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- ItemAerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters(Katlenburg-Lindau : EGU, 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.
- ItemCharacterization and source apportionment of organic aerosol using offline aerosol mass spectrometry(Katlenburg-Lindau : Copernicus, 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.
- ItemPotential of polarization lidar to provide profiles of CCN-and INP-relevant aerosol parameters(München : European Geopyhsical Union, 2016) Mamouri, Rodanthi-Elisavet; Ansmann, AlbertWe investigate the potential of polarization lidar to provide vertical profiles of aerosol parameters from which cloud condensation nucleus (CCN) and ice nucleating particle (INP) number concentrations can be estimated. We show that height profiles of particle number concentrations n50, dry considering dry aerosol particles with radius > 50 nm (reservoir of CCN in the case of marine and continental non-desert aerosols), n100, dry (particles with dry radius > 100 nm, reservoir of desert dust CCN), and of n250, dry (particles with dry radius > 250 nm, reservoir of favorable INP), as well as profiles of the particle surface area concentration sdry (used in INP parameterizations) can be retrieved from lidar-derived aerosol extinction coefficients σ with relative uncertainties of a factor of 1.5–2 in the case of n50, dry and n100, dry and of about 25–50 % in the case of n250, dry and sdry. Of key importance is the potential of polarization lidar to distinguish and separate the optical properties of desert aerosols from non-desert aerosol such as continental and marine particles. We investigate the relationship between σ, measured at ambient atmospheric conditions, and n50, dry for marine and continental aerosols, n100, dry for desert dust particles, and n250, dry and sdry for three aerosol types (desert, non-desert continental, marine) and for the main lidar wavelengths of 355, 532, and 1064 nm. Our study is based on multiyear Aerosol Robotic Network (AERONET) photometer observations of aerosol optical thickness and column-integrated particle size distribution at Leipzig, Germany, and Limassol, Cyprus, which cover all realistic aerosol mixtures. We further include AERONET data from field campaigns in Morocco, Cabo Verde, and Barbados, which provide pure dust and pure marine aerosol scenarios. By means of a simple CCN parameterization (with n50, dry or n100, dry as input) and available INP parameterization schemes (with n250, dry and sdry as input) we finally compute profiles of the CCN-relevant particle number concentration nCCN and the INP number concentration nINP. We apply the method to a lidar observation of a heavy dust outbreak crossing Cyprus and a case dominated by continental aerosol pollution.
- ItemAn overview of the first decade of PollyNET: An emerging network of automated Raman-polarization lidars for continuous aerosol profiling(München : European Geopyhsical Union, 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, FelixA 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.
- ItemInvestigation of the adiabatic assumption for estimating cloud micro- and macrophysical properties from satellite and ground observations(München : European Geopyhsical Union, 2016) Merk, D.; Deneke, H.; Pospichal, B.; Seifert, P.Cloud properties from both ground-based as well as from geostationary passive satellite observations have been used previously for diagnosing aerosol–cloud interactions. In this investigation, a 2-year data set together with four selected case studies are analyzed with the aim of evaluating the consistency and limitations of current ground-based and satellite-retrieved cloud property data sets. The typically applied adiabatic cloud profile is modified using a sub-adiabatic factor to account for entrainment within the cloud. Based on the adiabatic factor obtained from the combination of ground-based cloud radar, ceilometer and microwave radiometer, we demonstrate that neither the assumption of a completely adiabatic cloud nor the assumption of a constant sub-adiabatic factor is fulfilled (mean adiabatic factor 0.63 ± 0.22). As cloud adiabaticity is required to estimate the cloud droplet number concentration but is not available from passive satellite observations, an independent method to estimate the adiabatic factor, and thus the influence of mixing, would be highly desirable for global-scale analyses. Considering the radiative effect of a cloud described by the sub-adiabatic model, we focus on cloud optical depth and its sensitivities. Ground-based estimates are here compared vs. cloud optical depth retrieved from the Meteosat SEVIRI satellite instrument resulting in a bias of −4 and a root mean square difference of 16. While a synergistic approach based on the combination of ceilometer, cloud radar and microwave radiometer enables an estimate of the cloud droplet concentration, it is highly sensitive to radar calibration and to assumptions about the moments of the droplet size distribution. Similarly, satellite-based estimates of cloud droplet concentration are uncertain. We conclude that neither the ground-based nor satellite-based cloud retrievals applied here allow a robust estimate of cloud droplet concentration, which complicates its use for the study of aerosol–cloud interactions.
- ItemCloud water composition during HCCT-2010: Scavenging efficiencies, solute concentrations, and droplet size dependence of inorganic ions and dissolved organic carbon(München : European Geopyhsical Union, 2016) van Pinxteren, Dominik; Fomba, Khanneh Wadinga; Mertes, Stephan; Müller, Konrad; Spindler, Gerald; Schneider, Johannes; Lee, Taehyoung; Collett, Jeffrey L.; Herrmann, HartmutCloud water samples were taken in September/October 2010 at Mt. Schmücke in a rural, forested area in Germany during the Lagrange-type Hill Cap Cloud Thuringia 2010 (HCCT-2010) cloud experiment. Besides bulk collectors, a three-stage and a five-stage collector were applied and samples were analysed for inorganic ions (SO42−,NO3−, NH4+, Cl−, Na+, Mg2+, Ca2+, K+), H2O2 (aq), S(IV), and dissolved organic carbon (DOC). Campaign volume-weighted mean concentrations were 191, 142, and 39 µmol L−1 for ammonium, nitrate, and sulfate respectively, between 4 and 27 µmol L−1 for minor ions, 5.4 µmol L−1 for H2O2 (aq), 1.9 µmol L−1 for S(IV), and 3.9 mgC L−1 for DOC. The concentrations compare well to more recent European cloud water data from similar sites. On a mass basis, organic material (as DOC × 1.8) contributed 20–40 % (event means) to total solute concentrations and was found to have non-negligible impact on cloud water acidity. Relative standard deviations of major ions were 60–66 % for solute concentrations and 52–80 % for cloud water loadings (CWLs). The similar variability of solute concentrations and CWLs together with the results of back-trajectory analysis and principal component analysis, suggests that concentrations in incoming air masses (i.e. air mass history), rather than cloud liquid water content (LWC), were the main factor controlling bulk solute concentrations for the cloud studied. Droplet effective radius was found to be a somewhat better predictor for cloud water total ionic content (TIC) than LWC, even though no single explanatory variable can fully describe TIC (or solute concentration) variations in a simple functional relation due to the complex processes involved. Bulk concentrations typically agreed within a factor of 2 with co-located measurements of residual particle concentrations sampled by a counterflow virtual impactor (CVI) and analysed by an aerosol mass spectrometer (AMS), with the deviations being mainly caused by systematic differences and limitations of the approaches (such as outgassing of dissolved gases during residual particle sampling). Scavenging efficiencies (SEs) of aerosol constituents were 0.56–0.94, 0.79–0.99, 0.71–98, and 0.67–0.92 for SO42−, NO3−, NH4+, and DOC respectively when calculated as event means with in-cloud data only. SEs estimated using data from an upwind site were substantially different in many cases, revealing the impact of gas-phase uptake (for volatile constituents) and mass losses across Mt. Schmücke likely due to physical processes such as droplet scavenging by trees and/or entrainment. Drop size-resolved cloud water concentrations of major ions SO42−, NO3−, and NH4+ revealed two main profiles: decreasing concentrations with increasing droplet size and “U” shapes. In contrast, profiles of typical coarse particle mode minor ions were often increasing with increasing drop size, highlighting the importance of a species' particle concentration size distribution for the development of size-resolved solute concentration patterns. Concentration differences between droplet size classes were typically < 2 for major ions from the three-stage collector and somewhat more pronounced from the five-stage collector, while they were much larger for minor ions. Due to a better separation of droplet populations, the five-stage collector was capable of resolving some features of solute size dependencies not seen in the three-stage data, especially sharp concentration increases (up to a factor of 5–10) in the smallest droplets for many solutes.
- ItemParticle hygroscopicity and its link to chemical composition in the urban atmosphere of Beijing, China, during summertime(München : European Geopyhsical Union, 2016) Wu, Z.J.; Zheng, J.; Shang, D.J.; Du, Z.F.; Wu, Y.S.; Zeng, L.M.; Wiedensohler, A.; Hu, M.Simultaneous measurements of particle number size distribution, particle hygroscopic properties, and size-resolved chemical composition were made during the summer of 2014 in Beijing, China. During the measurement period, the mean hygroscopicity parameters (κs) of 50, 100, 150, 200, and 250 nm particles were respectively 0.16 ± 0.07, 0.19 ± 0.06, 0.22 ± 0.06, 0.26 ± 0.07, and 0.28 ± 0.10, showing an increasing trend with increasing particle size. Such size dependency of particle hygroscopicity was similar to that of the inorganic mass fraction in PM1. The hydrophilic mode (hygroscopic growth factor, HGF > 1.2) was more prominent in growth factor probability density distributions and its dominance of hydrophilic mode became more pronounced with increasing particle size. When PM2.5 mass concentration was greater than 50 μg m−3, the fractions of the hydrophilic mode for 150, 250, and 350 nm particles increased towards 1 as PM2.5 mass concentration increased. This indicates that aged particles dominated during severe pollution periods in the atmosphere of Beijing. Particle hygroscopic growth can be well predicted using high-time-resolution size-resolved chemical composition derived from aerosol mass spectrometer (AMS) measurements using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. The organic hygroscopicity parameter (κorg) showed a positive correlation with the oxygen to carbon ratio. During the new particle formation event associated with strongly active photochemistry, the hygroscopic growth factor or κ of newly formed particles is greater than for particles with the same sizes not during new particle formation (NPF) periods. A quick transformation from external mixture to internal mixture for pre-existing particles (for example, 250 nm particles) was observed. Such transformations may modify the state of the mixture of pre-existing particles and thus modify properties such as the light absorption coefficient and cloud condensation nuclei activation.
- ItemSize distributions of polycyclic aromatic hydrocarbons in urban atmosphere: Sorption mechanism and source contributions to respiratory deposition(München : European Geopyhsical Union, 2016) Lv, Yan; Li, Xiang; Xu, Ting Ting; Cheng, Tian Tao; Yang, Xin; Chen, Jian Min; Iinuma, Yoshiteru; Herrmann, HartmutIn order to better understand the particle size distribution of polycyclic aromatic hydrocarbons (PAHs) and their source contribution to human respiratory system, size-resolved PAHs have been studied in ambient aerosols at a megacity Shanghai site during a 1-year period (2012–2013). The results showed the PAHs had a bimodal distribution with one mode peak in the fine-particle size range (0.4–2.1 µm) and another mode peak in the coarse-particle size range (3.3–9.0 µm). Along with the increase in ring number of PAHs, the intensity of the fine-mode peak increased, while the coarse-mode peak decreased. Plotting of log(PAH / PM) against log(Dp) showed that all slope values were above −1, suggesting that multiple mechanisms (adsorption and absorption) controlled the particle size distribution of PAHs. The total deposition flux of PAHs in the respiratory tract was calculated as being 8.8 ± 2.0 ng h−1. The highest lifetime cancer risk (LCR) was estimated at 1.5 × 10−6, which exceeded the unit risk of 10−6. The LCR values presented here were mainly influenced by accumulation mode PAHs which came from biomass burning (24 %), coal combustion (25 %), and vehicular emission (27 %). The present study provides us with a mechanistic understanding of the particle size distribution of PAHs and their transport in the human respiratory system, which can help develop better source control strategies.
- ItemAn optical particle size spectrometer for aircraft-borne measurements in IAGOS-CARIBIC(München : European Geopyhsical Union, 2016) Hermann, Markus; Weigelt, Andreas; Assmann, Denise; Pfeifer, Sascha; Müller, Thomas; Conrath, Thomas; Voigtländer, Jens; Heintzenberg, Jost; Wiedensohler, Alfred; Martinsson, Bengt G.; Deshler, Terry; Brenninkmeijer, Carl A.M.; Zahn, AndreasThe particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOS-CARIBIC observatory: In-service Aircraft for a Global Observing System – Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130–1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50 % particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98 %. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOS-CARIBIC observatory.
- ItemVariation of CCN activity during new particle formation events in the North China Plain(München : European Geopyhsical Union, 2016) Ma, Nan; Zhao, Chunsheng; Tao, Jiangchuan; Wu, Zhijun; Kecorius, Simonas; Wang, Zhibin; Größ, Johannes; Liu, Hongjian; Bian, Yuxuan; Kuang, Ye; Teich, Monique; Spindler, Gerald; Müller, Konrad; van Pinxteren, Dominik; Herrmann, Hartmut; Hu, Min; Wiedensohler, AlfredThe aim of this investigation was to obtain a better understanding of the variability of the cloud condensation nuclei (CCN) activity during new particle formation (NPF) events in an anthropogenically polluted atmosphere of the North China Plain (NCP). We investigated the size-resolved activation ratio as well as particle number size distribution, hygroscopicity, and volatility during a 4-week intensive field experiment in summertime at a regional atmospheric observatory in Xianghe. Interestingly, based on a case study, two types of NPF events were found, in which the newly formed particles exhibited either a higher or a lower hygroscopicity. Therefore, the CCN activity of newly formed particles in different NPF events was largely different, indicating that a simple parameterization of particle CCN activity during NPF events over the NCP might lead to poor estimates of CCN number concentration (NCCN). For a more accurate estimation of the potential NCCN during NPF events, the variation of CCN activity has to be taken into account. Considering that a fixed activation ratio curve or critical diameter are usually used to calculate NCCN, the influence of the variation of particle CCN activity on the calculation of NCCN during NPF events was evaluated based on the two parameterizations. It was found that NCCN might be underestimated by up to 30 % if a single activation ratio curve (representative of the region and season) were to be used in the calculation; and might be underestimated by up to 50 % if a fixed critical diameter (representative of the region and season) were used. Therefore, we suggest not using a fixed critical diameter in the prediction of NCCN in NPF. If real-time CCN activity data are not available, using a proper fixed activation ratio curve can be an alternative but compromised choice.