Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydro- logical cycle and climate. We have measured and charac- terized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activ- ity of aerosol particles varied in the range of 0.1-0.4 (0.16±0.06 arithmetic mean and standard deviation). The overall median value of 0.15 was by a factor of two lower than the values typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles ( 0.1 at D 50 nm; 0.2 at D 200 nm), which is in agreement with earlier hygroscopicity tandem differential mobility ana- lyzer (H-TDMA) studies. The CCN measurement results are consistent with aerosol mass spectrometry (AMS) data, showing that the organic mass fraction (forg) was on average as high as 90% in the Aitken mode (D 100 nm) and decreased with increas- ing particle diameter in the accumulation mode ( 80% at D 200 nm). The values exhibited a negative linear cor-

[1]  G. Feingold Modeling of the first indirect effect: Analysis of measurement requirements , 2003 .

[2]  J. Seinfeld,et al.  Impact of biomass burning on cloud properties in the Amazon Basin , 2003 .

[3]  Spyros N. Pandis,et al.  An Algorithm for the Calculation of Secondary Organic Aerosol Density Combining AMS and SMPS Data , 2007 .

[4]  J. Slowik,et al.  Slower CCN growth kinetics of anthropogenic aerosol compared to biogenic aerosol observed at a rural site , 2010 .

[5]  A. Nenes,et al.  A Continuous-Flow Streamwise Thermal-Gradient CCN Chamber for Atmospheric Measurements , 2005 .

[6]  M. Andreae,et al.  Sensitivity of CCN spectra on chemical and physical properties of aerosol: A case study from the Amazon Basin , 2002 .

[7]  J. Martins,et al.  Large-scale aerosol source apportionment in Amazonia , 1998 .

[8]  M. Andreae,et al.  Size distribution and hygroscopic properties of aerosol particles from dry-season biomass burning in Amazonia , 2005 .

[9]  M. Petters,et al.  Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol: Part 1 – Evidence from measurements , 2009 .

[10]  Qi Chen,et al.  Increased cloud activation potential of secondary organic aerosol for atmospheric mass loadings , 2009 .

[11]  J. Martins,et al.  Cloud condensation nuclei from biomass burning during the Amazonian dry-to-wet transition season , 2009 .

[12]  A. Nenes,et al.  CCN closure and droplet growth kinetics , 2009 .

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

[14]  M. Andreae,et al.  Physical properties of the sub-micrometer aerosol over the Amazon rain forest during the wet-to-dry season transition - comparison of modeled and measured CCN concentrations , 2004 .

[15]  M. Andreae Aerosols Before Pollution , 2007, Science.

[16]  G. Feingold,et al.  Cloud–Aerosol Interactions from the Micro to the Cloud Scale , 2009 .

[17]  M. Andreae,et al.  Smoking Rain Clouds over the Amazon , 2004, Science.

[18]  Ernst Strüngmann Forum,et al.  Clouds in the perturbed climate system : their relationship to energy balance, atmospheric dynamics, and precipitation , 2009 .

[19]  Maria Cristina Facchini,et al.  The effect of physical and chemical aerosol properties on warm cloud droplet activation , 2005 .

[20]  Meinrat O. Andreae,et al.  Robust relations between CCN and the vertical evolution of cloud drop size distribution in deep convective clouds , 2005 .

[21]  J. Jimenez,et al.  Mass spectral characterization of submicron biogenic organic particles in the Amazon Basin , 2009 .

[22]  A. Nenes,et al.  Relating CCN activity, volatility, and droplet growth kinetics of β-caryophyllene secondary organic aerosol , 2008 .

[23]  Technical note: A method for measuring size-resolved CCN in the atmosphere , 2006 .

[24]  S. Martin,et al.  Cloud condensation nucleus activity of secondary organic aerosol particles mixed with sulfate , 2007 .

[25]  A. Slingo,et al.  Clouds in the Perturbed Climate System , 2010 .

[26]  G. Roberts Interactive comment on “ Cloud condensation nuclei in pristine tropical rainforest air of Amazonia : size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity ” by S . S . Gunthe et al . , 2009 .

[27]  Meinrat O. Andreae,et al.  Aerosol cloud precipitation interactions. Part 1. The nature and sources of cloud-active aerosols , 2008 .

[28]  M. Petters,et al.  A single parameter representation of hygroscopic growth and cloud condensation nucleus activity , 2006 .

[29]  Yoram J. Kaufman,et al.  Analysis of smoke impact on clouds in Brazilian biomass burning regions: An extension of Twomey's approach , 2001 .

[30]  M. Garstang,et al.  Aerosol chemistry during the wet season in central Amazonia - The influence of long-range transport , 1990 .

[31]  Douglas R. Worsnop,et al.  Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 1: Theory , 2004 .

[32]  Douglas R. Worsnop,et al.  Laboratory and Ambient Particle Density Determinations using Light Scattering in Conjunction with Aerosol Mass Spectrometry , 2007 .

[33]  M. Petters,et al.  Towards closing the gap between hygroscopic growth and activation for secondary organic aerosol - Part 2: Theoretical approaches , 2008 .

[34]  Martin Gysel,et al.  Cloud forming potential of secondary organic aerosol under near atmospheric conditions , 2008 .

[35]  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 .

[36]  S. Kinne Climatologies of cloud-related aerosols. Part 1: Particle number and size , 2009 .

[37]  Katrin Fuhrer,et al.  Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer. , 2006, Analytical chemistry.

[38]  S. Martin,et al.  An overview of the Amazonian Aerosol Characterization Experiment 2008 (AMAZE-08) , 2010 .

[39]  P. Paatero,et al.  Evaluation of an automatic algorithm for fitting the particle number size distributions , 2005 .

[40]  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 .

[41]  N. Takegawa,et al.  Rapid aerosol particle growth and increase of cloud condensation nucleus activity by secondary aerosol formation and condensation: A case study for regional air pollution in northeastern China , 2009 .

[42]  S. Martin,et al.  Sources and properties of Amazonian aerosol particles , 2010 .

[43]  Ruprecht Jaenicke,et al.  Chapter 1 Tropospheric Aerosols , 1993 .

[44]  S. Martin,et al.  Amorphous and crystalline aerosol particles interacting with water vapor - Part 1: Microstructure, phase transitions, hygroscopic growth and kinetic limitations , 2009 .

[45]  H. Tanimoto,et al.  Cloud condensation nuclei activity at Jeju Island, Korea in spring 2005 , 2007 .

[46]  M. Andreae,et al.  Cloud-nucleating properties of the Amazonian biomass burning aerosol: Cloud condensation nuclei measurements and modeling , 2007 .

[47]  Tomas Alsberg,et al.  Estimation of the average molecular weight of humic-like substances isolated from fine atmospheric aerosol , 2003 .

[48]  Y. H. Zhang,et al.  Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 1: Size-resolved measurements and implications for the modeling of aerosol particle hygroscopicity and CCN activity , 2008 .

[49]  Y. H. Zhang,et al.  Cloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 2: Size-resolved aerosol chemical composition, diurnal cycles, and externally mixed weakly CCN-active soot particles , 2010 .

[50]  S. Gunthe Cloud condensation nuclei in pristine tropical rainforest air of Amazonia , 2009 .

[51]  J. Jimenez,et al.  Aerosol optical properties relevant to regional remote sensing of CCN activity and links to their organic mass fraction : airborne observations over Central Mexico and the US West Coast during MILAGRO / , 2009 .

[52]  Spyros N. Pandis,et al.  CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol , 2008 .

[53]  M. Petters,et al.  Single-parameter estimates of aerosol water content , 2008 .

[54]  G. Láng,et al.  How many carboxyl groups does an average molecule of humic-like substances contain? , 2008 .

[55]  P. Artaxo,et al.  Aerosol characteristics and sources for the Amazon Basin during the wet season , 1990 .

[56]  D. Hauglustaine,et al.  Change in global aerosol composition since preindustrial times , 2006 .

[57]  J. Seinfeld,et al.  Atmospheric Chemistry and Physics: From Air Pollution to Climate Change , 1998 .

[58]  Jian Wang,et al.  Effects of aerosol organics on cloud condensation nucleus (CCN) concentration and first indirect aerosol effect , 2008 .

[59]  C. O'Dowd,et al.  Flood or Drought: How Do Aerosols Affect Precipitation? , 2008, Science.

[60]  J. Smith,et al.  Mapping the Operation of the DMT Continuous Flow CCN Counter , 2006 .

[61]  M. Petters,et al.  A single parameter representation of hygroscopic growth and cloud condensation nucleus activity – Part 2: Including solubility , 2008 .

[62]  H. L. Miller,et al.  Climate Change 2007: The Physical Science Basis , 2007 .

[63]  Sonia M. Kreidenweis,et al.  Cloud droplet activation of secondary organic aerosol , 2007 .

[64]  A. Nenes,et al.  Cloud condensation nuclei closure during the International Consortium for Atmospheric Research on Transport and Transformation 2004 campaign: Effects of size-resolved composition , 2007 .

[65]  M. Cubison,et al.  Prediction of cloud condensation nucleus number concentration using measurements of aerosol size distributions and composition and light scattering enhancement due to humidity , 2007 .

[66]  J. Klett,et al.  Microphysics of Clouds and Precipitation , 1978, Nature.

[67]  Ulrich Pöschl,et al.  Calibration and measurement uncertainties of a continuous-flow cloud condensation nuclei counter (DMT-CCNC): CCN activation of ammonium sulfate and sodium chloride aerosol particles in theory and experiment , 2007 .

[68]  M. Andreae,et al.  Enhanced organic mass fraction and decreased hygroscopicity of cloud condensation nuclei (CCN) during new particle formation events , 2010 .

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

[70]  Alfred Wiedensohler,et al.  Hygroscopic growth and measured and modeled critical super‐saturations of an atmospheric HULIS sample , 2007 .

[71]  Shao-Meng Li,et al.  Closure between measured and modeled cloud condensation nuclei ( CCN ) using size-resolved aerosol compositions in downtown Toronto , 2005 .

[72]  M. Andreae,et al.  Physical and chemical properties of aerosols in the wet and dry seasons in Rondônia, Amazonia , 2002 .

[73]  J. Seinfeld,et al.  Comprehensive airborne characterization of aerosol from a major bovine source , 2008 .

[74]  M. Andreae Correlation between cloud condensation nuclei concentration and aerosol optical thickness in remote and polluted regions , 2008 .

[75]  Cloud—Aerosol Interactions from the Micro to the Cloud Scale , 2009 .

[76]  M. Andreae,et al.  Size Matters More Than Chemistry for Cloud-Nucleating Ability of Aerosol Particles , 2006, Science.

[77]  M. Petters,et al.  Cloud Particle Precursors , 2009 .

[78]  W. Cotton,et al.  Aerosol pollution impact on precipitation : a scientific review , 2009 .

[79]  M. V. Ramana,et al.  Simultaneous observations of aerosol–cloud–albedo interactions with three stacked unmanned aerial vehicles , 2008, Proceedings of the National Academy of Sciences.

[80]  H. Hansson,et al.  Submicrometer aerosol particle size distribution and hygroscopic growth measured in the Amazon rain forest during the wet season , 2002 .

[81]  H. Masunaga,et al.  Temporal and spatial variability of clouds and related aerosols , 2009 .