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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

The Advantages of Combining Morphological and Molecular Methods to Characterise Zooplankton Communities: A Case Study of the UNESCO Biosphere Reserve of the Berlengas Archipelago, Portugal

Understanding the ecological dynamics of zooplankton communities is crucial to precisely assessing the health of marine ecosystems and their management. Metabarcoding has contributed to a better understanding of biodiversity in marine environments. However, this methodology still requires protocol optimisation. Here, we used a complementary approach combining molecular and morphological identification methods to identify the zooplankton community inhabiting the Berlengas Archipelago, Portugal. The presence of non-indigenous species was also assessed. The results showed that the metabarcoding approach outperformed the classical morphological identification method, detecting more species with higher resolution. Nevertheless, the classical method was able to identify species that were not detected by the molecular approaches, probably due to a lack of reference data in the databases. The comparison between different molecular approaches showed that COI and bulk DNA gave better results than 18S rRNA and eDNA by detecting higher species diversity. However, complementarities were observed between them. Molecular tools also proved effective in identifying several potential non-indigenous species, identifying, for the first time, several potentially unreported NIS inhabiting the Portuguese marine ecosystems. Overall, our results confirmed the importance of combining both classical and molecular methods to obtain a more refined assessment of the zooplanktonic communities in marine environments.

Simões, Marco (ORCID:0000000179957304)↗
DOE OSTI2025

Persistence of bacterial-mediated anti-rotifer protection in preliminary outdoor cultivation trial for Microchloropsis salina

Outdoor algal cultivation systems are susceptible to a wide variety of deleterious species. In previously published studies, we observed protection using microbial consortia at laboratory scale cultures; Microchloropsis salina in the presence of microbial consortia were protected from grazing from the marine rotifer, Brachionus plicatilis. Our objective for the present work was to determine if this protection conferred by microbial consortia in controlled laboratory experiments would persist in an open, outdoor multi-liter cultivation system. We found that algal protection did persist as evidenced by the presence of fewer motile rotifers and decreased rotifer-associated egg counts for the consortia-treated outdoor cultures. Due to the low temperature and light conditions that reduced growth of the algae outdoors, we performed an indoor laboratory assay which also confirmed the persistence of algal protection. Lastly, the lower numbers of motile rotifers and fewer rotifer-associated eggs in the consortia-treated algal cultures suggests a possible protective mechanism by the consortia through interfering with the rotifer lifecycle or reproduction. Finally, these initial results support the possibility that low cost, prophylactic treatments with microbial consortia can protect algae from deleterious species in outdoor cultivation systems.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Cloud processing of dimethyl sulfide (DMS) oxidation products limits sulfur dioxide (SO 2 ) and carbonyl sulfide (OCS) production in the eastern North Atlantic marine boundary layer

Dimethyl sulfide (DMS) is the major sulfur species emitted from the ocean. The gas-phase oxidation of DMS by hydroxyl radicals proceeds through the stable, soluble intermediate hydroperoxymethyl thioformate (HPMTF), eventually forming carbonyl sulfide (OCS) and sulfur dioxide (SO 2 ). Recent work has shown that HPMTF is efficiently lost to marine boundary layer (MBL) clouds, thus arresting OCS and SO 2 production and their contributions to new-particle formation and growth events. To date, no long-term field studies exist to assess the extent to which frequent cloud processing impacts the fate of HPMTF. Here, we present 6 weeks of measurements of the cloud fraction and the marine sulfur species methanethiol, DMS, and HPMTF made at the Atmospheric Radiation Measurement (ARM) research facility on Graciosa Island, Azores, Portugal. Using an observationally constrained chemical box model, we determine that cloud loss is the dominant sink of HPMTF in this region of the MBL during the study, accounting for 79 %–91 % of HPMTF loss on average. When accounting for HPMTF uptake to clouds, we calculate campaign average reductions in DMS-derived MBL SO 2 and OCS of 52 %–60 % and 80 %–92 % for the study period. Using yearly measurements of the site- and satellite-measured 3D cloud fraction and DMS climatology, we infer that HPMTF cloud loss is the dominant sink of HPMTF in the eastern North Atlantic during all seasons and occurs on timescales faster than what is prescribed in global chemical transport models. Accurately resolving this rapid loss of HPMTF to clouds has important implications for constraining drivers of MBL new-particle formation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Are Marine Low Cloud Droplet Concentrations Buffered by Entrained Aitken‐Mode Aerosol (Final Technical Report)

During the summertime, the high-latitude oceans come to life with green phytoplankton, which gain their energy from sunlight and are food for sea creatures small and large. When the phytoplankton are eaten or die, sulfur-rich gases are released under the ocean surface and mix into the air. Observations suggest that, over the Southern Ocean, frequent storms lift this air high into the atmosphere while raining out particulates like salt. As a result, the sulfur-rich air then spawns high concentrations of small ‘Aitken-mode’ aerosol particles. We hypothesize that these particles work their way down into the marine boundary layer, where they can replenish the supply of cloud-condensation nuclei scavenged by frequent precipitation. Further, this process maintains high concentrations of liquid cloud droplets in austral summer, promoting more sunlight to be reflected to space. We call this ‘Aitken buffering’. The primary objective of this project has been to document and test what role Aitken-mode aerosols play in clouds over the Southern Ocean and elsewhere. This effort has included three main components: 1) developing a computer model that realistically simulates the aerosol processes and the small-scale turbulent air motions that move aerosols around and create the clouds, 2) using that model to interpret and extend these observations for process understanding, by allowing different factors that contribute to the aerosol budget, such as surface wind speed, precipitation, surface gas exchange, etc. to be separated, and 3) studying Aitken-mode aerosol and its variability with a focus over the Southern Ocean and Antarctica, using data from Atmospheric Radiation Measurement (ARM) sites and other available observations. Initial computer studies in more idealized conditions found that elevated concentrations of Aitken-mode aerosols above the clouds could help prevent the breakup of those clouds by acting as cloud-condensation nuclei after they were entrained into the cloudy boundary layer. Simulations of a day during the ACE-ENA field campaign showed that Aitken-mode aerosols could also prevent cloud breakup under more realistic conditions. A new method that extracts information about Aitken-mode aerosols from measurements of aerosols onto which cloud droplets can form finds that Aitken-mode aerosols do vary seasonally over the Southern Ocean, with a peak in summertime, as described above. Other work during this project has focused on understanding how patterns of water vapor, clouds and precipitation are coupled within low-lying clouds over the oceans, and also on how cloud droplets cluster within clouds and how the distribution of cloud droplet sizes change as dry air is mixed into clouds, with the latter studies also using observations from ACE-ENA.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Baselining the Indirect Effect by Improving Quantification of Sea Spray and Marine Sources at Ascension Island (Final Report)

Oceans cover two-thirds of the Earth and understanding the interactions of aerosols with clouds in these large marine regions requires quantifying the man-made contributions to the budget of cloud-drop forming particles (known as cloud condensation nuclei, or CCN) relative to the non-manmade “baseline” conditions and understanding the meteorology of boundary layer clouds. Modeling studies have shown substantial uncertainties and sensitivities to natural marine CCN sources, meaning that to reduce uncertainties in indirect effects we must be able to better quantify the CCN budget in ocean regions. While models provide important constraints on these uncertainties, actually reducing uncertainties requires substantial observations in open-ocean and coastal regions in order to establish the baseline on which manmade emissions are added. The tropical South Atlantic Ocean is one of the least-sampled regions of the planet, making the comprehensive measurements of the Department of Energy Atmospheric Radiation Measurement Layered Atlantic Smoke Interactions with Clouds (LASIC) campaign provides the longest record of aerosol size distribution measurements from a differential mobility analyzer in a cloud-influenced marine location in the ARM database, with 17 months of ground-based aerosol size distribution measurements. This project addressed the research topic of Aerosol-Cloud Interactions (ACI) by supporting three publications from the LASIC measurements: 1. The ARM measurements were combined with a new value-added technique that was pioneered by the Russell group for quantifying sea salt. This quantification of sea salt uses supermicron scattering measurements for retrieving reasonable sea spray mass concentrations, providing the best-available, observationally-constrained estimate of the sea spray mode properties when supermicron size distribution measurements are not available. 2. The fitted modes of the distribution were used to investigate the signatures of cloud processing for very clean to very smoky aerosol conditions, revealing not only differences in the particles that activate in clouds but also in the mechanisms that control that droplet formation process. In clean air, the size required to form a cloud droplet is influenced by the number of particles, as well as how quickly particles take up water during growth in cloud. 3. Building on this aerosol characterization, cloud and meteorological conditions were used to evaluate aerosol-related changes in cloud albedo and optical depth. We introduced a new method of decomposing the impact of aerosols on clouds known as the Twomey effect by incorporating retrieved supersaturation from two independent sets of observations to constrain the feedback of aerosol particles on cloud properties. The method quantifies the reduction of the Twomey effect at high aerosol concentrations, which has never been explained quantitatively by observations. In addition, the results provide the first direct validation for the conditions observed in the tropical South Atlantic of a parcel-based approach that is embedded in many climate models. Together these findings illustrate how ARM extended field campaigns in stratocumulus-covered regions can be used to constrain ACI processes with direct observations, providing specific radiative effects without models. By making such process-specific constraints available to improve ACI in global climate models, ARM observations play a key role in supporting model development.

58 GEOSCIENCES↗
DOE OSTI2021

Experimental and theoretical determinations of hydrogen isotopic equilibrium in the system CH 4 —H 2 —H 2 O from 3 to 200°C

The stable isotopic composition of methane (CH 4 ) is commonly used to fingerprint natural gas origins. Over the past 50 years, there have been numerous proposals that both microbial and thermogenic CH 4 can form in or later attain hydrogen isotopic equilibrium with water (H 2 O) and carbon isotopic equilibrium with carbon dioxide (CO 2 ). Evaluation of such proposals requires knowledge of the equilibrium fractionation factors between CH 4 and H 2 O or CO 2 at the temperatures where microbial and thermogenic CH 4 form in or are found in the environment, which is generally less than 200°C. Experimental determinations of these fractionation factors are only available above 200°C, requiring extrapolation of these results beyond the calibrated range or the use of theoretical calculations at lower temperatures. Here, we provide a calibration of the equilibrium hydrogen isotopic fractionation factor for CH 4 and hydrogen gas (H 2 ) ( D α CH4(g)–H2(g) ) based on experiments using γ-Al 2 O 3 and Ni catalysts from 3 to 200°C. Results were regressed as a 2 nd order polynomial of 1000 × ln D α CH4(g)–H2(g) vs. 1/T (K -1 ) yielding: 1000 × l n D α C H 4 ( g ) - H 2 ( g ) = 3.5317 × 10 7 T 2 + 2.7749 × 10 5 T - 179.48 We combine this calibration with previous experimental determinations of hydrogen isotope equilibrium between H 2 , H 2 O(g), and H 2 O(l) and we provide an interpolatable experimental calibration of 1000 × ln D α CH4(g)–H2O(l) from 3 to 200°C. Our resulting 4th order polynomial is the following equation: 1000 × l n D α C H 4 ( g ) - H 2 O l = - 7.9443 × 10 12 T 4 + 8.7772 × 10 10 T 3 - 3.4973 × 10 8 T 2 + 5.4398 × 10 5 T - 382.05 At 3°C, the value from our calibration differs by 93‰ relative to what would be calculated based on the extrapolation of the only experimental calibration currently available to temperatures below its calibrated range (lowest temperature of 200°C; Horibe and Craig, 1995). We additionally provide new theoretical estimates of hydrogen isotopic equilibrium between CH 4 (g), H 2 (g), and H 2 O(g) and carbon isotopic equilibrium between CH 4 (g) and CO 2 (g) using Path Integral Monte Carlo (PIMC) calculations. Our PIMC calculations for hydrogen isotopic equilibrium between CH 4 and H 2 agree 1:1 with our experiments. Finally, we compile carbon and hydrogen isotopic measurements of CH 4 , CO 2 , and H 2 O from various environmental systems and compare observed differences between carbon and hydrogen isotopes to those expected based on isotopic equilibrium. We find that isotopic compositions of some microbial gases from marine sedimentary, coalbed, and shale environments are consistent with those expected for CH 4 H 2 O(l) hydrogen and CH 4 CO 2 carbon isotopic equilibrium. In contrast, microbial terrestrial and pure culture gases are not consistent with both CH 4 H 2 O(l) hydrogen and CH 4 CO 2 carbon isotopic equilibrium. Overall, these results are explained qualitatively using previously developed conceptual models that link free energy gradients available to microorganisms to the degree that their enzymes can promote isotope-exchange reactions between CH 4 , CO 2 , and H 2 O.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Carbon and Water Fluxes of the Boreal Evergreen Needleleaf Forest Biome Constrained by Assimilating Ecosystem Carbonyl Sulfide Flux Observations

Gross primary production (GPP) by boreal forests is highly sensitive to environmental changes. However, GPP simulated by land surface models (LSMs) remains highly uncertain due to the lack of direct photosynthesis observations at large scales. Carbonyl sulfide (COS) has emerged as a promising proxy to improve the representation of GPP in LSMs. Because COS is absorbed by vegetation following the same diffusion pathway as CO2 during photosynthesis and not emitted back to the atmosphere, incorporating a mechanistic representation of vegetation COS uptake in LSMs allows using COS observations to refine GPP representation. Here, we perform ecosystem COS flux and GPP data assimilations to constrain the COS- and GPP-related parameters in the ORCHIDEE LSM for boreal evergreen needleleaf forests (BorENF). Assimilating ecosystem COS fluxes at Hyytiälä forest increases the simulated net ecosystem COS uptake by 14%. This increase largely results from changes in the internal conductance to COS, highlighting the need to improve the representation of COS internal diffusion and consumption. Moreover, joint assimilation of ecosystem COS flux and GPP at Hyytiälä improves the simulated latent heat flux, contrary to the GPP-only data assimilation, which fails to do so. Finally, we scaled this assimilation framework up to the boreal region and find that the joint assimilation of COS at Hyytiälä and GPP fluxes at 10 BorENF sites increases the modeled vegetation COS uptake up to 18%, but not GPP. Therefore, this study encourages the use of COS flux observations to inform GPP and latent heat flux representations in LSMs.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Manganese-rich high entropy oxides for lithium-ion batteries:materials design approaches to address voltage fade

Lithium- and manganese-rich oxides are of interest as lithium-ion battery cathode materials as Mn is earth abundant, low cost, and can deliver high capacity. Herein, a high entropy strategy was used to prepare Mn rich high entropy oxide (HEO) materials by including four additional metals (Ni, Co, Fe and Al) in the compositions using a mild co-precipitation method. Two HEOs (Li x Ni 0.1 Mn 0.6 Co 0.1 Al 0.1 Fe 0.1 O y , where x = 1.5 for HEO-L and x = 0.5 for HEO-H) with layered and spinel-layered hybrid structures were investigated where the morphology, elemental composition, structure, atomic level phase distribution, and electrochemistry were determined. The HEO-L samples involve a Li 2 TMO 3 layered structure with ~39% stacking faults. HEO-H is a hybrid structure comprised of 80 wt% spinel and 20 wt% LiMO 2 layered structure. The high entropy manganese-rich HEO-L showed higher capacity and 93% retention of the average voltage after 100 cycles while HEO-H showed higher capacity retention and near 100% average voltage retention. Finally, operando X-ray absorption spectroscopy revealed that the Ni, Co, and Mn are redox active in both materials while the Fe center remains at the Fe 3+ oxidation state throughout cycling, where the changes in the oxidation states for both materials during discharge were consistent with the delivered electrochemical capacity rationalizing the observed electrochemistry.

25 ENERGY STORAGE↗
DOE OSTI2020

Targeting tRNA-synthetase interactions towards novel therapeutic discovery against eukaryotic pathogens

The development of chemotherapies against eukaryotic pathogens is especially challenging because of both the evolutionary conservation of drug targets between host and parasite, and the evolution of strain-dependent drug resistance. There is a strong need for new nontoxic drugs with broad-spectrum activity against trypanosome parasites such as Leishmania and Trypanosoma. A relatively untested approach is to target macromolecular interactions in parasites rather than small molecular interactions, under the hypothesis that the features specifying macromolecular interactions diverge more rapidly through coevolution. We computed tRNA Class-Informative Features in humans and independently in eight distinct clades of trypanosomes, identifying parasite-specific informative features, including base pairs and base mis-pairs, that are broadly conserved over approximately 250 million years of trypanosome evolution. Validating these observations, we demonstrated biochemically that tRNA:aminoacyl-tRNA synthetase (aaRS) interactions are a promising target for anti-trypanosomal drug discovery. From a marine natural products extract library, we identified several fractions with inhibitory activity toward Leishmania major alanyl-tRNA synthetase (AlaRS) but no activity against the human homolog. These marine natural products extracts showed cross-reactivity towards Trypanosoma cruzi AlaRS indicating the broad-spectrum potential of our network predictions. We also identified Leishmania major threonyl-tRNA synthetase (ThrRS) inhibitors from the same library. We discuss why chemotherapies targeting multiple aaRSs should be less prone to the evolution of resistance than monotherapeutic or synergistic combination chemotherapies targeting only one aaRS.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Characterization of the aerosol vertical distributions and their impacts on warm clouds based on multi-year ARM observations

Aerosol vertical distribution plays a crucial role in cloud development and thus precipitation since both aerosol indirect and semi-direct effects significantly depend on the relative position of aerosol layer in reference to cloud, but its precise influence on cloud remains unclear. In this study, we integrated multi-year Raman Lidar measurements of aerosol vertical profiles from the U.S. Department of Energy Atmospheric Radiation Measurement (ARM) facility with available Value-Added Products of cloud features to characterize aerosol vertical distributions and their impacts on warm clouds over the continental and marine ARM atmospheric observatories, i.e., Southern Great Plains (SGP) and Eastern North Atlantic (ENA). A unimodal seasonal distribution of aerosol optical depths (AODs) with a peak in summer is found at upper boundary layer over SGP, while a bimodal distribution is observed at ENA for the AODs at lower levels with a major winter-spring maximum. The diurnal mean of upper-level AOD at SGP shows a maximum in the early evening. According to the relative positions of aerosol layers to clouds we further identify three primary types of aerosol vertical distribution, including Random, Decreasing, and Bottom. It is found that the impacts of aerosols on cloud may or may not vary with aerosol vertical distribution depending on environmental conditions, as reflected by the wide variations of the relations between AOD and cloud properties. For example, as AOD increases, the liquid water paths (LWPs) tend to be reduced at SGP but enhanced at ENA. The relations of cloud droplet effective radius with AOD largely depend on aerosol vertical distributions, particularly showing positive values in the Random type under low-LWP condition (<50gm -2 ). In conclusion, the distinct features of aerosol-cloud interactions in relation to aerosol vertical distribution are likely attributed to the continental-marine contrast in thermodynamic environments and aerosol conditions between SGP and ENA.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

A Multicontinuum-Theory-Based Approach to the Analysis of Fiber-Reinforced Polymer Composites with Degraded Stiffness and Strength Properties Due to Moisture Absorption

Marine energy generation technologies such as wave and tidal power have great potential in meeting the need for renewable energy in the years ahead. Yet, many challenges remain associated with marine-based systems because of the corrosive environment. Conventional materials like metals are subject to rapid corrosive breakdown, crippling the lifespan of structures in such environments. Fiber-reinforced polymer composites offer an appealing alternative in their strength and corrosion resistance, but can experience degradation of mechanical properties as a result of moisture absorption. An investigation is conducted to test the application of a technique for micromechanical analysis of composites, known as multicontinuum theory and demonstrated in past works, as a mechanism for predicting the effects of prolonged moisture absorption on the performance of fiber-reinforced composites. Experimental tensile tests are performed on composite coupons with and without prolonged exposure to a salt water solution to obtain stiffness and strength properties. Multicontinuum theory is applied in conjunction with micromechanical modeling to deduce the effects of moisture absorption on the behavior of constituent materials within the composites. The results are consistent with experimental observations when guided by known mechanisms and trends from previous studies, indicating multicontinuum theory as a potentially effective tool in predicting the long-term performance of composites in marine environments.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Orbital-Radar v1.0.0: a tool to transform suborbital radar observations to synthetic EarthCARE cloud radar data

The Earth Cloud, Aerosol and Radiation Explorer (EarthCARE) satellite developed by the European Space Agency (ESA) and the Japan Aerospace Exploration Agency (JAXA) launched in May 2024 carries a novel 94 GHz cloud profiling radar (CPR) with Doppler capability. This work describes the open-source instrument simulator Orbital-Radar, which transforms high-resolution radar data from field observations or forward simulations of numerical models to CPR primary measurements and uncertainties. The transformation accounts for sampling geometry and surface effects. We demonstrate Orbital-Radar's ability to provide realistic CPR views of typical cloud and precipitation scenes. The presented case studies show small-scale convection, marine stratus clouds, and Arctic mixed-phase cloud cases. These results provide valuable insights into the capabilities and challenges of the EarthCARE CPR mission and its advantages over the CloudSat CPR. Finally, Orbital-Radar allows for evaluating kilometre-scale numerical weather prediction models with EarthCARE CPR observations. So, Orbital-Radar can generate calibration and validation (Cal/Val) data sets already pre-launch. Nevertheless, an evaluation of synthetic CPR output data to accurate EarthCARE CPR data is missing.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Characterizing the Roles of Biogeochemical Cycling and Ocean Circulation in Regulating Marine Copper Distributions

Copper (Cu) is a key micronutrient for marine phytoplankton. Its oceanic biogeochemical cycle has elicited considerable attention due to dissolved Cu exhibiting a unique linear profile with depth. Several processes have been proposed for explaining this behavior. Here, in this study, we characterize the relationships between the observed Cu, PO 4 3– , and Si on a global scale. We find that the depth profiles of Cu resemble those of Si more than of PO 4 3– in the global ocean. To understand their relationships, we couple the biogeochemical and internal circulation processes in a model, fitting optimal Cu:PO 4 3– uptake ratios and remineralization length-scales to replicate the marine Cu distributions. The modeling results suggest that Cu uptake needs in the Southern Ocean are substantially higher than those in other oceanic regions. In addition, our modeling results indicate a deep Cu remineralization in the global ocean. We offer an alternative mechanism that relies on biogeochemical cycling and internal circulation to produce the linear depth profiles of dissolved Cu. Our results suggest that diatoms are likely the major phytoplankton dominating oceanic Cu cycling.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Atmospheric H 2 observations from the NOAA Cooperative Global Air Sampling Network

Abstract. The NOAA Global Monitoring Laboratory (GML) measures atmospheric hydrogen (H2) in grab samples collected weekly as flask pairs at over 50 sites in the Cooperative Global Air Sampling Network. Measurements representative of background air sampling show higher H2 in recent years at all latitudes. The marine boundary layer (MBL) global mean H2 was 552.8 ppb in 2021, 20.2 ± 0.2 ppb higher compared to 2010. A 10 ppb or more increase over the 2010–2021 average annual cycle was detected in 2016 for MBL zonal means in the tropics and in the Southern Hemisphere. Carbon monoxide measurements in the same-air samples suggest large biomass burning events in different regions likely contributed to the observed interannual variability at different latitudes. The NOAA H2 measurements from 2009 to 2021 are now based on the World Meteorological Organization Global Atmospheric Watch (WMO GAW) H2 mole fraction calibration scale, developed and maintained by the Max Planck Institute for Biogeochemistry (MPI-BGC), Jena, Germany. GML maintains eight H2 primary calibration standards to propagate the WMO scale. These are gravimetric hydrogen-in-air mixtures in electropolished stainless steel cylinders (Essex Industries, St. Louis, MO), which are stable for H2. These mixtures were calibrated at the MPI-BGC, the WMO Central Calibration Laboratory (CCL) for H2, in late 2020 and span the range 250–700 ppb. We have used the CCL assignments to propagate the WMO H2 calibration scale to NOAA air measurements performed using gas chromatography and helium pulse discharge detector instruments since 2009. To propagate the scale, NOAA uses a hierarchy of secondary and tertiary standards, which consist of high-pressure whole-air mixtures in aluminum cylinders, calibrated against the primary and secondary standards, respectively. Hydrogen at the parts per billion level has a tendency to increase in aluminum cylinders over time. We fit the calibration histories of these standards with zero-, first-, or second-order polynomial functions of time and use the time-dependent mole fraction assignments on the WMO scale to reprocess all tank air and flask air H2 measurement records. The robustness of the scale propagation over multiple years is evaluated with the regular analysis of target air cylinders and with long-term same-air measurement comparison efforts with WMO GAW partner laboratories. Long-term calibrated, globally distributed, and freely accessible measurements of H2 and other gases and isotopes continue to be essential to track and interpret regional and global changes in the atmosphere composition. The adoption of the WMO H2 calibration scale and subsequent reprocessing of NOAA atmospheric data constitute a significant improvement in the NOAA H2 measurement records.

Pétron, Gabrielle↗
DOE OSTI2021

The Impact of Slantwise Descending Dry Intrusions on the Marine Boundary Layer and Air-Sea Interface Over the ARM Eastern North Atlantic Site

Dry intrusions (DIs) are synoptic-scale slantwise descending airstreams from the midlatitude upper troposphere toward the boundary layer at lower latitudes. Typically occurring behind cold fronts, such intrusions of dry air often reach the boundary layer and cause its deepening, thereby affecting boundary-layer clouds. Although subsidence is generally an inherent feature of the subtropical marine boundary layer (MBL), it is unclear how the MBL reacts to the transient, dynamically distinct DI. In this study, reanalysis data were combined with observations from the Atmospheric Radiation Measurement Eastern North Atlantic (ENA) site (39.1 degrees N,28.0 degrees W) to characterize the impact of DIs on MBL characteristics and clouds. Specifically, an objective criterion is applied to the observations made during the winter months of 2016-2018 to identify the DI days from those before and following DIs, and reference periods without DIs. The analyses suggest substantial deepening of the well-mixed boundary layer accompanied by changes in the cloud, precipitation and thermodynamic properties during the DI events. During the DI, the lower troposphere cooled and dried substantially thereby inducing strong surface sensible and latent heat fluxes. All while a strong inversion builds up at the elevated MBL top affecting cloud occurrence. The results show DIs to affect the boundary layer and cloud structure at the ENA site similar to 21% of the time in winter months, with the response of the cloud fields to the DI-fronts substantially different than that to the non-DI fronts. Hence, the DI events should be considered while studying boundary layer and cloud processes in the region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Temporal covariation of island arc Sr isotopes and seawater chemistry over the past 2 billion years

The chemical compositions of island arc basalts (IAB) reflect contributions from the mantle as well as fluids and melts from the subducting slab. Addition of radiogenic seawater Sr to oceanic crust through hydrothermal alteration and subsequent subduction is often invoked to explain elevated 87 Sr/ 86 Sr signatures in modern IAB. However, changes in the 87 Sr/ 86 Sr of island arc magmatic rocks through time has not been investigated, limiting our understanding of the factors influencing the Sr budgets of arcs throughout Earth’s history. To address this, we compiled 87 Sr/ 86 Sr values from island arc magmatic rocks ranging in age from modern to Paleoproterozoic, only including data from island arc localities that best preserve initial magmatic 87 Sr/ 86 Sr. Median initial 87 Sr/ 86 Sr values are consistently elevated compared to depleted mantle 87 Sr/ 86 Sr over this period, indicating persistent enrichment in radiogenic Sr in island arcs. Moreover, the elevation in island arc 87 Sr/ 86 Sr relative to the depleted mantle is variable. A notable rise in island arc 87 Sr/ 86 Sr during the late Neoproterozoic coincides with a steep increase in seawater 87 Sr/ 86 Sr and Sr concentration. To investigate this potential connectivity, we modeled the 87 Sr/ 86 Sr of island arc magmas between 0 and 830 Ma with inputs of depleted mantle 87 Sr/ 86 Sr, seawater 87 Sr/ 86 Sr, and seawater Sr concentration. The model reproduces the overall trajectory of the compiled data. We interpret the observed temporal variation in island arc 87 Sr/ 86 Sr values and its close association with fluctuations in seawater chemistry as evidence that changes in marine geochemistry have strongly influenced the Sr isotopic record of island arc magmas over time.

Science & Technology - Other Topics↗
DOE OSTI2025

Using stable isotopes in water vapor to study the interdependence of clouds, atmospheric aerosols, and precipitation processes

This project deployed water vapor isotope measurements at the La Porte, Texas TRACER site during June-September 2022 to quantify mixing processes in sea breeze circulations. Using a Picarro L2130 analyzer, we collected high-frequency measurements of δD and δ¹⁸O that revealed how marine and terrestrial air masses mix during 46 identified sea breeze events. The isotopic tracers showed systematic changes during frontal passages, with composite analyses demonstrating vertical mixing between cool marine air and warmer air aloft. We developed a transilient matrix model that explicitly treats non-local mixing and isotopic fractionation to interpret the observations. The work directly supports TRACER's core objective of understanding convective initiation by constraining the vertical transport of water vapor and its interaction with Houston's aerosol-laden urban plume during sea breeze-convection coupling.

58 GEOSCIENCES↗
DOE OSTI2024

Control of hydrogen concentrations by microbial sulfate reduction in two contrasting anoxic coastal sediments

Introduction Molecular hydrogen is produced by the fermentation of organic matter and consumed by organisms including hydrogenotrophic methanogens and sulfate reducers in anoxic marine sediment. The thermodynamic feasibility of these metabolisms depends strongly on organic matter reactivity and hydrogen concentrations; low organic matter reactivity and high hydrogen concentrations can inhibit fermentation so when organic matter is poor, fermenters might form syntrophies with methanogens and/or sulfate reducers who alleviate thermodynamic stress by keeping hydrogen concentrations low and tightly controlled. However, it is unclear how these metabolisms effect porewater hydrogen concentrations in natural marine sediments of different organic matter reactivities. Methods We measured aqueous concentrations of hydrogen, sulfate, methane, dissolved inorganic carbon, and sulfide with high-depth-resolution and 16S rRNA gene assays in sediment cores with low carbon reactivity in White Oak River (WOR) estuary, North Carolina, and those with high carbon reactivity in Cape Lookout Bight (CLB), North Carolina. We calculated the Gibbs energies of sulfate reduction and hydrogenotrophic methanogenesis. Results Hydrogen concentrations were significantly higher in the sulfate reduction zone at CLB than WOR (mean: 0.716 vs. 0.437 nM H 2 ) with highly contrasting hydrogen profiles. At WOR, hydrogen was extremely low and invariant (range: 0.41–0.52 nM H 2 ) in the upper 15 cm. Deeper than 15 cm, hydrogen became more variable (range: 0.312–2.56 nM H 2 ) and increased until methane production began at ~30 cm. At CLB, hydrogen was highly variable in the upper 15 cm (range: 0.08–2.18 nM H 2 ). Ratios of inorganic carbon production to sulfate consumption show AOM drives sulfate reduction in WOR while degradation of organics drive sulfate reduction in CLB. Discussion We conclude more reactive organic matter increases hydrogen concentrations and their variability in anoxic marine sediments. In our AOM-dominated site, WOR, sulfate reducers have tight control on hydrogen via consortia with fermenters which leads to the lower observed variance due to interspecies hydrogen transfer. After sulfate depletion, hydrogen accumulates and becomes variable, supporting methanogenesis. This suggests that CLB’s more reactive organic matter allows fermentation to occur without tight metabolic coupling of fermenters to sulfate reducers, resulting in high and variable porewater hydrogen concentrations that prevent AOM from occurring through reverse hydrogenotrophic methanogenesis.

Microbiology↗