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The Satellite Application Facility on Climate Monitoring (CM-SAF) aims at the provision of satellite-derived geophysical parameter data sets suitable for climate monitoring. CM-SAF provides climatologies for Essential Climate Variables (ECV), as required by the Global Climate Observing System implementation plan in support of the UNFCCC. Several cloud parameters, surface albedo, radiation fluxes at the top of the atmosphere and at the surface as well as atmospheric temperature and humidity products form a sound basis for climate monitoring of the atmosphere. The products are categorized in monitoring data sets obtained in near real time and data sets based on carefully intercalibrated radiances. The CM-SAF products are derived from several instruments on-board operational satellites in geostationary and polar orbit as the Meteosat and NOAA satellites, respectively. The existing data sets will be continued using data from the instruments on-board the new joint NOAA/EUMETSAT Meteorological Operational Polar satellite. The products have mostly been validated against several ground-based data sets both in situ and remotely sensed. The accomplished accuracy for products derived in near real time is sufficient to monitor variability on diurnal and seasonal scales. The demands on accuracy increase the longer the considered time scale is. Thus, interannual variability or trends can only be assessed if the sensor data are corrected for jumps created by instrument changes on successive satellites and more subtle effects like instrument and orbit drift and also changes to the spectral response function of an instrument. Thus, a central goal of the recently started Continuous Development and Operations Phase of the CM-SAF (2007–2012) is to further improve all CM-SAF data products to a quality level that allows for studies of interannual variability.
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Measurements of tropospheric hydroxyl (OH) and hydroperoxy (HO<sub>2</sub>) radicals were made during the MCMA (Mexico City Metropolitan Area) field campaign as part of the MILAGRO (Megacity Initiative: Local and Global Research Observations) project during March 2006. These radicals were measured using a laser-induced fluorescence instrument developed at Indiana University. This new instrument takes advantage of the Fluorescence Assay by Gas Expansion technique (FAGE) together with direct excitation and detection of OH at 308 nm. HO<sub>2</sub> is indirectly measured as OH by titration with NO inside the fluorescence cell. At this stage of development, IU-FAGE is capable of detecting 3.9×10<sup>5</sup> molecule/cm<sup>3</sup> of both OH and HO<sub>2</sub>, with a signal to noise ratio of 1, an averaged laser power of 10-mW and an averaging time of 5-min. The calibration accuracies (1σ) are ±17% for OH and ±18% for HO<sub>2</sub> using the water-vapor photolysis/O<sub>2</sub> actinometry calibration technique. <br><br> OH and HO<sub>2</sub> concentrations were successfully measured at an urban site in Mexico City, with observed concentrations comparable to those measured in other polluted environments. Enhanced levels of OH and HO<sub>2</sub> radicals were observed on several days between 09:30–11:00 a.m. and suggest an intense photochemistry during morning hours that may be due to elevated sources of HO<sub>x</sub> (OH+HO<sub>2</sub>) and a fast cycling between the radicals under the high NO<sub>x</sub> (NO+NO<sub>2</sub>) conditions of the MCMA.
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The first measurements of stratospheric bromine nitrate (BrONO<sub>2</sub>) are reported. Bromine nitrate has been clearly identified in atmospheric infrared emission spectra recorded with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European Envisat satellite, and stratospheric concentration profiles have been determined for different conditions (day and night, different latitudes). The BrONO<sub>2</sub> concentrations show strong day/night variations, with much lower concentrations during the day. Maximum volume mixing ratios observed during night are 20 to 25 pptv. The observed concentration profiles are in agreement with estimations from photochemical models and show that the current understanding of stratospheric bromine chemistry is generally correct.
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This paper presents a climatology and trends of tropospheric ozone in the Southwestern Indian Ocean (Reunion Island) and South Africa (Irene and Johannesburg). This study is based on a multi-instrumental dataset: PTU-O<sub>3</sub> ozonesondes, DIAL LIDAR and MOZAIC airborne instrumentation. <br><br> The seasonal profiles of tropospheric ozone at Reunion Island have been calculated from two different data sets: ozonesondes and LIDAR. The two climatological profiles are similar, except in austral summer when the LIDAR profiles show greater values in the free troposphere, and in the upper troposphere when the LIDAR profiles show lower values during all seasons. These results show that the climatological value of LIDAR profiles must be discussed with care since LIDAR measurements can be performed only under clear sky conditions, and the upper limit of the profile depends on the signal strength. <br><br> In addition, linear trends have been calculated from ozonesonde data at Reunion and Irene. Considering the whole tropospheric column, the trend is slightly positive for Reunion, and more clearly positive for Irene. Trend calculations have also been made separating the troposphere into three layers, and separating the dataset into seasons. Results show that the positive trend for Irene is governed by the lower layer that is affected by industrial pollution and biomass burning. On the contrary, for Reunion Island, the strongest trends are observed in the upper troposphere, and in winter when stratosphere-troposphere exchange is more frequently expected.
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The global aerosol-climate model ECHAM5-HAM was modified to improve the representation of new particle formation in the boundary layer. Activation-type nucleation mechanism was introduced to produce observed nucleation rates in the lower troposphere. A simple and computationally efficient model for biogenic secondary organic aerosol (BSOA) formation was implemented. Here we study the sensitivity of the aerosol and cloud droplet number concentrations (CDNC) to these additions. Activation-type nucleation significantly increases aerosol number concentrations in the boundary layer. Increased particle number concentrations have a significant effect also on cloud droplet number concentrations and therefore on cloud properties. We performed calculations with activation nucleation coefficient values of 2×10<sup>−7</sup>s<sup>−1</sup>, 2×10<sup>−6</sup>s<sup>−1</sup> and 2×10<sup>−5</sup>s<sup>−1</sup> to evaluate the sensitivity to this parameter. For BSOA we have used yields of 0.025, 0.07 and 0.15 to estimate the amount of monoterpene oxidation products available for condensation. The hybrid BSOA formation scheme induces large regional changes to size distribution of organic carbon, and therefore affects particle optical properties and cloud droplet number concentrations locally. Although activation-type nucleation improves modeled aerosol number concentrations in the boundary layer, the use of a global activation coefficient generally leads to overestimation of aerosol number. Overestimation can also arise from underestimation of primary emissions.
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This study shows that it is possible to retrieve the temporal evolution of cloud base heights in convective broken cloud fields from data of the SEVIRI instrument onboard the geostationary satellite Meteosat-9. Presented and discussed are time dependent base heights with a temporal resolution of 15 min from morning to afternoon. Cloud base heights retrieved from SEVIRI data are also compared with independent measurements of a ceilometer, with condensation levels calculated from radiosonde data and with base heights obtained from an application of the method to NOAA/AVHRR data. The validation has been performed for three days in the year 2007 and for seven test areas distributed over Germany and neighbouring countries. The standard deviations of the absolute differences between cloud base heights from Meteosat-9 and radiosonde measurements as well as between NOAA/AVHRR and Meteosat-9 results are both of the order of ±290 m. The correlation coefficient is 0.53 for the comparison of satellite with radiosonde measurements and 0.78 for the intercomparison of the satellite measurements. Furthermore, it is shown that the method retrieves the temporal evolution of cloud base heights in very good agreement with time dependent ceilometer measurements.
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An evaluation of the upper tropospheric humidity from the European Centre of Medium-Range Weather Forecasts (ECMWF) Integrated Forecast System (IFS) is presented. We first make an analysis of the spinup behaviour of ice supersaturation in weather forecasts. It shows that a spinup period of at least 12 h is necessary before using forecast humidity data from the upper troposphere. We compare the forecasted upper tropospheric humidity with coincident relative humidity fields retrieved from the Atmospheric InfraRed Sounder (AIRS) and with cloud vertical profiles from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). The analysis is made over one year, from October 2006 to September 2007, and we discuss how relative humidity and cloud features appear both in the IFS and in the observations. The comparison with AIRS is made difficult because of the vertical resolution of the sounder and the impossibility to retrieve humidity for high cloudiness. Clear sky relative humidities show a rather good correlation whereas cloudy situations reflect more the effect of a dry bias for AIRS increasing with the relative humidity. The comparison with CALIPSO shows that the IFS predicts high relative humidity where CALIPSO finds high clouds, which supports the good quality of the ECMWF upper tropospheric cloud forecast. In a last part, we investigate the presence of ice supersaturation within low vertical resolution pressure layers by comparing the IFS outputs for high-resolution and low-resolution humidity profiles and by simulating the interpolation of humidity over radiosonde data. A new correction method is proposed and tested with these data.
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Air-sea fluxes and bulk seawater and atmospheric concentrations of bromoform (CHBr<sub>3</sub>) and dibromomethane (CH<sub>2</sub>Br<sub>2</sub>) were measured during two research cruises in the northeast Atlantic (53–59° N, June–July 2006) and tropical eastern Atlantic Ocean including over the African coastal upwelling system (16–35° N May–June 2007). Saturations and sea-air fluxes of these compounds generally decreased in the order coastal > upwelling > shelf > open ocean, and outside of coastal regions, a broad trend of elevated surface seawater concentrations with high chlorophyll-<i>a</i> was observed. We show that upwelling regions (coastal and equatorial) represent regional hot spots of bromocarbons, but are probably not of major significance globally, contributing at most a few percent of the total global emissions of CHBr<sub>3</sub> and CH<sub>2</sub>Br<sub>2</sub>. From limited data from eastern Atlantic coastlines, we tentatively suggest that globally, coastal oceans (depth <180 m) together contribute ~2.5 (1.4–3.5) Gmol Br yr<sup>−1</sup> of CHBr<sub>3</sub>, excluding influences from anthropogenic sources such as coastal power stations. This flux estimate is close to current estimates of the total open ocean source. We also show that the concentration ratio of CH<sub>2</sub>Br<sub>2</sub>/CHBr<sub>3</sub> in seawater is a strong function of concentration (and location), with a lower CH<sub>2</sub>Br<sub>2</sub>/CHBr<sub>3</sub> ratio found in coastal regions near to macroalgal sources.
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Comparisons of aircraft measurements of carbon monoxide (CO) to the retrievals of CO using observations from the Measurements of Pollution in The Troposphere (MOPITT) instrument onboard the Terra satellite are presented. Observations made as part of the NASA INTEX-B and NSF MIRAGE field campaigns during March–May 2006 are used to validate the MOPITT CO retrievals, along with routine samples from 2001 through 2006 from NOAA and the MOZAIC measurements from commercial aircraft. A significant positive bias, around 20% for total column CO, in MOPITT CO was found in the comparison to in situ measurements during 2006. Comparisons to the long-term records of measurements from NOAA and MOZAIC revealed an increasing bias in the V3 MOPITT CO retrievals over time. The impact of an instrumental drift is illustrated through retrieval simulations.
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Methane and ozone are two important climate gases with significant tropospheric chemistry. Within chemistry-climate and transport models this chemistry is simplified for computational expediency. We compare the state of the art Master Chemical Mechanism (MCM) with six tropospheric chemistry schemes (CRI-reduced, GEOS-CHEM and a GEOS-CHEM adduct, MOZART-2, TOMCAT and CBM-IV) that could be used within composition transport models. We test the schemes within a box model framework under conditions derived from a composition transport model and from field observations from a regional scale pollution event. We find that CRI-reduced provides much skill in simulating the full chemistry, yet with greatly reduced complexity. We find significant variations between the other chemical schemes, and reach the following conclusions. 1) The inclusion of a gas phase N<sub>2</sub>O<sub>5</sub>+H<sub>2</sub>O reaction in one scheme and not others is a large source of uncertainty in the inorganic chemistry. 2) There are significant variations in the calculated concentration of PAN between the schemes, which will affect the long range transport of reactive nitrogen in global models. 3) The representation of isoprene chemistry differs hugely between the schemes, leading to significant uncertainties on the impact of isoprene on composition. 4) Differences are found in NO<sub>3</sub> concentrations in the nighttime chemistry. Resolving these four issues through further investigative laboratory studies will reduce the uncertainties within the chemical schemes of global tropospheric models.
