2016, Brock, Charles A., Wagner, Nicholas L., Anderson, Bruce E., Attwood, Alexis R., Beyersdorf, Andreas, Campuzano-Jost, Pedro, Carlton, Annmarie G., Day, Douglas A., Diskin, Glenn S., Gordon, Timothy D., Jimenez, Jose L., Lack, Daniel A., Liao, Jin, Markovic, Milos Z., Middlebrook, Ann M., Ng, Nga L., Perring, Anne E., Richardson, Matthews S., Schwarz, Joshua P., Washenfelder, Rebecca A., Welti, Andre, Xu, Lu, Ziemba, Luke D., Murphy, Daniel M.

Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of  ∼  25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction.

2015, Kim, P.S., Jacob, D.J., Fisher, J.A., Travis, K., Yu, K., Zhu, L., Yantosca, R.M., Sulprizio, M.P., Jimenez, J.L., Campuzano-Jost, P., Froyd, K.D., Liao, J., Hair, J.W., Fenn, M.A., Butler, C.F., Wagner, N.L., Gordon, T.D., Welti, A., Wennberg, P.O., Crounse, J.D., St. Clair, J.M., Teng, A.P., Millet, D.B., Schwarz, J.P., Markovic, M.Z., Perring, A.E.

We use an ensemble of surface (EPA CSN, IMPROVE, SEARCH, AERONET), aircraft (SEAC4RS), and satellite (MODIS, MISR) observations over the southeast US during the summer–fall of 2013 to better understand aerosol sources in the region and the relationship between surface particulate matter (PM) and aerosol optical depth (AOD). The GEOS-Chem global chemical transport model (CTM) with 25 × 25 km2 resolution over North America is used as a common platform to interpret measurements of different aerosol variables made at different times and locations. Sulfate and organic aerosol (OA) are the main contributors to surface PM2.5 (mass concentration of PM finer than 2.5 μm aerodynamic diameter) and AOD over the southeast US. OA is simulated successfully with a simple parameterization, assuming irreversible uptake of low-volatility products of hydrocarbon oxidation. Biogenic isoprene and monoterpenes account for 60 % of OA, anthropogenic sources for 30 %, and open fires for 10 %. 60 % of total aerosol mass is in the mixed layer below 1.5 km, 25 % in the cloud convective layer at 1.5–3 km, and 15 % in the free troposphere above 3 km. This vertical profile is well captured by GEOS-Chem, arguing against a high-altitude source of OA. The extent of sulfate neutralization (f = [NH4+]/(2[SO42−] + [NO3−]) is only 0.5–0.7 mol mol−1 in the observations, despite an excess of ammonia present, which could reflect suppression of ammonia uptake by OA. This would explain the long-term decline of ammonium aerosol in the southeast US, paralleling that of sulfate. The vertical profile of aerosol extinction over the southeast US follows closely that of aerosol mass. GEOS-Chem reproduces observed total column aerosol mass over the southeast US within 6 %, column aerosol extinction within 16 %, and space-based AOD within 8–28 % (consistently biased low). The large AOD decline observed from summer to winter is driven by sharp declines in both sulfate and OA from August to October. These declines are due to shutdowns in both biogenic emissions and UV-driven photochemistry. Surface PM2.5 shows far less summer-to-winter decrease than AOD and we attribute this in part to the offsetting effect of weaker boundary layer ventilation. The SEAC4RS aircraft data demonstrate that AODs measured from space are consistent with surface PM2.5. This implies that satellites can be used reliably to infer surface PM2.5 over monthly timescales if a good CTM representation of the aerosol vertical profile is available.

2016, Boose, Yvonne, Welti, André, Atkinson, James, Ramelli, Fabiola, Danielczok, Anja, Bingemer, Heinz G., Plötze, Michael, Sierau, Berko, Kanji, Zamin A., Lohmann, Ulrike

Desert dust is one of the most abundant ice nucleating particle types in the atmosphere. Traditionally, clay minerals were assumed to determine the ice nucleation ability of desert dust and constituted the focus of ice nucleation studies over several decades. Recently some feldspar species were identified to be ice active at much higher temperatures than clay minerals, redirecting studies to investigate the contribution of feldspar to ice nucleation on desert dust. However, so far no study has shown the atmospheric relevance of this mineral phase. For this study four dust samples were collected after airborne transport in the troposphere from the Sahara to different locations (Crete, the Peloponnese, Canary Islands, and the Sinai Peninsula). Additionally, 11 dust samples were collected from the surface from nine of the biggest deserts worldwide. The samples were used to study the ice nucleation behavior specific to different desert dusts. Furthermore, we investigated how representative surface-collected dust is for the atmosphere by comparing to the ice nucleation activity of the airborne samples. We used the IMCA-ZINC setup to form droplets on single aerosol particles which were subsequently exposed to temperatures between 233 and 250 K. Dust particles were collected in parallel on filters for offline cold-stage ice nucleation experiments at 253–263 K. To help the interpretation of the ice nucleation experiments the mineralogical composition of the dusts was investigated. We find that a higher ice nucleation activity in a given sample at 253 K can be attributed to the K-feldspar content present in this sample, whereas at temperatures between 238 and 245 K it is attributed to the sum of feldspar and quartz content present. A high clay content, in contrast, is associated with lower ice nucleation activity. This confirms the importance of feldspar above 250 K and the role of quartz and feldspars determining the ice nucleation activities at lower temperatures as found by earlier studies for monomineral dusts. The airborne samples show on average a lower ice nucleation activity than the surface-collected ones. Furthermore, we find that under certain conditions milling can lead to a decrease in the ice nucleation ability of polymineral samples due to the different hardness and cleavage of individual mineral phases causing an increase of minerals with low ice nucleation ability in the atmospherically relevant size fraction. Comparison of our data set to an existing desert dust parameterization confirms its applicability for climate models. Our results suggest that for an improved prediction of the ice nucleation ability of desert dust in the atmosphere, the modeling of emission and atmospheric transport of the feldspar and quartz mineral phases would be key, while other minerals are only of minor importance.

2016, Chaboureau, Jean-Pierre, Flamant, Cyrille, Dauhut, Thibaut, Kocha, Cécile, Lafore, Jean-Philippe, Lavaysse, Chistophe, Marnas, Fabien, Mokhtari, Mohamed, Pelon, Jacques, Reinares Martínez, Irene, Schepanski, Kerstin, Tulet, Pierre

In the framework of the Fennec international programme, a field campaign was conducted in June 2011 over the western Sahara. It led to the first observational data set ever obtained that documents the dynamics, thermodynamics and composition of the Saharan atmospheric boundary layer (SABL) under the influence of the heat low. In support to the aircraft operation, four dust forecasts were run daily at low and high resolutions with convection-parameterizing and convection-permitting models, respectively. The unique airborne and ground-based data sets allowed the first ever intercomparison of dust forecasts over the western Sahara. At monthly scale, large aerosol optical depths (AODs) were forecast over the Sahara, a feature observed by satellite retrievals but with different magnitudes. The AOD intensity was correctly predicted by the high-resolution models, while it was underestimated by the low-resolution models. This was partly because of the generation of strong near-surface wind associated with thunderstorm-related density currents that could only be reproduced by models representing convection explicitly. Such models yield emissions mainly in the afternoon that dominate the total emission over the western fringes of the Adrar des Iforas and the Aïr Mountains in the high-resolution forecasts. Over the western Sahara, where the harmattan contributes up to 80 % of dust emission, all the models were successful in forecasting the deep well-mixed SABL. Some of them, however, missed the large near-surface dust concentration generated by density currents and low-level winds. This feature, observed repeatedly by the airborne lidar, was partly forecast by one high-resolution model only.