Atmospheric Chemistry And Climate Model Intercomparison Project Research Articles

The enhanced role of atmospheric reduced nitrogen deposition in future over East Asia–Northwest Pacific

The atmospheric nitrogen deposition plays a crucial role in natural ecosystem, and the changes in emissions substantially affect the amount of nitrogen deposition. Along with the decrease in NOx emissions and increase in NH3 emissions, the reduced nitrogen deposition may play a more important role in future. However, to what extent these changes may modify the reduced nitrogen deposition across East Asia, which is fulfilled with a large amount of nitrogen deposition, to the northwestern Pacific has not yet to be clear. Based on the results of multi-model ensemble of Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), the future changes of reduced nitrogen (NHx) deposition is firstly examined. Here we show the changes of NHx deposition flux is substantially modulated by both climate change and emissions, exhibiting an increasing trend over East Asia-Northwest Pacific in future under representative concentration pathways (RCP) 8.5 scenario, largely controlled by increase of NH3 emissions, contrasting to the oxidized nitrogen deposition which is projected to decrease. Specifically, the ratio of NHx to total nitrogen deposition in eastern China increases from 38% at present to 56% by the end of the century under RCP 8.5, indicative of a transition in the form of dominant nitrogen deposition from oxidized to reduced one. The increase is clearly discernable over the marginal seas and northwestern Pacific. Moreover, we identify a meridional shift of high wet NHx deposition from northern China in summer to southern China in the other seasons. Based on simulations from regional models Weather Research and Forecasting (WRF) and Community Multi-scale Air Quality (CMAQ), we find that the synergistically nonlinear modulation of NHx concentration and precipitation triggers the north-south shift of wet NHx deposition. The findings in this study indicate a potentially more important role of reduced nitrogen deposition on the natural ecosystem in future.

Effect of model errors in ambient air humidity on the aerosol optical depth obtained via aerosol hygroscopicity in eastern China in the Atmospheric Chemistry and Climate Model Intercomparison Project datasets

This analysis of the multi-model aerosol optical depth (AOD) in eastern China using the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) datasets shows that the global models underestimate the AOD by 33% and 44% in southern and northern China, respectively, and decrease the relative humidity (RH) of the air in the surface layer to 71%–80%, which is less than the RH of 77%–92% in reanalysis meteorological datasets. This indicates that the low biases in the RH partially account for the errors in the AOD. The AOD is recalculated based on the model aerosol concentrations and the reanalysis humidity data. Improving the mean value of the RH increases the multi-model annual mean AOD by 45% in southern China and by 33% in June–August in northern China. This method of improving the AOD is successful in most of the ACCMIP models, but it is unlikely to be successful in GISS-E2-R, in which the plot of its AOD efficiency against RH strongly deviates from the rest of the models. The effe...

Impacts of climate change and emissions on atmospheric oxidized nitrogen deposition over East Asia

Abstract. A multi-model ensemble of Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) simulations is used to study the atmospheric oxidized nitrogen (NOy) deposition over East Asia under climate and emission changes projected for the future. Both dry and wet NOy deposition show significant decreases in the 2100s under RCP4.5 and RCP8.5, primarily due to large anthropogenic emission reduction over both land and sea. However, in the near future of the 2030s, both dry and wet NOy deposition increase significantly due to continued increase in emissions. Marine primary production from both dry and wet NOy deposition increases by 19 %–34 % in the 2030s and decreases by 34 %–63 % in the 2100s over the East China Sea. The individual effect of climate or emission changes on dry and wet NOy deposition is also investigated. The impact of climate change on dry NOy deposition is relatively minor, but the effect on wet deposition, primarily caused by changes in precipitation, is much higher. For example, over the East China Sea, wet NOy deposition increases significantly in summer due to climate change by the end of this century under RCP8.5, which may subsequently enhance marine primary production. Over the coastal seas of China, as the transport of NOy from land becomes weaker due to the decrease in anthropogenic emissions, the effect of ship emissions and lightning emissions becomes more important. On average, the seasonal mean contribution of ship emissions to total NOy deposition is projected to be enhanced by 24 %–48 % and 3 %–37 % over the Yellow Sea and East China Sea, respectively, by the end of this century. Therefore, continued control of both anthropogenic emissions over land and ship emissions may reduce NOy deposition to the Chinese coastal seas.

Multi-model impacts of climate change on pollution transport from global emission source regions

Abstract. The impacts of climate change on tropospheric transport, diagnosed from a carbon monoxide (CO)-like tracer species emitted from global CO sources, are evaluated from an ensemble of four chemistry–climate models (CCMs) contributing to the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). Model time-slice simulations for present-day and end-of-the-21st-century conditions were performed under the Representative Concentrations Pathway (RCP) climate scenario RCP 8.5. All simulations reveal a strong seasonality in transport, especially over the tropics. The highest CO-tracer mixing ratios aloft occur during boreal winter when strong vertical transport is co-located with biomass burning emission source regions. A consistent and robust decrease in future CO-tracer mixing ratios throughout most of the troposphere, especially in the tropics, and an increase around the tropopause is found across the four CCMs in both winter and summer. Decreases in CO-tracer mixing ratios in the tropical troposphere are associated with reduced convective mass fluxes in this region, which in turn may reflect a weaker Hadley cell circulation in the future climate. Increases in CO-tracer mixing ratios near the tropopause are largely attributable to a rise in tropopause height enabling lofting to higher altitudes, although a poleward shift in the mid-latitude jets may also play a minor role in the extratropical upper troposphere. An increase in CO-tracer mixing ratios also occurs near the Equator, centred over equatorial and Central Africa, extending from the surface to the mid-troposphere. This is most likely related to localised decreases in convection in the vicinity of the Intertropical Convergence Zone (ITCZ), resulting in larger CO-tracer mixing ratios over biomass burning regions and smaller mixing ratios downwind.

Observation- and Model-Based Estimates of Particulate Dry Nitrogen Deposition to the Oceans.

Anthropogenic nitrogen (N) emissions to the atmosphere have increased significantly the deposition of nitrate (NO3-) and ammonium (NH4+) to the surface waters of the open ocean, with potential impacts on marine productivity and the global carbon cycle. Global-scale understanding of the impacts of N deposition to the oceans is reliant on our ability to produce and validate models of nitrogen emission, atmospheric chemistry, transport and deposition. In this work, ~2900 observations of aerosol NO3- and NH4+ concentrations, acquired from sampling aboard ships in the period 1995 - 2012, are used to assess the performance of modelled N concentration and deposition fields over the remote ocean. Three ocean regions (the eastern tropical North Atlantic, the northern Indian Ocean and northwest Pacific) were selected, in which the density and distribution of observational data were considered sufficient to provide effective comparison to model products. All of these study regions are affected by transport and deposition of mineral dust, which alters the deposition of N, due to uptake of nitrogen oxides (NOx) on mineral surfaces. Assessment of the impacts of atmospheric N deposition on the ocean requires atmospheric chemical transport models to report deposition fluxes, however these fluxes cannot be measured over the ocean. Modelling studies such as the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), which only report deposition flux are therefore very difficult to validate for dry deposition. Here the available observational data were averaged over a 5° × 5° grid and compared to ACCMIP dry deposition fluxes (ModDep) of oxidised N (NOy) and reduced N (NHx) and to the following parameters from the TM4-ECPL (TM4) model: ModDep for NOy, NHx and particulate NO3- and NH4+, and surface-level particulate NO3- and NH4+ concentrations. As a model ensemble, ACCMIP can be expected to be more robust than TM4, while TM4 gives access to speciated parameters (NO3- and NH4+) that are more relevant to the observed parameters and which are not available in ACCMIP. Dry deposition fluxes (CalDep) were calculated from the observed concentrations using estimates of dry deposition velocities. Model - observation ratios, weighted by grid-cell area and numbers of observations, (RA,n) were used to assess the performance of the models. Comparison in the three study regions suggests that TM4 over-estimates NO3- concentrations (RA,n = 1.4 - 2.9) and under-estimates NH4+ concentrations (RA,n = 0.5 - 0.7), with spatial distributions in the tropical Atlantic and northern Indian Ocean not being reproduced by the model. In the case of NH4+ in the Indian Ocean, this discrepancy was probably due to seasonal biases in the sampling. Similar patterns were observed in the various comparisons of CalDep to ModDep (RA,n = 0.6 - 2.6 for NO3-, 0.6 - 3.1 for NH4+). Values of RA,n for NHx CalDep - ModDep comparisons were approximately double the corresponding values for NH4+ CalDep - ModDep comparisons due to the significant fraction of gas-phase NH3 deposition incorporated in the TM4 and ACCMIP NHx model products. All of the comparisons suffered due to the scarcity of observational data and the large uncertainty in dry deposition velocities used to derive deposition fluxes from concentrations. These uncertainties have been a major limitation on estimates of the flux of material to the oceans for several decades. Recommendations are made for improvements in N deposition estimation through changes in observations, modelling and model - observation comparison procedures. Validation of modelled dry deposition requires effective comparisons to observable aerosol-phase species concentrations and this cannot be achieved if model products only report dry deposition flux over the ocean.

Past, Present and Future Atmospheric Nitrogen Deposition.

Reactive nitrogen emissions into the atmosphere are increasing due to human activities, affecting nitrogen deposition to the surface and impacting the productivity of terrestrial and marine ecosystems. An atmospheric chemistry-transport model (TM4-ECPL) is here used to calculate the global distribution of total nitrogen deposition, accounting for the first time for both its inorganic and organic fractions in gaseous and particulate phases, and past and projected changes due to anthropogenic activities. The anthropogenic and biomass burning ACCMIP historical and RCP6.0 and RCP8.5 emissions scenarios are used. Accounting for organic nitrogen (ON) primary emissions, the present-day global nitrogen atmospheric source is about 60% anthropogenic, while total N deposition increases by about 20% relative to simulations without ON primary emissions. About 20-25% of total deposited N is ON. About 10% of the emitted nitrogen oxides are deposited as ON instead of inorganic nitrogen (IN) as is considered in most global models. Almost a 3-fold increase over land (2-fold over the ocean) has been calculated for soluble N deposition due to human activities from 1850 to present. The investigated projections indicate significant changes in the regional distribution of N deposition and chemical composition, with reduced compounds gaining importance relative to oxidized ones, but very small changes in the global total flux. Sensitivity simulations quantify uncertainties due to the investigated model parameterizations of IN partitioning onto aerosols and of N chemically fixed on organics to be within 10% for the total soluble N deposition and between 25-35% for the dissolved ON deposition. Larger uncertainties are associated with N emissions.

Stratospheric ozone change and related climate impacts over 1850–2100 as modelled by the ACCMIP ensemble

Abstract. Stratospheric ozone and associated climate impacts in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) simulations are evaluated in the recent past (1980–2000), and examined in the long-term (1850–2100) using the Representative Concentration Pathways (RCPs) low- and high-emission scenarios (RCP2.6 and RCP8.5, respectively) for the period 2000–2100. ACCMIP multi-model mean total column ozone (TCO) trends compare favourably, within uncertainty estimates, against observations. Particularly good agreement is seen in the Antarctic austral spring (−11.9 % dec−1 compared to observed ∼ −13.9 ± 10.4 % dec−1), although larger deviations are found in the Arctic's boreal spring (−2.1 % dec−1 compared to observed ∼ −5.3 ± 3.3 % dec−1). The simulated ozone hole has cooled the lower stratosphere during austral spring in the last few decades (−2.2 K dec−1). This cooling results in Southern Hemisphere summertime tropospheric circulation changes captured by an increase in the Southern Annular Mode (SAM) index (1.3 hPa dec−1). In the future, the interplay between the ozone hole recovery and greenhouse gases (GHGs) concentrations may result in the SAM index returning to pre-ozone hole levels or even with a more positive phase from around the second half of the century (−0.4 and 0.3 hPa dec−1 for the RCP2.6 and RCP8.5, respectively). By 2100, stratospheric ozone sensitivity to GHG concentrations is greatest in the Arctic and Northern Hemisphere midlatitudes (37.7 and 16.1 DU difference between the RCP2.6 and RCP8.5, respectively), and smallest over the tropics and Antarctica continent (2.5 and 8.1 DU respectively). Future TCO changes in the tropics are mainly determined by the upper stratospheric ozone sensitivity to GHG concentrations, due to a large compensation between tropospheric and lower stratospheric column ozone changes in the two RCP scenarios. These results demonstrate how changes in stratospheric ozone are tightly linked to climate and show the benefit of including the processes interactively in climate models.

Distribution and Variation of Carbon Monoxide in the Tropical Troposphere and Lower Stratosphere

AbstractThe authors examine the distribution and variation of carbon monoxide (CO) in the tropics from the surface to the lower stratosphere. By analyzing space-borne microwave limb sounder (MLS) measurements, measurements of pollution in the troposphere (MOPITT) and modern-era retrospective analysis for research and applications (MERRA) meteorological products, and atmospheric chemistry and climate model intercomparison project (ACCMIP) surface emission inventories, the influences of atmospheric dynamics and surface emissions are investigated. The results show that there are four centers of highly concentrated CO mixing ratio over tropical areas in different seasons: two in the Northern Hemisphere and another two in the Southern Hemisphere. All of these centers correspond to local deep convective systems and monsoons/anticyclones. The authors suggest that both deep convections and anticyclones affect CO in the tropical troposphere and lower stratosphere — the former helping to transport CO from the lower...

Multi-model mean nitrogen and sulfur deposition from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): evaluation of historical and projected future changes

Abstract. We present multi-model global datasets of nitrogen and sulfate deposition covering time periods from 1850 to 2100, calculated within the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The computed deposition fluxes are compared to surface wet deposition and ice core measurements. We use a new dataset of wet deposition for 2000–2002 based on critical assessment of the quality of existing regional network data. We show that for present day (year 2000 ACCMIP time slice), the ACCMIP results perform similarly to previously published multi-model assessments. For this time slice, we find a multi-model mean deposition of approximately 50 Tg(N) yr−1 from nitrogen oxide emissions, 60 Tg(N) yr−1 from ammonia emissions, and 83 Tg(S) yr−1 from sulfur emissions. The analysis of changes between 1980 and 2000 indicates significant differences between model and measurements over the United States but less so over Europe. This difference points towards a potential misrepresentation of 1980 NH3 emissions over North America. Based on ice core records, the 1850 deposition fluxes agree well with Greenland ice cores, but the change between 1850 and 2000 seems to be overestimated in the Northern Hemisphere for both nitrogen and sulfur species. Using the Representative Concentration Pathways (RCPs) to define the projected climate and atmospheric chemistry related emissions and concentrations, we find large regional nitrogen deposition increases in 2100 in Latin America, Africa and parts of Asia under some of the scenarios considered. Increases in South Asia are especially large, and are seen in all scenarios, with 2100 values more than double their 2000 counterpart in some scenarios and reaching > 1300 mg(N) m−2 yr−1 averaged over regional to continental-scale regions in RCP 2.6 and 8.5, ~ 30–50% larger than the values in any region currently (circa 2000). However, sulfur deposition rates in 2100 are in all regions lower than in 2000 in all the RCPs. The new ACCMIP multi-model deposition dataset provides state-of-the-science, consistent and evaluated time slice (spanning 1850–2100) global gridded deposition fields for use in a wide range of climate and ecological studies.

Corrigendum to "Evaluation of preindustrial to present-day black carbon and its albedo forcing from Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)" published in Atmos. Chem. Phys., 13, 2607–2634, 2013

Corrigendum to "Evaluation of preindustrial to present-day black carbon and its albedo forcing from Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)" published in Atmos. Chem. Phys., 13, 2607–2634, 2013

Preindustrial to present-day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Abstract. We have analysed time-slice simulations from 17 global models, participating in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), to explore changes in present-day (2000) hydroxyl radical (OH) concentration and methane (CH4) lifetime relative to preindustrial times (1850) and to 1980. A comparison of modeled and observation-derived methane and methyl chloroform lifetimes suggests that the present-day global multi-model mean OH concentration is overestimated by 5 to 10% but is within the range of uncertainties. The models consistently simulate higher OH concentrations in the Northern Hemisphere (NH) compared with the Southern Hemisphere (SH) for the present-day (2000; inter-hemispheric ratios of 1.13 to 1.42), in contrast to observation-based approaches which generally indicate higher OH in the SH although uncertainties are large. Evaluation of simulated carbon monoxide (CO) concentrations, the primary sink for OH, against ground-based and satellite observations suggests low biases in the NH that may contribute to the high north–south OH asymmetry in the models. The models vary widely in their regional distribution of present-day OH concentrations (up to 34%). Despite large regional changes, the multi-model global mean (mass-weighted) OH concentration changes little over the past 150 yr, due to concurrent increases in factors that enhance OH (humidity, tropospheric ozone, nitrogen oxide (NOx) emissions, and UV radiation due to decreases in stratospheric ozone), compensated by increases in OH sinks (methane abundance, carbon monoxide and non-methane volatile organic carbon (NMVOC) emissions). The large inter-model diversity in the sign and magnitude of preindustrial to present-day OH changes (ranging from a decrease of 12.7% to an increase of 14.6%) indicate that uncertainty remains in our understanding of the long-term trends in OH and methane lifetime. We show that this diversity is largely explained by the different ratio of the change in global mean tropospheric CO and NOx burdens (ΔCO/ΔNOx, approximately represents changes in OH sinks versus changes in OH sources) in the models, pointing to a need for better constraints on natural precursor emissions and on the chemical mechanisms in the current generation of chemistry-climate models. For the 1980 to 2000 period, we find that climate warming and a slight increase in mean OH (3.5 ± 2.2%) leads to a 4.3 ± 1.9% decrease in the methane lifetime. Analysing sensitivity simulations performed by 10 models, we find that preindustrial to present-day climate change decreased the methane lifetime by about four months, representing a negative feedback on the climate system. Further, we analysed attribution experiments performed by a subset of models relative to 2000 conditions with only one precursor at a time set to 1860 levels. We find that global mean OH increased by 46.4 ± 12.2% in response to preindustrial to present-day anthropogenic NOx emission increases, and decreased by 17.3 ± 2.3%, 7.6 ± 1.5%, and 3.1 ± 3.0% due to methane burden, and anthropogenic CO, and NMVOC emissions increases, respectively.

Evaluation of ACCMIP outgoing longwave radiation from tropospheric ozone using TES satellite observations

Abstract. We use simultaneous observations of tropospheric ozone and outgoing longwave radiation (OLR) sensitivity to tropospheric ozone from the Tropospheric Emission Spectrometer (TES) to evaluate model tropospheric ozone and its effect on OLR simulated by a suite of chemistry-climate models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean of ACCMIP models show a persistent but modest tropospheric ozone low bias (5–20 ppb) in the Southern Hemisphere (SH) and modest high bias (5–10 ppb) in the Northern Hemisphere (NH) relative to TES ozone for 2005–2010. These ozone biases have a significant impact on the OLR. Using TES instantaneous radiative kernels (IRK), we show that the ACCMIP ensemble mean tropospheric ozone low bias leads up to 120 mW m−2 OLR high bias locally but zonally compensating errors reduce the global OLR high bias to 39 ± 41 m Wm−2 relative to TES data. We show that there is a correlation (R2 = 0.59) between the magnitude of the ACCMIP OLR bias and the deviation of the ACCMIP preindustrial to present day (1750–2010) ozone radiative forcing (RF) from the ensemble ozone RF mean. However, this correlation is driven primarily by models whose absolute OLR bias from tropospheric ozone exceeds 100 m Wm−2. Removing these models leads to a mean ozone radiative forcing of 394 ± 42 m Wm−2. The mean is about the same and the standard deviation is about 30% lower than an ensemble ozone RF of 384 ± 60 m Wm−2 derived from 14 of the 16 ACCMIP models reported in a companion ACCMIP study. These results point towards a profitable direction of combining satellite observations and chemistry-climate model simulations to reduce uncertainty in ozone radiative forcing.

Radiative forcing in the ACCMIP historical and future climate simulations

Abstract. 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.

Tropospheric ozone changes, radiative forcing and attribution to emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Abstract. Ozone (O3) from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) has been used to calculate tropospheric ozone radiative forcings (RFs). All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP) scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750) to present-day (2010) tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (±1 standard deviation) in RFs of ±17%. Three different radiation schemes were used – we find differences in RFs between schemes (for the same ozone fields) of ±10%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified) uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44±12%), nitrogen oxides (31 ± 9%), carbon monoxide (15 ± 3%) and non-methane volatile organic compounds (9 ± 2%); earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m−2 DU−1, a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m−2; relative to 1750) for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5) of 350, 420, 370 and 460 (in 2030), and 200, 300, 280 and 600 (in 2100). Models show some coherent responses of ozone to climate change: decreases in the tropical lower troposphere, associated with increases in water vapour; and increases in the sub-tropical to mid-latitude upper troposphere, associated with increases in lightning and stratosphere-to-troposphere transport. Climate change has relatively small impacts on global mean tropospheric ozone RF.

Evaluation of preindustrial to present-day black carbon and its albedo forcing from Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Abstract. As part of the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), we evaluate the historical black carbon (BC) aerosols simulated by 8 ACCMIP models against observations including 12 ice core records, long-term surface mass concentrations, and recent Arctic BC snowpack measurements. We also estimate BC albedo forcing by performing additional simulations using offline models with prescribed meteorology from 1996–2000. We evaluate the vertical profile of BC snow concentrations from these offline simulations using the recent BC snowpack measurements. Despite using the same BC emissions, the global BC burden differs by approximately a factor of 3 among models due to differences in aerosol removal parameterizations and simulated meteorology: 34 Gg to 103 Gg in 1850 and 82 Gg to 315 Gg in 2000. However, the global BC burden from preindustrial to present-day increases by 2.5–3 times with little variation among models, roughly matching the 2.5-fold increase in total BC emissions during the same period. We find a large divergence among models at both Northern Hemisphere (NH) and Southern Hemisphere (SH) high latitude regions for BC burden and at SH high latitude regions for deposition fluxes. The ACCMIP simulations match the observed BC surface mass concentrations well in Europe and North America except at Ispra. However, the models fail to predict the Arctic BC seasonality due to severe underestimations during winter and spring. The simulated vertically resolved BC snow concentrations are, on average, within a factor of 2–3 of the BC snowpack measurements except for Greenland and the Arctic Ocean. For the ice core evaluation, models tend to adequately capture both the observed temporal trends and the magnitudes at Greenland sites. However, models fail to predict the decreasing trend of BC depositions/ice core concentrations from the 1950s to the 1970s in most Tibetan Plateau ice cores. The distinct temporal trend at the Tibetan Plateau ice cores indicates a strong influence from Western Europe, but the modeled BC increases in that period are consistent with the emission changes in Eastern Europe, the Middle East, South and East Asia. At the Alps site, the simulated BC suggests a strong influence from Europe, which agrees with the Alps ice core observations. At Zuoqiupu on the Tibetan Plateau, models successfully simulate the higher BC concentrations observed during the non-monsoon season compared to the monsoon season but overpredict BC in both seasons. Despite a large divergence in BC deposition at two Antarctic ice core sites, some models with a BC lifetime of less than 7 days are able to capture the observed concentrations. In 2000 relative to 1850, globally and annually averaged BC surface albedo forcing from the offline simulations ranges from 0.014 to 0.019 W m−2 among the ACCMIP models. Comparing offline and online BC albedo forcings computed by some of the same models, we find that the global annual mean can vary by up to a factor of two because of different aerosol models or different BC-snow parameterizations and snow cover. The spatial distributions of the offline BC albedo forcing in 2000 show especially high BC forcing (i.e., over 0.1 W m−2) over Manchuria, Karakoram, and most of the Former USSR. Models predict the highest global annual mean BC forcing in 1980 rather than 2000, mostly driven by the high fossil fuel and biofuel emissions in the Former USSR in 1980.

Pre-industrial to end 21st century projections of tropospheric ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP)

Abstract. Present day tropospheric ozone and its changes between 1850 and 2100 are considered, analysing 15 global models that participated in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP). The ensemble mean compares well against present day observations. The seasonal cycle correlates well, except for some locations in the tropical upper troposphere. Most (75 %) of the models are encompassed with a range of global mean tropospheric ozone column estimates from satellite data, but there is a suggestion of a high bias in the Northern Hemisphere and a low bias in the Southern Hemisphere, which could indicate deficiencies with the ozone precursor emissions. Compared to the present day ensemble mean tropospheric ozone burden of 337 ± 23 Tg, the ensemble mean burden for 1850 time slice is ~30% lower. Future changes were modelled using emissions and climate projections from four Representative Concentration Pathways (RCPs). Compared to 2000, the relative changes in the ensemble mean tropospheric ozone burden in 2030 (2100) for the different RCPs are: −4% (−16%) for RCP2.6, 2% (−7%) for RCP4.5, 1% (−9%) for RCP6.0, and 7% (18%) for RCP8.5. Model agreement on the magnitude of the change is greatest for larger changes. Reductions in most precursor emissions are common across the RCPs and drive ozone decreases in all but RCP8.5, where doubled methane and a 40–150% greater stratospheric influx (estimated from a subset of models) increase ozone. While models with a high ozone burden for the present day also have high ozone burdens for the other time slices, no model consistently predicts large or small ozone changes; i.e. the magnitudes of the burdens and burden changes do not appear to be related simply, and the models are sensitive to emissions and climate changes in different ways. Spatial patterns of ozone changes are well correlated across most models, but are notably different for models without time evolving stratospheric ozone concentrations. A unified approach to ozone budget specifications and a rigorous investigation of the factors that drive tropospheric ozone is recommended to help future studies attribute ozone changes and inter-model differences more clearly.

The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP): overview and description of models, simulations and climate diagnostics

Abstract. The Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP) consists of a series of time slice experiments targeting the long-term changes in atmospheric composition between 1850 and 2100, with the goal of documenting composition changes and the associated radiative forcing. In this overview paper, we introduce the ACCMIP activity, the various simulations performed (with a requested set of 14) and the associated model output. The 16 ACCMIP models have a wide range of horizontal and vertical resolutions, vertical extent, chemistry schemes and interaction with radiation and clouds. While anthropogenic and biomass burning emissions were specified for all time slices in the ACCMIP protocol, it is found that the natural emissions are responsible for a significant range across models, mostly in the case of ozone precursors. The analysis of selected present-day climate diagnostics (precipitation, temperature, specific humidity and zonal wind) reveals biases consistent with state-of-the-art climate models. The model-to-model comparison of changes in temperature, specific humidity and zonal wind between 1850 and 2000 and between 2000 and 2100 indicates mostly consistent results. However, models that are clear outliers are different enough from the other models to significantly affect their simulation of atmospheric chemistry.