Goddard Earth Observing System Chemistry Research Articles

A Potential Surface Warming Regime for Volcanic Super‐Eruptions Through Stratospheric Water Vapor Increases

AbstractLarge volcanic eruptions are known to influence the climate through a variety of mechanisms including aerosol‐forced cooling and warming via emitted CO2. The January 2022 Hunga shallow underwater eruption caused an increase in stratospheric water vapor, and demonstrated how the associated positive radiative forcing can be an important component of an eruption's climate forcing. We present interactive stratospheric aerosol model simulations of super‐volcanic eruptions with a range of SO2 emissions that can produce climate warming through feedback effects produced by a large igneous province (or “flood basalt”) mid‐latitude super‐eruption using Goddard Earth Observing System Chemistry Climate Model climate model simulations. The model experiments suggest total SO2 emissions ≳4,000 Tg/4 Gt generate a multi‐year period of sustained aerosol absorptive local‐heating of the upper troposphere and lower stratosphere and hence produce net climate warming after strong initial cooling. The eruptions produce stratospheric water vapor increases of factors of 8–600. The initiation of these feedbacks within the simulations suggest they could occur for individual stratovolcano eruptions of the scale of the Toba or Tambora eruptions. We note the sensitivity of our results to volcanic sulfate aerosol microphysics and model chemistry.

Change in Tropospheric Ozone in the Recent Decades and Its Contribution to Global Total Ozone

AbstractTropospheric ozone is a key chemically active trace gas and radiative forcer. Understanding its long‐term changes is important to properly interpret observed changes in total column ozone and stratospheric ozone recovery. We investigate global and regional tropospheric ozone changes and their impact on total column ozone during 2005–2018 using satellite measurements and the NASA Goddard Earth Observing System Chemistry Climate Model (GEOSCCM). Global total ozone increased ∼4 DU during 2005–2018 (+0.28 ± 0.06 DU yr−1) as inferred from Ozone Monitoring Instrument (OMI). Consistent with previous studies, the OMI/MLS (Microwave Limb Sounder) derived global tropospheric ozone increased 2.2 DU during this period, 60% of the global total column ozone increase. While GEOSCCM reproduces reasonably well the total column increase, it overestimates the stratospheric ozone increase and underestimates the tropospheric ozone increase. We find that the tropospheric ozone increases are likely attributed to a growth of regional emissions of key ozone precursors, especially volatile organic compounds as reflected by the positive trends in formaldehyde (CH2O). Although carbon monoxide (CO) has been decreasing everywhere around the globe, it has relatively small impact on the tropospheric ozone trend. Trends in nitrogen dioxide (NO2) vary with regions, and these changes counteract or reinforce the positive effects of CH2O on the tropospheric ozone increases. The model underestimates the observed tropospheric ozone increase, especially over the US and Europe, because of underestimated NO2 emissions changes used in the model. The stratospheric ozone contribution increases during this period in the Northern Hemisphere and contributes to the tropospheric ozone increase.

Dynamical perturbation of the stratosphere by a pyrocumulonimbus injection of carbonaceous aerosols

Abstract. The Pacific Northwest Pyrocumulonimbus Event (PNE) took place in British Columbia during the evening and nighttime hours between 12 and 13 August 2017. Several pyroconvective clouds erupted on this occasion, and released in the upper troposphere and lower stratosphere unprecedented amounts of carbonaceous aerosols (300 ktn). Only a few years later, an even larger pyrocumulonimbus (pyroCb) injection took place over Australia. This event, named “the Australian New Year (ANY) event”, injected up to 1100 ktn of aerosol between 29 December 2019 and 4 January 2020. Such large injections of carbonaceous aerosol modify the stratospheric radiative budgets, locally perturbing stratospheric temperatures and winds. In this study, we use the Goddard Earth Observing System Chemistry Climate Model (GEOS CCM) to study the perturbations on the stratospheric meteorology induced by an aerosol injection of the magnitude of the PNE. Our simulations include the radiative interactions of aerosols, so that their impact on temperatures and winds are explicitly simulated. We show how the presence of the carbonaceous aerosols from the pyroCb causes the formation and maintenance of a synoptic-scale stratospheric anticyclone. We follow this disturbance considering the potential vorticity anomaly and the brown carbon aerosol loading and we describe its dynamical and thermodynamical structure and its evolution in time. The analysis presented here shows that the simulated anticyclone undergoes daily expansion–compression cycles governed by the radiative heating, which are directly related to the vertical motion of the plume, and that the aerosol radiative heating is essential in maintaining the anticyclone itself.

Regional‐Scale, Sector‐Specific Evaluation of Global CO2 Inversion Models Using Aircraft Data From the ACT‐America Project

AbstractWe use 148 airborne vertical profiles of CO2 for frontal cases from the summer 2016 Atmospheric Carbon and Transport—America (ACT‐America) campaign to evaluate the skill of 10 global CO2 in situ inversion models from the version 7 Orbiting Carbon Observatory–2 (OCO‐2) Model Intercomparison Project (MIP). Model errors (model posterior—observed CO2 dry air mole fractions) were categorized by region (Mid‐Atlantic, Midwest, and South), frontal sector (warm or cold), and transport model (predominantly Tracer Model 5 (TM5) and Goddard Earth Observing System—Chemistry [GEOS‐Chem]). All inversions assimilated the same CO2 observations. Overall, the median inversion profiles reproduce the general structures of the observations (enhanced/depleted low‐level CO2 in warm/cold sectors), but 1) they underestimate the magnitude of the warm/cold sector mole fraction difference, and 2) the spread among individual inversions can be quite large (>5 ppm). Uniquely in the Mid‐Atlantic, inversion biases segregated according to atmospheric transport model, where TM5 inversions biases were −3 to −4 ppm in warm sectors, while those of GEOS‐Chem were +2 to +3 ppm in cold sectors. The large spread among the mean posterior CO2 profiles is not explained by the different atmospheric transport models. These results show that the inversion systems themselves are the dominant cause of this spread, and that the aircraft campaign data are clearly able to identify these large biases. Future controlled experiments should identify which inversions best reproduce mid‐latitude CO2 mole fractions, and how inversion system components are linked to system performance.

Mechanisms Linked to Recent Ozone Decreases in the Northern Hemisphere Lower Stratosphere

AbstractPrevious studies have robustly identified a decrease since 1998 in lower stratospheric (LS) ozone in the Northern Hemisphere (NH). While this ozone decrease is qualitatively explained as resulting from changes in the large‐scale circulation, there is not yet a quantitative mechanistic explanation of these changes. Here, we explore the drivers of recent ozone changes using two different configurations of the Goddard Earth Observing System (GEOS) general circulation model. The first configuration of GEOS includes a full chemistry module and is constrained with meteorological fields from the Modern‐Era Retrospective Analysis for Research and Applications, Version 2 (MERRA‐2). This configuration (M2GMI) is used to analyze an idealized tracer that covaries closely with ozone on interannual and decadal timescales, revealing that recent ozone decreases in the NH subtropics are associated with a poleward expansion of upwelling in the NH LS, with reduced (enhanced) downwelling over northern subtropics (midlatitudes). The second configuration of GEOS is a free‐running version of the GEOS Chemistry Climate Model (CCM) that is used to perform a 10‐member ensemble of free‐running simulations. Comparisons of the two configurations reveal that, while the free‐running model can produce negative ozone changes in the NH LS, the magnitude of these changes is significantly weaker, relative to both M2GMI and MERRA‐2; moreover, these weaker ozone decreases are consistent with weaker simulated changes in the residual circulation. Finally, we examine the GEOS model results in the broader context of the hindcast simulations performed as part of Phase 1 of the Chemistry Climate Modeling Initiative. We show that the majority of the free‐running simulations considered here also exhibit weaker long‐term residual circulation changes, compared to reanalyses.

Boundary Layer Ozone Across the Indian Subcontinent: Who Influences Whom?

AbstractBoundary layer ozone (BLO3) over the Indian subcontinent (IS) can be region‐specific with consequences to health and pollution management strategies. The Goddard Earth Observing System‐Chemistry (GEOS‐Chem) model was used to estimate the contributions of eight IS regions on each other for BLO3. BLO3 in northern India, Pakistan, and Sri Lanka is mostly (~65‐70%) influenced by regions outside the subcontinent. Roughly 30% of BLO3 over eastern India is from within the IS, mostly from the Indo‐Gangetic Plain and central India (CI). Southern India is influenced by CI; however, it hardly influences other regions. Northern India and Sri Lanka regions are essentially isolated from other regions in the IS. The meteorology is the primary factor in the redistribution of BLO3 and its precursors. Our results highlight the emerging importance of CI to O3 pollution in addition to the Indo‐Gangetic Plain and shed light on potential strategies for O3 control in the IS.

Measurements of nitric oxide and ammonia soil fluxes from a wet savanna ecosystem site in West Africa during the DACCIWA field campaign

Abstract. Biogenic fluxes from soil at a local and regional scale are crucial to study air pollution and climate. Here we present field measurements of soil fluxes of nitric oxide (NO) and ammonia (NH3) observed over four different land cover types, i.e. bare soil, grassland, maize field, and forest, at an inland rural site in Benin, West Africa, during the DACCIWA field campaign in June and July 2016. At the regional scale, urbanization and a massive growth in population in West Africa have been causing a strong increase in anthropogenic emissions. Anthropogenic pollutants are transported inland and northward from the megacities located on the coast, where the reaction with biogenic emissions may lead to enhanced ozone production outside urban areas, as well as secondary organic aerosol formation, with detrimental effects on humans, animals, natural vegetation, and crops. We observe NO fluxes up to 48.05 ngN m−2 s−1. NO fluxes averaged over all land cover types are 4.79±5.59 ngN m−2 s−1, and maximum soil emissions of NO are recorded over bare soil. NH3 is dominated by deposition for all land cover types. NH3 fluxes range between −6.59 and 4.96 ngN m−2 s−1. NH3 fluxes averaged over all land cover types are -0.91±1.27 ngN m−2 s−1, and maximum NH3 deposition is measured over bare soil. The observations show high spatial variability even for the same soil type, same day, and same meteorological conditions. We compare point daytime average measurements of NO emissions recorded during the field campaign with those simulated by GEOS-Chem (Goddard Earth Observing System Chemistry Model) for the same site and find good agreement. In an attempt to quantify NO emissions at the regional and national scale, we also provide a tentative estimate of total NO emissions for the entire country of Benin for the month of July using two distinct methods: upscaling point measurements and using the GEOS-Chem model. The two methods give similar results: 1.17±0.6 and 1.44 GgN month−1, respectively. Total NH3 deposition estimated by upscaling point measurements for the month of July is 0.21 GgN month−1.

DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry

Abstract. The oxidation of dimethyl sulfide (DMS) in the troposphere and subsequent chemical conversion into sulfur dioxide (SO2) and methane sulfonic acid (MSA) are key processes for the formation and growth of sulfur-containing aerosol and cloud condensation nuclei (CCN), but are highly simplified in large-scale models of the atmosphere. In this study, we implement a series of gas-phase and multiphase sulfur oxidation mechanisms into the Goddard Earth Observing System-Chemistry (GEOS-Chem) global chemical transport model – including two important intermediates, dimethyl sulfoxide (DMSO) and methane sulphinic acid (MSIA) – to investigate the sulfur cycle in the global marine troposphere. We found that DMS is mainly oxidized in the gas phase by OH (66 %), NO3 (16 %) and BrO (12 %) globally. DMS + BrO is important for the model's ability to reproduce the observed seasonality of surface DMS mixing ratio in the Southern Hemisphere. MSA is mainly produced from multiphase oxidation of MSIA by OH(aq) (66 %) and O3(aq) (30 %) in cloud droplets and aerosols. Aqueous-phase reaction with OH accounts for only 12 % of MSA removal globally, and a higher MSA removal rate is needed to reproduce observations of the MSA ∕ nssSO42- ratio. The modeled conversion yield of DMS into SO2 and MSA is 75 % and 15 %, respectively, compared to 91 % and 9 % in the standard model run that includes only gas-phase oxidation of DMS by OH and NO3. The remaining 10 % of DMS is lost via deposition of intermediates DMSO and MSIA. The largest uncertainties for modeling sulfur chemistry in the marine boundary layer (MBL) are unknown concentrations of reactive halogens (BrO and Cl) and OH(aq) concentrations in cloud droplets and aerosols. To reduce uncertainties in MBL sulfur chemistry, we should prioritize observations of reactive halogens and OH(aq).

Effects of convective ice evaporation on interannual variability of tropical tropopause layer water vapor

Abstract. Water vapor interannual variability in the tropical tropopause layer (TTL) is investigated using satellite observations and model simulations. We break down the influences of the Brewer–Dobson circulation (BDC), the quasi-biennial oscillation (QBO), and the tropospheric temperature (ΔT) on TTL water vapor as a function of latitude and longitude using a two-dimensional multivariate linear regression. This allows us to examine the spatial distribution of the impact of each process on TTL water vapor. In agreement with expectations, we find that the impacts from the BDC and QBO act on TTL water vapor by changing TTL temperature. For ΔT, we find that TTL temperatures alone cannot explain the influence. We hypothesize a moistening role for the evaporation of convective ice from increased deep convection as the troposphere warms. Tests using a chemistry–climate model, the Goddard Earth Observing System Chemistry Climate Model (GEOSCCM), support this hypothesis.

Chemical Mechanisms and Their Applications in the Goddard Earth Observing System (GEOS) Earth System Model.

NASA's Goddard Earth Observing System (GEOS) Earth System Model (ESM) is a modular, general circulation model (GCM), and data assimilation system (DAS) that is used to simulate and study the coupled dynamics, physics, chemistry, and biology of our planet. GEOS is developed by the Global Modeling and Assimilation Office (GMAO) at NASA Goddard Space Flight Center. It generates near‐real‐time analyzed data products, reanalyses, and weather and seasonal forecasts to support research targeted to understanding interactions among Earth System processes. For chemistry, our efforts are focused on ozone and its influence on the state of the atmosphere and oceans, and on trace gas data assimilation and global forecasting at mesoscale discretization. Several chemistry and aerosol modules are coupled to the GCM, which enables GEOS to address topics pertinent to NASA's Earth Science Mission. This paper describes the atmospheric chemistry components of GEOS and provides an overview of its Earth System Modeling Framework (ESMF)‐based software infrastructure, which promotes a rich spectrum of feedbacks that influence circulation and climate, and impact human and ecosystem health. We detail how GEOS allows model users to select chemical mechanisms and emission scenarios at run time, establish the extent to which the aerosol and chemical components communicate, and decide whether either or both influence the radiative transfer calculations. A variety of resolutions facilitates research on spatial and temporal scales relevant to problems ranging from hourly changes in air quality to trace gas trends in a changing climate. Samples of recent GEOS chemistry applications are provided.

Impacts of Stratospheric Sulfate Geoengineering on Global Solar Photovoltaic and Concentrating Solar Power Resource

AbstractIn recent years, the idea of geoengineering, artificially modifying the climate to reduce global temperatures, has received increasing attention because of the lack of progress in reducing global greenhouse gas emissions. Stratospheric sulfate injection (SSI) is a geoengineering method proposed to reduce planetary warming by reflecting a proportion of solar radiation back into space that would otherwise warm the surface and lower atmosphere. The authors analyze results from the Met Office Hadley Centre Global Environment Model, version 2, Carbon Cycle Stratosphere (HadGEM2-CCS) climate model with stratospheric emissions of 10 Tg yr−1 of SO2, designed to offset global temperature rise by around 1°C. A reduction in concentrating solar power output of 5.9% on average over land is shown under SSI relative to a baseline future climate change scenario (RCP4.5) caused by a decrease in direct radiation. Solar photovoltaic energy is generally less affected as it can use diffuse radiation, which increases under SSI, at the expense of direct radiation. The results from HadGEM2-CCS are compared with the Goddard Earth Observing System Chemistry–Climate Model (GEOSCCM) from the Geoengineering Model Intercomparison Project (GeoMIP), with 5 Tg yr−1 emission of SO2. In many regions, the differences predicted in solar energy output between the SSI and RCP4.5 simulations are robust, as the sign of the changes for both HadGEM2-CCS and GEOSCCM agree. Furthermore, the sign of the total and direct annual mean radiation changes evaluated by HadGEM2-CCS agrees with the sign of the multimodel mean changes of an ensemble of GeoMIP models over the majority of the world.

Time-varying changes in the simulated structure of the Brewer–Dobson Circulation

Abstract. A series of simulations using the NASA Goddard Earth Observing System Chemistry Climate Model are analyzed in order to assess changes in the Brewer–Dobson Circulation (BDC) over the past 55 years. When trends are computed over the past 55 years, the BDC accelerates throughout the stratosphere, consistent with previous modeling results. However, over the second half of the simulations (i.e., since the late 1980s), the model simulates structural changes in the BDC as the temporal evolution of the BDC varies between regions in the stratosphere. In the mid-stratosphere in the midlatitude Northern Hemisphere, the BDC does not accelerate in the ensemble mean of our simulations despite increases in greenhouse gas concentrations and warming sea surface temperatures, and it even decelerates in one ensemble member. This deceleration is reminiscent of changes inferred from satellite instruments and in situ measurements. In contrast, the BDC in the lower stratosphere continues to accelerate. The main forcing agents for the recent slowdown in the mid-stratosphere appear to be declining ozone-depleting substance (ODS) concentrations and the timing of volcanic eruptions. Changes in both mean age of air and the tropical upwelling of the residual circulation indicate a lack of recent acceleration. We therefore clarify that the statement that is often made that climate models simulate a decreasing age throughout the stratosphere only applies over long time periods and is not necessarily the case for the past 25 years, when most tracer measurements were taken.

The impact of snow nitrate photolysis on boundary layer chemistry and the recycling and redistribution of reactive nitrogen across Antarctica and Greenland in a global chemical transport model

Abstract. The formation and recycling of reactive nitrogen (NO, NO2, HONO) at the air–snow interface has implications for air quality and the oxidation capacity of the atmosphere in snow-covered regions. Nitrate (NO3−) photolysis in snow provides a source of oxidants (e.g., hydroxyl radical) and oxidant precursors (e.g., nitrogen oxides) to the overlying boundary layer, and alters the concentration and isotopic (e.g., δ15N) signature of NO3− preserved in ice cores. We have incorporated an idealized snowpack with a NO3− photolysis parameterization into a global chemical transport model (Goddard Earth Observing System (GEOS) Chemistry model, GEOS-Chem) to examine the implications of snow NO3− photolysis for boundary layer chemistry, the recycling and redistribution of reactive nitrogen, and the preservation of ice-core NO3− in ice cores across Antarctica and Greenland, where observations of these parameters over large spatial scales are difficult to obtain. A major goal of this study is to examine the influence of meteorological parameters and chemical, optical, and physical snow properties on the magnitudes and spatial patterns of snow-sourced NOx fluxes and the recycling and redistribution of reactive nitrogen across Antarctica and Greenland. Snow-sourced NOx fluxes are most influenced by temperature-dependent quantum yields of NO3− photolysis, photolabile NO3− concentrations in snow, and concentrations of light-absorbing impurities (LAIs) in snow. Despite very different assumptions about snowpack properties, the range of model-calculated snow-sourced NOx fluxes are similar in Greenland (0.5–11 × 108 molec cm−2 s−1) and Antarctica (0.01–6.4 × 108 molec cm−2 s−1) due to the opposing effects of higher concentrations of both photolabile NO3− and LAIs in Greenland compared to Antarctica. Despite the similarity in snow-sourced NOx fluxes, these fluxes lead to smaller factor increases in mean austral summer boundary layer mixing ratios of total nitrate (HNO3+ NO3−), NOx, OH, and O3 in Greenland compared to Antarctica because of Greenland's proximity to pollution sources. The degree of nitrogen recycling in the snow is dependent on the relative magnitudes of snow-sourced NOx fluxes versus primary NO3− deposition. Recycling of snow NO3− in Greenland is much less than in Antarctica Photolysis-driven loss of snow NO3− is largely dependent on the time that NO3− remains in the snow photic zone (up to 6.5 years in Antarctica and 7 months in Greenland), and wind patterns that redistribute snow-sourced reactive nitrogen across Antarctica and Greenland. The loss of snow NO3− is higher in Antarctica (up to 99 %) than in Greenland (up to 83 %) due to deeper snow photic zones and lower snow accumulation rates in Antarctica. Modeled enrichments in ice-core δ15N(NO3−) due to photolysis-driven loss of snow NO3− ranges from 0 to 363 ‰ in Antarctica and 0 to 90 ‰ in Greenland, with the highest fraction of NO3− loss and largest enrichments in ice-core δ15N(NO3−) at high elevations where snow accumulation rates are lowest. There is a strong relationship between the degree of photolysis-driven loss of snow NO3− and the degree of nitrogen recycling between the air and snow throughout all of Greenland and in Antarctica where snow accumulation rates are greater than 130 kg m−2 a−1 in the present day.

Air-mass Origin in the Arctic. Part II: Response to Increases in Greenhouse Gases

Abstract Future changes in transport from Northern Hemisphere (NH) midlatitudes into the Arctic are examined using rigorously defined air-mass fractions that partition air in the Arctic according to where it last had contact with the planetary boundary layer (PBL). Boreal winter (December–February) and summer (June–August) air-mass fraction climatologies are calculated for the modeled climate of the Goddard Earth Observing System Chemistry–Climate Model (GEOSCCM) forced with the end-of-twenty-first century greenhouse gases and ozone-depleting substances. The modeled projections indicate that the fraction of air in the Arctic that last contacted the PBL over NH midlatitudes (or air of “midlatitude origin”) will increase by about 10% in both winter and summer. The projected increases during winter are largest in the upper and middle Arctic troposphere, where they reflect an upward and poleward shift in the transient eddy meridional wind, a robust dynamical response among comprehensive climate models. The boreal winter response is dominated by (~5%–10%) increases in the air-mass fractions originating over the eastern Pacific and the Atlantic, while the response in boreal summer mainly reflects (~5%) increases in air of Asian and North American origin. The results herein suggest that future changes in transport from midlatitudes may impact the composition—and, hence, radiative budget—in the Arctic, independent of changes in emissions.

Constraining black carbon aerosol over Asia using OMI aerosol absorption optical depth and the adjoint of GEOS-Chem

Abstract. Accurate estimates of the emissions and distribution of black carbon (BC) in the region referred to here as Southeastern Asia (70–150° E, 11° S–55° N) are critical to studies of the atmospheric environment and climate change. Analysis of modeled BC concentrations compared to in situ observations indicates levels are underestimated over most of Southeast Asia when using any of four different emission inventories. We thus attempt to reduce uncertainties in BC emissions and improve BC model simulations by developing top-down, spatially resolved, estimates of BC emissions through assimilation of OMI (Ozone Monitoring Instrument) observations of aerosol absorption optical depth (AAOD) with the GEOS-Chem (Goddard Earth Observing System – chemistry) model and its adjoint for April and October 2006. Overwhelming enhancements, up to 500 %, in anthropogenic BC emissions are shown after optimization over broad areas of Southeast Asia in April. In October, the optimization of anthropogenic emissions yields a slight reduction (1–5 %) over India and parts of southern China, while emissions increase by 10–50 % over eastern China. Observational data from in situ measurements and AERONET (Aerosol Robotic Network) observations are used to evaluate the BC inversions and assess the bias between OMI and AERONET AAOD. Low biases in BC concentrations are improved or corrected in most eastern and central sites over China after optimization, while the constrained model still underestimates concentrations in Indian sites in both April and October, possibly as a consequence of low prior emissions. Model resolution errors may contribute up to a factor of 2.5 to the underestimation of surface BC concentrations over northern India. We also compare the optimized results using different anthropogenic emission inventories and discuss the sensitivity of top-down constraints on anthropogenic emissions with respect to biomass burning emissions. In addition, the impacts of brown carbon, the formulation of the observation operator, and different a priori constraints on the optimization are investigated. Overall, despite these limitations and uncertainties, using OMI AAOD to constrain BC sources improves model representation of BC distributions, particularly over China.

Model-Simulated Atmospheric Carbon Dioxide: Comparisons with Satellite Retrievals and Ground-Based Observations

AbstractAtmospheric CO2 concentrations from January 2010 to December 2010 were simulated using the GEOS-Chem (Goddard Earth Observing System-Chemistry) model and the results were compared to satellite Gases Observing Satellite (GOSAT) and ground-based the Total Carbon Column Observing Network (TCCON) data. It was found that CO2 concentrations based on GOSAT satellite retrievals were generally higher than those simulated by GEOS-Chem. The differences over the land area in January and April ranged from 1 to 2 ppm, and there were major differences in June and August. At high latitudes in the Northern Hemisphere in June, as well as south of the Sahara, the difference was greater than 5 ppm. In the high latitudes of the Northern Hemisphere the model results were higher than the GOSAT retrievals, while in South America the satellite data were higher. The trend of the difference in the high latitudes of the Northern Hemisphere and the Saharan region in August was opposite to June. Maximum correlation coefficient...

Airmass Origin in the Arctic. Part I: Seasonality

Abstract The first climatology of airmass origin in the Arctic is presented in terms of rigorously defined airmass fractions that partition air according to where it last contacted the planetary boundary layer (PBL). Results from a present-day climate integration of the Goddard Earth Observing System Chemistry–Climate Model (GEOSCCM) reveal that the majority of air in the Arctic below 700 mb last contacted the PBL poleward of 60°N. By comparison, 62% (±0.8%) of the air above 700 mb originates over Northern Hemisphere midlatitudes (i.e., “midlatitude air”). Seasonal variations in the airmass fractions above 700 mb reveal that during boreal winter air from midlatitudes originates primarily over the oceans, with 26% (±1.9%) last contacting the PBL over the eastern Pacific, 21% (±0.87%) over the Atlantic, and 16% (±1.2%) over the western Pacific. During summer, by comparison, midlatitude air originates primarily over land, overwhelmingly so over Asia [41% (±1.0%)] and, to a lesser extent, over North America [24% (±1.5%)]. Seasonal variations in the airmass fractions are interpreted in terms of changes in the large-scale ventilation of the midlatitude boundary layer and the midlatitude tropospheric jet.

The importance of interstitial particle scavenging by cloud droplets in shaping the remote aerosol size distribution and global aerosol-climate effects

Abstract. In this paper, we investigate the coagulation of interstitial aerosol particles (particles too small to activate to cloud droplets) with cloud drops, a process often ignored in aerosol-climate models. We use the GEOS-Chem-TOMAS (Goddard Earth Observing System-Chemistry TwO-Moment Aerosol Sectional) global chemical transport model with aerosol microphysics to calculate the changes in the aerosol size distribution, cloud-albedo aerosol indirect effect, and direct aerosol effect due to the interstitial coagulation process. We find that inclusion of interstitial coagulation in clouds lowers total particle number concentrations by 15–21% globally, where the range is due to varying assumptions regarding activation diameter, cloud droplet size, and ice cloud physics. The interstitial coagulation process lowers the concentration of particles with dry diameters larger than 80 nm (a proxy for larger CCN) by 10–12%. These 80 nm particles are not directly removed by the interstitial coagulation but are reduced in concentration because fewer smaller particles grow to diameters larger than 80 nm. The global aerosol indirect effect of adding interstitial coagulation varies from +0.4 to +1.3 W m−2 where again the range depends on our cloud assumptions. Thus, the aerosol indirect effect of this process is significant, but the magnitude depends greatly on assumptions regarding activation diameter, cloud droplet size, and ice cloud physics. The aerosol direct effect of the interstitial coagulation process is minor (< 0.01 W m−2) due to the shift in the aerosol size distribution at sizes where scattering is most effective being small. We recommend that this interstitial scavenging process be considered in aerosol models when the size distribution and aerosol indirect effects are important.

Air‐mass origin in the tropical lower stratosphere: The influence of Asian boundary layer air

AbstractA climatology of air‐mass origin in the tropical lower stratosphere is presented for the Goddard Earth Observing System Chemistry Climate Model. During late boreal summer and fall, air‐mass fractions reveal that as much as 20% of the air in the tropical lower stratosphere last contacted the planetary boundary layer (PBL) over Asia; by comparison, the air‐mass fractions corresponding to last PBL contact over North America and over Europe are negligible. Asian air reaches the extratropical tropopause within a few days of leaving the boundary layer and is quasi‐horizontally transported into the tropical lower stratosphere, where it persists until January. The rapid injection of Asian air into the lower stratosphere—and its persistence in the deep tropics through late (boreal) winter—is important as industrial emissions over East Asia continue to increase. Hence, the Asian monsoon may play an increasingly important role in shaping stratospheric composition.

Quantifying pyroconvective injection heights using observations of fire energy: sensitivity of spaceborne observations of carbon monoxide

Abstract. We use observations of active fire area and fire radiative power (FRP) from the NASA Moderate Resolution Imaging Spectroradiometers (MODIS), together with a parameterized plume rise model, to estimate biomass burning injection heights during 2006. We use these injection heights in the GEOS-Chem (Goddard Earth Observing System Chemistry) atmospheric chemistry transport model to vertically distribute biomass burning emissions of carbon monoxide (CO) and to study the resulting atmospheric distribution. For 2006, we use over half a million FRP and fire area observations as input to the plume rise model. We find that convective heat fluxes and active fire area typically lie in the range of 1–100 kW m−2 and 0.001–100 ha, respectively, although in rare circumstances the convective heat flux can exceed 500 kW m−2. The resulting injection heights have a skewed probability distribution with approximately 80% of the injections remaining within the local boundary layer (BL), with occasional injection height exceeding 8 km. We do not find a strong correlation between the FRP-inferred surface convective heat flux and the resulting injection height, with environmental conditions often acting as a barrier to rapid vertical mixing even where the convective heat flux and active fire area are large. We also do not find a robust relationship between the underlying burnt vegetation type and the injection height. We find that CO columns calculated using the MODIS-inferred injection height (MODIS-INJ) are typically −9 to +6% different to the control calculation in which emissions are emitted into the BL, with differences typically largest over the point of emission. After applying MOPITT (Measurement of Pollution in the Troposphere) v5 scene-dependent averaging kernels we find that we are much less sensitive to our choice of injection height profile. The differences between the MOPITT and the model CO columns (max bias ~ 50%), due largely to uncertainties in emission inventories, are much larger than those introduced by the injection heights. We show that including a realistic diurnal variation in FRP (peaking in the afternoon) or accounting for subgrid-scale emission errors does not alter our main conclusions. Finally, we use a Bayesian maximum a posteriori approach constrained by MOPITT CO profiles to estimate the CO emissions but because of the inherent bias between model and MOPITT we find little impact on the resulting emission estimates. Studying the role of pyroconvection in the distribution of gases and particles in the atmosphere using global MOPITT CO observations (or any current spaceborne measurement of the atmosphere) is still associated with large errors, with the exception of a small subset of large fires and favourable environmental conditions, which will consequently lead to a bias in any analysis on a global scale.