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Vaughan T. J. Phillips, Paul J. Demott, Constantin Andronache, Kerri A. Pratt, Kimberly A. Prather, R. Subramanian, and Cynthia Twohy

Abstract

A framework for an empirical parameterization (EP) of heterogeneous nucleation of ice crystals by multiple species of aerosol material in clouds was proposed in a 2008 paper by the authors. The present paper reports improvements to specification of a few of its empirical parameters. These include temperatures for onset of freezing, baseline surface areas of aerosol observed in field campaigns over Colorado, and new parameters for properties of black carbon, such as surface hydrophilicity and organic coatings. The EP’s third group of ice nucleus (IN) aerosols is redefined as that of primary biological aerosol particles (PBAPs), replacing insoluble organic aerosols. A fourth group of IN is introduced—namely, soluble organic aerosols.

The new EP predicts IN concentrations that agree well with aircraft data from selected traverses of shallow wave clouds observed in five flights (1, 3, 4, 6, and 12) of the 2007 Ice in Clouds Experiment–Layer Clouds (ICE-L). Selected traverses were confined to temperatures between about −25° and −29°C in layer cloud without homogeneously nucleated ice from aloft. Some of the wave clouds were affected by carbonaceous aerosols from biomass burning and by dust from dry lakebeds and elsewhere. The EP predicts a trend between number concentrations of heterogeneously nucleated ice crystals and apparent black carbon among the five wave clouds, observed by aircraft in ICE-L. It is predicted in terms of IN activity of black carbon.

The EP’s predictions are consistent with laboratory and field observations not used in its construction, for black carbon, dust, primary biological aerosols, and soluble organics. The EP’s prediction of biological ice nucleation is validated using coincident field observations of PBAP IN and PBAPs in Colorado.

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Allen B. White, Paul J. Neiman, Jessie M. Creamean, Timothy Coleman, F. Martin Ralph, and Kimberly A. Prather

Abstract

Atmospheric rivers (ARs) are narrow regions of enhanced water vapor transport, usually found on the warm-sector side of the polar cold front in many midlatitude storms formed primarily over the oceans. Nonbrightband (NBB) rain is a shallow orographic rainfall process driven by collision and coalescence that has been observed in some of these storms. NBB rain accounts for about one-third, on average, of the total winter season rainfall occurring at a coastal mountain site in Northern California. During the California Energy Commission’s CalWater project, nearly the same fraction of NBB rain was observed at a northern Sierra Nevada foothills site as compared to the coastal mountains, whereas less than half of the fractional amount of NBB rain was observed at a southern Sierra Nevada foothills site. Both Sierra Nevada sites often experience terrain-induced blocked flow, that is, Sierra barrier jet (SBJ) during landfalling winter storms. However, the northern Sierra Nevada site often is oriented geographically downwind of a gap in the coastal terrain near San Francisco during AR landfall. This gap allows maritime air in the AR to arrive at the northern site and enhance the collision–coalescence process in orographic feeder clouds as compared with the southern site. As a result, a greater amount and intensity of NBB rain and overall precipitation was produced at the northern site. This study uses a variety of observations collected in the coastal and Sierra Nevada ranges from the Hydrometeorology Testbed and CalWater field campaigns to document this behavior. A detailed case study provides additional context on the interaction between AR flow, the SBJ, and precipitation processes.

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Kerri A. Pratt, Andrew J. Heymsfield, Cynthia H. Twohy, Shane M. Murphy, Paul J. DeMott, James G. Hudson, R. Subramanian, Zhien Wang, John H. Seinfeld, and Kimberly A. Prather

Abstract

During the Ice in Clouds Experiment–Layer Clouds (ICE-L), aged biomass-burning particles were identified within two orographic wave cloud regions over Wyoming using single-particle mass spectrometry and electron microscopy. Using a suite of instrumentation, particle chemistry was characterized in tandem with cloud microphysics. The aged biomass-burning particles comprised ∼30%–40% by number of the 0.1–1.0-μm clear-air particles and were composed of potassium, organic carbon, elemental carbon, and sulfate. Aerosol mass spectrometry measurements suggested these cloud-processed particles were predominantly sulfate by mass. The first cloud region sampled was characterized by primarily homogeneously nucleated ice particles formed at temperatures near −40°C. The second cloud period was characterized by high cloud droplet concentrations (∼150–300 cm−3) and lower heterogeneously nucleated ice concentrations (7–18 L−1) at cloud temperatures of −24° to −25°C. As expected for the observed particle chemistry and dynamics of the observed wave clouds, few significant differences were observed between the clear-air particles and cloud residues. However, suggestive of a possible heterogeneous nucleation mechanism within the first cloud region, ice residues showed enrichments in the number fractions of soot and mass fractions of black carbon, measured by a single-particle mass spectrometer and a single-particle soot photometer, respectively. In addition, enrichment of biomass-burning particles internally mixed with oxalic acid in both the homogeneously nucleated ice and cloud droplets compared to clear air suggests either preferential activation as cloud condensation nuclei or aqueous phase cloud processing.

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Christina S. McCluskey, Thomas C. J. Hill, Camille M. Sultana, Olga Laskina, Jonathan Trueblood, Mitchell V. Santander, Charlotte M. Beall, Jennifer M. Michaud, Sonia M. Kreidenweis, Kimberly A. Prather, Vicki Grassian, and Paul J. DeMott

Abstract

The abundance of atmospheric ice nucleating particles (INPs) is a source of uncertainty for numerical representation of ice-phase transitions in mixed-phase clouds. While sea spray aerosol (SSA) exhibits less ice nucleating (IN) ability than terrestrial aerosol, marine INP emissions are linked to oceanic biological activity and are potentially an important source of INPs over remote oceans. Inadequate knowledge of marine INP identity limits the ability to parameterize this complex INP source. A previous manuscript described abundances of marine INPs in relation to several aerosol composition and ocean biology observations during two laboratory mesocosm experiments. In this study, the abundances and chemical and physical properties of INPs found during the same mesocosm experiments were directly probed in SSA, seawater, and surface microlayer samples. Two unique marine INP populations were found: 1) dissolved organic carbon INPs are suggested to be composed of IN-active molecules, and 2) particulate organic carbon INPs are attributed as intact cells or IN-active microbe fragments. Both marine INP types are likely to be emitted into SSA following decay of phytoplankton biomass when 1) the surface microlayer is significantly enriched with exudates and cellular detritus and SSA particles are preferentially coated with IN-active molecules or 2) diatom fragments and bacteria are relatively abundant in seawater and therefore more likely transferred into SSA. These findings inform future efforts for incorporating marine INP emissions into numerical models and motivate future studies to quantify specific marine molecules and isolate phytoplankton, bacteria, and other species that contribute to these marine INP types.

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Christina S. McCluskey, Thomas C. J. Hill, Francesca Malfatti, Camille M. Sultana, Christopher Lee, Mitchell V. Santander, Charlotte M. Beall, Kathryn A. Moore, Gavin C. Cornwell, Douglas B. Collins, Kimberly A. Prather, Thilina Jayarathne, Elizabeth A. Stone, Farooq Azam, Sonia M. Kreidenweis, and Paul J. DeMott

Abstract

Emission rates and properties of ice nucleating particles (INPs) are required for proper representation of aerosol–cloud interactions in atmospheric models. Few investigations have quantified marine INP emissions, a potentially important INP source for remote oceanic regions. Previous studies have suggested INPs in sea spray aerosol (SSA) are linked to oceanic biological activity. This proposed link was explored in this study by measuring INP emissions from nascent SSA during phytoplankton blooms during two mesocosm experiments. In a Marine Aerosol Reference Tank (MART) experiment, a phytoplankton bloom was produced with chlorophyll-a (Chl a) concentrations reaching 39 μg L−1, while Chl a concentrations more representative of natural ocean conditions were obtained during the Investigation into Marine Particle Chemistry and Transfer Science (IMPACTS; peak Chl a of 5 μg L−1) campaign, conducted in the University of California, San Diego, wave flume. Dynamic trends in INP emissions occurred for INPs active at temperatures > −30°C. Increases in INPs active between −25° and −15°C lagged the peak in Chl a in both studies, suggesting a consistent population of INPs associated with the collapse of phytoplankton blooms. Trends in INP emissions were also compared to aerosol composition, abundances of microbes, and enzyme activity. In general, increases in INP concentrations corresponded to increases in organic species in SSA and the emissions of heterotrophic bacteria, suggesting that both microbes and biomolecules contribute to marine INP populations. INP trends were not directly correlated with a single biological marker in either study. Direct measurements of INP chemistry are needed to accurately identify particles types contributing to marine INP populations.

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