As-received foils required surface treatment to achieve top performance. For Pd and Pd75Ag25 an oxidation treatment increased permeation an order of magnitude, but proved unstable as this desirable surface was reduced under hydrogen plasma exposure. In contrast, an Ar plasma cleaning step provided both high and stable flux. As-received FCC phase Pd60Cu40 foils required annealing to transform it into the high permeability BCC phase that delivered top performance. All foils displayed similar temperature dependence with flux declining with temperature, suggesting that the primary rate-limiting step is absorption of superthermal hydrogen. Among these foils the hydrogen flux through PdCu was 3 - 5X greater than that of Pd or PdAg, which were similar. The superiority of BCC PdCu is attributed to its superior hydrogen desorption kinetics. Using PdCu 100% permeation of supplied hydrogen was achieved, and the flux saturated with increasing plasma power at values >10 –2 mol H•m –2 •s– 1 , and under these conditions permeation rates are equivalent with or without the membrane present. The fluxes achieved are the highest reported to date at these conditions, and the results highlight the important roles of both surface and bulk properties.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

The Phase-Locking of Tropical North Atlantic and the Contribution of ENSO

The Tropical North Atlantic (TNA) is characterized by significant interannual variability in sea surface temperature (SST), which is phase-locked to the boreal spring. In this study, the phase-locking of TNA is investigated by adopting a linear stochastic-dynamical model (SDM) using seasonally modulated TNA feedbacks together with the seasonal modulation of ENSO forcing. In the observations, the role of local TNA feedbacks and ENSO forcing in TNA phase-locking are equivalently important with both preferring the peak of TNA variability to appear in the boreal spring. Besides, the seasonal modulation of TNA feedbacks and ENSO forcing strength are both mainly controlled by thermodynamic processes. In most climate models, the contribution of ENSO on TNA phase-locking is weaker than that in observations. The strength of ENSO-related TNA phase-locking is highly correlated with the relationship between ENSO and TNA, which is mainly determined by the amplitude of ENSO and its teleconnection patterns.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Gridded daily weather data for North America with comprehensive uncertainty quantification

Abstract Access to daily high-resolution gridded surface weather data based on direct observations and over long time periods is essential for many studies and applications including vegetation, wildlife, soil health, hydrological modelling, and as driver data in Earth system models. We present Daymet V4, a 40-year daily meteorological dataset on a 1 km grid for North America, Hawaii, and Puerto Rico, providing temperature, precipitation, shortwave radiation, vapor pressure, snow water equivalent, and day length. The dataset includes an objective quantification of uncertainty based on strict cross-validation analysis for temperature and precipitation results. The dataset represents several improvements from a previous version, and this data descriptor provides complete documentation for updated methods. Improvements include: reductions in the timing bias of input reporting weather station measurements; improvement to the three-dimensional regression model techniques in the core algorithm; and a novel approach to handling high elevation temperature measurement biases. We show cross-validation analyses with the underlying weather station data to demonstrate the technical validity of new dataset generation methods, and to quantify improved accuracy.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Multimerization of Ebola GPΔmucin on protein nanoparticle vaccines has minimal effect on elicitation of neutralizing antibodies

Ebola virus (EBOV), a member of the Filoviridae family of viruses and a causative agent of Ebola Virus Disease (EVD), is a highly pathogenic virus that has caused over twenty outbreaks in Central and West Africa since its formal discovery in 1976. The only FDA-licensed vaccine against Ebola virus, rVSV-ZEBOV-GP (Ervebo®), is efficacious against infection following just one dose. However, since this vaccine contains a replicating virus, it requires ultra-low temperature storage which imparts considerable logistical challenges for distribution and access. Additional vaccine candidates could provide expanded protection to mitigate current and future outbreaks. Here, we designed and characterized two multimeric protein nanoparticle subunit vaccines displaying 8 or 20 copies of GPΔmucin, a truncated form of the EBOV surface protein GP. Single-dose immunization of mice with GPΔmucin nanoparticles revealed that neutralizing antibody levels were roughly equivalent to those observed in mice immunized with non-multimerized GPΔmucin trimers. These results suggest that some protein subunit antigens do not elicit enhanced antibody responses when displayed on multivalent scaffolds and can inform next-generation design of stable Ebola virus vaccine candidates.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2024

Materials descriptors for advanced water dissociation catalysts in bipolar membranes

The voltage penalty driving water dissociation (WD) at high current density is a major obstacle in the commercialization of bipolar membrane (BPM) technology for energy devices. Here, in this study, we show that three materials descriptors, that is, electrical conductivity, microscopic surface area and (nominal) surface-hydroxyl coverage, effectively control the kinetics of WD in BPMs. Using these descriptors and optimizing mass loading, we design new earth-abundant WD catalysts based on nanoparticle SnO 2 synthesized at low temperature with high conductivity and hydroxyl coverage. These catalysts exhibit exceptional performance in a BPM electrolyser with low WD overvoltage (η wd ) of 100 ± 20 mV at 1.0 A cm -2 . The new catalyst works equivalently well with hydrocarbon proton-exchange layers as it does with fluorocarbon-based Nafion, thus providing pathways to commercializing advanced BPMs for a broad array of electrolysis, fuel-cell and electrodialys is applications.

Sasmal, Sayantan↗

DOE OSTI2021

Effect of the Addition of a Low Equivalent Stress Mechanism to the Analysis of Geomechanical Behavior of the SPR West Hackberry Site

Sandia National Laboratories has long used the Munson-Dawson (M-D) model to predict the geomechanical behavior of salt caverns used to store oil at the Strategic Petroleum Reserve (SPR). Salt creep causes storage caverns to deform inward, thus losing volume. This loss of volume affects the salt above and around the caverns, puts stresses and strains on borehole casings, and creates surface subsidence which affects surface infrastructure. Therefore, accurate evaluation of salt creep behavior drives decisions about cavern operations. Parameters for the M-D model are typically fit against laboratory creep tests, but nearly all historic creep tests have been performed at equivalent stresses of 8 MPa or higher. Creep rates at lower equivalent stresses are very slow, such that tests take months or years to run, and the tests are sensitive to small temperature perturbations (<0.1°C). A recent collaboration between US and German researchers, recently characterized the creep behavior at low equivalent (deviatoric) stresses (<8 MPa) of salt from the Waste Isolation Pilot Plant. In addition, the M-D model was recently extended to include a low stress creep “mechanism”. This paper details new simulations of SPR caverns that use this extended M-D model, called the M-D Viscoplastic model. The results show that the inclusion of low stress creep significantly alters the prediction of steady-state cavern closure behavior and indicate that low stress creep is the dominant displacement mechanism at the dome scale. The implications for evaluating cavern and well integrity are demonstrated by investigating three phenomena: the extent of stress changes around the cavern; the predicted vertical strains applied to wellbore casings; and the evaluation of oscillating stress changes around the cavern due to oil sale cycles and their potential effect on salt fatigue.

58 GEOSCIENCES↗

DOE OSTI2020

Modeling Nondestructive Defect Detection in Additively Manufactured Metallic Structures for Nuclear Applications

The future of quickly, economically produced metallic nuclear reactor parts with minimal supply-chain dependence lies in Laser Powder Bed Fusion (LPBF) Additive Manufacturing (AM): a 3D printing method involving laser melting and net shaping stainless steel and Inconel metallic powder into a solid structure. However, intrinsic features in LPBF frequently leads to the formation of materials defects, such as pores, within 3D printed structures. As safe long-term use in energy applications requires knowledge of all relevant defects before deployment in a reactor, we must develop methods for nondestructive detection of these defects. We are investigating Pulsed Thermal Tomography (PTT), which is a non-contact nondestructive imaging method scalable to arbitrary structure size. Thermal tomography (TT) is a computational method for 3D spatial reconstruction of material thermal effusivity from flash or pulsed thermography temperature data cube. Thermography data cube consists of 2D surface temperature measurements at different times. The objective of the present work is to investigate limits on defect detection in AM metallic structures with PTT. To this effect, we modeled PTT with COMSOL heat transfer computer simulations. We developed a layered media COMSOL simulation consisting of a Stainless Steel 316 (SS316) plate with an internal layer of un-sintered SS316 powder. Thermophysical properties of the powder layer were modeled with equivalent volume mixing model. To account for partial sintering at the boundary of the defect, the transition between solid and powder layers was modeled as a Gaussian. Using data from COMSOL simulations, we reconstructed depth-dependent thermal effusivity, which allowed defect visibility estimation. A series of parametric studies determined that at 1mm depth, 50µm is the smallest detectable defect. In addition, classification of the defects which can lead to early fatigue of the metallic structure in a reactor is briefly discussed.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2024

NPFTURBULENCE: Best Estimate Aerosol Size Distribution by airborne measurements

The original data were collected during the field campaign of “Turbulent layers promoting New Particle Formation” experiment (NPFTURBULENCE; https://www.arm.gov/research/campaigns/aaf2024npfturbulence) over the Atmospheric Radiation Measurement (ARM) Southern Great Plains (SGP) Atmospheric Observatory (https://www.arm.gov/capabilities/observatories/sgp ) in north-central Oklahoma. The ARM Aerial Facility ArcticShark uncrewed aerial system (UAS) was based at Blackwell–Tonkawa Municipal Airport (IATA: BWL, ICAO: KBKN, FAA LID: BKN, 36.74475° N, 97.34918° W, 313.9 m MSL), for the field campaign from May 5 through May 29, 2024. The ArcticShark UAS performed 11 flights, including 10 research flights over the Central Facility of the ARM SGP to measure atmospheric state, turbulence, surface IT temperature and imagery, aerosol number concentration and size distribution. The current data set presents Best Estimate Aerosol Size Distribution: a merged aerosol size distribution composed of the data from 2 sensors: miniaturized Scanning Electrical Mobility Sizer (mSEMS) and Portable Optical Particle Spectrometer (POPS). The mSEMS data were interpolated to 1 second from “native” time resolution of about 15 second to match the other probe. The POPS data were converted from equivalent optical size into geometric size using value of aerosol refractive index of 1.477 from the HISCALE field campaign (same geographical area, altitudes, and time of year; http://www.arm.gov/campaigns/aaf2016hiscale ).

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Oxidation and recharge of reactive structural Fe( II ) in titanomagnetite (Fe 3− x Ti x O 4 ) nanoparticles

Mixed-valent iron oxide minerals, such as magnetite (Fe(II)(Fe(III)) 2 O 4 ), are an important source of solid-state ferrous iron (Fe(II)) that can impact the speciation and transport of electron accepting contaminants in the Earth’s subsurface, such as radioactive pertechnetate ( 99 Tc(VII)O 4 − ). However, when oxidizing conditions are encountered, structural Fe(II) at the mineral surface is consumed yielding a maghemite (γ-Fe(III) 2 O 3 )-like layer that limits further electron transfer. This oxidized surface layer can be recharged back to the original Fe(II)/(III) ratio by re-exposure to reducing conditions, i.e., aqueous solutions containing Fe 2+ . However, for substituted magnetite (Fe 3−x M x O 4 , M = transition metal cation), the extent of this redox recyclability is unclear. Here, we examine oxidation and recharge for titanomagnetite (Fe 3−x Ti x O 4 ) nanoparticles, where the Fe(II)/Fe(III) ratio varies by the amount of Fe(II) required to charge balance the titanium (Ti(IV)) substituted into the structure. The nanoparticles were synthesized by aqueous precipitation from a solution containing ferrous, ferric and titanium chloride at room temperature. Transmission electron microscopy combined with electron energy loss spectroscopy revealed that rapid precipitation formed core–shell-like nanoparticles consisting of a hyperstoichiometric magnetite core, with Ti(IV) and charge balancing Fe(II) enriched at the surface. This surface enrichment made Fe(II) more available for electron transfer reactions with redox active solution species. Examination of oxidation by H 2 O 2 followed by recharge with aqueous Fe 2+ indicates recyclability of reducing equivalents in the nanoparticles, yielding a core recrystallized to stoichiometric magnetite and a shell bearing excess Fe(II) to charge balance the substituted Ti(IV). The recharged particles are shown to have restored redox reactivity with 99 Tc(VII)O 4 − resulting in reduction to 99 Tc(IV)O 2 and oxidation of the structural Fe(II) to Fe(III).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Significant impact of forcing uncertainty in a large ensemble of climate model simulations

Forcing due to solar and volcanic variability, on the natural side, and greenhouse gas and aerosol emissions, on the anthropogenic side, are the main inputs to climate models. Reliable climate model simulations of past and future climate change depend crucially upon them. Here we analyze large ensembles of simulations using a comprehensive Earth System Model to quantify uncertainties in global climate change attributable to differences in prescribed forcings. The different forcings considered here are those used in the two most recent phases of the Coupled Model Intercomparison Project (CMIP), namely CMIP5 and CMIP6. We show significant differences in simulated global surface air temperature due to volcanic aerosol forcing in the second half of the 19th century and in the early 21st century. The latter arise from small-to-moderate eruptions incorporated in CMIP6 simulations but not in CMIP5 simulations. We also find significant differences in global surface air temperature and Arctic sea ice area due to anthropogenic aerosol forcing in the second half of the 20th century and early 21st century. These differences are as large as those obtained in different versions of an Earth System Model employing identical forcings. In simulations from 2015 to 2100, we find significant differences in the rates of projected global warming arising from CMIP5 and CMIP6 concentration pathways that differ slightly but are equivalent in terms of their nominal radiative forcing levels in 2100. Our results highlight the influence of assumptions about natural and anthropogenic aerosol loadings on carbon budgets, the likelihood of meeting Paris targets, and the equivalence of future forcing scenarios.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Molecular beam epitaxy growth and characterization of GePb alloys

Pb based group-IV alloys such as GePb have been gaining interest as a potential alternative for infrared detectors, quantum materials, and high-speed electronic devices. Challenges remain in their growth due to the extremely low solid solubility of Pb in the Ge–Pb system. This paper reports molecular beam epitaxy growth of GePb alloy thin films on Ge(100) substrates. Effusion cells of Ge and Pb are used to control the flux ratio independently. The optimal substrate temperature is found to be near the thermocouple temperature of 300 °C based on the characterization of the grown films using high-resolution x-ray diffraction. A large change in the Ge:Pb beam equivalent pressure ratio from 10:1 to 1:1 results in only a minimal increase of the Pb composition from 0.74% to 2.84% as estimated from Raman spectroscopy and Rutherford backscattering spectrometry. Furthermore, scanning electron microscopy images show a large volume of Pb islands on the surface that form into either long trapezoidal rods or uniform droplets, with increasing Pb flux and growth time the density of Pb islands increased.

36 MATERIALS SCIENCE↗