• European Marine Science
• Atmospheric Chemistry and Physics (... close

Abstract. Sea spray aerosol particles are a recognised type of ice-nucleating particles under mixed-phase cloud conditions. Entities that are responsible for the heterogeneous ice nucleation ability include intact or fragmented cells of marine microorganisms as well as organic matter released by cell exudation. Only a small fraction of sea spray aerosol is transported to the upper troposphere, but there are indications from mass-spectrometric analyses of the residuals of sublimated cirrus particles that sea salt could also contribute to heterogeneous ice nucleation under cirrus conditions. Experimental studies on the heterogeneous ice nucleation ability of sea spray aerosol particles and their proxies at temperatures below 235 K are still scarce. In our article, we summarise previous measurements and present a new set of ice nucleation experiments at cirrus temperatures with particles generated from sea surface microlayer and surface seawater samples collected in three different regions of the Arctic and from a laboratory-grown diatom culture (Skeletonema marinoi). The particles were suspended in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber and ice formation was induced by expansion cooling. We confirmed that under cirrus conditions, apart from the ice-nucleating entities mentioned above, also crystalline inorganic salt constituents can contribute to heterogeneous ice formation. This takes place at temperatures below 220 K, where we observed in all experiments a strong immersion freezing mode due to the only partially deliquesced inorganic salts. The inferred ice nucleation active surface site densities for this nucleation mode reached a maximum of about 5×1010 m−2 at an ice saturation ratio of 1.3. Much smaller densities in the range of 108–109 m−2 were observed at temperatures between 220 and 235 K, where the inorganic salts fully deliquesced and only the organic matter and/or algal cells and cell debris could contribute to heterogeneous ice formation. These values are 2 orders of magnitude smaller than those previously reported for particles generated from microlayer suspensions collected in temperate and subtropical zones. While this difference might simply underline the strong variability of the number of ice-nucleating entities in the sea surface microlayer across different geographical regions, we also discuss how instrumental parameters like the aerosolisation method and the ice nucleation measurement technique might affect the comparability of the results amongst different studies.

Abstract. This study investigates how variations in Arctic sea ice and sea surface conditions influence δ18O of present-day Arctic precipitation. This is done using the model isoCAM3, an isotope-equipped version of the National Center for Atmospheric Research Community Atmosphere Model version 3. Four sensitivity experiments and one control simulation are performed with prescribed sea surface temperature (SST) and sea ice. Each of the four experiments simulates the atmospheric and isotopic response to Arctic oceanic conditions for selected years after the beginning of the satellite era in 1979. Changes in sea ice extent and SSTs have different impacts in Greenland and the rest of the Arctic. The simulated changes in central Arctic sea ice do not influence δ18O of Greenland precipitation, only anomalies of Baffin Bay sea ice. However, this does not exclude the fact that simulations based on other sea ice and sea surface temperature distributions might yield changes in the δ18O of precipitation in Greenland. For the Arctic, δ18O of precipitation and water vapour is sensitive to local changes in sea ice and sea surface temperature and the changes in water vapour are surface based. Reduced sea ice extent yields more enriched isotope values, whereas increased sea ice extent yields more depleted isotope values. The distribution of the sea ice and sea surface conditions is found to be essential for the spatial distribution of the simulated changes in δ18O.

Abstract. During austral summer 2015, the Microphysics of Antarctic Clouds (MAC) field campaign collected unique and detailed airborne and ground-based in situ measurements of cloud and aerosol properties over coastal Antarctica and the Weddell Sea. This paper presents the first results from the experiment and discusses the key processes important in this region, which is critical to predicting future climate change. The sampling was predominantly of stratus clouds, at temperatures between −20 and 0 °C. These clouds were dominated by supercooled liquid water droplets, which had a median concentration of 113 cm−3 and an interquartile range of 86 cm−3. Both cloud liquid water content and effective radius increased closer to cloud top. The cloud droplet effective radius increased from 4 ± 2 µm near cloud base to 8 ± 3 µm near cloud top. Cloud ice particle concentrations were highly variable with the ice tending to occur in small, isolated patches. Below approximately 1000 m, glaciated cloud regions were more common at higher temperatures; however, the clouds were still predominantly liquid throughout. When ice was present at temperatures higher than −10 °C, secondary ice production most likely through the Hallett–Mossop mechanism led to ice concentrations 1 to 3 orders of magnitude higher than the number predicted by commonly used primary ice nucleation parameterisations. The drivers of the ice crystal variability are investigated. No clear dependence on the droplet size distribution was found. The source of first ice in the clouds remains uncertain but may include contributions from biogenic particles, blowing snow or other surface ice production mechanisms. The concentration of large aerosols (diameters 0.5 to 1.6 µm) decreased with altitude and were depleted in air masses that originated over the Antarctic continent compared to those more heavily influenced by the Southern Ocean and sea ice regions. The dominant aerosol in the region was hygroscopic in nature, with the hygroscopicity parameter κ having a median value for the campaign of 0.66 (interquartile range of 0.38). This is consistent with other remote marine locations that are dominated by sea salt/sulfate.

Ice nucleating particles (INPs) in the troposphere can form ice in clouds via heterogeneous ice nucleation. Yet, atmospheric number concentrations of INPs (NINP) are not well characterized and although there is some understanding of their sources, it is still unclear to what extend different sources contribute, nor if all sources are known. In this work, we examined properties of INPs at Cape Verde from different sources, the oceanic sea surface microlayer (SML) and underlying water (ULW), the atmosphere close to both sea and cloud level as well as cloud water. Both enrichment and depletion of NINP in SML compared to ULW were observed. The enrichment factor (EF) varied from roughly 0.4 to 11, and there was no clear trend in EF with temperature. NINP in PM10 sampled at Cape Verde Atmospheric Observatory (CVAO) at any particular temperature spanned around 1 order of magnitude below −15 °C, and about 2 orders of magnitude at warmer temperatures (>−12 °C). NINP in PM1 were generally lower than those in PM10 at CVAO. About 83 ± 22 %, 67 ± 18 % and 77 ± 14 % (median ± standard deviation) of INPs had a diameter > 1 µm at ice activation temperatures of −12, −15, and −18 °C, respectively. Among the 17 PM10 samples at CVAO, three PM10 filters showed elevated NINP at warm temperatures, e.g., above 0.01 std L−1 at −10 °C. However, for NINP in PM1 at CVAO, this is not the case. At these higher temperatures, often biological particles have been found to be ice active. Consequently, the difference in NINP between PM1 and PM10 at CVAO, suggests that biological ice active particles were present in the super-micron size range. NINP in PM10 at CVAO was found to be similar to that on Monte Verde (MV, at 744 m a.s.l.) during non-cloud events. During cloud events, most INPs on MV were activated to cloud droplets. When highly ice active particles were present in PM10 filters at CVAO, they were not observed in PM10 filters on MV, but in cloud water samples, instead. This is direct evidence that these INPs which are likely biological are activated to cloud droplets during cloud events. In general, Cape Verde was often affected by dust from the Saharan desert during our measurement. For the observed air masses, atmospheric NINP in air fit well to the concentrations observed in cloud water. When comparing concentrations of both sea salt and INPs in both seawater and PM10 filters, it can be concluded that sea spray aerosol (SSA) only contributed a minor fraction to the atmospheric NINP. Therefore it can be said that, unless there would be a significant enrichment of NINP during the formation of SSA particles, NINP was mainly dominated by mineral dust at cold temperatures with few contributions from possible biological particles at warmer temperatures.

Abstract. Ice-nucleating particles (INPs) in the troposphere can form ice in clouds via heterogeneous ice nucleation. Yet, atmospheric number concentrations of INPs ( NINP ) are not well characterized, and, although there is some understanding of their sources, it is still unclear to what extend different sources contribute or if all sources are known. In this work, we examined properties of INPs at Cabo Verde (a.k.a. Cape Verde) from different environmental compartments: the oceanic sea surface microlayer (SML), underlying water (ULW), cloud water and the atmosphere close to both sea level and cloud level. Both enrichment and depletion of NINP in SML compared to ULW were observed. The enrichment factor (EF) varied from roughly 0.4 to 11, and there was no clear trend in EF with ice-nucleation temperature. NINP values in PM 10 sampled at Cape Verde Atmospheric Observatory (CVAO) at any particular ice-nucleation temperature spanned around 1 order of magnitude below −15 ∘ C, and about 2 orders of magnitude at warmer temperatures ( > - 12 ∘ C). Among the 17 PM 10 samples at CVAO, three PM 10 filters showed elevated NINP at warm temperatures, e.g., above 0.01 L −1 at −10 ∘ C. After heating samples at 95 ∘ C for 1 h, the elevated NINP at the warm temperatures disappeared, indicating that these highly ice active INPs were most likely biological particles. INP number concentrations in PM 1 were generally lower than those in PM 10 at CVAO. About 83±22 %, 67±18 % and 77±14 % (median ± standard deviation) of INPs had a diameter >1 µ m at ice-nucleation temperatures of −12 , −15 and −18 ∘ C, respectively. PM 1 at CVAO did not show such elevated NINP at warm temperatures. Consequently, the difference in NINP between PM 1 and PM 10 at CVAO suggests that biological ice-active particles were present in the supermicron size range. NINP in PM 10 at CVAO was found to be similar to that on Monte Verde (MV, at 744 m a.s.l.) during noncloud events. During cloud events, most INPs on MV were activated to cloud droplets. When highly ice active particles were present in PM 10 filters at CVAO, they were not observed in PM 10 filters on MV but in cloud water samples instead. This is direct evidence that these INPs, which are likely biological, are activated to cloud droplets during cloud events. For the observed air masses, atmospheric NINP values in air fit well to the concentrations observed in cloud water. When comparing concentrations of both sea salt and INPs in both seawater and PM 10 filters, it can be concluded that sea spray aerosol (SSA) only contributed a minor fraction to the atmospheric NINP . This latter conclusion still holds when accounting for an enrichment of organic carbon in supermicron particles during sea spray generation as reported in literature.

Abstract. Growing evidence suggests that the sea ice surface is an important source of sea salt aerosol and this has significant implications for polar climate and atmospheric chemistry. It also suggests the potential to use ice core sea salt records as proxies for past sea ice extent. To explore this possibility in the Arctic region, we use a chemical transport model to track the emission, transport, and deposition of sea salt from both the open ocean and the sea ice, allowing us to assess the relative importance of each. Our results confirm the importance of sea ice sea salt (SISS) to the winter Arctic aerosol burden. For the first time, we explicitly simulate the sea salt concentrations of Greenland snow, achieving values within a factor of two of Greenland ice core records. Our simulations suggest that SISS contributes to the winter maxima in sea salt characteristic of ice cores across Greenland. However, a north–south gradient in the contribution of SISS relative to open-ocean sea salt (OOSS) exists across Greenland, with 50 % of winter sea salt being SISS at northern sites such as NEEM (77° N), while only 10 % of winter sea salt is SISS at southern locations such as ACT10C (66° N). Our model shows some skill at reproducing the inter-annual variability in sea salt concentrations for 1991–1999, particularly at Summit where up to 62 % of the variability is explained. Future work will involve constraining what is driving this inter-annual variability and operating the model under different palaeoclimatic conditions.

Abstract. In recent years, sea spray as well as the biological material it contains has received increased attention as a source of ice-nucleating particles (INPs). Such INPs may play a role in remote marine regions, where other sources of INPs are scarce or absent. In the Arctic, these INPs can influence water–ice partitioning in low-level clouds and thereby the cloud lifetime, with consequences for the surface energy budget, sea ice formation and melt, and climate. Marine aerosol is of a diverse nature, so identifying sources of INPs is challenging. One fraction of marine bioaerosol (phytoplankton and their exudates) has been a particular focus of marine INP research. In our study we attempt to address three main questions. Firstly, we compare the ice-nucleating ability of two common phytoplankton species with Arctic seawater microlayer samples using the same instrumentation to see if these phytoplankton species produce ice-nucleating material with sufficient activity to account for the ice nucleation observed in Arctic microlayer samples. We present the first measurements of the ice-nucleating ability of two predominant phytoplankton species: Melosira arctica, a common Arctic diatom species, and Skeletonema marinoi, a ubiquitous diatom species across oceans worldwide. To determine the potential effect of nutrient conditions and characteristics of the algal culture, such as the amount of organic carbon associated with algal cells, on the ice nucleation activity, Skeletonema marinoi was grown under different nutrient regimes. From comparison of the ice nucleation data of the algal cultures to those obtained from a range of sea surface microlayer (SML) samples obtained during three different field expeditions to the Arctic (ACCACIA, NETCARE, and ASCOS), we found that they were not as ice active as the investigated microlayer samples, although these diatoms do produce ice-nucleating material. Secondly, to improve our understanding of local Arctic marine sources as atmospheric INPs we applied two aerosolization techniques to analyse the ice-nucleating ability of aerosolized microlayer and algal samples. The aerosols were generated either by direct nebulization of the undiluted bulk solutions or by the addition of the samples to a sea spray simulation chamber filled with artificial seawater. The latter method generates aerosol particles using a plunging jet to mimic the process of oceanic wave breaking. We observed that the aerosols produced using this approach can be ice active, indicating that the ice-nucleating material in seawater can indeed transfer to the aerosol phase. Thirdly, we attempted to measure ice nucleation activity across the entire temperature range relevant for mixed-phase clouds using a suite of ice nucleation measurement techniques – an expansion cloud chamber, a continuous-flow diffusion chamber, and a cold stage. In order to compare the measurements made using the different instruments, we have normalized the data in relation to the mass of salt present in the nascent sea spray aerosol. At temperatures above 248 K some of the SML samples were very effective at nucleating ice, but there was substantial variability between the different samples. In contrast, there was much less variability between samples below 248 K. We discuss our results in the context of aerosol–cloud interactions in the Arctic with a focus on furthering our understanding of which INP types may be important in the Arctic atmosphere.

Abstract. The Arctic sea ice is the central and essential component of the Arctic climate system. The depletion and areal decline of the Arctic sea ice cover, observed since the 1970's, have accelerated after the millennium shift. While a relationship to global warming is evident and is underpinned statistically, the mechanisms connected to the sea ice reduction are to be explored in detail. Sea ice erodes both from the top and from the bottom. Atmosphere, sea ice and ocean processes interact in non-linear ways on various scales. Feedback mechanisms lead to an Arctic amplification of the global warming system. The amplification is both supported by the ice depletion and is at the same time accelerating the ice reduction. Knowledge of the mechanisms connected to the sea ice decline has grown during the 1990's and has deepened when the acceleration became clear in the early 2000's. Record summer sea ice extents in 2002, 2005, 2007 and 2012 provided additional information on the mechanisms. This article reviews recent progress in understanding of the sea ice decline. Processes are revisited from an atmospheric, ocean and sea ice perspective. There is strong evidence for decisive atmospheric changes being the major driver of sea ice change. Feedbacks due to reduced ice concentration, surface albedo and thickness allow for additional local atmosphere and ocean influences and self-supporting feedbacks. Large scale ocean influences on the Arctic Ocean hydrology and circulation are highly evident. Northward heat fluxes in the ocean are clearly impacting the ice margins, especially in the Atlantic sector of the Arctic. Only little indication exists for a direct decisive influence of the warming ocean on the overall sea ice cover, due to an isolating layer of cold and fresh water underneath the sea ice.