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- ItemAerosol hygroscopicity derived from size-segregated chemical composition and its parameterization in the North China Plain(München : European Geopyhsical Union, 2014) Liu, H.J.; Zhao, C.S.; Nekat, B.; Ma, N.; Wiedensohler, A.; van Pinxteren, D.; Spindler, G.; Müller, K.; Herrmann, H.Hygroscopic growth of aerosol particles is of significant importance in quantifying the aerosol radiative effect in the atmosphere. In this study, hygroscopic properties of ambient particles are investigated based on particle chemical composition at a suburban site in the North China Plain during the HaChi campaign (Haze in China) in summer 2009. The size-segregated aerosol particulate mass concentration as well as the particle components such as inorganic ions, organic carbon and water-soluble organic carbon (WSOC) are identified from aerosol particle samples collected with a ten-stage impactor. An iterative algorithm is developed to evaluate the hygroscopicity parameter κ from the measured chemical composition of particles. During the HaChi summer campaign, almost half of the mass concentration of particles between 150 nm and 1 μm is contributed by inorganic species. Organic matter (OM) is abundant in ultrafine particles, and 77% of the particulate mass with diameter (Dp) of around 30 nm is composed of OM. A large fraction of coarse particle mass is undetermined and is assumed to be insoluble mineral dust and liquid water. The campaign's average size distribution of κ values shows three distinct modes: a less hygroscopic mode (Dp < 150 nm) with κ slightly above 0.2, a highly hygroscopic mode (150 nm < Dp < 1 μm) with κ greater than 0.3 and a nearly hydrophobic mode (Dp > 1 μm) with κ of about 0.1. The peak of the κ curve appears around 450 nm with a maximum value of 0.35. The derived κ values are consistent with results measured with a high humidity tandem differential mobility analyzer within the size range of 50–250 nm. Inorganics are the predominant species contributing to particle hygroscopicity, especially for particles between 150 nm and 1 μm. For example, NH4NO3, H2SO4, NH4HSO4 and (NH4)2SO4 account for nearly 90% of κ for particles of around 900 nm. For ultrafine particles, WSOC plays a critical role in particle hygroscopicity due to the predominant mass fraction of OM in ultrafine particles. WSOC for particles of around 30 nm contribute 52% of κ. Aerosol hygroscopicity is related to synoptic transport patterns. When southerly wind dominates, particles are more hygroscopic; when northerly wind dominates, particles are less hygroscopic. Aerosol hygroscopicity also has a diurnal variation, which can be explained by the diurnal evolution of planetary boundary layer, photochemical aging processes during daytime and enhanced black carbon emission at night. κ is highly correlated with mass fractions of SO42−, NO3− and NH4+ for all sampled particles as well as with the mass fraction of WSOC for particles of less than 100 nm. A parameterization scheme for κ is developed using mass fractions of SO42−, NO3−, NH4+ and WSOC due to their high correlations with κ, and κ calculated from the parameterization agrees well with κ derived from the particle's chemical composition. Further analysis shows that the parameterization scheme is applicable to other aerosol studies in China.
- ItemHygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain(München : European Geopyhsical Union, 2011) Liu, P.F.; Zhao, C.S.; Göbel, T.; Hallbauer, E.; Nowak, A.; Ran, L.; Xu, W.Y.; Deng, Z.Z.; Ma, N.; Mildenberger, K.; Henning, S.; Stratmann, F.; Wiedensohler, A.The hygroscopic properties of submicron aerosol particles were determined at a suburban site (Wuqing) in the North China Plain among a cluster of cities during the period 17 July to 12 August, 2009. A High Humidity Tandem Differential Mobility Analyser (HH-TDMA) instrument was applied to measure the hygroscopic growth factor (GF) at 90%, 95% and 98.5% relative humidity (RH) for particles with dry diameters between 50 and 250 nm. The probability distribution of GF (GF-PDF) averaged over the period shows a distinct bimodal pattern, namely, a dominant more-hygroscopic (MH) group and a smaller nearly-hydrophobic (NH) group. The MH group particles were highly hygroscopic, and their GF was relatively constant during the period with average values of 1.54 ± 0.02, 1.81 ± 0.04 and 2.45 ± 0.07 at 90%, 95% and 98.5% RH (D0 = 100 nm), respectively. The NH group particles grew very slightly when exposed to high RH, with GF values of 1.08 ± 0.02, 1.13 ± 0.06 and 1.24 ± 0.13 respectively at 90%, 95% and 98.5% RH (D0 = 100 nm). The hygroscopic growth behaviours at different RHs were well represented by a single-parameter Köhler model. Thus, the calculation of GF as a function of RH and dry diameter could be facilitated by an empirical parameterization of κ as function of dry diameter. A strong diurnal pattern in number fraction of different hygroscopic groups was observed. The average number fraction of NH particles during the day was about 8%, while during the nighttime fractions up to 20% were reached. Correspondingly, the state of mixing in terms of water uptake varied significantly during a day. Simulations using a particle-resolved aerosol box model (PartMC-MOSAIC) suggest that the diurnal variations of aerosol hygroscopicity and mixing state were mainly caused by the evolution of the atmospheric mixing layer. The shallow nocturnal boundary layer during the night facilitated the accumulation of freshly emitted carbonaceous particles (mainly hydrophobic) near the surface while in the morning turbulence entrained the more aged and more hygroscopic particles from aloft and diluted the NH particles near the surface resulting in a decrease in the fraction of NH particles.
- ItemSize-resolved measurement of the mixing state of soot in the megacity Beijing, China: Diurnal cycle, aging and parameterization(München : European Geopyhsical Union, 2012) Cheng, Y.F.; Su, H.; Rose, D.; Gunthe, S.S.; Berghof, M.; Wehner, B.; Achtert, P.; Nowak, A.; Takegawa, N.; Kondo, Y.; Shiraiwa, M.; Gong, Y.G.; Shao, M.; Hu, M.; Zhu, T.; Zhang, Y.H.; Carmichael, G.R.; Wiedensohler, A.; Andreae, M.O.; Pöschl, U.Soot particles are the most efficient light absorbing aerosol species in the atmosphere, playing an important role as a driver of global warming. Their climate effects strongly depend on their mixing state, which significantly changes their light absorbing capability and cloud condensation nuclei (CCN) activity. Therefore, knowledge about the mixing state of soot and its aging mechanism becomes an important topic in the atmospheric sciences. The size-resolved (30–320 nm diameter) mixing state of soot particles in polluted megacity air was measured at a suburban site (Yufa) during the CAREBeijing 2006 campaign in Beijing, using a volatility tandem differential mobility analyzer (VTDMA). Particles in this size range with non-volatile residuals at 300 °C were considered to be soot particles. On average, the number fraction of internally mixed soot in total soot particles (Fin), decreased from 0.80 to 0.57 when initial Dp increased from 30 to 320 nm. Further analysis reveals that: (1) Fin was well correlated with the aerosol hygroscopic mixing state measured by a CCN counter. More externally mixed soot particles were observed when particles showed more heterogeneous features with regard to hygroscopicity. (2) Fin had pronounced diurnal cycles. For particles in the accumulation mode (Dp at 100–320 nm), largest Fin were observed at noon time, with "apparent" turnover rates (kex → in) up to 7.8% h−1. (3) Fin was subject to competing effects of both aging and emissions. While aging increases Fin by converting externally mixed soot particles into internally mixed ones, emissions tend to reduce Fin by emitting more fresh and externally mixed soot particles. Similar competing effects were also found with air mass age indicators. (4) Under the estimated emission intensities, actual turnover rates of soot (kex → in) up to 20% h−1 were derived, which showed a pronounced diurnal cycle peaking around noon time. This result confirms that (soot) particles are undergoing fast aging/coating with the existing high levels of condensable vapors in the megacity Beijing. (5) Diurnal cycles of Fin were different between Aitken and accumulation mode particles, which could be explained by the faster growth of smaller Aitken mode particles into larger size bins. To improve the Fin prediction in regional/global models, we suggest parameterizing Fin by an air mass aging indicator, i.e., Fin = a + bx, where a and b are empirical coefficients determined from observations, and x is the value of an air mass age indicator. At the Yufa site in the North China Plain, fitted coefficients (a, b) were determined as (0.57, 0.21), (0.47, 0.21), and (0.52, 0.0088) for x (indicators) as [NOz]/[NOy], [E]/[X] ([ethylbenzene]/[m,p-xylene]) and ([IM] + [OM])/[EC] ([inorganic + organic matter]/[elemental carbon]), respectively. Such a parameterization consumes little additional computing time, but yields a more realistic description of Fin compared with the simple treatment of soot mixing state in regional/global models.
- 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.
- ItemCharacterization of aerosol properties at Cyprus, focusing on cloud condensation nuclei and ice-nucleating particles(Göttingen : Copernicus GmbH, 2019) Gong, X.; Wex, H.; Müller, T.; Wiedensohler, A.; Höhler, K.; Kandler, K.; Ma, N.; Dietel, B.; Schiebel, T.; Möhler, O.; Stratmann, F.As part of the A-LIFE (Absorbing aerosol layers in a changing climate: aging, LIFEtime and dynamics) campaign, ground-based measurements were carried out in Paphos, Cyprus, to characterize the abundance, properties, and sources of aerosol particles in general and cloud condensation nuclei (CCN) and ice-nucleating particles (INP) in particular. New particle formation (NPF) events with subsequent growth of the particles into the CCN size range were observed. Aitken mode particles featured k values of 0.21 to 0.29, indicating the presence of organic materials. Accumulation mode particles featured a higher hygroscopicity parameter, with a median k value of 0.57, suggesting the presence of sulfate and maybe sea salt particles mixed with organic carbon. A clear downward trend of k with increasing supersaturation and decreasing dcrit was found. Super-micron particles originated mainly from sea-spray aerosol (SSA) and partly from mineral dust. INP concentrations (NINP) were measured in the temperature range from-6:5 to-26:5 °C, using two freezing array-type instruments. NINP at a particular temperature span around 1 order of magnitude below-20 °C and about 2 orders of magnitude at warmer temperatures (T >-18 °C). Few samples showed elevated concentrations at temperatures >-15 °C, which suggests a significant contribution of biological particles to the INP population, which possibly could originate from Cyprus. Both measured temperature spectra and NINP probability density functions (PDFs) indicate that the observed INP (ice active in the temperature range between-15 and-20 °C) mainly originate from long-range transport. There was no correlation between NINP and particle number concentration in the size range> 500 nm (N>500 nm). Parameterizations based on N>500 nm were found to overestimate NINP by about 1 to 2 orders of magnitude. There was also no correlation between NINP and particle surface area concentration. The ice active surface site density (ns) for the polluted aerosol encountered in the eastern Mediterranean in this study is about 1 to 3 orders of magnitude lower than the ns found for dust aerosol particles in previous studies. This suggests that observed NINP PDFs such as those derived here could be a better choice for modeling NINP if the aerosol particle composition is unknown or uncertain.