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Suski, Kaitlyn J.

Publications and source records attributed to Suski, Kaitlyn J..

Field intercomparison of ice nucleation measurements: the Fifth International Workshop on Ice Nucleation Phase 3 (FIN-03)

Abstract. The third phase of the Fifth International Ice Nucleation Workshop (FIN-03) was conducted at the Storm Peak Laboratory in Steamboat Springs, Colorado, in September 2015 to facilitate the intercomparison of instruments measuring ice-nucleating particles (INPs) in the field. Instruments included two online and four offline measurement systems for INPs, which are a subset of those utilized in the laboratory study that comprised the second phase of FIN (FIN-02). The composition of the total aerosols was characterized using the Particle Analysis by Laser Mass Spectrometry (PALMS) and Wideband Integrated Bioaerosol Sensor (WIBS) instruments, and aerosol size distributions were measured by a laser aerosol spectrometer (LAS). The dominant total particle compositions present during FIN-03 were composed of sulfates, organic compounds, and nitrates, as well as particles derived from biomass burning. Mineral-dust-containing particles were ubiquitous throughout and represented 67 % of supermicron particles. Total WIBS fluorescing particle concentrations for particles with diameters of > 0.5 µm were 0.04 ± 0.02 cm−3 (0.1 cm−3 highest; 0.02 cm−3 lowest), typical of the warm season in this region and representing ≈ 9 % of all particles in this size range as a campaign average. The primary focus of FIN-03 was the measurement of INP concentrations via immersion freezing at temperatures > −33 °C. Additionally, some measurements were made in the deposition nucleation regime at these same temperatures, representing one of the first efforts to include both mechanisms within a field campaign. INP concentrations via immersion freezing agreed within factors ranging from nearly 1 to 5 times on average between matched (time and temperature) measurements, and disagreements only rarely exceeded 1 order of magnitude for sampling times coordinated to within 3 h. Comparisons were restricted to temperatures lower than −15 °C due to the limits of detection related to sample volumes and very low INP concentrations. Outliers of up to 2 orders of magnitude occurred between −25 and −18 °C; a better agreement was seen at higher and lower temperatures. Although the 5–10 factor agreement of INP measurements found in FIN-03 aligned with the results of the FIN-02 laboratory comparison phase, giving confidence in progress of this measurement field, this level of agreement still equates to temperature uncertainties of 3.5 to 5 °C that may not be sufficient for numerical cloud modeling applications that utilize INP information. INP activity in the immersion-freezing mode was generally found to be an order of magnitude or more, making it more efficient than in the deposition regime at 95 %–99 % water relative humidity, although this limited data set should be augmented in future efforts. To contextualize the study results, an assessment was made of the composition of INPs during the late-summer to early-fall period of this study inferred through comparison to existing ice nucleation parameterizations and through measurement of the influence of thermal and organic carbon digestion treatments on immersion-freezing ice nucleation activity. Consistent with other studies in continental regions, biological INPs dominated at temperatures of > −20 °C and sometimes colder, while arable dust-like or other organic-influenced INPs were inferred to dominate below −20 °C.

54 ENVIRONMENTAL SCIENCES↗

The contribution of black carbon to global ice nucleating particle concentrations relevant to mixed-phase clouds

Significance The Earth’s climate is affected by the radiative properties of clouds. In clouds containing both supercooled water droplets and ice particles (mixed-phase clouds), cloud lifetime and albedo are affected by the presence of ice nucleating particles (INP). After decades of research, the importance of black carbon (BC) as an INP remains unresolved. In this work, we determined the contribution of BC to INP concentrations ([INP]) from real-world wildfires and prescribed burns. We found that BC does not contribute significantly to [INP] in near-field biomass burning plumes. These results were applied as parameterizations to global climate model output. Combined with previous work on diesel-engine exhaust, we find that BC does not contribute significantly to global [INP] relevant to mixed-phase clouds.

54 ENVIRONMENTAL SCIENCES↗

Impact of Biofuel Blends on Black Carbon Emissions from a Gas Turbine Engine

With a view towards renewable feedstock while decreasing the CO2 footprint associated with jet travel, biofuels are receiving increasing interest. Presented here is an overview of non-volatile particulate matter (nvPM) emissions, i.e. “soot” as gauged by varied TEM analyses for a J-85 turbojet fueled with Jet-A as well as with blends of Jet-A using Camelina biofuel. A unifying explanation is provided encompassing fuels and spanning length scales across three orders of magnitude. The variation of primary particle size, aggregate size and nanostructure are analyzed as a function of biofuel blend across range of engine thrust levels. The postulate is based on where fuels start along the soot formation pathway. Increasing biofuel content lowers aromatic concentration while placing increasing dependence upon fuel pyrolysis reactions to form the requisite concentration of aromatics for particle inception and growth. The required “kinetic” time for pyrolysis reactions to produce benzene and multi-ring PAHs allows increased fuel-air mixing by turbulence, diluting the fuel-rich soot-forming regions, effectively lowering their equivalence ratio. With a lower precursor concentration, particle inception is slowed, the resulting concentration of primary particles is lowered and smaller aggregates. The lower equivalence ratio also results in smaller primary particles given the lower concentration of growth species.

Kumal, Raju R.↗

Direct online mass spectrometry measurements of ice nucleating particles at a California coastal site

The formation of ice in clouds can strongly impact cloud properties and precipitation processes during storms, including atmospheric rivers. Sea spray aerosol (SSA) particles are relatively inefficient as ice nucleating particles (INPs) compared to mineral dust. However, due to the vast coverage of the Earth’s surface by the oceans, a number of recent studies have focused on identifying sources of marine INPs, particularly in regions lacking a strong influence from dust. This study describes the integration, validation, and application of a system coupling a continuous flow diffusion chamber with a single particle mass spectrometer using a pumped counterflow virtual impactor to remove non-nucleated particles and selectively measure the composition of INPs with a detection efficiency of 3.10x10-4. In-situ measurements of immersion freezing INP composition were made at a coastal site in California using the integrated system. Mineral dust particles were the most abundant ice crystal residual type during the sampling period and found to be ice-active despite having undergone atmospheric processing. SSA were more abundant in ambient measurements but represented only a minor fraction of the ice crystal residual population at -31 ?C. Notably, the SSA particles that activated were enriched with organic-nitrogen species that were likely transferred from the ocean. Calculations of ice nucleation active site densities were within good agreement with previous studies of mineral dust and SSA.

Cornwell, Gavin C.↗

Characteristics of ice nucleating particles in and around California winter storms

A major component of California’s yearly precipitation comes from wintertime atmospheric river (AR) events which bring large amounts of moisture from the tropics up to the midlatitudes. Understanding these systems, specifically the effects of aerosol particles on precipitation associated with these storms, was a major focus of the 2015 Atmospheric Radiation Measurement (ARM) Cloud Aerosol Precipitation Experiment (ACAPEX), which was part of the wintertime CalWater 2015 campaign. The measurement campaign provided sampling platforms on four aircraft, including the ARM Aerial Facility G-1, as well as the NOAA Ronald H. Brown research vessel and at a ground station in Bodega Bay, CA. Measurements of ice nucleating particles (INPs) were made with the Colorado State University (CSU) Continuous Flow Diffusion Chamber (CFDC) aboard the G-1, and aerosol filters were collected on the G-1, at the Bodega Bay site and on the Ronald H. Brown for post-processing via immersion freezing in the CSU Ice Spectrometer. Aerosol composition was measured aboard the G-1 with the Aerosol Time-of-Flight Mass Spectrometer (ATOFMS). Here we present INP concentrations and aerosol chemical compositions during the course of the aircraft campaign. During the AR event we found that marine aerosol was the dominant aerosol type and that marine INPs were dominant at cloud activation temperatures, which is in stark contrast to the dominance of dust INPs during the AR events in the CalWater 2011 campaign.

Levin, Ezra↗

Release of micro- and nanoparticles from biodegradable plastic during in situ composting

Plastic is ubiquitous in modern life, but most conventional plastic is non-biodegradable and accumulates as waste after use. Biodegradable plastic is a promising alternative to conventional plastic. However, biodegradable plastics must be thoroughly evaluated to ensure that they undergo complete degradation and have no adverse impact on the environment. We evaluated the degradation of biodegradable plastics during 18-week full-scale composting, and determined whether additives from the plastics are released upon degradation. Two biodegradable plastic films—one containing polybutylene co-adipate co-terephthalate (PBAT) and the other containing polylactic acid/poly-hydroxy-alkanoate (PLA/PHA)—were placed into meshbags and buried in the compost. Degradation was assessed by image analysis, scanning electron microscopy, Fourier-transformed infrared spectroscopy, electrophoretic mobility, d13C isotope analyses, and single particle mass spectrometry of mulch fragments. The results showed >99% macroscopic degradation of PLA/PHA and 97% for PBAT film. Polymers in the biodegradable films degraded; however, micro- and nanoparticles, most likely carbon black, were observed on the meshbags. Overall, biodegradable plastics hold promise, but the release of micro- and nanoparticles from biodegradable plastic upon degradation warrants additional investigation and calls for longer field testing to ensure that either complete biodegradation occurs or that no long-term harm to the environment is caused.

Sintim, Henry Y.↗

Formation of Polycyclic Aromatic Hydrocarbon Oxidation Products in alpha-Pinene Secondary Organic Aerosol Particles Formed through Ozonolysis

Accurate long-range atmospheric transport (LRAT) modeling of polycyclic aromatic hydrocarbons (PAHs) and PAH oxidation products (PAH-OPs) in secondary organic aerosol (SOA) particles relies on the known chemical composition of the particles. Four PAHs, phenanthrene (PHE), dibenzothiophene (DBT), pyrene (PYR), and benz(a)anthracene (BaA), were studied individ-ually to identify and quantify PAH-OPs produced and incorporated into SOA particles formed by ozonolysis of a-pinene in the presence of PAH vapor. SOA particles were characterized using real-time in situ instrumentation, and collected on quartz ?ber ?lters for o?ine analysis of PAHs and PAH-OPs. PAH-OPs were measured in all PAH experiments at equal or greater concentrations than the individual PAHs they were produced from. The total mass of PAH and PAH-OPs, relative to the total SOA mass, varied for di?erent experiments on individual parent PAHs: PHE and 6 quanti?ed PHE-OPs (3.0%), DBT and dibenzothiophene sulfone (4.9%), PYR and 3 quanti?ed PYR-OPs (3.1%), and BaA and benz(a)anthracene-7,12-dione (0.26%). Further exposure of PAH-SOA to ozone generally increased the concentration ratio of PAH-OPs to PAH, suggesting longer atmospheric lifetimes for PAH-OPs, relative to PAHs. These data indicate that PAH-OPs are formed during SOA particle formation and growth.

Kramer, Amber L.↗

Overview of the HI-SCALE Field Campaign: A New Perspective on Shallow Convective Clouds

Shallow convective clouds are common, occurring over many areas of the world, and are an important component in the atmospheric radiation budget. In addition to synoptic and mesoscale meteorological conditions, land-atmosphere interactions and aerosol-radiation-cloud interactions can influence the formation of shallow clouds and their properties. However, these processes exhibit large spatial and temporal variability and occur at the sub-grid scale for all climate and operational forecast models and must be represented by parameterizations. Uncertainties in shallow cloud parameterization predictions arise from many sources, including insufficient coincident data needed to adequately represent the coupling of cloud macrophysical and microphysical properties with inhomogeneity in the surface layer, boundary layer, and aerosol properties. Predictions in the transition of shallow to deep convection and the onset of precipitation are also affected by errors in simulated shallow clouds. Coincident data is a key factor needed to achieve a more complete understanding of the lifecycle of shallow convective clouds and to develop improved model parameterizations. To address these issues, the Holistic Interactions of Shallow Clouds, Aerosols and Land Ecosystems (HI-SCALE) campaign was conducted near the Atmospheric Radiation and Measurement (ARM) Southern Great Plains site in north-central Oklahoma during 2016. We describe the scientific objectives of HI-SCALE as well as the experimental approach, the overall weather conditions during the campaign, and preliminary findings from the measurements. Finally, we discuss the remaining scientific gaps in our understanding of shallow clouds that can be addressed by analysis and modeling studies that use HI-SCALE data including: the effects of heterogeneous land-use, vegetation, and soil moisture conditions on boundary layer mixing and consequently cloud formation; factors that contribute to the transition of shallow to deep convection; the role of cloud population on

Fast, Jerome D.↗

Activation of intact bacteria and bacterial fragments mixed with agar as cloud droplets and ice crystals in cloud chamber experiments

Biological particles, including bacteria and bacterial fragments, have beenof much interest due to the special ability of some to nucleate ice atmodestly supercooled temperatures. This paper presents results from a recentstudy conducted on two strains of cultivated bacteria which suggest thatbacterial fragments mixed with agar, and not whole bacterial cells, serve ascloud condensation nuclei (CCN). Due to the absence of whole bacteria cellsin droplets, they are unable to serve as ice nucleating particles (INPs) inthe immersion mode under the experimental conditions. Experiments wereconducted at the Aerosol Interaction and Dynamics in the Atmosphere (AIDA)cloud chamber at the Karlsruhe Institute of Technology (KIT) by injectingbacteria-containing aerosol samples into the cloud chamber and inducing cloudformation by expansion over a temperature range of -5 to -12 ° C.Cloud droplets and ice crystals were sampled through a pumped counterflowvirtual impactor inlet (PCVI) and their residuals were characterized with asingle particle mass spectrometer (miniSPLAT). The size distribution of theoverall aerosol was bimodal, with a large particle mode composed of intactbacteria and a mode of smaller particles composed of bacterial fragmentsmixed with agar that were present in higher concentrations. Results fromthree expansions with two bacterial strains indicate that the cloud dropletresiduals had virtually the same size distribution as the smaller particlesize mode and had mass spectra that closely matched those of bacterialfragments mixed with agar. The characterization of ice residuals that weresampled through an ice-selecting PCVI (IS-PCVI) also shows that the sameparticles that activate to form cloud droplets, bacteria fragments mixed withagar, were the only particle type observed in ice residuals. These resultsindicate that the unavoidable presence of agar or other growth media inall laboratory studies conducted on cultivated bacteria can greatlyaffect the results and needs to be considered when interpreting CCN and INactivation data.

54 ENVIRONMENTAL SCIENCES↗

Background Free‐Tropospheric Ice Nucleating Particle Concentrations at Mixed‐Phase Cloud Conditions

Abstract Clouds containing ice are vital for precipitation formation and are important in determining the Earth's radiative budget. However, primary formation of ice in clouds is not fully understood. In the presence of ice nucleating particles (INPs), the phase change to ice is promoted, but identification and quantification of INPs in a natural environment remains challenging because of their low numbers. In this paper, we quantify INP number concentrations in the free troposphere (FT) as measured at the High Altitude Research Station Jungfraujoch (JFJ), during the winter, spring, and summer of the years 2014–2017. INPs were measured at conditions relevant for mixed‐phase cloud formation at T = 241/242 K. To date, this is the longest timeline of semiregular measurements akin to online INP monitoring at this site and sampling conditions. We find that INP concentrations in the background FT are on average capped at 10/stdL (liter of air at standard conditions [ T = 273 K and p = 1013 hPa]) with an interquartile range of 0.4–9.6/stdL, as compared to measurements during times when other air mass origins (e.g., Sahara or marine boundary layer) prevailed. Elevated concentrations were measured in the field campaigns of 2016, which might be due to enhanced influence from Saharan dust and marine boundary layer air arriving at the JFJ. The upper limit of INP concentrations in the background FT is supported by measurements performed at similar conditions, but at different locations in the FT, where we find INP concentrations to be below 13/stdL most of the time.

54 ENVIRONMENTAL SCIENCES↗

Using depolarization to quantify ice nucleating particle concentrations: a new method

We have developed a new method to determine ice nucleating particle (INP) concentrations observed by the Texas A&M University continuous flow diffusion chamber (CFDC) under a wide range of operating conditions. In this study, we evaluate differences in particle optical properties detected by the Cloud and Aerosol Spectrometer with POLarization (CASPOL) to differentiate between ice crystals, droplets, and aerosols. The depolarization signal from the CASPOL instrument is used to determine the occurrence of water droplet breakthrough (WDBT) conditions in the CFDC. The standard procedure for determining INP concentration is to count all particles that have grown beyond a nominal size cutoff as ice crystals. During WDBT this procedure overestimates INP concentration, because large droplets are miscounted as ice crystals. Here we design a new analysis method based on depolarization ratio that can extend the range of operating conditions of the CFDC. The method agrees reasonably well with the traditional method under non-WDBT conditions with a mean percent error of ±32.1 %. Additionally, a comparison with the Colorado State University CFDC shows that the new analysis method can be used reliably during WDBT conditions.

54 ENVIRONMENTAL SCIENCES↗

The effect of gas-phase polycyclic aromatic hydrocarbons on the formation and properties of biogenic secondary organic aerosol particles

When secondary organic aerosol (SOA) particles are formed by ozonolysis in the presence of gas-phase polycyclic aromatic hydrocarbons (PAHs), their formation and properties are significantly different from SOA particles formed without PAHs. For all SOA precursors and all PAHs, discussed in this study, the presence of the gas-phase PAHs during SOA formation significantly affects particle mass loadings, composition, growth, evaporation kinetics, and viscosity. SOA particles formed in the presence of PAHs have, as part of their compositions, trapped unreacted PAHs and products of heterogeneous reactions between PAHs and ozone. Compared to ‘pure’ SOA particles, these particles exhibit slower evaporation kinetics, have higher fractions of non-volatile components, like oligomers, and higher viscosities, assuring their longer atmospheric lifetimes. In turn, the increased viscosity and decreased volatility provide a shield that protects PAHs from chemical degradation and evaporation, allowing for the long-range transport of these toxic pollutants. The magnitude of the effect of PAHs on SOA formation is surprisingly large. The presence of PAHs during SOA formation increases mass loadings by factors of two to five, and particle number concentrations, in some cases, by more than a factor of 100. Increases in SOA mass, particle number concentrations, and lifetime have important implications to many atmospheric processes related to climate, weather, visibility, and human health, all of which relate to the interactions between biogenic SOA and anthropogenic PAHs. The synergistic relationship between SOA and PAHs presented here are clearly complex and call for future research to elucidate further the underlying processes and their exact atmospheric implications.

54 ENVIRONMENTAL SCIENCES↗