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Quantifying the carbonyl sulfide (OCS) land/ocean fluxes contributes to the understanding of both the sulfur and carbon cycles. The primary sources and sinks of OCS are very likely in a steady state because there is no significant observed trend or interannual variability in atmospheric OCS measurements. However, the magnitude and spatial distribution of the dominant ocean source are highly uncertain due to the lack of observations. In particular, estimates of the oceanic fluxes range from approximately 280 Gg S yr-1 to greater than 800 Gg S yr-1, with the larger flux needed to balance a similarly sized terrestrial sink that is inferred from NOAA continental sites. Here we estimate summer tropical oceanic fluxes of OCS in 2006 using a linear flux inversion algorithm and new OCS data acquired by the Aura Tropospheric Emissions Spectrometer (TES). Modeled OCS concentrations based on these updated fluxes are consistent with HIAPER Pole-to-Pole Observations during 4th airborne campaign and improve significantly over the a priori model concentrations. The TES tropical ocean estimate of 70±16GgS in June,when extrapolated over the whole year (about 840 ± 192 Gg S yr-1), supports the hypothesis proposed by Berry et al. (2013) that the ocean flux is in the higher range of approximately 800 Gg S yr-1.

We use an inorganic aerosol thermodynamic equilibrium model in a three-dimensional chemical transport model to understand the roles of ammonia chemistry and natural aerosols on the global distribution of aerosols. The thermodynamic equilibrium model partitions gas-phase precursors among modeled aerosol species self-consistently with ambient relative humidity and natural and anthropogenic aerosol emissions during the 1990s.Model simulations show that accounting for aerosol inorganic thermodynamic equilibrium, ammonia chemistry and dust and sea-salt aerosols improve agreement with observed SO4, NO3, and NH4 aerosols especially at North American sites. This study shows that the presence of sea salt, dust aerosol and ammonia chemistry significantly increases sulfate over polluted continental regions. In all regions and seasons, representation of ammonia chemistry is required to obtain reasonable agreement between modeled and observed sulfate and nitrate concentrations. Observed and modeled correlations of sulfate and nitrate with ammonium confirm that the sulfate and nitrate are strongly coupled with ammonium. SO4concentrations over East China peak in winter, while North American SO4 peaks in summer. Seasonal variations of NO3 and SO4 are the same in East China. In North America, the seasonal variation is much stronger for NO3 than SO4 and peaks in winter.Natural sea salt and dust aerosol significantly alter the regional distributions of other aerosols in three main ways. First, they increase sulfate formation by 10–70% in polluted areas. Second, they increase modeled nitrate over oceans and reduce nitrate over Northern hemisphere continents. Third, they reduce ammonium formation over oceans and increase ammonium over Northern Hemisphere continents. Comparisons of SO4, NO3 and NH4 deposition between pre-industrial, present, and year 2100 scenarios show that the present NO3and NH4 deposition are twice pre-industrial deposition and present SO4 deposition is almost five times pre-industrial deposition.

The Goddard Chemistry Aerosol Radiation and Transport (GOCART) model, which controls the sources, sinks, and chemistry of aerosols within the Goddard Earth Observing System (GEOS), recently underwent a major refactoring and update, including a revision of the emissions datasets and the addition of brown carbon. A 4-year benchmark simulation utilizing the new version of the model code, termed GOCART Second Generation (GOCART-2G) and coupled to the Goddard Earth Observing System (GEOS) model, was evaluated using in situ and spaceborne measurements to develop a baseline and prioritize future development. A comparison of simulated aerosol optical depth between GOCART-2G and MODIS retrievals indicates the model captures the overall spatial pattern and seasonal cycle of aerosol optical depth but overestimates aerosol extinction over dusty regions and underestimates aerosol extinction over Northern Hemisphere boreal forests, requiring further investigation and tuning of emissions. This MODIS-based analysis is corroborated by comparisons to MISR and selected AERONET stations; however, discrepancies between the Aqua and Terra satellites indicate there is a diurnal component to biases in aerosol optical depth over southern Asia and northern Africa. Despite the underestimate of aerosol optical depth in biomass burning regions in GEOS, there is an overestimate in the surface mass of organic carbon in the United States, especially during the summer months. Over Europe, GOCART-2G is unable to match the summertime peak in aerosol optical depth, opposing the observed late fall and early spring peaks in surface mass concentration. A comparison of the vertical profile of attenuated backscatter to observations from CALIPSO indicates the GEOS model is capable of capturing the vertical profile of aerosol; however, the mid-troposphere plumes of dust in the North Atlantic and smoke in the southeastern Atlantic are perhaps too low in altitude. The results presented highlight priorities for future development with GOCART-2G, including improvements for dust, biomass burning aerosols, and anthropogenic aerosols. [ABSTRACT FROM AUTHOR]

We investigate the influence of mineral dust on tropospheric chemistry in the present climate at the global scale. The analysis examines the effects of dust on photolysis and heterogeneous uptake, operating independently and together. In numerical experiments the size-resolved, time-varying mineral dust distribution predicted by the global Dust Entrainment and Deposition (DEAD) model perturbs the gas phase species in a global chemical transport model (University of California at Irvine (UCI) CTM). We find that the photolysis perturbation dominates limited regions in the low to middle troposphere, while heterogeneous uptake dominates the rest of atmosphere. Coupling of the photochemical and heterogeneous effects of dust is weak in the global mean but moderate in dusty regions, where coupling is sometimes responsible for more than 20% of local O3 changes. Ozone and odd-nitrogen concentrations are perturbed in opposite directions by photolysis and heterogeneous chemistry, resulting in a weak net change. However, both processes decrease the concentrations of OH and HO2. The global mean change due to dust is −0.7% for tropospheric O3, −11.1% for OH, −5.2% for HO2, and −3.5% for HNO3. Large seasonal signals are present near dust source regions. Over the North African region and tropical Atlantic Ocean downwind, OH decreases by −66.8%, six times more than the global mean reduction. Interestingly, net photolysis-induced annual mean O3 changes are greater in the Southern Hemisphere than in the Northern Hemisphere, where significantly more dust and O3 precursors reside. In polar regions, O3 change is dominated by transported O3 and is not sensitive to local dust concentration. O3 change due to photolysis depends not only on dust vertical structure but also on the availability of O3 precursors. O3 change due to heterogeneous reactions on dust is sensitive to dust vertical structure, mainly through the influence of temperature on uptake rates.

Aerosols affect the global budgets of O3, OH, and CH4 in part through their alteration of photolysis rates and in part through their direct chemical interactions with gases (i.e., “heterogeneous chemistry”). The first effect is evaluated here with a global tropospheric chemistry transport model using recently developed global climatologies of tropospheric aerosols: a satellite-derived aerosol climatology over the oceans by advanced very high resolution radiometer and a model-generated climatology for land plus oceans by the Center for Climate System Research. Globally averaged, the impact of aerosols on photolysis alone is to increase tropospheric O3 by 0.63 Dobson units and increase tropospheric CH4 by 130 ppb (via tropospheric OH decreases of 8%). These greenhouse gas increases lead to an aerosol indirect effect (counting both natural and anthropogenic aerosols) of +0.08 W/m2. Although the CH4 increases are, of course, global, the changes in tropospheric OH and O3 are mainly regional, with the largest impacts in northwest Africa for January and in India and southern Africa for July. The influence of aerosols is greater in July than in January and greater in the Northern Hemisphere than in the Southern Hemisphere, as expected given the pollution sources in the Northern Hemisphere. The predominant impact is due to the aerosols over land; aerosols over the ocean contribute less than a third to globally integrated changes.

Modeling photochemistry in the stratosphere requires solution of the equationof radiative transfer over an extreme range of wavelengths and atmosphericconditions, from transmission through the Schumann–Runge bands ofO2 in the mesosphere, to multiple scattering from troposphericclouds and aerosols. The complexity and range of conditions makes photolysiscalculations in 3-D chemical transport models computationally expensive. Thisstudy pesents a fast and accurate numerical method, Fast-J2, for calculatingphotolysis rates (J-values) and the deposition of solar flux in stratosphere.Fast-J2 develops an optimized, super-wide 11-bin quadrature for wavelengthsfrom 177 to 291 nm that concatenates with the 7-bin quadrature (291–850nm) already developed for the troposphere as Fast-J. Below 291 nm the effectsof Rayleigh scattering are implemented as a pseudo-absorption, and above 291nm the full multiple-scattering code of Fast-J is used. Fast-J2 calculates themean ultraviolet-visible radiation field for these 18 wavelength binsthroughout the stratosphere, and thus new species and new cross sections canbe readily implemented. In comparison with a standard, high-resolution,multiple-scattering photolysis model, worst-case errors in Fast-J2 do notexceed 5% over a wide range of solar zenith angles, altitudes(0–60 km), latitudes, and seasons where the rates are important inphotochemistry.

Monthly skeletal stable isotope measurements of a Porites australiensis coral from Abraham Reef, Australia, spanning the period from 1981 to 1991, are compared with monthly averaged SST (sea surface temperature) from satellite collected AVHRR (Advanced Very High Resolution Radiometer) and monthly downward surface short-wave insolation (SSI) measurements. We found that the δ18O values varied as a function of the change in seawater temperature. There were anomalously high δ18O values in coral that grew during the summer season of the three El Niño events 1982–83, 1987, and 1991. Advection of seawater with higher salinity (and higher δ18O values) to our site or discrepancies between ocean skin temperature and mixed layer SST are likely reasons for the reduced resolution of δ18O-based SST. Increased coral δ13C values occurred simultaneously with increases in SSI. During most El Niño events the maximum and minimum δ13C values were lower than during normal years.

The sulfur cycle plays a key role in atmospheric air quality, climate, and ecosystems. In this study, we compare the spatial and temporal distribution of four sulfur-containing species, dimethyl sulfide (DMS), sulfur dioxide (SO2), particulate methanesulfonate (MSA), and particulate sulfate (SO4), that were measured during the airborne NASA Atmospheric Tomography (ATom) mission and simulated by five AeroCom-III models to analyze the budget of sulfur cycle from the models. This study focuses on remote regions over the Pacific, Atlantic, and Southern Oceans from near the ocean surface to ~12-km altitude range, and covers all four seasons. These regions provide us with highly heterogeneous natural and anthropogenic source environments, which is not usually the case for traditional continental studies. We examine the vertical and seasonal variations of these sulfur species over tropical, mid-, and high-latitude regions in both hemispheres. We identify their origins from land versus ocean and from anthropogenic versus natural sources with sensitivity studies by applying tagged tracers linking to emission types and regions. In general, the differences among model results can be greater than one-order of magnitude. Comparing with observations, simulated SO2 is generally low while SO4 is high, and the model-observation agreement is much better in ATom-4 (April–May, 2018). There are much larger DMS concentrations simulated close to the sea surface than observed, indicating that the DMS emissions may be too high from all models. Anthropogenic emissions are the dominant source (40–60 % of the total amount) for atmospheric sulfate simulated at locations and times along the ATom flight tracks at almost every altitude, followed by volcanic emissions (18–32 %) and oceanic sources (16–32 %). Similar source contributions can also be derived at broad ocean basin and monthly scales, indicating that any reductions of anthropogenic sulfur emissions would have global impacts in modern times. [ABSTRACT FROM AUTHOR]

Anthropogenic emissions of aerosols and precursor compounds are known to significantly affect the energy balance of the Earth-atmosphere system, alter the formation of clouds and precipitation, and have substantial impact on human health and the environment. Global models are an essential tool for examining the impacts of these emissions. In this study, we examine the sensitivity of model results to the assumed height of SO2 injection, seasonality of SO2 and BC emissions, and the assumed fraction of SO2 emissions that is injected into the atmosphere as SO4 in 11 climate and chemistry models, including both chemical transport models and the atmospheric component of Earth system models. We find a large variation in atmospheric lifetime across models for SO2, SO4, and BC, with a particularly large relative variation for SO2, which indicates that fundamental aspects of atmospheric sulfur chemistry remain uncertain. Of the perturbations examined in this study, the assumed height of SO2 injection had the largest overall impacts, particularly on global mean net radiative flux (maximum difference of -0.35 W m-2), SO2 lifetime over northern hemisphere land (maximum difference of 0.8 days), surface SO2 concentration (up to 59 % decrease), and surface sulfate concentration (up to 23 % increase). Emitting SO2 at height consistently increased SO2 and SO4 column burdens and shortwave cooling, with varying magnitudes, but had inconsistent effects across models on the sign of the change in implied cloud forcing. The assumed SO4 emission fraction also had a significant impact on net radiative flux and surface sulfate concentration. Because these properties are not standardized across models this is a source of inter-model diversity typically neglected in model intercomparisons. These results imply a need to assure that anthropogenic emission injection height and SO4 emission fraction are accurately and consistently represented in global models. [ABSTRACT FROM AUTHOR]