2014, Crippa, M., Canonaco, F., Lanz, V.A., Äijälä, M., Allan, J.D., Carbone, S., Capes, G., Ceburnis, D., Dall'Osto, M., Day, D.A., DeCarlo, P.F., Ehn, M., Eriksson, A., Freney, E., Hildebrandt Ruiz, L., Hillamo, R., Jimenez, J.L., Junninen, H., Kiendler-Scharr, A., Kortelainen, A.-M., Kulmala, M., Laaksonen, A., Mensah, A.A., Mohr, C., Nemitz, E., O'Dowd, C., Ovadnevaite, J., Pandis, S.N., Petäjä, T., Poulain, L., Saarikoski, S., Sellegri, K., Swietlicki, E., Tiitta, P., Worsnop, D.R., Baltensperger, U., Prévôt, A.S.H.

Organic aerosols (OA) represent one of the major constituents of submicron particulate matter (PM1) and comprise a huge variety of compounds emitted by different sources. Three intensive measurement field campaigns to investigate the aerosol chemical composition all over Europe were carried out within the framework of the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) and the intensive campaigns of European Monitoring and Evaluation Programme (EMEP) during 2008 (May–June and September–October) and 2009 (February–March). In this paper we focus on the identification of the main organic aerosol sources and we define a standardized methodology to perform source apportionment using positive matrix factorization (PMF) with the multilinear engine (ME-2) on Aerodyne aerosol mass spectrometer (AMS) data. Our source apportionment procedure is tested and applied on 25 data sets accounting for two urban, several rural and remote and two high altitude sites; therefore it is likely suitable for the treatment of AMS-related ambient data sets. For most of the sites, four organic components are retrieved, improving significantly previous source apportionment results where only a separation in primary and secondary OA sources was possible. Generally, our solutions include two primary OA sources, i.e. hydrocarbon-like OA (HOA) and biomass burning OA (BBOA) and two secondary OA components, i.e. semi-volatile oxygenated OA (SV-OOA) and low-volatility oxygenated OA (LV-OOA). For specific sites cooking-related (COA) and marine-related sources (MSA) are also separated. Finally, our work provides a large overview of organic aerosol sources in Europe and an interesting set of highly time resolved data for modeling purposes.

2014, Schladitz, A., Merkel, M., Bastian, S., Birmili, W., Weinhold, K., Löschau, G., Wiedensohler, A.

An automated function control unit was developed to regularly check the ambient particle number concentration derived from a mobility particle size spectrometer as well as its zero-point behaviour. The function control allows unattended quality assurance experiments at remote air quality monitoring or research stations under field conditions. The automated function control also has the advantage of being able to get a faster system stability response than the recommended on-site comparisons with reference instruments. The method is based on a comparison of the total particle number concentration measured by a mobility particle size spectrometer and a condensation particle counter while removing diffusive particles smaller than 20 nm in diameter. In practice, the small particles are removed by a set of diffusion screens, as traditionally used in a diffusion battery. Another feature of the automated function control is to check the zero-point behaviour of the ambient aerosol passing through a high-efficiency particulate air (HEPA) filter. The performance of the function control is illustrated with the aid of a 1-year data set recorded at Annaberg-Buchholz, a station in the Saxon air quality monitoring network. During the period of concern, the total particle number concentration derived from the mobility particle size spectrometer slightly overestimated the particle number concentration recorded by the condensation particle counter by 2 % (grand average). Based on our first year of experience with the function control, we developed tolerance criteria that allow a performance evaluation of a tested mobility particle size spectrometer with respect to the total particle number concentration. We conclude that the automated function control enhances the quality and reliability of unattended long-term particle number size distribution measurements. This will have beneficial effects for intercomparison studies involving different measurement sites, and help provide a higher data accuracy for cohort health and climate research studies.

2015, Risius, S., Xu, H., Di Lorenzo, F., Xi, H., Siebert, H., Shaw, R.A., Bodenschatz, E.

Cloud measurements are usually carried out with airborne campaigns, which are expensive and are limited by temporal duration and weather conditions. Ground-based measurements at high-altitude research stations therefore play a complementary role in cloud study. Using the meteorological data (wind speed, direction, temperature, humidity, visibility, etc.) collected by the German Weather Service (DWD) from 2000 to 2012 and turbulence measurements recorded by multiple ultrasonic sensors (sampled at 10 Hz) in 2010, we show that the Umweltforschungsstation Schneefernerhaus (UFS) located just below the peak of Zugspitze in the German Alps, at a height of 2650 m, is a well-suited station for cloud–turbulence research. The wind at UFS is dominantly in the east–west direction and nearly horizontal. During the summertime (July and August) the UFS is immersed in warm clouds about 25 % of the time. The clouds are either from convection originating in the valley in the east, or associated with synoptic-scale weather systems typically advected from the west. Air turbulence, as measured from the second- and third-order velocity structure functions that exhibit well-developed inertial ranges, possesses Taylor microscale Reynolds numbers up to 104, with the most probable value at ~ 3000. In spite of the complex topography, the turbulence appears to be nearly as isotropic as many laboratory flows when evaluated on the "Lumley triangle".

2016, Baars, Holger, Kanitz, Thomas, Engelmann, Ronny, Althausen, Dietrich, Heese, Birgit, Komppula, Mika, Preißler, Jana, Tesche, Matthias, Ansmann, Albert, Wandinger, Ulla, Lim, Jae-Hyun, Ahn, Joon Young, Stachlewska, Iwona S., Amiridis, Vassilis, Marinou, Eleni, Seifert, Patric, Hofer, Julian, Skupin, Annett, Schneider, Florian, Bohlmann, Stephanie, Foth, Andreas, Bley, Sebastian, Pfüller, Anne, Giannakaki, Eleni, Lihavainen, Heikki, Viisanen, Yrjö, Hooda, Rakesh Kumar, Pereira, Sérgio Nepomuceno, Bortol, Daniele, Wagner, Frank, Mattis, Ina, Janicka, Lucja, Markowicz, Krzysztof M., Achtert, Peggy, Artaxo, Paulo, Pauliquevis, Theotonio, Souza, Rodrigo A.F., Sharma, Ved Prakesh, van Zyl, Pieter Gideon, Beukes, Johan Paul, Sun, Junying, Rohwer, Erich G., Deng, Ruru, Mamouri, Rodanthi-Elisavet, Zamorano, Felix

A global vertically resolved aerosol data set covering more than 10 years of observations at more than 20 measurement sites distributed from 63° N to 52° S and 72° W to 124° E has been achieved within the Raman and polarization lidar network PollyNET. This network consists of portable, remote-controlled multiwavelength-polarization-Raman lidars (Polly) for automated and continuous 24/7 observations of clouds and aerosols. PollyNET is an independent, voluntary, and scientific network. All Polly lidars feature a standardized instrument design with different capabilities ranging from single wavelength to multiwavelength systems, and now apply unified calibration, quality control, and data analysis. The observations are processed in near-real time without manual intervention, and are presented online at http://polly.tropos.de/. The paper gives an overview of the observations on four continents and two research vessels obtained with eight Polly systems. The specific aerosol types at these locations (mineral dust, smoke, dust-smoke and other dusty mixtures, urban haze, and volcanic ash) are identified by their Ångström exponent, lidar ratio, and depolarization ratio. The vertical aerosol distribution at the PollyNET locations is discussed on the basis of more than 55 000 automatically retrieved 30 min particle backscatter coefficient profiles at 532 nm as this operating wavelength is available for all Polly lidar systems. A seasonal analysis of measurements at selected sites revealed typical and extraordinary aerosol conditions as well as seasonal differences. These studies show the potential of PollyNET to support the establishment of a global aerosol climatology that covers the entire troposphere.

2013, Pappalardo, G., Mona, L., D'Amico, G., Wandinger, U., Adam, M., Amodeo, A., Ansmann, A., Apituley, A., Alados Arboledas, L., Balis, D., Boselli, A., Bravo-Aranda, J.A., Chaikovsky, A., Comeron, A., Cuesta, J., De Tomasi, F., Freudenthaler, V., Gausa, M., Giannakaki, E., Giehl, H., Giunta, A., Grigorov, I., Groß, S., Haeffelin, M., Hiebsch, A., Iarlori, M., Lange, D., Linné, H., Madonna, F., Mattis, I., Mamouri, R.-E., McAuliffe, M.A.P., Mitev, V., Molero, F., Navas-Guzman, F., Nicolae, D., Papayannis, A., Perrone, M.R., Pietras, C., Pietruczuk, A., Pisani, G., Preißler, J., Pujadas, M., Rizi, V., Ruth, A.A., Schmidt, J., Schnell, F., Seifert, P., Serikov, I., Sicard, M., Simeonov, V., Spinelli, N., Stebel, K., Tesche, M., Trickl, T., Wang, X., Wagner, F., Wiegner, M., Wilson, K.M.

The eruption of the Icelandic volcano Eyjafjallajökull in April–May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April–26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org. During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5–15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area. The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events.

2013, Clauss, T., Kiselev, A., Hartmann, S., Augustin, S., Pfeifer, S., Niedermeier, D., Wex, H., Stratmann, F.

We report on the development and test results of the new optical particle counter TOPS-Ice (Thermo-stabilized Optical Particle Spectrometer for the detection of Ice). The instrument uses measurements of the cross-polarized scattered light by single particles into the near-forward direction (42.5° ± 12.7°) to distinguish between spherical and non-spherical particles. This approach allows the differentiation between liquid water droplets (spherical) and ice particles (non-spherical) having similar volume-equivalent sizes and therefore can be used to determine the fraction of frozen droplets in a typical immersion freezing experiment. We show that the numerical simulation of the light scattered on non-spherical particles (spheroids in random orientation) considering the actual scattering geometry used in the instrument supports the validity of the approach, even though the cross-polarized component of the light scattered by spherical droplets does not vanish in this scattering angle. For the separation of the ice particle mode from the liquid droplet mode, we use the width of the pulse detected in the depolarization channel instead of the pulse height. Exploiting the intrinsic relationship between pulse height and pulse width for Gaussian pulses allows us to calculate the fraction of frozen droplets even if the liquid droplet mode dominates the particle ensemble. We present test results obtained with TOPS-Ice in the immersion freezing experiments at the laminar diffusion chamber LACIS (Leipzig Aerosol Cloud Interaction Simulator) and demonstrate the excellent agreement with the data obtained in similar experiments with a different optical instrument. Finally, the advantages of using the cross-polarized light measurements for the differentiation of liquid and frozen droplets in the realistic immersion freezing experiments are discussed.

2012, Wiedensohler, A., Birmili, W., Nowak, A., Sonntag, A., Weinhold, K., Merkel, M., Wehner, B., Tuch, T., Pfeifer, S., Fiebig, M., Fjäraa, A.M., Asmi, E., Sellegri, K., Depuy, R., Venzac, H., Villani, P., Laj, P., Aalto, P., Ogren, J.A., Swietlick, E., Williams, P., Roldin, P., Quincey, P., Hüglin, C., Fierz-Schmidhauser, R., Gysel, M., Weingartner, E., Riccobono, F., Santos, S., Grüning, C., Faloon, K., Beddows, D., Harrison, R., Monahan, C., Jennings, S.G., O'Dowd, C.D., Marinoni, A., Horn, H.-G., Keck, L., Jiang, J., Scheckman, J., McMurry, P.H., Deng, Z., Zhao, C.S., Moerman, M., Henzing, B., de Leeuw, G., Löschau, G., Bastian, S.

Mobility particle size spectrometers often referred to as DMPS (Differential Mobility Particle Sizers) or SMPS (Scanning Mobility Particle Sizers) have found a wide range of applications in atmospheric aerosol research. However, comparability of measurements conducted world-wide is hampered by lack of generally accepted technical standards and guidelines with respect to the instrumental set-up, measurement mode, data evaluation as well as quality control. Technical standards were developed for a minimum requirement of mobility size spectrometry to perform long-term atmospheric aerosol measurements. Technical recommendations include continuous monitoring of flow rates, temperature, pressure, and relative humidity for the sheath and sample air in the differential mobility analyzer. We compared commercial and custom-made inversion routines to calculate the particle number size distributions from the measured electrical mobility distribution. All inversion routines are comparable within few per cent uncertainty for a given set of raw data. Furthermore, this work summarizes the results from several instrument intercomparison workshops conducted within the European infrastructure project EUSAAR (European Supersites for Atmospheric Aerosol Research) and ACTRIS (Aerosols, Clouds, and Trace gases Research InfraStructure Network) to determine present uncertainties especially of custom-built mobility particle size spectrometers. Under controlled laboratory conditions, the particle number size distributions from 20 to 200 nm determined by mobility particle size spectrometers of different design are within an uncertainty range of around ±10% after correcting internal particle losses, while below and above this size range the discrepancies increased. For particles larger than 200 nm, the uncertainty range increased to 30%, which could not be explained. The network reference mobility spectrometers with identical design agreed within ±4% in the peak particle number concentration when all settings were done carefully. The consistency of these reference instruments to the total particle number concentration was demonstrated to be less than 5%. Additionally, a new data structure for particle number size distributions was introduced to store and disseminate the data at EMEP (European Monitoring and Evaluation Program). This structure contains three levels: raw data, processed data, and final particle size distributions. Importantly, we recommend reporting raw measurements including all relevant instrument parameters as well as a complete documentation on all data transformation and correction steps. These technical and data structure standards aim to enhance the quality of long-term size distribution measurements, their comparability between different networks and sites, and their transparency and traceability back to raw data.

2015, Zhang, Y., Mahowald, N., Scanza, R.A., Journet, E., Desboeufs, K., Albani, S., Kok, J.F., Zhuang, G., Chen, Y., Cohen, D.D., Paytan, A., Patey, M.D., Achterberg, E.P., Engelbrecht, J.P., Fomba, K.W.

Trace element deposition from desert dust has important impacts on ocean primary productivity, the quantification of which could be useful in determining the magnitude and sign of the biogeochemical feedback on radiative forcing. However, the impact of elemental deposition to remote ocean regions is not well understood and is not currently included in global climate models. In this study, emission inventories for eight elements primarily of soil origin, Mg, P, Ca, Mn, Fe, K, Al, and Si are determined based on a global mineral data set and a soil data set. The resulting elemental fractions are used to drive the desert dust model in the Community Earth System Model (CESM) in order to simulate the elemental concentrations of atmospheric dust. Spatial variability of mineral dust elemental fractions is evident on a global scale, particularly for Ca. Simulations of global variations in the Ca / Al ratio, which typically range from around 0.1 to 5.0 in soils, are consistent with observations, suggesting that this ratio is a good signature for dust source regions. The simulated variable fractions of chemical elements are sufficiently different; estimates of deposition should include elemental variations, especially for Ca, Al and Fe. The model results have been evaluated with observations of elemental aerosol concentrations from desert regions and dust events in non-dust regions, providing insights into uncertainties in the modeling approach. The ratios between modeled and observed elemental fractions range from 0.7 to 1.6, except for Mg and Mn (3.4 and 3.5, respectively). Using the soil database improves the correspondence of the spatial heterogeneity in the modeling of several elements (Ca, Al and Fe) compared to observations. Total and soluble dust element fluxes to different ocean basins and ice sheet regions have been estimated, based on the model results. The annual inputs of soluble Mg, P, Ca, Mn, Fe and K associated with dust using the mineral data set are 0.30 Tg, 16.89 Gg, 1.32 Tg, 22.84 Gg, 0.068 Tg, and 0.15 Tg to global oceans and ice sheets.

2018, Dai, Guangyao, Althausen, Dietrich, Hofer, Julian, Engelmann, Ronny, Seifert, Patric, Bühl, Johannes, Mamouri, Rodanthi-Elisavet, Wu, Songhua, Ansmann, Albert

We present a practical method to continuously calibrate Raman lidar observations of water vapor mixing ratio profiles. The water vapor profile measured with the multiwavelength polarization Raman lidar PollyXT is calibrated by means of co-located AErosol RObotic NETwork (AERONET) sun photometer observations and Global Data Assimilation System (GDAS) temperature and pressure profiles. This method is applied to lidar observations conducted during the Cyprus Cloud Aerosol and Rain Experiment (CyCARE) in Limassol, Cyprus. We use the GDAS temperature and pressure profiles to retrieve the water vapor density. In the next step, the precipitable water vapor from the lidar observations is used for the calibration of the lidar measurements with the sun photometer measurements. The retrieved calibrated water vapor mixing ratio from the lidar measurements has a relative uncertainty of 11 % in which the error is mainly caused by the error of the sun photometer measurements. During CyCARE, nine measurement cases with cloud-free and stable meteorological conditions are selected to calculate the precipitable water vapor from the lidar and the sun photometer observations. The ratio of these two precipitable water vapor values yields the water vapor calibration constant. The calibration constant for the PollyXT Raman lidar is 6.56 g kg−1 ± 0.72 g kg−1 (with a statistical uncertainty of 0.08 g kg−1 and an instrumental uncertainty of 0.72 g kg−1). To check the quality of the water vapor calibration, the water vapor mixing ratio profiles from the simultaneous nighttime observations with Raman lidar and Vaisala radiosonde sounding are compared. The correlation of the water vapor mixing ratios from these two instruments is determined by using all of the 19 simultaneous nighttime measurements during CyCARE. Excellent agreement with the slope of 1.01 and the R2 of 0.99 is found. One example is presented to demonstrate the full potential of a well-calibrated Raman lidar. The relative humidity profiles from lidar, GDAS (simulation) and radiosonde are compared, too. It is found that the combination of water vapor mixing ratio and GDAS temperature profiles allow us to derive relative humidity profiles with the relative uncertainty of 10–20 %.

2014, Tjernström, M., Leck, C., Birch, C.E., Bottenheim, J.W., Brooks, B.J., Brooks, I.M., Bäcklin, L., Chang, R.Y.-W., de Leeuw, G., Di Liberto, L., de la Rosa, S., Granath, E., Graus, M., Hansel, A., Heintzenberg, J., Held, A., Hind, A., Johnston, P., Knulst, J., Martin, M., Matrai, P.A., Mauritsen, T., Müller, M., Norris, S.J., Orellana, M.V., Orsini, D.A., Paatero, J., Persson, P.O.G., Gao, Q., Rauschenberg, C., Ristovski, Z., Sedlar, J., Shupe, M.D., Sierau, B., Sirevaag, A., Sjogren, S., Stetzer, O., Swietlicki, E., Szczodrak, M., Vaattovaara, P., Wahlberg, N., Westberg, M., Wheeler, C.R.

The climate in the Arctic is changing faster than anywhere else on earth. Poorly understood feedback processes relating to Arctic clouds and aerosol–cloud interactions contribute to a poor understanding of the present changes in the Arctic climate system, and also to a large spread in projections of future climate in the Arctic. The problem is exacerbated by the paucity of research-quality observations in the central Arctic. Improved formulations in climate models require such observations, which can only come from measurements in situ in this difficult-to-reach region with logistically demanding environmental conditions. The Arctic Summer Cloud Ocean Study (ASCOS) was the most extensive central Arctic Ocean expedition with an atmospheric focus during the International Polar Year (IPY) 2007–2008. ASCOS focused on the study of the formation and life cycle of low-level Arctic clouds. ASCOS departed from Longyearbyen on Svalbard on 2 August and returned on 9 September 2008. In transit into and out of the pack ice, four short research stations were undertaken in the Fram Strait: two in open water and two in the marginal ice zone. After traversing the pack ice northward, an ice camp was set up on 12 August at 87°21' N, 01°29' W and remained in operation through 1 September, drifting with the ice. During this time, extensive measurements were taken of atmospheric gas and particle chemistry and physics, mesoscale and boundary-layer meteorology, marine biology and chemistry, and upper ocean physics. ASCOS provides a unique interdisciplinary data set for development and testing of new hypotheses on cloud processes, their interactions with the sea ice and ocean and associated physical, chemical, and biological processes and interactions. For example, the first-ever quantitative observation of bubbles in Arctic leads, combined with the unique discovery of marine organic material, polymer gels with an origin in the ocean, inside cloud droplets suggests the possibility of primary marine organically derived cloud condensation nuclei in Arctic stratocumulus clouds. Direct observations of surface fluxes of aerosols could, however, not explain observed variability in aerosol concentrations, and the balance between local and remote aerosols sources remains open. Lack of cloud condensation nuclei (CCN) was at times a controlling factor in low-level cloud formation, and hence for the impact of clouds on the surface energy budget. ASCOS provided detailed measurements of the surface energy balance from late summer melt into the initial autumn freeze-up, and documented the effects of clouds and storms on the surface energy balance during this transition. In addition to such process-level studies, the unique, independent ASCOS data set can and is being used for validation of satellite retrievals, operational models, and reanalysis data sets.