Frost Flowers Research Articles

Arctic Sea ice leads detected using sentinel-1B SAR image and their responses to atmosphere circulation and sea ice dynamics

Arctic sea ice leads are linear fractures in pack ice, which provide narrow windows for the enhanced exchange of mass, energy, and momentum between the atmosphere and ocean. However, the parameterisations of the sub-grid (< 1 km) lead distribution and its associated dynamic processes are still challenging for numerical sea ice modelling. This study explores the dynamics governing lead formation in the Arctic Ocean using multiple data sources including Sentinel-1 synthetic aperture radar (SAR) images, buoy array, and atmospheric reanalysis. Random forest (RF) models trained based on the polarisation and texture features of SAR images were compared, and an optimal RF model sensitive to narrow leads was selected with implementation of screening based on lead geometry. As a case study, the lead distribution along the trajectory of buoy array in the central Arctic Ocean during the freezing period of 2018–2019 was obtained. An enhanced lead opening was observed as the sea ice motion swerved from clockwise circulation following the Beaufort Gyre (BG) to meridional advection when assembled into the Transpolar Drift (TPD). Synoptically, active lead-opening events associated with ice divergence were driven by episodic cyclones. We noticed a dramatic change in the backscatter signal over the leads caused by the growth of thin ice and formation of frost flowers. The identification and the evolution of narrow leads during the freezing season given in this study are conducive to increasing our understanding of the response mechanism of sea ice to atmospheric dynamic processes and supporting the numerical simulation of leads.

Modelling wintertime sea-spray aerosols under Arctic haze conditions

Abstract. Anthropogenic and natural emissions contribute to enhanced concentrations of aerosols in the Arctic winter and early spring, with most attention being paid to anthropogenic aerosols that contribute to so-called Arctic haze. Less-well-studied wintertime sea-spray aerosols (SSAs) under Arctic haze conditions are the focus of this study, since they can make an important contribution to wintertime Arctic aerosol abundances. Analysis of field campaign data shows evidence for enhanced local sources of SSAs, including marine organics at Utqiaġvik (formerly known as Barrow) in northern Alaska, United States, during winter 2014. Models tend to underestimate sub-micron SSAs and overestimate super-micron SSAs in the Arctic during winter, including the base version of the Weather Research Forecast coupled with Chemistry (WRF-Chem) model used here, which includes a widely used SSA source function based on Gong et al. (1997). Quasi-hemispheric simulations for winter 2014 including updated wind speed and sea-surface temperature (SST) SSA emission dependencies and sources of marine sea-salt organics and sea-salt sulfate lead to significantly improved model performance compared to observations at remote Arctic sites, notably for coarse-mode sodium and chloride, which are reduced. The improved model also simulates more realistic contributions of SSAs to inorganic aerosols at different sites, ranging from 20 %–93 % in the observations. Two-thirds of the improved model performance is from the inclusion of the dependence on SSTs. The simulation of nitrate aerosols is also improved due to less heterogeneous uptake of nitric acid on SSAs in the coarse mode and related increases in fine-mode nitrate. This highlights the importance of interactions between natural SSAs and inorganic anthropogenic aerosols that contribute to Arctic haze. Simulation of organic aerosols and the fraction of sea-salt sulfate are also improved compared to observations. However, the model underestimates episodes with elevated observed concentrations of SSA components and sub-micron non-sea-salt sulfate at some Arctic sites, notably at Utqiaġvik. Possible reasons are explored in higher-resolution runs over northern Alaska for periods corresponding to the Utqiaġvik field campaign in January and February 2014. The addition of a local source of sea-salt marine organics, based on the campaign data, increases modelled organic aerosols over northern Alaska. However, comparison with previous available data suggests that local natural sources from open leads, as well as local anthropogenic sources, are underestimated in the model. Missing local anthropogenic sources may also explain the low modelled (sub-micron) non-sea-salt sulfate at Utqiaġvik. The introduction of a higher wind speed dependence for sub-micron SSA emissions, also based on Arctic data, reduces biases in modelled sub-micron SSAs, while sea-ice fractions, including open leads, are shown to be an important factor controlling modelled super-micron, rather than sub-micron, SSAs over the north coast of Alaska. The regional results presented here show that modelled SSAs are more sensitive to wind speed dependence but that realistic modelling of sea-ice distributions is needed for the simulation of local SSAs, including marine organics. This study supports findings from the Utqiaġvik field campaign that open leads are the primary source of fresh and aged SSAs, including marine organic aerosols, during wintertime at Utqiaġvik; these findings do not suggest an influence from blowing snow and frost flowers. To improve model simulations of Arctic wintertime aerosols, new field data on processes that influence wintertime SSA production, in particular for fine-mode aerosols, are needed as is improved understanding about possible local anthropogenic sources.

Preparation of porous silicon by vacuum sublimation dealloying method

Porous silicon has many potential applications in lithium-ion battery anodes and medical sensors, owing to its high specific capacity and photoluminescence properties. In this work, porous silicon is prepared with vacuum sublimation dealloying method by heating Mg2Si precursor to 750 °C and holding it for 1 h under vacuum. The relationship between pressure and temperature, as well as the characteristics of the longitudinal section of condensation products show that the sublimation process of Mg in Mg2Si precursor can be divided into three stages. The aperture distribution curves of the Brunauer-Emmett-Teller (BET) and Mercury Intrusion Porosimetry (MIP) of porous silicon show that the pore size of mesopores is between 3.1 ± 0.2 and 6.3 ± 0.2 nm, and that of macropores is between 351.6 ± 1 and 2101.7 ± 1 nm. The prepared porous silicon has pores with frost flower shaped and shrub-shaped structures in the interior and polygonal contoured pores on the surface. This paper aims to investigate the reaction mechanism of vacuum sublimation dealloying method and provide a foundation for optimizing the performance of porous silicon in applications such as lithium-ion battery anodes and hydrogen generating materials by studying its unique pore structure.

Technical note: Sublimation of frozen CsCl solutions in an environmental scanning electron microscope (ESEM) – determining the number and size of salt particles relevant to sea salt aerosols

Abstract. We present a novel technique that elucidates the mechanism of the formation of small aerosolizable salt particles from salty frozen samples. We demonstrated that CsCl may be a suitable probe for sea salts due to its similar subzero properties and sublimation outcomes: CsCl substantially increased the visibility of the salt both during and after ice sublimation. Hence, we identified the factors that, during the sublimation of a frozen salty solution, are important in generating fine salt particles as a possible source of salt aerosol. The number, size, and structure of the particles that remain after ice sublimation were investigated with respect to the concentration of the salt in the sample, the freezing method, and the sublimation temperature. The last-named aspect is evidently of primary importance for the preference of fine salt crystals over a large compact piece of salt; we showed that the formation of small salt particles is generally restricted if the brine is liquid during the ice sublimation, i.e. at temperatures higher than the eutectic temperature (Teu). Small salt particles that might be a source of atmospheric aerosols were formed predominantly at temperatures below Teu, and their structures strongly depended on the concentration of the salt. For example, the sublimation of those samples that exhibited a concentration of less than 0.05 M often produced small aerosolizable isolated particles that are readily able to be windblown. Conversely, the sublimation of 0.5 M samples led to the formation of relatively stable and largely interconnected salt structures. Our findings are in good agreement with other laboratory studies which have unsuccessfully sought salt aerosols from, for example, frost flowers at temperatures above Teu. This study offers an explanation of the previously unexplored behaviour.

The mystery of the ice cold rose-Microbiome of an Arctic winter frost flower.

Under very cold conditions, delicate ice-crystal structures called frost flowers emerge on the surface of newly formed sea ice. These understudied, ephemeral structures include saline brine, organic material, inorganic nutrients, and bacterial and archaeal communities in their brine channels. Hitherto, only a few frost flowers have been studied during spring and these have been reported to be dominated by Rhizobia or members of the SAR11 clade. Here we report on the microbiome of frost flowers sampled during the winter and polar night in the Barents Sea. There was a distinct difference in community profile between the extracted DNA and RNA, but both were dominated by members of the SAR11 clade (78% relative abundance and 41.5% relative activity). The data further suggested the abundance and activity of Cand. Nitrosopumilus, Nitrospinia, and Nitrosomonas. Combined with the inference of marker genes based on the 16S rRNA gene data, this indicates that sulfur and nitrogen cycling are likely the major metabolism in these ephemeral structures.

Colloidal associations of major and trace elements in the snow pack across a 2800-km south-north gradient of western Siberia

Colloidal (size 1 nm to 1 μm) transport of major and trace elements, notably micronutrients and low-solubility geochemical tracers, is a ubiquitous and well-established feature for all surface and soil waters in boreal and subarctic regions. However, little is known on the colloidal associations of organic carbon (OC) and major and trace elements in atmospheric precipitation such as snow. This is despite significant efforts devoted to distinguishing the soluble and particulate transport of trace metals and contaminants by atmospheric aerosols. To acquire a snap-shot of major and trace element size fractionation in the snow cover of western Siberia, we sampled snow cores integrated over the entire depth (0–50 cm until bottom) across a sizable (2800 km) south - north transect in the Ob River watershed (western Siberia). A number of trace metal pollutants (Cr, Ni, Zn, Cd) exhibited significant linkage, pronounced over the first 20 km, to sources of local pollution. Some elements (P, Mn, Zn, Ba) also demonstrated an increase in their colloidal fraction in the proximity of pollution centers, possibly reflecting input from industrial centers and gas flares.Following centrifuginal ultrafiltration, we analyzed total dissolved (< 0.22 μm), two colloidal (high molecular weight, HMW50 kDa ̶ 0.22 μm; medium molecular weight MMW3 kDa ̶ 50 kDa) and low molecular weight (LMW < 3 kDa) fractions in the melted snow for all major and trace elements. We discovered sizable (20 to 70%) proportion of some major (Ca, SO4) and many trace (Fe, Y, Zn, Sb, La, Ce, Yb, Pb) elements in the colloidal (3 kDa - 0.22 μm) form, without significant link to latitude, type of biome, or the concentration of possible colloidal carrier (DOC, Fe, Al, Ca, SO4). The origin of snow water colloids in snow can be hypothesized to stem from solute freezing on lake surfaces (Fe, OC), frost flowers of the Arсtic ice (Ca, SO4), clays dispersion (Al, Si) and sulphur dioxide oxidation particles (SO4, oxyanions). Via hydrochemical mass balance calculations, we demonstrate an overwhelming impact of snow melt on spring-time riverine export of Cd, Pb, Zn, As, Sb and Cs. These preliminary results call for further studies of atmospheric colloids including those originating from rainwater.

Ediacaran periglacial sedimentary structures

Ediacaran fossils are sometimes reconstructed as colorful organisms of clear azure seas like tropical lagoons, or as ghostlike forms in deep, dark oceans. Alternatively, they can be envisaged as sessile organisms in frigid soils, to judge from associated Ediacaran periglacial paleosols and tillites. Additional evidence of cool Ediacaran paleoclimate now comes from reinterpretation of two supposed trace fossils: (1) grooves radiating from Ediacaran fossils interpreted as radular feeding traces (“Kimberichnus”) of supposed molluscs (Kimberella), and (2) chains of fossil impressions interpreted as feeding traces (“Epibaion”) of supposed worms or placozoans (Yorgia, Dickinsonia). The grooves are not curved with rounded ends like radular scratches, but with sharp or crudely bifid tips like frost flowers and frost needles extruded from plant debris. Fossil impressions in chains are not sequential feeding stations, but in polygonal arrays, like vagrant lichens and mosses displaced by wind gusts and periglacial frost boils. Thus, neither the taphomorph “Epibaion”, nor the ice crystal pseudomorphs “Kimberichnus” are valid ichnogenera. These newly recognized frost boils, needle ice, frost feathers, frost hair and frost shawls are additions to isotopic and glendonite evidence that the Ediacaran was another period in Earth history when even low paleolatitudes were cool.

Effect of ikaite precipitation on phosphate removal in sea ice

Ikaite (CaCO3·6H2O) precipitation in sea ice has been shown to affect CO2 exchange between the atmosphere and ocean. A laboratory study indicates that it could also co-precipitate phosphate from sea ice, which has the potential to affect sea-ice biogeochemical processes. However, the relative importance of ikaite precipitation on phosphate removal under sea-ice conditions remains unknown. We investigated ikaite precipitation in both frost flowers and seaice (under two scenarios: flooded by seawater and non-flooded) in an outdoor sea-ice mesocosm experiment, and in sea ice under natural conditions in north-eastern Greenland. The ice mesocosm experiment showed that ikaite was highly enriched in frost flowers with a concentration of up to 350 µmol·kg–1. Ikaite was also detected in the surface layer of sea ice, ranging from ca. 13 µmol·kg–1 in the non-flooded ice to ca. 95 µmol·kg–1 in the flooded ice. However, under all these conditions, no phosphate co-precipitation with ikaite was observed. The field study in Greenland showed similar results: ikaite was detected in surface ice with an average concentration of 13.8 µmol·kg–1, but no phosphate removal due to ikaite precipitation was observed. These results suggest that the impact of ikaite precipitation on phosphate and the sea-ice ecosystem might not be as significant as imagined previously.

Wintertime Arctic Sea Spray Aerosol Composition Controlled by Sea Ice Lead Microbiology.

The Arctic is experiencing the greatest warming on Earth, as most evident by rapid sea ice loss. Delayed sea ice freeze-up in the Alaskan Arctic is decreasing wintertime sea ice extent and changing marine biological activity. However, the impacts of newly open water on wintertime sea spray aerosol (SSA) production and atmospheric composition are unknown. Herein, we identify SSA, produced locally from open sea ice fractures (leads), as the dominant aerosol source in the coastal Alaskan Arctic during winter, highlighting the year-round nature of Arctic SSA emissions. Nearly all of the individual SSA featured thick organic coatings, consisting of marine saccharides, amino acids, fatty acids, and divalent cations, consistent with exopolymeric secretions produced as cryoprotectants by sea ice algae and bacteria. In contrast, local summertime SSA lacked these organic carbon coatings, or featured thin coatings, with only open water nearby. The individual SSA composition was not consistent with frost flowers or surface snow above sea ice, suggesting that neither hypothesized frost flower aerosolization nor blowing snow sublimation resulted in the observed SSA. These results further demonstrate the need for inclusion of lead-based SSA production in modeling of Arctic atmospheric composition. The identified connections between changing sea ice, microbiology, and SSA point to the significance of sea ice lead biogeochemistry in altering Arctic atmospheric composition, clouds, and climate feedbacks during winter.

Diversity of metals and metal-interactive bacterial populations in different types of Arctic snow and frost flowers: Implications on snow freeze-melt processes in a changing climate

Arctic snow has been shown to be a reactive interface for key physical, chemical, and microbiological processes, affecting the Arctic's oxidation, biodiversity, radiation, and climate. To explore the potential links between snow-borne metal contaminants and metal-interactive bacteria, to freezing/melting processes, we performed concurrent chemical characterization, genomic, and morphological analysis of five different Arctic snowpack (accumulated, blowing, fresh falling, surface hoar, and wind pack snow) and frost flower in Utqiaġvik (Barrow), Alaska, using Montreal urban snow as reference. Several complementary analytical techniques, including triple quad ICP-MS/MS along with various chromatography techniques, thermal ionization mass spectrometer (TIMS), high-resolution transition electron microscopy with electron dispersive X-ray spectroscopy (HR-TEM/EDS), and next generation sequencing (NGS), were deployed. Distinct metal composition and bacterial distribution among samples were observed. The concentration of 27 different transition, post-transition, rare, and radioactive metals were determined in molten snow and frost flower, as well as filtered samples. The range of three highest detected metal concentrations among samples were: Hg (3.294–134.485 μg/L), Fe (0.719–34.469 μg/L), and Sr (1.676–19,297.000 μg/L). NGS analysis led to the identification of metal interacting bacteria in all types of snow and frost flowers in the Arctic (blowing snow (1239), surface hoar snow (2243), windpack (2431), frost flowers (1440)), and Montreal urban snow (5498)) with specific bacterial genera such as: Acinetobacter, Arcenicella, Azospirillum (surface hoar snow), Arthrobacter, Paenibacillus (blowing snow), and Cycloclasticus, OM182 clade (frost flower). Several types of bacteria with confirmed or associated ice nucleation activity were observed in different types of snow, and frost flower including Pseudomonas genera (e.g., Pseudomonas fluorescens), Flavobacterium, Corynebacterium, and Pseudoxanthomonas. The implications of the above findings to snow-air interactions including nanoparticles, namely during melting and freezing cycles, and to probe the impact of various natural and anthropogenic activities are herein discussed.

Chemical characteristics of submicron aerosols observed at the King Sejong Station in the northern Antarctic Peninsula from fall to spring

The water-soluble ions and carbonaceous compounds of PM1 were measured at the King Sejong Station (KSG) in the northern part of Antarctic Peninsula from March to November in 2009. As the sum of all measured species including organic matter [OM; organic carbon (OC)*1.9], the PM1 mass reached a maximum of 936 ng m−3 with the mean of 686 ± 226 ng m−3. The most abundant constituents were OM (389 ± 109 ng m−3) and sea-salts (Na+ and Cl−, 193 ± 122 ng m−3), which comprised 85% of the PM1 mass. In contrast, the contribution of SO42− was below 1% and its depletion relative to Na+ was prevalent particularly during winter, which was attributed to the frost flowers on newly formed sea-ice surface. The OC concentration was the highest in fall and its subcomponents OC2 and OC3 were moderately correlated with sea-salts (r = 0.5), indicating the marine biogenic source for OC. The elemental carbon (EC) concentration was much lower than OC, leading to the mean OC/EC ratio over 10. While the charred fraction of EC (EC1) was elevated by the long-range transport of biomass burning plume from nearby continent, the mass fraction of soot-EC (EC23) was increased concurrently with enhanced NO3−, suggesting EC23 as a good indicator for local influence in pristine environments like Antarctic region.

Using CALIOP to constrain blowing snow emissions of sea salt aerosols over Arctic and Antarctic sea ice

Abstract. Sea salt aerosols (SSA) produced on sea ice surfaces by blowing snow events or the lifting of frost flower crystals have been suggested as important sources of SSA during winter over polar regions. The magnitude and relative contribution of blowing snow and frost flower SSA sources, however, remain uncertain. In this study, we use 2007–2009 aerosol extinction coefficients from the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument onboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite and the GEOS-Chem global chemical transport model to constrain sources of SSA over Arctic and Antarctic sea ice. CALIOP retrievals show elevated levels of aerosol extinction coefficients (10–20 Mm−1) in the lower troposphere (0–2 km) over polar regions during cold months. The standard GEOS-Chem model underestimates the CALIOP extinction coefficients by 50 %–70 %. Adding frost flower emissions of SSA fails to explain the CALIOP observations. With blowing snow SSA emissions, the model captures the overall spatial and seasonal variation of CALIOP aerosol extinction coefficients over the polar regions but underestimates aerosol extinction over Arctic sea ice in fall to early winter and overestimates winter-to-spring extinction over Antarctic sea ice. We infer the monthly surface snow salinity on first-year sea ice required to minimize the discrepancy between CALIOP extinction coefficients and the GEOS-Chem simulation. The empirically derived snow salinity shows a decreasing trend between fall and spring. The optimized blowing snow model with inferred snow salinities generally agrees with CALIOP extinction coefficients to within 10 % over sea ice but underestimates them over the regions where frost flowers are expected to have a large influence. Frost flowers could thus contribute indirectly to SSA production by increasing the local surface snow salinity and, therefore, the SSA production from blowing snow. We carry out a case study of an Arctic blowing snow SSA feature predicted by GEOS-Chem and sampled by CALIOP. Using back trajectories, we link this feature to a blowing snow event that occurred 2 days earlier over first-year sea ice and was also detected by CALIOP.

Investigations into Frost Flower Physical Characteristics and the C-Band Scattering Response

A dedicated study on the physical characteristics and C-band scattering response of frost-flower-covered sea ice was performed in an artificial sea ice mesocosm over a 36-h period in January 2017. Meteorological conditions were observed and recorded automatically at the facility when the sea ice grew and frost flowers formed while the C-band scattering measurements were conducted continuously over a range of incidence angles. Surface roughness was characterized using a LiDAR. During the experiment, frost flowers did not initially form on the extremely smooth ice surface even though suitable meteorological conditions prevailed during their development (low air temperature, low near-surface wind speed, and high near-surface relative humidity). This provides evidence that both the presence of (i) liquid brine at the surface and (ii) raised nodules as nucleation points are required to enable frost flower initiation. As the ice thickened, we observed that raised nodules gradually appeared, frost flowers formed, and flowers subsequently spread to cover the surface over a six-hour period. In contrast to previous experiments, the frost flower layer did not become visibly saturated with liquid brine. The C-band scattering measurements exhibited increases as high as 14.8 dB (vertical polarization) in response to the frost flower formation with low incidence angles (i.e., 25°) showing the largest dynamic range. Co-polarization ratios responded to the physical and thermodynamic changes associated with the frost flower formation process. Our results indicate that brine expulsion at the sea ice surface and frost flower salination can have substantial temporal variability, which can be detected by scatterometer time-series measurements. This work contributes towards the operational satellite image interpretation for Arctic waters by improving our understanding of the highly variable C-band microwave scattering properties of young sea ice types.

Horizontal and vertical structure of reactive bromine events probed by bromine monoxide MAX-DOAS

Abstract. Heterogeneous photochemistry converts bromide (Br−) to reactive bromine species (Br atoms and bromine monoxide, BrO) that dominate Arctic springtime chemistry. This phenomenon has many impacts such as boundary-layer ozone depletion, mercury oxidation and deposition, and modification of the fate of hydrocarbon species. To study environmental controls on reactive bromine events, the BRomine, Ozone, and Mercury EXperiment (BROMEX) was carried out from early March to mid-April 2012 near Barrow (Utqiaġvik), Alaska. We measured horizontal and vertical gradients in BrO with multiple-axis differential optical absorption spectroscopy (MAX-DOAS) instrumentation at three sites, two mobile and one fixed. During the campaign, a large crack in the sea ice (an open lead) formed pushing one instrument package ∼ 250 km downwind from Barrow (Utqiaġvik). Convection associated with the open lead converted the BrO vertical structure from a surface-based event to a lofted event downwind of the lead influence. The column abundance of BrO downwind of the re-freezing lead was comparable to upwind amounts, indicating direct reactions on frost flowers or open seawater was not a major reactive bromine source. When these three sites were separated by ∼ 30 km length scales of unbroken sea ice, the BrO amount and vertical distributions were highly correlated for most of the time, indicating the horizontal length scales of BrO events were typically larger than ∼ 30 km in the absence of sea ice features. Although BrO amount and vertical distribution were similar between sites most of the time, rapid changes in BrO with edges significantly smaller than this ∼ 30 km length scale episodically transported between the sites, indicating BrO events were large but with sharp edge contrasts. BrO was often found in shallow layers that recycled reactive bromine via heterogeneous reactions on snowpack. Episodically, these surface-based events propagated aloft when aerosol extinction was higher (&gt; 0.1 km−1); however, the presence of aerosol particles aloft was not sufficient to produce BrO aloft. Highly depleted ozone (&lt; 1 nmol mol−1) repartitioned reactive bromine away from BrO and drove BrO events aloft in cases. This work demonstrates the interplay between atmospheric mixing and heterogeneous chemistry that affects the vertical structure and horizontal extent of reactive bromine events.

Frost flowers and sea-salt aerosols over seasonal sea-ice areas in northwestern Greenland during winter–spring

Abstract. Sea salts and halogens in aerosols, frost flowers, and brine play an important role in atmospheric chemistry in polar regions. Simultaneous sampling and observations of frost flowers, brine, and aerosol particles were conducted around Siorapaluk in northwestern Greenland during December 2013 to March 2014. Results show that water-soluble frost flower and brine components are sea-salt components (e.g., Na+, Cl−, Mg2+, K+, Ca2+, Br−, and iodine). Concentration factors of sea-salt components of frost flowers and brine relative to seawater were 1.14–3.67. Sea-salt enrichment of Mg2+, K+, Ca2+, and halogens (Cl−, Br−, and iodine) in frost flowers is associated with sea-salt fractionation by precipitation of mirabilite and hydrohalite. High aerosol number concentrations correspond to the occurrence of higher abundance of sea-salt particles in both coarse and fine modes, and blowing snow and strong winds. Aerosol number concentrations, particularly in coarse mode, are increased considerably by release from the sea-ice surface under strong wind conditions. Sulfate depletion by sea-salt fractionation was found to be limited in sea-salt aerosols because of the presence of non-sea-salt (NSS) SO42−. However, coarse and fine sea-salt particles were found to be rich in Mg. Strong Mg enrichment might be more likely to proceed in fine sea-salt particles. Magnesium-rich sea-salt particles might be released from the surface of snow and slush layer (brine) on sea ice and frost flowers. Mirabilite-like and ikaite-like particles were identified only in aerosol samples collected near new sea-ice areas. From the field evidence and results from earlier studies, we propose and describe sea-salt cycles in seasonal sea-ice areas.

Evaporating brine from frost flowers with electron microscopy and implications for atmospheric chemistry and sea-salt aerosol formation

Abstract. An environmental scanning electron microscope (ESEM) was used for the first time to obtain well-resolved images, in both temporal and spatial dimensions, of lab-prepared frost flowers (FFs) under evaporation within the chamber temperature range from −5 to −18 °C and pressures above 500 Pa. Our scanning shows temperature-dependent NaCl speciation: the brine covering the ice was observed at all conditions, whereas the NaCl crystals were formed at temperatures below −10 °C as the brine oversaturation was achieved. Finger-like ice structures covered by the brine, with a diameter of several micrometres and length of tens to 100 µm, are exposed to the ambient air. The brine-covered fingers are highly flexible and cohesive. The exposure of the liquid brine on the micrometric fingers indicates a significant increase in the brine surface area compared to that of the flat ice surface at high temperatures; the NaCl crystals formed can become sites of heterogeneous reactivity at lower temperatures. There is no evidence that, without external forces, salty FFs could automatically fall apart to create a number of sub-particles at the scale of micrometres as the exposed brine fingers seem cohesive and hard to break in the middle. The fingers tend to combine together to form large spheres and then join back to the mother body, eventually forming a large chunk of salt after complete dehydration. The present microscopic observation rationalizes several previously unexplained observations, namely, that FFs are not a direct source of sea-salt aerosols and that saline ice crystals under evaporation could accelerate the heterogeneous reactions of bromine liberation.

A glaciochemical study of the 120 m ice core from Mill Island, East Antarctica

Abstract. A 120 m ice core was drilled on Mill Island, East Antarctica (65°30′ S, 100°40′ E) during the 2009/2010 Australian Antarctic field season. Contiguous discrete 5 cm samples were measured for hydrogen peroxide, water stable isotopes, and trace ion chemistry. The ice core was annually dated using a combination of chemical species and water stable isotopes. The Mill Island ice core preserves a climate record covering 97 years from 1913 to 2009 CE, with a mean snow accumulation of 1.35 m (ice-equivalent) per year (mIE yr−1). This northernmost East Antarctic coastal ice core site displays trace ion concentrations that are generally higher than other Antarctic ice core sites (e.g. mean sodium levels were 254 µEq L−1). The trace ion record at Mill Island is characterised by a unique and complex chemistry record with three distinct regimes identified. The trace ion record in regime A displays clear seasonality from 2000 to 2009 CE; regime B displays elevated concentrations with no seasonality from 1934 to 2000 CE; and regime C displays relatively low concentrations with seasonality from 1913 to 1934 CE. Sea salts were compared with instrumental data, including atmospheric models and satellite-derived sea-ice concentration, to investigate influences on the Mill Island ice core record. The mean annual sea salt record does not correlate with wind speed. Instead, sea-ice concentration to the east of Mill Island likely influences the annual mean sea salt record. A mechanism involving formation of frost flowers on sea ice is proposed to explain the extremely high sea salt concentration. The Mill Island ice core records are unexpectedly complex, with strong modulation of the trace chemistry on long timescales.

Wintertime enhancements of sea salt aerosol in polar regions consistent with a sea ice source from blowing snow

Abstract. Sea salt aerosols (SSA) are generated via air bubbles bursting at the ocean surface as well as by wind mobilization of saline snow and frost flowers over sea-ice-covered areas. The relative magnitude of these sources remains poorly constrained over polar regions, affecting our ability to predict their impact on halogen chemistry, cloud formation, and climate. We implement a blowing snow and a frost flower emission scheme in the GEOS-Chem global chemical transport model, which we validate against multiyear (2001–2008) in situ observations of SSA mass concentrations at three sites in the Arctic, two sites in coastal Antarctica, and from the 2008 ICEALOT cruise in the Arctic. A simulation including only open ocean emissions underestimates SSA mass concentrations by factors of 2–10 during winter–spring for all ground-based and ship-based observations. When blowing snow emissions are added, the model is able to reproduce observed wintertime SSA concentrations, with the model bias decreasing from a range of −80 to −34 % for the open ocean simulation to −2 to +9 % for the simulation with blowing snow emissions. We find that the frost flower parameterization cannot fully explain the high wintertime concentrations and displays a seasonal cycle decreasing too rapidly in early spring. Furthermore, the high day-to-day variability of observed SSA is better reproduced by the blowing snow parameterization. Over the Arctic (&gt; 60° N) (Antarctic, &gt; 60° S), we calculate that submicron SSA emissions from blowing snow account for 1.0 Tg yr−1 (2.5 Tg yr−1), while frost flower emissions lead to 0.21 Tg yr−1 (0.25 Tg yr−1) compared to 0.78 Tg yr−1 (1.0 Tg yr−1) from the open ocean. Blowing snow emissions are largest in regions where persistent strong winds occur over sea ice (east of Greenland, over the central Arctic, Beaufort Sea, and the Ross and Weddell seas). In contrast, frost flower emissions are largest where cold air temperatures and open leads are co-located (over the Canadian Arctic Archipelago, coastal regions of Siberia, and off the Ross and Ronne ice shelves). Overall, in situ observations of mass concentrations of SSA suggest that blowing snow is likely to be the dominant SSA source during winter, with frost flowers playing a much smaller role.

Seasonal Study of Mercury Species in the Antarctic Sea Ice Environment.

Limited studies have been conducted on mercury concentrations in the polar cryosphere and the factors affecting the distribution of mercury within sea ice and snow are poorly understood. Here we present the first comprehensive seasonal study of elemental and total mercury concentrations in the Antarctic sea ice environment covering data from measurements in air, sea ice, seawater, snow, frost flowers, and brine. The average concentration of total mercury in sea ice decreased from winter (9.7 ng L-1) to spring (4.7 ng L-1) while the average elemental mercury concentration increased from winter (0.07 ng L-1) to summer (0.105 ng L-1). The opposite trends suggest potential photo- or dark oxidation/reduction processes within the ice and an eventual loss of mercury via brine drainage or gas evasion of elemental mercury. Our results indicate a seasonal variation of mercury species in the polar sea ice environment probably due to varying factors such as solar radiation, temperature, brine volume, and atmospheric deposition. This study shows that the sea ice environment is a significant interphase between the polar ocean and the atmosphere and should be accounted for when studying how climate change may affect the mercury cycle in polar regions.

Potential sea salt aerosol sources from frost flowers in the pan‐Arctic region

AbstractIn order to better represent observed wintertime aerosol mass and number concentrations in the pan‐Arctic (60°N–90°N) region, we implemented an observationally based parameterization for estimating sea salt production from frost flowers in the Community Earth System Model (CESM, version 1.2.1). In this work, we evaluate the potential influence of this sea salt source on the pan‐Arctic climate. Results show that frost flower salt emissions increase the modeled surface sea salt aerosol mass concentration by roughly 200% at Barrow and 100% at Alert and accumulation‐mode number concentration by about a factor of 2 at Barrow and more than a factor of 10 at Alert in the winter months when new sea ice and frost flowers are present. The magnitude of sea salt aerosol mass and number concentrations at the surface in Barrow during winter simulated by the model configuration that includes this parameterization agrees better with observations by 48% and 12%, respectively, than the standard CESM simulation without a frost flower salt particle source. At Alert, the simulation with this parameterization overestimates observed sea salt aerosol mass concentration by 150% during winter in contrast to the underestimation of 63% in the simulation without this frost flower source, while it produces particle number concentration about 14% closer to observation than the standard CESM simulation. However, because the CESM version used here underestimates transported sulfate in winter, the reference accumulation‐mode number concentrations at Alert are also underestimated. Adding these frost flower salt particle emissions increases sea salt aerosol optical depth by 10% in the pan‐Arctic region and results in a small cooling at the surface. The increase in salt aerosol mass concentrations of a factor of 8 provides nearly two times the cloud condensation nuclei concentration at supersaturation of 0.1%, as well as 10% increases in cloud droplet number and 40% increases in liquid water content near coastal regions adjacent to continents. These cloud changes reduce longwave cloud forcing at the top of the atmosphere by 3% and cause a small surface warming, increasing the downward longwave flux at the surface by 1.8 W m−2 in the pan‐Arctic under the present‐day climate. This regional average longwave warming due to the presence of clouds attributed to frost flower sea salts is roughly half of previous observed surface longwave fluxes and cloud‐forcing estimates reported in Alaska, implying that the longwave enhancement due to frost flower salts may be comparable to those estimated for anthropogenic aerosol emissions. Since the potential frost flower area is parameterized as the maximum possible region on which frost flowers grow for the modeled atmospheric temperature and sea ice conditions and the model underestimates the number of accumulation‐mode particles from midlatitude anthropogenic sources transported in winter, the calculated aerosol indirect effect of frost flower sea salts in this work can be regarded an upper bound.