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Author Correction: Interfacial photochemistry at the ocean surface is a global source of organic vapors and aerosols
2018, Brüggemann, Martin, Hayeck, Nathalie, George, Christian
[no abstract available]
Novel insights on new particle formation derived from a pan-european observing system
2018, Dall’Osto, M., Beddows, D.C.S., Asmi, A., Poulain, L., Hao, L., Freney, E., Allan, J.D., Canagaratna, M., Crippa, M., Bianchi, F., de Leeuw, G., Eriksson, A., Swietlicki, E., Hansson, H.C., Henzing, J.S., Granier, C., Zemankova, K., Laj, P., Onasch, T., Prevot, A., Putaud, J. P., Sellegri, K., Vidal, M., Virtanen, A., Simo, R., Worsnop, D., O’Dowd, C., Kulmala, M., Harrison, Roy M.
The formation of new atmospheric particles involves an initial step forming stable clusters less than a nanometre in size (<~1 nm), followed by growth into quasi-stable aerosol particles a few nanometres (~1-10 nm) and larger (>~10 nm). Although at times, the same species can be responsible for both processes, it is thought that more generally each step comprises differing chemical contributors. Here, we present a novel analysis of measurements from a unique multi-station ground-based observing system which reveals new insights into continental-scale patterns associated with new particle formation. Statistical cluster analysis of this unique 2-year multi-station dataset comprising size distribution and chemical composition reveals that across Europe, there are different major seasonal trends depending on geographical location, concomitant with diversity in nucleating species while it seems that the growth phase is dominated by organic aerosol formation. The diversity and seasonality of these events requires an advanced observing system to elucidate the key processes and species driving particle formation, along with detecting continental scale changes in aerosol formation into the future.
Collocated observations of cloud condensation nuclei, particle size distributions, and chemical composition
2017, Schmale, Julia, Henning, Silvia, Henzing, Bas, Keskinen, Helmi, Sellegri, Karine, Ovadnevaite, Jurgita, Bougiatioti, Aikaterini, Kalivitis, Nikos, Stavroulas, Iasonas, Jefferson, Anne, Park, Minsu, Schlag, Patrick, Kristensson, Adam, Iwamoto, Yoko, Pringle, Kirsty, Reddington, Carly, Aalto, Pasi, Äijälä, Mikko, Baltensperger, Urs, Bialek, Jakub, Birmili, Wolfram, Bukowiecki, Nicolas, Ehn, Mikael, Fjæraa, Ann Mari, Fiebig, Markus, Frank, Göran, Fröhlich, Roman, Frumau, Arnoud, Furuya, Masaki, Hammer, Emanuel, Heikkinen, Liine, Herrmann, Erik, Holzinger, Rupert, Hyono, Hiroyuki, Kanakidou, Maria, Kiendler-Scharr, Astrid, Kinouchi, Kento, Kos, Gerard, Kulmala, Markku, Mihalopoulos, Nikolaos, Motos, Ghislain, Nenes, Athanasios, O’Dowd, Colin, Paramonov, Mikhail, Petäjä, Tuukka, Picard, David, Poulain, Laurent, Prévôt, André Stephan Henry, Slowik, Jay, Sonntag, Andre, Swietlicki, Erik, Svenningsson, Birgitta, Tsurumaru, Hiroshi, Wiedensohler, Alfred, Wittbom, Cerina, Ogren, John A., Matsuki, Atsushi, Yum, Seong Soo, Myhre, Cathrine Lund, Carslaw, Ken, Stratmann, Frank, Gysel, Martin
Cloud condensation nuclei (CCN) number concentrations alongside with submicrometer particle number size distributions and particle chemical composition have been measured at atmospheric observatories of the Aerosols, Clouds, and Trace gases Research InfraStructure (ACTRIS) as well as other international sites over multiple years. Here, harmonized data records from 11 observatories are summarized, spanning 98,677 instrument hours for CCN data, 157,880 for particle number size distributions, and 70,817 for chemical composition data. The observatories represent nine different environments, e.g., Arctic, Atlantic, Pacific and Mediterranean maritime, boreal forest, or high alpine atmospheric conditions. This is a unique collection of aerosol particle properties most relevant for studying aerosol-cloud interactions which constitute the largest uncertainty in anthropogenic radiative forcing of the climate. The dataset is appropriate for comprehensive aerosol characterization (e.g., closure studies of CCN), model-measurement intercomparison and satellite retrieval method evaluation, among others. Data have been acquired and processed following international recommendations for quality assurance and have undergone multiple stages of quality assessment.
Interfacial photochemistry at the ocean surface is a global source of organic vapors and aerosols
2018, Brüggemann, Martin, Hayeck, Nathalie, George, Christian
The surface of the oceans acts as a global sink and source for trace gases and aerosol particles. Recent studies suggest that photochemical reactions at this air/water interface produce organic vapors, enhancing particle formation in the atmosphere. However, current model calculations neglect this abiotic source of reactive compounds and account only for biological emissions. Here we show that interfacial photochemistry serves as a major abiotic source of volatile organic compounds (VOCs) on a global scale, capable to compete with emissions from marine biology. Our results indicate global emissions of 46.4-184 Tg C yr-1 of organic vapors from the oceans into the marine atmosphere and a potential contribution to organic aerosol mass of more than 60% over the remote ocean. Moreover, we provide global distributions of VOC formation potentials, which can be used as simple tools for field studies to estimate photochemical VOC emissions depending on location and season.
Intercomparison of in-situ aircraft and satellite aerosol measurements in the stratosphere
2019, Sandvik, Oscar S., Friberg, Johan, Martinsson, Bengt G., van Velthoven, Peter F. J., Hermann, Markus, Zahn, Andreas
Aerosol composition and optical scattering from particles in the lowermost stratosphere (LMS) have been studied by comparing in-situ aerosol samples from the IAGOS-CARIBIC passenger aircraft with vertical profiles of aerosol backscattering obtained from the CALIOP lidar aboard the CALIPSO satellite. Concentrations of the dominating fractions of the stratospheric aerosol, being sulphur and carbon, have been obtained from post-flight analysis of IAGOS-CARIBIC aerosol samples. This information together with literature data on black carbon concentrations were used to calculate the aerosol backscattering which subsequently is compared with measurements by CALIOP. Vertical optical profiles were taken in an altitude range of several kilometres from and above the northern hemispheric extratropical tropopause for the years 2006-2014. We find that the two vastly different measurement platforms yield different aerosol backscattering, especially close to the tropopause where the influence from tropospheric aerosol is strong. The best agreement is found when the LMS is affected by volcanism, i.e., at elevated aerosol loadings. At background conditions, best agreement is obtained some distance (>2 km) above the tropopause in winter and spring, i.e., at likewise elevated aerosol loadings from subsiding aerosol-rich stratospheric air. This is to our knowledge the first time the CALIPSO lidar measurements have been compared to in-situ long-term aerosol measurements. © 2019, The Author(s).
Direct estimation of the global distribution of vertical velocity within cirrus clouds
2017, Barahona, Donifan, Molod, Andrea, Kalesse, Heike
Cirrus clouds determine the radiative balance of the upper troposphere and the transport of water vapor across the tropopause. The representation of vertical wind velocity, W, in atmospheric models constitutes the largest source of uncertainty in the calculation of the cirrus formation rate. Using global atmospheric simulations with a spatial resolution of 7 km we obtain for the first time a direct estimate of the distribution of W at the scale relevant for cirrus formation, validated against long-term observations at two different ground sites. The standard deviation in W, σ w, varies widely over the globe with the highest values resulting from orographic uplift and convection, and the lowest occurring in the Arctic. Globally about 90% of the simulated σ w values are below 0.1 m s-1 and about one in 104 cloud formation events occur in environments with σ w > 0.8 m s-1. Combining our estimate with reanalysis products and an advanced cloud formation scheme results in lower homogeneous ice nucleation frequency than previously reported, and a decreasing average ice crystal concentration with decreasing temperature. These features are in agreement with observations and suggest that the correct parameterization of σ w is critical to simulate realistic cirrus properties.
Strong impact of wildfires on the abundance and aging of black carbon in the lowermost stratosphere
2018, Ditas, Jeannine, Ma, Nan, Zhang, Yuxuan, Assmann, Denise, Neumaier, Marco, Riede, Hella, Karu, Einar, Williams, Jonathan, Scharffe, Dieter, Wang, Qiaoqiao, Saturno, Jorge, Schwarz, Joshua P., Katich, Joseph M., McMeeking, Gavin R., Zahn, Andreas, Hermann, Markus, Brenninkmeijer, Carl A. M., Andreae, Meinrat O., Pöschl, Ulrich, Su, Hang, Cheng, Yafang
Wildfires inject large amounts of black carbon (BC) particles into the atmosphere, which can reach the lowermost stratosphere (LMS) and cause strong radiative forcing. During a 14-month period of observations on board a passenger aircraft flying between Europe and North America, we found frequent and widespread biomass burning (BB) plumes, influencing 16 of 160 flight hours in the LMS. The average BC mass concentrations in these plumes (∼140 ng·m−3, standard temperature and pressure) were over 20 times higher than the background concentration (∼6 ng·m−3) with more than 100-fold enhanced peak values (up to ∼720 ng·m−3). In the LMS, nearly all BC particles were covered with a thick coating. The average mass equivalent diameter of the BC particle cores was ∼120 nm with a mean coating thickness of ∼150 nm in the BB plume and ∼90 nm with a coating of ∼125 nm in the background. In a BB plume that was encountered twice, we also found a high diameter growth rate of ∼1 nm·h−1 due to the BC particle coatings. The observed high concentrations and thick coatings of BC particles demonstrate that wildfires can induce strong local heating in the LMS and may have a significant influence on the regional radiative forcing of climate.