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- ItemStudying the vertical aerosol extinction coefficient by comparing in situ airborne data and elastic backscatter lidar(München : European Geopyhsical Union, 2016) Rosati, Bernadette; Herrmann, Erik; Bucci, Silvia; Fierli, Federico; Cairo, Francesco; Gysel, Martin; Tillmann, Ralf; Größ, Johannes; Gobbi, Gian Paolo; Liberto, Luca Di; Di Donfrancesco, Guido; Wiedensohler, Alfred; Weingartner, Ernest; Virtanen, Annele; Mentel, Thomas F.; Baltensperger, UrsVertical profiles of aerosol particle optical properties were explored in a case study near the San Pietro Capofiume (SPC) ground station during the PEGASOS Po Valley campaign in the summer of 2012. A Zeppelin NT airship was employed to investigate the effect of the dynamics of the planetary boundary layer at altitudes between ∼ 50 and 800 m above ground. Determined properties included the aerosol particle size distribution, the hygroscopic growth factor, the effective index of refraction and the light absorption coefficient. The first three parameters were used to retrieve the light scattering coefficient. Simultaneously, direct measurements of both the scattering and absorption coefficient were carried out at the SPC ground station. Additionally, a single wavelength polarization diversity elastic lidar system provided estimates of aerosol extinction coefficients using the Klett method to accomplish the inversion of the signal, for a vertically resolved comparison between in situ and remote-sensing results. Note, however, that the comparison was for the most part done in the altitude range where the overlap function is incomplete and accordingly uncertainties are larger. First, the airborne results at low altitudes were validated with the ground measurements. Agreement within approximately ±25 and ±20 % was found for the dry scattering and absorption coefficient, respectively. The single scattering albedo, ranged between 0.83 and 0.95, indicating the importance of the absorbing particles in the Po Valley region. A clear layering of the atmosphere was observed during the beginning of the flight (until ∼ 10:00 LT – local time) before the mixing layer (ML) was fully developed. Highest extinction coefficients were found at low altitudes, in the new ML, while values in the residual layer, which could be probed at the beginning of the flight at elevated altitudes, were lower. At the end of the flight (after ∼ 12:00 LT) the ML was fully developed, resulting in constant extinction coefficients at all altitudes measured on the Zeppelin NT. Lidar estimates captured these dynamic features well and good agreement was found for the extinction coefficients compared to the in situ results, using fixed lidar ratios (LR) between 30 and 70 sr for the altitudes probed with the Zeppelin. These LR are consistent with values for continental aerosol particles that can be expected in this region.
- ItemVertical profiling of aerosol hygroscopic properties in the planetary boundary layer during the PEGASOS campaigns(München : European Geopyhsical Union, 2016) Rosati, Bernadette; Gysel, Martin; Rubach, Florian; Mentel, Thomas F.; Goger, Brigitta; Poulain, Laurent; Schlag, Patrick; Miettinen, Pasi; Pajunoja, Aki; Virtanen, Annele; Baltink, Henk Klein; Henzing, J.S. Bas; Größ, Johannes; Gobbi, Gian Paolo; Wiedensohler, Alfred; Kiendler-Scharr, Astrid; Decesari, Stefano; Facchini, Maria Cristina; Weingartner, Ernest; Baltensperger, UrsVertical profiles of the aerosol particles hygroscopic properties, their mixing state as well as chemical composition were measured above northern Italy and the Netherlands. An aerosol mass spectrometer (AMS; for chemical composition) and a white-light humidified optical particle spectrometer (WHOPS; for hygroscopic growth) were deployed on a Zeppelin NT airship within the PEGASOS project. This allowed one to investigate the development of the different layers within the planetary boundary layer (PBL), providing a unique in situ data set for airborne aerosol particles properties in the first kilometre of the atmosphere. Profiles measured during the morning hours on 20 June 2012 in the Po Valley, Italy, showed an increased nitrate fraction at ∼ 100 m above ground level (a.g.l.) coupled with enhanced hygroscopic growth compared to ∼ 700 m a. g. l. This result was derived from both measurements of the aerosol composition and direct measurements of the hygroscopicity, yielding hygroscopicity parameters (κ) of 0.34 ± 0.12 and 0.19 ± 0.07 for 500 nm particles, at ∼ 100 and ∼ 700 m a. g. l., respectively. The difference is attributed to the structure of the PBL at this time of day which featured several independent sub-layers with different types of aerosols. Later in the day the vertical structures disappeared due to the mixing of the layers and similar aerosol particle properties were found at all probed altitudes (mean κ ≈ 0.18 ± 0.07). The aerosol properties observed at the lowest flight level (100 m a. g. l.) were consistent with parallel measurements at a ground site, both in the morning and afternoon. Overall, the aerosol particles were found to be externally mixed, with a prevailing hygroscopic fraction. The flights near Cabauw in the Netherlands in the fully mixed PBL did not feature altitude-dependent characteristics. Particles were also externally mixed and had an even larger hygroscopic fraction compared to the results in Italy. The mean κ from direct measurements was 0.28 ± 0.10, thus considerably higher than κ values measured in Italy in the fully mixed PBL.
- ItemHeterogeneous ice nucleation of viscous secondary organic aerosol produced from ozonolysis of α-pinene(München : European Geopyhsical Union, 2016) Ignatius, Karoliina; Kristensen, Thomas B.; Järvinen, Emma; Nichman, Leonid; Fuchs, Claudia; Gordon, Hamish; Herenz, Paul; Hoyle, Christopher R.; Duplissy, Jonathan; Garimella, Sarvesh; Dias, Antonio; Frege, Carla; Höppel, Niko; Tröstl, Jasmin; Wagner, Robert; Yan, Chao; Amorim, Antonio; Baltensperger, Urs; Curtius, Joachim; Donahue, Neil M.; Gallagher, Martin W.; Kirkby, Jasper; Kulmala, Markku; Möhler, Ottmar; Saathoff, Harald; Schnaiter, Martin; Dulac, François; Tomé, Antonio; Virtanen, Annele; Worsnop, Douglas; Stratmann, FrankThere are strong indications that particles containing secondary organic aerosol (SOA) exhibit amorphous solid or semi-solid phase states in the atmosphere. This may facilitate heterogeneous ice nucleation and thus influence cloud properties. However, experimental ice nucleation studies of biogenic SOA are scarce. Here, we investigated the ice nucleation ability of viscous SOA particles. The SOA particles were produced from the ozone initiated oxidation of α-pinene in an aerosol chamber at temperatures in the range from −38 to −10 °C at 5–15 % relative humidity with respect to water to ensure their formation in a highly viscous phase state, i.e. semi-solid or glassy. The ice nucleation ability of SOA particles with different sizes was investigated with a new continuous flow diffusion chamber. For the first time, we observed heterogeneous ice nucleation of viscous α-pinene SOA for ice saturation ratios between 1.3 and 1.4 significantly below the homogeneous freezing limit. The maximum frozen fractions found at temperatures between −39.0 and −37.2 °C ranged from 6 to 20 % and did not depend on the particle surface area. Global modelling of monoterpene SOA particles suggests that viscous biogenic SOA particles are indeed present in regions where cirrus cloud formation takes place. Hence, they could make up an important contribution to the global ice nucleating particle budget.
- ItemObservation of viscosity transition in α-pinene secondary organic aerosol(München : European Geopyhsical Union, 2016) Järvinen, Emma; Ignatius, Karoliina; Nichman, Leonid; Kristensen, Thomas B.; Fuchs, Claudia; Hoyle, Christopher R.; Höppel, Niko; Corbin, Joel C.; Craven, Jill; Duplissy, Jonathan; Ehrhart, Sebastian; El Haddad, Imad; Frege, Carla; Gordon, Hamish; Jokinen, Tuija; Kallinger, Peter; Kirkby, Jasper; Kiselev, Alexei; Naumann, Karl-Heinz; Petäjä, Tuukka; Pinterich, Tamara; Prevot, Andre S.H.; Saathoff, Harald; Schiebel, Thea; Sengupta, Kamalika; Simon, Mario; Slowik, Jay G.; Tröstl, Jasmin; Virtanen, Annele; Vochezer, Paul; Vogt, Steffen; Wagner, Andrea C.; Wagner, Robert; Williamson, Christina; Winkler, Paul M.; Yan, Chao; Baltensperger, Urs; Donahue, Neil M.; Flagan, Rick C.; Gallagher, Martin; Hansel, Armin; Kulmala, Markku; Stratmann, Frank; Worsnop, Douglas R.; Möhler, Ottmar; Leisner, Thomas; Schnaiter, MartinUnder certain conditions, secondary organic aerosol (SOA) particles can exist in the atmosphere in an amorphous solid or semi-solid state. To determine their relevance to processes such as ice nucleation or chemistry occurring within particles requires knowledge of the temperature and relative humidity (RH) range for SOA to exist in these states. In the Cosmics Leaving Outdoor Droplets (CLOUD) experiment at The European Organisation for Nuclear Research (CERN), we deployed a new in situ optical method to detect the viscous state of α-pinene SOA particles and measured their transition from the amorphous highly viscous state to states of lower viscosity. The method is based on the depolarising properties of laboratory-produced non-spherical SOA particles and their transformation to non-depolarising spherical particles at relative humidities near the deliquescence point. We found that particles formed and grown in the chamber developed an asymmetric shape through coagulation. A transition to a spherical shape was observed as the RH was increased to between 35 % at −10 °C and 80 % at −38 °C, confirming previous calculations of the viscosity-transition conditions. Consequently, α-pinene SOA particles exist in a viscous state over a wide range of ambient conditions, including the cirrus region of the free troposphere. This has implications for the physical, chemical, and ice-nucleation properties of SOA and SOA-coated particles in the atmosphere.
- ItemEvaluation of European air quality modelled by CAMx including the volatility basis set scheme(München : European Geopyhsical Union, 2016) Ciarelli, Giancarlo; Aksoyoglu, Sebnem; Crippa, Monica; Jimenez, Jose-Luis; Nemitz, Eriko; Sellegri, Karine; Äijälä, Mikko; Carbone, Samara; Mohr, Claudia; O'Dowd, Colin; Poulain, Laurent; Baltensperger, Urs; Prévôt, André S.H.Four periods of EMEP (European Monitoring and Evaluation Programme) intensive measurement campaigns (June 2006, January 2007, September–October 2008 and February–March 2009) were modelled using the regional air quality model CAMx with VBS (volatility basis set) approach for the first time in Europe within the framework of the EURODELTA-III model intercomparison exercise. More detailed analysis and sensitivity tests were performed for the period of February–March 2009 and June 2006 to investigate the uncertainties in emissions as well as to improve the modelling of organic aerosol (OA). Model performance for selected gas phase species and PM2.5 was evaluated using the European air quality database AirBase. Sulfur dioxide (SO2) and ozone (O3) were found to be overestimated for all the four periods, with O3 having the largest mean bias during June 2006 and January–February 2007 periods (8.9 pbb and 12.3 ppb mean biases respectively). In contrast, nitrogen dioxide (NO2) and carbon monoxide (CO) were found to be underestimated for all the four periods. CAMx reproduced both total concentrations and monthly variations of PM2.5 for all the four periods with average biases ranging from −2.1 to 1.0 µg m−3. Comparisons with AMS (aerosol mass spectrometer) measurements at different sites in Europe during February–March 2009 showed that in general the model overpredicts the inorganic aerosol fraction and underpredicts the organic one, such that the good agreement for PM2.5 is partly due to compensation of errors. The effect of the choice of VBS scheme on OA was investigated as well. Two sensitivity tests with volatility distributions based on previous chamber and ambient measurements data were performed. For February–March 2009 the chamber case reduced the total OA concentrations by about 42 % on average. In contrast, a test based on ambient measurement data increased OA concentrations by about 42 % for the same period bringing model and observations into better agreement. Comparison with the AMS data at the rural Swiss site Payerne in June 2006 shows no significant improvement in modelled OA concentration. Further sensitivity tests with increased biogenic and anthropogenic emissions suggest that OA in Payerne was affected by changes in emissions from residential heating during the February–March 2009 whereas it was more sensitive to biogenic precursors in June 2006.