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Ice nuclei properties within a Saharan dust event at the Jungfraujoch in the Swiss Alps

The new portable ice nucleation chamber (PINC) developed by the Institute for Atmospheric and Climate Sciences of ETH Zurich was operated during two measurement campaigns at the high alpine research station Jungfraujoch situated at 3580 m a.s.l, in March and June 2009. During this time of the year, a high probability of Saharan dust events (SDE) at the Jungfraujoch has been observed. We used an impactor with a cutoff size of 1 μm aerodynamic diameter and operated the system at −31 °C and relative humidities of 127 % and 91 % with respect to ice and water, respectively. Investigation of the ambient number concentration of ice nuclei (IN) in the deposition nucleation mode and during a SDE in the free troposphere is reported. The results discussed in this paper are the first continuous IN measurements over a period of several days at the Jungfraujoch. The average IN concentration found during the campaign in March was 8 particles per liter whereas during the campaign in June, the average number concentration was higher up to 14 particles per liter. Two SDEs were detected on 15 and 16 June 2009. Our measurements show that the SDEs had IN number concentration up to several hundreds per liter. We found the best correlation between the number concentration of the larger particle fraction measured by an optical particle counter and the IN number concentration during a Saharan dust event. This correlation factor is higher for particles larger than 0.5 μm meaning that a higher concentration of larger particles induced higher IN number concentration. No correlation could be found between the black carbon mass concentration and the variations in IN number concentration.
The 2009 stratospheric major warming described from synergistic use of BASCOE water vapour analyses and MLS observations

The record-breaking major stratospheric warming of northern winter 2009 (January–February) is studied using BASCOE (Belgian Assimilation System for Chemical ObsErvation) stratospheric water vapour analyses and MLS (Microwave Limb Sounder) water vapour observations, together with meteorological data from the European Centre for Medium-Range Weather Forecasts (ECMWF) and potential vorticity (PV) derived from ECMWF meteorological data. We focus on the interaction between the cyclonic wintertime stratospheric polar vortex and subsidiary anticyclonic stratospheric circulations during the build-up, peak and aftermath of the major warming. We show dynamical consistency between the water vapour analysed fields and the meteorological and PV fields. Using various approaches, we use the analysed water vapour fields to estimate descent in the polar vortex during this period of between ~0.5 km day−1 and ~0.7 km day−1. New results include the analysis of water vapour during the major warming and demonstration of the benefit of assimilating MLS satellite data into the BASCOE model.
Corrigendum to "Geomagnetic activity related NOx enhancements and polar surface air temperature variability in a chemistry climate model: modulation of the NAM index" published in Atmos. Chem. Phys., 11, 4521–4531, 2011
Optimizing global CO emission estimates using a four-dimensional variational data assimilation system and surface network observations

We apply a four-dimensional variational (4D-VAR) data assimilation system to optimize carbon monoxide (CO) emissions for 2003 and 2004 and to reduce the uncertainty of emission estimates from individual sources using the chemistry transport model TM5. The system is designed to assimilate large (satellite) datasets, but in the current study only a limited amount of surface network observations from the National Oceanic and Atmospheric Administration Earth System Research Laboratory (NOAA/ESRL) Global Monitoring Division (GMD) is used to test the 4D-VAR system. By design, the system is capable to adjust the emissions in such a way that the posterior simulation reproduces background CO mixing ratios and large-scale pollution events at background stations. Uncertainty reduction up to 60 % in yearly emissions is observed over well-constrained regions and the inferred emissions compare well with recent studies for 2004. However, with the limited amount of data from the surface network, the system becomes data sparse resulting in a large solution space. Sensitivity studies have shown that model uncertainties (e.g., vertical distribution of biomass burning emissions and the OH field) and the prior inventories used, influence the inferred emission estimates. Also, since the observations only constrain total CO emissions, the 4D-VAR system has difficulties in separating anthropogenic and biogenic sources in particular. The inferred emissions are validated with NOAA aircraft data over North America and the agreement is significantly improved from the prior to posterior simulation. Validation with the Measurements Of Pollution In The Troposphere (MOPITT) instrument version 4 (V4) shows a slight improved agreement over the well-constrained Northern Hemisphere and in the tropics (except for the African continent). However, the model simulation with posterior emissions underestimates MOPITT CO total columns on the remote Southern Hemisphere (SH) by about 10 %. This is caused by a reduction in SH CO sources mainly due to surface stations on the high southern latitudes.
The effect of trimethylamine on atmospheric nucleation involving H2SO4

Field observations and quantum chemical calculations have shown that organic amine compounds may be important for new particle formation involving H2SO4. Here, we report laboratory observations that investigate the effect of trimethylamine (TMA) on H2SO4-H2O nucleation made under aerosol precursor concentrations typically found in the lower troposphere ([H2SO4] of 106−107 cm−3; [TMA] of 180–1350 pptv). The threshold [H2SO4] needed to produce the unity J was from 106−107 cm−3 and the slopes of Log J vs. Log [H2SO4] and Log J vs. Log [TMA] were 4–6 and 1, respectively, strikingly similar to the case of ammonia (NH3 ternary nucleation (Benson et al., 2011). At lower RH, however, enhancement in J due to TMA was up to an order of magnitude greater than that due to NH3. These findings imply that both amines and NH3 are important nucleation species, but under dry atmospheric conditions, amines may have stronger effects on H2SO4 nucleation than NH3. Aerosol models should therefore take into account inorganic and organic base compounds together to fully understand the widespread new particle formation events in the lower troposphere.
Ternary homogeneous nucleation of H2SO4, NH3, and H2O under conditions relevant to the lower troposphere

Ternary homogeneous nucleation (THN) of H2SO4, NH3 and H2O has been used to explain new particle formation in various atmospheric regions, yet laboratory measurements of THN have failed to reproduce atmospheric observations. Here, we report first laboratory observations of THN made under conditions relevant to the lower troposphere ([H2SO4] of 106–107 cm−3, [NH3] of 0.08–20 ppbv, and a temperature of 288 K). Our observations show that NH3 can enhance atmospheric H2SO4 aerosol nucleation and the enhancement factor (EF) in nucleation rate (J) due to NH3 (the ratio of J measured with vs. without NH3) increases linearly with increasing [NH3] and increases with decreasing [H2SO4] and RH. Two chemical ionization mass spectrometers (CIMS) are used to measure [H2SO4] and [NH3], as well as possible impurities of amines in the nucleation system. Aerosol number concentrations are measured with a water condensation counter (CPC, TSI 3786). The slopes of Log J vs. Log [H2SO4], Log J vs. Log RH, and Log J vs. Log [NH3] are 3–5, 1–4, and 1, respectively. These slopes and the threshold of [H2SO4] required for the unity nucleation vary only fractionally in the presence and absence of NH3. These observations can be used to improve aerosol nucleation models to assess how man-made SO2 and NH3 affect aerosol formation and CCN production at the global scale.
Worldwide trend of atmospheric mercury since 1995

Concern about the adverse effects of mercury on human health and ecosystems has led to tightening emission controls since the mid 1980s. But the resulting mercury emissions reductions in many parts of the world are believed to be offset or even surpassed by the increasing emissions in rapidly industrializing countries. Consequently, concentrations of atmospheric mercury are expected to remain roughly constant. Here we show that the worldwide atmospheric mercury concentrations have decreased by about 20 to 38 % since 1996 as indicated by long-term monitoring at stations in the Southern and Northern Hemispheres combined with intermittent measurements of latitudinal distribution over the Atlantic Ocean. The total reduction of the atmospheric mercury burden of this magnitude within 14 years is unusually large among most atmospheric trace gases and is at odds with the current mercury emission inventories with nearly constant anthropogenic emissions over this period. This suggests a major shift in the biogeochemical cycle of mercury including oceans and soil reservoirs. Decreasing reemissions from the legacy of historical mercury emissions are the most likely explanation for this decline since the hypothesis of an accelerated oxidation rate of elemental mercury in the atmosphere is not supported by the observed trends of other trace gases. Acidification of oceans, climate change, excess nutrient input and pollution may also contribute by their impact on the biogeochemistry of ocean and soils. Consequently, models of the atmospheric mercury cycle have to include soil and ocean mercury pools and their dynamics to be able to make projections of future trends.
Corrigendum to "Chemical apportionment of southern African aerosol mass and optical depth" published in Atmos. Chem. Phys., 9, 7643–7655, 2009

A correction to results by Magi (2009) is presented here. By combining the in situ measurements of speciated aerosol mass concentrations with concurrent measurements of total aerosol optical properties at a wavelength of 550 nm, it is shown that ~66 % of scattering is due to carbonaceous aerosol, where derived mass scattering cross sections (MSC) for OC and BC are 3.8 ± 0.5 m2 g−1 and 2.9 ± 0.8 m2 g−1, respectively. Derived values of mass absorption cross sections (MAC) for OC and BC are 0.7 ± 0.2 m2 g−1 and 12.1 ± 0.8 m2 g−1, respectively. The values of MAC imply that ~21 % of the mid-visible aerosol absorption in southern Africa is due to OC, with the remainder due to BC. SSA for BC and OC are about the same as Magi (2009). The results here are determined using an approach that accounts for the fact that OC and BC are partially scattering and absorbing.
Impacts of future climate change and effects of biogenic emissions on surface ozone and particulate matter concentrations in the United States

Simulations of present and future average regional ozone and PM2.5 concentrations over the United States were performed to investigate the potential impacts of global climate change and emissions on regional air quality using CMAQ. Various emissions and climate conditions with different biogenic emissions and domain resolutions were implemented to study the sensitivity of future air quality trends from the impacts of changing biogenic emissions. A comparison of GEOS-Chem and CMAQ was performed to investigate the effect of downscaling on the prediction of future air quality trends. For ozone, the impacts of global climate change are relatively smaller when compared to the impacts of anticipated future emissions reduction, except for the Northeast area, where increasing biogenic emissions due to climate change have stronger positive effects (increases) to the regional ozone air quality. The combination effect from both climate change and emission reductions leads to approximately a 10 % or 5 ppbv decrease of the maximum daily average eight-hour ozone (MDA8) over the Eastern United States. For PM2.5, the impacts of global climate change have shown insignificant effect, where as the impacts of anticipated future emissions reduction account for the majority of overall PM2.5 reductions. The annual average 24-h PM2.5 of the future-year condition was found to be about 40 % lower than the one from the present-year condition, of which 60 % of its overall reductions are contributed to by the decrease of SO4 and NO3 particulate matters. Changing the biogenic emissions model increases the MDA8 ozone by about 5–10 % or 3–5 ppbv in the Northeast area. Conversely, it reduces the annual average PM2.5 by 5 % or 1.0 μg m−3 in the Southeast region.
Comparison of two different sea-salt aerosol schemes as implemented in air quality models applied to the Mediterranean Basin

A number of attempts have been made to incorporate sea-salt aerosol (SSA) source functions in chemistry transport models with varying results according to the complexity of the scheme considered. This contribution compares the inclusion of two different SSA algorithms in two chemistry transport models: CMAQ and CHIMERE. The main goal is to examine the differences in average SSA mass and composition and to study the seasonality of the prediction of SSA when applied to the Mediterranean area with high resolution for a reference year. Dry and wet deposition schemes are also analyzed to better understand the differences observed between both models in the target area. The applied emission algorithm in CHIMERE uses a semi-empirical formulation which obtains the surface emission rate of SSA as a function of the particle size and the surface wind speed raised to the power 3.41. The emission parameterization included within CMAQ is somehow more sophisticated, since fluxes of SSA are corrected with relative humidity. In order to evaluate their strengths and weaknesses, the participating algorithms as implemented in the chemistry transport models were evaluated against AOD measurements from Aeronet and available surface measurements in Southern Europe and the Mediterranean area, showing biases around −0.002 and −1.2 μg m−3, respectively. The results indicate that both models represent accurately the patterns and dynamics of SSA and its non-uniform behavior in the Mediterranean basin, showing a strong seasonality. The levels of SSA strongly vary across the Western and the Eastern Mediterranean, reproducing CHIMERE higher annual levels in the Aegean Sea (12 μg m−3) and CMAQ in the Gulf of Lion (9 μg m−3). The large difference found for the ratio PM2.5/total SSA in CMAQ and CHIMERE is also investigated. The dry and wet removal rates are very similar for both models despite the different schemes implemented. Dry deposition essentially follows the surface drag stress patterns, meanwhile wet deposition is more scattered over the continent. CMAQ tends to provide larger amounts of SSA dry deposition over the Northern Mediterranean (0.7–1.0 g m−2 yr−1), meanwhile the Southeastern Mediterranean accounts for the maximum annual dry deposition in the CHIMERE model (0.9–1.5 g m−2 yr−1). The wet deposition is dominated by the accumulation mode and is strongly correlated to the precipitation patterns, showing CMAQ a higher wet deposition/total deposition ratio over coastal mountain chains. The results of both models constitute a step towards increasing the understanding of the SSA dynamics in a complex area as the Mediterranean.