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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.
- ItemDetecting impacts of extreme events with ecological in situ monitoring networks(München : European Geopyhsical Union, 2017) Mahecha, Miguel D.; Gans, Fabian; Sippel, Sebastian; Donges, Jonathan F.; Kaminski, Thomas; Metzger, Stefan; Migliavacca, Mirco; Papale, Dario; Rammig, Anja; Zscheischler, Jakob; Arneth, AlmutExtreme hydrometeorological conditions typically impact ecophysiological processes on land. Satellite-based observations of the terrestrial biosphere provide an important reference for detecting and describing the spatiotemporal development of such events. However, in-depth investigations of ecological processes during extreme events require additional in situ observations. The question is whether the density of existing ecological in situ networks is sufficient for analysing the impact of extreme events, and what are expected event detection rates of ecological in situ networks of a given size. To assess these issues, we build a baseline of extreme reductions in the fraction of absorbed photosynthetically active radiation (FAPAR), identified by a new event detection method tailored to identify extremes of regional relevance. We then investigate the event detection success rates of hypothetical networks of varying sizes. Our results show that large extremes can be reliably detected with relatively small networks, but also reveal a linear decay of detection probabilities towards smaller extreme events in log–log space. For instance, networks with  ≈  100 randomly placed sites in Europe yield a  ≥  90 % chance of detecting the eight largest (typically very large) extreme events; but only a  ≥  50 % chance of capturing the 39 largest events. These findings are consistent with probability-theoretic considerations, but the slopes of the decay rates deviate due to temporal autocorrelation and the exact implementation of the extreme event detection algorithm. Using the examples of AmeriFlux and NEON, we then investigate to what degree ecological in situ networks can capture extreme events of a given size. Consistent with our theoretical considerations, we find that today's systematically designed networks (i.e. NEON) reliably detect the largest extremes, but that the extreme event detection rates are not higher than would be achieved by randomly designed networks. Spatio-temporal expansions of ecological in situ monitoring networks should carefully consider the size distribution characteristics of extreme events if the aim is also to monitor the impacts of such events in the terrestrial biosphere.
- 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.
- ItemChemical composition and droplet size distribution of cloud at the summit of Mount Tai, China(Katlenburg-Lindau : EGU, 2017) Li, Jiarong; Wang, Xinfeng; Chen, Jianmin; Zhu, Chao; Li, Weijun; Li, Chengbao; Liu, Lu; Xu, Caihong; Wen, Liang; Xue, Likun; Wang, Wenxing; Ding, Aijun; Herrmann, HartmutThe chemical composition of 39 cloud samples and droplet size distributions in 24 cloud events were investigated at the summit of Mt. Tai from July to October 2014. Inorganic ions, organic acids, metals, HCHO, H2O2, sulfur( IV), organic carbon, and elemental carbon as well as pH and electrical conductivity were analyzed. The acidity of the cloud water significantly decreased from a reported value of pH 3.86 during 2007-2008 (Guo et al., 2012) to pH 5.87 in the present study. The concentrations of nitrate and ammonium were both increased since 2007-2008, but the overcompensation of ammonium led to an increase in the mean pH value. The microphysical properties showed that cloud droplets were smaller than 26.0 μm and most were in the range of 6.0-9.0 μm at Mt. Tai. The maximum droplet number concentration (Nd) was associated with a droplet size of 7.0 μm. High liquid water content (LWC) values could facilitate the formation of larger cloud droplets and broadened the droplet size distribution. Cloud droplets exhibited a strong interaction with atmospheric aerosols. Higher PM2.5 levels resulted in higher concentrations of water-soluble ions and smaller sizes with increased numbers of cloud droplets. The lower pH values were likely to occur at higher PM2.5 concentrations. Clouds were an important sink for soluble materials in the atmosphere. The dilution effect of cloud water should be considered when estimating concentrations of soluble components in the cloud phase.
- ItemNew particle formation in the Svalbard region 2006-2015(Katlenburg-Lindau : EGU, 2017) Heintzenberg, Jost; Tunved, Peter; GalÃ, MartÃ; Leck, CarolineEvents of new particle formation (NPF) were analyzed in a 10-year data set of hourly particle size distributions recorded on Mt. Zeppelin, Spitsbergen, Svalbard. Three different types of NPF events were identified through objective search algorithms. The first and simplest algorithm utilizes short-term increases in particle concentrations below 25 nm (PCT (percentiles) events). The second one builds on the growth of the sub-50 nm diameter median (DGR (diameter growth) events) and is most closely related to the classical "banana type" of event. The third and most complex, multiple-size approach to identifying NPF events builds on a hypothesis suggesting the concurrent production of polymer gel particles at several sizes below ca. 60 nm (MEV (multisize growth) events). As a first and general conclusion, we can state that NPF events are a summer phenomenon and not related to Arctic haze, which is a late winter to early spring feature. The occurrence of NPF events appears to be somewhat sensitive to the available data on precipitation. The seasonal distribution of solar flux suggests some photochemical control that may affect marine biological processes generating particle precursors and/or atmospheric photochemical processes that generate condensable vapors from precursor gases. Notably, the seasonal distribution of the biogenic methanesulfonate (MSA) follows that of the solar flux although it peaks before the maxima in NPF occurrence. A host of ancillary data and findings point to varying and rather complex marine biological source processes. The potential source regions for all types of new particle formation appear to be restricted to the marginal-ice and open-water areas between northeastern Greenland and eastern Svalbard. Depending on conditions, yet to be clarified new particle formation may become visible as short bursts of particles around 20 nm (PCT events), longer events involving condensation growth (DGR events), or extended events with elevated concentrations of particles at several sizes below 100 nm (MEV events). The seasonal distribution of NPF events peaks later than that of MSA and DGR, and in particular than that of MEV events, which reach into late summer and early fall with open, warm, and biologically active waters around Svalbard. Consequently, a simple model to describe the seasonal distribution of the total number of NPF events can be based on solar flux and sea surface temperature, representing environmental conditions for marine biological activity and condensation sink, controlling the balance between new particle nucleation and their condensational growth. Based on the sparse knowledge about the seasonal cycle of gel-forming marine microorganisms and their controlling factors, we hypothesize that the seasonal distribution of DGR and, more so, MEV events reflect the seasonal cycle of the gel-forming phytoplankton.
- ItemA novel method for deriving the aerosol hygroscopicity parameter based only on measurements from a humidified nephelometer system(Katlenburg-Lindau : EGU, 2017) Kuang, Ye; Zhao, Chunsheng; Tao, Jiangchuan; Bian, Yuxuan; Ma, Nan; Zhao, GangAerosol hygroscopicity is crucial for understanding roles of aerosol particles in atmospheric chemistry and aerosol climate effects. Light-scattering enhancement factor f (RH, λ) is one of the parameters describing aerosol hygroscopicity, which is defined as f (RH, λ) = δsp(RH, λ)=δsp(dry, λ), where δsp(RH, λ) or δsp(dry, λ) represents δsp at wavelength λ under certain relative humidity (RH) or dry conditions. Traditionally, an overall hygroscopicity parameter κ can be retrieved from measured f (RH, λ), hereinafter referred to as κf(RH), by combining concurrently measured particle number size distribution (PNSD) and mass concentration of black carbon. In this paper, a new method is proposed to directly derive κf(RH) based only on measurements from a three-wavelength humidified nephelometer system. The advantage of this newly proposed approach is that κf(RH) can be estimated without any additional information about PNSD and black carbon. This method is verified with measurements from two different field campaigns. Values of κf(RH) estimated from this new method agree very well with those retrieved by using the traditional method: all points lie near the 1 : 1 line and the square of correlation coefficient between them is 0.99. The verification results demonstrate that this newly proposed method of deriving κf(RH) is applicable at different sites and in seasons of the North China Plain and might also be applicable in other regions around the world.
- ItemContributions of transported Prudhoe Bay oil field emissions to the aerosol population in Utqiaġvik, Alaska(Katlenburg-Lindau : EGU, 2017) Gunsch, Matthew J.; Kirpes, Rachel M.; Kolesar, Katheryn R.; Barrett, Tate E.; China, Swarup; Sheesley, Rebecca J.; Laskin, Alexander; Wiedensohler, Alfred; Tuch, Thomas; Pratt, Kerri A.Loss of sea ice is opening the Arctic to increasing development involving oil and gas extraction and shipping. Given the significant impacts of absorbing aerosol and secondary aerosol precursors emitted within the rapidly warming Arctic region, it is necessary to characterize local anthropogenic aerosol sources and compare to natural conditions. From August to September 2015 in Utqiaġvik (Barrow), AK, the chemical composition of individual atmospheric particles was measured by computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (0.13-4 μm projected area diameter) and real-time single-particle mass spectrometry (0.2-1.5 μm vacuum aerodynamic diameter). During periods influenced by the Arctic Ocean (70 % of the study), our results show that fresh sea spray aerosol contributed ∼ 20 %, by number, of particles between 0.13 and 0.4 μm, 40-70 % between 0.4 and 1 μm, and 80-100 % between 1 and 4 μm particles. In contrast, for periods influenced by emissions from Prudhoe Bay (10 % of the study), the third largest oil field in North America, there was a strong influence from submicron (0.13-1 μm) combustion-derived particles (20-50 % organic carbon, by number; 5-10 % soot by number). While sea spray aerosol still comprised a large fraction of particles (90 % by number from 1 to 4 μm) detected under Prudhoe Bay influence, these particles were internally mixed with sulfate and nitrate indicative of aging processes during transport. In addition, the overall mode of the particle size number distribution shifted from 76 nm during Arctic Ocean influence to 27 nm during Prudhoe Bay influence, with particle concentrations increasing from 130 to 920 cm-3 due to transported particle emissions from the oil fields. The increased contributions of carbonaceous combustion products and partially aged sea spray aerosol should be considered in future Arctic atmospheric composition and climate simulations.
- 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.