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1. Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions

   https://doi.org/10.5194/acp-24-911-2024  

   Patnaude, Ryan J; Moore, Kathryn A; Perkins, Russell J; Hill, Thomas_C J; DeMott, Paul J; Kreidenweis, Sonia M (January 2024, Atmospheric Chemistry and Physics)

   Abstract. Sea spray aerosols (SSAs) represent one of the most abundant aerosol types on a global scale and have been observed at all altitudes including the upper troposphere. SSA has been explored in recent years as a source of ice-nucleating particles (INPs) in cirrus clouds due to the ubiquity of cirrus clouds and the uncertainties in their radiative forcing. This study expands upon previous works on low-temperature ice nucleation of SSA by investigating the effects of atmospheric aging of SSA and the ice-nucleating activity of newly formed secondary marine aerosols (SMAs) using an oxidation flow reactor. Polydisperse aerosol distributions were generated from a marine aerosol reference tank (MART) filled with 120 L of real or artificial seawater and were dried to very low relative humidity to crystallize the salt constituents of SSA prior to their subsequent freezing, which was measured using a continuous flow diffusion chamber (CFDC). Results show that for primary SSA (pSSA), as well as aged SSA and SMA (aSSA+SMA) at temperatures >220 K, homogeneous conditions (92 %–97 % relative humidity with respect to water – RHw) were required to freeze 1 % of the particles. However, below 220 K, heterogeneous nucleation occurs for both pSSA and aSSA+SMA at much lower RHw, where up to 1 % of the aerosol population freezes between 75 % and 80 % RHw. Similarities between freezing behaviors of the pSSA and aSSA+SMA at all temperatures suggest that the contributions of condensed organics onto the pSSA or alteration of functional groups in pSSA via atmospheric aging did not hinder the major heterogeneous ice nucleation process at these cirrus temperatures, which have previously been shown to be dominated by the crystalline salts. Occurrence of a 1 % frozen fraction of SMA, generated in the absence of primary SSA, was observed at or near water saturation below 220 K, suggesting it is not an effective INP at cirrus temperatures, similar to findings in the literature on other organic aerosols. Thus, any SMA coatings on the pSSA would only decrease the ice nucleation behavior of pSSA if the organic components were able to significantly delay water uptake of the inorganic salts, and apparently this was not the case. Results from this study demonstrate the ability of lofted primary sea spray particles to remain an effective ice nucleator at cirrus temperatures, even after atmospheric aging has occurred over a period of days in the marine boundary layer prior to lofting. We were not able to address aging processes under upper-tropospheric conditions. 

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2. Marine aerosol generation experiments in the High Arctic during summertime

   https://doi.org/10.1525/elementa.2023.00134  

   Mirrielees, Jessica A; Kirpes, Rachel M; Costa, Emily J; Porter, Grace_C E; Murray, Benjamin J; Lata, Nurun N; Boschi, Vanessa; China, Swarup; Grannas, Amanda M; Ault, Andrew P; et al (October 2024, Elem Sci Anth)

   The rapidly warming Arctic has transitioned to thinner sea ice which fractures, producing leads. Few studies have investigated Arctic sea spray aerosol (SSA) produced from open ocean, leads, and melt ponds, which vary in salinity and organic and microbial community composition. A marine aerosol reference tank was deployed aboard an icebreaker to the Arctic Ocean during August–September 2018 to study SSA generated from locally collected surface waters. Aerosol generation experiments were carried out using water collected from the marginal ice zone, a human-made hole in sea ice near the North Pole, and both lead and melt pond water during an ice floe drift period. Salinity, chlorophyll a, organic carbon, nitrogen, and microbial community composition were measured. Eukaryotic plankton and bacterial abundance were elevated in experimental water from the marginal ice zone, but the relative contributions from major eukaryotic taxonomic groups varied little across the experiments. The chemical composition of individual SSA particles was analyzed using Raman microspectroscopy and computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy. Individual sea salt aerosol, primary organic aerosol, and mineral dust particles were observed. Sea salt aerosol constituted 44–95% of individual submicrometer and 68–100% of supermicrometer particles, by number, generated during each experiment. Carbon was detected in 85%, by number, of the individual sea salt particles, with visible organic coatings. Carbohydrates were detected in 72% of particles, by number, with smaller contributions from long-chain fatty acids (13%) and siliceous material (15%). SSA generated from melt pond water contained only long-chain fatty acids and siliceous material. Quantification of the ice-nucleating activity showed that locally produced SSA may define the High Arctic background ice-nucleating particle population, but cannot account for the peak atmospheric concentrations observed. As the Arctic warms, the increasing SSA emissions have a complex dependence on changing biological and physical processes. 

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3. High Arctic Ocean seawater and aerosol data, August-September 2018

   https://doi.org/10.18739/A2QZ22J9F  

   Matrai, Patricia; Pratt, Kerri; Grannas, Amanda; Ault, Andrew; Boschi, Vanessa (January 2024, NSF Arctic Data Center)

   The Arctic is rapidly warming and has transitioned to thinner sea ice which fractures, producing leads. Sea ice loss is expected to be increasing sea spray aerosol production in the High Arctic. Few studies have investigated Arctic sea spray aerosol (SSA) produced from open ocean, leads, and melt ponds, characterized by varied salinity, microbial community, and organic composition. The concentrations, size distributions, single-particle composition, and ice-nucleating activity of the SSA experimentally-generated were measured and compared to the chemical and biological properties of the surface waters. A marine aerosol reference tank (MART) was deployed aboard the Swedish Icebreaker Oden to the high Arctic Ocean during August – September 2018 to study SSA generated from locally-collected surface water. Surface water salinity, chlorophyll-a, organic carbon, nitrogen, and microbial community composition (18s and 16s DNA-derived, flow cytometry of nano- and picoplankton) data are submitted. Experimental aerosol data submitted include type, size, mole ratio, Raman spectra, Raman type, and ice nucleating particles. High resolution Fourier Transform Ion Cyclotron Resonance mass spectrometry (FTICR-MS) data for surface water and experimentally-generated aerosol dissolved organic matter are included . 

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4. SNICAR-ADv4: a physically based radiative transfer model to represent the spectral albedo of glacier ice

   https://doi.org/10.5194/tc-16-1197-2022  

   Whicker, Chloe A.; Flanner, Mark G.; Dang, Cheng; Zender, Charles S.; Cook, Joseph M.; Gardner, Alex S. (January 2022, The Cryosphere)

   Abstract. Accurate modeling of cryospheric surface albedo is essential for ourunderstanding of climate change as snow and ice surfaces regulate the globalradiative budget and sea-level through their albedo and massbalance. Although significant progress has been made using physicalprinciples to represent the dynamic albedo of snow, models of glacier icealbedo tend to be heavily parameterized and not explicitly connected withphysical properties that govern albedo, such as the number and size of airbubbles, specific surface area (SSA), presence of abiotic and biotic lightabsorbing constituents (LACs), and characteristics of any overlyingsnow. Here, we introduce SNICAR-ADv4, an extension of the multi-layertwo-stream delta-Eddington radiative transfer model with theadding–doubling solver that has been previously applied to represent snowand sea-ice spectral albedo. SNICAR-ADv4 treats spectrally resolved Fresnelreflectance and transmittance between overlying snow and higher-densityglacier ice, scattering by air bubbles of varying sizes, and numerous typesof LACs. SNICAR-ADv4 simulates a wide range of clean snow and ice broadbandalbedo (BBA), ranging from 0.88 for (30 µm) fine-grain snow to 0.03for bare and bubble-free ice under direct light. Our results indicate thatrepresenting ice with a density of 650 kg m−3 as snow with norefractive Fresnel layer, as done previously, generally overestimates theBBA by an average of 0.058. However, because mostnaturally occurring ice surfaces are roughened “white ice”, we recommendmodeling a thin snow layer over bare ice simulations. We find optimalagreement with measurements by representing cryospheric media with densitiesless than 650 kg m−3 as snow and larger-density media as bubbly icewith a Fresnel layer. SNICAR-ADv4 also simulates the non-linear albedoimpacts from LACs with changing ice SSA, with peak impact per unit mass ofLACs near SSAs of 0.1–0.01 m2 kg−1. For bare, bubble-free ice, LACsactually increase the albedo. SNICAR-ADv4 represents smooth transitionsbetween snow, firn, and ice surfaces and accurately reproduces measuredspectral albedos of a variety of glacier surfaces. This work paves the wayfor adapting SNICAR-ADv4 to be used in land ice model components of Earthsystem models. 

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5. Evaluating the impact of blowing-snow sea salt aerosol on springtime BrO and O₃ in the Arctic

   https://doi.org/10.5194/acp-20-7335-2020  

   Huang, Jiayue; Jaeglé, Lyatt; Chen, Qianjie; Alexander, Becky; Sherwen, Tomás; Evans, Mat J.; Theys, Nicolas; Choi, Sungyeon (January 2020, Atmospheric Chemistry and Physics)

   Abstract. We use the GEOS-Chem chemical transport model to examine theinfluence of bromine release from blowing-snow sea salt aerosol (SSA) onspringtime bromine activation and O3 depletion events (ODEs) in theArctic lower troposphere. We evaluate our simulation against observations oftropospheric BrO vertical column densities (VCDtropo) from the GOME-2 (second Global Ozone Monitoring Experiment)and Ozone Monitoring Instrument (OMI) spaceborne instruments for 3 years (2007–2009), as well asagainst surface observations of O3. We conduct a simulation withblowing-snow SSA emissions from first-year sea ice (FYI; with a surface snowsalinity of 0.1 psu) and multi-year sea ice (MYI; with a surface snowsalinity of 0.05 psu), assuming a factor of 5 bromide enrichment of surfacesnow relative to seawater. This simulation captures the magnitude ofobserved March–April GOME-2 and OMI VCDtropo to within 17 %, as wellas their spatiotemporal variability (r=0.76–0.85). Many of the large-scalebromine explosions are successfully reproduced, with the exception of eventsin May, which are absent or systematically underpredicted in the model. Ifwe assume a lower salinity on MYI (0.01 psu), some of the bromine explosionsevents observed over MYI are not captured, suggesting that blowing snow overMYI is an important source of bromine activation. We find that the modeledatmospheric deposition onto snow-covered sea ice becomes highly enriched inbromide, increasing from enrichment factors of ∼5 inSeptember–February to 10–60 in May, consistent with composition observations of freshly fallen snow. We propose that this progressive enrichment indeposition could enable blowing-snow-induced halogen activation to propagateinto May and might explain our late-spring underestimate in VCDtropo.We estimate that the atmospheric deposition of SSA could increase snow salinityby up to 0.04 psu between February and April, which could be an importantsource of salinity for surface snow on MYI as well as FYI covered by deepsnowpack. Inclusion of halogen release from blowing-snow SSA in oursimulations decreases monthly mean Arctic surface O3 by 4–8 ppbv(15 %–30 %) in March and 8–14 ppbv (30 %–40 %) in April. We reproduce atransport event of depleted O3 Arctic air down to 40∘ Nobserved at many sub-Arctic surface sites in early April 2007. While oursimulation captures 25 %–40 % of the ODEs observed at coastal Arctic surfacesites, it underestimates the magnitude of many of these events and entirelymisses 60 %–75 % of ODEs. This difficulty in reproducing observed surfaceODEs could be related to the coarse horizontal resolution of the model, theknown biases in simulating Arctic boundary layer exchange processes, thelack of detailed chlorine chemistry, and/or the fact that we did not includedirect halogen activation by snowpack chemistry. 

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