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Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013. (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water (up to 75 nM) and the overlying atmosphere (up to 1 ppbv) in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source (with DMS concentrations of up to 6 nM and a potential contribution to atmospheric DMS of 20 % in the study area). (2) Evidence of widespread particle nucleation and growth in the marine boundary layer was found in the CAA in the summertime, with these events observed on 41 % of days in a 2016 cruise. As well, at Alert, Nunavut, particles that are newly formed and grown under conditions of minimal anthropogenic influence during the months of July and August are estimated to contribute 20 % to 80 % of the 30–50 nm particle number density. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from seabird-colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic aerosol (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds (OVOCs) were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol–climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms, with evidence for a dominant springtime contribution from eastern and southern Asia to the middle troposphere, and a major contribution from northern Asia to the surface. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow (0.03 cm s−1).

Peak stratospheric chlorofluorocarbon (CFC) and other ozone depleting substance (ODS) concentrations were reached in the mid to late 1990s. Detection and attribution of the expected recovery of the stratospheric ozone layer in an atmosphere with reduced ODSs as well as efforts to understand the evolution of stratospheric ozone in the presence of increasing greenhouse gases are key current research topics. These require a critical examination of the ozone changes with an accurate knowledge of the spatial (geographical and vertical) and temporal ozone response. For such an examination, it is vital that the quality of the measurements used be as high as possible and measurement uncertainties well quantified. In preparation for the 2014 United Nations Environment Programme (UNEP)/World Meteorological Organization (WMO) Scientific Assessment of Ozone Depletion, the SPARC/IO3C/IGACO-O3/NDACC (SI2N) initiative was designed to study and document changes in the global ozone profile distribution. This requires assessing long-term ozone profile data sets in regards to measurement stability and uncertainty characteristics. The ultimate goal is to establish suitability for estimating long-term ozone trends to contribute to ozone recovery studies. Some of the data sets have been improved as part of this initiative with updated versions now available. This summary presents an overview of stratospheric ozone profile measurement data sets (ground- and satellite-based) available for ozone recovery studies. Here we document measurement techniques, spatial and temporal coverage, vertical resolution, native units and measurement uncertainties. In addition, the latest data versions are briefly described (including data version updates as well as detailing multiple retrievals when available for a given satellite instrument). Archive location information is for each data set is also given.

Starting in 1969 and comprising three launches a week, the Uccle (Brussels, Belgium) ozonesonde dataset is one of longest and densest in the world. Moreover, as the only major change was the switch from Brewer-Mast (BM) to electrochemical concentration cell (ECC) ozonesonde types in 1997 (when the emissions of ozone-depleting substances peaked), the Uccle time series is very homogenous. In this paper, we briefly describe the efforts that were undertaken during the first 3 decades of the 50 years of ozonesonde observations to guarantee the homogeneity between ascent and descent profiles, under changing environmental conditions (e.g. SO2), and between the different ozonesonde types. This paper focuses on the 50-year-long Uccle ozonesonde dataset and aims to demonstrate its past, present, and future relevance to ozone research in two application areas: (i) the assessment of the temporal evolution of ozone from the surface to the (middle) stratosphere, and (ii) as the backbone for validation and stability analysis of both stratospheric and tropospheric satellite ozone retrievals. Using the Long-term Ozone Trends and Uncertainties in the Stratosphere (LOTUS) multiple linear regression model (SPARC/IO3C/GAW, 2019), we found that the stratospheric ozone concentrations at Uccle have declined at a significant rate of around 2 % per decade since 1969, which is also rather consistent over the different stratospheric levels. This overall decrease can mainly be assigned to the 1969–1996 period with a rather consistent rate of decrease of around −4 % per decade. Since 2000, a recovery of between +1 % per decade and +3 % per decade of the stratospheric ozone levels above Uccle has been observed, although it is not significant and is not seen for the upper stratospheric levels measured by ozonesondes. Throughout the entire free troposphere, a very consistent increase in the ozone concentrations of 2 % per decade to 3 % per decade has been measured since both 1969 and 1995, with the trend since 1995 being in almost perfect agreement with the trends derived from the In-service Aircraft for a Global Observing System (IAGOS) ascent/descent profiles at Frankfurt. As the number of tropopause folding events in the Uccle time series has increased significantly over time, increased stratosphere-to-troposphere transport of recovering stratospheric ozone might partly explain these increasing tropospheric ozone concentrations, despite the levelling-off of (tropospheric) ozone precursor emissions and notwithstanding the continued increase in mean surface ozone concentrations. Furthermore, we illustrate the crucial role of ozonesonde measurements for the validation of satellite ozone profile retrievals. With the operational validation of the Global Ozone Monitoring Experiment-2 (GOME-2), we show how the Uccle dataset can be used to evaluate the performance of a degradation correction for the MetOp-A/GOME-2 UV (ultraviolet) sensors. In another example, we illustrate that the Microwave Limb Sounder (MLS) overpass ozone profiles in the stratosphere agree within ±5 % with the Uccle ozone profiles between 10 and 70 hPa. Another instrument on the same Aura satellite platform, the Tropospheric Emission Spectrometer (TES), is generally positively biased with respect to the Uccle ozonesondes in the troposphere by up to ∼ 10 ppbv, corresponding to relative differences of up to ∼ 15 %. Using the Uccle ozonesonde time series as a reference, we also demonstrate that the temporal stability of those last two satellite retrievals is excellent.

7 Be and 210 Pb air concentration and depositional flux data provide key information on the origins and movements of air masses, as well as atmospheric deposition processes and residence time of aerosols. After their deposition onto the Earth's surface, they are utilized for tracing soil redistribution processes on land, particle dynamics in aquatic systems, and mixing processes in open ocean. Here we present a global dataset of air concentration and depositional flux measurements of atmospheric 7 Be and 210 Pb made by a large number of global research communities. Data were collected from published papers between 1955 and early 2020. It includes the annual surface air concentration data of 7 Be from 367 sites and 210 Pb from 270 sites, the annual depositional flux data of 7 Be from 279 sites and 210 Pb from 602 sites. When available, appropriate metadata have also been summarized, including geographic location, sampling date, methodology, annual precipitation, and references. The dataset is archived at https://doi.org/10.5281/zenodo.4785136 (Zhang et al., 2021) and is freely available for the scientific community. The purpose of this paper is to provide an overview of the scope and nature of this dataset and its potential utility as baseline data for future research.

The amount of ice injected into the tropical tropopause layer has a strong radiative impact on climate. A companion paper (Part 1) used the amplitude of the diurnal cycle of ice water content (IWC) as an estimate of ice injection by deep convection, showed that the Maritime Continent (MariCont) region provides the largest injection to the upper troposphere (UT; 146 hPa) and to the tropopause level (TL; 100 hPa). This study focuses on the MariCont region and extends that approach to assess the processes, the areas and the diurnal amount and duration of ice injected over islands and over seas during the austral convective season. The model presented in the companion paper is again used to estimate the amount of ice injected (ΔIWC) by combining ice water content (IWC) measured twice a day by the Microwave Limb Sounder (MLS; Version 4.2) from 2004 to 2017 and precipitation (Prec) measurements from the Tropical Rainfall Measurement Mission (TRMM; Version 007) binned at high temporal resolution (1 h). The horizontal distribution of ΔIWC estimated from Prec (ΔIWCPrec) is presented at 2∘×2∘ horizontal resolution over the MariCont. ΔIWC is also evaluated by using the number of lightning events (Flash) from the TRMM-LIS instrument (Lightning Imaging Sensor, from 2004 to 2015 at 1 h and 0.25∘ × 0.25∘ resolution). ΔIWCPrec and ΔIWC estimated from Flash (ΔIWCFlash) are compared to ΔIWC estimated from the ERA5 reanalyses (ΔIWCERA5) with the vertical resolution degraded to that of MLS observations (ΔIWCERA5). Our study shows that the diurnal cycles of Prec and Flash are consistent with each other in phase over land but different over offshore and coastal areas of the MariCont. The observational ΔIWC range between ΔIWCPrec and ΔIWCFlash, interpreted as the uncertainty of our model in estimating the amount of ice injected, is smaller over land (where ΔIWCPrec and ΔIWCFlash agree to within 22 %) than over ocean (where differences are up to 71 %) in the UT and TL. The impact of the MLS vertical resolution on the estimation of ΔIWC is greater in the TL (difference between ΔIWCERA5 and 〈ΔIWCERA5〉 of 32 % to 139 %, depending on the study zone) than in the UT (difference of 9 % to 33 %). Considering all the methods, in the UT, estimates of ΔIWC span 4.2 to 10.0 mg m−3 over land and 0.4 to 4.4 mg m−3 over sea, and in the TL estimates of ΔIWC span 0.5 to 3.9 mg m−3 over land and 0.1 to 0.7 mg m−3 over sea. Finally, based on IWC from MLS and ERA5, Prec and Flash, this study highlights that (1) at both levels, ΔIWC estimated over land can be more than twice that estimated over sea and (2) small islands with high topography present the largest ΔIWC (e.g., island of Java).

The paper describes the dataset of concentrations and related meteorological measurements collected during the field campaign of the Bolzano Tracer Experiment (BTEX). The experiment was performed to characterize the dispersion of pollutants emitted from a waste incinerator in the basin of the city of Bolzano, in the Italian Alps. As part of the experiment, two controlled releases of a passive gas tracer (sulfur hexafluoride, SF6) were performed through the stack of the incinerator on 14 February 2017 for two different time lags, starting, respectively, at 07:00 and 12:45 LST. Samples of ambient air were collected at target sites with vacuum-filled glass bottles and polyvinyl fluoride bags, and they were later analyzed by means of a mass spectrometer (detectability limit 30 pptv). Meteorological conditions were monitored by a network of 15 surface weather stations, 1 microwave temperature profiler, 1 sodar and 1 Doppler wind lidar. The dataset represents one of the few examples available in the literature concerning dispersion processes in a typical mountain valley environment, and it provides a useful benchmark for testing atmospheric dispersion models in complex terrain. The dataset described in this paper is available at https://doi.org/10.1594/PANGAEA.898761 (Falocchi et al., 2019).

This paper presents the water vapor heavy isotope ratio measurement system developed for aircraft in-situ measurements and used in the NASA ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project. The resultant dataset collected, which includes measurements of specific humidity and the heavy isotope ratios D / H and 18O / 16O, is also presented. Aircraft sampling took place in the southeast Atlantic marine boundary layer and lower troposphere (equator to 22° S) over the months of Sept. 2016, Aug. 2017, and Oct. 2018. Isotope measurements were made using cavity ring-down spectroscopic analyzers integrated into the Water Isotope System for Precipitation and Entrainment Research (WISPER). The water concentration and isotopic data accompanied a suite of other variables including standard meteorological quantities (wind, temperature, moisture), trace gas and aerosol concentrations, radar, and lidar remote sensing. From an isotope perspective, the 300+ hours of 1 Hz in-situ data at levels in the atmosphere ranging from 70 m to 6 km represents a remarkably large and vertically resolved dataset. This paper provides a brief overview of the ORACLES mission and describes how water vapor heavy isotope ratios fit within the experimental design. Overviews of the sampling region and WISPER system setup are presented, along with calibration details, measurement uncertainties, and suggested data usage. Characteristics in the spatial variability of the study region over the three sampling periods are highlighted with latitude-altitude curtains. A number of individual tropospheric profiles are presented to illustrate the fidelity with which a series of different hydrologic processes are captured by the observations. The curtains and profiles demonstrate the dataset’s potential to provide a comprehensive perspective on moisture transport and isotopic content in this region. Readers interested in a quick reference to data usage and uncertainty estimation can consult the beginning of section 5. Data for the Sept. 2016, Aug. 2017, and Oct. 2018 sampling periods can be accessed at https://doi.org/10.5067/Suborbital/ORACLES/P3/2016_V2, https://doi.org/10.5067/Suborbital/ORACLES/P3/2017_V2, and https://doi.org/10.5067/Suborbital/ORACLES/P3/2018_V2, respectively (see references for ORACLES Science Team, 2020 – 2016 P3 data, 2017 P3 data, and 2018 P3 data).&nbsp

This paper reports spectral analyses, using Singular Spectral Analysis, of variations of the Arctic and Antarctic sea-ice extents (SI), and of the atmospheric surface pressure (AP) in both hemispheres (NH and SH). The ice-extents are dominated by a quasi-linear trend over the 42 yr period when data are available (1978–2020) and an annual component. Taken together, these two components represent more than 98 % of the signal variance. Both ice-extent series share the same 5 set of harmonics of the annual component (1/2, 1/3, 1/4 and 1/5 yr). The multi-decadal trends of sea-ice extent in the Arctic and Antarctic are of opposite sign. The series of harmonics of 1 year are consequences of the Earth’s revolution about the Sun. The components with period longer than a year form a set of even harmonics of the Schwabe cycle. The pressure series also exhibits the four harmonics of 1 year, that is not found in many series previously analysed in the same way. This could suggest a connection between variations in pressure and sea-ice extent. Geographical pressure structures (SSA trends) are stable on a 10 decadal to centennial time scale and exhibit a three-fold symmetry in the NH. In the SH that order-3 symmetry is altered by the Ross-Weddell “dipole” pressure anomaly. This anomaly is seen in maps of correlations of variations in sea-ice extent with atmospheric pressure, surface temperature and winds. It fits topographic forcing. There is phase opposition between the annual components of SI and AP in the SH, and the same decreasing phase lag from −30 to −60 days over 42 years for the four harmonic components of SHSI and SHAP. The (negative) sign of the trend of pressure and (positive) sign of the trend of temperature 15 beg for an explanation. The relative change in pressure over the past 50 years is two orders of magnitude smaller than that of warming. This relatively strong warming would be expected to have a larger effect on pressure. The ratio of relative changes of sea-ice extent vs pressure is 400 for the NH and 17 for the SH. The SSA components reported in this paper should help in understanding the mechanisms that govern changes in sea-ice extent: these changes reflect forcings related to the Earth’s revolution about the Sun on the shorter period side, and on the longer period side to the Sun and planets (Jupiter). Advanced 20 explanation of the physics underling these observations may need advances in solving the generalized Navier-Stokes equations, which is very difficult in the spherical case.

In this paper, a long-term large-scale Sahara dust transport event occurred during 14 June and 27 June 2020 is tracked with the spaceborne lidars ALADIN and CALIOP observations and the models ECMWF and HYSPLIT analysis. We evaluate the performance of the ALADIN and CALIOP on the observations of dust optical properties and wind fields and explore the capability in tracking the dust events and in calculating the dust horizontal mass fluxes with the combination of measurement data from ALADIN and CALIOP coupled with the products from ECMWF and HYSPLIT. Compared with the traditional assessments based on the data from CALIOP and models, the complement of Aeolus-produced aerosol optical properties and wind data will significantly improve the accuracy of dust horizontal flux estimations. The dust plumes are identified with AIRS/Aqua Dust Score Index and with the Vertical Feature Mask products from CALIPSO. The emission, dispersion, transport and deposition of the dust event are monitored using the data from HYSPLIT, CALIPSO and AIRS/Aqua. With the quasi-synchronization observations by ALADIN and CALIOP, combining the wind vectors and relative humidity, the dust horizontal fluxes are calculated. From this study, it is found that the dust event generated on 14 and 15 June 2020 from Sahara Desert in North Africa, and then dispersed and transported westward over the Atlantic Ocean, and finally deposited in the Atlantic Ocean, the Americas and the Caribbean Sea. During the transport and deposition processes, the dust plumes are trapped in the Northeasterly Trade-wind zone between the latitudes of 5° N and 30° N and altitudes of 0 km and 6 km (in this paper we name this space area as “Saharan dust eastward transport tunnel”). From the measurement results on 19 June 2020, influenced by the hygroscopic effect and mixing with other types aerosols, the backscatter coefficients of dust plumes are increasing along the transport routes, with 3.88 × 10−6 ± 2.59 × 10−6 m−1 sr−1 in “dust portion during emission phase”, 7.09 × 10−6 ± 3.34 × 10−6 m−1 sr−1 in “dust portion during development phase” and 7.76 × 10−6 ± 3.74 × 10−6 m−1 sr−1 in “dust portion during deposition phase”. Finally, the horizontal fluxes at different dust parts and heights on 19 June and on entire transport routine during transportation are computed. On 19 June, the dust horizontal fluxes are about 2.17 ± 1.83 mg m−2 s−1 in dust portion during emission phase, 2.72 ± 1.89 mg m−2 s−1 in dust portion during development phase and 3.01 ± 2.77 mg m−2 s−1 in dust portion during deposition phase. In the whole life-time of the dust event, the dust horizontal fluxes are about 1.30 ± 1.07 mg m−2 s−1 on 15 June 2020, 2.62 ± 1.88 mg m−2 s−1 on 16 June 2020, 2.72 ± 1.89 mg m−2 s−1 on 19 June 2020, 1.98 ± 1.41 mg m−2 s−1 on 24 June 2020 and 2.11 ± 1.74 mg m−2 s−1 on 27 June 2020. From this study, it is found that the minimum of the fluxes appears when the dust event is initially generated on 15 June. During the dust development stage, the horizontal fluxes gradually increase and reach to the maximum value on 19 June with the enhancement of the dust event. Then, the horizontal fluxes gradually decrease since most of the dust deposited in the Atlantic Ocean, the Americas and the Caribbean Sea. Combining the Chlorophyll concentrations data provided by MODIS-Aqua, the Saharan Dust is found transported across the oligotrophic regions Atlantic Ocean towards the Americas and Caribbean Sea, which are also oligotrophic regions. The mineral dust delivers micronutrients including soluble Fe and P to the deposition zones and has the potential to fertilizing the ocean and increase the primary productivity in the Atlantic Ocean and Caribbean Sea.

Beijing suffers from poor air quality particularly during wintertime haze episodes when concentrations of PM2.5 can peak at > 400 ug/m3. Black carbon (BC), an aerosol which strongly absorbs solar radiation can make up to 10 % of PM2.5 in Beijing. Black carbon is of interest due to its climatic and health impacts. Black carbon has also been found to impact planetary boundary layer (PBL) meteorology. Through interacting with radiation and altering the thermal profile of the lower atmosphere, BC can either suppress or enhance PBL development to various degrees depending on the properties and altitude of the BC layer.Previous research assessing the impact of BC on PBL meteorology has been investigated through the use of regional models which are limited both by resolution and the chosen boundary layer schemes. In this work, we apply a high resolution coupled large eddy simulation-aerosol-radiation model (UCLALES-SALSA) to quantify the impact of black carbon at different altitudes on PBL dynamics using conditions from a specific haze episode which occurred from 1st–4th Dec 2016 in Beijing. Results presented in this paper quantify the heating rate of BC at various altitudes to be between 0.01 and 0.016 K/h per μg/m3 of BC, increasing with altitude but decreasing across the PBL. Through utilising a high resolution model which explicitly calculates turbulent dynamics, this paper showcases the impact of BC on PBL dynamics both within and above the PBL. These results show that BC within the PBL increases maximum PBL height by 0.4 % but that the same loading of BC above the PBL can suppress PBL height by 6.5 %. Furthermore, when BC is present throughout the column the impact of BC suppressing PBL development is further maximised, with BC causing a 17 % decrease in maximum PBL height compared to only scattering aerosols. Combining these results in this paper, we present a mechanism through which BC may play a prominent role in the intensity and longevity of Beijing’s pollution episodes.

Aerosol particles are essential constituents of the Earth’s atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence time resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in-situ near-surface segment of the atmospheric observations system. This paper will provide the widest effort so far to document variability of climate-relevant in-situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High quality data from more than 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single scattering albedo and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information including data provision procedures, quality control and analysis, data policy and usage of the ground-based aerosol measurements network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully-characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.

TROPOMI (the TROPOspheric Monitoring Instrument), on-board the Sentinel-5 Precursor satellite, has been monitoring the Earth's atmosphere since October 2017, with an unprecedented horizontal resolution (initially 7×3.5 km2, upgraded to 5.5×3.5 km2 since August 2019). Monitoring air quality is one of the main objectives of TROPOMI, with the measurements of important pollutants such as nitrogen dioxide, carbon monoxide, and formaldehyde (HCHO). In this paper we assess the quality of the latest HCHO TROPOMI products (version 1.1.[5-7]), using ground-based solar-absorption FTIR (Fourier Transform Infrared) measurements of HCHO from twenty-five stations around the world, including high, mid, and low latitude sites. Most of these stations are part of the Network for the Detection of Atmospheric Composition Change (NDACC), and they provide a wide range of observation conditions from very clean remote sites to those with high HCHO levels from anthropogenic or biogenic emissions. The ground-based HCHO retrieval settings have been optimized and harmonized at all the stations, ensuring a consistent validation among the sites. In this validation work, we first assess the accuracy of TROPOMI HCHO tropospheric columns, using the median of the relative differences between TROPOMI and FTIR ground-based data (BIAS). We observe that, at all sites, the TROPOMI accuracy is below the upper limit of the pre-launch requirements of 80 %, and below the lower limit of 40 % for 20 of the 25 stations. The provided TROPOMI systematic uncertainties are well in agreement with the observed biases at most of the stations, except for the highest HCHO levels site where it is found to be underestimated. We find that, while the BIAS has no latitudinal dependence, it is dependent on the HCHO concentration levels: an overestimation (+26 ± 5 %) of TROPOMI is observed for very small HCHO levels ( 8.0 × 1015 molec/cm2). This demonstrates the great value of such a harmonized network covering a wide range of concentration levels, the sites with high HCHO concentrations being crucial for the determination of the satellite bias at the regions of emissions, and the clean sites allowing a small TROPOMI offset to be determined. The wide range of sampled HCHO levels within the network allows the robust determination of the significant constant and proportional TROPOMI HCHO biases (TROPOMI=+ 1.10 (± 0.05) × 1015+ 0.64 (± 0.03) × FTIR, in molec/cm2). Second, the precision of TROPOMI HCHO data is estimated by the median absolute deviation (MAD) of the relative differences between TROPOMI and FTIR ground-based data. The clean sites are especially useful to minimize a possible additional collocation error. The precision requirement of 1.2 × 1016 molec/cm2 for a single pixel is reached at most of the clean sites, where it is found that the TROPOMI precision can even be twice better (0.5–0.8 × 1015 molec/cm2 for a single pixel). However, we find that the provided TROPOMI random uncertainties may be underestimated by a factor of 1.6 (for clean sites) to 2.3 (for high HCHO levels). The correlation is very good between TROPOMI and FTIR data (R = 0.88 for 3 hours-mean coincidences; R = 0.91 for monthly means coincidences). Using about 17 months of data (from May 2018 to September 2019), we show that the TROPOMI seasonal variability is in very good agreement at all of the FTIR sites. The FTIR network demonstrates the very good quality of the TROPOMI HCHO products which is well within the pre-launch requirements for both accuracy and precision. This paper advises for a refinement of the TROPOMI random uncertainty budget and of the TROPOMI quality assurance values for a better filtering of the remaining outliers.

Atmospheric levels of reactive nitrogen have increased substantially during the last century resulting in increased nitrogen deposition to ecosystems, causing harmful effects such as soil acidification, reduction in plant biodiversity and eutrophication in lakes and the ocean. Recent developments in the use of atmospheric remote sensing enabled us to resolve concentration fields of NH3 with larger spatial coverage. These observations may be used to improve the quantification of NH3 deposition. In this paper, we use a relatively simple, data-driven method to derive dry deposition fluxes and surface concentrations of NH3 for Europe and for the Netherlands. The aim of this paper is to determine the applicability and the limitations of this method for NH3 . Space-born observations of the Infrared Atmospheric Sounding Interferometer (IASI) and the LOTOS-EUROS atmospheric transport model are used. The original modelled dry NH3 deposition flux from LOTOS-EUROS and the flux inferred from IASI are compared to indicate areas with large discrepancies between the two. In these areas, potential model or emission improvements are needed. The largest differences in derived dry deposition fluxes occur in large parts of central Europe, where the satellite-observed NH3 concentrations are higher than the modelled ones, and in Switzerland, northern Italy (Po Valley) and southern Turkey, where the modelled NH3 concentrations are higher than the satellite-observed ones. A sensitivity analysis of eight model input parameters important for NH3 dry deposition modelling showed that the IASI-derived dry NH3 deposition fluxes may vary from ∼ 20 % up to ∼50 % throughout Europe. Variations in the NH3 dry deposition velocity led to the largest deviations in the IASI-derived dry NH3 deposition flux and should be focused on in the future. A comparison of NH3 surface concentrations with in situ measurements of several established networks – the European Monitoring and Evaluation Programme (EMEP), Meetnet Ammoniak in Natuurgebieden (MAN) and Landelijk Meetnet Luchtkwaliteit (LML) – showed no significant or consistent improvement in the IASI-derived NH3 surface concentrations compared to the originally modelled NH3 surface concentrations from LOTOS-EUROS. It is concluded that the IASI-derived NH3 deposition fluxes do not show strong improvements compared to modelled NH3 deposition fluxes and there is a future need for better, more robust, methods to derive NH3 dry deposition fluxes.

The Green Ocean Amazon (GoAmazon 2014/5) campaign, conducted from January 2014 to December 2015 in the vicinity of Manaus, Brazil, was designed to study the aerosol life cycle and aerosol–cloud interactions in both pristine and anthropogenically influenced conditions. As part of this campaign, the U.S. Department of Energy (DOE) Gulfstream 1 (G-1) research aircraft was deployed from 17 February to 25 March 2014 (wet season) and 6 September to 5 October 2014 (dry season) to investigate aerosol and cloud properties aloft. Here, we present results from the G-1 deployments focusing on measurements of the aerosol chemical composition and secondary organic aerosol (SOA) formation and aging.In the first portion of the paper, we provide an overview of the data and compare and contrast the data from the wet and dry season. Organic aerosol (OA) dominates the deployment-averaged chemical composition, comprising 80 % of the non-refractory PM1 aerosol mass, with sulfate comprising 14 %, nitrate 2 %, and ammonium 4 %. This product distribution was unchanged between seasons, despite the fact that total aerosol loading was significantly higher in the dry season and that regional and local biomass burning was a significant source of OA mass in the dry, but not wet, season. However, the OA was more oxidized in the dry season, with the median of the mean carbon oxidation state increasing from −0.45 in the wet season to −0.02 in the dry season.In the second portion of the paper, we discuss the evolution of the Manaus plume, focusing on 13 March 2014, one of the exemplary days in the wet season. On this flight, we observe a clear increase in OA concentrations in the Manaus plume relative to the background. As the plume is transported downwind and ages, we observe dynamic changes in the OA. The mean carbon oxidation state of the OA increases from −0.6 to −0.45 during the 4–5 h of photochemical aging. Hydrocarbon-like organic aerosol (HOA) mass is lost, with ΔHOA∕ΔCO values decreasing from 17.6 µg m−3 ppmv−1 over Manaus to 10.6 µg m−3 ppmv−1 95 km downwind. Loss of HOA is balanced out by formation of oxygenated organic aerosol (OOA), with ΔOOA∕ΔCO increasing from 9.2 to 23.1 µg m−3 ppmv−1. Because hydrocarbon-like organic aerosol (HOA) loss is balanced by OOA formation, we observe little change in the net Δorg∕ΔCO values; Δorg∕ΔCO averages 31 µg m−3 ppmv−1 and does not increase with aging. Analysis of the Manaus plume evolution using data from two additional flights in the wet season showed similar trends in Δorg∕ΔCO to the 13 March flight; Δorg∕ΔCO values averaged 34 µg m−3 ppmv−1 and showed little change over 4–6.5 h of aging. Our observation of constant Δorg∕ΔCO are in contrast to literature studies of the outflow of several North American cities, which report significant increases in Δorg∕ΔCO for the first day of plume aging. These observations suggest that SOA formation in the Manaus plume occurs, at least in part, by a different mechanism than observed in urban outflow plumes in most other literature studies. Constant Δorg∕ΔCO with plume aging has been observed in many biomass burning plumes, but we are unaware of reports of fresh urban emissions aging in this manner. These observations show that urban pollution emitted from Manaus in the wet season forms less particulate downwind as it ages than urban pollution emitted from North American cities.

We evaluate four high-resolution model simulations of pollutant emissions, chemical transformation, and downwind transport for the Athabasca oil sands using the Global Environmental Multiscale – Modelling Air-quality and Chemistry (GEM-MACH) model, and compare model results with surface monitoring network and aircraft observations of multiple pollutants, for simulations spanning a time period corresponding to an aircraft measurement campaign in the summer of 2013. We have focussed here on the impact of different representations of the model's aerosol size distribution and plume-rise parameterization on model results. The use of a more finely resolved representation of the aerosol size distribution was found to have a significant impact on model performance, reducing the magnitude of the original surface PM2.5 negative biases 32 %, from −2.62 to −1.72 µg m−3. We compared model predictions of SO2, NO2, and speciated particulate matter concentrations from simulations employing the commonly used Briggs (1984) plume-rise algorithms to redistribute emissions from large stacks, with stack plume observations. As in our companion paper (Gordon et al., 2017), we found that Briggs algorithms based on estimates of atmospheric stability at the stack height resulted in under-predictions of plume rise, with 116 out of 176 test cases falling below the model : observation 1 : 2 line, 59 cases falling within a factor of 2 of the observed plume heights, and an average model plume height of 289 m compared to an average observed plume height of 822 m. We used a high-resolution meteorological model to confirm the presence of significant horizontal heterogeneity in the local meteorological conditions driving plume rise. Using these simulated meteorological conditions at the stack locations, we found that a layered buoyancy approach for estimating plume rise in stable to neutral atmospheres, coupled with the assumption of free rise in convectively unstable atmospheres, resulted in much better model performance relative to observations (124 out of 176 cases falling within a factor of 2 of the observed plume height, with 69 of these cases above and 55 of these cases below the 1 : 1 line and within a factor of 2 of observed values). This is in contrast to our companion paper, wherein this layered approach (driven by meteorological observations not co-located with the stacks) showed a relatively modest impact on predicted plume heights. Persistent issues with over-fumigation of plumes in the model were linked to a more rapid decrease in simulated temperature with increasing height than was observed. This in turn may have led to overestimates of near-surface diffusivity, resulting in excessive fumigation.

Atmospheric levels of reactive nitrogen have substantially increased during the last century resulting in increased nitrogen deposition to ecosystems, causing harmful effects such as soil acidification, reduction in plant biodiversity and eutrophication in lakes and the ocean. Recent developments in the use of atmospheric remote sensing enabled us to resolve concentration fields of NH3 with larger spatial coverage and these observations may be used to improve the quantification of NH3 deposition. In this paper we use a relatively simple, data-driven method to derive dry deposition fluxes and surface concentrations of NH3 for Europe and for the Netherlands. The aim of this paper is to determine for the applicability and the limitations of this method for NH3 using space-born observations of the Infrared Atmospheric Sounding Interferometer (IASI) and the LOTOS-EUROS atmospheric transport model. The original modelled dry NH3 deposition flux from LOTOS-EUROS and the flux inferred from IASI are compared to indicate areas with large discrepancies between the two and where potential model improvements are needed. The largest differences in derived dry deposition fluxes occur in large parts of Central Europe, where the satellite-observed NH3 concentrations are higher than the modelled ones, and in Switzerland, northern Italy (Po Valley) and southern Turkey, where the modelled NH3 concentrations are higher than the satellite-observed ones. A sensitivity analysis of 8 model input parameters important for NH3 dry deposition modelling showed that the IASI-derived dry NH3 deposition fluxes may vary from ~ 20 % up to ~ 50 % throughout Europe. Variations in the dry deposition velocity used for NH3 led to the largest deviations in the IASI-derived dry NH3 deposition flux and should be focused on in the future. A comparison of NH3 surface concentrations with in-situ measurements of several established networks (EMEP, MAN and LML) showed no significant, or consistent improvement in the IASI-derived NH3 surface concentrations compared to the originally modelled NH3 surface concentrations from LOTOS-EUROS. It is concluded that the IASI-derived NH3 deposition fluxes do not show strong improvements compared to modelled NH3 deposition fluxes and there is future need for better, more robust, methods to derive NH3 dry deposition fluxes.

This paper discusses impacts of cloud and precipitation processes on macrophysical properties of shallow convective clouds as simulated by a large eddy model applying warm-rain bin microphysics. Simulations with and without collision–coalescence are considered with cloud condensation nuclei (CCN) concentrations of 30, 60, 120, and 240 mg−1. Simulations with collision–coalescence include either the standard gravitational collision kernel or a novel kernel that includes enhancements due to the small-scale cloud turbulence. Simulations with droplet collisions were discussed in Wyszogrodzki et al. (2013) focusing on the impact of the turbulent collision kernel. The current paper expands that analysis and puts model results in the context of previous studies. Despite a significant increase of the drizzle/rain with the decrease of CCN concentration, enhanced by the effects of the small-scale turbulence, impacts on the macroscopic cloud field characteristics are relatively minor. Model results show a systematic shift in the cloud-top height distributions, with an increasing contribution of deeper clouds for stronger precipitating cases. We show that this is consistent with the explanation suggested in Wyszogrodzki et al. (2013); namely, the increase of drizzle/rain leads to a more efficient condensate offloading in the upper parts of the cloud field. A second effect involves suppression of the cloud droplet evaporation near cloud edges in low-CCN simulations, as documented in previous studies (e.g., Xue and Feingold, 2006). We pose the question whether the effects of cloud turbulence on drizzle/rain formation in shallow cumuli can be corroborated by remote sensing observations, for instance, from space. Although a clear signal is extracted from model results, we argue that the answer is negative due to uncertainties caused by the temporal variability of the shallow convective cloud field, sampling and spatial resolution of the satellite data, and overall accuracy of remote sensing retrievals.

Biomass burning releases trace gases and aerosol particles that significantly affect the composition and chemistry of the atmosphere. Australia contributes approximately 8% of gross global carbon emissions from biomass burning, yet there are few previous measurements of emissions from Australian forest fires available in the literature. This paper describes the results of field measurements of trace gases emitted during hazard reduction burns in Australian temperate forests using open-path Fourier transform infrared spectroscopy. In a companion paper, similar techniques are used to characterise the emissions from hazard reduction burns in the savanna regions of the Northern Territory. Details of the experimental methods are explained, including both the measurement set-up and the analysis techniques employed. The advantages and disadvantages of different ways to estimate whole-fire emission factors are discussed and a measurement uncertainty budget is developed. Emission factors for Australian temperate forest fires are measured locally for the first time for many trace gases. Where ecosystem-relevant data are required, we recommend the following emission factors for Australian temperate forest fires (in grams of gas emitted per kilogram of dry fuel burned) which are our mean measured values: 1620 ± 160 g kg−1 of carbon dioxide; 120 ± 20 g kg−1 of carbon monoxide; 3.6 ± 1.1 g kg−1 of methane; 1.3 ± 0.3 g kg−1 of ethylene; 1.7 ± 0.4 g kg−1 of formaldehyde; 2.4 ± 1.2 g kg−1 of methanol; 3.8 ± 1.3 g kg−1 of acetic acid; 0.4 ± 0.2 g kg−1 of formic acid; 1.6 ± 0.6 g kg−1 of ammonia; 0.15 ± 0.09 g kg−1 of nitrous oxide and 0.5 ± 0.2 g kg−1 of ethane.

We describe a hierarchical statistical state space model for ozone profile time series. The time series are from satellite measurements by the Stratospheric Aerosol and Gas Experiment (SAGE) II and the Global Ozone Monitoring by Occultation of Stars (GOMOS) instruments spanning the years 1984–2011. Vertical ozone profiles were linearly interpolated on an altitude grid with 1 km resolution covering 20–60 km. Monthly averages were calculated for each altitude level and 10° wide latitude bins between 60° S and 60° N. In the analysis, mean densities are studied separately for the 25–35, 35–45, and 45–55 km layers. Model variables include the ozone mean level, local trend, seasonal oscillations, and proxy variables for solar activity, the Quasi-Biennial Oscillation (QBO), and the El Niño–Southern Oscillation (ENSO). This is a companion paper to Kyrölä et al. (2013), where a piecewise linear model was used together with the same proxies as in this work (excluding ENSO). The piecewise linear trend was allowed to change at the beginning of 1997 in all latitudes and altitudes. In the modelling of the present paper such an assumption is not needed as the linear trend is allowed to change continuously at each time step. This freedom is also allowed for the seasonal oscillations whereas other regression coefficients are taken independent of time. According to our analyses, the slowly varying ozone background shows roughly three general development patterns. A continuous decay for the whole period 1984–2011 is evident in the southernmost latitude belt 50–60° S in all altitude regions and in 50–60° N in the lowest altitude region 25–35 km. A second pattern, where a recovery after an initial decay is followed by a further decay, is found at northern latitudes from the equator to 50° N in the lowest altitude region (25–35 km) and between 40° N and 60° N in the 35–45 km altitude region. Further ozone loss occurred after 2007 in these regions. Everywhere else a decay is followed by a recovery. This pattern is shown at all altitudes and latitudes in the Southern Hemisphere (10–50° S) and in the 45–55 km layer in the Northern Hemisphere (from the equator to 40° N). In the 45–55 km range the trend, measured as an average change in 10 years, has mostly turned from negative to positive before the year 2000. In those regions where the "V" type of change of the trend is appropriate, the turning point is around the years 1997–2001. To compare results for the trend changes with the companion paper, we studied the difference in trends between the years from 1984 to 1997 and from 1997 to 2011. Overall, the two methods produce very similar ozone recovery patterns with the maximum trend change of 10% in 35–45 km. The state space method (used in this paper) shows a somewhat faster recovery than the piecewise linear model. For the percent change of the ozone density per decade the difference between the results is below three percentage units.

This paper uses a method of atmospheric flow analogues to reconstruct an ensemble of atmospheric variables (namely sea-level pressure, surface temperature and wind speed) between 1781 and 1785. The properties of this ensemble are investigated and tested against observations of temperature. The goal of the paper is to assess whether the atmospheric circulation during the Laki volcanic eruption (in 1783) and the subsequent winter were similar to the conditions that prevailed in the winter 2009/2010 and during spring 2010. We find that the three months following the Laki eruption in June 1783 barely have analogues in 2010. The cold winter of 1783/1784 yields circulation analogues in 2009/2010. Our analysis suggests that it is unlikely that the Laki eruption was responsible for the cold winter of 1783/1784, of the relatively short memory of the atmospheric circulation.

Abrupt drought–flood change events caused by atmospheric circulation anomalies have occurred frequently and widely in recent years, which has caused great losses and casualties in China. In this paper, we focus on investigating whether there will be a rainfall occurrence with higher intensity after a drought period in the Huang–Huai–Hai River basin. Combined with the Chinese climate divisions and the basin's DEM (digital elevation model), the basin is divided into seven sub-regions by means of cluster analysis of the basin meteorological stations using the self-organizing map (SOM) neural network method. Based on the daily precipitation data of 171 stations for the years 1961–2011, the changes of drought times with different magnitudes are analyzed, and the number of consecutive days without precipitation is used to identify the drought magnitudes. The first precipitation intensity after a drought period is analyzed with the Pearson-III frequency curve, then the relationship between rainfall intensity and different drought magnitudes is observed, as are the changes of drought times for different years. The results of the study indicated that the occurrence times of different drought levels show an overall increasing trend; there is no clear interdecadal change shown, but the spatial difference is significant. (2) As the drought level increases, the probability of extraordinary rainstorm becomes lower, and the frequency of occurrence of spatial changes in different precipitation intensities vary. In the areas I and II, as the drought level increases, the occurrence frequency of different precipitation intensities first shows a decreasing trend, which becomes an increasing trend when extraordinary drought occurs. In the area III, IV and V, the probability of the different precipitation intensities shows an overall decreasing trend. The areas VI and VII are located at the mountains with high altitudes where the variation of different precipitation intensities with the increase in drought level is relatively complex. (3) As the drought times increase, areas I, II and V, which are located on the coastal and in the valley or basin, are vulnerable to extreme precipitation processes; areas III, IV, VI and VII are located in the inland area, where heavier precipitation is not likely to occur. (4) The local rainfall affected by multiple factors is closely related with drought occurrence. The characteristics between the first rainfall intensity after a drought period and different drought magnitudes (or drought occurrence times) are preliminarily examined in this paper, but its formation mechanism still requires further research.

NorESM is a generic name of the Norwegian earth system model. The first version is named NorESM1, and has been applied with medium spatial resolution to provide results for CMIP5 (http://cmip-pcmdi.llnl.gov/cmip5/index.html) without (NorESM1-M) and with (NorESM1-ME) interactive carbon-cycling. Together with the accompanying paper by Bentsen et al. (2012), this paper documents that the core version NorESM1-M is a valuable global climate model for research and for providing complementary results to the evaluation of possible anthropogenic climate change. NorESM1-M is based on the model CCSM4 operated at NCAR, but the ocean model is replaced by a modified version of MICOM and the atmospheric model is extended with online calculations of aerosols, their direct effect and their indirect effect on warm clouds. Model validation is presented in the companion paper (Bentsen et al., 2012). NorESM1-M is estimated to have equilibrium climate sensitivity of ca. 2.9 K and a transient climate response of ca. 1.4 K. This sensitivity is in the lower range amongst the models contributing to CMIP5. Cloud feedbacks dampen the response, and a strong AMOC reduces the heat fraction available for increasing near-surface temperatures, for evaporation and for melting ice. The future projections based on RCP scenarios yield a global surface air temperature increase of almost one standard deviation lower than a 15-model average. Summer sea-ice is projected to decrease considerably by 2100 and disappear completely for RCP8.5. The AMOC is projected to decrease by 12%, 15–17%, and 32% for the RCP2.6, 4.5, 6.0, and 8.5, respectively. Precipitation is projected to increase in the tropics, decrease in the subtropics and in southern parts of the northern extra-tropics during summer, and otherwise increase in most of the extra-tropics. Changes in the atmospheric water cycle indicate that precipitation events over continents will become more intense and dry spells more frequent. Extra-tropical storminess in the Northern Hemisphere is projected to shift northwards. There are indications of more frequent occurrence of spring and summer blocking in the Euro-Atlantic sector, while the amplitude of ENSO events weakens although they tend to appear more frequently. These indications are uncertain because of biases in the model's representation of present-day conditions. Positive phase PNA and negative phase NAO both appear less frequently under the RCP8.5 scenario, but also this result is considered uncertain. Single-forcing experiments indicate that aerosols and greenhouse gases produce similar geographical patterns of response for near-surface temperature and precipitation. These patterns tend to have opposite signs, although with important exceptions for precipitation at low latitudes. The asymmetric aerosol effects between the two hemispheres lead to a southward displacement of ITCZ. Both forcing agents, thus, tend to reduce Northern Hemispheric subtropical precipitation.

Land surface models (LSMs) are pushing towards improved realism owing to an increasing number of observations at the local scale, constantly improving satellite data-sets and the associated methodologies to best exploit such data, improved computing resources, and in response to the user community. As a part of the trend in LSM development, there have been ongoing efforts to improve the representation of the land surface processes in the Interactions between the Surface Biosphere Atmosphere (ISBA) LSM within the EXternalized SURFace (SURFEX) model platform. The Force-Restore approach in ISBA has been replaced in recent years by improved realism with respect to for example, multi-layer explicit physically-based options for sub-surface heat transfer, soil hydrological processes, and the composite snowpack. The representation of vegetation processes in SURFEX has also become much more sophisticated in recent years, including photosynthesis and respiration and biochemical processes. It become clear that the conceptual limits of the composite soil-vegetation scheme within ISBA have been reached and there is a need to explicitly separate the canopy vegetation from the soil surface. In response to this issue, a collaboration began in 2008 between the High-Resolution Limited Area Model (HIRLAM) consortium and Météo-France with the intention to develop an explicit representation of the vegetation in ISBA under the SURFEX platform. A new parameterization has been developed called the ISBA Multi-Energy Budget (MEB) in order to address these issues. ISBA-MEB consists in a fully-implicit numerical coupling between a multi-layer physically-based snowpack model, a variable-layer soil scheme, an explicit litter layer, a bulk vegetation scheme, and the atmosphere. It also includes a feature which permits a coupling transition of the snowpack from the canopy air to the free atmosphere. It shares many of the routines and physics parameterizations with the standard version of ISBA. This paper is the first of two parts: in part one, the ISBA-MEB model equations, numerical schemes and theoretical background are presented. In part two which is a separate companion paper, a local scale evaluation of the new scheme is presented along with a detailed description of the new forest litter scheme.

Mercury (Hg) is a worldwide contaminant that can cause adverse health effects to wildlife and humans. While atmospheric modeling traces the link from emissions to deposition of Hg onto environmental surfaces, large uncertainties arise from our incomplete understanding of atmospheric processes (oxidation pathways, deposition, and reemission). Atmospheric Hg reactivity is exacerbated in high latitudes and there is still much to be learned from Polar Regions in terms of atmospheric processes. This paper provides a synthesis of the atmospheric Hg monitoring data available in recent years (2011–2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. The cycle of atmospheric Hg in the Arctic and in Antarctica presents both similarities and differences. Coastal sites in the two regions are both influenced by springtime atmospheric Hg depletion events and by summertime snowpack reemission and oceanic evasion of Hg. The cycle of atmospheric Hg differs between the two regions primarily because of their different geography. While Arctic sites are significantly influenced by Northern Hemispheric Hg emissions especially in winter, coastal Antarctic sites are significantly influenced by the reactivity observed on the East Antarctic ice sheet due to katabatic winds. Based on the comparison of multi-model simulations with observations, this paper discusses whether the processes that affect atmospheric Hg seasonality and inter-annual variability are appropriately represented in the models, and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes.

Accurate representation of ozone in the extratropical upper troposphere (UT) remains a challenge. However, the implementation of hyper-spectral remote sensing using satellite instruments such as the Tropospheric Emission Spectrometer (TES) provides an avenue for mapping ozone in this region, from 500 to 300 hPa. As a polar orbiting satellite TES observations are limited, but in this paper they are combined with geostationary satellite observations of water vapor. This paper describes a validation of the Multi-sensor UT Ozone Product (MUTOP). MUTOP, based on a statistical retrieval method, is an image product derived from the multiple regression of remotely sensed TES ozone, against geostationary (GOES) specific humidity (remotely sensed) and potential vorticity (a modeled dynamical tracer in the UT). These TES-derived UT ozone mixing ratios are compared to coincident ozonesonde measurements of layer-average UT ozone mixing ratios made during the NASA INTEX/B field campaign in the spring of 2006; the region for this study is effectively the GOES west domain covering the eastern North Pacific Ocean and the western United States. This intercomparison evaluates MUTOP skill at representing ozone magnitude and variability in this region of complex dynamics. In total, 11 ozonesonde launch sites were available for this study, providing 127 individual sondes for comparison; the overall mean ozone of the 500–300 hPa layer for these sondes was 78.0 ppbv. MUTOP reproduces in~situ measurements reasonably well, producing an UT mean of 82.3 ppbv, with a mean absolute error of 12.2 ppbv and a root mean square error of 16.4 ppbv relative to ozonesondes across all sites. An overall UT mean bias of 4.3 ppbv relative to sondes was determined for MUTOP. Considered in the context of past TES validation studies, these results illustrate that MUTOP is able to maintain accuracy similar to TES while expanding coverage to the entire GOES-West satellite domain. In addition MUTOP provides six-hour temporal resolution throughout the INTEX-B study period, making the visualization of UT ozone dynamics possible. This paper presents the overall statistical validation as well as a selection of ozonesonde case studies. The case studies illustrate that error may not always represent a lack of TES-derived product skill, but often results from discrepancies driven by observations made in the presence of strong meteorological gradients.

The water vapor expedition experiment campaign was operated in the Tibetan Plateau during July and August 2014, by utilizing the Water vapor, Cloud and Aerosol Lidar (WACAL). The observation was carried out in Nagqu area (31.5° N, 92.05° E), which is 4508 m above the mean sea level. During the observation, the water vapor mixing ratio at high elevation was obtained. In this paper, the methodology of the WACAL and the retrieval method are presented in particular. The validation of water vapor mixing ratio measured during the field campaigns is completed by comparing the Lidar measurements to the radiosonde data. WACAL observations from July to August illustrate the diurnal variation of water vapor mixing ratio in the planetary boundary layer in this high elevation area. The mean water vapor mixing ratio in Nagqu in July and August is about 9.4 g kg−1 and the values vary from 6.0 to 11.7 g kg−1 near ground. The SNRs and relative errors of the data are analyzed and discussed as well in this paper. Finally, combining the vertical wind speed profiles measured by the coherent wind lidar, the vertical flux of water vapor is calculated and the upwelling and deposition of the water vapor are monitored. It is the first application, to our knowledge, to operate continuously atmospheric observation by utilizing multi-disciplinary lidar at altitude higher than 4000 m which is significant for research on the boundary dynamics and meteorology of Tibetan Plateau.

In this paper we describe the development and application of a new web based facility, UManSysProp (http://umansysprop.seaes.manchester.ac.uk), for automating predictions of molecular and atmospheric aerosol properties. Current facilities include: pure component vapour pressures, critical properties and sub-cooled densities of organic molecules; activity coefficient predictions for mixed inorganic–organic liquid systems; hygroscopic growth factors and CCN activation potential of mixed inorganic/organic aerosol particles; absorptive partitioning calculations with/without a treatment of non-ideality. The aim of this new facility is to provide a single point of reference for all properties relevant to atmospheric aerosol that have been checked for applicability to atmospheric compounds where possible. The group contribution approach allows users to upload molecular information in the form of SMILES strings and UManSysProp will automatically extract the relevant information for calculations. Built using open source chemical informatics, and hosted at the University of Manchester, the facilities are provided via a browser and device-friendly web-interface, or can be accessed using the user's own code via a JSON API. In this paper we demonstrate its use with specific examples that can be simulated using the web-browser interface.

Understanding the vertical electron density profile, which is the altitudinal variation of ionospheric electron density distribution is an important aspect for the ionospheric investigations. In this paper, the bottom-side electron density profiles derived from ground based ionosonde data and the ROCSAT-1 in-situ electron density data were used to determine the estimates of the topside electron density profiles using α-Chapman function over an equatorial station Trivandrum (8.47° N, 76.91° E) and a low latitude station Waltair (17.7° N, 83.3° E) in the Indian region. The reconstructed electron density profiles are compared with IRI (2007) model derived vertical electron density profiles which resulted in significant deviations between the two different profiles. Both the reconstructed electron density profiles and the IRI model derived profiles are integrated independently to derive the Total Electron Content (TEC) values which are compared with GPS derived TEC values. TEC values derived from the reconstructed electron density profiles give better estimates with the GPS-TEC compared to those of IRI model derived TEC values. Compared to the GPS-TEC, the IRI model is underestimating the TEC values during day-time and is overestimating during night-time at both the stations. The percentage deviations of IRI derived TEC from GPS-TEC are larger compared to those between reconstructed profile derived TEC and GPS-TEC. F2-layer peak electron density, peak height and electron density at ROCSAT altitudes (≈600 km) are used to derive the effective scale heights (HT) of the topside ionosphere during the period from July 2003 to June 2004. The diurnal and seasonal variations of HT and E×B drift velocities are presented in this paper. The diurnal variation of the effective scale height (HT) shows peak values around noon hours with higher values during day-time and lower values during night-time both at Trivandrum and Waltair. The E×B drift velocities at both the places also have shown a clear diurnal variation with a negative peak around 04:00 LT and maximum during day-time hours. The higher and lower values of HT seem to be associated with positive and negative phases of the E×B drift velocities, respectively.

Our ability to predict future climate change relies on our understanding of current and future CO2 fluxes, particularly on a regional scale (100–1000 km). CO2 regional sources and sinks are still poorly understood. Inverse transport modeling, a method often used to quantify these fluxes, relies on atmospheric CO2 measurements. One of the main challenges for the transport models used in the inversions is to properly reproduce CO2 vertical gradients between the boundary layer and the free troposphere, as these gradients impact on the partitioning of the calculated fluxes between the different model regions. Vertical CO2 profiles are very well suited to assess the performances of the models. In this paper, we conduct a comparison between observed and modeled CO2 profiles recorded during two CAATER campaigns that occurred in May 2001 and October 2002 over Western Europe, as described in a companion paper. We test different combinations between a global transport model (LMDZt), a mesoscale transport model (CHIMERE), and different sets of biospheric fluxes, all chosen with a diurnal cycle (CASA, SiB2 and ORCHIDEE). The vertical profile comparison shows that: 1) in most cases the influence of the biospheric flux is small but sometimes not negligible, ORCHIDEE giving the best results in the present study; 2) LMDZt is most of the time too diffuse, as it simulates a too high boundary layer height; 3) CHIMERE better reproduces the observed gradients between the boundary layer and the free troposphere, but is sometimes too variable and gives rise to incoherent structures. We conclude there is a need for more vertical profiles to conduct further studies to improve the parameterization of vertical transport in the models used for CO2 flux inversions. Furthermore, we use a modeling method to quantify CO2 fluxes at the regional scale from a chosen observing point, coupling influence functions from the transport model LMDZt (that works quite well at the synoptic scale) with information on the space-time distribution of fluxes. This modeling method is compared to a dual tracer method (the so-called Radon method) for a case study on 25 May 2001 during which simultaneous well-correlated in situ CO2 and Radon 222 measurements have been collected. Both methods give a similar result: a flux within the Radon 222 method uncertainty (35%), that is an atmospheric CO2 sink of −4.2 to −4.4 gC m−2 day−1. We have estimated the uncertainty of the modeling method to be at least 33% on average, and even more for specific individual events. This method allows the determination of the area that contributed to the CO2 observed concentration. In our case, the observation point located at 1700 m a.s.l. in the north of France, is influenced by an area of 1500×700 km2 that covers the Benelux region, part of Germany and western Poland. Furthermore, this method allows deconvolution between the different contributing fluxes. In this case study, the biospheric sink contributes 73% of the total flux, fossil fuel emissions for 27%, the oceanic flux being negligible. However, the uncertainties of the influence function method need to be better assessed. This could be possible by applying it to other cases where the calculated fluxes can be checked independently, for example at tall towers where simultaneous CO2 and Radon 222 measurements can be conducted. The use of optimized fluxes (from atmospheric inversions) and of mesoscale models for atmospheric transport may also significantly reduce the uncertainties.

Because the TIMED satellite orbit precesses slowly in local time, 3 degrees (12 min) per day, thus apparently covering all local times at low and mid latitudes in 2 months when ascending and descending nodes are included, there is a potential for determining migrating and non-migrating tides from temperatures. Many papers have been written on the subject, but none have taken a realistic model atmosphere with high time resolution and tested tidal analysis. The present paper contains results from a tidal analysis of a SABER-sampled global model, the Canadian Middle Atmosphere (data assimilated) Model, CMAM-DAS, which has hourly values, and compares these with analysis using the full model. Fits to 60 d intervals at the equator show reasonable agreement between full and SABER-sampled data analysis for mean, diurnal and semidiurnal tides, with or without inclusion of a linear detrend term. At 50° N where there is irregular coverage of local times, there are serious disagreements in all parameters except the background mean, and detrending has a significant effect.

Ocean tides are deemed to become a stable source of renewable energy for the future. Tidal energy has two components, the first is the potential energy due to sea level variations and the second comes from the kinetic energy of the tidal streams. This paper is concerned with the backward effect on the ocean currents by a tidal stream farm located in the open shallow sea. Recent studies in channels with 1-D models have indicated that the power potential is not given purely by the flux of kinetic energy, as has been commonly assumed. In this study, a 3-D ocean circulation model is used to estimate (i) maximum extractable energy at different levels of rated generation capacity of the farm, (ii) changes in the strength of currents due to energy extraction, and (iii) alterations in the pattern of residual currents and pathways of passive tracers. As water flow is influenced both by tidal and non-tidal currents, the model takes into account wind-driven and density-driven currents generated by meteorological forcing. Numerical modelling has been carried out for a hypothetical circular farm located in the Celtic Sea north of Cornwall, an area known for its high level of tidal energy. Modelling results clearly indicate that extracted power does not grow linearly with the increase in the rated capacity of the farm. For the case studies covered in this paper, a 100-fold increase in rated generation capacity of the farm results only in 7-fold increase in extracted power, this loss of efficiency is much greater than was estimated earlier with 1-D models. In case of high rated capacity of the farm, kinetic energy of currents is altered significantly as far as 10–20 km away from the farm. At high levels of extracted energy the currents tend to avoid flowing through the farm, an effect which is not captured with 1-D models. Residual currents are altered as far as a hundred kilometres. The magnitude of changes in the dispersion of tracers is highly sensitive to the location. For the drifters analysed in this study, variations in the end-to-start distance due to energy extraction range from 13% to 238%.

This article describes the Integrated Forecasting System aerosol scheme (IFS-AER) used operationally in the IFS cycle 47R1, which was operated by the European Centre for Medium Range Weather Forecasts (ECMWF) in the framework of the Copernicus Atmospheric Monitoring Services (CAMS). It represents an update of the Rémy et al. (2019) article, which described cycle 45R1 of IFS-AER in detail. Here, we detail only the parameterisations of sources and sinks that have been updated since cycle 45R1, as well as recent changes in the configuration used operationally within CAMS. Compared to cycle 45R1, a greater integration of aerosol and chemistry has been achieved. Primary aerosol sources have been updated, with the implementation of new dust and sea salt aerosol emission schemes. New dry and wet deposition parameterisations have also been implemented. Sulfate production rates are now provided by the global chemistry component of IFS. This paper aims to describe most of the updates that have been implemented since cycle 45R1, not just the ones that are used operationally in cycle 47R1; components that are not used operationally will be clearly flagged. Cycle 47R1 of IFS-AER has been evaluated against a wide range of surface and total column observations. The final simulated products, such as particulate matter (PM) and aerosol optical depth (AOD), generally show a significant improvement in skill scores compared to results obtained with cycle 45R1. Similarly, the simulated surface concentration of sulfate, organic matter and sea salt aerosol are improved by cycle 47R1 compared to cycle 45R1. Some biases persist, such as the surface concentrations of nitrate and organic matter being simulated too high. The new wet and dry deposition schemes that have been implemented into cycle 47R1 have a mostly positive impact on simulated AOD, PM and speciated aerosol surface concentration.

This paper documents the chemical composition of 7 rain events associated with mesoscale convective systems sampled at the supersite of Banizoumbou, Niger, during the first special observation periods (June–July 2006) of the African Monsoon Multidisciplinary Analyses (AMMA) experiment. Time-resolved rain sampling was performed in order to discriminate the local dust scavenged at the beginning of rain event from the aerosol particles incorporated in the cloud at the end of the rain. The total elemental composition is dominated by Al, Si, Fe and Ca, indicating a high influence of dust and limited marine or anthropogenic contribution. After the aerosol wash-out, the elemental concentrations normalized to Al and the microscopic observations of diatoms, a tracer of the Bodélé depression, both indicate that the total elemental composition of rainwater is controlled by dust originating from North-eastern Saharan sources and probably incorporated in the convective cloud from the Harmattan layer. The low variability of the rain composition over the measurement period indicates a regional and temporal homogeneity of dust composition in the Harmattan layer. In the dissolved phase, the dominant anions are nitrate (NO3−), sulphate (SO42−) and chloride (Cl−). However, between June and July we observe an increasing contribution of the organic anions (formate, acetate, oxalate) associated with biogenic emissions to the total ion composition. These results confirm the large influence of biogenic emissions on the rain composition over Sahel during the wet season. The paper concludes on the capacity of mesoscale convective systems to carry simultaneously dust and biogenic compounds originating from different locations and depose them jointly. It also discusses the potential biogeochemical impact of such a phenomenon.

This paper presents a comprehensive characterization of a very deep stratospheric intrusion which occurred over the British Isles on 15 August 2007. The signature of this event is diagnosed using ozonesonde measurements over Lerwick, UK (60.14 N, 1.19 W) and is also well characterized using meteorological analyses from the global operational weather prediction model of Meteo-France, ARPEGE. Modelled as well as assimilated fields of both ozone (O3) and carbon monoxide (CO) have been used in order to better document this event. O3 and CO from Aura/MLS and Terra/MOPITT instruments, respectively, are assimilated into the three-dimensional chemical transport model MOCAGE of Meteo-France using a variational 3-DFGAT (First Guess at Appropriate Time) method. The validation of O3 and CO assimilated fields is done using selfconsistency diagnostics and by comparison with independent observations such as MOZAIC (O3 and CO), AIRS (CO) and OMI (O3). It particularly shows in the upper troposphere and lower stratosphere region that the assimilated fields are closer to MOZAIC than the free model run. The O3 bias between MOZAIC and the analyses is −11.5 ppbv with a RMS of 22.4 ppbv and a correlation coefficient of 0.93, whereas between MOZAIC and the free model run, the corresponding values are 33 ppbv, 38.5 ppbv and 0.83, respectively. In the same way, for CO, the bias, RMS and correlation coefficient between MOZAIC and the analyses are −3.16 ppbv, 13 ppbv and 0.79, respectively, whereas between MOZAIC and the free model run, the corresponding values are 33 ppbv, 38.5 ppbv and 0.83, respectively. In the same way, for CO, the bias, RMS and correlation coefficient between MOZAIC and the analyses are −3.16 ppbv, 13 ppbv and 0.79, respectively, whereas between MOZAIC and the free model they are 6.3 ppbv, 16.6 ppbv and 0.71, respectively. The paper also presents a demonstration of the capability of O3 and CO assimilated fields to better describe a stratosphere-troposphere exchange (STE) event in comparison with the free run modelled O3 and CO fields. Although the assimilation of MLS data improves the distribution of O3 above the tropopause compared to the free model run, it is not sufficient to reproduce the STE event well. Assimilated MOPITT CO allows a better qualitative description of the stratospheric intrusion event. The MOPITT CO analyses appear more promising than the MLS O3 analyses in terms of their ability to capture a deep STE event. Therefore, the results of this study open the perspectives for using MOPITT CO in the STE studies.

Recent results from diverse air, ground, and laboratory studies using both radiometric and in situ techniques show that the fractions of black carbon, organic matter, and mineral dust in atmospheric aerosols determine the wavelength dependence of absorption (often expressed as Absorption Angstrom Exponent, or AAE). Taken together, these results hold promise of improving information on aerosol composition from remote measurements. The main purpose of this paper is to show that AAE values for an Aerosol Robotic Network (AERONET) set of retrievals from Sun-sky measurements describing full aerosol vertical columns are also strongly correlated with aerosol composition or type. In particular, we find AAE values near 1 (the theoretical value for black carbon) for AERONET-measured aerosol columns dominated by urban-industrial aerosol, larger AAE values for biomass burning aerosols, and the largest AAE values for Sahara dust aerosols. These AERONET results are consistent with results from other, very different, techniques, including solar flux-aerosol optical depth (AOD) analyses and airborne in situ analyses examined in this paper, as well as many other previous results. Ambiguities in aerosol composition or mixtures thereof, resulting from intermediate AAE values, can be reduced via cluster analyses that supplement AAE with other variables, for example Extinction Angstrom Exponent (EAE), which is an indicator of particle size. Together with previous results, these results strengthen prospects for determining aerosol composition from space, for example using the Glory Aerosol Polarimetry Sensor (APS), which seeks to provide retrievals of multiwavelength single-scattering albedo (SSA) and aerosol optical depth (and therefore aerosol absorption optical depth (AAOD) and AAE), as well as shape and other aerosol properties. Multidimensional cluster analyses promise additional information content, for example by using the Ozone Monitoring Instrument (OMI) to add AAOD in the near ultraviolet and CALIPSO aerosol layer heights to reduce height-absorption ambiguity.

In this paper we analyze distributions of water vapour isotopologues in the troposphere using infrared spectra recorded by the Infrared Atmospheric Sounding Interferometer (IASI), which operates onboard the Metop satellite in nadir geometry. The simultaneous uncorrelated retrievals of H 2 16 O and HDO are performed on radiance measurements using a line-by-line radiative transfer model and an inversion procedure based on the Optimal Estimation Method (OEM). The characterizations of the retrieved products in terms of vertical sensitivity and error budgets show that IASI measurements contain up to 6 independent pieces of information on the vertical distribution of H 2 16 O and up to 3.5 for HDO from the surface up to the upper troposphere (0–20 km). Although the purpose of the paper is not validation, a restricted comparison with sonde measurements shows that the retrieved H 2 16 O profiles capture the seasonal/latitudinal variations of the water content, with good accuracy in the lowest layer but with larger uncertainties higher in the free and upper troposphere. Our results then demonstrate the ability of the IASI instrument to monitor atmospheric isotopologic water vapour distributions and to provide information on the partitioning of HDO as compared to H 2 16 O. The derivation of the δ D is challenging and associated with large errors in the uncorrelated retrieval approach chosen here. As a result averaging on the vertical to produce a column-averaged δ D is required to produce meaningful results for geophysical interpretation. As a case study, we analyse concentration distributions and spatio-temporal variations of H 2 16 O and δ D during the October 2007 Krosa super-typhoon over South-East Asia. We show that individual δ D have uncertainties of 37‰ for the vertically averaged values. Using the latter, we suggest that the typhoon produces a so-called amount-effect, where the δ D is negatively correlated to the water amounts as a result of intense depletion of the deuterated species.

Version-4 of the Goddard Earth Observing System (GEOS-4) General Circulation Model (GCM) was employed to assess the influence of potential changes in aerosols on the regional circulation, ambient temperatures, and precipitation in four selected regions: India and Africa (current paper), as well as North and South America (companion paper). Ensemble-simulations were carried out with the GCM to assess the aerosol direct and indirect effects, hereafter ADE and AIE. Each simulation was started from the NCEP-analyzed initial conditions for 1 May and was integrated through May-June-July-August of each year: 1982–1987 to provide an ensemble set of six simulations. In the first set, called experiment (#1), climatological aerosols were prescribed. The next two experiments (#2 and #3) had two sets of simulations each: one with 2X and other with 1/2X the climatological aerosols over each of the four selected regions. In experiment #2, the anomaly regions were advectively restricted (AR), i.e., the large-scale prognostic fields outside the aerosol anomaly regions were prescribed while in experiment #3, the anomaly regions were advectively Interactive (AI) as is the case in a normal GCM integrations, but with the same aerosols anomalies as in experiment #2. Intercomparisons of circulation, diabatic heating, and precipitation difference fields showed large disparities among the AR and AI simulations, which raised serious questions about the proverbial AR assumption, commonly invoked in regional climate simulation studies. Consequently AI simulation mode was chosen for the subsequent studies. Two more experiments (#4 and #5) were performed in the AI mode in which ADE and AIE were activated one at a time. The results showed that ADE and AIE work in concert to make the joint influences larger than sum of each acting alone. Moreover, the ADE and AIE influences were vastly different for the Indian and Africa regions, which suggest an imperative need to include them rationally in climate models. We also found that the aerosol induced increase of tropical cirrus clouds would potentially offset any cirrus thinning that may occur due to warming in response to CO2 increase.

Field research campaigns in 2019 and 2020 collected hourly atmospheric profiles via radiosonde surrounding the 2 July 2019 and 14 December 2020 total solar eclipses over South America from locations within the paths of eclipse totality. As part of these atmospheric data collection campaigns, the eclipse module of the Advanced Research Weather Research & Forecast (WRF-ARW) model was utilized to model meteorological conditions before, during, and after the eclipse events. The surface and upper air measurements collected through these campaigns have enabled further assessment and validation of the WRF-ARW eclipse module’s performance in simulating atmospheric responses to total solar eclipses. We provide here descriptions of both field campaigns and present results from comparisons of meteorological variables both at the surface and aloft using observational datasets obtained through the campaigns. The paper concludes by recommending further scientific analyses to be explored utilizing the unique datasets presented.

Chemical and meteorological parameters measured on board the Facility for Airborne Atmospheric Measurements (FAAM) BAe 146 Atmospheric Research Aircraft during the African Monsoon Multidisciplinary Analysis (AMMA) campaign are presented to show the impact of NOx emissions from recently wetted soils in West Africa. NO emissions from soils have been previously observed in many geographical areas with different types of soil/vegetation cover during small scale studies and have been inferred at large scales from satellite measurements of NOx. This study is the first dedicated to showing the emissions of NOx at an intermediate scale between local surface sites and continental satellite measurements. The measurements reveal pronounced mesoscale variations in NOx concentrations closely linked to spatial patterns of antecedent rainfall. Fluxes required to maintain the NOx concentrations observed by the BAe-146 in a number of cases studies and for a range of assumed OH concentrations (1×106 to 1×107 molecules cm−3) are calculated to be in the range 8.4 to 36.1 ng N m−2 s−1. These values are comparable to the range of fluxes from 0.5 to 28 ng N m−2 s−1 reported from small scale field studies in a variety of non-nutrient rich tropical and sub-tropical locations reported in the review of Davidson and Kingerlee (1997). The fluxes calculated in the present study have been scaled up to cover the area of the Sahel bounded by 10 to 20 N and 10 E to 20 W giving an estimated emission of 0.03 to 0.30 Tg N from this area for July and August 2006. The observed chemical data also suggest that the NOx emitted from soils is taking part in ozone formation as ozone concentrations exhibit similar fine scale structure to the NOx, with enhancements over the wet soils. Such variability can not be explained on the basis of transport from other areas. Delon et al. (2008) is a companion paper to this one which models the impact of soil NOx emissions on the NOx and ozone concentration over West Africa during AMMA. It employs an artificial neural network to define the emissions of NOx from soils, integrated into a coupled chemistry-dynamics model. The results are compared to the observed data presented in this paper. Here we compare fluxes deduced from the observed data with the model-derived values from Delon et al. (2008).

As part of a series of papers on the sources, distribution and potential impact of biological particles in the atmosphere, this paper introduces and summarizes the potential role of biological particles in atmospheric clouds. Biological particles like bacteria or pollen may be active as both cloud condensation nuclei (CCN) and heterogeneous ice nuclei (IN) and thereby can contribute to the initial cloud formation stages and the development of precipitation through giant CCN and IN processes. The paper gives an introduction to aerosol-cloud processes like CCN and IN in general and provides a short summary of previous laboratory, field and modelling work investigating the CCN and IN activity of bacterial cells and pollen. Recent measurements of atmospheric ice nuclei with a continuous flow diffusion chamber (CFDC) and of the heterogeneous ice nucleation efficiency of bacterial cells are also briefly discussed. As a main result of this overview paper we conclude that a proper assessment of the impact of biological particles on tropospheric clouds needs new laboratory, field and modelling work investigating the abundance of biological particles in the atmosphere and their CCN and heterogeneous IN properties.

In spring 2006, the European Arctic was abnormally warm, setting new historical temperature records. During this warm period, smoke from agricultural fires in Eastern Europe intruded into the European Arctic and caused the most severe air pollution episodes ever recorded there. This paper confirms that biomass burning (BB) was indeed the source of the observed air pollution, studies the transport of the smoke into the Arctic, and presents an overview of the observations taken during the episode. Fire detections from the MODIS instruments aboard the Aqua and Terra satellites were used to estimate the BB emissions. The FLEXPART particle dispersion model was used to show that the smoke was transported to Spitsbergen and Iceland, which was confirmed by MODIS retrievals of the aerosol optical depth (AOD) and AIRS retrievals of carbon monoxide (CO) total columns. Concentrations of halocarbons, carbon dioxide and CO, as well as levoglucosan and potassium, measured at Zeppelin mountain near Ny Ålesund, were used to further corroborate the BB source of the smoke at Spitsbergen. The ozone (O3) and CO concentrations were the highest ever observed at the Zeppelin station, and gaseous elemental mercury was also elevated. A new O3 record was also set at a station on Iceland. The smoke was strongly absorbing – black carbon concentrations were the highest ever recorded at Zeppelin – and strongly perturbed the radiation transmission in the atmosphere: aerosol optical depths were the highest ever measured at Ny Ålesund. We furthermore discuss the aerosol chemical composition, obtained from filter samples, as well as the aerosol size distribution during the smoke event. Photographs show that the snow at a glacier on Spitsbergen became discolored during the episode and, thus, the snow albedo was reduced. Samples of this polluted snow contained strongly elevated levels of potassium, sulphate, nitrate and ammonium ions, thus relating the discoloration to the deposition of the smoke aerosols. This paper shows that, to date, BB has been underestimated as a source of aerosol and air pollution for the Arctic, relative to emissions from fossil fuel combustion. Given its significant impact on air quality over large spatial scales and on radiative processes, the practice of agricultural waste burning should be banned in the future.

Within the framework of the Network for Detection of Atmospheric Composition Change (NDACC), regular ground-based Fourier transform infrared (FTIR) measurements of many species are performed at several locations. Inversion schemes provide vertical profile information and characterization of the retrieved products which are therefore relevant for contributing to the validation of MIPAS profiles in the stratosphere and upper troposphere. We have focused on the species HNO3 and N2O at 5 NDACC-sites distributed in both hemispheres, i.e., Jungfraujoch (46.5° N) and Kiruna (68° N) for the northern hemisphere, and Wollongong (34° S), Lauder (45° S) and Arrival Heights (78° S) for the southern hemisphere. These ground-based data have been compared with MIPAS offline profiles (v4.61) for the year 2003, collocated within 1000 km around the stations, in the lower to middle stratosphere. To get around the spatial collocation problem, comparisons have also been made between the same ground-based FTIR data and the corresponding profiles resulting from the stratospheric 4D-VAR data assimilation system BASCOE constrained by MIPAS data. This paper discusses the results of the comparisons and the usefullness of using BASCOE profiles as proxies for MIPAS data. It shows good agreement between MIPAS and FTIR N2O partial columns: the biases are below 5% for all the stations and the standard deviations are below 7% for the three mid-latitude stations, and below 10% for the high latitude ones. The comparisons with BASCOE partial columns give standard deviations below 4% for the mid-latitude stations to less than 8% for the high latitude ones. After making some corrections to take into account the known bias due to the use of different spectroscopic parameters, the comparisons of HNO3 partial columns show biases below 3% and standard deviations below 15% for all the stations except Arrival Heights (bias of 5%, standard deviation of 21%). The results for this species, which has a larger spatial variability, highlight the necessity of defining appropriate collocation criteria and of accounting for the spread of the observed airmasses. BASCOE appears to have more deficiencies in producing proxies of MIPAS HNO3 profiles compared to N2O, but the obtained standard deviation of less than 10% between BASCOE and FTIR is reasonable. Similar results on profiles comparisons are also shown in the paper, in addition to partial column ones.

The estimation of CO2 exchange between the ocean and the atmosphere is essential to understand the global carbon cycle. The eddy-covariance technique offers a very direct approach to observe these fluxes. The turbulent CO2 flux is measured, as well as the sensible and latent heat flux and the momentum flux, a few meters above the ocean in the atmosphere. Assuming a constant-flux layer in the near-surface part of the atmospheric boundary layer, this flux equals the exchange flux between ocean and atmosphere. The purpose of this paper is the comparison of long-term flux measurements at two different heights above the Baltic Sea to investigate this assumption. The results are based on a 1.5-year record of quality-controlled eddy-covariance measurements. Concerning the flux of momentum and of sensible and latent heat, the constant-flux layer theory can be confirmed because flux differences between the two heights are insignificantly small more than 95 % of the time. In contrast, significant differences, which are larger than the measurement error, occur in the CO2 flux about 35 % of the time. Data used for this paper are published at http://doi.pangaea.de/10.1594/PANGAEA.808714.

A high-order modelling approach to interpret "continental-type" particle formation bursts in the anthropogenically influenced convective boundary layer (CBL) is proposed. The model considers third-order closure for planetary boundary layer turbulence, sulphur and ammonia chemistry as well as aerosol dynamics. In Paper I of four papers, previous observations of ultrafine particle evolution are reviewed, model equations are derived, the model setup for a conceptual study on binary and ternary homogeneous nucleation is defined and shortcomings of process parameterisation are discussed. In the subsequent Papers II, III and IV simulation results, obtained within the framework of a conceptual study on the CBL evolution and new particle formation (NPF), will be presented and compared with observational findings.

A significant gap now of some 16 years in length has been shown to exist between the observed global surface temperature trend and that expected from the majority of climate simulations, and this gap is presently continuing to increase. For its own sake, and to enable better climate prediction for policy use, the reasons behind this mismatch need to be better understood. While an increasing number of possible causes have been proposed, the candidate causes have not yet converged. The standard model which is now displaying the disparity has it that temperature will rise roughly linearly with atmospheric CO2. However research also exists showing correlation between the interannual variability in the growth rate of atmospheric CO2 and temperature. Rate of change of CO2 had not been a causative mechanism for temperature because it was concluded that causality ran from temperature to rate of change of CO2. However more recent studies have found little or no evidence for temperature leading rate of change of CO2 but instead evidence for simultaneity. With this background, this paper reinvestigated the relationship between rate of change of CO2 and two of the major climate variables, atmospheric temperature and the El Niño–Southern Oscillation (ENSO). Using time series analysis in the form of dynamic regression modelling with autocorrelation correction, it is demonstrated that first-derivative CO2 leads temperature and that there is a highly statistically significant correlation between first-derivative CO2 and temperature. Further, a correlation is found for second-derivative CO2, with the Southern Oscillation Index, the atmospheric-pressure component of ENSO. This paper also demonstrates that both these correlations display Granger causality. It is shown that the first-derivative CO2 and climate model shows no trend mismatch in recent years. These results may contribute to the prediction of future trends for global temperature and ENSO. Interannual variability in the growth rate of atmospheric CO2 is standardly attributed to variability in the carbon sink capacity of the terrestrial biosphere. The terrestrial biosphere carbon sink is created by photosynthesis: a major way of measuring global terrestrial photosynthesis is by means of satellite measurements of vegetation reflectance, such as the Normalized Difference Vegetation Index (NDVI). This study finds a~close correlation between an increasing NDVI and the increasing climate model/temperature mismatch (as quantified by the difference between the trend in the level of CO2 and the trend in temperature).

Scintillometry, a form of ground-based remote sensing, provides the capability to estimate surface heat fluxes over scales of a few hundred metres to kilometres. Measurements are spatial averages, making this technique particularly valuable over areas with moderate heterogeneity such as mixed agricultural or urban environments. In this study, we present the structure parameters of temperature and humidity, which can be related to the sensible and latent heat fluxes through similarity theory, for a suburban area in the UK. The fluxes are provided in the second paper of this two-part series. A unique millimetre-wave scintillometer was combined with an infrared scintillometer along a 5.5 km path over northern Swindon. The pairing of these two wavelengths offers sensitivity to both temperature and humidity fluctuations and the so-called "bichromatic-correlation" method is also used to retrieve the path-averaged temperature-humidity correlation. Comparison is made with structure parameters calculated from an eddy covariance station located close to the centre of the scintillometer path. The performance of the techniques under different conditions is discussed. Similar behaviour is seen between the two datasets at sub-daily timescales. For the two summer-to-winter periods presented here, similar evolution is displayed across the seasons. A higher vegetation fraction within the scintillometer source area is consistent with the lower Bowen ratio observed (midday Bowen ratio < 1) compared with more built-up areas around the eddy covariance station. The energy partitioning is further explored in the copanion paper.

A millimetre-wave scintillometer was paired with an infrared scintillometer, enabling estimation of large-area evapotranspiration across northern Swindon, a suburban area in the UK. Both sensible and latent heat fluxes can be obtained using this "two-wavelength" technique, as it is able to provide both temperature and humidity structure parameters, offering a major advantage over conventional single-wavelength scintillometry. The first paper of this two-part series presented the measurement theory and structure parameters. In this second paper, heat fluxes are obtained and analysed. These fluxes, estimated using two-wavelength scintillometry over an urban area, are the first of their kind. Source area modelling suggests the scintillometric fluxes are representative of 5–10 km2. For comparison, local-scale (0.05–0.5 km2) fluxes were measured by an eddy covariance station. Similar responses to seasonal changes are evident at the different scales but the energy partitioning varies between source areas. The response to moisture availability is explored using data from 2 consecutive years with contrasting rainfall patterns (2011–2012). This extensive data set offers insight into urban surface-atmosphere interactions and demonstrates the potential for two-wavelength scintillometry to deliver fluxes over mixed land cover, typically representative of an area 1–2 orders of magnitude greater than for eddy covariance measurements. Fluxes at this scale are extremely valuable for hydro-meteorological model evaluation and assessment of satellite data products.