Direct observation of completely processed calcium carbonate dust particles.

This study presents, for the first time, field evidence of complete, irreversible processing of solid calcium carbonate (calcite)-containing particles and quantitative formation of liquid calcium nitrate particles apparently as a result of heterogeneous reaction of calcium carbonate-containing mineral dust particles with gaseous nitric acid. Formation of nitrates from individual calcite and sea salt particles was followed as a function of time in aerosol samples collected at Shoresh, Israel. Morphology and compositional changes of individual particles were observed using conventional scanning electron microscopy with energy dispersive analysis of X-rays (SEM/EDX) and computer controlled SEM/EDX. Environmental scanning electron microscopy (ESEM) was utilized to determine and demonstrate the hygroscopic behavior of calcium nitrate particles found in some of the samples. Calcium nitrate particles are exceptionally hygroscopic and deliquesce even at very low relative humidity (RH) of 9-11% which is lower than typical atmospheric environments. Transformation of non-hygroscopic dry mineral dust particles into hygroscopic wet aerosol may have substantial impacts on light scattering properties, the ability to modify clouds and heterogeneous chemistry.

[1]  Y. Mamane,et al.  Nitrate formation on sea-salt and mineral particles—A single particle approach , 1992 .

[2]  G. Carmichael,et al.  Gas-Particle Partitioning of Nitric Acid Modulated by Alkaline Aerosol , 2001 .

[3]  Daniel J. Jacob,et al.  Minerals in the Air: An Environmental Perspective , 2000 .

[4]  Sonia M. Kreidenweis,et al.  African dust aerosols as atmospheric ice nuclei , 2003 .

[5]  Yinon Rudich,et al.  Desert dust suppressing precipitation: A possible desertification feedback loop , 2001, Proceedings of the National Academy of Sciences of the United States of America.

[6]  Olga Khersonsky,et al.  Treating clouds with a grain of salt , 2002 .

[7]  S. Doney,et al.  Erratum: ``Iron supply and demand in the upper ocean'' , 2000 .

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

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

[10]  P. Falkowski,et al.  Biogeochemical Controls and Feedbacks on Ocean Primary Production , 1998, Science.

[11]  Faraday Discuss , 1985 .

[12]  Paul J. DeMott,et al.  Saharan dust storms and indirect aerosol effects on clouds: CRYSTAL‐FACE results , 2003 .

[13]  L. Horowitz,et al.  Impact of air pollution on wet deposition of mineral dust aerosols , 2004 .

[14]  Mian Chin,et al.  Contribution of different aerosol species to the global aerosol extinction optical thickness: Estimates from model results , 1997 .

[15]  Younan Hua.  Studies on Quantification Analysis of Thin Film Layers (Si3N4, SiO2, and TiW) in Wafer Fabrication Using Energy-Dispersive X-Ray Microanalysis Technique and SEC Factors , 2003 .

[16]  Zev Levin,et al.  Chemical and mineralogical analysis of individual mineral dust particles , 2001 .

[17]  Z. Levin,et al.  Cloud processing of dust particles and subsequent effects on drop size distributions , 1997 .

[18]  E. Ganor,et al.  Transport of Saharan dust across the eastern Mediterranean , 1982 .

[19]  D. M. Murphy,et al.  Measurements of the concentration and composition of nuclei for cirrus formation , 2003, Proceedings of the National Academy of Sciences of the United States of America.

[20]  M. Ebert,et al.  Chemical characterization of North Sea aerosol particles , 2000 .

[21]  J. Crowley,et al.  Ozone decomposition on Saharan dust: an experimental investigation , 2002 .

[22]  J. Osán,et al.  Determination of low-Z elements in individual environmental particles using windowless EPMA. , 1999, Analytical chemistry.

[23]  A. Laskin,et al.  Heterogeneous chemistry of individual mineral dust particles from different dust source regions: the importance of particle mineralogy , 2004 .

[24]  K. H. Fung,et al.  Hydration and Raman scattering studies of levitated microparticles: Ba(NO3)2, Sr(NO3)2, and Ca(NO3)2 , 1997 .

[25]  J. Lacaux,et al.  Heterogeneous processes involving nitrogenous compounds and saharan dust inferred from measurements and model calculations , 2001 .

[26]  B. Finlayson‐Pitts.  The tropospheric chemistry of sea salt: a molecular-level view of the chemistry of NaCl and NaBr. , 2003, Chemical reviews.

[27]  S. Doney,et al.  Iron supply and demand in the upper ocean , 2000 .

[28]  Yinon Rudich,et al.  Influence of the Kuwait oil fires plume (1991) on the microphysical development of clouds , 2003 .

[29]  A. Laskin,et al.  Time-Resolved Aerosol Collector for CCSEM/EDX Single-Particle Analysis , 2003 .

[30]  C. Ro,et al.  Single-particle characterization of urban aerosol particles collected in three Korean cites using low-Z electron probe X-ray microanalysis. , 2002, Environmental science & technology.

[31]  J. Osán,et al.  Determination of Chemical Species in Individual Aerosol Particles Using Ultrathin Window EPMA , 2000 .

[32]  T. Pakkanen.  Study of formation of coarse particle nitrate aerosol , 1996 .

[33]  C. Usher,et al.  Heterogeneous and catalytic uptake of ozone on mineral oxides and dusts: A Knudsen cell investigation , 2002 .

[34]  Irina N. Sokolik,et al.  Incorporation of mineralogical composition into models of the radiative properties of mineral aerosol from UV to IR wavelengths , 1999 .

[35]  M. Chin,et al.  Sources and distributions of dust aerosols simulated with the GOCART model , 2001 .

[36]  J. Crowley,et al.  Heterogeneous reactivity of NO and HNO3 on mineral dust in the presence of ozone , 2003 .

[37]  K. Noone,et al.  Single Particle Analysis of Aerosols, Observed in the Marine Boundary Layer during the Monterey Area Ship Tracks Experiment (MAST), with Respect to Cloud Droplet Formation , 2000 .

[38]  Vicki H. Grassian,et al.  The transformation of solid atmospheric particles into liquid droplets through heterogeneous chemistry: Laboratory insights into the processing of calcium containing mineral dust aerosol in the troposphere , 2003 .

[39]  Peter J. Lamb,et al.  African Droughts and Dust Transport to the Caribbean: Climate Change Implications , 2003, Science.

[40]  J. Armstrong.  Quantitative Elemental Analysis of Individual Microparticles with Electron Beam Instruments , 1991 .

[41]  A. Laskin,et al.  Quantitative time-resolved monitoring of nitrate formation in sea salt particles using a CCSEM/EDX single particle analysis. , 2002, Environmental science & technology.

[42]  C. Ro,et al.  Heterogeneity assessment in individual CaCO3-CaSO4 particles using ultrathin window electron probe X-ray microanalysis. , 2001, Analytical chemistry.

[43]  G. Carmichael,et al.  Heterogeneous reactions of NO2 and HNO3 on oxides and mineral dust: A combined laboratory and modeling study , 2001 .

[44]  Y. Rudich,et al.  Adsorption of organic compounds pertinent to urban environments onto mineral dust particles , 2004 .

[45]  H. Mouri,et al.  Shattering and modification of sea‐salt particles in the marine atmosphere , 1993 .

[46]  Natalie M. Mahowald,et al.  Mineral aerosol and cloud interactions , 2003 .

[47]  A. Laskin,et al.  Sodium nitrate particles: physical and chemical properties during hydration and dehydration, and implications for aged sea salt aerosols , 2004 .

[48]  J. Crowley,et al.  The heterogeneous reactivity of gaseous nitric acid on authentic mineral dust samples, and on individual mineral and clay mineral components , 2001 .

[49]  P. Buseck,et al.  Compositional variations of sea‐salt‐mode aerosol particles from the North Atlantic , 1995 .

[50]  Y. Mamane,et al.  Heterogeneous reactions of minerals with sulfur and nitrogen oxides , 1989 .

[51]  I. Tang.  Deliquescence properties and particle size change of hygroscopic aerosols , 1979 .

[52]  A. Wexler,et al.  Formation of nitrate and non-sea-salt sulfate on coarse particles , 1999 .

[53]  G. Danilatos.  Introduction to the ESEM instrument , 1993, Microscopy research and technique.

[54]  O. Boucher,et al.  Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review , 2000 .

[55]  P. Minnett,et al.  Observations of large aerosol infrared forcing at the surface , 2003 .

[56]  D. Covert,et al.  The number of sea-salt, sulfate, and carbonaceous particles in the marine atmosphere: , 1997 .

[57]  R. Toumi,et al.  Non‐sea‐salt‐sulphate formation in sea‐salt aerosol , 1998 .

[58]  J. Prospero.  Long-range transport of mineral dust in the global atmosphere: impact of African dust on the environment of the southeastern United States. , 1999, Proceedings of the National Academy of Sciences of the United States of America.

[59]  C. Usher,et al.  Reactions on mineral dust. , 2003, Chemical reviews.

[60]  R. Robinson,et al.  Ionic hydration and activity in electrolyte solutions. , 1948, Journal of the American Chemical Society.

[61]  P. Buseck,et al.  Constituents of a remote pacific marine aerosol: A tem study , 1994 .

[62]  O. Torres,et al.  ENVIRONMENTAL CHARACTERIZATION OF GLOBAL SOURCES OF ATMOSPHERIC SOIL DUST IDENTIFIED WITH THE NIMBUS 7 TOTAL OZONE MAPPING SPECTROMETER (TOMS) ABSORBING AEROSOL PRODUCT , 2002 .

[63]  Yan Yin,et al.  The effects of giant cloud condensation nuclei on the development of precipitation in convective clouds — a numerical study , 2000 .

[64]  J. Hemminger,et al.  Physical Chemistry of Airborne Sea Salt Particles and Their Components , 2000 .

[65]  G. Stenchikov,et al.  The impact of aerosols on solar ultraviolet radiation and photochemical smog. , 1997, Science.

[66]  S. Doney,et al.  Iron cycling and nutrient-limitation patterns in surface waters of the World Ocean , 2001 .

[67]  C. Usher,et al.  A laboratory study of the heterogeneous uptake and oxidation of sulfur dioxide on mineral dust particles , 2002 .

[68]  P. Quinn,et al.  Clear‐sky infrared aerosol radiative forcing at the surface and the top of the atmosphere , 2003 .

[69]  Sonia M. Kreidenweis,et al.  The Impact of Giant Cloud Condensation Nuclei on Drizzle Formation in Stratocumulus: Implications for Cloud Radiative Properties , 1999 .

[70]  J. Lelieveld,et al.  Role of mineral aerosol as a reactive surface in the global troposphere , 1996 .

[71]  C. Usher,et al.  Laboratory studies of ozone uptake on processed mineral dust , 2003 .

[72]  Irina N. Sokolik,et al.  Direct radiative forcing by anthropogenic airborne mineral aerosols , 1996, Nature.

[73]  J. Osán,et al.  Single-particle analysis of aerosols at Cheju Island, Korea, using low-Z electron probe X-ray microanalysis: a direct proof of nitrate formation from sea salts. , 2001, Environmental science & technology.

[74]  K. Okada,et al.  Nature of coarse nitrate particles in the atmosphere—A single particle approach , 1994 .

[75]  Alexander Khain,et al.  The Role of Sea Spray in Cleansing Air Pollution over Ocean via Cloud Processes , 2002, Science.

[76]  M. Khoder.  Atmospheric conversion of sulfur dioxide to particulate sulfate and nitrogen dioxide to particulate nitrate and gaseous nitric acid in an urban area. , 2002, Chemosphere.

[77]  I. Tang,et al.  Aerosol growth studies—III ammonium bisulfate aerosols in a moist atmosphere , 1977 .

[78]  P. Quinn,et al.  Measurements of chloride depletion and sulfur enrichment in individual sea‐salt particles collected from the remote marine boundary layer , 1994 .

[79]  Hiroshi L. Tanaka,et al.  Elemental Composition of Individual Aerosol Particles Collected from the Coastal Marine Boundary Layer , 1996 .

[80]  A. Laskin,et al.  Probing heterogeneous chemistry of individual atmospheric particles using scanning electron microscopy and energy-dispersive X-ray analysis , 2003 .