2016, Engelmann, Ronny, Kanitz, Thomas, Baars, Holger, Heese, Birgit, Althausen, Dietrich, Skupin, Annett, Wandinger, Ulla, Komppula, Mika, Stachlewska, Iwona S., Amiridis, Vassilis, Marinou, Eleni, Mattis, Ina, Linné, Holger, Ansmann, Albert

The atmospheric science community demands autonomous and quality-assured vertically resolved measurements of aerosol and cloud properties. For this purpose, a portable lidar called Polly was developed at TROPOS in 2003. The lidar system was continuously improved with gained experience from the EARLINET community, involvement in worldwide field campaigns, and international institute collaborations within the last 10 years. Here we present recent changes of the setup of the portable multiwavelength Raman and polarization lidar PollyXT and discuss the improved capabilities of the system by means of a case study. The latest system developments include an additional near-range receiver unit for Raman measurements of the backscatter and extinction coefficient down to 120 m above ground, a water-vapor channel, and channels for simultaneous measurements of the particle linear depolarization ratio at 355 and 532 nm. Quality improvements were achieved by systematically following the EARLINET guidelines and the international PollyNET quality assurance developments. A modified ship radar ensures measurements in agreement with air-traffic safety regulations and allows for 24∕7 monitoring of the atmospheric state with PollyXT.

2016, Brock, Charles A., Wagner, Nicholas L., Anderson, Bruce E., Attwood, Alexis R., Beyersdorf, Andreas, Campuzano-Jost, Pedro, Carlton, Annmarie G., Day, Douglas A., Diskin, Glenn S., Gordon, Timothy D., Jimenez, Jose L., Lack, Daniel A., Liao, Jin, Markovic, Milos Z., Middlebrook, Ann M., Ng, Nga L., Perring, Anne E., Richardson, Matthews S., Schwarz, Joshua P., Washenfelder, Rebecca A., Welti, Andre, Xu, Lu, Ziemba, Luke D., Murphy, Daniel M.

Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of  ∼  25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction.

2016, Pfeifer, Sascha, Müller, Thomas, Weinhold, Kay, Zikova, Nadezda, dos Santos, Sebastiao Martins, Marinoni, Angela, Bischof, Oliver F., Kykal, Carsten, Ries, Ludwig, Meinhardt, Frank, Aalto, Pasi, Mihalopoulos, Nikolaos, Wiedensohler, Alfred

Aerodynamic particle size spectrometers are a well-established method to measure number size distributions of coarse mode particles in the atmosphere. Quality assurance is essential for atmospheric observational aerosol networks to obtain comparable results with known uncertainties. In a laboratory study within the framework of ACTRIS (Aerosols, Clouds, and Trace gases Research Infrastructure Network), 15 aerodynamic particle size spectrometers (APS model 3321, TSI Inc., St. Paul, MN, USA) were compared with a focus on flow rates, particle sizing, and the unit-to-unit variability of the particle number size distribution. Flow rate deviations were relatively small (within a few percent), while the sizing accuracy was found to be within 10 % compared to polystyrene latex (PSL) reference particles. The unit-to-unit variability in terms of the particle number size distribution during this study was within 10 % to 20 % for particles in the range of 0.9 up to 3 µm, which is acceptable for atmospheric measurements. For particles smaller than that, the variability increased up to 60 %, probably caused by differences in the counting efficiencies of individual units. Number size distribution data for particles smaller than 0.9 µm in aerodynamic diameter should only be used with caution. For particles larger than 3 µm, the unit-to-unit variability increased as well. A possible reason is an insufficient sizing accuracy in combination with a steeply sloping particle number size distribution and the increasing uncertainty due to decreasing counting. Particularly this uncertainty of the particle number size distribution must be considered if higher moments of the size distribution such as the particle volume or mass are calculated, which require the conversion of the aerodynamic diameter measured to a volume equivalent diameter. In order to perform a quantitative quality assurance, a traceable reference method for the particle number concentration in the size range 0.5–3 µm is needed.

2016, Kohn, Monika, Lohmann, Ulrike, Welti, André, Kanji, Zamin A.

The new Portable Immersion Mode Cooling chAmber (PIMCA) has been developed for online immersion freezing of single-immersed aerosol particles. PIMCA is a vertical extension of the established Portable Ice Nucleation Chamber (PINC). PIMCA immerses aerosol particles into cloud droplets before they enter PINC. Immersion freezing experiments on cloud droplets with a radius of 5–7 μm at a prescribed supercooled temperature (T) and water saturation can be conducted, while other ice nucleation mechanisms (deposition, condensation, and contact mode) are excluded. Validation experiments on reference aerosol (kaolinite, ammonium sulfate, and ammonium nitrate) showed good agreement with theory and literature. The PIMCA-PINC setup was tested in the field during the Zurich AMBient Immersion freezing Study (ZAMBIS) in spring 2014 in Zurich, Switzerland. Significant concentrations of submicron ambient aerosol triggering immersion freezing at T > 236 K were rare. The mean frozen cloud droplet number concentration was estimated to be 7.22·105 L−1 for T < 238 K and determined from the measured frozen fraction and cloud condensation nuclei (CCN) concentrations predicted for the site at a typical supersaturation of SS = 0.3%. This value should be considered as an upper limit of cloud droplet freezing via immersion and homogeneous freezing processes. The predicted ice nucleating particle (INP) concentration based on measured total aerosol larger than 0.5 μm and the parameterization by DeMott et al. (2010) at T = 238 K is INPD10=54 ± 39 L−1. This is a lower limit as supermicron particles were not sampled with PIMCA-PINC during ZAMBIS.

2016, Wandinger, Ulla, Freudenthaler, Volker, Baars, Holger, Amodeo, Aldo, Engelmann, Ronny, Mattis, Ina, Groß, Silke, Pappalardo, Gelsomina, Giunta, Aldo, D'Amico, Giuseppe, Chaikovsky, Anatoli, Osipenko, Fiodor, Slesar, Alexander, Nicolae, Doina, Belegante, Livio, Talianu, Camelia, Serikov, Ilya, Linné, Holger, Jansen, Friedhelm, Apituley, Arnoud, Wilson, Keith M., de Graaf, Martin, Trickl, Thomas, Giehl, Helmut, Adam, Mariana, Comerón, Adolfo, Muñoz-Porcar, Constantino, Rocadenbosch, Francesc, Sicard, Michaël, Tomás, Sergio, Lange, Diego, Kumar, Dhiraj, Pujadas, Manuel, Molero, Francisco, Fernández, Alfonso J., Alados-Arboledas, Lucas, Bravo-Aranda, Juan Antonio, Navas-Guzmán, Francisco, Guerrero-Rascado, Juan Luis, Granados-Muñoz, María José, Preißler, Jana, Wagner, Frank, Gausa, Michael, Grigorov, Ivan, Stoyanov, Dimitar, Iarlori, Marco, Rizi, Vincenco, Spinelli, Nicola, Boselli, Antonella, Wang, Xuan, Feudo, Teresa Lo, Perrone, Maria Rita, De Tomas, Ferdinando, Burlizzi, Pasquale

This paper introduces the recent European Aerosol Research Lidar Network (EARLINET) quality-assurance efforts at instrument level. Within two dedicated campaigns and five single-site intercomparison activities, 21 EARLINET systems from 18 EARLINET stations were intercompared between 2009 and 2013. A comprehensive strategy for campaign setup and data evaluation has been established. Eleven systems from nine EARLINET stations participated in the EARLINET Lidar Intercomparison 2009 (EARLI09). In this campaign, three reference systems were qualified which served as traveling standards thereafter. EARLINET systems from nine other stations have been compared against these reference systems since 2009. We present and discuss comparisons at signal and at product level from all campaigns for more than 100 individual measurement channels at the wavelengths of 355, 387, 532, and 607 nm. It is shown that in most cases, a very good agreement of the compared systems with the respective reference is obtained. Mean signal deviations in predefined height ranges are typically below ±2 %. Particle backscatter and extinction coefficients agree within ±2  ×  10−4 km−1 sr−1 and ± 0.01 km−1, respectively, in most cases. For systems or channels that showed larger discrepancies, an in-depth analysis of deficiencies was performed and technical solutions and upgrades were proposed and realized. The intercomparisons have reinforced confidence in the EARLINET data quality and allowed us to draw conclusions on necessary system improvements for some instruments and to identify major challenges that need to be tackled in the future.

2016, Bravo-Aranda, Juan Antonio, Belegante, Livio, Freudenthaler, Volker, Alados-Arboledas, Lucas, Nicolae, Doina, Granados-Muñoz, María José, Guerrero-Rascado, Juan Luis, Amodeo, Aldo, D'Amico, Giusseppe, Engelmann, Ronny, Pappalardo, Gelsomina, Kokkalis, Panos, Mamouri, Rodanthy, Papayannis, Alex, Navas-Guzmán, Francisco, Olmo, Francisco José, Wandinger, Ulla, Amato, Francesco, Haeffelin, Martial

Lidar depolarization measurements distinguish between spherical and non-spherical aerosol particles based on the change of the polarization state between the emitted and received signal. The particle shape information in combination with other aerosol optical properties allows the characterization of different aerosol types and the retrieval of aerosol particle microphysical properties. Regarding the microphysical inversions, the lidar depolarization technique is becoming a key method since particle shape information can be used by algorithms based on spheres and spheroids, optimizing the retrieval procedure. Thus, the identification of the depolarization error sources and the quantification of their effects are crucial. This work presents a new tool to assess the systematic error of the volume linear depolarization ratio (δ), combining the Stokes–Müller formalism and the complete sampling of the error space using the lidar model presented in Freudenthaler (2016a). This tool is applied to a synthetic lidar system and to several EARLINET lidars with depolarization capabilities at 355 or 532 nm. The lidar systems show relative errors of δ larger than 100 % for δ values around molecular linear depolarization ratios (∼ 0.004 and up to ∼  10 % for δ = 0.45). However, one system shows only relative errors of 25 and 0.22 % for δ = 0.004 and δ = 0.45, respectively, and gives an example of how a proper identification and reduction of the main error sources can drastically reduce the systematic errors of δ. In this regard, we provide some indications of how to reduce the systematic errors.

2016, Daellenbach, K.R., Bozzetti, C., Křepelová, A., Canonaco, F., Wolf, R., Zotter, P., Fermo, P., Crippa, M., Slowik, J.G., Sosedova, Y., Zhang, Y., Huang, R.-J., Poulain, L., Szidat, S., Baltensperger, U., El Haddad, I., Prévôt, A.S.H.

Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make its deployment at sufficient sites to determine regional characteristics impractical. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, and PM10, i.e., PM with aerodynamic diameters smaller than 1, 2.5, and 10 µm, respectively), collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g., AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60–91 %) achieved using this technique, together with low detection limits (0.8 µg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon ions, ions containing oxygen, and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning, and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g., filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.

2016, Babkovskaia, Natalia, Rannik, Ullar, Phillips, Vaughan, Siebert, Holger, Wehner, Birgit, Boy, Michael

The purpose of this study is to investigate the interaction between small-scale turbulence and aerosol and cloud microphysical properties using direct numerical simulations (DNS). We consider the domain located at the height of about 2000 m from the sea level, experiencing transient high supersaturation due to atmospheric fluctuations of temperature and humidity. To study the effect of total number of particles (Ntot) on air temperature, activation and supersaturation, we vary Ntot. To investigate the effect of aerosol dynamics on small-scale turbulence and vertical air motion, we vary the intensity of turbulent fluctuations and the buoyant force. We find that even a small number of aerosol particles (55.5 cm−3), and therefore a small droplet number concentration, strongly affects the air temperature due to release of latent heat. The system comes to an equilibrium faster and the relative number of activated particles appears to be smaller for larger Ntot. We conclude that aerosol particles strongly affect the air motion. In a case of updraught coursed by buoyant force, the presence of aerosol particles results in acceleration of air motion in vertical direction and increase of turbulent fluctuations.

2016, Su, Hang, Cheng, Yafang, Ma, Nan, Wang, Zhibin, Wang, Xiaoxiang, Pöhlker, Mira L., Nillius, Björn, Wiedensohler, Alfred, Pöschl, Ulrich

The activation and hygroscopicity of cloud condensation nuclei (CCN) are key to the understanding of aerosol–cloud interactions and their impact on climate. They can be measured by scanning the particle size and supersaturation in CCN measurements. The scanning of supersaturation is often time-consuming and limits the temporal resolution and performance of CCN measurements. Here we present a new approach, termed the broad supersaturation scanning (BS2) method, in which a range of supersaturation is simultaneously scanned, reducing the time interval between different supersaturation scans. The practical applicability of the BS2 approach is demonstrated with nano-CCN measurements of laboratory-generated aerosol particles. Model simulations show that the BS2 approach may also be applicable for measuring CCN activation of ambient mixed particles. Due to its fast response and technical simplicity, the BS2 approach may be well suited for aircraft and long-term measurements. Since hygroscopicity is closely related to the fraction of organics/inorganics in aerosol particles, a BS2-CCN counter can also serve as a complementary sensor for fast detection/estimation of aerosol chemical compositions.

2016, Boose, Yvonne, Welti, André, Atkinson, James, Ramelli, Fabiola, Danielczok, Anja, Bingemer, Heinz G., Plötze, Michael, Sierau, Berko, Kanji, Zamin A., Lohmann, Ulrike

Desert dust is one of the most abundant ice nucleating particle types in the atmosphere. Traditionally, clay minerals were assumed to determine the ice nucleation ability of desert dust and constituted the focus of ice nucleation studies over several decades. Recently some feldspar species were identified to be ice active at much higher temperatures than clay minerals, redirecting studies to investigate the contribution of feldspar to ice nucleation on desert dust. However, so far no study has shown the atmospheric relevance of this mineral phase. For this study four dust samples were collected after airborne transport in the troposphere from the Sahara to different locations (Crete, the Peloponnese, Canary Islands, and the Sinai Peninsula). Additionally, 11 dust samples were collected from the surface from nine of the biggest deserts worldwide. The samples were used to study the ice nucleation behavior specific to different desert dusts. Furthermore, we investigated how representative surface-collected dust is for the atmosphere by comparing to the ice nucleation activity of the airborne samples. We used the IMCA-ZINC setup to form droplets on single aerosol particles which were subsequently exposed to temperatures between 233 and 250 K. Dust particles were collected in parallel on filters for offline cold-stage ice nucleation experiments at 253–263 K. To help the interpretation of the ice nucleation experiments the mineralogical composition of the dusts was investigated. We find that a higher ice nucleation activity in a given sample at 253 K can be attributed to the K-feldspar content present in this sample, whereas at temperatures between 238 and 245 K it is attributed to the sum of feldspar and quartz content present. A high clay content, in contrast, is associated with lower ice nucleation activity. This confirms the importance of feldspar above 250 K and the role of quartz and feldspars determining the ice nucleation activities at lower temperatures as found by earlier studies for monomineral dusts. The airborne samples show on average a lower ice nucleation activity than the surface-collected ones. Furthermore, we find that under certain conditions milling can lead to a decrease in the ice nucleation ability of polymineral samples due to the different hardness and cleavage of individual mineral phases causing an increase of minerals with low ice nucleation ability in the atmospherically relevant size fraction. Comparison of our data set to an existing desert dust parameterization confirms its applicability for climate models. Our results suggest that for an improved prediction of the ice nucleation ability of desert dust in the atmosphere, the modeling of emission and atmospheric transport of the feldspar and quartz mineral phases would be key, while other minerals are only of minor importance.