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Arctic column ozone reached record low values (∼310 DU) during March of 2011, exposing Arctic ecosystems to enhanced UV-B. We identify the cause of this anomaly using the Oslo CTM2 atmospheric chemistry model driven by ECMWF meteorology to simulate Arctic ozone from 1998 through 2011. CTM2 successfully reproduces the variability in column ozone, from week to week, and from year to year, correctly identifying 2011 as an extreme anomaly over the period. By comparing parallel model simulations, one with all Arctic ozone chemistry turned off on January 1, we find that chemical ozone loss in 2011 is enhanced relative to previous years, but it accounted for only 23% of the anomaly. Weakened transport of ozone from middle latitudes, concurrent with an anomalously strong polar vortex, was the primary cause of the low ozone When the zonal winds relaxed in mid-March 2011, Arctic column ozone quickly recovered.

The future impact of traffic emissions on atmospheric ozone and OH has been investigated separately for the three sectors AIRcraft, maritime SHIPping and ROAD traffic. To reduce uncertainties we present results from an ensemble of six different atmospheric chemistry models, each simulating the atmospheric chemical composition in a possible high emission scenario (A1B), and with emissions from each transport sector reduced by 5% to estimate sensitivities. Our results are compared with optimistic future emission scenarios (B1 and B1 ACARE), presented in a companion paper, and with the recent past (year 2000). Present-day activity indicates that anthropogenic emissions so far evolve closer to A1B than the B1 scenario. As a response to expected changes in emissions, AIR and SHIP will have increased impacts on atmospheric O3 and OH in the future while the impact of ROAD traffic will decrease substantially as a result of technological improvements. In 2050, maximum aircraft-induced O3 occurs near 80° N in the UTLS region and could reach 9 ppbv in the zonal mean during summer. Emissions from ship traffic have their largest O3 impact in the maritime boundary layer with a maximum of 6 ppbv over the North Atlantic Ocean during summer in 2050. The O3 impact of road traffic emissions in the lower troposphere peaks at 3 ppbv over the Arabian Peninsula, much lower than the impact in 2000. Radiative forcing (RF) calculations show that the net effect of AIR, SHIP and ROAD combined will change from a marginal cooling of −0.44 ± 13 mW m−2 in 2000 to a relatively strong cooling of −32 ± 9.3 (B1) or −32 ± 18 mW m−2 (A1B) in 2050, when taking into account RF due to changes in O3, CH4 and CH4-induced O3. This is caused both by the enhanced negative net RF from SHIP, which will change from −19 ± 5.3 mW m−2 in 2000 to −31 ± 4.8 (B1) or −40 ± 9 mW m−2 (A1B) in 2050, and from reduced O3 warming from ROAD, which is likely to turn from a positive net RF of 12 ± 8.5 mW m−2 in 2000 to a slightly negative net RF of −3.1 ± 2.2 (B1) or −3.1 ± 3.4 (A1B) mW m−2 in the middle of this century. The negative net RF from ROAD is temporary and induced by the strong decline in ROAD emissions prior to 2050, which only affects the methane cooling term due to the longer lifetime of CH4 compared to O3. The O3 RF from AIR in 2050 is strongly dependent on scenario and ranges from 19 ± 6.8 (B1 ACARE) to 61 ± 14 mW m−2 (A1B). There is also a considerable span in the net RF from AIR in 2050, ranging from −0.54 ± 4.6 (B1 ACARE) to 12 ± 11 (A1B) mW m−2 compared to 6.6 ± 2.2 mW m−2 in 2000.

We present here the global chemical transport model Oslo CTM3, an update of the Oslo CTM2. The update comprises a faster transport scheme, an improved wet scavenging scheme for large scale rain, updated photolysis rates and a new lightning parameterization. Oslo CTM3 is better parallelized and allows for stable, large time steps for advection, enabling more complex or high spatial resolution simulations. A new treatment of the horizontal distribution of lightning is presented and found to compare well with measurements. The vertical distribution of lightning is updated and found to be a large contributor to CTM2–CTM3 differences, producing more NOx in the tropical middle troposphere, and less at the surface and at high altitudes. Compared with Oslo CTM2, Oslo CTM3 is faster, more capable and has better conceptual models for scavenging, vertical transport and fractional cloud cover. CTM3 captures stratospheric O3 better than CTM2, but shows minor improvements in terms of matching atmospheric observations in the troposphere. Use of the same meteorology to drive the two models shows that some features related to transport are better resolved by the CTM3, such as polar cap transport, while features like transport close to the vortex edge are resolved better in the Oslo CTM2 due to its required shorter transport time step. The longer transport time steps in CTM3 result in larger errors, e.g., near the jets, and when necessary the errors can be reduced by using a shorter time step. Using a time step of 30 min, the new transport scheme captures both large-scale and small-scale variability in atmospheric circulation and transport, with no loss of computational efficiency. We present a version of the new transport scheme which has been specifically tailored for polar studies, resulting in more accurate polar cap transport than the standard CTM3 transport, confirmed by comparison to satellite observations. Inclusion of tropospheric sulfur chemistry and nitrate aerosols in CTM3 is shown to be important to reproduce tropospheric O3, OH and the CH4 lifetime well.

The impact of future emissions from aviation and shipping on the atmospheric chemical composition has been estimated using an ensemble of six different atmospheric chemistry models. This study considers an optimistic emission scenario (B1) taking into account e.g. rapid introduction of clean and resource-efficient technologies, and a mitigation option for the aircraft sector (B1 ACARE), assuming further technological improvements. Results from sensitivity simulations, where emissions from each of the transport sectors were reduced by 5%, show that emissions from both aircraft and shipping will have a larger impact on atmospheric ozone and OH in near future (2025; B1) and for longer time horizons (2050; B1) compared to recent time (2000). However, the ozone and OH impact from aircraft can be reduced substantially in 2050 if the technological improvements considered in the B1 ACARE will be achieved. Shipping emissions have the largest impact in the marine boundary layer and their ozone contribution may exceed 4 ppbv (when scaling the response of the 5% emission perturbation to 100% by applying a factor 20) over the North Atlantic Ocean in the future (2050; B1) during northern summer (July). In the zonal mean, ship-induced ozone relative to the background levels may exceed 12% near the surface. Corresponding numbers for OH are 6.0 × 105 molecules cm−3 and 30%, respectively. This large impact on OH from shipping leads to a relative methane lifetime reduction of 3.92 (±0.48) on the global average in 2050 B1 (ensemble mean CH4 lifetime is 8.0 (±1.0) yr), compared to 3.68 (±0.47)% in 2000. Aircraft emissions have about 4 times higher ozone enhancement efficiency (ozone molecules enhanced relative to NOx molecules emitted) than shipping emissions, and the maximum impact is found in the UTLS region. Zonal mean aircraft-induced ozone could reach up to 5 ppbv at northern mid- and high latitudes during future summer (July 2050; B1), while the relative impact peaks during northern winter (January) with a contribution of 4.2%. Although the aviation-induced impact on OH is lower than for shipping, it still causes a reduction in the relative methane lifetime of 1.68 (±0.38)% in 2050 B1. However, for B1 ACARE the perturbation is reduced to 1.17 (±0.28)%, which is lower than the year 2000 estimate of 1.30 (±0.30)%. Based on the fully scaled perturbations we calculate net radiative forcings from the six models taking into account ozone, methane (including stratospheric water vapour), and methane-induced ozone changes. For the B1 scenario, shipping leads to a net cooling with radiative forcings of −28.0 (±5.1) and −30.8 (±4.8) mW m−2 in 2025 and 2050, respectively, due to the large impact on OH and, thereby, methane lifetime reductions. Corresponding values for the aviation sector shows a net warming effect with 3.8 (±6.1) and 1.9 (±6.3) mW m−2, respectively, but with a small net cooling of -0.6 (±4.6) mW m−2 for B1 ACARE in 2050.

To estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH in the present-day atmosphere six different atmospheric chemistry models have been used. Based on newly developed global emission inventories for road, ship and aircraft emission data sets each model performed sensitivity simulations reducing the emissions of each transport sector by 5%. The model results indicate that on global annual average lower tropospheric ozone responds most sensitive to ship emissions (50.6%±10.9% of the total traffic induced perturbation), followed by road (36.7%±9.3%) and aircraft exhausts (12.7%±2.9%), respectively. In the northern upper troposphere between 200–300 hPa at 30–60° N the maximum impact from road and ship are 93% and 73% of the maximum effect of aircraft, respectively. The latter is 0.185 ppbv for ozone (for the 5% case) or 3.69 ppbv when scaling to 100%. On the global average the impact of road even dominates in the UTLS-region. The sensitivity of ozone formation per NOx molecule emitted is highest for aircraft exhausts. The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 0.2 DU and occurs over the northern subtropical Atlantic extending to central Europe. Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine lower troposphere over the Atlantic. Based on the 5% perturbation the effect on ozone can exceed 0.6% close to the marine surface (global zonal mean) which is 80% of the total traffic induced ozone perturbation. In the southern hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%–80% throughout the year. Methane lifetime changes against OH are affected strongest by ship emissions up to 0.21 (± 0.05)%, followed by road (0.08 (±0.01)%) and air traffic (0.05 (± 0.02)%).Based on the full scale ozone and methane perturbations positive radiative forcings were calculated for road emissions (7.3±6.2 mWm−2) and for aviation (2.9±2.3 mWm−2). Ship induced methane lifetime changes dominate over the ozone forcing and therefore lead to a net negative forcing (−25.5±13.2 mWm−2).

We analyze present-day and future carbon monoxide (CO) simulations in 26 state-of-the-art atmospheric chemistry models run to study future air quality and climate change. In comparison with near-global satellite observations from the MOPITT instrument and local surface measurements, the models show large underestimates of Northern Hemisphere (NH) extratropical CO, while typically performing reasonably well elsewhere. The results suggest that year-round emissions, probably from fossil fuel burning in east Asia and seasonal biomass burning emissions in south-central Africa, are greatly underestimated in current inventories such as IIASA and EDGAR3.2. Variability among models is large, likely resulting primarily from intermodel differences in representations and emissions of nonmethane volatile organic compounds (NMVOCs) and in hydrologic cycles, which affect OH and soluble hydrocarbon intermediates. Global mean projections of the 2030 CO response to emissions changes are quite robust. Global mean midtropospheric (500 hPa) CO increases by 12.6 ± 3.5 ppbv (16%) for the high-emissions (A2) scenario, by 1.7 ± 1.8 ppbv (2%) for the midrange (CLE) scenario, and decreases by 8.1 ± 2.3 ppbv (11%) for the low-emissions (MFR) scenario. Projected 2030 climate changes decrease global 500 hPa CO by 1.4 ± 1.4 ppbv. Local changes can be much larger. In response to climate change, substantial effects are seen in the tropics, but intermodel variability is quite large. The regional CO responses to emissions changes are robust across models, however. These range from decreases of 10–20 ppbv over much of the industrialized NH for the CLE scenario to CO increases worldwide and year-round under A2, with the largest changes over central Africa (20–30 ppbv), southern Brazil (20–35 ppbv) and south and east Asia (30–70 ppbv). The trajectory of future emissions thus has the potential to profoundly affect air quality over most of the world's populated areas.

We present a systematic comparison of tropospheric NO2 from 17 global atmospheric chemistry models with three state-of-the-art retrievals from the Global Ozone Monitoring Experiment (GOME) for the year 2000. The models used constant anthropogenic emissions from IIASA/EDGAR3.2 and monthly emissions from biomass burning based on the 1997–2002 average carbon emissions from the Global Fire Emissions Database (GFED). Model output is analyzed at 10:30 local time, close to the overpass time of the ERS-2 satellite, and collocated with the measurements to account for sampling biases due to incomplete spatiotemporal coverage of the instrument. We assessed the importance of different contributions to the sampling bias: correlations on seasonal time scale give rise to a positive bias of 30–50% in the retrieved annual means over regions dominated by emissions from biomass burning. Over the industrial regions of the eastern United States, Europe and eastern China the retrieved annual means have a negative bias with significant contributions (between –25% and +10% of the NO2 column) resulting from correlations on time scales from a day to a month. We present global maps of modeled and retrieved annual mean NO2 column densities, together with the corresponding ensemble means and standard deviations for models and retrievals. The spatial correlation between the individual models and retrievals are high, typically in the range 0.81–0.93 after smoothing the data to a common resolution. On average the models underestimate the retrievals in industrial regions, especially over eastern China and over the Highveld region of South Africa, and overestimate the retrievals in regions dominated by biomass burning during the dry season. The discrepancy over South America south of the Amazon disappears when we use the GFED emissions specific to the year 2000. The seasonal cycle is analyzed in detail for eight different continental regions. Over regions dominated by biomass burning, the timing of the seasonal cycle is generally well reproduced by the models. However, over Central Africa south of the Equator the models peak one to two months earlier than the retrievals. We further evaluate a recent proposal to reduce the NOx emission factors for savanna fires by 40% and find that this leads to an improvement of the amplitude of the seasonal cycle over the biomass burning regions of Northern and Central Africa. In these regions the models tend to underestimate the retrievals during the wet season, suggesting that the soil emissions are higher than assumed in the models. In general, the discrepancies between models and retrievals cannot be explained by a priori profile assumptions made in the retrievals, neither by diurnal variations in anthropogenic emissions, which lead to a marginal reduction of the NO2 abundance at 10:30 local time (by 2.5–4.1% over Europe). Overall, there are significant differences among the various models and, in particular, among the three retrievals. The discrepancies among the retrievals (10–50% in the annual mean over polluted regions) indicate that the previously estimated retrieval uncertainties have a large systematic component. Our findings imply that top-down estimations of NOx emissions from satellite retrievals of tropospheric NO2 are strongly dependent on the choice of model and retrieval.

Changes in atmospheric ozone have occurred since the preindustrial era as a result of increasing anthropogenic emissions. Within ACCENT, a European Network of Excellence, ozone changes between 1850 and 2000 are assessed for the troposphere and the lower stratosphere (up to 30 km) by a variety of seven chemistry-climate models and three chemical transport models. The modeled ozone changes are taken as input for detailed calculations of radiative forcing.When only changes in chemistry are considered (constant climate) the modeled global-mean tropospheric ozone column increase since preindustrial times ranges from 7.9 DU to 13.8 DU among the ten participating models, while the stratospheric column reduction lies between 14.1 DU and 28.6 DU in the models considering stratospheric chemistry. The resulting radiative forcing is strongly dependent on the location and altitude of the modeled ozone change and varies between 0.25 Wm−2 and 0.45 Wm−2 due to ozone change in the troposphere and −0.123 Wm−2 and +0.066 Wm−2 due to the stratospheric ozone change.Changes in ozone and other greenhouse gases since preindustrial times have altered climate. Six out of the ten participating models have performed an additional calculation taking into account both chemical and climate change. In most models the isolated effect of climate change is an enhancement of the tropospheric ozone column increase, while the stratospheric reduction becomes slightly less severe. In the three climate-chemistry models with detailed tropospheric and stratospheric chemistry the inclusion of climate change increases the resulting radiative forcing due to tropospheric ozone change by up to 0.10 Wm−2, while the radiative forcing due to stratospheric ozone change is reduced by up to 0.034 Wm−2.Considering tropospheric and stratospheric change combined, the total ozone column change is negative while the resulting net radiative forcing is positive.

Global atmospheric dust is simulated using the Dust Entrainment and Deposition (DEAD) model in combination with the global-scale Oslo chemical transport model CTM2 using meteorological data for 1996. Dust sources are calculated using both mean wind speeds with model resolution T63 and subgrid wind speeds. Different data sets are used to describe soil erodibility. We explain how the different assumptions about dust production affect atmospheric dust burden and deposition. Some aspects of the annual dust cycle, such as the east Asian dust emissions, are largely dependent on the data used to determine soil erodibility. Other aspects, such as the timing of the maximum in the African plume at Northern Hemisphere summer, are well modeled with all data sets applied here. We show that the daily variation in optical depth at Cape Verde on the west coast of Africa is well simulated when we assume that erodibility is correlated with surface reflectivity from Moderate-Resolution Imaging Spetroradiometer (MODIS) satellite data. Using a subgrid probability density function of wind speed to drive the dust sources facilitates dust emissions in areas with low wind speeds. Dust concentrations in remote areas are sensitive to the parameterization of wet deposition. Our results point out the need for a detailed soil erodibility data set for global dust modeling, and they suggest that surface reflectivity is potentially valuable for producing or evaluating such data sets.

The spatial and temporal variation in ozone production over major source regions in East Asia during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) measurement campaign in spring 2001 is assessed using a global chemical transport model. There is a strong latitudinal gradient in ozone production in springtime, driven by regional photochemistry, which rapidly diminishes as the season progresses. The great variability in meteorological conditions characteristic of East Asia in springtime leads to large daily variability in regional ozone formation, but we find that it has relatively little impact on the total global production. We note that transport processes effectively modulate and thus stabilize total ozone production through their influence over its location. However, the impact on the global ozone burden, important for assessing the effects of precursor emissions on tropospheric oxidizing capacity and climate, is sensitive to local meteorology through the effects of location on chemical lifetime. Stagnant, anticyclonic conditions conducive to substantial boundary layer ozone production typically allow little lifting of precursors into the free troposphere where greater ozone production could occur, and the consequent shorter chemical lifetime for ozone leads to relatively small impacts on global ozone. Conversely, cyclonic conditions with heavy cloud cover suppressing regional ozone production are often associated with substantial cloud convection, enhancing subsequent production in the free troposphere where chemical lifetimes are longer, and the impacts on global ozone are correspondingly greater. We find that ozone formation in the boundary layer and free troposphere outside the region of precursor emissions dominates total gross production from these sources in springtime, and that it makes a big contribution to the long range transport of ozone, which is greatest in this season.

Observations of CO and O3 from the Transport and Chemical Evolution over the Pacific (TRACE-P) campaign are compared with modeled distributions from the FRSGC/UCI CTM driven by the Oslo T63L40 ECMWF forecast meteorology. The model-measurement comparison is made within the context of how well the TRACE-P observations represent the springtime chemistry and ozone distributions over eastern Asia and the western Pacific in March 2001 and uses the four-dimensional (4-D) extended domain from the model to provide unbiased statistics. A key question is whether the limited sampling density or mission strategy led to a statistically biased sample. To address this question, we examine a diverse range of statistical analyses of the observations of CO and O3. The middle percentiles of the cumulative probability functions for CO in the free troposphere are representative (and reproduced by the CTM), but those in the boundary layer are not. The frequency of low-CO, stratospheric influence is well matched along flight tracks but is atypical of the extended domain. The percentiles of the latitude-by-height distribution of lidar O3 show how the CTM reproduces the nonrepresentative clumpy nature of the observations but has too low a tropopause about the jet region (30–35N). Adaptive kernel estimation of the 2-D probability density of O3-CO correlations shows a very good simulation of two different chemical regimes (stratospheric and polluted) that is quite different from the extended domain but also highlights the failure to predict CO > 400 ppb. Empirical orthogonal function analysis of the O3 vertical profiles shows how six EOFs can effectively describe the 4-D structures of O3 over this entire domain. The latitude-by-longitude maps of the principal components provide an excellent test of the CTM simulation along flight tracks and clearly show the unique sampling of O3events by the TRACE-P flights. In many cases the ability of the model to simulate the nonrepresentative observations implies a clear skill in matching the unique meteorological and chemical features of the region.

Two closely related chemical transport models (CTMs) employing the same high-resolution meteorological data (∼180 km × ∼180 km × ∼600 m) from the European Centre for Medium-Range Weather Forecasts are used to simulate the ozone total column and tropospheric distribution over the western Pacific region that was explored by the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) measurement campaign in February–April 2001. We make extensive comparisons with ozone measurements from the lidar instrument on the NASA DC-8, with ozonesondes taken during the period around the Pacific Rim, and with TOMS total column ozone. These demonstrate that within the uncertainties of the meteorological data and the constraints of model resolution, the two CTMs (FRSGC/UCI and Oslo CTM2) can simulate the observed tropospheric ozone and do particularly well when realistic stratospheric ozone photochemistry is included. The greatest differences between the models and observations occur in the polluted boundary layer, where problems related to the simplified chemical mechanism and inadequate horizontal resolution are likely to have caused the net overestimation of about 10 ppb mole fraction. In the upper troposphere, the large variability driven by stratospheric intrusions makes agreement very sensitive to the timing of meteorological features.

Two sets of sea surface temperature/sea ice changes are used to test the sensitivity of tracer transport to the pattern of warming in the doubled CO2 climate. One set (2CO2WT) has greater tropical and high latitude sea surface temperature changes than the other (2CO2), although both fall within the range of plausible response. Simulations were done both with and without interactive ozone. Results show that the SST pattern affects the circulation change throughout the troposphere and middle atmosphere; the ozone interaction affects primarily the upper stratosphere, but through wave-mean flow interaction has effects that extend down into the upper troposphere. Both experiments feature increased tropospheric/stratospheric exchange at low latitudes and greater vertical mixing within the troposphere; only the WT experiments result in increased interhemispheric transport and a more direct circulation in the high latitude stratosphere. Ozone increases in the upper stratosphere and decreases in the lower stratosphere in all the simulations, with greater transport of high latitude ozone into the troposphere in the WT runs. At sea level there is a more positive phase of the Arctic Oscillation (AO)-type oscillation, and this is also true at 100 mbar, but there is no significance in the middle troposphere and the sign is different in the middle stratosphere. Many of these results differ from those generated in older versions of the GISS GCMAM despite the same SST forcing due to differences in control run characteristics, which has implications for model intercomparison experiments.

Radiative forcing due to changes in ozone is expected for the 21st century. An assessment on changes in the tropospheric oxidative state through a model intercomparison (“OxComp”) was conducted for the IPCC Third Assessment Report (IPCC-TAR). OxComp estimated tropospheric changes in ozone and other oxidants during the 21st century based on the “SRES” A2p emission scenario. In this study we analyze the results of 11 chemical transport models (CTMs) that participated in OxComp and use them as input for detailed radiative forcing calculations. We also address future ozone recovery in the lower stratosphere and its impact on radiative forcing by applying two models that calculate both tropospheric and stratospheric changes. The results of OxComp suggest an increase in global-mean tropospheric ozone between 11.4 and 20.5 DU for the 21st century, representing the model uncertainty range for the A2p scenario. As the A2p scenario constitutes the worst case proposed in IPCC-TAR we consider these results as an upper estimate. The radiative transfer model yields a positive radiative forcing ranging from 0.40 to 0.78 W m−2 on a global and annual average. The lower stratosphere contributes an additional 7.5–9.3 DU to the calculated increase in the ozone column, increasing radiative forcing by 0.15–0.17 W m−2. The modeled radiative forcing depends on the height distribution and geographical pattern of predicted ozone changes and shows a distinct seasonal variation. Despite the large variations between the 11 participating models, the calculated range for normalized radiative forcing is within 25%, indicating the ability to scale radiative forcing to global-mean ozone column change.

An upper limit for aircraft-produced perturbations to aerosols and gaseous exhaust products in the upper troposphere and lower stratosphere (UT/LS) is derived using the 1992 aviation fuel tracer simulation performed by eleven global atmospheric models. Key findings are that subsonic aircraft emissions: 1) have not be responsible for the observed water vapor trends at 40°N; 2) could be a significant source of soot mass near 12 km, but not at 20 km, 3) might cause a noticeable increase in the background sulfate aerosol surface area and number densities (but not mass density) near the northern mid-latitude tropopause, and 4) could provide a global, annual mean top of the atmosphere radiative forcing up to +0.006 W/m² and −0.013 W/m² due to emitted soot and sulfur, respectively.

An open workshop on 'Climatic Effects of Atmospheric Trace Constituents' was held in Vienna, Austria, on 19-20 August 1991 as part of the IUGG-IAMAP General Assembly. The objectives of the workshop were to review available information on spatial and temporal variations of atmospheric radiatively-chemically important trace constituents and their radiative properties, and discuss their chemical interactions and impact on climate. The workshop included six sessions: trace constituent distributions, spectroscopy and radiation models of the trace constituents, GCM climate studies, climate-chemistry interactions, research programs, and future research activities. Twenty-eight invited and contributed papers were presented and five papers were posted. A summary of the individual sessions is given below.