ALBERT

Description: We validate the Ozone Monitoring Instrument (OMI) Ozone Profile (PROFOZ) product from October 2004 through December 2014 retrieved by the Smithsonian Astrophysical Observatory (SAO) algorithm against ozonesonde observations. We also evaluate the effects of OMI row anomaly (RA) on the retrieval by dividing the dataset into before and after the occurrence of serious OMI RA, i.e., pre-RA (2004–2008) and post-RA (2009–2014). The retrieval shows good agreement with ozonesondes in the tropics and midlatitudes and for pressure  

Description: The algorithm presented in this paper was developed to retrieve ice water content (IWC) profiles in cirrus clouds. It is based on optimal estimation theory and combines ground-based visible lidar and thermal infrared (TIR) radiometer measurements in a common retrieval framework in order to retrieve profiles of IWC together with a correction factor for the backscatter intensity of cirrus cloud particles. As a first step, we introduce a method to retrieve extinction and IWC profiles in cirrus clouds from the lidar measurements alone and demonstrate the shortcomings of this approach due to the backscatter-to-extinction ambiguity. As a second step, we show that TIR radiances constrain the backscattering of the ice crystals at the visible lidar wavelength by constraining the ice water path (IWP) and hence the IWC, which is linked to the optical properties of the ice crystals via a realistic bulk ice microphysical model. The scattering phase function obtained from the microphysical model is flat around the backscatter direction (i.e., there is no backscatter peak). We show that using this flat backscattering phase function to define the backscatter-to-extinction ratio of the ice crystals in the retrievals with the lidar-only algorithm results in an overestimation of the IWC, which is inconsistent with the TIR radiometer measurements. Hence, a synergy algorithm was developed that combines the attenuated backscatter profiles measured by the lidar and the measurements of TIR radiances in a common optimal estimation framework to retrieve the IWC profile together with a correction factor for the phase function of the bulk ice crystals in the backscattering direction. We show that this approach yields consistent lidar and TIR results. The resulting lidar ratios for cirrus clouds are found to be consistent with previous independent studies.

Description: A network of three tall tower measurement stations was set up in 2012 across the United Kingdom to expand measurements made at the long-term background northern hemispheric site, Mace Head, Ireland. Reliable and precise in situ greenhouse gas (GHG) analysis systems were developed and deployed at three sites in the UK with automated instrumentation measuring a suite of GHGs. The UK Deriving Emissions linked to Climate Change (UK DECC) network uses tall (165–230 m) open-lattice telecommunications towers, which provide a convenient platform for boundary layer trace gas sampling. In this paper we describe the automated measurement system and first results from the UK DECC network for CO2, CH4, N2O, SF6, CO and H2. CO2 and CH4 are measured at all of the UK DECC sites by cavity ring-down spectroscopy (CRDS) with multiple inlet heights at two of the three tall tower sites to assess for boundary layer stratification. The short-term precisions (1σ on 1 min means) of CRDS measurements at background mole fractions for January 2012 to September 2015 is

Description: Aerosol–cloud interactions (ACI) constitute the single largest uncertainty in anthropogenic radiative forcing. To reduce the uncertainties and gain more confidence in the simulation of ACI, models need to be evaluated against observations, in particular against measurements of cloud condensation nuclei (CCN). Here we present a data set – ready to be used for model validation – of long-term observations of CCN number concentrations, particle number size distributions and chemical composition from 12 sites on 3 continents. Studied environments include coastal background, rural background, alpine sites, remote forests and an urban surrounding. Expectedly, CCN characteristics are highly variable across site categories. However, they also vary within them, most strongly in the coastal background group, where CCN number concentrations can vary by up to a factor of 30 within one season. In terms of particle activation behaviour, most continental stations exhibit very similar activation ratios (relative to particles 〉 20 nm) across the range of 0.1 to 1.0 % supersaturation. At the coastal sites the transition from particles being CCN inactive to becoming CCN active occurs over a wider range of the supersaturation spectrum. Several stations show strong seasonal cycles of CCN number concentrations and particle number size distributions, e.g. at Barrow (Arctic haze in spring), at the alpine stations (stronger influence of polluted boundary layer air masses in summer), the rain forest (wet and dry season) or Finokalia (wildfire influence in autumn). The rural background and urban sites exhibit relatively little variability throughout the year, while short-term variability can be high especially at the urban site. The average hygroscopicity parameter, κ, calculated from the chemical composition of submicron particles was highest at the coastal site of Mace Head (0.6) and lowest at the rain forest station ATTO (0.2–0.3). We performed closure studies based on κ–Köhler theory to predict CCN number concentrations. The ratio of predicted to measured CCN concentrations is between 0.87 and 1.4 for five different types of κ. The temporal variability is also well captured, with Pearson correlation coefficients exceeding 0.87. Information on CCN number concentrations at many locations is important to better characterise ACI and their radiative forcing. But long-term comprehensive aerosol particle characterisations are labour intensive and costly. Hence, we recommend operating “migrating-CCNCs” to conduct collocated CCN number concentration and particle number size distribution measurements at individual locations throughout one year at least to derive a seasonally resolved hygroscopicity parameter. This way, CCN number concentrations can only be calculated based on continued particle number size distribution information and greater spatial coverage of long-term measurements can be achieved.

Description: Aerosol radiative properties are investigated in southeastern Spain during a dust event on 16–17 June 2013 in the framework of the ChArMEx/ADRIMED (Chemistry-Aerosol Mediterranean Experiment/Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) campaign. Particle optical and microphysical properties from ground-based sun/sky photometer and lidar measurements, as well as in situ measurements on board the SAFIRE ATR 42 French research aircraft, are used to create a set of different levels of input parameterizations, which feed the 1-D radiative transfer model (RTM) GAME (Global Atmospheric ModEl). We consider three datasets: (1) a first parameterization based on the retrievals by an advanced aerosol inversion code (GRASP; Generalized Retrieval of Aerosol and Surface Properties) applied to combined photometer and lidar data, (2) a parameterization based on the photometer columnar optical properties and vertically resolved lidar retrievals with the two-component Klett–Fernald algorithm, and (3) a parameterization based on vertically resolved optical and microphysical aerosol properties measured in situ by the aircraft instrumentation. Once retrieved, the outputs of the RTM in terms of both shortwave and longwave radiative fluxes are compared against ground and in situ airborne measurements. In addition, the outputs of the model in terms of the aerosol direct radiative effect are discussed with respect to the different input parameterizations. Results show that calculated atmospheric radiative fluxes differ no more than 7 % from the measured ones. The three parameterization datasets produce a cooling effect due to mineral dust both at the surface and the top of the atmosphere. Aerosol radiative effects with differences of up to 10 W m−2 in the shortwave spectral range (mostly due to differences in the aerosol optical depth) and 2 W m−2 for the longwave spectral range (mainly due to differences in the aerosol optical depth but also to the coarse mode radius used to calculate the radiative properties) are obtained when comparing the three parameterizations. The study reveals the complexity of parameterizing 1-D RTMs as sizing and characterizing the optical properties of mineral dust is challenging. The use of advanced remote sensing data and processing, in combination with closure studies on the optical and microphysical properties from in situ aircraft measurements when available, is recommended.

Description: Observing stratospheric ozone is essential to assess whether the Montreal Protocol has succeeded in saving the ozone layer by banning ozone depleting substances. Recent studies have reported positive trends, indicating that ozone is recovering in the upper stratosphere at mid-latitudes, but the trend magnitudes differ, and uncertainties are still high. Trends and their uncertainties are influenced by factors such as instrumental drifts, sampling patterns, discontinuities, biases, or short-term anomalies that may all mask a potential ozone recovery. The present study investigates how anomalies, temporal measurement sampling rates, and trend period lengths influence resulting trends. We present an approach for handling suspicious anomalies in trend estimations. For this, we analysed multiple ground-based stratospheric ozone records in central Europe to identify anomalous periods in data from the GROund-based Millimetre-wave Ozone Spectrometer (GROMOS) located in Bern, Switzerland. The detected anomalies were then used to estimate ozone trends from the GROMOS time series by considering the anomalous observations in the regression. We compare our improved GROMOS trend estimate with results derived from the other ground-based ozone records (lidars, ozonesondes, and microwave radiometers), that are all part of the Network for the Detection of Atmospheric Composition Change (NDACC). The data indicate positive trends of 1 % decade−1 to 3 % decade−1 at an altitude of about 39 km (3 hPa), providing a confirmation of ozone recovery in the upper stratosphere in agreement with satellite observations. At lower altitudes, the ground station data show inconsistent trend results, which emphasize the importance of ongoing research on ozone trends in the lower stratosphere. Our presented method of a combined analysis of ground station data provides a useful approach to recognize and to reduce uncertainties in stratospheric ozone trends by considering anomalies in the trend estimation. We conclude that stratospheric trend estimations still need improvement and that our approach provides a tool that can also be useful for other data sets.

Description: Methane emissions on the national scale in France in 2012 are inferred by assimilating continuous atmospheric mixing ratio measurements from nine stations of the European network ICOS located in France and surrounding countries. To assess the robustness of the fluxes deduced by our inversion system based on an objectified quantification of uncertainties, two complementary inversion set-ups are computed and analysed: (i) a regional run correcting for the spatial distribution of fluxes in France and (ii) a sectorial run correcting fluxes for activity sectors on the national scale. In addition, our results for the two set-ups are compared with fluxes produced in the framework of the inversion inter-comparison exercise of the InGOS project. The seasonal variability in fluxes is consistent between different set-ups, with maximum emissions in summer, likely due to agricultural activity. However, very high monthly posterior uncertainties (up to ≈ 65 to 74 % in the sectorial run in May and June) make it difficult to attribute maximum emissions to a specific sector. On the yearly and national scales, the two inversions range from 3835 to 4050 Gg CH4 and from 3570 to 4190 Gg CH4 for the regional and sectorial runs, respectively, consistently with the InGOS products. These estimates are 25 to 55 % higher than the total national emissions from bottom-up approaches (biogeochemical models from natural emissions, plus inventories for anthropogenic ones), consistently pointing at missing or underestimated sources in the inventories and/or in natural sources. More specifically, in the sectorial set-up, agricultural emissions are inferred as 66% larger than estimates reported to the UNFCCC. Uncertainties in the total annual national budget are 108 and 312 Gg CH4, i.e, 3 to 8 %, for the regional and sectorial runs respectively, smaller than uncertainties in available bottom-up products, proving the added value of top-down atmospheric inversions. Therefore, even though the surface network used in 2012 does not allow us to fully constrain all regions in France accurately, a regional inversion set-up makes it possible to provide estimates of French methane fluxes with an uncertainty in the total budget of less than 10 % on the yearly timescale. Additional sites deployed since 2012 would help to constrain French emissions on finer spatial and temporal scales and attributing missing emissions to specific sectors.

Description: Detailed measurements of radiation, atmospheric and aerosol properties were carried out in summer 2013 during the Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region (ADRIMED) campaign in the framework of the Chemistry-Aerosol Mediterranean Experiment (ChArMEx) experiment. This study focusses on the characterization of infrared (IR) optical properties and direct radiative effects of mineral dust, based on three vertical profiles of atmospheric and aerosol properties and IR broadband and narrowband radiation from airborne measurements, made in conjunction with radiosonde and ground-based observations at Lampedusa, in the central Mediterranean. Satellite IR spectra from the Infrared Atmospheric Sounder Interferometer (IASI) are also included in the analysis. The atmospheric and aerosol properties are used as input to a radiative transfer model, and various IR radiation parameters (upward and downward irradiance, nadir and zenith brightness temperature at different altitudes) are calculated and compared with observations. The model calculations are made for different sets of dust particle size distribution (PSD) and refractive index (RI), derived from observations and from the literature. The main results of the analysis are that the IR dust radiative forcing is non-negligible and strongly depends on PSD and RI. When calculations are made using the in situ measured size distribution, it is possible to identify the refractive index that produces the best match with observed IR irradiances and brightness temperatures (BTs). The most appropriate refractive indices correspond to those determined from independent measurements of mineral dust aerosols from the source regions (Tunisia, Algeria, Morocco) of dust transported over Lampedusa, suggesting that differences in the source properties should be taken into account. With the in situ size distribution and the most appropriate refractive index the estimated dust IR radiative forcing efficiency is +23.7 W m−2 at the surface, −7.9 W m−2 within the atmosphere, and +15.8 W m−2 at the top of the atmosphere. The use of column-integrated dust PSD from AERONET may also produce a good agreement with measured irradiances and BTs, but with significantly different values of the RI. This implies large differences, up to a factor of 2.5 at surface, in the estimated dust radiative forcing, and in the IR heating rate. This study shows that spectrally resolved measurements of BTs are important to better constrain the dust IR optical properties, and to obtain a reliable estimate of its radiative effects. Efforts should be directed at obtaining an improved description of the dust size distribution and its vertical distribution, as well as at including regionally resolved optical properties.

Description: We use remote sensing of the proton aurora with the IMAGE-FUV SI12 (Imager for Magnetopause to Aurora Global Exploration–Far Ultraviolet–Spectrographic Imaging at 121.8 nm) instrument and radar measurements of the ionospheric convection from the SuperDARN (Super Dual Aurora Radar Network) facility to estimate the open magnetic flux in the Earth's magnetosphere and the reconnection rates at the dayside magnetopause and in the magnetotail during intervals of steady magnetospheric convection (SMC). We find that SMC intervals occur with relatively high open magnetic flux (average  ∼  0.745 GWb, standard deviation  ∼  0.16 GWb), which is often found to be nearly steady, when the magnetic flux opening and closure rates approximately balance around 55 kV on average, with a standard deviation of 21 kV. We find that the residence timescale of open magnetic flux, defined as the ratio between the open magnetospheric flux and the flux closure rate, is roughly 4 h during SMCs. Interestingly, this number is approximately what can be deduced from the discussion of the length of the tail published by Dungey (1965), assuming a solar wind speed of  ∼  450 km s−1. We also infer an enhanced convection velocity in the tail, driving open magnetic flux to the nightside reconnection site. We compare our results with previously published studies in order to identify different magnetospheric modes. These are ordered by increasing open magnetic flux and reconnection rate as quiet conditions, SMCs, substorms (with an important overlap between these last two) and sawtooth intervals.

Description: Most of the global fossil fuel CO2 emissions arise from urbanized and industrialized areas. Bottom-up inventories quantify them but with large uncertainties. In 2010–2011, the first atmospheric in situ CO2 measurement network for Paris, the capital of France, began operating with the aim of monitoring the regional atmospheric impact of the emissions coming from this megacity. Five stations sampled air along a northeast–southwest axis that corresponds to the direction of the dominant winds. Two stations are classified as rural (Traînou – TRN; Montgé-en-Goële – MON), two are peri-urban (Gonesse – GON; Gif-sur-Yvette – GIF) and one is urban (EIF, located on top of the Eiffel Tower). In this study, we analyze the diurnal, synoptic and seasonal variability of the in situ CO2 measurements over nearly 1 year (8 August 2010–13 July 2011). We compare these datasets with remote CO2 measurements made at Mace Head (MHD) on the Atlantic coast of Ireland and support our analysis with atmospheric boundary layer height (ABLH) observations made in the center of Paris and with both modeled and observed meteorological fields. The average hourly CO2 diurnal cycles observed at the regional stations are mostly driven by the CO2 biospheric cycle, the ABLH cycle and the proximity to urban CO2 emissions. Differences of several µmol mol−1 (ppm) can be observed from one regional site to the other. The more the site is surrounded by urban sources (mostly residential and commercial heating, and traffic), the more the CO2 concentration is elevated, as is the associated variability which reflects the variability of the urban sources. Furthermore, two sites with inlets high above ground level (EIF and TRN) show a phase shift of the CO2 diurnal cycle of a few hours compared to lower sites due to a strong coupling with the boundary layer diurnal cycle. As a consequence, the existence of a CO2 vertical gradient above Paris can be inferred, whose amplitude depends on the time of the day and on the season, ranging from a few tenths of ppm during daytime to several ppm during nighttime. The CO2 seasonal cycle inferred from monthly means at our regional sites is driven by the biospheric and anthropogenic CO2 flux seasonal cycles, the ABLH seasonal cycle and also synoptic variations. Enhancements of several ppm are observed at peri-urban stations compared to rural ones, mostly from the influence of urban emissions that are in the footprint of the peri-urban station. The seasonal cycle observed at the urban station (EIF) is specific and very sensitive to the ABLH cycle. At both the diurnal and the seasonal scales, noticeable differences of several ppm are observed between the measurements made at regional rural stations and the remote measurements made at MHD, that are shown not to define background concentrations appropriately for quantifying the regional (∼ 100 km) atmospheric impact of urban CO2 emissions. For wind speeds less than 3 m s−1, the accumulation of local CO2 emissions in the urban atmosphere forms a dome of several tens of ppm at the peri-urban stations, mostly under the influence of relatively local emissions including those from the Charles de Gaulle (CDG) Airport facility and from aircraft in flight. When wind speed increases, ventilation transforms the CO2 dome into a plume. Higher CO2 background concentrations of several ppm are advected from the remote Benelux–Ruhr and London regions, impacting concentrations at the five stations of the network even at wind speeds higher than 9 m s−1. For wind speeds ranging between 3 and 8 m s−1, the impact of Paris emissions can be detected in the peri-urban stations when they are downwind of the city, while the rural stations often seem disconnected from the city emission plume. As a conclusion, our study highlights a high sensitivity of the stations to wind speed and direction, to their distance from the city, but also to the ABLH cycle depending on their elevation. We learn some lessons regarding the design of an urban CO2 network: (1) careful attention should be paid to properly setting regional (∼ 100 km) background sites that will be representative of the different wind sectors; (2) the downwind stations should be positioned as symmetrically as possible in relation to the city center, at the peri-urban/rural border; (3) the stations should be installed at ventilated sites (away from strong local sources) and the air inlet set up above the building or biospheric canopy layer, whichever is the highest; and (4) high-resolution wind information should be available with the CO2 measurements.