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At least 307 records · Page 17

Southern Ocean Sulfate Aerosol Sources Quantified From Sulfur Isotopes in Antarctic Ice Cores

The Southern Ocean has emerged as a key region for constraining aerosol-climate interactions due to its relatively low anthropogenic influence. Sulfate is an important aerosol over the Southern Ocean, and models suggest dimethyl sulfide (DMS) is the largest source of sulfate during summer. However, sulfur isotopes of sulfate (δ 34 S(SO 4 2− )) in Antarctic ice cores suggest a significant contribution from a previously unexplained non-DMS source. Here we show that the fractional contribution from passive volcanic degassing (f volc ) explains observed δ 34 S(SO 4 2− ), and that a global chemical transport model underestimates f volc across Antarctica. Underestimated f volc implies that the model mischaracterizes sulfate sources in this important region. The discrepancy between observed and modeled sulfate sources can be reconciled by increasing passive volcanic sulfur degassing emissions and decreasing DMS emissions. Our results imply that current biases in emissions inventories could bias assessments of aerosol-cloud interactions in the Southern Ocean region and globally.

Jongebloed, Ursula A. [Univ. of Washington, Seattl↗

Future Projections of the El Niño—Southern Oscillation and Tropical Pacific Mean State in CMIP6

Abstract The El Niño—Southern Oscillation (ENSO) is an important mode of tropical Pacific atmosphere‐ocean variability that drives teleconnections with weather and climate globally. However, prior studies using state‐of‐the‐art climate models lack consensus regarding future ENSO projections and are often impacted by tropical Pacific sea‐surface temperature (SST) biases. We used 173 simulations from 29 climate models participating in the Coupled Model Intercomparison Project, version 6 (CMIP6) to analyze model biases and future ENSO projections. We analyzed two ENSO indices, namely the ENSO Longitude Index (ELI), which measures zonal shifts in tropical Pacific deep convection and accounts for changes in background SST, and the Niño 3.4 index, which measures SST anomalies in the central‐eastern equatorial Pacific. We found that the warm eastern tropical‐subtropical Pacific SST bias typical of previous generations of climate models persists into many of the CMIP6 models. Future projections of ENSO shift toward more El Niño‐like conditions based on ELI in 48% of simulations and 55% of models, in association with a future weakening of the zonal equatorial Pacific SST gradient. On the other hand, none of the models project a significant shift toward La Niña‐like conditions. The standard deviation of the Niño 3.4 index indicates a lack of consensus on whether an increase or decrease in ENSO variability is expected in the future. Finally, we found a possible relationship between historical SST and low‐level cloud cover biases in the ENSO region and future changes in ELI; however, this result may be impacted by limitations in data availability.

54 ENVIRONMENTAL SCIENCES↗

Exploring dimethyl sulfide (DMS) oxidation and implications for global aerosol radiative forcing

Abstract. Aerosol indirect radiative forcing (IRF), which characterizes how aerosols alter cloud formation and properties, is very sensitive to the preindustrial (PI) aerosol burden. Dimethyl sulfide (DMS), emitted from the ocean, is a dominant natural precursor of non-sea-salt sulfate in the PI and pristine present-day (PD) atmospheres. Here we revisit the atmospheric oxidation chemistry of DMS, particularly under pristine conditions, and its impact on aerosol IRF. Based on previous laboratory studies, we expand the simplified DMS oxidation scheme used in the Community Atmospheric Model version 6 with chemistry (CAM6-chem) to capture the OH-addition pathway and the H-abstraction pathway and the associated isomerization branch. These additional oxidation channels of DMS produce several stable intermediate compounds, e.g., methanesulfonic acid (MSA) and hydroperoxymethyl thioformate (HPMTF), delay the formation of sulfate, and, hence, alter the spatial distribution of sulfate aerosol and radiative impacts. The expanded scheme improves the agreement between modeled and observed concentrations of DMS, MSA, HPMTF, and sulfate over most marine regions, based on the NASA Atmospheric Tomography (ATom), the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA), and the Variability of the American Monsoon Systems (VAMOS) Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-REx) measurements. We find that the global HPMTF burden and the burden of sulfate produced from DMS oxidation are relatively insensitive to the assumed isomerization rate, but the burden of HPMTF is very sensitive to a potential additional cloud loss. We find that global sulfate burden under PI and PD emissions increase to 412 Gg S (+29 %) and 582 Gg S (+8.8 %), respectively, compared to the standard simplified DMS oxidation scheme. The resulting annual mean global PD direct radiative effect of DMS-derived sulfate alone is −0.11 W m−2. The enhanced PI sulfate produced via the gas-phase chemistry updates alone dampens the aerosol IRF as anticipated (−2.2 W m−2 in standard versus −1.7 W m−2, with updated gas-phase chemistry). However, high clouds in the tropics and low clouds in the Southern Ocean appear particularly sensitive to the additional aqueous-phase pathways, counteracting this change (−2.3 W m−2). This study confirms the sensitivity of aerosol IRF to the PI aerosol loading and the need to better understand the processes controlling aerosol formation in the PI atmosphere and the cloud response to these changes.

54 ENVIRONMENTAL SCIENCES↗

Observed declines in upper ocean phosphate-to-nitrate availability

Climate warming is increasing ocean stratification, which in turn should decrease the nutrient flux to the upper ocean. This may slow marine primary productivity, causing cascading effects throughout food webs. However, observing changes in upper ocean nutrients is challenging because surface concentrations are often below detection limits. We show that the nutricline depth, where nutrient concentrations reach well-detected levels, is tied to productivity and upper ocean nutrient availability. Next, we quantify nutricline depths from a global database of observed vertical nitrate and phosphate profiles to assess contemporary trends in global nutrient availability (1972–2022). We find strong evidence that the P-nutricline (phosphacline) is mostly deepening, especially throughout the southern hemisphere, but the N-nutricline (nitracline) remains mostly stable. Earth System Model (ESM) simulations support the hypothesis that reduced iron stress and increased nitrogen fixation buffer the nitracline, but not phosphacline, against increasing stratification. These contemporary trends are expected to continue in the coming decades, leading to increasing phosphorus but not nitrogen stress for marine phytoplankton, with important ramifications for ocean biogeochemistry and food web dynamics.

54 ENVIRONMENTAL SCIENCES↗

Reaching 1.5 and 2.0 °C global surface temperature targets using stratospheric aerosol geoengineering

A new set of stratospheric aerosol geoengineering (SAG) model experiments has been performed with Community Earth System Model version 2 (CESM2) with the Whole Atmosphere Community Climate Model (WACCM6) that are based on the Coupled Model Intercomparison Project phase 6 (CMIP6) overshoot scenario (SSP5-34-OS) as a baseline scenario to limit global warming to 1.5 or 2.0 °C above 1850–1900 conditions. The overshoot scenario allows us to applying a peak-shaving scenario that reduces the needed duration and amount of SAG application compared to a high forcing scenario. In addition, a feedback algorithm identifies the needed amount of sulfur dioxide injections in the stratosphere at four pre-defined latitudes, 30 °N, 15 °N, 15 °S, and 30 °S, to reach three surface temperature targets: global mean temperature, and interhemispheric and pole-to-Equator temperature gradients. These targets further help to reduce side effects, including overcooling in the tropics, warming of high latitudes, and large shifts in precipitation patterns. These experiments are therefore relevant for investigating the impacts on society and ecosystems. Comparisons to SAG simulations based on a high emission pathway baseline scenario (SSP5-85) are also performed to investigate the dependency of impacts using different injection amounts to offset surface warming by SAG. We find that changes from present-day conditions around 2020 in some variables depend strongly on the defined temperature target (1.5 °C vs. 2.0 °C). These include surface air temperature and related impacts, the Atlantic Meridional Overturning Circulation, which impacts ocean net primary productivity, and changes in ice sheet surface mass balance, which impacts sea level rise. Others, including global precipitation changes and the recovery of the Antarctic ozone hole, depend strongly on the amount of SAG application. Furthermore, land net primary productivity as well as ocean acidification depend mostly on the global atmospheric CO 2 concentration and therefore the baseline scenario. Multi-model comparisons of experiments that include strong mitigation and carbon dioxide removal with some SAG application are proposed to assess the robustness of impacts on societies and ecosystems.

42 ENGINEERING↗

The Importance of Protein Phosphorylation for Signaling and Metabolism in Response to Diel Light Cycling and Nutrient Availability in a Marine Diatom

Diatoms are major contributors to global primary production and their populations in the modern oceans are affected by availability of iron, nitrogen, phosphate, silica, and other trace metals, vitamins, and infochemicals. However, little is known about the role of phosphorylation in diatoms and its role in regulation and signaling. We report a total of 2759 phosphorylation sites on 1502 proteins detected in Phaeodactylum tricornutum. Conditionally phosphorylated peptides were detected at low iron (n = 108), during the diel cycle (n = 149), and due to nitrogen availability (n = 137). Through a multi-omic comparison of transcript, protein, phosphorylation, and protein homology, we identify numerous proteins and key cellular processes that are likely under control of phospho-regulation. We show that phosphorylation regulates: (1) carbon retrenchment and reallocation during growth under low iron, (2) carbon flux towards lipid biosynthesis after the lights turn on, (3) coordination of transcription and translation over the diel cycle and (4) in response to nitrogen depletion. We also uncover phosphorylation sites for proteins that play major roles in diatom Fe sensing and utilization, including flavodoxin and phytotransferrin (ISIP2A), as well as identify phospho-regulated stress proteins and kinases. These findings provide much needed insight into the roles of protein phosphorylation in diel cycling and nutrient sensing in diatoms.

59 BASIC BIOLOGICAL SCIENCES↗

The hazard components of representative key risks. The physical climate perspective

The framework of Representative Key Risks (RKRs) has been adopted by the Intergovernmental Panel on Climate Change Working Group II in order to categorize, assess and communicate a wide range of regional and sectoral key risks, expected to become severe as a consequence of the potentially detrimental convergence of changing climate conditions, exposure and vulnerability of human and natural systems, and responses through (mal)adaptation measures. Other papers in this special issue treat each of eight RKRs by holistically assessing their current status and future evolution as a result of this convergence. However, their treatment cannot always organize such assessment according to a systematic gradation of climatic changes, often times having to extrapolate the big-picture evolution of risk from either qualitative effects of “low” medium” and “high” warming, or limited/focused analysis of the consequences of particular mitigation choices (e.g., benefits of limiting warming to 1.5 or 2C). In this study we offer as systematic a representation as possible – given current literature and assessments – of the future evolution of the hazard components of RKRs. We draw on the assessment of changes in climatic impact-drivers relevant to RKRs described in the 6th Assessment Report by Working Group 1 (WGI) supplemented when needed by more recent literature. We identify the relevant hazards for each RKR, based upon the WGII authors’ assessment, and we report on their current state and expected future changes in magnitude, intensity and/or frequency, linking these changes to Global Warming Levels to the extent possible. For some of these quantities - like regional trends in oceanic and atmospheric temperature and precipitation, some heat and precipitation extremes, permafrost thaw and Northern Hemisphere snow cover - a strong and quantitative relationship with global average temperature change has been assessed. For others - like frequency and intensity of tropical cyclones and extra-tropical storms, and fire weather - the link to increasing global temperatures can only be described qualitatively. For some processes - like the behavior of ice-sheets, or changes in circulation dynamics - large uncertainties about the effects of different levels of warming remain, and for a few others - like ocean pH and air pollution - the composition of the scenario of anthropogenic emissions is most relevant, rather than the warming reached. In almost all cases, however, the basic message remains that every small increment in CO2 concentration in the atmosphere and associated warming will bring changes in climate phenomena that will contribute to increasing risk of impacts on human and natural systems when these changes happen in conjunction with these systems’ conditions of exposure and vulnerability, and in lack of effective adaptation. Our picture of the evolution of RKR-relevant climatic impact-drivers complements and enriches the treatment of RKRs in the other papers in at least two ways: by filling in an often only cursory or limited representation of the physical climate aspects driving impacts, and by providing a fuller representation of their future possible evolution which represents an important component – if never the only one – of the potential future evolution of risk severity.

54 ENVIRONMENTAL SCIENCES↗

Giant Virus Infection Signatures Are Modulated by Euphotic Zone Depth Strata and Iron Regimes of the Subantarctic Southern Ocean

Viruses can alter the abundance, evolution, and metabolism of microorganisms in the ocean, playing a key role in water column biogeochemistry and global carbon cycles. Large efforts to measure the contribution of eukaryotic microorganisms (e.g., protists) to the marine food web have been made, yet the in situ activities of the ecologically relevant viruses that infect these organisms are not well characterized. Viruses within the phylum Nucleocytoviricota (“giant viruses”) are known to infect a diverse range of ecologically relevant marine protists, yet how these viruses are influenced by environmental conditions remains under-characterized. By employing metatranscriptomic analyses of in situ microbial communities along a temporal and depthresolved gradient, we describe the diversity of giant viruses at the Southern Ocean Time Series (SOTS), a site within the subpolar Southern Ocean. Using a phylogeny-guided taxonomic assessment of detected giant virus genomes and metagenome-assembled genomes, we observed depth-dependent structuring of divergent giant virus families mirroring dynamic physicochemical gradients in the stratified euphotic zone. Analyses of transcribed metabolic genes from giant viruses suggest viral metabolic reprogramming of hosts from the surface to a 200-m depth. Lastly, using on-deck incubations reflecting a gradient of iron availability, we show that modulating iron regimes influences the activity of giant viruses in the field. Specifically, we show enhanced infection signatures of giant viruses under both iron-replete and iron-limited conditions. Collectively, these results expand our understanding of how the water column’s vertical biogeography and chemical surroundings affect an important group of viruses within the Southern Ocean

59 BASIC BIOLOGICAL SCIENCES↗

Tropical Cirrus in Global Storm-Resolving Models: 1. Role of Deep Convection

Pervasive cirrus clouds in the upper troposphere and tropical tropopause layer (TTL) influence the climate by altering the top-of-atmosphere radiation balance and stratospheric water vapor budget. These cirrus are often associated with deep convection, which global climate models must parameterize and struggle to accurately simulate. By comparing high-resolution global storm-resolving models from the Dynamics of the Atmospheric general circulation Modeled On Non-hydrostatic Domains (DYAMOND) intercomparison that explicitly simulate deep convection to satellite observations, we assess how well these models simulate deep convection, convectively generated cirrus, and deep convective injection of water into the TTL over representative tropical land and ocean regions. The DYAMOND models simulate deep convective precipitation, organization, and cloud structure fairly well over land and ocean regions, but with clear intermodel differences. All models produce frequent overshooting convection whose strongest updrafts humidify the TTL and are its main source of frozen water. Intermodel differences in cloud properties and convective injection exceed differences between land and ocean regions in each model. We argue that, with further improvements, global storm-resolving models can better represent tropical cirrus and deep convection in present and future climates than coarser-resolution climate models. To realize this potential, they must use available observations to perfect their ice microphysics and dynamical flow solvers.

54 ENVIRONMENTAL SCIENCES↗

Multi-year assessment of the impact of ship-borne radiosonde observations on polar WRF forecasts in the Arctic

Abstract To compensate for the lack of conventional observations over the Arctic Ocean, ship-borne radiosonde observations have been regularly carried out during summer Arctic expeditions and the observed data have been broadcast via the global telecommunication system since 2017. With these data obtained over the data-sparse Arctic Ocean, observing system experiments were carried out using a polar-optimized version of the Weather Research and Forecasting (WRF) model and the WRF Data Assimilation (WRFDA) system to investigate their effects on analyses and forecasts over the Arctic. The results of verification against reanalysis data reveal: (1) DA effects on analyses and forecasts; (2) the reason for the year-to-year variability of DA effects; and (3) the possible role of upper-level potential vorticity in delayed DA effects. The overall assimilation effects of the extra data on the analyses and forecasts over the Arctic are positive. Initially, the DA effects are the most apparent in the temperature variables in the middle/lower troposphere, which spread to the wind variables in the upper troposphere. The effects decrease with time but reappear after approximately 120 h, even in the 240-h forecasts. The effects on forecasts vary depending on the proximity of the radiosonde observation locations to the high synoptic variability. The upper-level potential vorticity is known to play an important role in the development of Arctic cyclones, and it is suggested as a possible explanation for the delayed DA effects after about 120 h.

Geology↗

Sustainable Biofuels for Low-Carbon Maritime Transportation

The marine shipping sector heavily depends on fossil fuels and is one of the largest petroleum fuel consumers [1,2]. The annual global marine fuel consumption was estimated to be around 400 million metric tons in 2019 (2.5 billion barrels). Moreover, ocean shipping is one of the most significant contributors to sulfur oxides, nitrogen oxides, and particulate matter emissions. Global shipping contributes 13% of human-caused sulfur emissions and 2.6% of anthropogenic carbon dioxide emissions. As a major source of pollutant emissions, the marine industry faces several challenges related to emission regulations. The International Maritime Organization (IMO) has established a framework for reducing the carbon intensity of shipping: 40% reduction relative to 2008 levels by 2030 and 70% reduction by 2050. As the aviation sector, the maritime shipping sector is difficult to decarbonize through electrification. Biofuels offer the best opportunities for decarbonizing marine shipping in the near and medium-term. Advanced biofuels such as pyrolysis bio-oil offer the low-cost potential for meeting carbon reduction goals. For instance, the pyrolysis bio-oil exhibited promising marginal CO2 abatement costs at less than $100/tonne CO2-equivalent at a heavy fuel oil price greater than $1.10/gal [1]. As a potential biofuel option for low-carbon maritime shipping, this presentation focuses on a comparative techno-economic analysis (TEA) of bio-oils produced via a fast pyrolysis-based conversion pathway. The pathway converts a 50/50 blend of forest residues and clean pine to bio-oil via three process options: fast pyrolysis without vapor upgrading, and fast pyrolysis with vapor phase upgrading over ZSM-5 zeolite catalyst and Pt/TiO2 catalyst. The process configuration and operation variation led to different capital and operating costs, as well as the resulting raw bio-oil’s yield and quality, e.g., the water content, total acid number, and carboxylic acid number. The study also determined the minimum upgrading of bio-oils required to enable blending with very low sulfur fuel oil (VLSFO), with the associated costs reflected in TEA. This study shows that bio-oil could be a cost-effective fuel option for decarbonizing maritime shipping. Further research is required with respect to biofuel blending properties, such as compatibility with existing fuel system infrastructure and suitable engine performance.

BIOMASS FUELS↗

Ejection of Dust From the Ocean as a Potential Source of Marine Ice Nucleating Particles

Oceans are, generally, relatively weak sources of ice nucleating particles (INPs). Thus, dust transported from terrestrial regions can dominate atmospheric INP concentrations even in remote marine regions. Studies of ocean-emitted INPs have focused upon sea spray aerosols containing biogenic species. Even though large concentrations of dust are transported over marine regions, resuspended dust has never been explicitly considered as another possible source of ocean-emitted INPs. Current models assume that deposited dust is not re-emitted from surface waters. Our laboratory studies of aerosol particles produced from coastal seawater and synthetic seawater doped with dust show that dust can indeed be ejected from water during bubble bursting. INP concentration measurements show these ejected dust particles retain ice nucleating activity. Doping synthetic seawater to simulate a strong dust deposition event produced INPs active at temperatures colder than -13 °C and INP concentrations one to two orders of magnitude greater than either lab sea spray or marine boundary layer measurements. The relevance of these laboratory findings is highlighted by single particle composition measurements along the Californian coast where at least 9% of dust particles were mixed with sea salt. Additionally, global modeling studies show that resuspension of dust from the ocean could exert the most impact over the Southern Ocean, where ocean-emitted INPs are thought to dominate atmospheric INP populations. More work characterizing the factors governing the resuspension of dust particles is required to understand the potential impact upon clouds.

54 ENVIRONMENTAL SCIENCES↗

Technical descriptions of the experimental dynamical downscaling simulations over North America by the CAM–MPAS variable-resolution model

Abstract. Comprehensive assessment of climate datasets is important for communicating model projections and associated uncertainties to stakeholders. Uncertainties can arise not only from assumptions and biases within the model but also from external factors such as computational constraint and data processing. To understand sources of uncertainties in global variable-resolution (VR) dynamical downscaling, we produced a regional climate dataset using the Model for Prediction Across Scales (MPAS; dynamical core version 4.0) coupled to the Community Atmosphere Model (CAM; version 5.4), which we refer to as CAM–MPAS hereafter. This document provides technical details of the model configuration, simulations, computational requirements, post-processing, and data archive of the experimental CAM–MPAS downscaling data. The CAM–MPAS model is configured with VR meshes featuring higher resolutions over North America as well as quasi-uniform-resolution meshes across the globe. The dataset includes multiple uniform- (240 and 120 km) and variable-resolution (50–200, 25–100, and 12–46 km) simulations for both the present-day (1990–2010) and future (2080–2100) periods, closely following the protocol of the North American Coordinated Regional Climate Downscaling Experiment. A deviation from the protocol is the pseudo-warming experiment for the future period, using the ocean boundary conditions produced by adding the sea surface temperature and sea-ice changes from the low-resolution version of the Max Planck Institute Earth System Model (MPI-ESM-LR) in the Coupled Model Intercomparison Project Phase 5 to the present-day ocean state from a reanalysis product. Some unique aspects of global VR models are evaluated to provide background knowledge to data users and to explore good practices for modelers who use VR models for regional downscaling. In the coarse-resolution domain, strong resolution sensitivity of the hydrological cycles exists over the tropics but does not appear to affect the midlatitude circulations in the Northern Hemisphere, including the downscaling target of North America. The pseudo-warming experiment leads to similar responses of large-scale circulations to the imposed radiative and boundary forcings in the CAM–MPAS and MPI-ESM-LR models, but their climatological states in the historical period differ over various regions, including North America. Such differences are carried to the future period, suggesting the importance of the base state climatology. Within the refined domain, precipitation statistics improve with higher resolutions, and such statistical inference is verified to be negligibly influenced by horizontal remapping during post-processing. Limited (≈50 % slower) throughput of the current code is found on a recent many-core/wide-vector high-performance computing system, which limits the lengths of the 12–46 km simulations and indirectly affects sampling uncertainty. Our experience shows that global and technical aspects of the VR downscaling framework require further investigations to reduce uncertainties for regional climate projection.

58 GEOSCIENCES↗

Sensitivity of the pseudo-global warming method under flood conditions: a case study from the northeastern US

Abstract. Intensified extreme precipitation and corresponding floods are the most relevant consequences of climate change over the northeastern US (NEUS). To evaluate the impacts of climate change or certain climate perturbations on future extreme weather events which are dynamically similar to historic analogs, the pseudo-global warming (PGW) method has been frequently employed; however, this method lacks precise definition and guidelines, thus limiting its application. More specifically, three key questions related to the application of the PGW method remain unanswered: at what spatial scale should climate perturbations be applied? Among the different meteorological variables available, which ones should be perturbed? And will PGW projections vary significantly when different perturbations are applied? To address these questions, we examine the sensitivity and robustness of conclusions drawn from the PGW method over the NEUS by conducting multiple PGW experiments with varied perturbation spatial scales and choice of perturbed meteorological variables. The results show that the projections of precipitation and other essential variables at the regional mean scale are consistent across the PGW simulations, with a relative difference of much less than 10 %; however, different perturbation modifications can cause significant displacements of the storm events being simulated. Several previously assumed advantages of modifying only the temperature at regional mean scale, such as the preservation of geostrophic balance, do not appear to hold. Also, for these experiments, we find the regional mean perturbation produces a positive precipitation bias because it ignores the land–ocean warming contrast, which is a robust regional response to global warming. Overall, PGW experiments with perturbations from temperature or the combination of temperature and wind at the grid point scale are both recommended, depending on the research questions. The first approach can isolate the spatially dependent thermodynamic impact, and the latter incorporates both the thermodynamic and dynamic impacts.

54 ENVIRONMENTAL SCIENCES↗

Stepping on the Gas to a Circular Economy: Accelerating Development of Carbon-Negative Chemical Production from Gas Fermentation

Owing to rising levels of greenhouse gases in our atmosphere and oceans, climate change poses significant environmental, economic, and social challenges globally. Technologies that enable carbon capture and conversion of greenhouse gases into useful products will help mitigate climate change by enabling a new circular carbon economy. Gas fermentation using carbon-fixing microorganisms offers an economically viable and scalable solution with unique feedstock and product flexibility that has been commercialized recently. Here, we review the state of the art of gas fermentation and discuss opportunities to accelerate future development and rollout. We discuss the current commercial process for conversion of waste gases to ethanol, including the underlying biology, challenges in process scale-up, and progress on genetic tool development and metabolic engineering to expand the product spectrum. We emphasize key enabling technologies to accelerate strain development for acetogens and other nonmodel organisms.

59 BASIC BIOLOGICAL SCIENCES↗

Assessing Effects of Climate Change on Legacy Waste at the Enewetak Atoll

The Republic of the Marshall Islands (RMI) is in the central Pacific Ocean ~4,500 km west of Hawaii. The Enewetak Atoll, located in the northwest part of the RMI, was the site for 43 nuclear weapon tests between 1948 and 1958. Fallout and deposition from the tests contaminated the island surfaces, lagoon waters and sediment, and nearby ocean waters at the atoll. In the 1970s, a cleanup effort collected radioactive waste and placed it in the Cactus Crater on Runit Island (also called the Runit Dome). In December 2021, Congress directed the U.S. Department of Energy to study the impacts of climate change on the Runit Dome nuclear waste disposal site. Pacific Northwest National Laboratory (PNNL) assembled a multidisciplinary team of climate scientists, ocean modelers, environmental scientists, and health physicists to assess the likely effects of remaining radionuclides at the Enewetak Atoll. PNNL’s approach focused on effects of tropical cyclones that were postulated to mobilize and transport contaminated lagoon sediments and result in human and biota exposure. PNNL’s study estimated (1) the radionuclide source term, (2) the effects of climate change on severe storms, (3) mobilization and transport of radionuclides, and (4) radiation dose to humans and biota. Radionuclides in the lagoon and/or ocean waters of the Enewetak Atoll were characterized by the U.S. Atomic Energy Commission (AEC) in 1972, Woods Hole Oceanographic Institution in 2015, and Lawrence Livermore National Laboratory in 2018. The RMI Nationwide Radiological Study was conducted in the early 1990s for radionuclides remaining in island soils. The 1972 AEC survey remains the most comprehensive source of radionuclide data on lagoon sediments. Climate change modeling at a regional scale in the central Pacific Ocean is limited. PNNL climate scientists simulated severe historical storms postulated to occur both in a recent climate (2015) and in the future (2090) using the Advanced Research Weather Research and Forecasting (WRF-ARW) model, employing a pseudo-global-warming technique. A postulated complete, future failure of the Runit Dome was also considered. PNNL developed a high-resolution regional ocean hydrodynamics model covering the entire RMI extended economic zone using the Finite Volume Coastal Ocean Model (FVCOM). The FVCOM model was run using global reanalysis data for current climate and WRF-ARW simulation for the future climate. PNNL also developed a radionuclide fate and transport model using the FVCOM Integrated Compartment Model (FVCOM-ICM) to simulate the current and future mobilization and transport of radionuclides sorbed to lagoon sediments and the exchange of radionuclides between the water and sediment. FVCOM-ICM-predicted radionuclide concentrations were then used to estimate radiation dose to humans and biota at all islands of the Enewetak Atoll. Under current climate conditions, annual radiation exposures for the southern islands including Enewetak (Fred) and Medren (Elmer) were below the current U.S. standards. Radiation doses were somewhat elevated starting at Runit Island northward and westward to Enjebi Island (Janet). The islands in the northwest quadrant, particularly Bokoluo (Alice) and Bokombako (Belle), remain relatively contaminated. The islands in the southwestern quadrant have low contamination. The highest contribution to radiation doses comes from consumption of locally grown foods. Two radionuclides, 90Sr and 137Cs, contributed the greatest fraction for most terrestrial foods. In current climate conditions, the storms temporarily increased radionuclide concentrations in the lagoon waters, increasing the radiation dose slightly. In future conditions, doses are expected to be smaller, primarily because of the radioactive decay of the shorter-lived radioisotopes of 90Sr and 137Cs. This could make all islands in the far northwest of the atoll – except Bokombako (Belle) and perhaps Bokoluo (Alice) – suitable for residency. For the f

Prasad, Rajiv↗

Characterization of organic aerosol across the global remote troposphere: a comparison of ATom measurements and global chemistry models

The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of non-refractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 µg sm -3 ). Lower concentrations (~0.1–0.3 µg sm -3 ) are observed in the northern middle and high latitudes and very low concentrations (<0.1 µg sm -3 ) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the secondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA/OC) ratios of ~2.2–2.8, and is 30 %–60 % more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model–measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations.

54 ENVIRONMENTAL SCIENCES↗

Ocean liming effect on a North Atlantic microbial community: changes in composition and rates

The ongoing rise in atmospheric CO 2 levels and the consequent global warming make it increasingly difficult to maintain the global temperature within the 1.5 - 2°C target set by the Paris Agreement. Therefore, strategies to remove carbon dioxide from the atmosphere are being developed, with ocean alkalinity enhancement (OAE) gaining most attention. Within OAE, ocean liming- the addition of quicklime (CaO) or hydrated lime (Ca(OH) 2 )- can not only remove CO 2 from the atmosphere but potentially counteract the effects of ocean acidification. Although quite attractive, these technologies have yet to be tested regarding ecological safety and efficacy. Here we report the impacts of ocean liming on the abundance, composition and extracellular enzymatic activity (EEA) rates of a North Atlantic planktonic community. The results demonstrate that OAE led to a decreased phytoplankton development, mainly diatoms. The bacterial response to OAE was community-specific, with a consistent increase in the relative abundance of the order Oceanospirillales. OAE also led to increased EEA rates, especially within the bacterial community. These findings suggest that while initial effects on phytoplankton may be limited, the specific impacts on bacterial groups suggest that OAE could influence the remineralization of organic matter. If our results apply to other communities, OAE might initially affect marine microbial dynamics, but further studies are needed to determine if these effects are long-term.

16S↗