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At least 55 records · Page 3

What causes the spread of model projections of ocean dynamic sea-level change in response to greenhouse gas forcing?

Abstract Sea levels of different atmosphere–ocean general circulation models (AOGCMs) respond to climate change forcing in different ways, representing a crucial uncertainty in climate change research. We isolate the role of the ocean dynamics in setting the spatial pattern of dynamic sea-level ( ζ ) change by forcing several AOGCMs with prescribed identical heat, momentum (wind) and freshwater flux perturbations. This method produces a ζ projection spread comparable in magnitude to the spread that results from greenhouse gas forcing, indicating that the differences in ocean model formulation are the cause, rather than diversity in surface flux change. The heat flux change drives most of the global pattern of ζ change, while the momentum and water flux changes cause locally confined features. North Atlantic heat uptake causes large temperature and salinity driven density changes, altering local ocean transport and ζ . The spread between AOGCMs here is caused largely by differences in their regional transport adjustment, which redistributes heat that was already in the ocean prior to perturbation. The geographic details of the ζ change in the North Atlantic are diverse across models, but the underlying dynamic change is similar. In contrast, the heat absorbed by the Southern Ocean does not strongly alter the vertically coherent circulation. The Arctic ζ change is dissimilar across models, owing to differences in passive heat uptake and circulation change. Only the Arctic is strongly affected by nonlinear interactions between the three air-sea flux changes, and these are model specific.

54 ENVIRONMENTAL SCIENCES↗

AeroCom Phase III Multi-Model Evaluation of the Aerosol Life Cycle and Optical Properties Using Ground and Space-Based Remote Sensing as Well as Surface In Situ Observations

Within the framework of the AeroCom (Aerosol Comparisons between Observations and Models) initiative, the state-of-the-art modelling of aerosol optical properties is assessed from 14 global models participating in the phase III control experiment (AP3). The models are similar to CMIP6/AerChemMIP Earth System Models (ESMs) and provide a robust multi-model ensemble. Inter-model spread of aerosol species lifetimes and emissions appears to be similar to that of mass extinction coefficients (MECs), suggesting that aerosol optical depth (AOD) uncertainties are associated with a broad spectrum of parameterised aerosol processes. Total AOD is approximately the same as in AeroCom phase I (AP1) simulations. However, we find a 50 % decrease in the optical depth (OD) of black carbon (BC), attributable to a combination of decreased emissions and lifetimes. Relative contributions from sea salt (SS) and dust (DU) have shifted from being approximately equal in AP1 to SS contributing about 2∕3 of the natural AOD in AP3. This shift is linked with a decrease in DU mass burden, a lower DU MEC, and a slight decrease in DU lifetime, suggesting coarser DU particle sizes in AP3 compared to AP1. Relative to observations, the AP3 ensemble median and most of the participating models underestimate all aerosol optical properties investigated, that is, total AOD as well as fine and coarse AOD (AODf, AODc), Ångström exponent (AE), dry surface scattering (SCdry), and absorption (ACdry) coefficients. Compared to AERONET, the models underestimate total AOD by ca. 21 % ± 20 % (as inferred from the ensemble median and interquartile range). Against satellite data, the ensemble AOD biases range from −37 % (MODIS-Terra) to −16 % (MERGED-FMI, a multi-satellite AOD product), which we explain by differences between individual satellites and AERONET measurements themselves. Correlation coefficients (R) between model and observation AOD records are generally high (R>0.75), suggesting that the models are capable of capturing spatio-temporal variations in AOD. We find a much larger underestimate in coarse AODc (∼ −45 % ± 25 %) than in fine AODf (∼ −15 % ± 25 %) with slightly increased inter-model spread compared to total AOD. These results indicate problems in the modelling of DU and SS. The AODc bias is likely due to missing DU over continental land masses (particularly over the United States, SE Asia, and S. America), while marine AERONET sites and the AATSR SU satellite data suggest more moderate oceanic biases in AODc. Column AEs are underestimated by about 10 % ± 16 %. For situations in which measurements show AE > 2, models underestimate AERONET AE by ca. 35 %. In contrast, all models (but one) exhibit large overestimates in AE when coarse aerosol dominates (bias ca. +140 % if observed AE < 0.5). Simulated AE does not span the observed AE variability. These results indicate that models overestimate particle size (or underestimate the fine-mode fraction) for fine-dominated aerosol and underestimate size (or overestimate the fine-mode fraction) for coarse-dominated aerosol. This must have implications for lifetime, water uptake, scattering enhancement, and the aerosol radiative effect, which we can not quantify at this moment. Comparison against Global Atmosphere Watch (GAW) in situ data results in mean bias and inter-model variations of −35 % ± 25 % and −20 % ± 18 % for SCdry and ACdry, respectively. The larger underestimate of SCdry than ACdry suggests the models will simulate an aerosol single scattering albedo that is too low. The larger underestimate of SCdry than ambient air AOD is consistent with recent findings that models overestimate scattering enhancement due to hygroscopic growth. The broadly consistent negative bias in AOD and surface scattering suggests an underestimate of aerosol radiative effects in current global aerosol models. Considerable inter-model diversity in the simulated optical properties is often found in regions that are, unfortunately, not or only sparsely covered by ground-based observations. This includes, for instance, the Sahara, Amazonia, central Australia, and the South Pacific. This highlights the need for a better site coverage in the observations, which would enable us to better assess the models, but also the performance of satellite products in these regions. Using fine-mode AOD as a proxy for present-day aerosol forcing estimates, our results suggest that models underestimate aerosol forcing by ca. −15 %, however, with a considerably large interquartile range, suggesting a spread between −35 % and +10 %.

space-based remote sensing↗

PSF–NET: A Nonparametric Point-spread Function Model for Ground-based Optical Telescopes

Ground-based optical telescopes are seriously affected by atmospheric turbulence induced aberrations. Understanding properties of these aberrations is important both for instrument design and image restoration method development. Because the point-spread function can reflect performance of the whole optic system, it is appropriate to use the point-spread function to describe atmospheric turbulence induced aberrations. Assuming point-spread functions induced by the atmospheric turbulence with the same profile belong to the same manifold space, we propose a nonparametric point-spread function—PSF–NET. The PSF–NET has a cycle convolutional neural network structure and is a statistical representation of the manifold space of PSFs induced by the atmospheric turbulence with the same profile. Testing the PSF–NET with simulated and real observation data, we find that a well trained PSF–NET can restore any short exposure images blurred by atmospheric turbulence with the same profile. Besides, we further use the impulse response of the PSF–NET, which can be viewed as the statistical mean PSF, to analyze interpretation properties of the PSF–NET. We find that variations of statistical mean PSFs are caused by variations of the atmospheric turbulence profile: as the difference of the atmospheric turbulence profile increases, the difference between statistical mean PSFs also increases. The PSF–NET proposed in this paper provides a new way to analyze atmospheric turbulence induced aberrations, which would benefit the development of new observation methods for ground-based optical telescopes.

79 ASTRONOMY AND ASTROPHYSICS↗

Estuarine density fronts and their effect on oil slicks

The author has identified the following significant results. Estuarine fronts represent regions of extremely high gradient or discontinuity in various parameters of physical interest, the most important being the water velocity and density fields. Aircraft and boats were combined to study the behavior of different types of fronts in Delaware Bay and their effect on pollutants in order to provide a basis for improving an oil drift and spreading model. Imagery from the LANDSAT satellites provided the most effective means of determining the location and extent of frontal systems over all portions of the tidal cycle. This data is being used to modify the oil drift and spreading model.

Klemas, V.↗

Remote sensing of estuarine fronts and their effects on pollutants

Estuarine fronts represent regions of extremely high gradient or discontinuity in various parameters of physical interest, the most important being the water velocity and density fields. Such fronts strongly influence pollutant dispersion by capturing oil slicks and other pollutants concentrated in surface films and drawing them down into the water column. Aircraft and boats were combined to study the behavior of different types of fronts in Delaware Bay and their effect on pollutants in order to provide a basis for improving an oil drift and spreading model. Imagery from the Landsat satellites provided the most effective means of determining the location and extent of frontal systems over all portions of the tidal cycle. This information is being used to modify the oil drift and spreading model.

Klemas, V.↗

Probabilistic Discrete‐Time Models for Spreading Processes in Complex Networks: A Review

Abstract Research into network dynamics of spreading processes typically employs both discrete and continuous time methodologies. Although each approach offers distinct insights, integrating them can be challenging, particularly when maintaining coherence across different time scales. This review focuses on the Microscopic Markov Chain Approach (MMCA), a probabilistic f ramework originally designed for epidemic modeling. MMCA uses discrete dynamics to compute the probabilities of individuals transitioning between epidemiological states. By treating each time step—usually a day—as a discrete event, the approach captures multiple concurrent changes within this time frame. The approach allows to estimate the likelihood of individuals or populations being in specific states, which correspond to distinct epidemiological compartments. This review synthesizes key findings from the application of this approach, providing a comprehensive overview of its utility in understanding epidemic spread.

Granell, Clara↗

Differentially Private Map Matching (DPMM) v1.0

Human mobility trajectories provide valuable information for developing mobility applications, as they contain diverse and rich information about the users. User mobility data is valuable for various applications such as intelligent transportation systems (ITS), commercial business models, and disease-spread models. However, such spatio-temporal traces may pose a threat to user privacy. GPS trajectories in their raw form are not suitable for transportation studies, as they require matching locations with nearest road links — a process called map-matching. This software implements a differential privacy (DP)-based map-matching algorithm, called DPMM, that generates link-level location trajectories in a privacy-preserving manner to protect users' origin destinations (OD) and travel paths. OD privacy is achieved by injecting Planar Laplace noise to the user OD GPS points. Travel-path privacy is provided with randomized travel path construction using exponential DP mechanism. The injected noise level is selected adaptively, by considering the link density of the location and the functional category of the localized links. For path privacy, our mechanism samples waypoints and selects candidate paths between waypoints. DPMM provides privacy effectively with respect to link density instead of other trajectory samples in the database compared to other privacy mechanisms. Compared to the different baseline models our DP-based privacy model offers closer query responses to the raw data in terms of individual and aggregate trajectory-level statistics with an average at absolute deviation from the baseline for individual statistics on ϵ = 1.0. Beyond individual trajectory statistics, the DPMM outperforms the other benchmark DP-based mechanisms on different aggregate statistics with up to 8x improvement in utility.

Peisert, Sean [Lawrence Berkeley National Laborato↗

A theoretical model of artificial spread F echoes

A theoretical model is developed for artificial spread F echoes elicited by irradiating the ionospheric F region with signals from ground-based HF transmitters. Account is taken of the irregularity polarizations, scale length and the magnetic dip angle of the echo. Ray tracing equations are defined for wave propagation in a horizontally stratified ionosphere which has been bathed with HF signals and therefore contains wavelike structures. Irregularities polarized within the meridian plane are found to cause the spread F echoes, while perpendicularly polarized irregularities do not. A magnetic dip angle of 5 deg must be exceeded for the spread F to become strong. The irregularities need scale lengths exceeding 100 m. Modes of operation are identified for inducing the required spread F echoes using ground-based radiotelescopes.

Kuo, S. P.↗

Improved Representation of Atmospheric Dynamics in CMIP6 Models Removes Climate Sensitivity Dependence on Hadley Cell Climatological Extent

The persistent inter-model spread in the response of global mean surface temperature to increased CO. (known as the “Equilibrium Climate Sensitivity”, or “ECS”) is a crucial problem across model generations. This work examines the influence of the models’ present-day atmospheric circulation climatologies, and the accompanying climatological cloud radiative effects, in explaining that spread. We analyze the Coupled Model Intercomparison Project Phase 6 (CMIP6) models and _nd that they simulate a more poleward, and thus more realistic, edge of the Hadley Circulation (HC) in the SouthernHemisphere than the CMIP5 models, although the climatological shortwave cloud radiative effects are similar in the two generations of models. A few CMIP5 models with extreme equatorward biases in the HC edge exhibited high ECS due to strong Southern midlatitude shortwave cloud radiative warming in response to climate change, suggesting an ECS dependence on HC position. We find that such constraint no longer holds for the CMIP6 models, due to absence of models with extreme HC climatologies. In spite of this, however, the CMIP6 models show an increased spread in ECS, with more models in the high ECS range. Additionally, an improved representation of the climatological jet dynamics does not lead to a new emergent constraint in the CMIP6 models either.

Equilibrium Climate Sensitivity↗

Osmotic forces and gap junctions in spreading depression: a computational model

In a computational model of spreading depression (SD), ionic movement through a neuronal syncytium of cells connected by gap junctions is described electrodiffusively. Simulations predict that SD will not occur unless cells are allowed to expand in response to osmotic pressure gradients and K+ is allowed to move through gap junctions. SD waves of [K+]out approximately 25 to approximately 60 mM moving at approximately 2 to approximately 18 mm/min are predicted over the range of parametric values reported in gray matter, with extracellular space decreasing up to approximately 50%. Predicted waveform shape is qualitatively similar to laboratory reports. The delayed-rectifier, NMDA, BK, and Na+ currents are predicted to facilitate SD, while SK and A-type K+ currents and glial activity impede SD. These predictions are consonant with recent findings that gap junction poisons block SD and support the theories that cytosolic diffusion via gap junctions and osmotic forces are important mechanisms underlying SD.

Spreading Cortical Depression/physiology↗

Assessment of the Pan-Arctic Accelerated Rate of Sea Ice Decline in CMIP6 Historical Simulations

Abstract Arctic sea ice loss in response to a warming climate is assessed in 42 models participating in phase 6 of the Coupled Model Intercomparison Project (CMIP6). Sea ice observations show a significant acceleration in the rate of decline commencing near the turn of the twenty-first century. It is our assertion that state-of-the-art climate models should qualitatively reflect this accelerated trend within the limitations of internal variability and observational uncertainty. Our analysis shows that individual CMIP6 simulations of sea ice depict a wide range of model spread on biases and anomaly trends both across models and among their ensemble members. While the CMIP6 multimodel mean captures the observed sea ice area (SIA) decline relatively well, an individual model’s ability to represent the acceleration in sea ice decline remains a challenge. Seventeen (40%) out of 42 CMIP6 models and 37 (13%) out of the total 286 ensemble members reasonably capture the observed trends and acceleration in SIA decline. In addition, a larger ensemble size appears to increase the odds for a model to include at least one ensemble member skillfully representing the accelerated SIA trends. Simulations of sea ice volume (SIV) show much larger spread and uncertainty than SIA; however, due to limited availability of sea ice thickness data, these are not as well constrained by observations. Finally, we find that models with more ocean heat transport simulate larger sea ice declines, which suggests an emergent constraint in CMIP6 ensembles. This relationship points to the need for better understanding and modeling of ice–ocean interactions, especially with respect to frazil ice growth.

54 ENVIRONMENTAL SCIENCES↗

Uncertainty in Twenty-First-Century CMIP5 Sea Level Projections

The representative concentration pathway (RCP) simulations included in phase 5 of the Coupled Model Intercomparison Project (CMIP5) quantify the response of the climate system to different natural and anthropogenic forcing scenarios. These simulations differ because of 1) forcing, 2) the representation of the climate system in atmosphere-ocean general circulation models (AOGCMs), and 3) the presence of unforced (internal) variability. Global and local sea level rise projections derived from these simulations, and the emergence of distinct responses to the four RCPs depend on the relative magnitude of these sources of uncertainty at different lead times. Here, the uncertainty in CMIP5 projections of sea level is partitioned at global and local scales, using a 164-member ensemble of twenty-first-century simulations. Local projections at New York City (NYSL) are highlighted. The partition between model uncertainty, scenario uncertainty, and internal variability in global mean sea level (GMSL) is qualitatively consistent with that of surface air temperature, with model uncertainty dominant for most of the twenty-first century. Locally, model uncertainty is dominant through 2100, with maxima in the North Atlantic and the Arctic Ocean. The model spread is driven largely by 4 of the 16 AOGCMs in the ensemble; these models exhibit outlying behavior in all RCPs and in both GMSL and NYSL. The magnitude of internal variability varies widely by location and across models, leading to differences of several decades in the local emergence of RCPs. The AOGCM spread, and its sensitivity to model exclusion and/or weighting, has important implications for sea level assessments, especially if a local risk management approach is utilized.

Variability↗

Arctic Sea Ice Simulation in the PlioMIP Ensemble

Eight general circulation models have simulated the mid-Pliocene warm period (mid-Pliocene, 3.264 to 3.025 Ma) as part of the Pliocene Modelling Intercomparison Project (PlioMIP). Here, we analyse and compare their simulation of Arctic sea ice for both the pre-industrial period and the mid-Pliocene. Mid-Pliocene sea ice thickness and extent is reduced, and the model spread of extent is more than twice the pre-industrial spread in some summer months. Half of the PlioMIP models simulate ice-free conditions in the mid-Pliocene. This spread amongst the ensemble is in line with the uncertainties amongst proxy reconstructions for mid-Pliocene sea ice extent. Correlations between mid-Pliocene Arctic temperatures and sea ice extents are almost twice as strong as the equivalent correlations for the pre-industrial simulations. The need for more comprehensive sea ice proxy data is highlighted, in order to better compare model performances.

simulation↗

Satellite Perspective of Aerosol Intercontinental Transport: From Qualitative Tracking to Quantitative Characterization

Evidence of aerosol intercontinental transport (ICT) is both widespread and compelling. Model simulations suggest that ICT could significantly affect regional air quality and climate, but the broad inter-model spread of results underscores a need of constraining model simulations with measurements. Satellites have inherent advantages over in situ measurements to characterize aerosol ICT, because of their spatial and temporal coverage. Significant progress in satellite remote sensing of aerosol properties during the Earth Observing System (EOS) era offers opportunity to increase quantitative characterization and estimates of aerosol ICT, beyond the capability of pre-EOS era satellites that could only qualitatively track aerosol plumes. EOS satellites also observe emission strengths and injection heights of some aerosols, aerosol precursors, and aerosol-related gases, which can help characterize aerosol ICT. After an overview of these advances, we review how the current generation of satellite measurements have been used to (1) characterize the evolution of aerosol plumes (e.g., both horizontal and vertical transport, and properties) on an episodic basis, (2) understand the seasonal and inter-annual variations of aerosol ICT and their control factors, (3) estimate the export and import fluxes of aerosols, and (4) evaluate and constrain model simulations. Substantial effort is needed to further explore an integrated approach using measurements from on-orbit satellites (e.g., A-Train synergy) for observational characterization and model constraint of aerosol intercontinental transport and to develop advanced sensors for future missions.

Yu, Hongbin↗

Evaluating Northern Hemisphere Growing Season Net Carbon Flux in Climate Models Using Aircraft Observations

Understanding terrestrial ecosystems and their response to anthropogenic climate change requires quantification of land-atmosphere carbon exchange. However, top-down and bottom-up estimates of large-scale land-atmosphere fluxes, including the northern extratropical growing season net flux (GSNF), show significant discrepancies. We developed a data-driven metric for the GSNF using atmospheric carbon dioxide concentration observations collected during the High-Performance Instrumented Airborne Platform for Environmental Research Pole-to-Pole Observations and Atmospheric Tomography Mission flight campaigns. This aircraft-derived metric is bias-corrected using three independent atmospheric inversion systems. We estimate the northern extratropical GSNF to be 5.7 ± 0.3 Pg C and use it to evaluate net biosphere productivity from the Coupled Model Intercomparison Project phase 5 and 6 (CMIP5 and CMIP6) models. While the model-to-model spread in the GSNF has decreased in the CMIP6 models relative to that of the CMIP5 models, there is still disagreement on the magnitude and timing of seasonal carbon uptake with most models underestimating the GSNF and overestimating the length of the growing season relative to the observations. We also use an emergent constraint approach to estimate annual northern extratropical gross primary productivity to be 56 ± 17 Pg C, heterotrophic respiration to be 25 ± 13 Pg C, and net primary productivity to be 28 ± 12 Pg C. The flux inferred from these aircraft observations provides an additional constraint on large-scale gross fluxes in prognostic Earth system models that may ultimately improve our ability to accurately predict carbon-climate feedbacks.

54 ENVIRONMENTAL SCIENCES↗

Identifying the sources of uncertainty in climate model simulations of solar radiation modification with the G6sulfur and G6solar Geoengineering Model Intercomparison Project (GeoMIP) simulations

We present here results from the Geoengineering Model Intercomparison Project (GeoMIP) simulations for the experiments G6sulfur and G6solar for six Earth system models participating in the Climate Model Intercomparison Project (CMIP) Phase 6. The aim of the experiments is to reduce the warming that results from a high-tier emission scenario (Shared Socioeconomic Pathways SSP5-8.5) to that resulting from a medium-tier emission scenario (SSP2-4.5). These simulations aim to analyze the response of climate models to a reduction in incoming surface radiation as a means to reduce global surface temperatures, and they do so either by simulating a stratospheric sulfate aerosol layer or, in a more idealized way, through a uniform reduction in the solar constant in the model. We find that over the final two decades of this century there are considerable inter-model spreads in the needed injection amounts of sulfate (29 ± 9 Tg-SO 2 /yr between 2081 and 2100), in the latitudinal distribution of the aerosol cloud and in the stratospheric temperature changes resulting from the added aerosol layer. Even in the simpler G6solar experiment, there is a spread in the needed solar dimming to achieve the same global temperature target (1.91 ± 0.44 %). The analyzed models already show significant differences in the response to the increasing CO 2 concentrations for global mean temperatures and global mean precipitation (2.05 K ± 0.42 K and 2.28 ± 0.80 %, respectively, for SSP5-8.5 minus SSP2-4.5 averaged over 2081–2100). With aerosol injection, the differences in how the aerosols spread further change some of the underlying uncertainties, such as the global mean precipitation response (–3.79 ± 0.76 % for G6sulfur compared to –2.07 ± 0.40 % for G6solar against SSP2-4.5 between 2081 and 2100). These differences in the behavior of the aerosols also result in a larger uncertainty in the regional surface temperature response among models in the case of the G6sulfur simulations, suggesting the need to devise various, more specific experiments to single out and resolve particular sources of uncertainty. The spread in the modeled response suggests that a degree of caution is necessary when using these results for assessing specific impacts of geoengineering in various aspects of the Earth system. However, all models agree that compared to a scenario with unmitigated warming, stratospheric aerosol geoengineering has the potential to both globally and locally reduce the increase in surface temperatures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Validation study of sodium pool fire modeling efforts in $\mathrm{MELCOR}$ and $\mathrm{SPHINCS}$ codes

Discharge of sodium coolant into containment from a sodium-cooled fast reactor vessel can occur in the event of a pipe leak or break. In this situation, some of the liquid sodium droplets discharged from the coolant system will react with oxygen in the air before reaching the containment. This phase of the event is normally termed the sodium spray fire phase. Unreacted sodium droplets pool on the containment floor where continued reaction with containment atmospheric oxygen occurs. This phase of the event is normally termed the sodium pool fire phase. Both phases of these sodium-oxygen reactions (or fires) are important to model because of the heat addition and aerosol generation that occur. Any fission products trapped in the sodium coolant may also be released during this progression of events, which if released from containment could pose a health risk to workers and the public. The paper describes progress of an international collaborative research in the area of the sodium fire modeling in the sodium-cooled fast reactors between the United States and Japan under the framework of the Civil Nuclear Energy Research and Development Working Group. In this collaboration between Sandia National Laboratories and Japan Atomic Energy Agency, the validation basis for and modeling capabilities of sodium spray and pool fires in MELCOR of Sandia National Laboratories and SPHINCS of Japan Atomic Energy Agency are being enhanced. Here this study documents MELCOR and SPHINCS sodium pool fire model validation exercises against the JAEA’s sodium pool fire experiments, F7-1 and F7-2. The proposed enhancement of the sodium pool fire models in MELCOR through addition of thermal hydraulic and sodium spreading models that enable a better representation of experimental results is also described.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

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↗