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Understanding carbon sources and sinks across the Earth's surface is fundamental in climate science and policy; thus, these topics have been extensively studied but have yet to be fully resolved and are associated with massive debate regarding the sign and magnitude of the carbon budget from global to regional scales. Developing new models and estimates based on state-of-the-art algorithms and data constraints can provide valuable knowledge and contribute to a final ensemble model in which various optimal carbon budget estimates are integrated, such as the annual global carbon budget paper. Here, we develop a new atmospheric inversion system based on the 4D local ensemble transform Kalman filter (4D-LETKF) coupled with the GEOS-Chem global transport model to infer surface-to-atmosphere net carbon fluxes from Orbiting Carbon Observatory-2 (OCO-2) V10r XCO 2 retrievals. The 4D-LETKF algorithm is adapted to an OCO-2-based global carbon inversion system for the first time in this work. On average, the mean annual terrestrial and oceanic fluxes between 2015 and 2020 are estimated as - 2.02 and - 2.34 GtC yr -1 , respectively, compensating for 21 % and 24 %, respectively, of global fossil carbon dioxide (CO 2) emissions (9.80 GtC yr -1). Our inversion results agree with the CO 2 atmospheric growth rates reported by the National Oceanic and Atmospheric Administration (NOAA) and reduce the modeled CO 2 concentration biases relative to the prior fluxes against surface and aircraft measurements. Our inversion-based carbon fluxes are broadly consistent with those provided by other global atmospheric inversion models, although discrepancies still occur in the land–ocean flux partitioning schemes and seasonal flux amplitudes over boreal and tropical regions, possibly due to the sparse observational constraints of the OCO-2 satellite and the divergent prior fluxes used in different inversion models. Four sensitivity experiments are performed herein to vary the prior fluxes and uncertainties in our inversion system, suggesting that regions that lack OCO-2 coverage are sensitive to the priors, especially over the tropics and high latitudes. In the further development of our inversion system, we will optimize the data-assimilation configuration to fully utilize current observations and increase the spatial and seasonal representativeness of the prior fluxes over regions that lack observations. [ABSTRACT FROM AUTHOR]

A 30-year (1980–2010) climatology of the major variables and terms of the transformed Eulerian-mean (TEM) momentum and thermodynamic equations is constructed by using four global atmospheric reanalyses: the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2); the Japanese 55-year Reanalysis (JRA-55); the European Centre for Medium-Range Weather Forecasts (ECMWF) interim reanalysis (ERA-Interim); and the Climate Forecast System Reanalysis (CFSR). Both the reanalysis ensemble mean (REM) and the differences in each reanalysis from the REM are investigated in the latitude–pressure domain for December–January–February and for June–July–August. For the REM investigation, two residual vertical velocities (the original one and one evaluated from residual meridional velocity) and two mass streamfunctions (from meridional and vertical velocities) are compared. Longwave (LW) radiative heating and shortwave (SW) radiative heating are also shown and discussed. For the TEM equations, the residual terms are also calculated and investigated for their potential usefulness, as the residual term for the momentum equation should include the effects of parameterized processes such as gravity waves, while that for the thermodynamic equation should indicate the analysis increment. Inter-reanalysis differences are investigated for the mass streamfunction, LW and SW heating, the two major terms of the TEM momentum equation (the Coriolis term and the Eliassen–Palm flux divergence term), and the two major terms of the TEM thermodynamic equation (the vertical temperature advection term and the total diabatic heating term). The spread among reanalysis TEM momentum balance terms is around 10 % in Northern Hemisphere winter and up to 50 % in Southern Hemisphere winter. The largest uncertainties in the thermodynamic equation (about 50 %) are found in the vertical advection, for which the structure is inconsistent with the differences in heating. The results shown in this paper provide basic information on the degree of agreement among recent reanalyses in the stratosphere and upper troposphere in the TEM framework. [ABSTRACT FROM AUTHOR]

An artificial neural network cloud classification scheme is combined with A-Train observations to characterize the physical properties and radiative effects of marine low clouds based on their morphology and type of mesoscale cellular convection (MCC) on a global scale. The cloud morphological categories are (i) organized closed MCC, (ii) organized open MCC and (iii) cellular but disorganized MCC. Global distributions of the frequency of occurrence of MCC types show clear regional signatures. Organized closed and open MCCs are most frequently found in subtropical regions and in mid-latitude storm tracks of both hemispheres. Cellular but disorganized MCC are the predominant type of marine low clouds in regions with warmer sea surface temperature such as in the tropics and trade wind zones. All MCC types exhibit a pronounced seasonal cycle. The physical properties of MCCs such as cloud fraction, radar reflectivity, drizzle rates and cloud top heights as well as the radiative effects of MCCs are found highly variable and a function of the type of MCC. On a global scale, the cloud fraction is largest for closed MCC with mean cloud fractions of about 90%whereas cloud fractions of open and cellular but disorganized MCC are only about 51% and 40 %, respectively. Probability density functions (PDFs) of cloud fractions are heavily skewed and exhibit modest regional variability. PDFs of column maximum radar reflectivities and inferred cloud base drizzle rates indicate fundamental differences in the cloud and precipitation characteristics of different MCC types. Similarly, the radiative effects of MCCs differ substantially from each other in terms of shortwave reflectance and transmissivity. These differences highlight the importance of low cloud morphologies and their associated cloudiness on the shortwave cloud forcing. [ABSTRACT FROM AUTHOR]

The ammonia cycle and nitrate particle formation have been introduced in the LMDz- INCA global model. Both fine nitrate particles formation in the accumulation mode and coarse nitrate forming on existing dust and sea-salt particles are considered. The model simulates distributions of nitrates and related species in agreement with previous studies and observations. The calculated present-day total nitrate direct radiative forcing since the pre-industrial is -0.056Wm-2. This forcing has the same magnitude than the forcing associated with organic carbon particles and represents 18% of the sulfate forcing. Fine particles largely dominate the nitrate forcing representing close to 90% of this value. The model has been used to investigate the future changes in nitrates and direct radiative forcing of climate based on snapshot simulations for the four Representative Concentration Pathway (RCP) scenarios and for the 2030, 2050 and 2100 time horizons. Due to a decrease in fossil fuel emissions in the future, the concentrations of most of the species involved in the nitrate-ammonium-sulfate system drop by 2100 except for ammonia which originates from agricultural practices and for which emissions significantly increase in the future. Despite the decrease of nitrate surface levels in Europe and Northern America, the global burden of accumulation mode nitrates increases by up to a factor of 2.6 in 2100. This increase in nitrate in the future arises despite decreasing NOx emissions due to increased availability of ammonia to form ammonium nitrate. The total aerosol direct forcing decreases from its present-day value of -0.234Wm-2 to a range of -0.070 to -0.130Wm-2 in 2100 based on the considered scenario. The direct forcing decreases for all aerosols except for nitrates for which the direct negative forcing increases to a range of -0.060 to -0.115Wm-2 in 2100. Including nitrates in the radiative forcing calculations increases the total direct forcing of aerosols by a factor of 1.3 in 2000, by a factor of 1.7-2.6 in 2030, by 1.9-4.8 in 2050 and by 6.4-8.6 in 2100. These results show that agricultural emissions of ammonia will play a key role in the future mitigation of climate change with nitrates becoming the dominant contributor to the anthropogenic aerosol optical depth during the second half of the XXIst century and significantly increasing the calculated aerosol direct forcing. This significant increase in the influence that nitrate exert on climate in the future will at the same time affect regional air quality and nitrogen deposition to the ecosystems. [ABSTRACT FROM AUTHOR]

Frequent SO2 noontime peak phenomenon was discovered in a detailed analysis on the SO2 concentrations in the North China Plain (NCP). The possible causes and their contributions are analysed. The impacts of such a phenomenon on the sulphur cycle were studied and the implications of the phenomenon for atmospheric chemistry, cloud physics and climate were discussed. Different from the common SO2 diurnal patterns with high nighttime concentrations, NCP witnessed high frequencies of SO2 noontime peaks, with an occurrence frequency of 50-72% at the four stations. Downmixing of elevated pollution layers, plume transport processes, mountain-valley-winds and fog/high RH haze events were the possible causes. The contribution of each process varies from each other and from station to station, however, neither of those four processes can be neglected. SO2 peaks occurring during noontime instead of nighttime will lead to a 13-35% increase in sulphur dry deposition, 9-23% increase in gas phase oxidation and 8-33% increase in aqueous phase conversions, which will increase the hygroscopicity and the light scattering of aerosols, thus having important impacts on atmospheric chemistry, cloud physics and climate. [ABSTRACT FROM AUTHOR]

Long-term (1984-2012) surface observations from 70 stations in the Sahara and Sahel are used to explore the diurnal, seasonal and geographical variations in dust emission events and thresholds. The frequency of dust emission (FDE) is calculated using the present weather codes of SYNOP reports. Thresholds are estimated as the wind speed for which there is a 50% probability of dust emission and are then used to calculate strong wind frequency (SWF) and dust uplift potential (DUP), where the latter is an estimate of the dust-generating power of winds. Stations are grouped into six coherent geographical areas for more in-depth analysis. FDE is highest at stations in Sudan and overall peaks in spring north of 23° N. South of this, where stations are directly influenced by the summer monsoon, the annual cycle in FDE is more variable. Thresholds are highest in northern Algeria, lowest in the latitude band 16-21° N and have greatest seasonal variations in the Sahel. Spatial variability in thresholds partly explain spatial variability in frequency of dust emission events on an annual basis. However, seasonal variations in thresholds for the six grouped areas are not the main control on seasonal variations in FDE. This is demonstrated by highly correlated seasonal cycles of FDE and SWF which are not significantly changed by using a fixed, or seasonally varying, threshold. The likely meteorological mechanisms generating these patterns such as low-level jets and haboobs are discussed. [ABSTRACT FROM AUTHOR]

A new climatology of stratospheric BrO profiles based on a parameterization using dynamical and chemical indicators has been developed, with the aim to apply it to the retrieval of tropospheric BrO columns from space nadir measurements. The adopted parameterization is based on three years of output data from the 3-D chemistry transport model BASCOE. The impact of the atmospheric dynamics on the stratospheric BrO distribution is treated by means of Bry/ozone correlations built from 3-D-CTM model results, while photochemical effects are taken into account using stratospheric NO2 columns as an indicator of the BrO/Bry ratio. The model simulations have been optimized for bromine chemistry and budget, and validated through comparisons using an extensive data set of ground-based, balloon-borne and satellite limb (SCIAMACHY) stratospheric BrO observations. [ABSTRACT FROM AUTHOR]

In 2016–2018, the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project undertook 3-month-long deployments to the southeastern (SE) Atlantic Ocean using research aircraft to better understand the impact of biomass burning (BB) aerosol transport to the SE Atlantic Ocean on climate. In this (part 1 of the meteorological overview) paper, the climatological features at monthly timescales are investigated. The southern African easterly jet (AEJ-S), defined as the zonal easterlies over 600–700 hPa exceeding 6 m s -1 around 5–15 ∘ S, is a characteristic feature of the mid-level circulation over southern Africa that was also during the deployment months of August 2017, September 2016, and October 2018. Climatologically, the AEJ-S develops at lower altitudes (∼ 3 km; 700 hPa) between 5–10 ∘ S in August, while it develops at around 4 km (∼ 600 hPa) and further south (5–15 ∘ S) in September and October, largely driven by the strong sensible heating over the African plateau. Notable meteorological anomalous characteristics during the 3 deployment months, compared to climatology (2000–2018), include the following: (1) during August 2017, the AEJ-S was weaker than the climatological mean, with an additional anomalous upper-level jet aloft (∼ 6 km) around 10 ∘ S. August 2017 was also drier over the SE Atlantic at 600–700 hPa than climatology, with a stronger Benguela low-level jet (LLJ) at 925–950 hPa along the Namibian coast of the SE Atlantic. Consistent with this, the southern Atlantic anticyclone was also stronger and closer to the coast than the August climatological mean. (2) During September 2016, the AEJ-S intensity was similar to the climatological mean, although the heat low and vertical motion over the land was slightly stronger compared to the September climatology. The LLJ and the large-scale southern Atlantic anticyclone were stronger than the climatological mean. (3) During October 2018, the AEJ-S was slightly weaker compared to the climatological mean, as was the LLJ and the southern Atlantic anticyclone. October 2018 was wetter over the Benguela coastal region at 600 hPa than the climatological mean. During all the deployment months, the sea surface temperatures (SST) over the SE Atlantic were warmer than the climatological means, but the monthly mean low cloud fraction was only noticeably reduced in August 2017. A weak August 2017 AEJ-S can explain low offshore black carbon (BC) mixing ratios within the European Centre for Medium-Range Weather Forecasts (ECMWF) Copernicus Atmosphere Monitoring Service (CAMS) reanalysis, although the BC peak altitude, at 2–3 km, is below that of the AEJ-S. The upper-level wave disturbance and the associated anomalous circulation also explain the weakening of AEJ-S through the reduction of the strength of the heat low over the land during August 2017. [ABSTRACT FROM AUTHOR]

Sub-Saharan Africa (SSA) is a global hot spot for aerosol emissions, which affect the regional climate and air quality. In this paper, we use ground-based observations to address the large uncertainties in the source-resolved emission estimation of carbonaceous aerosols. Ambient fine fraction aerosol was collected on filters at the high-altitude (2590 m a.s.l.) Rwanda Climate Observatory (RCO), a SSA background site, during the dry and wet seasons in 2014 and 2015. The concentrations of both the carbonaceous and inorganic ion components show a strong seasonal cycle, with highly elevated concentrations during the dry season. Source marker ratios, including carbon isotopes, show that the wet and dry seasons have distinct aerosol compositions. The dry season is characterized by elevated amounts of biomass burning products, which approach ∼95 % for carbonaceous aerosols. An isotopic mass-balance estimate shows that the amount of the carbonaceous aerosol stemming from savanna fires may increase from 0.2 µ g m -3 in the wet season up to 10 µ g m -3 during the dry season. Based on these results, we quantitatively show that savanna fire is the key modulator of the seasonal aerosol composition variability at the RCO. [ABSTRACT FROM AUTHOR]

A suite of aerosol physical and chemical measurements were made at the Mace Head Atmospheric Research Station, Co. Galway, Ireland, a coastal site on the eastern seaboard of the north Atlantic Ocean during NAMBLEX. The data have been used in this paper to show that over a wide range of aerosol sizes there is no impact of the inter-tidal zone or the surf zone on measurements made at 7m above ground level or higher. During the measurement period a range of air mass types were observed. During anticyclonic periods and conditions of continental outflow Aitken and accumulation mode were enhanced by a factor of 5 compared to the marine sector, whilst coarse mode particles were enhanced during westerly conditions. Baseline marine conditions were rarely met at Mace Head during NAMBLEX and high wind speeds were observed for brief periods only. The NAMBLEX experiment focussed on a detailed assessment of photochemistry in the marine environment, investigating the linkage between the HOx and the halogen radical cycles. Heterogeneous losses are important in both these cycles. In this paper loss rates of gaseous species to aerosol surfaces were calculated for a range of uptake coefficients. Even when the accommodation coefficient is unity, lifetimes due to heterogeneous loss of less than 10 s were never observed and rarely were they less than 500 s. Diffusional limitation to mass transfer is important in most conditions as the coarse mode is always significant. We calculate a minimum overestimate of 50% in the loss rate if this is neglected and so it should always be considered when calculating loss rates of gaseous species to particle surfaces. HO2 and HOI have accommodation coefficients of around 0.03 and hence we calculate lifetimes due to loss to particle surfaces of 2000 s or greater under the conditions experienced during NAMBLEX. Aerosol composition data collected during this experiment provide representative information on the input aerosol characteristics to western Europe. During NAMBLEX the submicron aerosol was predominately acidified sulphate and organic material, which was most likely internally mixed. The remaining accumulation mode aerosol was sea salt. The organic and sulphate fractions were approximately equally important, though the mass ratio varies considerably between air masses. Mass spectral fingerprints of the organic fraction in polluted conditions are similar to those observed at other locations that are characterised by aged continental aerosol. In marine conditions, the background input of both sulphate and organic aerosol into Europe was observed to be between 0.5 and 1µgm-3. Key differences in the mass spectra were observed during the few clean periods but were insufficient to ascertain whether these changes reflect differences in the source fingerprint of the organic aerosol. The coarse mode was composed of sea salt and showed significant displacement of chloride by nitrate and to a lesser extent sulphate in polluted conditions. [ABSTRACT FROM AUTHOR]

This paper presents a summary of the work done within the European Union's Seventh Framework Programme project ECLIPSE (Evaluating the Climate and Air Quality Impacts of Short-Lived Pollutants). ECLIPSE had a unique systematic concept for designing a realistic and effective mitigation scenario for short-lived climate pollutants (SLCPs; methane, aerosols and ozone, and their precursor species) and quantifying its climate and air quality impacts, and this paper presents the results in the context of this overarching strategy. The first step in ECLIPSE was to create a new emission inventory based on current legislation (CLE) for the recent past and until 2050. Substantial progress compared to previous work was made by including previously unaccounted types of sources such as flaring of gas associated with oil production, and wick lamps. These emission data were used for present-day reference simulations with four advanced Earth system models (ESMs) and six chemistry transport models (CTMs). The model simulations were compared with a variety of ground-based and satellite observational data sets from Asia, Europe and the Arctic. It was found that the models still underestimate the measured seasonality of aerosols in the Arctic but to a lesser extent than in previous studies. Problems likely related to the emissions were identified for northern Russia and India, in particular. To estimate the climate impacts of SLCPs, ECLIPSE followed two paths of research: the first path calculated radiative forcing (RF) values for a large matrix of SLCP species emissions, for different seasons and regions independently. Based on these RF calculations, the Global Temperature change Potential metric for a time horizon of 20 years (GTP20) was calculated for each SLCP emission type. This climate metric was then used in an integrated assessment model to identify all emission mitigation measures with a beneficial air quality and short-term (20-year) climate impact. These measures together defined a SLCP mitigation (MIT) scenario. Compared to CLE, the MIT scenario would reduce global methane (CH4) and black carbon (BC) emissions by about 50 and 80%, respectively. For CH4, measures on shale gas production, waste management and coal mines were most important. For non-CH4 SLCPs, elimination of high-emitting vehicles and wick lamps, as well as reducing emissions from gas flaring, coal and biomass stoves, agricultural waste, solvents and diesel engines were most important. These measures lead to large reductions in calculated surface concentrations of ozone and particulate matter. We estimate that in the EU, the loss of statistical life expectancy due to air pollution was 7.5 months in 2010, which will be reduced to 5.2 months by 2030 in the CLE scenario. The MIT scenario would reduce this value by another 0.9 to 4.3 months. Substantially larger reductions due to the mitigation are found for China (1.8 months) and India (11-12 months). The climate metrics cannot fully quantify the climate response. Therefore, a second research path was taken. Transient climate ensemble simulations with the four ESMs were run for the CLE and MIT scenarios, to determine the climate impacts of the mitigation. In these simulations, the CLE scenario resulted in a surface temperature increase of 0.70±0.14K between the years 2006 and 2050. For the decade 2041-2050, the warming was reduced by 0.22±0.07K in the MIT scenario, and this result was in almost exact agreement with the response calculated based on the emission metrics (reduced warming of 0.22±0.09 K). The metrics calculations suggest that non-CH4 SLCPs contribute ~22% to this response and CH4 78%. This could not be fully confirmed by the transient simulations, which attributed about 90% of the temperature response to CH4 reductions. Attribution of the observed temperature response to non-CH4 SLCP emission reductions and BC specifically is hampered in the transient simulations by small forcing and co-emitted species of the emission basket chosen. Nevertheless, an important conclusion is that our mitigation basket as a whole would lead to clear benefits for both air quality and climate. The climate response from BC reductions in our study is smaller than reported previously, possibly because our study is one of the first to use fully coupled climate models, where unforced variability and sea ice responses cause relatively strong temperature fluctuations that may counteract (and, thus, mask) the impacts of small emission reductions. The temperature responses to the mitigation were generally stronger over the continents than over the oceans, and with a warming reduction of 0.44K (0.39- 0.49)K the largest over the Arctic. Our calculations suggest particularly beneficial climate responses in southern Europe, where surface warming was reduced by about 0.3K and precipitation rates were increased by about 15 (6-21)mmyr??1 (more than 4% of total precipitation) from spring to autumn. Thus, the mitigation could help to alleviate expected future drought and water shortages in the Mediterranean area. We also report other important results of the ECLIPSE project. [ABSTRACT FROM AUTHOR]

Trace gases and aerosols play a crucial role in shaping Arctic climate through their impacts on radiation and chemistry. The concentration of these substances over the Arctic is largely determined by long-range transport originating from midlatitude and tropical source regions. In this study, we explore how atmospheric circulation modulates the interannual variability of long-range transport into the Arctic by utilizing a chemistry–climate model. Idealized tracers, which have fixed lifetimes and spatially varying but temporally fixed surface emissions corresponding to the climatology of anthropogenic emissions of the year 2000, are employed to isolate the role of atmospheric transport from emission and chemistry in modulating interannual variability. Tracers emitted from different source regions are tagged to quantify their relative contributions. Model simulations reveal that tracers from Europe, East Asia, and North America contribute the most to Arctic tracer mass, followed by those from the Tibetan Plateau and South Asia, as well as the Middle East. These regional tracers are predominantly transported into the Arctic middle to upper troposphere, with the exception of tracers from Europe during winter, which are transported into the Arctic lower troposphere. Our analysis shows that the interannual variability of transport into the Arctic for each regional tracer is determined by the atmospheric circulation over the corresponding emission region; i.e., anomalous poleward and eastward winds over the source region promote transport into the Arctic. Considering tracers with global emissions, a southward shift of the midlatitude jet during winter favors increased transport into the Arctic, particularly for tracers emitted over Asia, aligning with previous studies. Comparisons of tracers with different lifetimes indicate that the interannual variability of shorter lifetime tracers is predominantly influenced by regional tracers with shorter transport pathways into the Arctic (e.g., Europe), while the interannual variability of longer lifetime tracers is more contributed by regional tracers with higher emissions (e.g., East Asia). [ABSTRACT FROM AUTHOR]

The interactions that occur between aerosols and a mixed-phase cloud system, and the subsequent alteration of the microphysical state of such clouds, are a problem that has yet to be well constrained. Advancing our understanding of aerosol--ice processes is necessary to determine the impact of natural and anthropogenic emissions on Earth's climate and to improve our capability to predict future climate states. This paper deals specifically with how aerosols influence ice mass production in low-level Arctic mixed-phase clouds. In this study, a 9-year record of aerosol, cloud and atmospheric state properties is used to quantify aerosol influence on ice production in mixed-phase clouds. It is found that mixed-phase clouds present in a clean aerosol state have higher ice water content (IWC) by a factor of 1.22 to 1.63 at cloud base than do similar clouds in cases with higher aerosol loading. We additionally analyze radar-derived mean Doppler velocities to better understand the drivers behind this relationship, and we conclude that aerosol induced reduction of the ice crystal nucleation rate, together with decreased riming rates in polluted clouds, are likely influences on the observed reductions in IWC. [ABSTRACT FROM AUTHOR]

The retrieval of aerosol properties from satellite observations provides their spatial distribution over a wide area in cloud-free conditions. As such, they complement ground-based measurements by providing information over sparsely instrumented areas, albeit that significant differences may exist in both the type of information obtained and the temporal information from satellite and ground-based observations. In this paper, information from different types of satellite-based instruments is used to provide a 3-D climatology of aerosol properties over mainland China, i.e., vertical profiles of extinction coefficients from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP), a lidar flying aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite and the columnintegrated extinction (aerosol optical depth – AOD) available from three radiometers: the European Space Agency (ESA)’s Along-Track Scanning Radiometer version 2 (ATSR-2), Advanced Along-Track Scanning Radiometer (AATSR) (together referred to as ATSR) and NASA’s Moderate Resolution Imaging Spectroradiometer (MODIS) aboard the Terra satellite, together spanning the period 1995–2015. AOD data are retrieved from ATSR using the ATSR dual view (ADV) v2.31 algorithm, while for MODIS Collection 6 (C6) the AOD data set is used that was obtained from merging the AODs obtained from the dark target (DT) and deep blue (DB) algorithms, further referred to as the DTDB merged AOD product. These data sets are validated and differences are compared using Aerosol Robotic Network (AERONET) version 2 L2.0 AOD data as reference. The results show that, over China, ATSR slightly underestimates the AOD and MODIS slightly overestimates the AOD. Consequently, ATSR AOD is overall lower than that from MODIS, and the difference increases with increasing AOD. The comparison also shows that neither of the ATSR and MODIS AOD data sets is better than the other one everywhere. However, ATSR ADV has limitations over bright surfaces which the MODIS DB was designed for. To allow for comparison of MODIS C6 results with previous analyses where MODIS Collection 5.1 (C5.1) data were used, also the difference between the C6 and C5.1 merged DTDB data sets from MODIS/Terra over China is briefly discussed. The AOD data sets show strong seasonal differences and the seasonal features vary with latitude and longitude across China. Two-decadal AOD time series, averaged over all of mainland China, are presented and briefly discussed. Using the 17 years of ATSR data as the basis and MODIS/Terra to follow the temporal evolution in recent years when the environmental satellite Envisat was lost requires a comparison of the data sets for the overlapping period to show their complementarity. ATSR precedes the MODIS time series between 1995 and 2000 and shows a distinct increase in the AOD over this period. The two data series show similar variations during the overlapping period between 2000 and 2011, with minima and maxima in the same years. MODIS extends this time series beyond the end of the Envisat period in 2012, showing decreasing AOD. [ABSTRACT FROM AUTHOR]

Two of the most basic parameters generated from a reanalysis are temperature and winds. Temperatures in the reanalyses are derived from conventional (surface and balloon), aircraft, and satellite observations. Winds are observed by conventional systems, cloud tracked, and derived from height fields, which are in turn derived from the vertical temperature structure. In this paper we evaluate as part of the SPARC Reanalysis Intercomparison Project (S-RIP) the temperature and wind structure of all the recent and past reanalyses. This evaluation is mainly among the reanalyses themselves, but comparisons against independent observations, such as HIRDLS and COSMIC temperatures, are also presented. This evaluation uses monthly mean and 2.5° zonal mean data sets and spans the satellite era from 1979-2014. There is very good agreement in temperature seasonally and latitudinally among the more recent reanalyses (CFSR, MERRA, ERA-Interim, JRA-55, and MERRA-2) between the surface and 10 hPa. At lower pressures there is increased variance among these reanalyses that changes with season and latitude. This variance also changes during the time span of these reanalyses with greater variance during the TOVS period (1979-1998) and less variance afterward in the ATOVS period (1999-2014). There is a distinct change in the temperature structure in the middle and upper stratosphere during this transition from TOVS to ATOVS systems. Zonal winds are in greater agreement than temperatures and this agreement extends to lower pressures than the temperatures. Older reanalyses (NCEP/NCAR, NCEP/DOE, ERA-40, JRA-25) have larger temperature and zonal wind disagreement from the more recent reanalyses. All reanalyses to date have issues analysing the quasi-biennial oscillation (QBO) winds. Comparisons with Singapore QBO winds show disagreement in the amplitude of the westerly and easterly anomalies. The disagreement with Singapore winds improves with the transition from TOVS to ATOVS observations. Temperature bias characteristics determined via comparisons with a reanalysis ensemble mean (MERRA, ERA-Interim, JRA-55) are similarly observed when compared with Aura HIRDLS and Aura MLS observations. There is good agreement among the NOAA TLS, SSU1, and SSU2 Climate Data Records and layer mean temperatures from the more recent reanalyses. Caution is advised for using reanalysis temperatures for trend detection and anomalies from a long climatology period as the quality and character of reanalyses may have changed over time. [ABSTRACT FROM AUTHOR]

Reanalysis data sets are widely used to understand atmospheric processes and past variability, and are often used to stand in as "observations" for comparisons with climate model output. Because of the central role of water vapor (WV) and ozone (O3) in climate change, it is important to understand how accurately and consistently these species are represented in existing global reanalyses. In this paper, we present the results of WV and O3 intercomparisons that have been performed as part of the SPARC (Stratosphere- troposphere Processes and their Role in Climate) Reanalysis Intercomparison Project (S-RIP). The comparisons cover a range of timescales and evaluate both inter-reanalysis and observation-reanalysis differences. We also provide a systematic documentation of the treatment of WV and O3 in current reanalyses to aid future research and guide the interpretation of differences amongst reanalysis fields. The assimilation of total column ozone (TCO) observations in newer reanalyses results in realistic representations of TCO in reanalyses except when data coverage is lacking, such as during polar night. The vertical distribution of ozone is also relatively well represented in the stratosphere in reanalyses, particularly given the relatively weak constraints on ozone vertical structure provided by most assimilated observations and the simplistic representations of ozone photochemical processes in most of the reanalysis forecast models. However, significant biases in the vertical distribution of ozone are found in the upper troposphere and lower stratosphere in all reanalyses. In contrast to O3, reanalysis estimates of stratospheric WV are not directly constrained by assimilated data. Observations of atmospheric humidity are typically used only in the troposphere, below a specified vertical level at or near the tropopause. The fidelity of reanalysis stratospheric WV products is therefore mainly dependent on the reanalyses' representation of the physical drivers that influence stratospheric WV, such as temperatures in the tropical tropopause layer, methane oxidation, and the stratospheric overturning circulation. The lack of assimilated observations and known deficiencies in the representation of stratospheric transport in reanalyses result in much poorer agreement amongst observational and reanalysis estimates of stratospheric WV. Hence, stratospheric WV products from the current generation of reanalyses should generally not be used in scientific studies. [ABSTRACT FROM AUTHOR]

The acquisition and dissemination of essential information for understanding global biogeochemical interactions between the atmosphere and ecosystems and how climate–ecosystem feedback loops may change atmospheric composition in the future comprise a fundamental prerequisite for societal resilience in the face of climate change. In particular, the detection of trends and seasonality in the abundance of greenhouse gases and short-lived climate-active atmospheric constituents is an important aspect of climate science. Therefore, easy and fast access to reliable, long-term, and high-quality observational environmental data is recognised as fundamental to research and the development of environmental forecasting and assessment services. In our opinion article, we discuss the potential role that environmental research infrastructures in Europe (ENVRI RIs) can play in the context of an integrated global observation system. In particular, we focus on the role of the atmosphere-centred research infrastructures ACTRIS (Aerosol, Clouds and Trace Gases Research Infrastructure), IAGOS (In-service Aircraft for a Global Observing System), and ICOS (Integrated Carbon Observation System), also referred to as ATMO-RIs, with their capabilities for standardised collection and provision of long-term and high-quality observational data, complemented by rich metadata. The ATMO-RIs provide data through open access and offer data interoperability across different research fields including all fields of environmental sciences and beyond. As a result of these capabilities in data collection and provision, we elaborate on the novel research opportunities in atmospheric sciences which arise from the combination of open-access and interoperable observational data, tools, and technologies offered by data-intensive science and the emerging collaboration platform ENVRI-Hub, hosted by the European Open Science Cloud (EOSC). [ABSTRACT FROM AUTHOR]

The contrail formation potential as well as its temporal and spatial distribution is estimated using meteorological conditions of temperature and relative humidity from the ERA5 re-analysis provided by the European Centre for Medium-Range Weather Forecasts. Contrail formation is estimated with the Schmidt–Appleman criterion (SAc), solely considering thermodynamic effects. The focus is on a region ranging from the Eastern United States (110–65° W) to central Europe (5° W–30° E). Around 18 000 flight trajectories from the In-service Aircraft for a Global Observing System (IAGOS) are used as a representative subset of transatlantic, commercial flights. The typical crossing distance through a contrail-prone area is determined based on IAGOS measurements of temperature T and relative humidity r and then based on co-located ERA5 simulations of the same quantities. Differences in spatial resolution between IAGOS and ERA5 are addressed from an aircraft-centered perspective, using 1 km segments, and a model-centered perspective, using 19 km flight sections. Using the aircraft-centered approach, 50 % of the crossings of persistent contrail (PC) regions based on IAGOS are shorter than 9 km, while in ERA5 the median is 155 km. Time-averaged IAGOS data lead to a median crossing length of 66 km. The difference between the two data sets is attributed to the higher variability of r in IAGOS compared to ERA5. The model-centered approach yields similar results, but typical crossing lengths are larger by only up to 10 %. Binary masks of PC formation are created by applying the SAc on the two-dimensional fields of T and r from ERA5. In a second step the morphology of PC regions is also assessed. Half of the PC regions in ERA5 are found to be smaller than ≈ 35 000 km2 (at 200 hPa), and the median of the maximum dimension is shorter than 760 km (at 200 hPa). Furthermore, PC regions tend to be of near-circular shape with a tendency to a slight oval shape and a preferred alignment along the dominant westerly flow. Seasonal, vertical distributions of PC formation potential P are characterized by a maximum between 250 and 200 hPa. P is subject to seasonal variations with a maximum in magnitude and extension during the winter months and a minimum during summer. The horizontal distribution of PC regions suggests that PC regions are likely to appear in the same location on adjacent pressure levels. Climatologies of T , r , wind speed U , and resulting PC formation potential are calculated to identify the constraining effects of T and r on P. PC formation is primarily limited by conditions that are too warm below and conditions that are too dry above the formation region. The distribution of PCs is slanted towards lower altitudes from 30 to 70° N, following lines of constant T and r. For an observed co-location of high U and P , it remains unclear whether PC formation and the jet stream are favored by the same meteorological conditions or if the jet stream itself favors PC occurrence. This analysis suggests that some PC regions will be difficult to avoid by rerouting aircraft because of their large vertical and horizontal extents. [ABSTRACT FROM AUTHOR]

Classical error analysis in remote sounding distinguishes between four classes: "smoothing errors," "model parameter errors," "forward model errors," and "retrieval noise errors". For infrared sounding "interference errors", which, in general, cannot be described by these four terms, can be significant. Interference errors originate from spectral residuals due to "interfering species" whose spectral features overlap with the signatures of the target species. A general method for quantification of interference errors is presented, which covers all possible algorithmic implementations, i.e., fine-grid retrievals of the interfering species or coarse-grid retrievals, and cases where the interfering species are not retrieved. In classical retrieval setups interference errors can exceed smoothing errors and can vary by orders of magnitude due to state dependency. An optimum strategy is suggested which practically eliminates interference errors by systematically minimizing the regularization strength applied to joint profile retrieval of the interfering species. This leads to an interfering-species selective deweighting of the retrieval. Details of microwindow selection are no longer critical for this optimum retrieval and widened microwindows even lead to reduced overall (smoothing and interference) errors. Since computational power will increase, more and more operational algorithms will be able to utilize this optimum strategy in the future. The findings of this paper can be applied to soundings of all infrared-active atmospheric species, which include more than two dozen different gases relevant to climate and ozone. This holds for all kinds of infrared remote sounding systems, i.e., retrievals from ground-based, balloon-borne, airborne, or satellite spectroradiometers. [ABSTRACT FROM AUTHOR]

This paper presents key results achieved by an analysis of the relation between high-quality simultaneous Dobson, Brewer ground and TOMS-V8, GOME-WFDOAS satellite total ozone observations for Hradec Kralove, Czech Republic. Statistically significant seasonal differences with maxima up to 4% of monthly averages have been found between Dobson and Brewer measurements during the winter/ spring months. These differences can influence estimations of ozone trends if combined data series are used after replacing a Dobson instrument by a Brewer spectrophotometer. The differences can be attributed mostly to the influence of temperature on ozone absorption coefficients and to total sulphur dioxide. Similar seasonal differences exist between Dobson, GOME and Brewer, TOMS data sets at Hradec Kralove while Dobson versus TOMS and Brewer versus GOME observations fit well with each other within the instrumental accuracy of spectrophotometers. The above findings are supposed to be relevant to other mid and high latitude stations and they have been confirmed by several independent analyses. The conclusions should be considered by data users because the differences between particular ground and satellite data sets can influence validation of satellite ozone observing systems and analyses of recovery of the ozone layer in mid and high latitudes, among others. [ABSTRACT FROM AUTHOR]

The North Atlantic Marine Boundary Layer Experiment (NAMBLEX), involving over 50 scientists from 12 institutions, took place at Mace Head, Ireland (53.32° N, 9.90° W), between 23 July and 4 September 2002. A wide range of state-of-the-art instrumentation enabled detailed measurements of the boundary layer structure and atmospheric composition in the gas and aerosol phase to be made, providing one of the most comprehensive in situ studies of the marine boundary layer to date. This overview paper describes the aims of the NAMBLEX project in the context of previous field campaigns in the Marine Boundary Layer (MBL), the overall layout of the site, a summary of the instrumentation deployed, the temporal coverage of the measurement data, and the numerical models used to interpret the field data. Measurements of some trace species were made for the first time during the campaign, which was characterised by predominantly clean air of marine origin, but more polluted air with higher levels of NOx originating from continental regions was also experienced. This paper provides a summary of the meteorological measurements and Planetary Boundary Layer (PBL) structure measurements, presents time series of some of the longer-lived trace species (O3, CO, H2, DMS, CH4, NMHC, NOx, NOy, PAN) and summarises measurements of other species that are described in more detail in other papers within this special issue, namely oxygenated VOCs, HCHO, peroxides, organohalogenated species, a range of shorter lived halogen species (I2, OIO, IO, BrO), NO3 radicals, photolysis frequencies, the free radicals OH, HO2 and (HO2+ΣRO2), as well as a summary of the aerosol measurements. NAMBLEX was supported by measurements made in the vicinity of Mace Head using the NERC Dornier-228 aircraft. Using ECMWF windfields, calculations were made of the air-mass trajectories arriving at Mace Head during NAMBLEX, and were analysed together with both meteorological and trace-gas measurements. In this paper a chemical climatology for the duration of the campaign is presented to interpret the distribution of air-mass origins and emission sources, and to provide a convenient framework of air-mass classification that is used by other papers in this issue for the interpretation of observed variability in levels of trace gases and aerosols. [ABSTRACT FROM AUTHOR]

In spite of impressive advances in recent years, our present understanding of organic aerosol (OA) composition, physical and chemical properties, sources and transformation characteristics is still rather limited, and their environmental effects remain highly uncertain. This paper discusses and prioritizes issues related to organic aerosols and their effects on atmospheric processes and climate, providing a basis for future activities in the field. Four main topical areas are addressed: i) sources of OA; ii) formation transformation and removal of OA; iii) physical, chemical and mixing state of OA; iv) atmospheric modelling of OA. Key questions and research priorities regarding these four areas are synthesized in this paper, and outstanding issues for future research are presented for each topical area. In addition, an effort is made to formulate a basic set of consistent and universally applicable terms and definitions for coherent description of atmospheric OA across different scales and disciplines. [ABSTRACT FROM AUTHOR]

The purpose of this study is to investigate horizontal transport processes in the winter stratosphere using data with a resolution relevant for chemistry and climate modeling. For this reason the Freie Universität Berlin Climate Middle Atmosphere Model (FUB-CMAM) with its model top at 83 km altitude, increased horizontal resolution T42 and the semi-Lagrangian transport scheme for advecting passive tracers is used. A new approach of this paper is the classification of specific transport phenomena within the stratosphere into tropical-subtropical streamers (e.g. Offermann et al., 1999) and polar vortex extrusions hereafter called polar vortex streamers. To investigate the role played by these largescale structures on the inter-annual and seasonal variability of transport processes in northern mid-latitudes, the global occurrence of such streamers was calculated based on a 10- year model climatology, concentrating on the existence of the Arctic polar vortex. For the identification and counting of streamers, the new method of zonal anomaly was chosen. The analysis of the months October-May yielded a maximum occurrence of tropical-subtropical streamers during Arctic winter and spring in the middle and upper stratosphere. Synoptic maps revealed highest intensities in the subtropics over East Asia with a secondary maximum over the Atlantic in the northern hemisphere. Furthermore, tropicalsubtropical streamers exhibited a higher occurrence than polar vortex streamers, indicating that the subtropical barrier is more permeable than the polar vortex barrier (edge) in the model, which is in good correspondence with observations (e.g. Plumb, 2002; Neu et al., 2003). Interesting for the total ozone decrease in mid-latitudes is the consideration of the lower stratosphere for tropical-subtropical streamers and the stratosphere above ∼20 km altitude for polar vortex streamers, where strongest ozone depletion is observed at polar latitudes (WMO, 2003). In the lower stratosphere the FUBCMAM simulated a climatological maximum of 10% occurrence of tropical-subtropical streamers over East-Asia/West Pacific and the Atlantic during early- and mid-winter. The results of this paper demonstrate that stratospheric streamers e.g. large-scale, tongue-like structures transporting tropical-subtropical and polar vortex air masses into midlatitudes occur frequently during Arctic winter. They can therefore play a significant role on the strength and variability of the observed total ozone decrease at mid-latitudes and should not be neglected in future climate change studies. [ABSTRACT FROM AUTHOR]

Massive amounts of Saharan dust are blown from the coast of northern Africa across the Atlantic Ocean towards the Americas each year. This dust has, depending on its chemistry, direct and indirect effects on global climate which include reflection and absorption of solar radiation as well as transport and deposition of nutrients and metals fertilizing both ocean and land. To determine the temporal and spatial variability of Saharan dust transport and deposition and their marine environmental effects across the equatorial North Atlantic Ocean, we have set up a monitoring experiment using deep-ocean sediment traps as well as land-based dust collectors. The sediment traps were deployed at five ocean sites along a transatlantic transect between north-west Africa and the Caribbean along 12° N, in a downwind extension of the land-based dust collectors placed at 19° N on the Mauritanian coast in Iouîk. In this paper, we lay out the setup of the monitoring experiment and present the particle fluxes from sediment trap sampling over 24 continuous and synchronized intervals from October 2012 through to November 2013. We establish the temporal distribution of the particle fluxes deposited in the Atlantic and compare chemical compositions with the land-based dust collectors propagating to the downwind sediment trap sites, and with satellite observations of Saharan dust outbreaks. First-year results show that the total mass fluxes in the ocean are highest at the sampling sites in the east and west, closest to the African continent and the Caribbean, respectively. Element ratios reveal that the lithogenic particles deposited nearest to Africa are most similar in composition to the Saharan dust collected in Iouîk. Downwind increasing Al, Fe and K contents suggest a downwind change in the mineralogical composition of Saharan dust and indicate an increasing contribution of clay minerals towards the west. In the westernmost Atlantic Ocean, admixture of re-suspended clay-sized sediments advected towards the deep sediment trap cannot be excluded. Seasonality is most prominent near both continents but generally weak, with mass fluxes dominated by calcium carbonate and clear seasonal maxima of biogenic silica towards the west. The monitoring experiment is now extended, with autonomous dust sampling buoys for better quantification of Saharan dust transport and deposition from source to sink and their impact on fertilization and carbon export to the deep ocean. [ABSTRACT FROM AUTHOR]

This paper analyses for the first time the impact of high-latitude blocks and subtropical ridges on near-surface ozone (O3) in Europe during a 15-year period. For this purpose, a catalogue of blocks and ridges over the Euro-Atlantic region is used together with a gridded dataset of maximum daily 8 h running average ozone (MDA8 O3) covering the period 1998-2012. The response of ozone to the location of blocks and ridges with centres in three longitudinal sectors (Atlantic, ATL, 30-0° W; European, EUR, 0-30° E; Russian, RUS, 30-60° E) is examined. The impact of blocks on ozone is regionally and seasonally dependent. In particular, blocks within the EUR sector yield positive ozone anomalies of ∼5-10 ppb over large parts of central Europe in spring and northern Europe in summer. Over 20 and 30% of the days with blocks in that sector register exceedances of the 90th percentile of the seasonal ozone distribution at many European locations during spring and summer, respectively. The impacts of ridges during those seasons are subtle and more sensitive to their specific location, although they can trigger ozone anomalies above 10 ppb in northern Italy and the surrounding countries in summer, eventually exceeding European air quality (AQ) targets. During winter, surface ozone in the north-west of Europe presents completely opposite responses to blocks and ridges. The anticyclonic circulation associated with winter EUR blocking, and to a lesser extent with ATL blocking, yields negative ozone anomalies between -5 and -10 ppb over the UK, northern France and the Benelux. Conversely, the enhanced zonal flow around 50-60° N during the occurrence of ATL ridges favours the arrival of background air masses from the Atlantic and the ventilation of the boundary layer, producing positive ozone anomalies of ∼5 ppb in an area spanning from the British Isles to the northern half of Germany. We also show that multiple linear models on the seasonal frequency of occurrence of these synoptic patterns can explain a considerable fraction of the interannual variability in some winter and summer ozone statistics (mean levels and number of exceedances of the 90th percentile) over some regions of western Europe. Thus, this work provides the first quantitative assessments of the remarkable but distinct impacts that the anticyclonic circulation and the diversion of the zonal flow associated with blocks and ridges exert on surface ozone in Europe. The findings reported here can be exploited in the future to evaluate the modelled responses of ozone to circulation changes within chemical transport models (CTMs) and chemistry- climate models (CCMs). [ABSTRACT FROM AUTHOR]

The Earth's mesopause region between about 75 and 105 km is characterised by chemiluminescent emission from various lines of different molecules and atoms. This emission was and is important for the study of the chemistry and dynamics in this altitude region at nighttime. However, our understanding is still very limited with respect to molecular emissions with low intensities and high line densities that are challenging to resolve. Based on 10 years of data from the astronomical X-shooter echelle spectrograph at Cerro Paranal in Chile, we have characterised in detail this nightglow (pseudo-)continuum in the wavelength range from 300 to 1800 nm. We studied the spectral features, derived continuum components with similar variability, calculated climatologies, studied the response to solar activity, and even estimated the effective emission heights. The results indicate that the nightglow continuum at Cerro Paranal essentially consists of only two components, which exhibit very different properties. The main structures of these components peak at 595 and 1510 nm. While the former was previously identified as the main peak of the FeO "orange arc" bands, the latter is a new discovery. Laboratory data and theory indicate that this feature and other structures between about 800 and at least 1800 nm are caused by emission from the low-lying A′′ and A′ states of HO2. In order to test this assumption, we performed runs with the Whole Atmosphere Community Climate Model (WACCM) with modified chemistry and found that the total intensity, layer profile, and variability indeed support this interpretation, where the excited HO2 radicals are mostly produced from the termolecular recombination of H and O2. The WACCM results for the continuum component that dominates at visual wavelengths show good agreement for FeO from the reaction of Fe and O3. However, the simulated total emission appears to be too low, which would require additional mechanisms where the variability is dominated by O3. A possible (but nevertheless insufficient) process could be the production of excited OFeOH by the reaction of FeOH and O3. [ABSTRACT FROM AUTHOR]

Evaluating global chemistry models in the upper troposphere–lower stratosphere (UTLS) is an important step toward an improved understanding of the chemical composition in this region. This composition is regularly sampled through in situ measurements based on passenger aircraft, in the framework of the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. This study focuses on the comparison of the IAGOS measurements in ozone, carbon monoxide (CO), nitrogen reactive species (NOy) and water vapour, with a 25-year simulation output from the LMDZ-OR-INCA chemistry–climate model. For this purpose, we present and apply an extension of the Interpol-IAGOS software that projects the IAGOS data onto any model grid, in order to derive a gridded IAGOS product and a masked (sub-sampled) model product that are directly comparable to one another. Climatologies are calculated in the upper troposphere (UT) and in the lower stratosphere (LS) separately but also in the UTLS as a whole, as a demonstration for the models that do not sort out the physical variables necessary to distinguish between the UT and the LS. In the northern extratropics, the comparison in the UTLS layer suggests that the geographical distribution in the tropopause height is well reproduced by the model. In the separated layers, the model simulates well the water vapour climatologies in the UT and the ozone climatologies in the LS. There are opposite biases in CO in both UT and LS, which suggests that the cross-tropopause transport is overestimated. The NOy observations highlight the difficulty of the model in parameterizing the lightning emissions. In the tropics, the upper-tropospheric climatologies are remarkably well simulated for water vapour. They also show realistic CO peaks due to biomass burning in the most convective systems, and the ozone latitudinal variations are well correlated between the observations and the model. Ozone is more sensitive to lightning emissions than to biomass burning emissions, whereas the CO sensitivity to biomass burning emissions strongly depends on location and season. The present study demonstrates that the Interpol-IAGOS software is a tool facilitating the assessment of global model simulations in the UTLS, which is potentially useful for any modelling experiment involving chemistry climate or chemistry transport models. [ABSTRACT FROM AUTHOR]

While nocturnal low-level jets (NLLJs) occur frequently in many parts of the world, the occurrence and other detailed characteristics of NLLJs over the Taklimakan Desert (TD) are not well known. This paper presents a climatology of NLLJs and coincident dust over the TD by analyzing multi-year ERA-Interim reanalysis and satellite observations. It is found that the ERA-Interim dataset can capture the NLLJs' features well by comparison with radiosonde data from two surface sites. The NLLJs occur in more than 60% of nights, which are primarily easterly to east-northeasterly. They typically appear at 100 to 400m above the surface with a speed of 4 to 10ms-1. Most NLLJs are located above the nocturnal inversion during the warm season, while they are embedded in the inversion layer during the cold season. NLLJs above the inversion have a strong annual cycle with a maximum frequency in August. We also quantify the convective boundary layer (CBL) height and construct an index to measure the magnitude of the momentum in the CBL. We find that the magnitude of momentum in the lower atmosphere from the top of the surface layer to the top of mixed layer is larger for NLLJ cases than for non-NLLJ cases, and in the warm season the downward momentum transfer process is more intense and rapid. The winds below the NLLJ core to the desert surface gain strength in summer and autumn, and these summer and autumn winds are coincident with an enhancement of aerosol optical depth. This indicates that the NLLJ is an important mechanism for dust activity and transport during the warm season over the Taklimakan. [ABSTRACT FROM AUTHOR]

The Tibetan Plateau (TP) has been contaminated by persistent organic pollutants (POPs), including legacy organochlorine pesticides (OCPs) and polychlorinated biphenyls (PCBs) through atmospheric transport. The exact source regions, transport pathways and time trends of POPs to the TP are not well understood. Here polystyrene-divinylbenzene copolymer resin (XAD)-based passive air samplers (PASs) were deployed at 16 Tibetan background sites from 2007 to 2012 to gain further insight into spatial patterns and temporal trends of OCPs and PCBs. The southeastern TP was characterized by dichlorodipheny-ltrichloroethane (DDT)-related chemicals delivered by Indian monsoon air masses. The northern and northwestern TP displayed the greatest absolute concentration and relative abundance of hexachlorobenzene (HCB) in the atmosphere, caused by the westerly-driven European air masses. The interactions between the DDT polluted Indian monsoon air and the clean westerly winds formed a transition zone in central Tibet, where both DDT and HCB were the dominant chemicals. Based on 5 years of continuous sampling, our data indicated declining concentrations of HCB and hexachlorocyclohexanes (HCHs) across the Tibetan region. Inter-annual trends of DDT class chemicals, however, showed less variation during this 5-year sampling period, which may be due to the ongoing usage of DDT in India. This paper demonstrates the possibility of using POP fingerprints to investigate the climate interactions and the validity of using PAS to derive inter-annual atmospheric POP time trends. [ABSTRACT FROM AUTHOR]

Wind predictions in complex terrain are important for a number of applications. Dynamic downscaling of numerical weather prediction (NWP) model winds with a highresolution wind model is one way to obtain a wind forecast that accounts for local terrain effects, such as wind speedup over ridges, flow channeling in valleys, flow separation around terrain obstacles, and flows induced by local surface heating and cooling. In this paper we investigate the ability of a mass-consistent wind model for downscaling near-surface wind predictions from four NWP models in complex terrain. Model predictions are compared with surface observations from a tall, isolated mountain. Downscaling improved nearsurface wind forecasts under high-wind (near-neutral atmospheric stability) conditions. Results were mixed during upslope and downslope (non-neutral atmospheric stability) flow periods, although wind direction predictions generally improved with downscaling. This work constitutes evaluation of a diagnostic wind model at unprecedented high spatial resolution in terrain with topographical ruggedness approaching that of typical landscapes in the western US susceptible to wildland fire. [ABSTRACT FROM AUTHOR]

The seasonal cycle and optical properties of mineral dust aerosols in northern Africa were simulated for the period from 2006 to 2010 using the numerical atmospheric model ALADIN (Aire Limitée Adaptation dynamique Développement InterNational) coupled to the surface scheme SURFEX (SURFace EXternalisée). The particularity of the simulations is that the major physical processes responsible for dust emission and transport, as well as radiative effects, are taken into account on short timescales and at mesoscale resolution. The aim of these simulations is to quantify the dust emission and deposition, locate the major areas of dust emission and establish a climatology of aerosol optical properties in northern Africa. The mean monthly aerosol optical thickness (AOT) simulated by ALADIN is compared with the AOTs derived from the standard Dark Target (DT) and Deep Blue (DB) algorithms of the Aqua-MODIS (MODerate resolution Imaging Spectroradiometer) products over northern Africa and with a set of sun photometer measurements located at Banizoumbou, Cinzana, Soroa,Mbour and Cape Verde. The vertical distribution of dust aerosol represented by extinction profiles is also analysed using CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) observations. The annual dust emission simulated by ALADIN over northern Africa is 878 Tg year-1. The Bodélé Depression appears to be the main area of dust emission in northern Africa, with an average estimate of about 21.6 Tg year-1. The simulated AOTs are in good agreement with satellite and sun photometer observations. The positions of the maxima of the modelled AOTs over northern Africa match the observed positions, and the ALADIN simulations satisfactorily reproduce the various dust events over the 2006-2010 period. The AOT climatology proposed in this paper provides a solid database of optical properties and consolidates the existing climatology over this region derived from satellites, the AERONET network and regional climate models. Moreover, the 3-D distribution of the simulated AOTs also provides information about the vertical structure of the dust aerosol extinction. [ABSTRACT FROM AUTHOR]

Erythemal ultraviolet (UVER) irradiation was reconstructed at nine Spanish locations, with series starting around 1950 in five of these places. Each series was checked by applying homogeneity tests in order to discard nonhomogeneous series. Available series were used to create an averaged Iberian Peninsula UVER series. Results indicate that annual UVER irradiation in the Iberian Peninsula increased by 155Jm-2 (6.5%) between 1950 and 2011 due to the decrease observed in atmospheric ozone rather than changes in aerosol and clouds. By contrast, annual UVER irradiation increased by 135 Jm-2 (5.6%) between 1985 and 2011, mainly due to changes in aerosol and clouds. [ABSTRACT FROM AUTHOR]

Stratospheric water vapor (H 2 O) is a substantial component of the global radiation budget and therefore important to variability in the climate system. Efforts to understand the distribution, transport, and sources of stratospheric water vapor have increased in recent years, with many studies utilizing long-term satellite observations. Previous work to examine stratospheric H 2 O extrema has typically focused on the stratospheric overworld (pressures ≤ 100 hPa) to ensure the observations used are truly stratospheric. However, this leads to the broad exclusion of the lowermost stratosphere, which can extend over depths of more than 5 km below the 100 hPa level in the midlatitudes and polar regions and has been shown to be the largest contributing layer to the stratospheric H 2 O feedback. Moreover, focusing on the overworld only can lead to a large underestimation of stratospheric H 2 O extrema occurrence. Therefore, we expand on previous work by examining 16 years of Microwave Limb Sounder (MLS) observations of water vapor extrema (≥ 8 ppmv) in both the stratospheric overworld and the lowermost stratosphere to create a new lower-stratosphere climatology. The resulting frequency of H 2 O extrema increases by more than 300 % globally compared to extrema frequencies within stratospheric overworld observations only, though the percentage increase varies substantially by region and season. Additional context is provided for this climatology through a backward isentropic trajectory analysis to identify potential sources of the extrema. We show that, in general, tropopause-overshooting convection presents itself as a likely source of H 2 O extrema in much of the world, while meridional isentropic transport of air from the tropical upper troposphere to the extratropical lower stratosphere is also possible. [ABSTRACT FROM AUTHOR]

The aerosol optical depth (AOD) is a derived measurement useful to investigate the aerosol load and its distribution at different spatio-temporal scales. In this work we use long-term (2000–2021) MAIAC (Multi-Angle Implementation of Atmospheric Correction) retrievals with 1 km resolution to investigate the climatological AOD variability and trends at different scales in Europe: a continental (30–60 ∘ N, 20 ∘ W–40 ∘ E), a regional (100 × 100 km 2) and an urban–local scale (3 × 3 km 2). The AOD climatology at the continental scale shows the highest values during summer (JJA) and the lowest during winter (DJF) seasons. Regional and urban–local scales are investigated for 21 cities in Europe, including capitals and large urban agglomerations. Analyses show AOD average (550 nm) values between 0.06 and 0.16 at the urban–local scale while also displaying a strong north–south gradient. This gradient corresponds to a similar one in the European background, with higher AOD being located over the Po Valley, the Mediterranean Basin and eastern Europe. Average enhancements of the local with respect to regional AOD of 57 %, 55 %, 39 % and 32 % are found for large metropolitan centers such as Barcelona, Lisbon, Paris and Athens, respectively, suggesting a non-negligible enhancement of the aerosol burden through local emissions. Negative average deviations are observed for other cities, such as Amsterdam (- 17 %) and Brussels (- 6 %), indicating higher regional background signal and suggesting a heterogeneous aerosol spatial distribution that conceals the urban–local signal. Finally, negative statistically significant AOD trends for the entire European continent are observed. A stronger decrease rate at the regional scale with respect to the local scale occurs for most of the cities under investigation. [ABSTRACT FROM AUTHOR]

The bottom part of the Earth's ionosphere is the so-called D region, which is typically less dense than the upper regions. Despite the comparably lower electron density, the ionization state of the D region has a significant influence on signal absorption for propagating lower to medium radio frequencies. We present local noon climatologies of electron densities in the upper middle atmosphere (50–90 km) at high latitudes as observed by an active radar experiment. The radar measurements cover 9 years (2014–2022) from the solar maximum of cycle 24 to the beginning of cycle 25. Reliable electron densities are derived by employing signal processing, applying interferometry methods, and applying the Faraday-International Reference Ionosphere (FIRI) model. For all years a consistent spring–fall asymmetry of the electron density pattern with a gradual increase during summer as well as a sharp decrease at the beginning of October was found. These findings are consistent with very low frequency (VLF) studies showing equivalent signatures for nearby propagation paths. It is suggested that the meridional circulation associated with downwelling in winter could cause enhanced electron densities through NO transport. However, this mechanism can not explain the reduction in electron density in early October. [ABSTRACT FROM AUTHOR]

Stratospheric ozone is important for both stratospheric and surface climate. In the lower stratosphere during winter, its variability is governed primarily by transport dynamics induced by wave–mean flow interactions. In this work, we analyze interannual co-variations between the distribution of zonal-mean ozone and the strength of the polar vortex as a measure of dynamical activity during northern hemispheric winter. Specifically, we study co-variability between the seasonal means of the ozone field from modern reanalyses and polar-cap-averaged temperature at 100 hPa, which represents a robust and well-defined index for polar vortex strength. We focus on the vertically resolved structure of the associated extratropical ozone anomalies relative to the winter climatology and shed light on the transport mechanisms that are responsible for this response pattern. In particular, regression analysis in pressure coordinates shows that anomalously weak polar vortex years are associated with three pronounced local ozone maxima just above the polar tropopause, in the lower to mid-stratosphere and near the stratopause. In contrast, in isentropic coordinates, using ERA-Interim reanalysis data, only the mid- to lower stratosphere shows increased ozone, while a small negative ozone anomaly appears in the lowermost stratosphere. These differences are related to contributions due to anomalous adiabatic vertical motion, which are implicit in potential temperature coordinates. Our analyses of the ozone budget in the extratropical middle stratosphere show that the polar ozone response maximum around 600 K and the negative anomalies around 450 K beneath both reflect the combined effects of anomalous diabatic downwelling and quasi-isentropic eddy mixing, which are associated with consecutive counteracting anomalous ozone tendencies on daily timescales. We find that approx. 71 % of the total variability in polar column ozone in the stratosphere is associated with year-by-year variations in polar vortex strength based on ERA5 reanalyses for the winter seasons 1980–2022. MLS observations for 2005–2020 show that around 86 % can be explained by these co-variations with the polar vortex. [ABSTRACT FROM AUTHOR]

Aerosol particles in Southeast Asia are challenging to characterize due to their complex life cycle within the diverse topography and weather of the region. An emerging aerosol climatology was established based on AErosol RObotic NETwork (AERONET) data (December 2009 to October 2018) for clear-sky days in Metro Manila, the Philippines. Aerosol optical depth (AOD) values were highest from August to October, partly from fine urban aerosol particles, including soot, coinciding with the burning season in insular Southeast Asia when smoke is often transported to Metro Manila during the southwest monsoon. Clustering of AERONET volume size distributions (VSDs) resulted in five aerosol particle sources based on the position and magnitude of their peaks in the VSD and the contributions of specific particle species to AOD per cluster based on MERRA-2. The clustering showed that the majority of aerosol particles above Metro Manila were from a clean marine source (58 %), which could be related to AOD values there being relatively low compared to other cities in the region. The following are the other particle sources over Metro Manila: fine polluted sources (20 %), mixed-dust sources (12 %), urban and industrial sources (5 %), and cloud processing sources (5 %). Furthermore, MERRA-2 AOD data over Southeast Asia were analyzed using empirical orthogonal functions. Along with AOD fractional compositional contributions and wind regimes, four dominant aerosol particle air masses emerged: two sulfate air masses from East Asia, an organic carbon source from Indonesia, and a sulfate source from the Philippines. Knowing the local and regional aerosol particle air masses that impact Metro Manila is useful in identifying the sources while gaining insight into how aerosol particles are affected by long-range transport and their impact on regional weather. [ABSTRACT FROM AUTHOR]

The objective of this paper is to deliver the most accurate ozone (O3) and carbon monoxide (CO) climatology for the pure troposphere only, i.e. exclusively from the ground to the dynamical tropopause on an individual profile basis. The results (profiles and columns) are derived solely from the Measurements of OZone and water vapour by in-service AIrbus airCraft programme (MOZAIC) over 15 years (1994-2009). The study, focused on the northern midlatitudes [24-50° N] and [119°W-140° E], includes more than 40 000 profiles over 11 sites to give a quasi-global zonal picture. Considering all the sites, the pure tropospheric column peak-to-peak seasonal cycle ranges are 23.7-43.2DU for O3 and 1.7-6.9×1018 moleculescm-2 for CO. The maxima of the seasonal cycles are not in phase, occurring in February-April for CO and May-July for O3. The phase shift is related to the photochemistry and OH removal efficiencies. The purely tropospheric seasonal profiles are characterized by a typical autumn-winter/spring-summer O3 dichotomy (except in Los Angeles, Eastmed - a cluster of Cairo and Tel Aviv - and the regions impacted by the summer monsoon) and a summer-autumn/winter-spring CO dichotomy. We revisit the boundary-layer, mid-tropospheric (MT) and uppertropospheric (UT) partial columns using a new monthly varying MT ceiling. Interestingly, the seasonal cycle maximum of the UT partial columns is shifted from summer to spring for O3 and to very early spring for CO. Conversely, the MT maximum is shifted from spring to summer and is associated with a summer (winter) MT thickening (thinning). Lastly, the pure tropospheric seasonal cycles derived from our analysis are consistent with the cycles derived from spaceborne measurements, the correlation coefficients being r = 0.6-0.9 for O3 and r > 0.9 for CO. The cycles observed from space are nevertheless greater than MOZAIC for O3 (by 9-18 DU) and smaller for CO (up to 1×1018 moleculescm-2). The larger winter O3 difference between the two data sets suggests probable stratospheric contamination in satellite data due to the tropopause position. The study underlines the importance of rigorously discriminating between the stratospheric and tropospheric reservoirs and avoiding use of a monthly averaged tropopause position without this strict discrimination in order to assess the pure O3 and CO tropospheric trends. [ABSTRACT FROM AUTHOR]

Aircraft at cruise levels can cause two kinds of contrails, the well known exhaust contrails and the less wellknown aerodynamic contrails. While the possible climate impact of exhaust contrails has been studied for many years, research on aerodynamic contrails began only a few years ago and nothing is known about a possible contribution of these ice clouds to climate impact. In order to make progress in this respect, we first need a climatology of their formation conditions and this is given in the present paper. Aerodynamic contrails are defined here as line shaped ice clouds caused by aerodynamically triggered cooling over the wings of an aircraft in cruise which become visible immediately at the trailing edge of the wing or close to it. Effects at low altitudes like condensation to liquid droplets and their potential heterogeneous freezing are excluded from our definition. We study atmospheric conditions that allow formation of aerodynamic contrails. These conditions are stated and then applied to atmospheric data: first to a special case where an aerodynamic contrail was actually observed and then to a full year of global reanalysis data. We show where, when (seasonal variation), and how frequently (probability) aerodynamic contrails can form, and how this relates to actual patterns of air traffic. We study the formation of persistent aerodynamic contrails as well. Furthermore, we check whether aerodynamic and exhaust contrails can coexist in the atmosphere. We show that visible aerodynamic contrails are possible only in an altitude range between roughly 540 and 250 hPa, and that the ambient temperature is the most important parameter, not the relative humidity. Finally, we argue that currently aerodynamic contrails have a much smaller climate effect than exhaust contrails, which may however change in future with more air traffic in the tropics. [ABSTRACT FROM AUTHOR]

We present a vertically resolved zonal mean monthly mean global ozone data set spanning the period 1901 to 2007, called HISTOZ.1.0. It is based on a new approach that combines information from an ensemble of chemistry climate model (CCM) simulations with historical total column ozone information. The CCM simulations incorporate important external drivers of stratospheric chemistry and dynamics (in particular solar and volcanic effects, greenhouse gases and ozone depleting substances, sea surface temperatures, and the quasi-biennial oscillation). The historical total column ozone observations include groundbased measurements from the 1920s onward and satellite observations from 1970 to 1976. An off-line data assimilation approach is used to combine model simulations, observations, and information on the observation error. The period starting in 1979 was used for validation with existing ozone data sets and therefore only ground-based measurements were assimilated. Results demonstrate considerable skill from the CCM simulations alone. Assimilating observations provides additional skill for total column ozone. With respect to the vertical ozone distribution, assimilating observations increases on average the correlation with a reference data set, but does not decrease the mean squared error. Analyses of HISTOZ.1.0 with respect to the effects of El Niño- Southern Oscillation (ENSO) and of the 11 yr solar cycle on stratospheric ozone from 1934 to 1979 qualitatively confirm previous studies that focussed on the post-1979 period. The ENSO signature exhibits a much clearer imprint of a change in strength of the Brewer-Dobson circulation compared to the post-1979 period. The imprint of the 11 yr solar cycle is slightly weaker in the earlier period. Furthermore, the total column ozone increase from the 1950s to around 1970 at northern mid-latitudes is briefly discussed. Indications for contributions of a tropospheric ozone increase, greenhouse gases, and changes in atmospheric circulation are found. Finally, the paper points at several possible future improvements of HISTOZ.1.0. [ABSTRACT FROM AUTHOR]

Abstract. This paper introduces and evaluates the second version of the global aerosol-climate model ECHAM-HAM. Major changes have been brought into the model, including new parameterizations for aerosol nucleation and water uptake, an explicit treatment of secondary organic aerosols, modified emission calculations for sea salt and mineral dust, the coupling of aerosol microphysics to a two-moment stratiform cloud microphysics scheme, and alternative wet scavenging parameterizations. These revisions extend the model's capability to represent details of the aerosol lifecycle and its interaction with climate. Nudged simulations of the year 2000 are carried out to compare the aerosol properties and global distribution in HAM1 and HAM2, and to evaluate them against various observations. Sensitivity experiments are performed to help identify the impact of each individual update in model formulation. Results indicate that from HAM1 to HAM2 there is a marked weakening of aerosol water uptake in the lower troposphere, reducing the total aerosol water burden from 75 Tg to 51 Tg. The main reason is the newly introduced κ-Köhler-theory-based water uptake scheme uses a lower value for the maximum relative humidity cutoff. Particulate organic matter loading in HAM2 is considerably higher in the upper troposphere, because the explicit treatment of secondary organic aerosols allows highly volatile oxidation products of the precursors to be vertically transported to regions of very low temperature and to form aerosols there. Sulfate, black carbon, particulate organic matter and mineral dust in HAM2 have longer lifetimes than in HAM1 because of weaker in- cloud scavenging, which is in turn related to lower autoconversion efficiency in the newly introduced two-moment cloud microphysics scheme. Modification in the sea salt emission scheme causes a significant increase in the ratio (from 1.6 to 7.7) between accumulation mode and coarse mode emission fluxes of aerosol number concentration. This leads to a general increase in the number concentration of smaller particles over the oceans in HAM2, as reflected by the higher Ångström parameters. Evaluation against observation reveals that in terms of model performance, main improvements in HAM2 include a marked decrease of the systematic negative bias in the absorption aerosol optical depth, as well as smaller biases over the oceans in Ångström parameter and in the accumulation mode number concentration. The simulated geographical distribution of aerosol optical depth (AOD) is better correlated with the MODIS data, while the surface aerosol mass concentrations are very similar to those in the old version. The total aerosol water content in HAM2 is considerably closer to the multi-model average from Phase I of the AeroCom intercomparison project. Model deficiencies that require further efforts in the future include (I) positive biases in AOD over the ocean, (ii) negative biases in AOD and aerosol mass concentration in high-latitude regions, and (iii) negative biases in particle number concentration, especially that of the Aitken mode, in the lower troposphere in heavily polluted regions. [ABSTRACT FROM AUTHOR]

The high complexity of cloud parameterizations now held in models puts more pressure on observational studies to provide useful means to evaluate them. One approach to the problem put forth in the modelling community is to evaluate under what atmospheric conditions the parameterizations fail to simulate the cloud properties and under what conditions they do a good job. It is the ambition of this paper to characterize the variability of the statistical properties of tropical ice clouds in different tropical "regimes" recently identified in the literature to aid the development of better process-oriented parameterizations in models. For this purpose, the statistical properties of non-precipitating tropical ice clouds over Darwin, Australia are characterized using ground-based radar-lidar observations from the Atmospheric Radiation Measurement (ARM) Program. The ice cloud properties analysed are the frequency of ice cloud occurrence, the morphological properties (cloud top height and thickness), and the microphysical and radiative properties (ice water content, visible extinction, effective radius, and total concentration). The variability of these tropical ice cloud properties is then studied as a function of the large-scale cloud regimes derived from the International Satellite Cloud Climatology Project (ISCCP), the amplitude and phase of the Madden-Julian Oscillation (MJO), and the large-scale atmospheric regime as derived from a long-term record of radiosonde observations over Darwin. The vertical variability of ice cloud occurrence and microphysical properties is largest in all regimes (1.5 order of magnitude for ice water content and extinction, a factor 3 in effective radius, and three orders of magnitude in concentration, typically). 98% of ice clouds in our dataset are characterized by either a small cloud fraction (smaller than 0.3) or a very large cloud fraction (larger than 0.9). In the ice part of the troposphere three distinct layers characterized by different statistically-dominant microphysical processes are identified. The variability of the ice cloud properties as a function of the large-scale atmospheric regime, cloud regime, and MJO phase is large, producing mean differences of up to a factor 8 in the frequency of ice cloud occurrence between large-scale atmospheric regimes and mean differences of a factor 2 typically in all microphysical properties. Finally, the diurnal cycle of the frequency of occurrence of ice clouds is also very different between regimes and MJO phases, with diurnal amplitudes of the vertically-integrated frequency of ice cloud occurrence ranging from as low as 0.2 (weak diurnal amplitude) to values in excess of 2.0 (very large diurnal amplitude). Modellers should now use these results to check if their model cloud parameterizations are capable of translating a given atmospheric forcing into the correct statistical ice cloud properties. [ABSTRACT FROM AUTHOR]

Deriving a parameterisation of ammonia emissions for use in chemistry-transport models (CTMs) is a complex problem as the emission varies locally as a result of local climate and local agricultural management. In current CTMs such factors are generally not taken into account. This paper demonstrates how local climate and local management can be accounted for in CTMs by applying a modular approach for deriving data as input to a dynamic ammonia emission model for Europe. Default data are obtained from information in the RAINS system, and it is demonstrated how this dynamic emission model based on these input data improves the NH3 calculations in a CTM model when the results are compared with calculations obtained by traditional methods in emission handling. It is also shown how input data can be modified over a specific target region resulting in even further improvement in performance over this domain. The model code and the obtained default values for the modelling experiments are available as supplementary information to this article for use by the modelling community on similar terms as the EMEP CTM model: the GPL licencse v3. [ABSTRACT FROM AUTHOR]

The new portable ice nucleation chamber (PINC) developed by the Institute for Atmospheric and Climate Sciences of ETH Zurich was operated during two measurement campaigns at the high alpine research station Jungfraujoch situated at 3580 m a.s.l, in March and June 2009. During this time of the year, a high probability of Saharan dust events (SDE) at the Jungfraujoch has been observed. We used an impactor with a cutoff size of 1 µm aerodynamic diameter and operated the system at -31 °C and relative humidities of 127 % and 91% with respect to ice and water, respectively. Investigation of the ambient number concentration of ice nuclei (IN) in the deposition nucleation mode and during a SDE in the free troposphere is reported. The results discussed in this paper are the first continuous IN measurements over a period of several days at the Jungfraujoch. The average IN concentration found during the campaign in March was 8 particles per liter whereas during the campaign in June, the average number concentration was higher up to 14 particles per liter. Two SDEs were detected on 15 and 16 June 2009. Our measurements show that the SDEs had IN number concentration up to several hundreds per liter. We found the best correlation between the number concentration of the larger particle fraction measured by an optical particle counter and the IN number concentration during a Saharan dust event. This correlation factor is higher for particles larger than 0.5 µm meaning that a higher concentration of larger particles induced higher IN number concentration. No correlation could be found between the black carbon mass concentration and the variations in IN number concentration. [ABSTRACT FROM AUTHOR]

In this paper, the stellar occultation instrument GOMOS is compared with ozonesondes from the SHADOZ network. We only used nighttime O3 profiles and selected 8 Southern Hemisphere stations. 7 years of GOMOS datasets (GOPR 6.0cf and IPF 5.0) and 11 years of balloon-sondes are used in this study. A monthly distribution of GOMOS O3 mixing ratios was performed in the upper-troposphere and in the stratosphere (15-50 km). A comparison with SHADOZ was made in the altitude range between 15 km and 30 km. In the 21-30 km altitude range, a satisfactory agreement was observed between GOMOS and SHADOZ, although some differences were observed depending on the station. The range for monthly differences generally decreases with increasing height and is within ±15%. It was found that the agreement between GOMOS and SHADOZ declines below ~20 km. The median differences are almost within ±5%, particularly above 23 km. But a large positive bias was found below 21 km, in comparison to SHADOZ. [ABSTRACT FROM AUTHOR]

The Global Ozone Monitoring by Occultation of Stars (GOMOS) instrument onboard the European Space Agency's ENVISAT satellite measures ozone, NO2, NO3, H2O, O2, and aerosols using the stellar occultation method. Global coverage, good vertical resolution and the self-calibrating measurement method make GOMOS observations a promising data set for building various climatologies and time series. In this paper we present GOMOS nighttime measurements of ozone, NO2, and NO3 during six years 2002-2008. Using zonal averages we show the time evolution of the vertical profiles as a function of latitude. In order to get continuous coverage in time we restrict the latitudinal region to 50° S-50° N. Time development is analysed by fitting constant, annual and semi-annual terms as well as solar and QBO proxies to the daily time series. Ozone data cover the stratosphere, mesosphere and lower thermosphere (MLT). NO2 and NO3 data cover the stratosphere. In addition to detailed analysis of profiles we derive total column distributions using the fitted time series. The time-independent constant term is determined with a good accuracy (better than 1%) for all the three gases. The median retrieval accuracy for the annual and semi-annual term varies in the range 5-20%. For ozone the annual terms dominate in the stratosphere giving early winter ozone maxima at mid-latitudes. Above the ozone layer the annual terms change the phase which results in ozone summer maximum up to 80 km. In the MLT the annual terms dominate up to 80 km where the semiannual terms start to grow. In the equatorial MLT the semi-annual terms dominate the temporal evolution whereas in the mid-latitude MLT annual and semiannual terms compete evenly. In the equatorial stratosphere the QBO dominates the time development but the solar term is too weak to be determined. In the MLT above 85 km the solar term grows significantly and ozone has 15-20% dependence on the solar cycle. For NO2 below 32 km the annual summer maxima dominates at mid-latitudes whereas in the equatorial region a strong QBO prevails. In northern mid-latitudes a strong solar term appears in the upper stratosphere. For NO3 the annual variation dominates giving rise to summer maxima. The NO3 distribution is controlled by temperature and ozone. [ABSTRACT FROM AUTHOR]

Two 3-dimensional global atmospheric transport models for persistent organic pollutants (POPs) have been employed to investigate the association between the largescale atmospheric motions and poleward transports of persistent semi-volatile organic chemicals (SVOCs). We examine the modeled daily air concentration of α- and γ- hexachlorocyclohexane (HCH) over a period from 1997 through 1999 during which a number of episodic atmospheric transport events were detected in this modeling study. These events provide modeling evidence for improving the interpretation on the cold condensation effect and poleward atmospheric transport of SVOCs in the mid-troposphere. Two episodic transport events of γ-HCH (lindane) to the high Arctic (80-90° N), one from Asian and another from Eurasian sources, are reported in this paper. Both events suggest that the episodic atmospheric transports occurring in the mid-troposphere (e.g. from 3000m to 5500m height) are driven by atmospheric horizontal and vertical motions. The association of the transport events with atmospheric circulation is briefly discussed. Strong southerly winds, forced by the evolution of two semi-permanent high pressure systems over mid-high latitudes in the Northern Hemisphere, play an important role in the long-range transport (LRT) of HCHs to the high latitudes from its sources. Being consistent with the cold condensation effect and poleward atmospheric transport in a mean meridional atmospheric circulation simulated by a 2-D atmospheric transport model, as reported by the first part of this study, this modeling study indicates that cold condensation is likely occurring more intensively in the mid-troposphere where rapid declining air temperature results in condensed phase of the chemical over and near its source regions and where stronger winds convey the chemical more rapidly to the polar region during the episodic poleward atmospheric transport events. [ABSTRACT FROM AUTHOR]

The main objective of this study is to compare the erythemal UV irradiance (UVER) and spectral UV irradiances (at 305, 310 and 324 nm) from the Ozone Monitoring Instrument (OMI) onboard NASA EOS/Aura polar sun-synchronous satellite (launched in July 2004, local equator crossing time 01:45 p.m.) with ground-based measurements from the Brewer spectrophotometer #150 located at El Arenosillo (South of Spain). The analyzed period comprises more than four years, from October 2004 to December 2008. The effects of several factors (clouds, aerosols and the solar elevation) on OMI-Brewer comparisons were analyzed. The proxies used for each factor were: OMI Lambertian Equivalent Reflectivity (LER) at 360 nm (clouds), the aerosol optical depth (AOD) at 440 nm measured from the ground-based Cimel sun-photometer (http://aeronet.gsfc.nasa.gov), and solar zenith angle (SZA) at OMI overpass time. The comparison for all sky conditions reveals positive biases (OMI higher than Brewer) 12.3% for UVER, 14.2% for UV irradiance at 305 nm, 10.6% for 310 nm and 8.7% for 324 nm. The OMI-Brewer root mean square error (RMSE) is reduced when cloudy cases are removed from the analysis, (e.g., RMSE~20% for all sky conditions and RMSE smaller than 10% for cloud-free conditions). However, the biases remain and even become more significant for the cloud-free cases with respect to all sky conditions. The mentioned overestimation is partially due to aerosol extinction influence. In addition, the differences OMI-Brewer typically decrease with SZA except days with high aerosol loading, when the bias is near constant. The seasonal dependence of the OMI-Brewer difference for cloud-free conditions is driven by aerosol climatology. To account for the aerosol effect, a first evaluation in order to compare with previous TOMS results (Antón et al., 2007) was performed. This comparison shows that the OMI bias is between +14% and +19% for UVER and spectral UV irradiances for moderately-high aerosol load (AOD>0.25). The OMI bias is decreased by a factor of 2 (the typical bias varies from +8% to +12%) under cloud-free and low aerosol load conditions (AOD<0.1). More detailed analysis of absorbing aerosols influence on OMI bias at our station is presented in a companion paper (Cachorro et al., 2010). [ABSTRACT FROM AUTHOR]

As a part of the IPY project POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate Chemistry, Aerosols and Transport), this paper studies the sources of equivalent black carbon (EBC), sulphate, light-scattering aerosols and ozone measured at the Arctic stations Zeppelin, Alert, Barrow and Summit during the years 2000-2007. These species are important pollutants and climate forcing agents, and sulphate and EBC are main components of Arctic haze. To determine where these substances originate, the measurement data were combined with calculations using FLEXPART, a Lagrangian particle dispersion model. The climatology of atmospheric transport from surrounding regions on a twenty-day time scale modelled by FLEXPART shows that the stations Zeppelin, Alert and Barrow are highly sensitive to surface emissions in the Arctic and to emissions in high-latitude Eurasia in winter. Emission sensitivities over southern Asia and southern North America are small throughout the year. The high-altitude station Summit is an order of magnitude less sensitive to surface emissions in the Arctic whereas emissions in the southern parts of the Northern Hemisphere continents are more influential relative to the other stations. Our results show that for EBC and sulphate measured at Zeppelin, Alert and Barrow, northern Eurasia is the dominant source region. For sulphate, Eastern Europe and the metal smelting industry in Norilsk are particularly important. For EBC, boreal forest fires also contribute in summer. No evidence for any substantial contribution to EBC from sources in southern Asia is found. European air masses are associated with low ozone concentrations in winter due to titration by nitric oxides, but are associated with high ozone concentrations in summer due to photochemical ozone formation. There is also a strong influence of ozone depletion events in the Arctic boundary layer on measured ozone concentrations in spring and summer. These results will be useful for developing emission reduction strategies for the Arctic. [ABSTRACT FROM AUTHOR]

This paper describes a methodology for water vapor retrieval in the mesosphere-lower thermosphere (MLT) using 6.6μm daytime broadband emissions measured by SABER, the limb scanning infrared radiometer on board the TIMED satellite. Particular attention is given to accounting for the non-local thermodynamic equilibrium (non-LTE) nature of the H2O 6.6μm emission in the MLT. The non- LTE H2O(ν2) vibrational level populations responsible for this emission depend on energy exchange processes within the H2O vibrational system as well as on interactions with vibrationally excited states of the O2, N2, and CO2 molecules. The rate coefficients of these processes are known with large uncertainties that undermines the reliability of the H2O retrieval procedure. We developed a methodology of finding the optimal set of rate coefficients using the nearly coincidental solar occultation H2O density measurements by the ACE-FTS satellite and relying on the better signal-to-noise ratio of SABER daytime 6.6μm measurements. From this comparison we derived an update to the rate coefficients of the three most important processes that affect the H2O(ν2) populations in the MLT: a) the vibrational-vibrational (V-V) exchange between the H2O and O2 molecules; b) the vibrational-translational (V-T) process of the O2(1) level quenching by collisions with atomic oxygen, and c) the V-T process of the H2O(010) level quenching by collisions with N2, O2, and O. Using the advantages of the daytime retrievals in the MLT, which are more stable and less susceptible to uncertainties of the radiance coming from below, we demonstrate that applying the updated H2O non-LTE model to the SABER daytime radiances makes the retrieved H2O vertical profiles in 50-85 km region consistent with climatological data and model predictions. The H2O retrieval uncertainties in this approach are about 10% at and below 70 km, 20% at 80 km, and 30% at 85 km altitude. [ABSTRACT FROM AUTHOR]