2012, Setyan, A., Zhang, Q., Merkel, M., Knighton, W.B., Sun, Y., Song, C., Shilling, J.E., Onasch, T.B., Herndon, S.C., Worsnop, D.R., Fast, J.D., Zaveri, R.A., Berg, L.K., Wiedensohler, A., Flowers, B.A., Dubey, M.K., Subramanian, R.

An Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed during the Carbonaceous Aerosols and Radiative Effects Study (CARES) that took place in northern California in June 2010. We present results obtained at Cool (denoted as the T1 site of the project) in the foothills of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. During this study, the average mass loading of submicrometer particles (PM1) was 3.0 μg m−3, dominated by organics (80%) and sulfate (9.9%). The organic aerosol (OA) had a nominal formula of C1H1.38N0.004OM0.44, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two distinct oxygenated OA factors were identified via Positive matrix factorization (PMF) of the high-resolution mass spectra of organics. The more oxidized MO-OOA (O/C = 0.54) was interpreted as a surrogate for secondary OA (SOA) influenced by biogenic emissions whereas the less oxidized LO-OOA (O/C = 0.42) was found to represent SOA formed in photochemically processed urban emissions. LO-OOA correlated strongly with ozone and MO-OOA correlated well with two 1st generation isoprene oxidation products (methacrolein and methyl vinyl ketone), indicating that both SOAs were relatively fresh. A hydrocarbon like OA (HOA) factor was also identified, representing primary emissions mainly due to local traffic. On average, SOA (= MO-OOA + LO-OOA) accounted for 91% of the total OA mass and 72% of the PM1 mass observed at Cool. Twenty three periods of urban plumes from T0 (Sacramento) to T1 (Cool) were identified using the Weather Research and Forecasting model coupled with Chemistry (WRF-Chem). The average PM1 mass loading was considerably higher in urban plumes than in air masses dominated by biogenic SOA. The change in OA mass relative to CO (ΔOA/ΔCO) varied in the range of 5-196 μg m−3 ppm−1, reflecting large variability in SOA production. The highest ΔOA/ΔCO was reached when air masses were dominated by anthropogenic emissions in the presence of a high concentration of biogenic volatile organic compounds (BVOCs). This ratio, which was 97 μg m−3 ppm−1 on average, was much higher than when urban plumes arrived in a low BVOC environment (~36 μg m−3 ppm−1) or during other periods dominated by biogenic SOA (35 μg m−3 ppm−1). These results demonstrate that SOA formation is enhanced when anthropogenic emissions interact with biogenic precursors.

2017, Schrod, Jann, Weber, Daniel, Drücke, Jaqueline, Keleshis, Christos, Pikridas, Michael, Ebert, Martin, Cvetković, Bojan, Nickovic, Slobodan, Marinou, Eleni, Baars, Holger, Ansmann, Albert, Vrekoussis, Mihalis, Mihalopoulos, Nikos, Sciare, Jean, Curtius, Joachim, Bingemer, Heinz G.

During an intensive field campaign on aerosol, clouds, and ice nucleation in the Eastern Mediterranean in April 2016, we measured the abundance of ice nucleating particles (INPs) in the lower troposphere from unmanned aircraft systems (UASs). Aerosol samples were collected by miniaturized electrostatic precipitators onboard the UASs at altitudes up to 2.5 km. The number of INPs in these samples, which are active in the deposition and condensation modes at temperatures from -20 to -30 °C, were analyzed immediately after collection on site using the ice nucleus counter FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment). During the 1-month campaign, we encountered a series of Saharan dust plumes that traveled at several kilometers' altitude. Here we present INP data from 42 individual flights, together with aerosol number concentrations, observations of lidar backscattering, dust concentrations derived by the dust transport model DREAM (Dust Regional Atmospheric Model), and results from scanning electron microscopy. The effect of the dust plumes is reflected by the coincidence of INPs with the particulate matter (PM), the lidar signal, and the predicted dust mass of the model. This suggests that mineral dust or a constituent related to dust was a major contributor to the ice nucleating properties of the aerosol. Peak concentrations of above 100 INPs std L-1 were measured at -30 °C. The INP concentration in elevated plumes was on average a factor of 10 higher than at ground level. Since desert dust is transported for long distances over wide areas of the globe predominantly at several kilometers' altitude, we conclude that INP measurements at ground level may be of limited significance for the situation at the level of cloud formation.

2014, Setyan, A., Song, C., Merkel, M., Knighton, W.B., Onasch, T.B., Canagaratna, M.R., Worsnop, D.R., Wiedensohler, A., Shilling, J.E., Zhang, Q.

Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, Dm, measured by a mobility particle size spectrometer operating in the range 10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h−1) than at T1 (6.2 ± 2.5 nm h−1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+, C2H3N+, and C2H4N+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NOx, and toluene) were significantly higher whereas the photo-oxidation products of biogenic VOCs (volatile organic compounds) and the biogenically influenced SOA also increased moderately during the NPE days compared to the non-event days. These results indicate that the frequently occurring NPEs over the Sacramento and Sierra Nevada regions were mainly driven by urban plumes from Sacramento and the San Francisco Bay Area, and that the interaction of regional biogenic emissions with the urban plumes has enhanced the new particle growth. This finding has important implications for quantifying the climate impacts of NPEs on global scale.

2015, Pikridas, M., Sciare, J., Freutel, F., Crumeyrolle, S., von der Weiden-Reinmüller, S.-L., Borbon, A., Schwarzenboeck, A., Merkel, M., Crippa, M., Kostenidou, E., Psichoudaki, M., Hildebrandt, L., Engelhart, G.J., Petäjä, T., Prévôt, A.S.H., Drewnick, F., Baltensperger, U., Wiedensohler, A., Kulmala, M., Beekmann, M., Pandis, S.N.

Ambient particle number size distributions were measured in Paris, France, during summer (1–31 July 2009) and winter (15 January to 15 February 2010) at three fixed ground sites and using two mobile laboratories and one airplane. The campaigns were part of the Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation (MEGAPOLI) project. New particle formation (NPF) was observed only during summer on approximately 50 % of the campaign days, assisted by the low condensation sink (about 10.7 ± 5.9 × 10−3 s−1). NPF events inside the Paris plume were also observed at 600 m altitude onboard an aircraft simultaneously with regional events identified on the ground. Increased particle number concentrations were measured aloft also outside of the Paris plume at the same altitude, and were attributed to NPF. The Paris plume was identified, based on increased particle number and black carbon concentration, up to 200 km away from the Paris center during summer. The number concentration of particles with diameters exceeding 2.5 nm measured on the surface at the Paris center was on average 6.9 ± 8.7 × 104 and 12.1 ± 8.6 × 104 cm−3 during summer and winter, respectively, and was found to decrease exponentially with distance from Paris. However, further than 30 km from the city center, the particle number concentration at the surface was similar during both campaigns. During summer, one suburban site in the NE was not significantly affected by Paris emissions due to higher background number concentrations, while the particle number concentration at the second suburban site in the SW increased by a factor of 3 when it was downwind of Paris.

2018, Bohlmann, S., Baars, H., Radenz, M., Engelmann, R., Macke, A.

The multi-wavelength Raman lidar PollyXT has been regularly operated aboard the research vessel Polarstern on expeditions across the Atlantic Ocean from north to south and vice versa. The lidar measurements of the RV Polarstern cruises PS95 from Bremerhaven, Germany, to Cape Town, Republic of South Africa (November 2015), and PS98 from Punta Arenas, Chile, to Bremerhaven, Germany (April/May 2016), are presented and analysed in detail. The latest set-up of PollyXT allows improved coverage of the marine boundary layer (MBL) due to an additional near-range receiver. Three case studies provide an overview of the aerosol detected over the Atlantic Ocean. In the first case, marine conditions were observed near South Africa on the autumn cruise PS95. Values of optical properties (depolarisation ratios close to zero, lidar ratios of 23 sr at 355 and 532 nm) within the MBL indicate pure marine aerosol. A layer of dried marine aerosol, indicated by an increase of the particle depolarisation ratio to about 10% at 355 nm (9% at 532 nm) and thus confirming the non-sphericity of these particles, could be detected on top of the MBL. On the same cruise, an almost pure Saharan dust plume was observed near the Canary Islands, presented in the second case. The third case deals with several layers of Saharan dust partly mixed with biomass-burning smoke measured on PS98 near the Cabo Verde islands. While the MBL was partly mixed with dust in the pure Saharan dust case, an almost marine MBL was observed in the third case. A statistical analysis showed latitudinal differences in the optical properties within the MBL, caused by the downmixing of dust in the tropics and anthropogenic influences in the northern latitudes, whereas the optical properties of the MBL in the Southern Hemisphere correlate with typical marine values. The particle depolarisation ratio of dried marine layers ranged between 4 and 9% at 532 nm. Night measurements from PS95 and PS98 were used to illustrate the potential of aerosol classification using lidar ratio, particle depolarisation ratio at 355 and 532 nm, and Angström exponent. Lidar ratio and particle depolarisation ratio have been found to be the main indicator for particle type, whereas the Ångström exponent is rather variable.