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Sensitivity of aerosol and cloud effects on radiation to cloud types: comparison between deep convective clouds and warm stratiform clouds over one-day period

Cloud and aerosol effects on radiation in two contrasting cloud types, a deep mesoscale convective system (MCS) and warm stratocumulus clouds, are simulated and compared. At the top of the atmosphere, 45–81% of shortwave cloud forcing (SCF) is offset by longwave cloud forcing (LCF) in the MCS, whereas warm stratiform clouds show the offset of less than ~20%. 28% of increased negative SCF is offset by increased LCF with increasing aerosols in the MCS at the top of the atmosphere. However, the stratiform clouds show the offset of just around 2–5%. Ice clouds as well as liquid clouds play an important role in the larger offset in the MCS. Lower cloud-top height and cloud depth, characterizing cloud types, lead to the smaller offset of SCF by LCF and the offset of increased negative SCF by increased LCF at high aerosol in stratocumulus clouds than in the MCS. Supplementary simulations show that this dependence of modulation of LCF on cloud depth and cloud-top height is also simulated among different types of convective clouds.
Impact of primary formaldehyde on air pollution in the Mexico City Metropolitan Area

Formaldehyde (HCHO) is a radical source that plays an important role in urban atmospheric chemistry and ozone formation. The Mexico City Metropolitan Area (MCMA) is characterized by high anthropogenic emissions of HCHO (primary HCHO), which together with photochemical production of HCHO from hydrocarbon oxidation (secondary HCHO), lead to high ambient HCHO levels. The CAMx chemical transport model was employed to evaluate the impact of primary HCHO on its ambient concentration, on the ROx radical budget, and on ozone (O3) formation in the MCMA. Important radical sources, including HCHO, HONO, and O3-olefin reactions, were constrained by measurements from routine observations of the local ambient air monitoring network and the MCMA-2003 field campaign. Primary HCHO was found not only to contribute significantly to the ambient HCHO concentration, but also to enhance the radical budget and O3 production in the urban atmosphere of the MCMA. Overall in the urban area, total daytime radical production is enhanced by up to 10% and peak O3 concentration by up to 8%; moreover primary HCHO tends to make O3 both production rates and ambient concentration peak half an hour earlier. While primary HCHO contributes predominantly to the ambient HCHO concentration between nighttime and morning rush hours, significant influence on the radical budget and O3 production starts early in the morning, peaks at mid-morning and is sustained until early afternoon.
Elemental content of PM2.5 aerosol particles collected in Göteborg during the Göte-2005 campaign in February 2005

The Göte–2005 measurement campaign aimed at studying the influence of the winter thermal inversions on urban air pollution. Elemental speciation of PM2.5 aerosol particles, collected on Teflon filters at three urban sites and one rural site in the Göteborg region, was a major part of the study. Trace element analysis was done by Energy Dispersive X-Ray Fluorescence (EDXRF) spectrometry and the concentrations of S, Cl, K, Ca, Ti, V, Mn, Fe, Ni, Cu, Zn, Br and Pb were determined. The elemental content of the particles, local wind speed and direction, and backward trajectories were used to investigate possible sources for the pollutants. We concluded that S, V, Ni, Br, and Pb had their main sources outside the central Göteborg area, since elevated concentrations of these elements were not observed during an inversion episode. Sea traffic and harbour activities were identified, primarily by the S and V content of the particles. This study showed that the elemental analysis by EDXRF presents valuable information for tracing the origin of air masses arriving at a measurement site.
Estimating surface CO2 fluxes from space-borne CO2 dry air mole fraction observations using an ensemble Kalman Filter

We have developed an ensemble Kalman Filter (EnKF) to estimate 8-day regional surface fluxes of CO2 from space-borne CO2 dry-air mole fraction observations (XCO2) and evaluate the approach using a series of synthetic experiments, in preparation for data from the NASA Orbiting Carbon Observatory (OCO). The 32-day duty cycle of OCO alternates every 16 days between nadir and glint measurements of backscattered solar radiation at short-wave infrared wavelengths. The EnKF uses an ensemble of states to represent the error covariances to estimate 8-day CO2 surface fluxes over 144 geographical regions. We use a 12×8-day lag window, recognising that XCO2 measurements include surface flux information from prior time windows. The observation operator that relates surface CO2 fluxes to atmospheric distributions of XCO2 includes: a) the GEOS-Chem transport model that relates surface fluxes to global 3-D distributions of CO2 concentrations, which are sampled at the time and location of OCO measurements that are cloud-free and have aerosol optical depths <0.3; and b) scene-dependent averaging kernels that relate the CO2 profiles to XCO2, accounting for differences between nadir and glint measurements, and the associated scene-dependent observation errors. We show that OCO XCO2 measurements significantly reduce the uncertainties of surface CO2 flux estimates. Glint measurements are generally better at constraining ocean CO2 flux estimates. Nadir XCO2 measurements over the terrestrial tropics are sparse throughout the year because of either clouds or smoke. Glint measurements provide the most effective constraint for estimating tropical terrestrial CO2 fluxes by accurately sampling fresh continental outflow over neighbouring oceans. We also present results from sensitivity experiments that investigate how flux estimates change with 1) bias and unbiased errors, 2) alternative duty cycles, 3) measurement density and correlations, 4) the spatial resolution of estimated flux estimates, and 5) reducing the length of the lag window and the size of the ensemble. At the revision stage of this manuscript, the OCO instrument failed to reach its orbit after it was launched on 24 February 2009. The EnKF formulation presented here is also applicable to GOSAT measurements of CO2 and CH4.
Microphysical and radiative characterization of a subvisible midlevel Arctic ice cloud by airborne observations – a case study

During the Arctic Study of Tropospheric Aerosol, Clouds and Radiation (ASTAR) campaign, which was conducted in March and April 2007, an optically thin ice cloud was observed south of Svalbard at around 3 km altitude. The microphysical and radiative properties of this particular subvisible midlevel cloud were investigated with complementary remote sensing and in situ instruments. Collocated airborne lidar remote sensing and spectral solar radiation measurements were performed at a flight altitude of 2300 m below the cloud base. Under almost stationary atmospheric conditions, the same subvisible midlevel cloud was probed with various in situ sensors roughly 30 min later. From individual ice crystal samples detected with the Cloud Particle Imager and the ensemble of particles measured with the Polar Nephelometer, microphysical properties were retrieved with a bi-modal inversion algorithm. The best agreement with the measurements was obtained for small ice spheres and deeply rough hexagonal ice crystals. Furthermore, the single-scattering albedo, the scattering phase function as well as the volume extinction coefficient and the effective diameter of the crystal population were determined. A lidar ratio of 21(±6) sr was deduced by three independent methods. These parameters in conjunction with the cloud optical thickness obtained from the lidar measurements were used to compute spectral and broadband radiances and irradiances with a radiative transfer code. The simulated results agreed with the observed spectral downwelling radiance within the range given by the measurement uncertainty. Furthermore, the broadband radiative simulations estimated a net (solar plus thermal infrared) radiative forcing of the subvisible midlevel ice cloud of −0.4 W m−2 (−3.2 W m−2 in the solar and +2.8 W m−2 in the thermal infrared wavelength range).
Intercomparison of ammonia measurement techniques at an intensively managed grassland site (Oensingen, Switzerland)

As part of a field campaign in the framework of the NitroEurope project, three different instruments for atmospheric ammonia (NH3) measurements were operated side-by-side on a managed grassland site in Switzerland: a modified Proton Transfer Reaction Mass Spectrometer (PTR-MS), a GRadient of AErosol and Gases Online Registrator (GRAEGOR), and an Automated Ammonia Analyzer (AiRRmonia). The modified PTR-MS approach is based on chemical ionization of NH3 using O2+ instead of H3O+ as ionizing agent, GRAEGOR and AiRRmonia measure NH4+ in liquids after absorption of gaseous NH3 in a rotating wet-annular denuder and through a gas permeable membrane, respectively. Bivariate regression slopes using uncorrected data from all three instruments ranged from 0.78 to 0.97 while measuring ambient NH3 levels between 2 and 25 ppbv during a 5 days intercomparison period. Correlation coefficients r2 were in the range of 0.79 to 0.94 for hourly average mixing ratios. Observed discrepancies could be partly attributed to temperature effects on the GRAEGOR calibration. Bivariate regression slopes using corrected data were >0.92 with offsets ranging from 0.22 to 0.58 ppbv. The intercomparison demonstrated the potential of PTR-MS to resolve short-time NH3 fluctuations which could not be measured by the two other slow-response instruments. During conditions favoring condensation in inlet lines, the PTR-MS underestimated NH3 mixing ratios, underlining the importance of careful inlet designs as an essential component for any inlet-based instrument.
The impact of weather and atmospheric circulation on O3 and PM10 levels at a rural mid-latitude site

In spite of the strict EU regulations, concentrations of surface ozone and PM10 often exceed the pollution standards for the Netherlands and Europe. Their concentrations are controlled by (precursor) emissions, social and economic developments and a complex combination of meteorological actors. This study tackles the latter, and provides insight in the meteorological processes that play a role in O3 and PM10 levels in rural mid-latitudes sites in the Netherlands. The relations between meteorological actors and air quality are studied on a local scale based on observations from four rural sites and are determined by a comprehensive correlation analysis and a multiple regression (MLR) analysis in 2 modes, with and without air quality variables as predictors. Furthermore, the objective Lamb Weather Type approach is used to assess the influence of the large-scale circulation on air quality. Keeping in mind its future use in downscaling future climate scenarios for air quality purposes, special emphasis is given to an appropriate selection of the regressor variables readily available from operational meteorological forecasts or AOGCMs (Atmosphere-Ocean coupled General Circulation Models). The regression models perform satisfactory, especially for O3, with an (R2 of 57.0% and 25.0% for PM10. Including previous day air quality information increases significantly the models performance by 15% (O3) and 18% (PM10). The Lamb weather types show a seasonal distinct pattern for high (low) episodes of average O3 and PM10 concentrations, and these are clear related with the meteorology-air quality correlation analysis. Although using a circulation type approach can provide important additional physical relations forward, our analysis reveals the circulation method is limited in terms of short-term air quality forecast for both O3 and PM10 (R2 between 0.12 and 23%). In summary, it is concluded that the use of a regression model is more promising for short-term downscaling from climate scenarios than the use of a weather type classification approach.
Influence of modelled soil biogenic NO emissions on related trace gases and the atmospheric oxidizing efficiency

The emission of nitric oxide (NO) by soils (SNOx) is an important source of oxides of nitrogen (NOx=NO+NO2) in the troposphere, with estimates ranging from 4 to 21 Tg of nitrogen per year. Previous studies have examined the influence of SNOx on ozone (O3) chemistry. We employ the ECHAM5/MESSy atmospheric chemistry model (EMAC) to go further in the reaction chain and investigate the influence of SNOx on lower tropospheric NOx, O3, peroxyacetyl nitrate (PAN), nitric acid (HNO3), the hydroxyl radical (OH) and the lifetime of methane (τCH4). We show that SNOx is responsible for a significant contribution to the NOx mixing ratio in many regions, especially in the tropics. Furthermore, the concentration of OH is substantially increased due to SNOx, resulting in an enhanced oxidizing efficiency of the global troposphere, reflected in a ~10% decrease in τCH4 due to soil NO emissions. On the other hand, in some regions SNOx has a negative feedback on the lifetime of NOx through O3 and OH, which results in regional increases in the mixing ratio of NOx despite lower total emissions in a simulation without SNOx. In a sensitivity simulation in which we reduce the other surface NOx emissions by the same amount as SNOx, we find that they have a much weaker impact on OH and τCH4 and do not result in an increase in the NOx mixing ratio anywhere.
Anthropogenic influence on SOA and the resulting radiative forcing

The effect of chemical changes in the atmosphere since the pre-industrial period on the distributions and burdens of Secondary Organic Aerosol (SOA) has been calculated using the off-line aerosol chemistry transport model Oslo CTM2. The production of SOA was found to have increased from about 35 Tg yr−1 to 53 Tg yr−1 since pre-industrial times, leading to an increase in the global annual mean SOA burden from 0.33 Tg to 0.50 Tg, or about 51%. The effect of allowing semi-volatile species to partition to sulphate aerosol was also tested, leading to an increase in SOA production from about 43 Tg yr−1 to 69 Tg yr−1 since pre-industrial times, while the annual mean SOA burden increased from 0.44 Tg to 0.70 Tg, or about 59%. The increases were greatest over industrialised areas, especially when partitioning to sulphate aerosol was allowed, as well as over regions with high biogenic precursor emissions. The contribution of emissions from different sources to the larger SOA burdens has been calculated. The results suggest that the majority of the increase was caused by emissions of primary organic aerosols (POA), from fossil fuel and bio fuel combustion. As yet, very few radiative forcing estimates of SOA exist, and no such estimates were provided in the latest IPCC report. In this study, we found that the change in SOA burden caused a radiative forcing (defined here as the difference between the pre-industrial and the present day run) of −0.09 W m−2, when SOA was allowed to partition to both organic and sulphate aerosols, and −0.06 W m−2 when only partitioning to organic aerosols was assumed. Therefore, the radiative forcing of SOA was found to be stronger than the best estimate for POA in the latest IPCC assessment.
Water vapour transport in the tropical tropopause region in coupled Chemistry-Climate Models and ERA-40 reanalysis data

In this study backward trajectories from the tropical lower stratosphere were calculated for the Northern Hemisphere (NH) winters 1995–1996, 1997–1998 (El Niño) and 1998–1999 (La Niña) and summers 1996, 1997 and 1999 using both ERA-40 reanalysis data of the European Centre for Medium-Range Weather Forecast (ECMWF) and coupled Chemistry-Climate Model (CCM) data. The calculated trajectories were analysed to determine the distribution of points where individual air masses encounter the minimum temperature and thus minimum water vapour mixing ratio during their ascent through the tropical tropopause layer (TTL) into the stratosphere. The geographical distribution of these dehydration points and the local conditions there determine the overall water vapour entry into the stratosphere. Results of two CCMs are presented: the ECHAM4.L39(DLR)/CHEM (hereafter: E39/C) from the German Aerospace Center (DLR) and the Freie Universität Berlin Climate Middle Atmosphere Model with interactive chemistry (hereafter: FUB-CMAM-CHEM). In the FUB-CMAM-CHEM model the minimum temperatures are overestimated by about 9 K in NH winter and about 3 K in NH summer, resulting in too high water vapour entry values compared to ERA-40. However, the geographical distribution of dehydration points is fairly similar to ERA-40 for NH winter 1995–1996 and 1998–1999. The distribution of dehydration points in the boreal summer 1996 suggests an influence of the Indian monsoon upon the water vapour transport. The E39/C model displays a temperature bias of about +5 K. Hence, the minimum water vapour mixing ratios are higher relative to ERA-40. The geographical distribution of dehydration points is fairly well in NH winter 1995–1996 and 1997–1998 with respect to ERA-40. The distribution is not reproduced for the NH winter 1998–1999 (La Niña event) compared to ERA-40. There is an excessive water vapour flux through warm regions e.g. Africa in the NH winter and summer. The possible influence of the Indian monsoon on the transport is not seen in the boreal summer 1996. Further, the residence times of air parcels in the TTL were derived from the trajectory calculations. The analysis of the residence times reveals that in both CCMs residence times in the TTL are lower compared to ERA-40 and the seasonal variation is hardly present.