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, Zscheischler, J., Reichstein, M., Harmeling, S., Rammig, A., Tomelleri, E., Mahecha, M.D.

Climate extremes can affect the functioning of terrestrial ecosystems, for instance via a reduction of the photosynthetic capacity or alterations of respiratory processes. Yet the dominant regional and seasonal effects of hydrometeorological extremes are still not well documented and in the focus of this paper. Specifically, we quantify and characterize the role of large spatiotemporal extreme events in gross primary production (GPP) as triggers of continental anomalies. We also investigate seasonal dynamics of extreme impacts on continental GPP anomalies. We find that the 50 largest positive extremes (i.e., statistically unusual increases in carbon uptake rates) and negative extremes (i.e., statistically unusual decreases in carbon uptake rates) on each continent can explain most of the continental variation in GPP, which is in line with previous results obtained at the global scale. We show that negative extremes are larger than positive ones and demonstrate that this asymmetry is particularly strong in South America and Europe. Our analysis indicates that the overall impacts and the spatial extents of GPP extremes are power-law distributed with exponents that vary little across continents. Moreover, we show that on all continents and for all data sets the spatial extents play a more important role for the overall impact of GPP extremes compared to the durations or maximal GPP. An analysis of possible causes across continents indicates that most negative extremes in GPP can be attributed clearly to water scarcity, whereas extreme temperatures play a secondary role. However, for Europe, South America and Oceania we also identify fire as an important driver. Our findings are consistent with remote sensing products. An independent validation against a literature survey on specific extreme events supports our results to a large extent.

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.

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.

2013, Wilms, H., Rapp, M., Hoffmann, P., Fiedler, J., Baumgarten, G.

The influence of gravity waves on noctilucent clouds (NLC) at ALOMAR (69° N) is analysed by relating gravity wave activity to NLC occurrence from common-volume measurements. Gravity wave kinetic energies are derived from MF-radar wind data and filtered into different period ranges by wavelet transformation. From the dataset covering the years 1999–2011, a direct correlation between gravity wave kinetic energy and NLC occurrence is not found, i.e., NLC appear independently of the simultaneously measured gravity wave kinetic energy. In addition, gravity wave activity is divided into weak and strong activity as compared to a 13 yr mean. The NLC occurrence rates during strong and weak activity are calculated separately for a given wave period and compared to each other. Again, for the full dataset no dependence of NLC occurrence on relative gravity wave activity is found. However, concentrating on 12 h of NLC detections during 2008, we do find an NLC-amplification with strong long-period gravity wave occurrence. Our analysis hence confirms previous findings that in general NLC at ALOMAR are not predominantly driven by gravity waves while exceptions to this rule are at least possible.

2014, Forkel, M., Carvalhais, N., Schaphoff, S., v. Bloh, W., Migliavacca, M., Thurner, M., Thonicke, K.

Existing dynamic global vegetation models (DGVMs) have a limited ability in reproducing phenology and decadal dynamics of vegetation greenness as observed by satellites. These limitations in reproducing observations reflect a poor understanding and description of the environmental controls on phenology, which strongly influence the ability to simulate longer-term vegetation dynamics, e.g. carbon allocation. Combining DGVMs with observational data sets can potentially help to revise current modelling approaches and thus enhance the understanding of processes that control seasonal to long-term vegetation greenness dynamics. Here we implemented a new phenology model within the LPJmL (Lund Potsdam Jena managed lands) DGVM and integrated several observational data sets to improve the ability of the model in reproducing satellite-derived time series of vegetation greenness. Specifically, we optimized LPJmL parameters against observational time series of the fraction of absorbed photosynthetic active radiation (FAPAR), albedo and gross primary production to identify the main environmental controls for seasonal vegetation greenness dynamics. We demonstrated that LPJmL with new phenology and optimized parameters better reproduces seasonality, inter-annual variability and trends of vegetation greenness. Our results indicate that soil water availability is an important control on vegetation phenology not only in water-limited biomes but also in boreal forests and the Arctic tundra. Whereas water availability controls phenology in water-limited ecosystems during the entire growing season, water availability co-modulates jointly with temperature the beginning of the growing season in boreal and Arctic regions. Additionally, water availability contributes to better explain decadal greening trends in the Sahel and browning trends in boreal forests. These results emphasize the importance of considering water availability in a new generation of phenology modules in DGVMs in order to correctly reproduce observed seasonal-to-decadal dynamics of vegetation greenness.

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.

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.

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.

2012, Hildebrand, J., Baumgarten, G., Fiedler, J., Hoppe, U.-P., Kaifler, B., Lübken, F.-J., Williams, B.P.

During a joint campaign in January 2009, the Rayleigh/Mie/Raman (RMR) lidar and the sodium lidar at the ALOMAR Observatory (69 N, 16 E) in Northern Norway were operated simultaneously for more than 40 h, collecting data for wind measurements in the middle atmosphere from 30 up to 110 km altitude. As both lidars share the same receiving telescopes, the upper altitude range of the RMR lidar and the lower altitude range of the sodium lidar overlap in the altitude region of ≈80-85 km. For this overlap region we are thus able to present the first simultaneous wind measurements derived from two different lidar instruments. The comparison of winds derived by RMR and sodium lidar is excellent for long integration times of 10 h as well as shorter ones of 1 h. Combination of data from both lidars allows identifying wavy structures between 30 and 110 km altitude, whose amplitudes increase with height. We have also performed vertical wind measurements and measurements of the same horizontal wind component using two independent lasers and telescopes of the RMR lidar and show how to use this data to calibrate and validate the wind retrieval. For the latter configuration we found a good agreement of the results but also identified inhomogeneities in the horizontal wind at about 55 km altitude of up to 20 ms-1 for an integration time of nearly 4 h. Such small-scale inhomogeneities in the horizontal wind field are an essential challenge when comparing data from different instruments.