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- ItemHygroscopic properties of the Paris urban aerosol in relation to its chemical composition(München : European Geopyhsical Union, 2014) Kamilli, K.A.; Poulain, L.; Held, A.; Nowak, A.; Birmili, W.; Wiedensohler, A.Aerosol hygroscopic growth factors and chemical properties were measured as part of the MEGAPOLI "Megacities Plume Case Study" at the urban site Laboratoire d'Hygiène de la Ville de Paris (LHVP) in the city center of Paris from June to August 2009, and from January to February 2010. Descriptive hygroscopic growth factors (DGF) were derived in the diameter range from 25 to 350 nm at relative humidities of 30, 55, 75, and 90% by applying the summation method on humidified and dry aerosol size distributions measured simultaneously with a humidified differential mobility particle sizer (HDMPS) and a twin differential mobility particle sizer (TDMPS). For 90% relative humidity, the DGF varied from 1.06 to 1.46 in summer, and from 1.06 to 1.66 in winter. Temporal variations in the observed mean DGF could be well explained with a simple growth model based on the aerosol chemical composition measured by aerosol mass spectrometry (AMS) and black carbon photometry (MAAP). In particular, good agreement was observed when sulfate was the predominant inorganic factor. A clear overestimation of the predicted growth factor was found when the nitrate mass concentration exceeded values of 10 μg m−3, e.g., during winter.
- 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.
- ItemThe impact of aerosol hygroscopic growth on the single-scattering albedo and its application on the NO2 photolysis rate coefficient(München : European Geopyhsical Union, 2014) Tao, J.C.; Zhao, C.S.; Ma, N.; Liu, P.F.Hygroscopic growth of aerosol particles can significantly affect their single-scattering albedo (ω), and consequently alters the aerosol effect on tropospheric photochemistry. In this study, the impact of aerosol hygroscopic growth on ω and its application to the NO2 photolysis rate coefficient (JNO2) are investigated for a typical aerosol particle population in the North China Plain (NCP). The variations of aerosol optical properties with relative humidity (RH) are calculated using a Mie theory aerosol optical model, on the basis of field measurements of number–size distribution and hygroscopic growth factor (at RH values above 90%) from the 2009 HaChi (Haze in China) project. Results demonstrate that ambient ω has pronouncedly different diurnal patterns from ω measured at dry state, and is highly sensitive to the ambient RHs. Ambient ω in the NCP can be described by a dry state ω value of 0.863, increasing with the RH following a characteristic RH dependence curve. A Monte Carlo simulation shows that the uncertainty of ω from the propagation of uncertainties in the input parameters decreases from 0.03 (at dry state) to 0.015 (RHs > 90%). The impact of hygroscopic growth on ω is further applied in the calculation of the radiative transfer process. Hygroscopic growth of the studied aerosol particle population generally inhibits the photolysis of NO2 at the ground level, whereas accelerates it above the moist planetary boundary layer. Compared with dry state, the calculated JNO2 at RH of 98% at the height of 1 km increases by 30.4%, because of the enhancement of ultraviolet radiation by the humidified scattering-dominant aerosol particles. The increase of JNO2 due to the aerosol hygroscopic growth above the upper boundary layer may affect the tropospheric photochemical processes and this needs to be taken into account in the atmospheric chemical models.
- ItemHygroscopic properties of atmospheric aerosol particles over the Eastern Mediterranean: Implications for regional direct radiative forcing under clean and polluted conditions(München : European Geopyhsical Union, 2011) Stock, M.; Cheng, Y.F.; Birmili, W.; Massling, A.; Wehner, B.; Müller, T.; Leinert, S.; Kalivitis, N.; Mihalopoulos, N.; Wiedensohler, A.This work examines the effect of direct radiative forcing of aerosols in the eastern Mediterranean troposphere as a function of air mass composition, particle size distribution and hygroscopicity, and relative humidity (RH). During intensive field measurements on the island of Crete, Greece, the hygroscopic properties of atmospheric particles were determined using a Hygroscopicity Tandem Differential Mobility Analyzer (H-TDMA) and a Hygroscopicity Differential Mobility Analyzer-Aerodynamic Particle Sizer (H-DMA-APS). Similar to former studies, the H-TDMA identified three hygroscopic sub-fractions of particles in the sub-μm range: a more hygroscopic group, a less hygroscopic group and a nearly hydrophobic particle group. The average hygroscopic particle growth factors at 90 % RH were a significant function of particle mobility diameter (Dp): 1.42 (± 0.05) at 30 nm compared to 1.63 (± 0.07) at 250 nm. The H-DMA-APS identified up to three hygroscopic sub-fractions at mobility diameters of 1.0 and 1.2 μm. The data recorded between 12 August and 20 October 2005 were classified into four distinct synoptic-scale air mass types distinguishing between different regions of origin (western Mediterranean vs. the Aegean Sea) as well as the degree of continental pollution (marine vs. continentally influenced). The hygroscopic properties of particles with diameter Dp≥150 nm showed the most pronounced dependency on air mass origin, with growth factors in marine air masses exceeding those in continentally influenced air masses. Particle size distributions and hygroscopic growth factors were used to calculate aerosol light scattering coefficients at ambient RH using a Mie model. A main result was the pronounced enhancement of particle scattering over the eastern Mediterranean due to hygroscopic growth, both in the marine and continentally influenced air masses. When RH reached its summer daytime values around 70–80 %, up to 50–70 % of the calculated visibility reduction was due to the hygroscopic growth of the particles by water compared to the effect of the dry particles alone. The estimated aerosol direct radiative forcings for both, marine and continentally influenced air masses were negative indicating a net cooling of the atmosphere due to the aerosol. The radiative forcing ΔFr was nevertheless governed by the total aerosol concentration most of the time: ΔFr was typically more negative for continentally influenced aerosols (ca. −4 W m−2) compared to rather clean marine aerosols (ca. −1.5 W m−2). When RH occasionally reached 90 % in marine air masses, ΔFr even reached values down to −7 W m−2. Our results emphasize, on the basis of explicit particle hygroscopicity measurements, the relevance of ambient RH for the radiative forcing of regional atmospheres.
- ItemA parameterization of low visibilities for hazy days in the North China Plain(München : European Geopyhsical Union, 2012) Chen, J.; Zhao, C.S.; Ma, N.; Liu, P.F.; Göbel, T.; Hallbauer, E.; Deng, Z.Z.; Ran, L.; Xu, W.Y.; Liang, Z.; Liu, H.J.; Yan, P.; Zhou, X.J.; Wiedensohler, A.Visibility degradation is a pervasive and urgent environmental problem in China. The occurrence of low visibility events is frequent in the North China Plain, where the aerosol loading is quite high and aerosols are strongly hygroscopic. A parameterization of light extinction (Kex) for low visibilities on hazy days is proposed in this paper, based on visibility, relative humidity (RH), aerosol hygroscopic growth factors and particle number size distributions measured during the Haze in China (HaChi) Project. Observational results show that a high aerosol volume concentration is responsible for low visibility at RH <90%; while for RH >90%, decrease of visibility is mainly influenced by the increase of RH. The parameterization of Kex is developed on the basis of aerosol volume concentrations and RH, taking into accounts the sensitivity of visibility to the two factors and the availability of corresponding data. The extinction coefficients calculated with the parameterization schemes agree well with the directly measured values.
- ItemMobility particle size spectrometers: Harmonization of technical standards and data structure to facilitate high quality long-term observations of atmospheric particle number size distributions(München : European Geopyhsical Union, 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.
- ItemThe Fifth International Workshop on Ice Nucleation phase 2 (FIN-02): Laboratory intercomparison of ice nucleation measurements(Katlenburg-Lindau : Copernicus, 2018) DeMott, Paul J.; Möhler, Ottmar; Cziczo, Daniel J.; Hiranuma, Naruki; Petters, Markus D.; Petters, Sarah S.; Belosi, Franco; Bingemer, Heinz G.; Brooks, Sarah D.; Budke, Carsten; Burkert-Kohn, Monika; Collier, Kristen N.; Danielczok, Anja; Eppers, Oliver; Felgitsch, Laura; Garimella, Sarvesh; Grothe, Hinrich; Herenz, Paul; Hill, Thomas C. J.; Höhler, Kristina; Kanji, Zamin A.; Kiselev, Alexei; Koop, Thomas; Kristensen, Thomas B.; Krüger, Konstantin; Kulkarni, Gourihar; Levin, Ezra J. T.; Murray, Benjamin J.; Nicosia, Alessia; O'Sullivan, Daniel; Peckhaus, Andreas; Polen, Michael J.; Price, Hannah C.; Reicher, Naama; Rothenberg, Daniel A.; Rudich, Yinon; Santachiara, Gianni; Schiebel, Thea; Schrod, Jann; Seifried, Teresa M.; Stratmann, Frank; Sullivan, Ryan C.; Suski, Kaitlyn J.; Szakáll, Miklós; Taylor, Hans P.; Ullrich, Romy; Vergara-Temprado, Jesus; Wagner, Robert; Whale, Thomas F.; Weber, Daniel; Welti, André; Wilson, Theodore W.; Wolf, Martin J.; Zenker, JakeThe second phase of the Fifth International Ice Nucleation Workshop (FIN-02) involved the gathering of a large number of researchers at the Karlsruhe Institute of Technology's Aerosol Interactions and Dynamics of the Atmosphere (AIDA) facility to promote characterization and understanding of ice nucleation measurements made by a variety of methods used worldwide. Compared to the previous workshop in 2007, participation was doubled, reflecting a vibrant research area. Experimental methods involved sampling of aerosol particles by direct processing ice nucleation measuring systems from the same volume of air in separate experiments using different ice nucleating particle (INP) types, and collections of aerosol particle samples onto filters or into liquid for sharing amongst measurement techniques that post-process these samples. In this manner, any errors introduced by differences in generation methods when samples are shared across laboratories were mitigated. Furthermore, as much as possible, aerosol particle size distribution was controlled so that the size limitations of different methods were minimized. The results presented here use data from the workshop to assess the comparability of immersion freezing measurement methods activating INPs in bulk suspensions, methods that activate INPs in condensation and/or immersion freezing modes as single particles on a substrate, continuous flow diffusion chambers (CFDCs) directly sampling and processing particles well above water saturation to maximize immersion and subsequent freezing of aerosol particles, and expansion cloud chamber simulations in which liquid cloud droplets were first activated on aerosol particles prior to freezing. The AIDA expansion chamber measurements are expected to be the closest representation to INP activation in atmospheric cloud parcels in these comparisons, due to exposing particles freely to adiabatic cooling. The different particle types used as INPs included the minerals illite NX and potassium feldspar (K-feldspar), two natural soil dusts representative of arable sandy loam (Argentina) and highly erodible sandy dryland (Tunisia) soils, respectively, and a bacterial INP (Snomax®). Considered together, the agreement among post-processed immersion freezing measurements of the numbers and fractions of particles active at different temperatures following bulk collection of particles into liquid was excellent, with possible temperature uncertainties inferred to be a key factor in determining INP uncertainties. Collection onto filters for rinsing versus directly into liquid in impingers made little difference. For methods that activated collected single particles on a substrate at a controlled humidity at or above water saturation, agreement with immersion freezing methods was good in most cases, but was biased low in a few others for reasons that have not been resolved, but could relate to water vapor competition effects. Amongst CFDC-style instruments, various factors requiring (variable) higher supersaturations to achieve equivalent immersion freezing activation dominate the uncertainty between these measurements, and for comparison with bulk immersion freezing methods. When operated above water saturation to include assessment of immersion freezing, CFDC measurements often measured at or above the upper bound of immersion freezing device measurements, but often underestimated INP concentration in comparison to an immersion freezing method that first activates all particles into liquid droplets prior to cooling (the PIMCA-PINC device, or Portable Immersion Mode Cooling chAmber-Portable Ice Nucleation Chamber), and typically slightly underestimated INP number concentrations in comparison to cloud parcel expansions in the AIDA chamber; this can be largely mitigated when it is possible to raise the relative humidity to sufficiently high values in the CFDCs, although this is not always possible operationally. Correspondence of measurements of INPs among direct sampling and post-processing systems varied depending on the INP type. Agreement was best for Snomax® particles in the temperature regime colder than -10°C, where their ice nucleation activity is nearly maximized and changes very little with temperature. At temperatures warmer than -10°C, Snomax® INP measurements (all via freezing of suspensions) demonstrated discrepancies consistent with previous reports of the instability of its protein aggregates that appear to make it less suitable as a calibration INP at these temperatures. For Argentinian soil dust particles, there was excellent agreement across all measurement methods; measures ranged within 1 order of magnitude for INP number concentrations, active fractions and calculated active site densities over a 25 to 30°C range and 5 to 8 orders of corresponding magnitude change in number concentrations. This was also the case for all temperatures warmer than -25°C in Tunisian dust experiments. In contrast, discrepancies in measurements of INP concentrations or active site densities that exceeded 2 orders of magnitude across a broad range of temperature measurements found at temperatures warmer than -25°C in a previous study were replicated for illite NX. Discrepancies also exceeded 2 orders of magnitude at temperatures of -20 to -25°C for potassium feldspar (K-feldspar), but these coincided with the range of temperatures at which INP concentrations increase rapidly at approximately an order of magnitude per 2°C cooling for K-feldspar. These few discrepancies did not outweigh the overall positive outcomes of the workshop activity, nor the future utility of this data set or future similar efforts for resolving remaining measurement issues. Measurements of the same materials were repeatable over the time of the workshop and demonstrated strong consistency with prior studies, as reflected by agreement of data broadly with parameterizations of different specific or general (e.g., soil dust) aerosol types. The divergent measurements of the INP activity of illite NX by direct versus post-processing methods were not repeated for other particle types, and the Snomax° data demonstrated that, at least for a biological INP type, there is no expected measurement bias between bulk collection and direct immediately processed freezing methods to as warm as -10°C. Since particle size ranges were limited for this workshop, it can be expected that for atmospheric populations of INPs, measurement discrepancies will appear due to the different capabilities of methods for sampling the full aerosol size distribution, or due to limitations on achieving sufficient water supersaturations to fully capture immersion freezing in direct processing instruments. Overall, this workshop presents an improved picture of present capabilities for measuring INPs than in past workshops, and provides direction toward addressing remaining measurement issues.
- ItemAerosol hygroscopicity parameter derived from the light scattering enhancement factor measurements in the North China Plain(Göttingen : Copernicus, 2014) Chen, J.; Zhao, C.S.; Ma, N.; Yan, P.The relative humidity (RH) dependence of aerosol light scattering is an essential parameter for accurate estimation of the direct radiative forcing induced by aerosol particles. Because of insufficient information on aerosol hygroscopicity in climate models, a more detailed parameterization of hygroscopic growth factors and resulting optical properties with respect to location, time, sources, aerosol chemistry and meteorology are urgently required. In this paper, a retrieval method to calculate the aerosol hygroscopicity parameter, κ, is proposed based on the in situ measured aerosol light scattering enhancement factor, namely f(RH), and particle number size distribution (PNSD) obtained from the HaChi (Haze in China) campaign. Measurements show that f(RH) increases sharply with increasing RH, and that the time variance of f(RH) is much greater at higher RH. A sensitivity analysis reveals that the f(RH) is more sensitive to the aerosol hygroscopicity than PNSD. f(RH) for polluted cases is distinctly higher than that for clean periods at a specific RH. The derived equivalent κ, combined with the PNSD measurements, is applied in the prediction of the cloud condensation nuclei (CCN) number concentration. The predicted CCN number concentration with the derived equivalent κ agrees well with the measured ones, especially at high supersaturations. The proposed calculation algorithm of κ with the f(RH) measurements is demonstrated to be reasonable and can be widely applied.
- ItemWater uptake by biomass burning aerosol at sub- and supersaturated conditions: closure studies and implications for the role of organics(München : European Geopyhsical Union, 2011) Dusek, U.; Frank, G.P.; Massling, A.; Zeromskiene, K.; Iinuma, Y.; Schmid, O.; Helas, G.; Hennig, T.; Wiedensohler, A.; Andreae, M.O.We investigate the CCN activity of freshly emitted biomass burning particles and their hygroscopic growth at a relative humidity (RH) of 85%. The particles were produced in the Mainz combustion laboratory by controlled burning of various wood types. The water uptake at sub- and supersaturations is parameterized by the hygroscopicity parameter, κ (c.f. Petters and Kreidenweis, 2007). For the wood burns, κ is low, generally around 0.06. The main emphasis of this study is a comparison of κ derived from measurements at sub- and supersaturated conditions (κG and κCCN), in order to see whether the water uptake at 85% RH can predict the CCN properties of the biomass burning particles. Differences in κGand κCCN can arise through solution non-idealities, the presence of slightly soluble or surface active compounds, or non-spherical particle shape. We find that κG and κCCN agree within experimental uncertainties (of around 30%) for particle sizes of 100 and 150 nm; only for 50 nm particles is κCCN larger than κG by a factor of 2. The magnitude of this difference and its dependence on particle size is consistent with the presence of surface active organic compounds. These compounds mainly facilitate the CCN activation of small particles, which form the most concentrated solution droplets at the point of activation. The 50 nm particles, however, are only activated at supersaturations higher than 1% and are therefore of minor importance as CCN in ambient clouds. By comparison with the actual chemical composition of the biomass burning particles, we estimate that the hygroscopicity of the water-soluble organic carbon (WSOC) fraction can be represented by a κWSOC value of approximately 0.2. The effective hygroscopicity of a typical wood burning particle can therefore be represented by a linear mixture of an inorganic component with κ ≅ 0.6, a WSOC component with κ ≅ 0.2, and an insoluble component with κ = 0.
- ItemA study of aerosol liquid water content based on hygroscopicity measurements at high relative humidity in the North China Plain(München : European Geopyhsical Union, 2014) Bian, Y.X.; Zhao, C.S.; Ma, N.; Chen, J.; Xu, W.Y.Water can be a major component of aerosol particles, also serving as a medium for aqueous-phase reactions. In this study, a novel method is presented to calculate the aerosol liquid water content at high relative humidity based on measurements of aerosol hygroscopic growth factor, particle number size distribution and relative humidity in the Haze in China (HaChi) summer field campaign (July–August 2009) in the North China Plain. The aerosol liquid water content calculated using this method agreed well with that calculated using a thermodynamic equilibrium model (ISORROPIA II) at high relative humidity (>60%) with a correlation coefficient of 0.96. At low relative humidity (<60%), an underestimation was found in the calculated aerosol liquid water content by the thermodynamic equilibrium model. This discrepancy mainly resulted from the ISORROPIA II model, which only considered limited aerosol chemical compositions. The mean and maximum values of aerosol liquid water content during the HaChi campaign reached 1.69 × 10−4 g m−3 and 9.71 × 10−4 g m−3, respectively. A distinct diurnal variation of the aerosol liquid water content was found, with lower values during daytime and higher ones at night. The aerosol liquid water content depended strongly on the relative humidity. The aerosol liquid water content in the accumulation mode dominated the total aerosol liquid water content.