Ambient concentrations of ice-forming particles measured during ship expeditions are collected and summarised with the aim of determining the spatial distribution and variability in ice nuclei in ...oceanic regions.
The presented data from literature and previously unpublished data from over 23 months of ship-based measurements stretch from the Arctic to the Southern Ocean and include a circumnavigation of Antarctica. In comparison to continental observations, ship-based measurements of ambient ice nuclei show 1 to 2 orders of magnitude lower mean concentrations. To quantify the geographical variability in oceanic areas, the concentration range of potential ice nuclei in different climate zones is analysed by meridionally dividing the expedition tracks into tropical, temperate and polar climate zones. We find that concentrations of ice nuclei in these meridional zones follow temperature spectra with similar slopes but vary in absolute concentration. Typically, the frequency with which specific concentrations of ice nuclei are observed at a certain temperature follows a log-normal distribution. A consequence of the log-normal distribution is that the mean concentration is higher than the most frequently measured concentration. Finally, the potential contribution of ship exhaust to the measured ice nuclei concentration on board research vessels is analysed as function of temperature. We find a sharp onset of the influence at approximately −36 ∘C but none at warmer temperatures that could bias ship-based measurements.
Abstract
The Arctic is warming faster than anywhere else on Earth, prompting glacial melt, permafrost thaw, and sea ice decline. These severe consequences induce feedbacks that contribute to ...amplified warming, affecting weather and climate globally. Aerosols and clouds play a critical role in regulating radiation reaching the Arctic surface. However, the magnitude of their effects is not adequately quantified, especially in the central Arctic where they impact the energy balance over the sea ice. Specifically, aerosols called ice nucleating particles (INPs) remain understudied yet are necessary for cloud ice production and subsequent changes in cloud lifetime, radiative effects, and precipitation. Here, we report observations of INPs in the central Arctic over a full year, spanning the entire sea ice growth and decline cycle. Further, these observations are size-resolved, affording valuable information on INP sources. Our results reveal a strong seasonality of INPs, with lower concentrations in the winter and spring controlled by transport from lower latitudes, to enhanced concentrations of INPs during the summer melt, likely from marine biological production in local open waters. This comprehensive characterization of INPs will ultimately help inform cloud parameterizations in models of all scales.
As the Arctic warms at twice the global rate, radiative feedbacks from clouds will lead to compounding impacts on the surface energy budget that affect both regional and global weather, and climate. ...In a future warmer world, the Arctic is projected to become cloudier. However, the formation and evolution of Arctic clouds remain highly uncertain in part due to a limited understanding of current and future sources of ice nucleating particles (INPs). In particular, the sources and abundance of biologically-derived INPs are poorly characterized, yet they may be pivotal for cloud ice formation, especially at temperatures in which Arctic mixed-phase clouds (AMPCs) persist (i.e. >−15 °C). Here, we show for the first time that permafrost is a remarkably rich source of biologically-derived INPs, both heat labile (probably proteinaceous) and other organic INPs of biomolecular origin (41%-100% and 99%-100% of the total INPs, respectively). INP concentrations in 1000 to 30 000 year old permafrost were comparable to the most active of other Arctic and midlatitude soil sources (up to 1010 INPs per gram of soil). Thawing of permafrost-which promotes metabolic activity in microbes-and subsequent mobilization of those soils directly into the atmosphere or into lakes, rivers, and the ocean, suggests the intriguing possibility that increasing emissions of INPs from this hitherto overlooked reservoir could be widespread, and, in time, greatly impact Arctic cloud cloud glaciation and radiative properties. This discovery is timely given the rapidly-thawing permafrost in Alaska and across Earth's high latitudes. Since permafrost covers 15% of Northern Hemisphere land, this novel and prevalent INP source may become central to predictions of aerosol-cloud-precipitation interactions in AMPCs.
With 18% of the total U.S. landmass devoted to croplands, farmland and farming activities are potentially major sources of biogenic particles to the atmosphere. Farms harbor large populations of ...microbes both in the soil and on plant surfaces which, if injected into the atmosphere, may serve as nuclei for clouds. In this study, we investigated two farms as potential sources of biological ice nuclei (IN): an organic farm in Colorado and a cornfield in Nebraska. We used a continuous‐flow diffusion chamber (CFDC) to obtain real‐time measurements of IN at these farm sites. Total aerosol particles were also collected at the sites, and their temperature‐dependent ice nucleating activity was determined using the drop freezing method. Quantitative polymerase chain reaction and DNA sequencing of 16S rDNA clone libraries were used to test aerosols and washings of local vegetation for abundance of theinagene in ice nucleation active bacteria (from the well‐known group within theγ‐Proteobacteria) and to identify airborne primary biological aerosol particles. The vegetation in each of these farms contained 6 × 105 to 2 × 107 ina genes per gram vegetation. In contrast to the vegetation, airborne ina gene concentrations at the organic farm were typically below detectable limits, demonstrating a disconnect between local vegetative sources and the air above them. However, for measurements made during combine harvesting at the Nebraska corn field, ina gene concentrations were 19 L−1, with maximum IN concentrations of 50 L−1 determined from the CFDC at −20°C and above water saturation. At both farms, there was also an apparent biological contribution to the IN population which did not contain the ina gene.
Key Points
IN concentrations were characterized over two agricultural regions
While the ina gene was abundant on the ground, few were found in the air
There was a biogenic contribution to the IN which did not contain the ina gene
Rapid Arctic climate warming, amplified relative to lower-latitude regions, has led to permafrost thaw and associated thermokarst processes. Recent work has shown permafrost is a rich source of ...ice-nucleating particles (INPs) that can initiate ice formation in supercooled liquid clouds. Since the phase of Arctic clouds strongly affects the surface energy budget, especially over ice-laden surfaces, characterizing INP sources in this region is critical. For the first time, we provide a large-scale survey of potential INP sources in tundra terrain where thermokarst processes are active and relate to INPs in the air. Permafrost, seasonally thawed active layer, ice wedge, vegetation, water, and aerosol samples were collected near Utqiaġvik, Alaska, in late summer and analyzed for their INP contents. Permafrost was confirmed as a rich source of INPs that was enhanced near the coast. Sensitivity to heating revealed differences in INPs from similar sources, such as the permafrost and active layer. Water, vegetation, and ice wedge INPs had the highest heat-labile percentage. The aerosol likely contained a mixture of known and unsurveyed INP types that were inferred as biological. Arctic water bodies were shown to be potential important links of sources to the atmosphere in thermokarst regions. Therefore, a positive relationship found with total organic carbon considering all water bodies gives a mechanism for future parameterization as permafrost continues to thaw and drive regional landscape shifts.
Microorganisms are ubiquitous and highly diverse in the atmosphere. Despite the potential impacts of airborne bacteria found in the lower atmosphere over the Southern Ocean (SO) on the ecology of ...Antarctica and on marine cloud phase, no previous region-wide assessment of bioaerosols over the SO has been reported. We conducted bacterial profiling of boundary layer shipboard aerosol samples obtained during an Austral summer research voyage, spanning 42.8 to 66.5°S. Contrary to findings over global subtropical regions and the Northern Hemisphere, where transport of microorganisms from continents often controls airborne communities, the great majority of the bacteria detected in our samples were marine, based on taxonomy, back trajectories, and source tracking analysis. Further, the beta diversity of airborne bacterial communities varied with latitude and temperature, but not with other meteorological variables. Limited meridional airborne transport restricts southward community dispersal, isolating Antarctica and inhibiting microorganism and nutrient deposition from lower latitudes to these same regions. A consequence and implication for this region’s marine boundary layer and the clouds that overtop it is that it is truly pristine, free from continental and anthropogenic influences, with the ocean as the dominant source controlling low-level concentrations of cloud condensation nuclei and ice nucleating particles.
A number of new measurement methods for ice nucleating particles (INPs) have been introduced in recent years, and it is important to address how these methods compare. Laboratory comparisons of ...instruments sampling major INP types are common, but few comparisons have occurred for ambient aerosol measurements exploring the utility, consistency and complementarity of different methods to cover the large dynamic range of INP concentrations that exists in the atmosphere. In this study, we assess the comparability of four offline immersion freezing measurement methods (Colorado State University ice spectrometer, IS; North Carolina State University cold stage, CS; National Institute for Polar Research Cryogenic Refrigerator Applied to Freezing Test, CRAFT; University of British Columbia micro-orifice uniform deposit impactor–droplet freezing technique, MOUDI-DFT) and an online method (continuous flow diffusion chamber, CFDC) used in a manner deemed to promote/maximize immersion freezing, for the detection of INPs in ambient aerosols at different locations and in different sampling scenarios. We also investigated the comparability of different aerosol collection methods used with offline immersion freezing instruments. Excellent agreement between all methods could be obtained for several cases of co-sampling with perfect temporal overlap. Even for sampling periods that were not fully equivalent, the deviations between atmospheric INP number concentrations measured with different methods were mostly less than 1 order of magnitude. In some cases, however, the deviations were larger and not explicable without sampling and measurement artifacts. Overall, the immersion freezing methods seem to effectively capture INPs that activate as single particles in the modestly supercooled temperature regime (> −20 °C), although more comparisons are needed in this temperature regime that is difficult to access with online methods. Relative to the CFDC method, three immersion freezing methods that disperse particles into a bulk liquid (IS, CS, CRAFT) exhibit a positive bias in measured INP number concentrations below −20 °C, increasing with decreasing temperature. This bias was present but much less pronounced for a method that condenses separate water droplets onto limited numbers of particles prior to cooling and freezing (MOUDI-DFT). Potential reasons for the observed differences are discussed, and further investigations proposed to elucidate the role of all factors involved.
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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