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DOE OSTI2022

Hurricane‐Like Vortices in Conditionally Unstable Moist Convection

Abstract This study investigates the emergence of hurricane‐like vortices in idealized simulations of rotating moist convection. A Boussinesq atmosphere with simplified thermodynamics for phase transitions is forced by prescribing the temperature and humidity at the upper and lower boundaries. The governing equations are solved numerically using a variable‐density incompressible Navier‐Stokes solver with adaptive mesh refinement to explore the behavior of moist convection under a broad range of conditions. In the absence of rotation, convection aggregates into active patches separated by large unsaturated regions. Rotation modulates this statistical equilibrium state so that the self‐aggregated convection organizes hurricane‐like vortices. The warm and saturated air converges to the center of the vortices, and the latent heat released through the upwelling, forms the warm core structure. These hurricane‐like vortices share characteristics similar to tropical cyclones in the earth's atmosphere. The hurricane‐like vortices occur under conditionally unstable conditions where the potential energy given at the boundaries is large enough, corresponding to a moderate rate of rotation. This regime shares many similar characteristics to the tropical atmosphere indicating that the formation of intense meso‐scale vortices is a general characteristic of rotating moist convection. The model used here does not include any interactions with radiation, wind‐evaporation feedback, or cloud microphysics, indicating that, while these processes may be relevant for tropical cyclogenesis in the Earth atmosphere, they are not its primary cause. Instead, our results confirm that the formation and maintenance of hurricane‐like vortices involve a combination of atmospheric dynamics under the presence of rotation and of phase transitions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Using Ensemble Data Assimilation to Estimate Transient Hydrologic Exchange Flow Under Highly Dynamic Flow Conditions

Abstract Quantifying dynamic hydrologic exchange flows (HEFs) within river corridors that experience high‐frequency flow variations caused by dam regulations is important for understanding the biogeochemical processes at the river water and groundwater interfaces. Heat has been widely used as a tracer to infer steady‐state flow velocities through analytical solutions of heat transport defined by the diurnal temperature signals. Under sub‐daily dynamic flow conditions, however, such analytical solutions are not applicable due to the violation of their fundamental assumptions. In this study, we developed a data assimilation‐based approach to estimate the sub‐daily flux under highly dynamic flow conditions using multi‐depth temperature observations at a 5‐min resolution. If the hydraulic gradient is measured, Darcy's law was used to calculate the flux with permeability estimated from temperature responses below the riverbed. Otherwise, flux was estimated directly by assimilating multi‐depth temperature data at 1‐ or 2‐hr time intervals assuming one‐dimensional flow and heat transport governing equation. By comparing estimated fluxes with model‐generated synthetic truth, we demonstrated that both schemes have robust performance in estimating fluxes under highly dynamic flow conditions. This data assimilation‐based flux estimation method was able to capture the vertical sub‐daily fluxes using multi‐depth high‐resolution temperature data alone, even in the presence of multi‐dimensional flow. This approach has been successfully applied to real field temperature data collected at the Hanford site, which experiences highly dynamic HEFs. Our study shows the promise of adopting distributed 1‐D temperature monitoring to capture spatial and temporal exchange dynamics in river corridors at a watershed scale or beyond.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Aerosol‐Correlated Cloud Activation for Clean Conditions in the Tropical Atlantic Boundary Layer During LASIC

Abstract Aerosol measurements during the DOE ARM Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign were used to quantify the differences between clean and smoky cloud condensation nuclei (CCN) budgets. Accumulation‐mode particles accounted for ∼70% of CCN at supersaturations <0.3% in clean and smoky conditions. Aitken‐mode particles contributed <20% and sea‐spray‐mode particles <10% at supersaturations <0.3%, but at supersaturations >0.3% Aitken particles contributions increased to 30%–40% of clean CCN. For clean conditions, the Hoppel minimum diameter was correlated to the accumulation‐mode number concentration, indicating aerosol‐correlated cloud activation was controlling the lower diameter cutoff for which particles serve as CCN. For smoky conditions, the contributions of Aitken particles increase and the correlation of cloud activation to accumulation‐mode particles is masked by the lower‐hygroscopicity smoke. These results provide the first multi‐month in situ quantitative constraints on the role of aerosol number size distributions in controlling cloud activation in the tropical Atlantic boundary layer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Heterogeneity in Permeability and Particulate Organic Carbon Content Controls the Redox Condition of Riverbed Sediments at Different Timescales

Abstract The hydrological and biogeochemical properties of the hyporheic zone in stream and riverine ecosystems have been extensively studied over the past two decades. Although it is widely acknowledged that sediment heterogeneity can influence biogeochemical reactions, little effort has been made to understand the role of heterogeneity on the spatiotemporal variability of riverbed redox conditions under changing flow dynamics at different timescales. Here we integrate a mechanistic model and field data to demonstrate that heterogeneity in permeability plays a vital role in modulating sediment redox conditions at both seasonal (annual) and event (daily‐to‐weekly) timescales, whereas heterogeneity in particulate organic carbon (POC) content only has a comparable influence on redox conditions at the seasonal timescale. These findings underscore the importance of accurately characterizing sediment heterogeneity, in terms of permeability and POC content, in quantifying biogeochemical dynamics in the riverbed and hyporheic zones of riverine ecosystems.

Geology↗

DOE OSTI2025

Variability of Eastern North Atlantic Summertime Marine Boundary Layer Clouds and Aerosols Across Different Synoptic Regimes Identified With Multiple Conditions

Abstract This study estimates the meteorological covariations of aerosol and marine boundary layer (MBL) cloud properties in the eastern North Atlantic (ENA) region, characterized by diverse synoptic conditions. Using a deep‐learning‐based clustering model with mid‐level and surface daily meteorological data, we identify seven distinct synoptic regimes during the summer from 2016 to 2021. Our analysis, incorporating reanalysis data and satellite retrievals, shows that surface aerosols and MBL clouds exhibit clear regime‐dependent characteristics, whereas lower tropospheric aerosols do not. This discrepancy likely arises from synoptic regimes determined by daily large‐scale conditions, which may overlook air mass histories that predominantly dictate lower tropospheric aerosol conditions. Focusing on three regimes dominated by northerly winds, we analyze the Atmospheric Radiation Measurement Program (ARM) ENA observations on Graciosa Island in the Azores. In the subtropical anticyclone regime, fewer cumulus clouds and more single‐layer stratocumulus clouds with light drizzle are observed, along with the highest cloud droplet number concentration (Nd), surface cloud condensation nuclei (CCN) and surface aerosol levels. The post‐trough regime features more broken or multi‐layer stratocumulus clouds with slightly higher surface rain rate, and lower Nd and surface CCN levels. The weak trough regime is characterized by the deepest MBL clouds, primarily cumulus and broken stratocumulus clouds, with the strongest surface rain rate and the lowest Nd, surface CCN and surface aerosol levels, indicating strong wet scavenging. These findings highlight the importance of considering the covariation of cloud and aerosol properties driven by large‐scale regimes when assessing aerosol indirect effects using observations.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2011

Quantitative proteomic analyses of the response of acidophilic microbial communities to different pH conditions

Extensive genomic characterization of multi-species acid mine drainage microbial consortia combined with laboratory cultivation has enabled the application of quantitative proteomic analyses at the community level. In this study, quantitative proteomic comparisons were used to functionally characterize laboratory-cultivated acidophilic communities sustained in pH 1.45 or 0.85 conditions. The distributions of all proteins identified for individual organisms indicated biases for either high or low pH, and suggests pH-specific niche partitioning for low abundance bacteria and archaea. Although the proteome of the dominant bacterium, Leptospirillum group II, was largely unaffected by pH treatments, analysis of functional categories indicated proteins involved in amino acid and nucleotide metabolism, as well as cell membrane/envelope biogenesis were overrepresented at high pH. Comparison of specific protein abundances indicates higher pH conditions favor Leptospirillum group III, whereas low pH conditions promote the growth of certain archaea. Thus, quantitative proteomic comparisons revealed distinct differences in community composition and metabolic function of individual organisms during different pH treatments. Proteomic analysis revealed other aspects of community function. Different numbers of phage proteins were identified across biological replicates, indicating stochastic spatial heterogeneity of phage outbreaks. Additionally, proteomic data were used to identify a previously unknown genotypic variant of Leptospirillum group II, an indication of selection for a specific Leptospirillum group II population in laboratory communities. Our results confirm the importance of pH and related geochemical factors in fine-tuning acidophilic microbial community structure and function at the species and strain level, and demonstrate the broad utility of proteomics in laboratory community studies.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2015

Complex structural dynamics of nanocatalysts revealed in Operando conditions by correlated imaging and spectroscopy probes

Understanding how heterogeneous catalysts change size, shape and structure during chemical reactions is limited by the paucity of methods for studying catalytic ensembles in working state, that is, in operando conditions. Here by a correlated use of synchrotron X-ray absorption spectroscopy and scanning transmission electron microscopy in operando conditions, we quantitatively describe the complex structural dynamics of supported Pt catalysts exhibited during an exemplary catalytic reaction—ethylene hydrogenation. This work exploits a microfabricated catalytic reactor compatible with both probes. The results demonstrate dynamic transformations of the ensemble of Pt clusters that spans a broad size range throughout changing reaction conditions. Lastly, this method is generalizable to quantitative operando studies of complex systems using a wide variety of X-ray and electron-based experimental probes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2017

Thermonuclear reactions probed at stellar-core conditions with laser-based inertial-confinement fusion

Stars are giant thermonuclear plasma furnaces that slowly fuse the lighter elements in the universe into heavier elements, releasing energy, and generating the pressure required to prevent collapse. To understand stars, we must rely on nuclear reaction rate data obtained, up to now, under conditions very different from those of stellar cores. Here we show thermonuclear measurements of the 2 H(d, n) 3 He and 3 H(t,2n) 4 He S-factors at a range of densities (1.2–16 g cm –3 ) and temperatures (2.1–5.4 keV) that allow us to test the conditions of the hydrogen-burning phase of main-sequence stars. The relevant conditions are created using inertial-confinement fusion implosions at the National Ignition Facility. Here, our data agree within uncertainty with previous accelerator-based measurements and establish this approach for future experiments to measure other reactions and to test plasma-nuclear effects present in stellar interiors, such as plasma electron screening, directly in the environments where they occur.

42 ENGINEERING↗

DOE OSTI2016

State-conditional coherent charge qubit oscillations in a Si/SiGe quadruple quantum dot

Universal quantum computation requires high-fidelity single-qubit rotations and controlled two-qubit gates. Along with high-fidelity single-qubit gates, strong efforts have been made in developing robust two-qubit logic gates in electrically gated quantum dot systems to realise a compact and nanofabrication-compatible architecture. Here we perform measurements of state-conditional coherent oscillations of a charge qubit. Using a quadruple quantum dot formed in a Si/SiGe heterostructure, we show the first demonstration of coherent two-axis control of a double quantum dot charge qubit in undoped Si/SiGe, performing Larmor and Ramsey oscillation measurements. We extract the strength of the capacitive coupling between a pair of double quantum dots by measuring the detuning energy shift (≈75 μeV) of one double dot depending on the excess charge configuration of the other double dot. Finally, we further demonstrate that the strong capacitive coupling allows fast, state-conditional Landau–Zener–Stückelberg oscillations with a conditional π phase flip time of about 80 ps, showing a promising pathway towards multi-qubit entanglement and control in semiconductor quantum dots.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2017

Clay mineral formation under oxidized conditions and implications for paleoenvironments and organic preservation on Mars

Clay mineral-bearing locations have been targeted for martian exploration as potentially habitable environments and as possible repositories for the preservation of organic matter. Although organic matter has been detected at Gale Crater, Mars, its concentrations are lower than expected from meteoritic and indigenous igneous and hydrothermal reduced carbon. We conducted synthesis experiments motivated by the hypothesis that some clay mineral formation may have occurred under oxidized conditions conducive to the destruction of organics. Previous work has suggested that anoxic and/or reducing conditions are needed to synthesize the Fe-rich clay mineral nontronite at low temperatures. In contrast, our experiments demonstrated the rapid formation of Fe-rich clay minerals of variable crystallinity from aqueous Fe 3+ with small amounts of aqueous Mg 2+ . Furthermore, our results suggest that Fe-rich clay minerals such as nontronite can form rapidly under oxidized conditions, which could help explain low concentrations of organics within some smectite-containing rocks or sediments on Mars.

58 GEOSCIENCES↗

DOE OSTI2018

Uranium transport in acidic brines under reducing conditions

The behavior of uranium in environments, ranging from those of natural systems responsible for the formation of uranium deposits to those of nuclear reactors providing 11% of the world’s electricity, is governed by processes involving high-temperature aqueous solutions. It has been well documented that uranium is mobile in aqueous solutions in its oxidized, U 6+ state, whereas in its reduced, U 4+ state, uranium has been assumed to be immobile. Here, we present experimental evidence from high temperature (>100 °C) acidic brines that invalidates this assumption. Our experiments have identified a new uranium chloride species (UCl 4 °) that is more stable under reducing than oxidized conditions. Furthermore, these results indicate that uranium is mobile under reducing conditions and necessitate a re-evaluation of the mobility of uranium, particularly in ore deposit models involving this metal. Regardless of the scenario considered, reducing conditions can no longer be considered a guarantee of uranium immobility.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2018

Corrosion of the International Simple Glass under acidic to hyperalkaline conditions

Assessment of glass dissolution kinetics, under disposal relevant temperature and pH environments, is required to credibly estimate radionuclide release rates from vitrified radioactive waste. Leaching of the International Simple Glass (ISG) under acidic to hyperalkaline conditions was examined. Forward rate measurements have been obtained using the dynamic leaching SPFT protocol and rate parameters for B, Na and Si in the basic regime; errors in rates predicted using these parameters at high pH and temperature are significant because the fitting uses logarithmic data. Longer term behaviour under hyperalkaline conditions, representative of some disposal environments, was investigated using the PCT and MCC-1 static leaching protocols with Ca(OH) 2 solutions for up to 120 days (PCT) and 720 days (MCC-1). In hyperalkaline conditions dissolution was incongruent for all elements and the presence of alternating zirconia-rich and zirconia-poor alteration layers was viewed on all leached monoliths, indicating the occurrence of a self-organisation phenomenon during leaching.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Wind plants can impact long-term local atmospheric conditions

Abstract Long-term weather and climate observatories can be affected by the changing environments in their vicinity, such as the growth of urban areas or changing vegetation. Wind plants can also impact local atmospheric conditions through their wakes, characterized by reduced wind speed and increased turbulence. We explore the extent to which the wind plants near an atmospheric measurement site in the central United States have affected their long-term measurements. Both direct observations and mesoscale numerical weather prediction simulations demonstrate how the wind plants induce a wind deficit aloft, especially in stable conditions, and a wind speed acceleration near the surface, which extend $$\sim 30$$ ∼ 30 km downwind of the wind plant. Turbulence kinetic energy is significantly enhanced within the wind plant wake in stable conditions, with near-surface observations seeing an increase of more than 30% a few kilometers downwind of the plants.

17 WIND ENERGY↗

DOE OSTI2021

Soil texture and environmental conditions influence the biogeochemical responses of soils to drought and flooding

Abstract Climate change is intensifying the global water cycle, with increased frequency of drought and flood. Water is an important driver of soil carbon dynamics, and it is crucial to understand how moisture disturbances will affect carbon availability and fluxes in soils. Here we investigate the role of water in substrate-microbe connectivity and soil carbon cycling under extreme moisture conditions. We collected soils from Alaska, Florida, and Washington USA, and incubated them under Drought and Flood conditions. Drought had a stronger effect on soil respiration, pore-water carbon, and microbial community composition than flooding. Soil response was not consistent across sites, and was influenced by site-level pedological and environmental factors. Soil texture and porosity can influence microbial access to substrates through the pore network, driving the chemical response. Further, the microbial communities are adapted to the historic stress conditions at their sites and therefore show site-specific responses to drought and flood.

58 GEOSCIENCES↗

DOE OSTI2022

Genotype to ecotype in niche environments: adaptation of Arthrobacter to carbon availability and environmental conditions

Niche environmental conditions influence both the structure and function of microbial communities and the cellular function of individual strains. The terrestrial subsurface is a dynamic and diverse environment that exhibits specific biogeochemical conditions associated with depth, resulting in distinct environmental niches. Here, we present the characterization of seven distinct strains belonging to the genus Arthrobacter isolated from varying depths of a single sediment core and associated groundwater from an adjacent well. We characterized genotype and phenotype of each isolate to connect specific cellular functions and metabolisms to ecotype. Arthrobacter isolates from each ecotype demonstrated functional and genomic capacities specific to their biogeochemical conditions of origin, including laboratory-demonstrated characterization of salinity tolerance and optimal pH, and genes for utilization of carbohydrates and other carbon substrates. Analysis of the Arthrobacter pangenome revealed that it is notably open with a volatile accessory genome compared to previous pangenome studies on other genera, suggesting a high potential for adaptability to environmental niches.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Optimal thermodynamic conditions to minimize kinetic by-products in aqueous materials synthesis

Abstract Phase diagrams offer substantial predictive power for materials synthesis by identifying the stability regions of target phases. However, thermodynamic phase diagrams do not offer explicit information regarding the kinetic competitiveness of undesired by-product phases. Here we propose a quantitative and computable thermodynamic metric to identify synthesis conditions under which the propensity to form kinetically competing by-products is minimized. We hypothesize that thermodynamic competition is minimized when the difference in free energy between a target phase and the minimal energy of all other competing phases is maximized. We validate this hypothesis for aqueous materials synthesis through two empirical approaches: first, by analysing 331 aqueous synthesis recipes text-mined from the literature; and second, by systematic experimental synthesis of LiIn(IO 3 ) 4 and LiFePO 4 across a wide range of aqueous electrochemical conditions. Our results show that even for synthesis conditions that are within the stability region of a thermodynamic Pourbaix diagram, phase-pure synthesis occurs only when thermodynamic competition with undesired phases is minimized.

Wang, Zheren (ORCID:0000000227429451)↗

DOE OSTI2016

The influence of ns- and fs-LA plume local conditions on the performance of a combined LIBS/LA-ICP-MS sensor

Both laser-induced breakdown spectroscopy (LIBS) and laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) are well-established analytical techniques with their own unique advantages and disadvantages. The combination of the two analytical methods is a very promising way to overcome the challenges faced by each method individually. We made a comprehensive comparison of local plasma conditions between nanosecond (ns) and femtosecond (fs) laser ablation (LA) sources in a combined LIBS and LA-ICP-MS system. The optical emission spectra and ICP-MS signal were recorded simultaneously for both ns- and fs-LA and figures of merit of the system were analyzed. Characterization of the plasma was conducted by evaluating temperature and density of the plume under various irradiation conditions using optical emission spectroscopy, and correlations to ns- and fs-LIBS and LA-ICP-MS signal were made. The present study is very useful for providing conditions for a multimodal system as well as giving insight into how laser ablation plume parameters are related to LA-ICP-MS and LIBS results for both ns- and fs-LA.

LaHaye, Nicole L.↗

DOE OSTI2019

AuPd-nNiO as an effective catalyst for the base-free oxidation of HMF under mild reaction conditions

In this work, Au-Based catalysts supported on nanosized NiO (nNiO) were synthesized and were investigated in the oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) under base-free conditions using molecular oxygen as the oxidant, at 90 °C. By choosing the optimal composition of Au–Pd nanoparticles (6 : 4 Au/Pd atomic ratio), we report an efficient and stable nNiO-supported Au–Pd alloy catalyst. The presence of nNiO and Au–Pd nanoparticles on the surface was essential to achieve high conversion (95%) and high activity, high yield of FDCA (70%) and good level of stability. Significant synergistic effects were observed between Au and Pd in the alloy as well as on NiO. The present work provides mechanistic insights into the alloying effect and support-metal interaction in terms of understanding better the role of the alloy and support in affecting specific reaction pathways. Finally, the outcome of this knowledge can help develop efficient catalysts for the aerobic oxidation of biomass-derived molecules under base-free conditions in water and under mild reaction conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗