Size distribution of EC and OC in the aerosol of Alpine valleys during summer and winter

Abstract. Collections of samples were conducted for the determination of the size distributions of EC and OC during the intensive sampling campaigns of the POVA program, in two Alpine valleys of the French Alps, in summer and in winter. The comparison of concentrations obtained for samples collected in parallel with impactor- and filter-based methods is rather positive with slopes of 0.95 and 0.76 for OC and EC, respectively and correlations close to 1 (0.92 and 0.90 for OC and EC, respectively, n=26). This is an indication that the correction of pyrolysis seems to work for the impactor samples despite non even deposits. The size distributions of the concentrations of EC and OC present large evolutions between winter and summer, and between a suburban and a rural site. In winter, an overwhelming proportion of the mass fraction of both species is found in the droplet and accumulation modes, often (but not always) in association with sulfate and other chemical species resulting from secondary formation processes. Some indications of gas/particles exchanges can be found for the other parts of the size spectrum (the Aitken and super micron modes) in the case of the rural site. In summer, the changes are more drastic with, according to the case, a dominant droplet or accumulation mode. Particularly at the rural site, the large extent of processing of the aerosol due to gas/particles exchanges is evident for the Aitken and super micron modes, with increasing of the OC mass fractions in these size ranges. All of these observations give indications on the degree of internal vs. external mixing of the species investigated in the different modes.

[1]  Glen R. Cass,et al.  Sources of fine organic aerosol. 2. Noncatalyst and catalyst-equipped automobiles and heavy-duty diesel trucks , 1993 .

[2]  P. Masclet,et al.  Polycyclic aromatic hydrocarbons (PAHs) in the atmospheres of two French alpine valleys: sources and temporal patterns , 2004 .

[3]  J. Putaud,et al.  INTERCOMP2000: the comparability of methods in use in Europe for measuring the carbon content of aerosol , 2004 .

[4]  R. Hitzenberger,et al.  Comparison of black carbon (BC) aerosols in two urban areas – concentrations and size distributions , 2001 .

[5]  J. Jaffrezo,et al.  Seasonal variations of the water soluble organic carbon mass fraction of aerosol in two valleys of the French Alps , 2005 .

[6]  Sonia M. Kreidenweis,et al.  A modeling study of aqueous production of dicarboxylic acids: 1. Chemical pathways and speciated organic mass production , 2004 .

[7]  B. Turpin Options for characterizing organic particulate matter new research strategies could help elucidate the mechanisms and causes of aerosol health effects , 1999 .

[8]  Timo Mäkelä,et al.  Characterization of the Particulate Phase in the Exhaust from a Diesel Car , 1997 .

[9]  Barbara J. Turpin,et al.  Secondary organic aerosol formation in cloud and fog droplets: a literature evaluation of plausibility , 2000 .

[10]  Delbert J. Eatough,et al.  Semi-volatile secondary organic aerosol in urban atmospheres: meeting a measurement challenge , 2003 .

[11]  K. Dreher,et al.  Particulate Matter Physicochemistry and Toxicology: In Search of Causality—A Critical Perspective , 2000, Inhalation toxicology.

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

[13]  Ilhan Olmez,et al.  Physical and Chemical Characterization of Atmospheric Ultrafine Particles in the Los Angeles Area , 1998 .

[14]  Guillaume Brulfert Modélisation des circulations atmosphériques pour l'étude de la pollution des vallées alpines , 2004 .

[15]  S. Pandis,et al.  Evaluation of secondary organic aerosol formation in winter , 1999 .

[16]  J. C. Cabada,et al.  Mass size distributions and size resolved chemical composition of fine particulate matter at the Pittsburgh supersite , 2004 .

[17]  W. John,et al.  Modes in the size distributions of atmospheric inorganic aerosol , 1990 .

[18]  Á. Molnár,et al.  Seasonal and diurnal variation in the size distribution of fine carbonaceous particles over rural Hungary , 2003 .

[19]  G R Cass,et al.  Measurement of emissions from air pollution sources. 3. C1-C29 organic compounds from fireplace combustion of wood. , 2001, Environmental science & technology.

[20]  N. Marchand Etude de la composante organique de l'aérosol atmosphérique : cas de deux vallées alpines (Chamonix et Maurienne) et développement analytique , 2003 .

[21]  N. Mihalopoulos,et al.  Characterization of carbonaceous aerosols during the MINOS campaign in Crete, July–August 2001: a multi-analytical approach , 2003 .

[22]  Erik Swietlicki,et al.  Organic aerosol and global climate modelling: a review , 2004 .

[23]  R. Cary,et al.  Elemental Carbon-Based Method for Monitoring Occupational Exposures to Particulate Diesel Exhaust , 1996 .

[24]  R. Hillamo,et al.  Measuring the Size Distribution of Atmospheric Organic and Black Carbon Using Impactor Sampling Coupled with Thermal Carbon Analysis: Method Development and Uncertainties , 2002 .

[25]  Michael J. Kleeman,et al.  SIZE AND COMPOSITION DISTRIBUTION OF FINE PARTICULATE MATTER EMITTED FROM MOTOR VEHICLES , 2000 .

[26]  M. Hays,et al.  Nature of unresolved complex mixture in size-distributed emissions from residential wood combustion as measured by thermal desorption-gas chromatography-mass spectrometry , 2004 .

[27]  Hong Yang,et al.  Charring characteristics of atmospheric organic particulate matter in thermal analysis. , 2002, Environmental science & technology.

[28]  Hans Moosmüller,et al.  Equivalence of elemental carbon by thermal/optical reflectance and transmittance with different temperature protocols. , 2004, Environmental science & technology.

[29]  Michael J. Kleeman,et al.  MEASUREMENT OF EMISSIONS FROM AIR POLLUTION SOURCES. 2. C1 THROUGH C30 ORGANIC COMPOUNDS FROM MEDIUM DUTY DIESEL TRUCKS , 1999 .

[30]  C. Chemel,et al.  Modelling photochemistry in alpine valleys , 2005 .

[31]  Michael J Kleeman,et al.  Measurement of emissions from air pollution sources. 5. C1-C32 organic compounds from gasoline-powered motor vehicles. , 2002, Environmental science & technology.

[32]  K. Sellegri,et al.  Measurements of organic gases during aerosol formation events in the boreal forest atmosphere during QUEST , 2004 .

[33]  R. Hillamo,et al.  Two years of continuous aerosol measurements in northern Finland , 2002 .

[34]  Jian Zhen Yu,et al.  Uncertainties in charring correction in the analysis of elemental and organic carbon in atmospheric particles by thermal/optical methods. , 2002, Environmental science & technology.