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Southeast Pacific stratocumulus clouds, precipitation and boundary layer structure sampled along 20° S during VOCALS-REx

Multiplatform airborne, ship-based, and land-based observations from 16 October–15 November 2008 during the VOCALS Regional Experiment (REx) are used to document the typical structure of the Southeast Pacific stratocumulus-topped boundary layer and lower free troposphere on a~transect along 20° S between the coast of Northern Chile and a buoy 1500 km offshore. Strong systematic gradients in clouds, precipitation and vertical structure are modulated by synoptically and diurnally-driven variability. The boundary layer is generally capped by a strong (10–12 K), sharp inversion. In the coastal zone, the boundary layer is typically 1 km deep, fairly well mixed, and topped by thin, nondrizzling stratocumulus with accumulation-mode aerosol and cloud droplet concentrations exceeding 200 cm−3. Far offshore, the boundary layer depth is typically deeper (1600 m) and more variable, and the vertical structure is usually decoupled. The offshore stratocumulus typically have strong mesoscale organization, much higher peak liquid water paths, extensive drizzle, and cloud droplet concentrations below 100 cm−3, sometimes with embedded pockets of open cells with lower droplet concentrations. The lack of drizzle near the coast is not just a microphysical response to high droplet concentrations; smaller cloud depth and liquid water path than further offshore appear comparably important. Moist boundary layer air is heated and mixed up along the Andean slopes, then advected out over the top of the boundary layer above adjacent coastal ocean regions. Well offshore, the lower free troposphere is typically much drier. This promotes strong cloud-top radiative cooling and stronger turbulence in the clouds offshore. In conjunction with a slightly cooler free troposphere, this may promote stronger entrainment that maintains the deeper boundary layer seen offshore. Winds from ECMWF and NCEP operational analyses have an rms difference of only 1 m s−1 from collocated airborne leg-mean observations in the boundary layer and 2 m s−1 above the boundary layer. This supports the use of trajectory analysis for interpreting REx observations. Two-day back-trajectories from the 20° S transect suggest that eastward of 75° W, boundary layer (and often free-tropospheric) air has usually been exposed to South American coastal aerosol sources, while at 85° W, neither boundary-layer or free-tropospheric air has typically had such contact.
CO2, δO2/N2 and APO: observations from the Lutjewad, Mace Head and F3 platform flask sampling network

We report results from our atmospheric flask sampling network for three European sites: Lutjewad in the Netherlands, Mace Head in Ireland and the North Sea F3 platform. The air samples from these stations are analyzed for their CO2 and O2 concentrations. In this paper we present the CO2 and O2 data series from these sites between 1998 and 2009, as well as the atmospheric potential oxygen (APO). The seasonal pattern and long term trends agree to a large extent between our three measurement locations. We however find a changing gradient between Mace Head and Lutjewad, both for CO2 and O2. To explain the potential contribution of fossil fuel emissions to this changing gradient we use an atmospheric transport model in combination with CO2 emission data and information on the fossil fuel mix per region. Using the APO trend from Mace Head we obtain an estimate for the global oceanic CO2 uptake of 1.8 ± 0.8 PgC/year.
Some implications of sampling choices on comparisons between satellite and model aerosol optical depth fields

The comparison of satellite and model aerosol optical depth (AOD) fields provides useful information on the strengths and weaknesses of both. However, the sampling of satellite and models is very different and some subjective decisions about data selection and aggregation must be made in order to perform such comparisons. This work examines some implications of these decisions, using GlobAerosol AOD retrievals at 550 nm from Advanced Along-Track Scanning Radiometer (AATSR) measurements, and aerosol fields from the GEOS-Chem chemistry transport model. It is recommended to sample the model only where the satellite flies over on a particular day; neglecting this can cause regional differences in model AOD of up to 0.1 on monthly and annual timescales. The comparison is observed to depend strongly upon thresholds for sparsity of satellite retrievals in the model grid cells. Requiring at least 25% coverage of the model grid cell by satellite data decreases the observed difference between the two by approximately half over land. The impact over ocean is smaller. In both model and satellite datasets, there is an anticorrelation between the proportion p of a model grid cell covered by satellite retrievals and the AOD. This is attributed to small p typically occuring due to high cloud cover and lower AODs being found in large clear-sky regions. Daily median AATSR AODs were found to be closer to GEOS-Chem AODs than daily means (with the root mean squared difference being approximately 0.05 smaller). This is due to the decreased sensitivity of medians to outliers such as cloud-contaminated retrievals, or aerosol point sources not included in the model.
13-month climatology of the aerosol hygroscopicity at the free tropospheric site Jungfraujoch (3580 m a.s.l.)

A hygroscopicity tandem differential mobility analyzer (HTDMA) was operated at the high-alpine site Jungfraujoch in order to characterize the hygroscopic diameter growth factors of the free tropospheric Aitken and accumulation mode aerosol. More than ~5000 h of valid data were collected for the dry diameters D0 = 35, 50, 75, 110, 165, and 265 nm during the 13-month measurement period from 1 May 2008 through 31 May 2009. No distinct seasonal variability of the hygroscopic properties was observed. Annual mean hygroscopic diameter growth factors (D/D0) at 90% relative humidity were found to be 1.34, 1.43, and 1.46 for D0 = 50, 110, and 265 nm, respectively. This size dependence can largely be attributed to the Kelvin effect because corresponding values of the hygroscopicity parameter κ are nearly independent of size. The mean hygroscopicity of the Aitken and accumulation mode aerosol at the free tropospheric site Jungfraujoch was found to be κ≈0.24 with little variability throughout the year. The impact of Saharan dust events, a frequent phenomenon at the Jungfraujoch, on aerosol hygroscopicity was shown to be negligible for D0<265 nm. Thermally driven injections of planetary boundary layer (PBL) air, particularly observed in the early afternoon of summer days with convective anticyclonic weather conditions, lead to a decrease of aerosol hygroscopicity. However, the effect of PBL influence is not seen in the annual mean hygroscopicity data because the effect is small and those conditions (weather class, season and time of day) with PBL influence are relatively rare. Aerosol hygroscopicity was found to be virtually independent of synoptic wind direction during advective weather situations, i.e. when horizontal motion of the atmosphere dominates over thermally driven convection. This indicates that the hygroscopic behavior of the aerosol observed at the Jungfraujoch can be considered representative of the lower free troposphere on at least a regional if not continental scale.
Feedback between dust particles and atmospheric processes over West Africa during dust episodes in March 2006 and June 2007

We used the comprehensive model system COSMO-ART to quantify the impact of mineral dust on the radiative fluxes, the temperature and the feedback between dust particles and their emissions. We simulated two dust storms over West Africa in March 2006 and in June 2007. Simulations with and without coupling of the actual dust concentration with the radiative fluxes and the thermodynamics were carried out for each case. The model results for the 2006 case were compared with observations of the AMMA campaign. At the surface the shortwave radiative effect of mineral dust can be described by a linear relation between the changes in net surface radiation and the aerosol optical depth (AOD). For an AOD at 450 nm of 1 the average shortwave radiation reduction amounts −140 W m−2 during noon. The longwave radiative effect of mineral dust is nonlinear, with an average increase of +70 W m−2 for an AOD (450 nm) of 1. At the top of the atmosphere the effect of the dust layer with an AOD of 1 on radiative fluxes is not as significant as at the surface. It is slightly positive for the shortwave and approximately 26 W m−2 for the longwave radiation. The height range and the extension of the dust layer determine the effect of dust particles on the 2 m temperature. When the dust layer is attached to the surface and lasts for several days it leads to an increase of the surface temperature even during daytime. In case of an elevated dust layer there is a decrease in 2 m temperature of up to 4 K during noon. It is shown, that the temperature changes caused by mineral dust may result in horizontal temperature gradients which also modify near surface winds. Since surface wind thresholds decide the uptake of dust from the surface, a feedback on total emission fluxes is established. The coupled model provides an increase in the total emission fluxes of dust particles by about 16% during the dust storm in March 2006 and 25% during the dust episode in June 2007.
The impact of different nitrous acid sources in the air quality levels of the Iberian Peninsula

Hydroxyl radical (OH) is a primary oxidant in the atmosphere and affects both gas-phase pollutants and particulate matter levels. Nitrous acid (HONO) acts as an important source of OH in the urban atmosphere. Therefore it is important to account accurately for HONO sources within air quality models in order to predict air pollution dynamics. HONO observations in urban areas are characterized by high concentrations at night and low concentrations around midday. Existing gas-phase chemical mechanisms do not reproduce the observed HONO levels, suggesting a lack of sources, such as direct emissions or heterogeneous reactions. Specific HONO emission rates, heterogeneous chemical mechanisms leading to its formation and related kinetics are still unclear. Therefore, most air quality models consider exclusively gas-phase chemistry related to HONO. This work applies the WRF-ARW/HERMES/CMAQ modeling system to quantify the effect of the addition of HONO sources in the predictability of HONO profiles, and its subsequent effect on secondary pollutants formation (mainly O3 and PM2.5). The modeling episode is based on a 2004 severe summertime pollution event in the Iberian Peninsula, using high resolution of 4 × 4 km2. Two different parameterizations for emissions and the hydrolysis of NO2 on wet surfaces are added as HONO sources in the atmosphere. Emissions have the largest impact on HONO levels, especially in urban areas, where they can contribute from 66% to 94% to the HONO peak concentration. Additionally, in urban environments, NO2 hydrolysis on building and vegetation surfaces contributes up to 30% to the HONO peak. Both, the available surface area and the relative humidity must be included as parameters affecting the NO2 hydrolysis kinetics. As a result, NO2 hydrolysis is negligible on aerosol surfaces, due to the small surface area available for reaction, and it is more effective in producing HONO below high relative humidity conditions. The addition of HONO sources affects the concentration of secondary pollutants. In particular, major changes are produced in the early morning, due to the higher OH release via HONO photolysis. Significant changes in PM2.5 concentrations are predicted, that can be 16% (2.6 μg m−3) higher in the new scenarios. When accounting for HONO sources, nitrate levels increase especially in urban areas and sulfates in areas downwind from conventional power plants in the Iberian Peninsula. Also, O3 peak concentrations are slightly affected (from 0.7 to 4 ppb, 1% to 4.5%). The improvement of the HONO sources representation within air quality models produces changes in O3 peak predictions and significantly affects the reaction pathways leading to aerosols formation. Therefore, HONO sources other than gas-phase chemistry should be accurately included within modeling frameworks.
A refinement of the emission data for Kola Peninsula based on inverse dispersion modelling

The study reviews the emission estimates of sulphur oxides (SOx) and primary particulate matter (PM) from the major industrial sources of Kola Peninsula. Analysis of the disagreements between the existing emission inventories for the Kola region combined with forward and inverse ensemble dispersion modelling, analysis of observation time-series and model-measurement comparison showed that the emission of the Nikel metallurgy plant was missing or strongly under-estimated in the major European emission inventories, such as EMEP, EDGAR, TNO-GEMS, and PAREST-MEGAPOLI. In some cases it was misplaced or mis-attributed to other sources of the region. A more consistent inventory of the anthropogenic emissions of SOx and PM has been compiled for the Peninsula, compared with the existing estimates and verified by means of dispersion modelling. In particular, the SILAM model simulations for 2003 and 2006 with the revised emission data showed much smaller under-estimation of SO2 concentrations at 8 Finnish and Norwegian observational stations. For the nearest site to the plant the 10-fold underestimation turned to a 1.5-fold over-prediction. Temporal correlation improved more moderately (up to 45% for concentrations, up to 3 times for deposition). The study demonstrates the value of a combined usage of forward and inverse ensemble modelling for source apportionment in case of limited observational data.
Atmospheric nucleation: highlights of the EUCAARI project and future directions

Within the project EUCAARI (European Integrated project on Aerosol Cloud Climate and Air Quality interactions), atmospheric nucleation was studied by (i) developing and testing new air ion and cluster spectrometers, (ii) conducting homogeneous nucleation experiments for sulphate and organic systems in the laboratory, (iii) investigating atmospheric nucleation mechanism under field conditions, and (iv) applying new theoretical and modelling tools for data interpretation and development of parameterisations. The current paper provides a synthesis of the obtained results and identifies the remaining major knowledge gaps related to atmospheric nucleation. The most important technical achievement of the project was the development of new instruments for measuring sub-3 nm particle populations, along with the extensive application of these instruments in both the laboratory and the field. All the results obtained during EUCAARI indicate that sulphuric acid plays a central role in atmospheric nucleation. However, also vapours other than sulphuric acid are needed to explain the nucleation and the subsequent growth processes, at least in continental boundary layers. Candidate vapours in this respect are some organic compounds, ammonia, and especially amines. Both our field and laboratory data demonstrate that the nucleation rate scales to the first or second power of the nucleating vapour concentration(s). This agrees with the few earlier field observations, but is in stark contrast with classical thermodynamic nucleation theories. The average formation rates of 2-nm particles were found to vary by almost two orders of magnitude between the different EUCAARI sites, whereas the formation rates of charged 2-nm particles varied very little between the sites. Overall, our observations are indicative of frequent, yet moderate, ion-induced nucleation usually outweighed by much stronger neutral nucleation events in the continental lower troposphere. The most concrete outcome of the EUCAARI nucleation studies are the new semi-empirical nucleation rate parameterizations based on field observations, along with updated aerosol formation parameterizations.
Observed 20th century desert dust variability: impact on climate and biogeochemistry

Desert dust perturbs climate by directly and indirectly interacting with incoming solar and outgoing long wave radiation, thereby changing precipitation and temperature, in addition to modifying ocean and land biogeochemistry. While we know that desert dust is sensitive to perturbations in climate and human land use, previous studies have been unable to determine whether humans were increasing or decreasing desert dust in the global average. Here we present observational estimates of desert dust based on paleodata proxies showing a doubling of desert dust during the 20th century over much, but not all the globe. Large uncertainties remain in estimates of desert dust variability over 20th century due to limited data. Using these observational estimates of desert dust change in combination with ocean, atmosphere and land models, we calculate the net radiative effect of these observed changes (top of atmosphere) over the 20th century to be −0.14 ± 0.11 W/m2 (1990–1999 vs. 1905–1914). The estimated radiative change due to dust is especially strong between the heavily loaded 1980–1989 and the less heavily loaded 1955–1964 time periods (−0.57 ± 0.46 W/m2), which model simulations suggest may have reduced the rate of temperature increase between these time periods by 0.11 °C. Model simulations also indicate strong regional shifts in precipitation and temperature from desert dust changes, causing 6 ppm (12 PgC) reduction in model carbon uptake by the terrestrial biosphere over the 20th century. Desert dust carries iron, an important micronutrient for ocean biogeochemistry that can modulate ocean carbon storage; here we show that dust deposition trends increase ocean productivity by an estimated 6% over the 20th century, drawing down an additional 4 ppm (8 PgC) of carbon dioxide into the oceans. Thus, perturbations to desert dust over the 20th century inferred from observations are potentially important for climate and biogeochemistry, and our understanding of these changes and their impacts should continue to be refined.
Atmospheric lifetimes and Ozone Depletion Potentials of trans-1-chloro-3,3,3-trifluoropropylene and trans-1,2-dichloroethylene in a three-dimensional model

The chloroalkenes trans-1-chloro-3,3,3-trifluoropropylene (tCFP) and trans-1,2-dichloroethylene (tDCE) have been proposed as candidate replacements for other compounds in current use that cause concerns regarding potential environmental effects including destruction of stratospheric ozone. Because tCFP and tDCE contain chlorine atoms, the effects of these short-lived compounds on stratospheric ozone must be established. In this study, we derive the atmospheric lifetimes and Ozone Depletion Potentials (ODPs) for tCFP and for tDCE assuming emissions from land surfaces at latitudes 30° N to 60° N using the MOZART 3 three-dimensional model of atmospheric chemistry and physics. 53% of the ozone loss due to tCFP and 98% of the ozone loss due to tDCE take place in the troposphere, rather than in the stratosphere as generally expected from longer-lived chlorocarbons. The atmospheric lifetime of tCFP against chemical reaction is 40.4 days, and its ODP is quite small at 0.00034. The tDCE atmospheric lifetime is 12.7 days, and its ODP is 0.00024, which is the lowest ODP found for any chlorocarbon we have studied. Our study suggests that chlorine from tCFP and tDCE are unlikely to affect ozone at quantities likely to be emitted to the atmosphere.