Characterization of particle cloud droplet activity and composition in the free troposphere and the boundary layer during INTEX-B

Abstract. Measurements of cloud condensation nuclei (CCN), aerosol size distributions, and submicron aerosol composition were made as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign during spring 2006. Measurements were conducted from an aircraft platform over the northeastern Pacific and western North America with a focus on how the transport and evolution of Asian pollution across the Pacific Ocean affected CCN properties. A broad range of air masses were sampled and here we focus on three distinct air mass types defined geographically: the Pacific free troposphere (FT), the marine boundary layer (MBL), and the polluted continental boundary layer in the California Central Valley (CCV). These observations add to the few observations of CCN in the FT. CCN concentrations showed a large range of concentrations between air masses, however CCN activity was similar for the MBL and CCV (κ~0.2–0.25). FT air masses showed evidence of long-range transport from Asia and CCN activity was consistently higher than for the boundary layer air masses. Bulk chemical measurements predicted CCN activity reasonably well for the CCV and FT air masses. Decreasing trends in κ with organic mass fraction were observed for the combination of the FT and CCV air masses and can be explained by the measured soluble inorganic chemical components. Changes in hygroscopicity associated with differences in the non-refractory organic composition were too small to be distinguished from the simultaneous changes in inorganic ion composition in the FT and MBL, although measurements for the large organic fractions (0.6–0.8) found in the CCV showed values of the organic fraction hygroscopicity consistent with other polluted regions (κorg~0.1–0.2). A comparison of CCN-derived κ (for particles at the critical diameter) to H-TDMA-derived κ (for particles at 100 nm diameter) showed similar trends, however the CCN-derived κ values were significantly higher.

[1]  Z. Ristovski,et al.  Intercomparison study of six HTDMAs: results and recommendations , 2009 .

[2]  J. Hudson Variability of the relationship between particle size and cloud‐nucleating ability , 2007 .

[3]  A. Prévôt,et al.  Aerosol quantification with the Aerodyne Aerosol Mass Spectrometer: Detection limits and ionizer background effects , 2008 .

[4]  J. Behnke A New Look at Aging , 1975 .

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

[6]  S. Kreidenweis,et al.  Predicting Particle Critical Supersaturation from Hygroscopic Growth Measurements in the Humidified TDMA. Part II: Laboratory and Ambient Studies , 2000 .

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

[8]  Sonia M. Kreidenweis,et al.  A single parameter representation of hygroscopic growth and cloud condensation nucleus activity – Part 3: Including surfactant partitioning , 2012 .

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

[10]  Satoshi Takahama,et al.  Classification of Multiple Types of Organic Carbon Composition in Atmospheric Particles by Scanning Transmission X-Ray Microscopy Analysis , 2007 .

[11]  M. Andreae A New Look at Aging Aerosols , 2009, Science.

[12]  Teresa L. Campos,et al.  Source signatures of carbon monoxide and organic functional groups in Asian Pacific Regional Aerosol Characterization Experiment (ACE-Asia) submicron aerosol types , 2003 .

[13]  P. Quinn,et al.  Carbohydrate-like composition of submicron atmospheric particles and their production from ocean bubble bursting , 2009, Proceedings of the National Academy of Sciences.

[14]  William H. Brune,et al.  Chemistry and transport of pollution over the Gulf of Mexico and the Pacific: spring 2006 INTEX-B campaign overview and first results , 2009 .

[15]  R. Charlson,et al.  Correction to "Dissolution behavior and surface tension effects of organic compounds in nucleating cloud droplets" by Michelle L. Shulman, , 1996 .

[16]  E. Bigg Technique for studying the chemistry of cloud condensation nuclei , 1986 .

[17]  Z. Ristovski,et al.  Observation of the suppression of water uptake by marine particles , 2010 .

[18]  D. Toom‐Sauntry,et al.  Atmospheric Chemistry and Physics the Effect of Organic Compounds on the Growth Rate of Cloud Droplets in Marine and Forest Settings , 2022 .

[19]  W. R. Leaitch,et al.  The hygroscopicity parameter (κ) of ambient organic aerosol at a field site subject to biogenic and anthropogenic influences: relationship to degree of aerosol oxidation , 2010 .

[20]  Mark J. Rood,et al.  Impact of particulate organic matter on the relative humidity dependence of light scattering: A simplified parameterization , 2005 .

[21]  Barry J. Huebert,et al.  Size distributions and mixtures of dust and black carbon aerosol in Asian outflow: Physiochemistry and optical properties , 2004 .

[22]  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 .

[23]  V. Ramanathan,et al.  An overview of aircraft observations from the Pacific Dust Experiment campaign , 2009 .

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

[25]  D. Collins,et al.  Integration of size distributions and size-resolved hygroscopicity measured during the Houston Supersite for compositional categorization of the aerosol , 2004 .

[26]  D. Murphy,et al.  Observations of organic material in individual marine particles at Cape Grim during the First Aerosol Characterization Experiment (ACE 1) , 1998 .

[27]  S. Martin,et al.  Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity , 2009 .

[28]  D. Worsnop,et al.  Physicochemical properties and origin of organic groups detected in boreal forest using an aerosol mass spectrometer , 2009 .

[29]  A. Clarke,et al.  A Pacific Aerosol Survey. Part I: A Decade of Data on Particle Production, Transport, Evolution, and Mixing in the Troposphere* , 2002 .

[30]  V. Ramanathan,et al.  North American and Asian aerosols over the eastern Pacific Ocean and their role in regulating cloud condensation nuclei , 2006 .

[31]  J. Abbatt,et al.  Comparison between measured and predicted CCN concentrations at Egbert, Ontario: Focus on the organic aerosol fraction at a semi-rural site , 2007 .

[32]  I. S. McDermid,et al.  Increasing springtime ozone mixing ratios in the free troposphere over western North America , 2010, Nature.

[33]  R. Synovec,et al.  Dissolution behavior and surface tension effects of organic compounds in nucleating cloud droplets , 1996 .

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

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

[36]  W. G. Collins,et al.  Dust and pollution transport on global scales: Aerosol measurements and model predictions , 2001 .

[37]  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 .

[38]  S. Howell,et al.  Size-distributions and mixtures of black carbon and dust aerosol in Asian outflow: physio-chemistry, optical properties and humidity growth , 2003 .

[39]  D. Collins,et al.  Physical and chemical properties of the aerosol within the southeastern Pacific marine boundary layer , 2007 .

[40]  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 .

[41]  D. Lide Handbook of Chemistry and Physics , 1992 .

[42]  R. Martin,et al.  Evidence for Asian dust effects from aerosol plume measurements during INTEX-B 2006 near Whistler, BC , 2009 .

[43]  Youhua Tang,et al.  Trans‐Pacific transport of black carbon and fine aerosols (D < 2.5 μm) into North America , 2007 .

[44]  Yutaka Kondo,et al.  Oxygenated and water‐soluble organic aerosols in Tokyo , 2007 .

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

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

[47]  D. Topping,et al.  Consistency between parameterisations of aerosol hygroscopicity and CCN activity during the RHaMBLe discovery cruise , 2009 .

[48]  B. Stephens,et al.  Black carbon over Mexico: the effect of atmospheric transport on mixing state, mass absorption cross-section, and BC/CO ratios , 2009 .

[49]  U. Baltensperger,et al.  Hygroscopic properties of submicrometer atmospheric aerosol particles measured with H-TDMA instruments in various environments—a review , 2008 .

[50]  John H. Seinfeld,et al.  The formation, properties and impact of secondary organic aerosol: current and emerging issues , 2009 .

[51]  D. Lenschow,et al.  Bidirectional mixing in an ACE 1 marine boundary layer overlain by a second turbulent layer , 1998 .

[52]  Louisa Emmons,et al.  © Author(s) 2008. This work is distributed under the Creative Commons Attribution 3.0 License. Atmospheric Chemistry and Physics Fast airborne aerosol size and chemistry measurements above , 2008 .

[53]  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 .

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

[55]  J. Penner,et al.  Organic aerosols in the Caribbean trade winds: A natural source? , 1997 .

[56]  J. Jimenez,et al.  A simplified description of the evolution of organic aerosol composition in the atmosphere , 2010 .

[57]  Antony D. Clarke,et al.  Particle production in the remote marine atmosphere: Cloud outflow and subsidence during ACE 1 , 1998 .

[58]  S. Takahama,et al.  Organic composition of single and submicron particles in different regions of western North America and the eastern Pacific during INTEX-B 2006 , 2009 .

[59]  R. C. Weast CRC Handbook of Chemistry and Physics , 1973 .

[60]  Qi Zhang,et al.  O/C and OM/OC ratios of primary, secondary, and ambient organic aerosols with high-resolution time-of-flight aerosol mass spectrometry. , 2008, Environmental science & technology.

[61]  P. DeCarlo,et al.  Elemental analysis of organic species with electron ionization high-resolution mass spectrometry. , 2007, Analytical chemistry.

[62]  Charles E. Kolb,et al.  Ambient aerosol sampling using the Aerodyne Aerosol Mass Spectrometer , 2003 .

[63]  L. Russell,et al.  Mapping organic coatings on atmospheric particles , 2002 .

[64]  T. Bond,et al.  Light Absorption by Carbonaceous Particles: An Investigative Review , 2006 .

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

[66]  U. Lohmann,et al.  Characterization of the aerosol over the sub-arctic north east Pacific Ocean , 2006 .

[67]  Louisa Emmons,et al.  Evolution of Asian aerosols during transpacific transport in INTEX-B , 2008 .

[68]  D. R. Worsnop,et al.  Evolution of Organic Aerosols in the Atmosphere , 2009, Science.

[69]  S. Howell,et al.  Biomass burning and pollution aerosol over North America: Organic components and their influence on spectral optical properties and humidification response , 2007 .