A data assimilation system has been developed to estimate global nitrogen oxides (NOx ) emissions using OMI tropospheric NO2 columns (DOMINO product) and a global chemical transport model (CTM), the ...Chemical Atmospheric GCM for Study of Atmospheric Environment and Radiative Forcing (CHASER). The data assimilation system, based on an ensemble Kalman filter approach, was applied to optimize daily NOx emissions with a horizontal resolution of 2.8° during the years 2005 and 2006. The background error covariance estimated from the ensemble CTM forecasts explicitly represents non-direct relationships between the emissions and tropospheric columns caused by atmospheric transport and chemical processes. In comparison to the a priori emissions based on bottom-up inventories, the optimized emissions were higher over eastern China, the eastern United States, southern Africa, and central-western Europe, suggesting that the anthropogenic emissions are mostly underestimated in the inventories. In addition, the seasonality of the estimated emissions differed from that of the a priori emission over several biomass burning regions, with a large increase over Southeast Asia in April and over South America in October. The data assimilation results were validated against independent data: SCIAMACHY tropospheric NO2 columns and vertical NO2 profiles obtained from aircraft and lidar measurements. The emission correction greatly improved the agreement between the simulated and observed NO2 fields; this implies that the data assimilation system efficiently derives NOx emissions from concentration observations. We also demonstrated that biases in the satellite retrieval and model settings used in the data assimilation largely affect the magnitude of estimated emissions. These dependences should be carefully considered for better understanding NOx sources from top-down approaches.
We examine contributions from various source regions to global distributions and budgets of tropospheric ozone (O3) in the context of intercontinental transport, using tagged tracer simulation with a ...global chemical transport model. For tagging O3, we consider regional separation of the model domain on the basis of the distributions of O3 chemical production. We define 14 polluted source regions (14 tracers) in the boundary layer (North America, Europe, China, etc.) and 8 regions (8 tracers) in the free troposphere; O3 production in the remaining (remote) tropospheric region and O3 transport from the stratosphere are also tagged as separate tracers. O3 transport from the polluted source regions like North America, Europe, and Asia generally accounts for more than 40% of ozone abundances even in remote locations. O3 exports from boundary layer in China and Asian free troposphere are discerned through much of the Northern Hemisphere, suggesting significant and extensive impacts of eastern Asian pollution. In particular, O3 from Asian free troposphere plays the most important roles in distribution and seasonal variation of O3 in the middle‐upper troposphere almost globally. In June–September, the model calculates a large O3 contribution (5–10 ppbv) from Asian free troposphere in the upper troposphere over the South Pacific associated with long‐range interhemispheric transport from Asia to the southern midlatitudes (via the western Indian Ocean, Africa, and Atlantic) in the upper troposphere. O3 transported from biomass burning regions such as South America, Africa, and Australia widely distributes in the Southern Hemisphere. Our simulation demonstrates that there is a significant interhemispheric O3 transport from South America to the northern midlatitudes in the upper troposphere which reaches Japan, North Pacific, and the United States in conjunction with O3 export from North Africa. Our tagged O3 simulation estimates that the annual mean global tropospheric O3 burden, as calculated to be 344 Tg in this study, comes from chemical production in the source regions (48%) and in the remote regions (29%) and from stratosphere‐troposphere exchange (23%).
We present the results from an 8-year tropospheric chemistry reanalysis for the period 2005-2012 obtained by assimilating multiple data sets from the OMI, MLS, TES, and MOPITT satellite instruments. ...The reanalysis calculation was conducted using a global chemical transport model and an ensemble Kalman filter technique that simultaneously optimises the chemical concentrations of various species and emissions of several precursors. The optimisation of both the concentration and the emission fields is an efficient method to correct the entire tropospheric profile and its year-to-year variations, and to adjust various tracers chemically linked to the species assimilated. Comparisons against independent aircraft, satellite, and ozonesonde observations demonstrate the quality of the analysed O3, NO2, and CO concentrations on regional and global scales and for both seasonal and year-to-year variations from the lower troposphere to the lower stratosphere. The data assimilation statistics imply persistent reduction of model error and improved representation of emission variability, but they also show that discontinuities in the availability of the measurements lead to a degradation of the reanalysis. The decrease in the number of assimilated measurements increased the ozonesonde-minus-analysis difference after 2010 and caused spurious variations in the estimated emissions. The Northern/Southern Hemisphere OH ratio was modified considerably due to the multiple-species assimilation and became closer to an observational estimate, which played an important role in propagating observational information among various chemical fields and affected the emission estimates. The consistent concentration and emission products provide unique information on year-to-year variations in the atmospheric environment.
The global source of lightning-produced NOx (LNOx ) is estimated by assimilating observations of NO2 , O3 , HNO3 , and CO measured by multiple satellite measurements into a chemical transport model. ...Included are observations from the Ozone Monitoring Instrument (OMI), Microwave Limb Sounder (MLS), Tropospheric Emission Spectrometer (TES), and Measurements of Pollution in the Troposphere (MOPITT) instruments. The assimilation of multiple chemical data sets with different vertical sensitivity profiles provides comprehensive constraints on the global LNOx source while improving the representations of the entire chemical system affecting atmospheric NOx , including surface emissions and inflows from the stratosphere. The annual global LNOx source amount and NO production efficiency are estimated at 6.3 Tg N yr-1 and 310 mol NO flash-1 , respectively. Sensitivity studies with perturbed satellite data sets, model and data assimilation settings lead to an error estimate of about 1.4 Tg N yr-1 on this global LNOx source. These estimates are significantly different from those estimated from a parameter inversion that optimizes only the LNOx source from NO2 observations alone, which may lead to an overestimate of the source adjustment. The total LNOx source is predominantly corrected by the assimilation of OMI NO2 observations, while TES and MLS observations add important constraints on the vertical source profile. The results indicate that the widely used lightning parameterization based on the C-shape assumption underestimates the source in the upper troposphere and overestimates the peak source height by up to about 1 km over land and the tropical western Pacific. Adjustments are larger over ocean than over land, suggesting that the cloud height dependence is too weak over the ocean in the Price and Rind (1992) approach. The significantly improved agreement between the analyzed ozone fields and independent observations gives confidence in the performance of the LNOx source estimation.
This study investigates ozone changes and the individual impacts of transport and chemistry on those changes. We specifically examine (1) variation related to El Niño Southern Oscillation, which is a ...dominant mode of interannual variation of tropospheric ozone, and (2) long‐term change between the 2000s and 2100s. During El Niño, the simulated ozone shows an increase (1 ppbv/K) over Indonesia, a decrease (2–10 ppbv/K) over the eastern Pacific in the tropical troposphere, and an increase (50 ppbv/K) over the eastern Pacific in the midlatitude lower stratosphere. These variations fundamentally agree with those observed by Microwave Limb Sounder/Tropospheric Emission Spectrometer instruments. The model demonstrates that tropospheric chemistry has a strong impact on the variation over the eastern Pacific in the tropical lower troposphere and that transport dominates the variation in the midlatitude lower stratosphere. Between the 2000s and 2100s, the model predicts an increase in the global burden of stratospheric ozone (0.24%/decade) and a decrease in the global burden of tropospheric ozone (0.82%/decade). The increase in the stratospheric burden is controlled by stratospheric chemistry. Tropospheric chemistry reduces the tropospheric burden by 1.07%/decade. However, transport (i.e., stratosphere‐troposphere exchange and tropospheric circulation) causes an increase in the burden (0.25%/decade). Additionally, we test the sensitivity of ozone changes to increased horizontal resolution of the representation of atmospheric circulation and advection apart from any aspects of the nonlinearity of chemistry sensitivity to horizontal resolution. No marked difference is found in medium‐resolution or high‐resolution simulations, suggesting that the increased horizontal resolution of transport has a minor impact.
Key Points
Roles of transport and chemistry in ozone changes are investigated
Transport and chemistry play important roles in ENSO‐related ozone variation
Future change in tropospheric ozone is caused by transport as well as chemistry
An earth system model (MIROC-ESM 2010) is fully described in terms of each model component and their interactions. Results for the CMIP5 (Coupled Model Inter-comparison Project phase 5) historical ...simulation are presented to demonstrate the model's performance from several perspectives: atmosphere, ocean, sea-ice, land-surface, ocean and terrestrial biogeochemistry, and atmospheric chemistry and aerosols. An atmospheric chemistry coupled version of MIROC-ESM (MIROC-ESM-CHEM 2010) reasonably reproduces transient variations in surface air temperatures for the period 1850-2005, as well as the present-day climatology for the zonal-mean zonal winds and temperatures from the surface to the mesosphere. The historical evolution and global distribution of column ozone and the amount of tropospheric aerosols are reasonably simulated in the model based on the Representative Concentration Pathways' (RCP) historical emissions of these precursors. The simulated distributions of the terrestrial and marine biogeochemistry parameters agree with recent observations, which is encouraging to use the model for future global change projections.
The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) examined the short-lived drivers of climate change in current climate models. Here we evaluate the 10 ACCMIP models that ...included aerosols, 8 of which also participated in the Coupled Model Intercomparison Project phase 5 (CMIP5). The models reproduce present-day total aerosol optical depth (AOD) relatively well, though many are biased low. Contributions from individual aerosol components are quite different, however, and most models underestimate east Asian AOD. The models capture most 1980–2000 AOD trends well, but underpredict increases over the Yellow/Eastern Sea. They strongly underestimate absorbing AOD in many regions. We examine both the direct radiative forcing (RF) and the forcing including rapid adjustments (effective radiative forcing; ERF, including direct and indirect effects). The models' all-sky 1850 to 2000 global mean annual average total aerosol RF is (mean; range) −0.26 W m−2; −0.06 to −0.49 W m−2. Screening based on model skill in capturing observed AOD yields a best estimate of −0.42 W m−2; −0.33 to −0.50 W m−2, including adjustment for missing aerosol components in some models. Many ACCMIP and CMIP5 models appear to produce substantially smaller aerosol RF than this best estimate. Climate feedbacks contribute substantially (35 to −58%) to modeled historical aerosol RF. The 1850 to 2000 aerosol ERF is −1.17 W m−2; −0.71 to −1.44 W m−2. Thus adjustments, including clouds, typically cause greater forcing than direct RF. Despite this, the multi-model spread relative to the mean is typically the same for ERF as it is for RF, or even smaller, over areas with substantial forcing. The largest 1850 to 2000 negative aerosol RF and ERF values are over and near Europe, south and east Asia and North America. ERF, however, is positive over the Sahara, the Karakoram, high Southern latitudes and especially the Arctic. Global aerosol RF peaks in most models around 1980, declining thereafter with only weak sensitivity to the Representative Concentration Pathway (RCP). One model, however, projects approximately stable RF levels, while two show increasingly negative RF due to nitrate (not included in most models). Aerosol ERF, in contrast, becomes more negative during 1980 to 2000. During this period, increased Asian emissions appear to have a larger impact on aerosol ERF than European and North American decreases due to their being upwind of the large, relatively pristine Pacific Ocean. There is no clear relationship between historical aerosol ERF and climate sensitivity in the CMIP5 subset of ACCMIP models. In the ACCMIP/CMIP5 models, historical aerosol ERF of about −0.8 to −1.5 W m−2 is most consistent with observed historical warming. Aerosol ERF masks a large portion of greenhouse forcing during the late 20th and early 21st century at the global scale. Regionally, aerosol ERF is so large that net forcing is negative over most industrialized and biomass burning regions through 1980, but remains strongly negative only over east and southeast Asia by 2000. Net forcing is strongly positive by 1980 over most deserts, the Arctic, Australia, and most tropical oceans. Both the magnitude of and area covered by positive forcing expand steadily thereafter.
This study investigates the role of aerosol microphysics in stratospheric sulfate aerosol changes after the 1991 Mount Pinatubo eruption using an atmospheric general circulation model that is coupled ...interactively with a chemistry module and a modal aerosol microphysical module with three modes. Our model can reproduce the global mean stratospheric aerosol optical depth (SAOD) observed by the Stratospheric Aerosol and Gas Experiment (SAGE) II during June 1991 to January 1993. The model underestimates the observed SAOD before the eruption and after January 1993. The model also underestimates the integrated backscatter coefficient observed by ground‐based lidar at Tsukuba, Naha, and Lauder. The modeled effective radius becomes larger (about 0.5 μm) and agrees with the balloon‐borne measurements at Laramie, Wyoming (41°N, 105°W). We further investigate effects of the inclusion of evaporation along with the condensation processes and the inclusion of van der Waals and viscous forces in the coagulation processes. The inclusion of evaporation along with the condensation processes reduces the global mean effective radius by up to 0.04 μm and increases the global burden of stratospheric sulfate aerosols (about 15% in late 1993). The inclusion of van der Waals and viscous forces in the coagulation processes increases the global mean effective radius by up to 0.06–0.07 μm and decreases the global burden (15–30% in late 1993). The effects of van der Waals and viscous forces differ between two schemes. However, we do not conclude which simulation is superior because all simulations fall within error bars.
Key Points
Microphysical model suggests that evaporation shrinks sulfate and increases the global burden (15%)
Van der Waals and viscous forces enhance coagulation and decrease the global sulfate burden by 30%
None of the simulations are superior as they all fall within error bars
Sharp rises in the atmospheric abundance of ethane (C2H6) have been detected from 2009 onwards in the Northern Hemisphere as a result of the unprecedented growth in the exploitation of shale gas and ...tight oil reservoirs in North America. Using time series of C2H6 total columns derived from ground-based Fourier transform infrared (FTIR) observations made at five selected Network for the Detection of Atmospheric Composition Change sites, we characterize the recent C2H6 evolution and determine growth rates of ∼5% yr−1 at mid-latitudes and of ∼3% yr−1 at remote sites. Results from CAM-chem simulations with the Hemispheric Transport of Air Pollutants, Phase II bottom-up inventory for anthropogenic emissions are found to greatly underestimate the current C2H6 abundances. Doubling global emissions is required to reconcile the simulations and the observations prior to 2009. We further estimate that North American anthropogenic C2H6 emissions have increased from 1.6 Tg yr−1 in 2008 to 2.8 Tg yr−1 in 2014, i.e. by 75% over these six years. We also completed a second simulation with new top-down emissions of C2H6 from North American oil and gas activities, biofuel consumption and biomass burning, inferred from space-borne observations of methane (CH4) from Greenhouse Gases Observing SATellite. In this simulation, GEOS-Chem is able to reproduce FTIR measurements at the mid-latitudinal sites, underscoring the impact of the North American oil and gas development on the current C2H6 abundance. Finally we estimate that the North American oil and gas emissions of CH4, a major greenhouse gas, grew from 20 to 35 Tg yr−1 over the period 2008-2014, in association with the recent C2H6 rise.
We estimated the source-receptor relationship for surface O3 in East Asia during the early 2000s using a method that tags O3 tracers according to their region of chemical production (tagged tracer ...method) with a global chemical transport model. The estimation demonstrated the importance of intracontinental transport of O3 inside East Asia as well as of the transport of O3 from distant source regions. The model well simulated the absolute concentration and seasonal variation of surface O3 in East Asia and demonstrated significant seasonal differences in the origin of surface O3. In the cold season (October to March), more than half of surface O3 in East Asia is attributable to the O3 transported from distant sources outside of East Asia. In the warm season (April to September), most of the surface O3 is attributable to O3 created within East Asia in most areas of East Asia. In spring the contribution of domestically created O3 accounted for 20% of the surface O3 in Japan and the Korean Peninsula, 40% in the North China Plain, and around 50% in the southern part of China, and the domestic contribution increased greatly in summer. The contributions of O3 created in China and the Korean Peninsula to O3 in Japan were estimated at about 10% and 5%, respectively. We also demonstrated a large contribution (20%) from China to the Korean Peninsula. In the northern and southern parts of China, large contributions of over 10% from East Siberia and the Indochina Peninsula, respectively, were identified. The contribution from intercontinental transport increased with latitude; it was 21% in Northeast China and 13% in Japan and the Korean Peninsula in spring. As for the hourly mean of surface O3, domestically created O3 was the main contributor in most areas of East Asia, except for the low O3 class (<30 ppbv), and accounted for more than 50% in the very high O3 class (>90 ppbv). The mean relative contribution of O3 created in China to O3 in central Japan was about 10% in every class, but that created in the Korean Peninsula was significant in all except the low O3 class. We identified the substantial impact of foreign sources on Japan's ambient air quality standard in the high O3 class (60–90 ppbv) in spring.
PDF
