-
High-accuracy measurements of snow Bidirectional Reflectance Distribution Function (BRDF) were performed for four natural snow samples with a spectrogonio-radiometer in the 500–2600 nm wavelength range. These measurements are one of the first sets of direct snow BRDF values over a wide range of lighting and viewing geometry. They were compared to BRDF calculated with two optical models. Variations of the snow anisotropy factor with lighting geometry, wavelength and snow physical properties were investigated. Results show that at wavelengths with small penetration depth, scattering mainly occurs in the very top layers and the anisotropy factor is controlled by the phase function. In this condition, forward scattering peak or double scattering peak is observed. In contrast at shorter wavelengths, the penetration of the radiation is much deeper and the number of scattering events increases. The anisotropy factor is thus nearly constant and decreases at grazing observation angles. The whole dataset is available on demand from the corresponding author.
-
Large cloud condensation nuclei (CCN) (e.g., aged dust particles and seasalt) cannot attain their equilibrium size during the typical timescale of cloud droplet activation. Cloud activation parameterizations applied to aerosol with a large fraction of large CCN often do not account for this limitation adequately and can give biased predictions of cloud droplet number concentration (CDNC). Here we present a simple approach to address this problem that can easily be incorporated into cloud activation parameterizations. This method is demonstrated with activation parameterizations based on the "population splitting" concept of Nenes and Seinfeld (2003); it is shown that accounting for large CCN effects eliminates a positive bias in CDNC where the aerosol dry geometric diameter is greater than 0.5 μm. The method proposed here can also be extended to include the water vapor depletion from pre-existing droplets and ice crystals in global and regional atmospheric models.
-
While Antarctica is often described as a pristine environment, there is an increasing awareness of the potential threats from local pollution sources including tourist ships and emissions associated with scientific activities. However, to date there has been no systematic attempt to model the impacts of such pollutants at the continental scale. Indeed, until very recently there was not even a sulphur emission budget available for Antarctica. Here we present the first comprehensive study of atmospheric pollution in Antarctica using a limited area chemistry climate model, and a monthly emissions inventory for sulphur from maintenance of research stations, ground and air traffic, shipping and the active Erebus volcano. We find that ship emissions, both sulphurous and black carbon, dominate anthropogenic pollution near the ground. Their prevalence is likely to rise dramatically if recent trends in tourism continue.
-
Recent ground-based and space borne observations suggest the presence of significant amounts of iodine monoxide in the boundary layer of Antarctica, which are expected to have an impact on the ozone budget and might contribute to the formation of new airborne particles. So far, the source of these iodine radicals has been unknown. This paper presents long-term measurements of iodine monoxide at the German Antarctic research station Neumayer, which indicate that high IO concentrations in the order of 50 ppb are present in the snow interstitial air. The measurements have been performed using multi-axis differential optical absorption spectroscopy (MAX-DOAS). Using a coupled atmosphere – snowpack radiative transfer model, the comparison of the signals observed from scattered skylight and from light reflected by the snowpack yields several ppb of iodine monoxide in the upper layers of the sunlit snowpack throughout the year. Snow pit samples from Neumayer Station contain up to 700 ng/l of total iodine, representing a sufficient reservoir for these extraordinarily high IO concentrations.
-
China is regarded as the largest contributor of mercury (Hg) to the global atmospheric Hg budget. However, concentration levels and depositions of atmospheric Hg in China are poorly known. Continuous measurements of atmospheric gaseous elemental mercury (GEM) were carried out from May 2008 to May 2009 at the summit of Mt. Leigong in south China. Simultaneously, deposition fluxes of THg and MeHg in precipitation, throughfall and litterfall were also studied. Atmospheric GEM concentrations averaged 2.80±1.51 ng m<sup>−3</sup>, which was highly elevated compared to global background values but much lower than semi-rural and industrial/urban areas in China. Sources identification indicates that both regional industrial emissions and long range transport of Hg from central, south and southwest China were corresponded to the elevated GEM level. Seasonal and diurnal variations of GEM were observed, which reflected variations in source intensity, deposition processes and meteorological factors. Precipitation and throughfall deposition fluxes of THg and MeHg in Mt. Leigong were comparable or lower compared to those reported in Europe and North America, whereas litterfall deposition fluxes of THg and MeHg were higher compared to Europe and North America. This highlights the importance of vegetation to Hg atmospheric cycling. In th remote forest ecosystem of China, deposition of GEM via uptake of foliage followed by litterfall was very important for the depletion of atmospheric Hg. Elevated GEM level in ambient air may accelerate the foliar uptake of Hg through air which may partly explain the elevated litterfall deposition fluxes of Hg observed in Mt. Leigong.
-
In this study we investigate ultrafine particle (UFP) fluxes using a first order eddy viscosity turbulence closure Computational Fluid Dynamics (CFD) model and determine the different factors that influence emissions of UFP into the urban boundary layer. Both vertical turbulent fluxes as well as the fluxes due to mean circulatory flow are shown to contribute to the overall ventilation characteristics of street canyons. We then derive a simple parameterised numerical prediction model for canyon top UFP venting which is then compared with tower based micrometeorological flux measurements obtained during the REPARTEE & CityFlux field experiments.
-
We have run a chemistry transport model (CTM) to systematically examine the drivers of interannual variability of tropospheric composition during 1996–2000. This period was characterised by anomalous meteorological conditions associated with the strong El Niño of 1997–1998 and intense wildfires, which produced a large amount of pollution. On a global scale, changing meteorology (winds, temperatures, humidity and clouds) is found to be the most important factor driving interannual variability of NO<sub>2</sub> and ozone on the timescales considered. Changes in stratosphere-troposphere exchange, which are largely driven by meteorological variability, are found to play a particularly important role in driving ozone changes. The strong influence of emissions on NO<sub>2</sub> and ozone interannual variability is largely confined to areas where intense biomass burning events occur. For CO, interannual variability is almost solely driven by emission changes, while for OH meteorology dominates, with the radiative influence of clouds being a very strong contributor. Through a simple attribution analysis for 1996–2000 we conclude that changing cloudiness drives 25% of the interannual variability of OH over Europe by affecting shortwave radiation. Over Indonesia this figure is as high as 71%. Changes in cloudiness contribute a small but non-negligible amount (up to 6%) to the interannual variability of ozone over Europe and Indonesia. This suggests that future assessments of trends in tropospheric oxidizing capacity should account for interannual variability in cloudiness, a factor neglected in many previous studies.
-
We validate OMI ozone profiles between 0.22–215 hPa and stratospheric ozone columns down to 215 hPa (SOC215) against v2.2 MLS data from 2006. The validation demonstrates convincingly that SOC can be derived accurately from OMI data alone, with errors comparable to or smaller than those from current MLS retrievals, and it demonstrates implicitly that tropospheric ozone column can be retrieved accurately from OMI or similar nadir-viewing ultraviolet measurements alone. The global mean biases are within 2.5% above 100 hPa and 5–10% below 100 hPa; the standard deviations of the differences (1σ) are 3.5–5% between 1–50 hPa, 6–9% above 1 hPa and 8–15% below 50 hPa. OMI shows some latitude and solar zenith angle dependent biases, but the mean biases are mostly within 5% and the standard deviations are mostly within 2–5% except for low altitudes and high latitudes. The excellent agreement with MLS data shows that OMI retrievals can be used to augment the validation of MLS and other stratospheric ozone measurements made with even higher vertical resolution than that for OMI. OMI SOC215 shows a small bias of −0.6% with a standard deviation of 2.8%. When compared as a function of latitude and solar zenith angle, the mean biases are within 2% and the standard deviations range from 2.1 to 3.4%. Assuming 2% precision for MLS SOC215, we deduce that the upper limits of random-noise and smoothing errors for OMI SOC215 range from 0.6% in the southern tropics to 2.8% at northern middle latitudes.
-
We present a global aerosol assimilation system based on an Ensemble Kalman filter, which we believe leads to a significant improvement in aerosol fields. The ensemble allows realistic, spatially and temporally variable model covariances (unlike other assimilation schemes). As the analyzed variables are mixing ratios (prognostic variables of the aerosol transport model), there is no need for the extra assumptions required by previous assimilation schemes analyzing aerosol optical thickness (AOT). <br><br> We describe the implementation of this assimilation system and in particular the construction of the ensemble. This ensemble should represent our estimate of current model uncertainties. Consequently, we construct the ensemble around randomly modified emission scenarios. <br><br> The system is tested with AERONET observations of AOT and Angström exponent (AE). Particular care is taken in prescribing the observational errors. The assimilated fields (AOT and AE) are validated through independent AERONET, SKYNET and MODIS Aqua observations. We show that, in general, assimilation of AOT observations leads to improved modelling of global AOT, while assimilation of AE only improves modelling when the AOT is high.
-
Ozone profiles from the surface to about 60 km are retrieved from Ozone Monitoring Instrument (OMI) ultraviolet radiances using the optimal estimation technique. OMI provides daily ozone profiles for the entire sunlit portion of the earth at a horizontal resolution of 13 km×48 km for the nadir position. The retrieved profiles have sufficient accuracy in the troposphere to see ozone perturbations caused by convection, biomass burning and anthropogenic pollution, and to track their spatiotemporal transport. However, to achieve such accuracy it has been necessary to calibrate OMI radiances carefully (using two days of Aura/Microwave Limb Sounder data taken in the tropics). The retrieved profiles contain ~6–7 degrees of freedom for signal, with 5–7 in the stratosphere and 0–1.5 in the troposphere. Vertical resolution varies from 7–11 km in the stratosphere to 10–14 km in the troposphere. Retrieval precisions range from 1% in the middle stratosphere to 10% in the lower stratosphere and troposphere. Solution errors (i.e., root sum square of precisions and smoothing errors) vary from 1–6% in the middle stratosphere to 6–35% in the troposphere, and are dominated by smoothing errors. Total, stratospheric, and tropospheric ozone columns can be retrieved with solution errors typically in the few Dobson unit range at solar zenith angles less than 80°.
