Relationships of Biomass-Burning Aerosols to Ice in Orographic Wave Clouds

Ice concentrations in orographic wave clouds at temperatures between −24° and −29°C were shown to be related to aerosol characteristics in nearby clear air during five research flights over the Rocky Mountains. When clouds with influence from colder temperatures were excluded from the dataset, mean ice nuclei and cloud ice number concentrations were very low, on the order of 1–5 L^(−1). In this environment, ice number concentrations were found to be significantly correlated with the number concentration of larger particles, those larger than both 0.1- and 0.5-μm diameter. A variety of complementary techniques was used to measure aerosol size distributions and chemical composition. Strong correlations were also observed between ice concentrations and the number concentrations of soot and biomass-burning aerosols. Ice nuclei concentrations directly measured in biomass-burning plumes were the highest detected during the project. Taken together, this evidence indicates a potential role for biomass-burning aerosols in ice formation, particularly in regions with relatively low concentrations of other ice nucleating aerosols

Observation of playa salts as nuclei in orographic wave clouds

During the Ice in Clouds Experiment-Layer Clouds (ICE-L), dry lakebed, or playa, salts from the Great Basin region of the United States were observed as cloud nuclei in orographic wave clouds over Wyoming. Using a counterflow virtual impactor in series with a single-particle mass spectrometer, sodium-potassium-magnesium-calcium-chloride salts were identified as residues of cloud droplets. Importantly, these salts produced similar mass spectral signatures to playa salts with elevated cloud condensation nuclei (CCN) efficiencies close to sea salt. Using a suite of chemical characterization instrumentation, the playa salts were observed to be internally mixed with oxidized organics, presumably produced by cloud processing, as well as carbonate. These salt particles were enriched as residues of large droplets (>19 μm) compared to smaller droplets (>7 μm). In addition, a small fraction of silicate-containing playa salts were hypothesized to be important in the observed heterogeneous ice nucleation processes. While the high CCN activity of sea salt has been demonstrated to play an important role in cloud formation in marine environments, this study provides direct evidence of the importance of playa salts in cloud formation in continental North America has not been shown previously. Studies are needed to model and quantify the impact of playas on climate globally, particularly because of the abundance of playas and expected increases in the frequency and intensity of dust storms in the future due to climate and land use changes

Snowpack measurements suggest role for multi-year sea ice regions in Arctic atmospheric bromine and chlorine chemistry

As sources of reactive halogens, snowpacks in sea ice regions control the oxidative capacity of the Arctic atmosphere. However, measurements of snowpack halide concentrations remain sparse, particularly in the high Arctic, limiting our understanding of and ability to parameterize snowpack participation in tropospheric halogen chemistry. To address this gap, we measured concentrations of chloride, bromide, and sodium in snow samples collected during polar spring above remote multi-year sea ice (MYI) and first-year sea ice (FYI) north of Greenland and Alaska, as well as in the central Arctic, and compared these measurements to a larger dataset collected in the Alaskan coastal Arctic by Krnavek et al. (2012). Regardless of sea ice region, these surface snow samples generally featured lower salinities, compared to coastal snow. Surface snow in FYI regions was typically enriched in bromide and chloride compared to seawater, indicating snowpack deposition of bromine and chlorine-containing trace gases and an ability of the snowpack to participate further in bromine and chlorine activation processes. In contrast, surface snow in MYI regions was more often depleted in bromide, indicating it served as a source of bromine-containing trace gases to the atmosphere prior to sampling. Measurements at various snow depths indicate that the deposition of sea salt aerosols and halogen-containing trace gases to the snowpack surface played a larger role in determining surface snow halide concentrations compared to upward brine migration from sea ice. Calculated enrichment factors for bromide and chloride, relative to sodium, in the MYI snow samples suggests that MYI regions, in addition to FYI regions, have the potential to play an active role in Arctic boundary layer bromine and chlorine chemistry. The ability of MYI regions to participate in springtime atmospheric halogen chemistry should be considered in regional modeling of halogen activation and interpretation of satellite-based tropospheric bromine monoxide column measurements

Changes in precipitating snow chemistry with location and elevation in the California Sierra Nevada

Orographic snowfall in the Sierra Nevada Mountains is an important source of water for California and can vary significantly on an annual basis. The microphysical properties of orographic clouds and subsequent formation of precipitation are impacted, in part, by aerosols of varying size, number, and chemical composition, which are incorporated into clouds formed along the Sierra barrier. Herein, the physicochemical properties and sources of insoluble residues and soluble ions found in precipitation samples were explored for three sites of variable elevation in the Sierra Nevada during the 2012–2013 winter season. Residues were characterized using a suite of physicochemical techniques to determine the size‐resolved number concentrations and associated chemical composition. A transition in the aerosol sources that served as cloud seeds or were scavenged in‐cloud and below‐cloud was observed as a function of location and elevation. Anthropogenic influence from the Central Valley was dominant at the two lowest elevation sites (1900 and 2200 m above mean sea level (AMSL)), whereas long‐range transported mineral dust was a larger contributor at the highest elevation site where cleaner conditions were observed (2600 m AMSL). The residues and soluble ions observed provide insight into how multiple aerosol sources can impact cloud and precipitation formation processes, even over relatively small spatial scales. The transition with increasing elevation to aerosols that serve as ice nucleating particles may impact the properties and extent of snowfall in remote mountain regions where snowpack provides a vital supply of water.Key PointsPhysiochemical properties of particles found in precipitation were determinedBoth anthropogenic and natural sources contributed to the snow residue chemistrySnow residue sources varied depending on location and elevationPeer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/133563/1/jgrd53083-sup-0001-SI.pdfhttp://deepblue.lib.umich.edu/bitstream/2027.42/133563/2/jgrd53083_am.pdfhttp://deepblue.lib.umich.edu/bitstream/2027.42/133563/3/jgrd53083.pd

Contributions of transported Prudhoe Bay oil field emissions to the aerosol population in Utqiaġvik, Alaska

Loss of sea ice is opening the Arctic to increasing development involving oil and gas extraction and shipping. Given the significant impacts of absorbing aerosol and secondary aerosol precursors emitted within the rapidly warming Arctic region, it is necessary to characterize local anthropogenic aerosol sources and compare to natural conditions. From August to September 2015 in Utqiaġvik (Barrow), AK, the chemical composition of individual atmospheric particles was measured by computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (0.13-4 μm projected area diameter) and real-time single-particle mass spectrometry (0.2-1.5 μm vacuum aerodynamic diameter). During periods influenced by the Arctic Ocean (70 % of the study), our results show that fresh sea spray aerosol contributed ∼ 20 %, by number, of particles between 0.13 and 0.4 μm, 40-70 % between 0.4 and 1 μm, and 80-100 % between 1 and 4 μm particles. In contrast, for periods influenced by emissions from Prudhoe Bay (10 % of the study), the third largest oil field in North America, there was a strong influence from submicron (0.13-1 μm) combustion-derived particles (20-50 % organic carbon, by number; 5-10 % soot by number). While sea spray aerosol still comprised a large fraction of particles (90 % by number from 1 to 4 μm) detected under Prudhoe Bay influence, these particles were internally mixed with sulfate and nitrate indicative of aging processes during transport. In addition, the overall mode of the particle size number distribution shifted from 76 nm during Arctic Ocean influence to 27 nm during Prudhoe Bay influence, with particle concentrations increasing from 130 to 920 cm-3 due to transported particle emissions from the oil fields. The increased contributions of carbonaceous combustion products and partially aged sea spray aerosol should be considered in future Arctic atmospheric composition and climate simulations

Improvements to an Empirical Parameterization of Heterogeneous Ice Nucleation and Its Comparison with Observations

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 degrees and -29 degrees 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.Keywords: Ice particles, Ice crystals, Aerosol

The Role of Open Lead Interactions in Atmospheric Ozone Variability Between Arctic Coastal and Inland Sites

Boundary layer atmospheric ozone depletion events (ODEs) are commonly observed across polar sea ice regions following polar sunrise. During March-April 2005 in Alaska, the coastal site of Barrow and inland site of Atqasuk experienced ODEs (O3 \u3c 10 nmol mol-1) concurrently for 31% of the observations, consistent with large spatial scale ozone depletion. However, 7% of the time ODEs were exclusively observed inland at Atqasuk. This phenomenon also occurred during one of nine flights during the BRomine, Ozone, and Mercury EXperiment (BROMEX), when atmospheric vertical profiles at both sites showed near-surface ozone depletion only at Atqasuk on 28 March 2012. Concurrent in-flight BrO measurements made using nadir scanning differential optical absorption spectroscopy (DOAS) showed the differences in ozone vertical profiles at these two sites could not be attributed to differences in locally occurring halogen chemistry. During both studies, backward air mass trajectories showed that the Barrow air masses observed had interacted with open sea ice leads, causing increased vertical mixing and recovery of ozone at Barrow and not Atqasuk, where the air masses only interacted with tundra and consolidated sea ice. These observations suggest that, while it is typical for coastal and inland sites to have similar ozone conditions, open leads may cause heterogeneity in the chemical composition of the springtime Arctic boundary layer over coastal and inland areas adjacent to sea ice regions

In Situ Chemical Characterization of Aged Biomass-Burning Aerosols Impacting Cold Wave Clouds

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

In Situ Chemical Characterization of Aged Biomass-Burning Aerosols Impacting Cold Wave Clouds

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