Showing papers by "Karl D. Froyd published in 2013"
TL;DR: Results demonstrate that mineral dust and metallic particles are the dominant source of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent.
Abstract: Formation of cirrus clouds depends on the availability of ice nuclei to begin condensation of atmospheric water vapor. Although it is known that only a small fraction of atmospheric aerosols are efficient ice nuclei, the critical ingredients that make those aerosols so effective have not been established. We have determined in situ the composition of the residual particles within cirrus crystals after the ice was sublimated. Our results demonstrate that mineral dust and metallic particles are the dominant source of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent. Further, composition analysis combined with relative humidity measurements suggests that heterogeneous freezing was the dominant formation mechanism of these clouds.
458 citations
University of Colorado Boulder1, National Oceanic and Atmospheric Administration2, University of California, Davis3, Peking University4, University of Houston5, University of Manchester6, Georgia Institute of Technology7, University of California, San Diego8, University of California, Berkeley9, University of North Carolina at Chapel Hill10, Research Triangle Park11, Indiana University12, university of lille13
TL;DR: In this paper, five organic aerosols (OA) components are identified using positive matrix factorization including hydrocarbon-like OA (HOA) and two types of oxygenated OA(OOA) components, and the Pasadena OA elemental composition when plotted as H:C versus O:C follows a line less steep than that observed for Riverside, CA.
Abstract: [1] Organic aerosols (OA) in Pasadena are characterized using multiple measurements from the California Research at the Nexus of Air Quality and Climate Change (CalNex) campaign. Five OA components are identified using positive matrix factorization including hydrocarbon-like OA (HOA) and two types of oxygenated OA (OOA). The Pasadena OA elemental composition when plotted as H : C versus O : C follows a line less steep than that observed for Riverside, CA. The OOA components from both locations follow a common line, however, indicating similar secondary organic aerosol (SOA) oxidation chemistry at the two sites such as fragmentation reactions leading to acid formation. In addition to the similar evolution of elemental composition, the dependence of SOA concentration on photochemical age displays quantitatively the same trends across several North American urban sites. First, the OA/ΔCO values for Pasadena increase with photochemical age exhibiting a slope identical to or slightly higher than those for Mexico City and the northeastern United States. Second, the ratios of OOA to odd-oxygen (a photochemical oxidation marker) for Pasadena, Mexico City, and Riverside are similar, suggesting a proportional relationship between SOA and odd-oxygen formation rates. Weekly cycles of the OA components are examined as well. HOA exhibits lower concentrations on Sundays versus weekdays, and the decrease in HOA matches that predicted for primary vehicle emissions using fuel sales data, traffic counts, and vehicle emission ratios. OOA does not display a weekly cycle—after accounting for differences in photochemical aging —which suggests the dominance of gasoline emissions in SOA formation under the assumption that most urban SOA precursors are from motor vehicles.
243 citations
University of Indianapolis1, University of Calgary2, University of California, Los Angeles3, National Oceanic and Atmospheric Administration4, Cooperative Institute for Research in Environmental Sciences5, Max Planck Society6, University of Colorado Boulder7, Memorial University of Newfoundland8, University of Houston9, Georgia Institute of Technology10
TL;DR: In this article, the authors present a comprehensive measurement data set acquired at Pasadena, California, during the CalNex-LA campaign 2010 that included measurements of odd nitrogen and its major components.
Abstract: [1] The nocturnal conversion of dinitrogen pentoxide (N2O5) to nitryl chloride (ClNO2) on chloride-containing aerosol can be a regionally important NOx (= NO + NO2) recycling and halogen activation pathway that affects oxidant photochemistry the following day. Here we present a comprehensive measurement data set acquired at Pasadena, California, during the CalNex-LA campaign 2010 that included measurements of odd nitrogen and its major components (NOy = NOx + NO3 + 2N2O5 + ClNO2 + HNO3 + HONO + peroxyacyl, alkyl, and aerosol nitrates) and aerosol size distribution and composition. Nitryl chloride was present during every night of the study (median mixing ratio at sunrise 800 pptv) and was usually a more significant nocturnal NOx and odd oxygen (Ox = O3 + NO2 + 3N2O5 + ClNO2) reservoir species than N2O5 (whose concentrations were calculated from its equilibrium with NO2 and NO3). At sunrise, ClNO2 accounted for 21% of NOz (=NOy − NOx), 4% of NOy, and 2.5% of Ox, respectively (median values). Kinetic parameters for the N2O5 to ClNO2 conversion were estimated by relating ClNO2 concentrations to their time-integrated heterogeneous production from N2O5 and were highly variable between nights. Production of ClNO2 required conversion of N2O5 on submicron aerosol with average yield (φ) and N2O5 reactive uptake probability (γ) of γφ = 0.008 (maximum 0.04), scaled with submicron aerosol chloride content, and was suppressed by aerosol organic matter and liquid water content. Not all of the observed variability of ClNO2 production efficiency could be rationalized using current literature parameterizations.
70 citations
01 May 2013
TL;DR: In this paper, the composition of the residual particles within cirrus crystals after the ice was sublimated was determined in situ, showing that mineral dust and metallic particles are the dominant sources of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent.
Abstract: Formation of cirrus clouds depends on the availability of ice nuclei to begin condensation of atmospheric water vapor. Although it is known that only a small fraction of atmospheric aerosols are efficient ice nuclei, the critical ingredients that make those aerosols so effective have not been established. We have determined in situ the composition of the residual particles within cirrus crystals after the ice was sublimated. Our results demonstrate that mineral dust and metallic particles are the dominant source of residual particles, whereas sulfate and organic particles are underrepresented, and elemental carbon and biological materials are essentially absent. Further, composition analysis combined with relative humidity measurements suggests that heterogeneous freezing was the dominant formation mechanism of these clouds.
44 citations
01 Jul 2013
TL;DR: In this article, the United States National Aeronautomautics and Space Administration (NASA Earth Science Division Atmospheric Composition Program, award NNH11AQ58UI)
Abstract: United States National Aeronautics and Space Administration (NASA Earth Science Division Atmospheric Composition Program, award NNH11AQ58UI)
12 citations
26 Apr 2013
TL;DR: In this paper, the size and composition of sublimated cirrus particles sampled from a high altitude research aircraft using both in situ and offline techniques were analyzed, and it was inferred that heterogeneous nucleation is a dominant cirrus formation mechanism for the mid-latitude, subtropical, and tropical regions under study.
Abstract: Composition, size, and phase are key properties that define the ability of an aerosol particle to initiate ice in cirrus clouds. Properties of cirrus ice nuclei (IN) have not been well constrained due to a lack of systematic measurements in the upper troposphere. We have analyzed the size and composition of sublimated cirrus particles sampled from a high altitude research aircraft using both in situ and offline techniques. Mineral dust and metallic particles are the most enhanced residue types relative to background aerosol. Using a combination of cirrus residue composition, relative humidity, and cirrus particle concentration measurements, we infer that heterogeneous nucleation is a dominant cirrus formation mechanism for the mid-latitude, subtropical, and tropical regions under study. Other proposed heterogeneous IN including biomass burning particles, elemental carbon, and biological material were not abundant in cirrus residuals.
4 citations