Impact of cloud processes on aerosol particle properties: results from two ATR-42 flights in an extended stratocumulus cloud layer during the EUCAARI campaign (2008)

Abstract. Within the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) project, the Meteo France research aircraft ATR-42 was operated from Rotterdam airport during May 2008, to perform scientific flights dedicated to the investigation of aerosol-cloud interactions. Therein, the objective of this study is to illustrate the impact of cloud processing on the aerosol particles physical and chemical properties. The presented results are retrieved from measurements during a double-flight mission from Rotterdam (Netherlands) to Newcastle (UK) and back using data measured with compact Time of Flight Aerosol Mass Spectrometer (cToF-AMS) and Scanning Mobility Particle Sizer (SMPS). Cloud-related measurements during these flights were performed over the North Sea within as well as in close vicinity of a marine stratocumulus cloud layer. Particle physical and chemical properties observed in the close vicinity (V), below and above the stratocumulus cloud show strong differences. Firstly, measurements at constant altitude above the cloud layer show decreasing mass concentrations with decreasing horizontal distance (210–0 km) to the cloud layer by a factor up to 7, whereas below the cloud and by same means of distance, the mass concentrations merely decrease by a factor of 2 on average. Secondly, the averaged aerosol size distributions, observed above and below the cloud layer, are of bimodal character with pronounced minima between Aitken and accumulation mode which is potentially the consequence of cloud processing. Finally, the chemical composition of aerosol particles is strongly dependent on the location relative to the cloud layer (vicinity or below/above cloud). In general, the nitrate and organic fractions decrease with decreasing distance to the cloud, in the transit from cloud–free conditions towards the cloud boundaries. The decrease of nitrate and organic compounds ranges at a factor of three to ten, affecting sulfate and ammonium compounds to be increasingly abundant in the aerosol chemical composition while approaching the cloud layer. Finally, the chemical composition of non-refractory evaporated cloud droplets measured within the cloud shows increased fractions of nitrate and organics (with respect to concentrations found below clouds), but also large amounts of sulfate, thus, related to activation of particles, made up of soluble compounds.

[1]  A.J.H. Visschedijk,et al.  General overview: European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) - integrating aerosol research from nano to global scales , 2011 .

[2]  Alan Gadian,et al.  Cloud‐aerosol interactions for boundary layer stratocumulus in the Lagrangian Cloud Model , 2010 .

[3]  Evgueni I. Kassianov,et al.  The multi-scale aerosol-climate model PNNL-MMF: model description and evaluation , 2010 .

[4]  J. Jimenez,et al.  Characterization of particle cloud droplet activity and composition in the free troposphere and the boundary layer during INTEX-B , 2010 .

[5]  J. Abbatt,et al.  Chemical evolution of secondary organic aerosol from OH-initiated heterogeneous oxidation , 2010 .

[6]  L. Gomes,et al.  Cloud processing of mineral dust: direct comparison of cloud residual and clear sky particles during AMMA aircraft campaign in summer 2006 , 2010 .

[7]  H. Wernli,et al.  Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN) , 2009 .

[8]  Sonia M. Kreidenweis,et al.  Effect of chemical mixing state on the hygroscopicity and cloud nucleation properties of calcium mineral dust particles , 2009 .

[9]  L. Gomes,et al.  Increase of the aerosol hygroscopicity by cloud processing in a mesoscale convective system: a case study from the AMMA campaign , 2008 .

[10]  J. Jimenez,et al.  Design and Operation of a Pressure-Controlled Inlet for Airborne Sampling with an Aerodynamic Aerosol Lens , 2008 .

[11]  P. Laj,et al.  Design and Validation of a 6-Volatility Tandem Differential Mobility Analyzer (VTDMA) , 2007 .

[12]  Kenneth A. Smith,et al.  Transmission Efficiency of an Aerodynamic Focusing Lens System: Comparison of Model Calculations and Laboratory Measurements for the Aerodyne Aerosol Mass Spectrometer , 2007 .

[13]  S. Howell,et al.  Results from the DC-8 Inlet Characterization Experiment (DICE): Airborne Versus Surface Sampling of Mineral Dust and Sea Salt Aerosols , 2005 .

[14]  Stephan Borrmann,et al.  A New Time-of-Flight Aerosol Mass Spectrometer (TOF-AMS)—Instrument Description and First Field Deployment , 2005 .

[15]  D. R. Worsnop,et al.  Density changes of aerosol particles as a result of chemical reaction , 2004 .

[16]  Kenneth A. Smith,et al.  Numerical Characterization of Particle Beam Collimation: Part II Integrated Aerodynamic-Lens–Nozzle System , 2004 .

[17]  U. Lohmann,et al.  How efficient is cloud droplet formation of organic aerosols? , 2004 .

[18]  D. Worsnop,et al.  Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 2: Application to Combustion-Generated Soot Aerosols as a Function of Fuel Equivalence Ratio , 2004 .

[19]  P. Formenti,et al.  Radiative properties and direct radiative effect of Saharan dust measured by the C-130 aircraft during SHADE: 1. Solar spectrum , 2003 .

[20]  J. Seinfeld,et al.  Parameterization of cloud droplet formation in global climate models , 2003 .

[21]  J. Putaud,et al.  Size‐dependent scavenging efficiencies of multicomponent atmospheric aerosols in clouds , 2003 .

[22]  W. Cotton,et al.  Simulations of aerosol-cloud-dynamical feedbacks resulting from entrainment of aerosol into the marine boundary layer during the Atlantic Stratocumulus Transition Experiment , 2002 .

[23]  Z. Levin,et al.  Interactions of mineral dust particles and clouds: Effects on precipitation and cloud optical properties , 2002 .

[24]  Jingchuan Zhou,et al.  Cloud condensation nuclei in the Amazon Basin: “marine” conditions over a continent? , 2001 .

[25]  S. Ghan,et al.  Kinetic limitations on cloud droplet formation and impact on cloud albedo , 2001 .

[26]  R. Harrison Cloud Formation and the Possible Significance of Charge for Atmospheric Condensation and Ice Nuclei , 2000 .

[27]  Zev Levin,et al.  Modification of mineral dust particles by cloud processing and subsequent effects on drop size distributions , 2000 .

[28]  A. Clarke,et al.  Nucleation in the equatorial free troposphere: Favorable environments during PEM‐Tropics , 1999 .

[29]  A. Stohl,et al.  Validation of the lagrangian particle dispersion model FLEXPART against large-scale tracer experiment data , 1998 .

[30]  Mahoney,et al.  In situ measurements of organics, meteoritic material, mercury, and other elements in aerosols at 5 to 19 kilometers , 1998, Science.

[31]  Fred Gelbard,et al.  A one-dimensional sectional model to simulate multicomponent aerosol dynamics in the marine boundary layer 1. Model description , 1998 .

[32]  M. Wendisch,et al.  Observations and modelling of the processing of aerosol by a hill cap cloud , 1997 .

[33]  Joyce E. Penner,et al.  An assessment of the radiative effects of anthropogenic sulfate , 1997 .

[34]  B. Stevens,et al.  Numerical simulations of stratocumulus processing of cloud condensation nuclei through , 1996 .

[35]  Z. Levin,et al.  The Effects of Desert Particles Coated with Sulfate on Rain Formation in the Eastern Mediterranean , 1996 .

[36]  A. Wexler,et al.  Growth laws for atmospheric aerosol particles: An examination of the bimodality of the accumulation mode , 1995 .

[37]  J. W. Fitzgerald,et al.  Marine boundary layer measurements of new particle formation and the effects nonprecipitating clouds have on aerosol size distribution , 1994 .

[38]  D. Hartmann,et al.  The Effect of Cloud Type on Earth's Energy Balance: Global Analysis , 1992 .

[39]  J. Seinfeld,et al.  Heterogeneous sulfate production in an urban fog , 1992 .

[40]  R. Chervin,et al.  Global distribution of total cloud cover and cloud type amounts over the ocean , 1988 .

[41]  G. M. Frick,et al.  Effect of nonprecipitating clouds on the aerosol size distribution in the marine boundary layer , 1986 .

[42]  Jost Heintzenberg,et al.  In situ sampling of clouds with a droplet to aerosol converter , 1985 .

[43]  William C. Hinds Aerosol Technology: Properties, Behavior, and Measurement of Airborne Particles , 1982 .

[44]  M. Facchini,et al.  Introduction: European Integrated Project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) – integrating aerosol research from nano to global scales , 2009 .

[45]  Kazuhiro Tsuboi,et al.  © Author(s) 2008. This work is distributed under the Creative Commons Attribution 3.0 License. Atmospheric Chemistry and Physics , 2008 .

[46]  Martial Haeffelin,et al.  Le projet Rali: Combinaison d'un radar et d'un lidar pour l'étude des nuages faiblement précipitants , 2004 .

[47]  Ping Yang,et al.  Atmospheric Chemistry and Physics , 2004 .

[48]  J. Heintzenberg,et al.  Incorporation of aerosol particles between 25 and 850 nm into cloud elements: measurements with a new complementary sampling system , 2000 .

[49]  F. Joos,et al.  A field study on chemistry, S(IV) oxidation rates and vertical transport during fog conditions , 1991 .

[50]  Christian Seigneur,et al.  A theoretical investigation of sulfate formation in clouds , 1988 .

[51]  L. Martin Measurements of sulfate production in natural clouds , 1983 .

[52]  P. Hobbs,et al.  Measurements of sulfate production in natural clouds , 1982 .

[53]  H. Köhler The nucleus in and the growth of hygroscopic droplets , 1936 .

[54]  C E Kolb,et al.  Guest Editor: Albert Viggiano CHEMICAL AND MICROPHYSICAL CHARACTERIZATION OF AMBIENT AEROSOLS WITH THE AERODYNE AEROSOL MASS SPECTROMETER , 2022 .