| 1. |
- Christiansen, Sigurd, et al.
(author)
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Influence of Arctic Microlayers and Algal Cultures on Sea Spray Hygroscopicity and the Possible Implications for Mixed-Phase Clouds
- 2020
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In: Journal of Geophysical Research: Atmospheres. - 2169-8996 .- 2169-897X. ; 125:19
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Journal article (peer-reviewed)abstract
- As Arctic sea ice cover diminishes, sea spray aerosols (SSA) have a larger potential to be emitted into the Arctic atmosphere. Emitted SSA can contain organic material, but how it affects the ability of particles to act as cloud condensation nuclei (CCN) is still not well understood. Here we measure the CCN-derived hygroscopicity of three different types of aerosol particles: (1) Sea salt aerosols made from artificial seawater, (2) aerosol generated from artificial seawater spiked with diatom species cultured in the laboratory, and (3) aerosols made from samples of sea surface microlayer (SML) collected during field campaigns in the North Atlantic and Arctic Ocean. Samples are aerosolized using a sea spray simulation tank (plunging jet) or an atomizer. We show that SSA containing diatom and microlayer exhibit similar CCN activity to inorganic sea salt with a κ value of ∼1.0. Large-eddy simulation (LES) is then used to evaluate the general role of aerosol hygroscopicity in governing mixed-phase low-level cloud properties in the high Arctic. For accumulation mode aerosol, the simulated mixed-phase cloud properties do not depend strongly on κ, unless the values are lower than 0.4. For Aitken mode aerosol, the hygroscopicity is more important; the particles can sustain the cloud if the hygroscopicity is equal to or higher than 0.4, but not otherwise. The experimental and model results combined suggest that the internal mixing of biogenic organic components in SSA does not have a substantial impact on the cloud droplet activation process and the cloud lifetime in Arctic mixed-phase clouds.
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| 2. |
- Frostenberg, Hannah, 1989, et al.
(author)
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The chance of freezing - a conceptional study to parameterize temperature-dependent freezing by including randomness of ice-nucleating particle concentrations
- 2023
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In: ATMOSPHERIC CHEMISTRY AND PHYSICS. - 1680-7316 .- 1680-7324. ; 23:19, s. 10883-10900
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Journal article (peer-reviewed)abstract
- Ice-nucleating particle concentrations (INPCs) can spread over several orders of magnitude at any given temperature. However, this variability is rarely accounted for in heterogeneous ice-nucleation parameterizations. In this paper, we present an approach to incorporate the random variation in the INPC into the parameterization of immersion freezing and analyze this novel concept with various sensitivity tests. In the new scheme, the INPC is drawn from a relative frequency distribution of cumulative INPCs. At each temperature, this distribution describing the INPCs is expressed as a lognormal frequency distribution. The new parameterization scheme does not require aerosol information from the driving model to represent the heterogeneity of INPCs. The scheme's performance is tested in a large-eddy simulation of a relatively warm Arctic mixed-phase stratocumulus. We find that it leads to reasonable ice masses in the cloud, especially when compared to immersion freezing schemes that yield one fixed INPC per temperature and lead to almost no ice production in the simulated cloud. The scheme is sensitive to the median of the frequency distribution and highly sensitive to the standard deviation of the distribution, as well as to the frequency of drawing a new INPC and the resolution of the model. Generally, a higher probability of drawing large INPCs leads to substantially more ice in the simulated cloud. We expose inherent challenges to introducing such a parameterization and explore possible solutions and potential developments.
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| 3. |
- Ickes, Luisa, 1986, et al.
(author)
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The ice-nucleating activity of Arctic sea surface microlayer samples and marine algal cultures
- 2020
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:18, s. 11089-11117
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Journal article (peer-reviewed)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 248K 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.
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| 4. |
- Porter, Grace C.E., et al.
(author)
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Highly Active Ice-Nucleating Particles at the Summer North Pole
- 2022
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In: Journal of Geophysical Research: Atmospheres. - 2169-8996 .- 2169-897X. ; 127:6
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Journal article (peer-reviewed)abstract
- The amount of ice versus supercooled water in clouds is important for their radiative properties and role in climate feedbacks. Hence, knowledge of the concentration of ice-nucleating particles (INPs) is needed. Generally, the concentrations of INPs are found to be very low in remote marine locations allowing cloud water to persist in a supercooled state. We had expected the concentrations of INPs at the North Pole to be very low given the distance from open ocean and terrestrial sources coupled with effective wet scavenging processes. Here we show that during summer 2018 (August and September) high concentrations of biological INPs (active at >−20°C) were sporadically present at the North Pole. In fact, INP concentrations were sometimes as high as those recorded at mid-latitude locations strongly impacted by highly active biological INPs, in strong contrast to the Southern Ocean. Furthermore, using a balloon borne sampler we demonstrated that INP concentrations were often different at the surface versus higher in the boundary layer where clouds form. Back trajectory analysis suggests strong sources of INPs near the Russian coast, possibly associated with wind-driven sea spray production, whereas the pack ice, open leads, and the marginal ice zone were not sources of highly active INPs. These findings suggest that primary ice production, and therefore Arctic climate, is sensitive to transport from locations such as the Russian coast that are already experiencing marked climate change.
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| 5. |
- Sotiropoulou, Georgia, et al.
(author)
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Ice multiplication from ice-ice collisions in the high Arctic: Sensitivity to ice habit, rimed fraction, ice type and uncertainties in the numerical description of the process
- 2021
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:12, s. 9741-9760
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Journal article (peer-reviewed)abstract
- Atmospheric models often fail to correctly reproduce the microphysical structure of Arctic mixed-phase clouds and underpredict ice water content even when the simulations are constrained by observed levels of ice nucleating particles. In this study we investigate whether ice multiplication from breakup upon ice-ice collisions, a process missing in most models, can account for the observed cloud ice in a stratocumulus cloud observed during the Arctic Summer Cloud Ocean Study (ASCOS) campaign. Our results indicate that the efficiency of this process in these conditions is weak; increases in fragment generation are compensated for by subsequent enhancement of precipitation and subcloud sublimation. Activation of collisional breakup improves the representation of cloud ice content, but cloud liquid remains overestimated. In most sensitivity simulations, variations in ice habit and prescribed rimed fraction have little effect on the results. A few simulations result in explosive multiplication and cloud dissipation; however, in most setups, the overall multiplication effects become substantially weaker if the precipitation sink is enhanced through cloud-ice-to-snow autoconversion. The largest uncertainty stems from the correction factor for ice enhancement due to sublimation included in the breakup parameterization; excluding this correction results in rapid glaciation, especially in simulations with plates. Our results indicate that the lack of a detailed treatment of ice habit and rimed fraction in most bulk microphysics schemes is not detrimental for the description of the collisional breakup process in the examined conditions as long as cloud-ice-to-snow autoconversion is considered.
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| 6. |
- Villanueva, Diego, et al.
(author)
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Constraining the Impact of Dust-Driven Droplet Freezing on Climate Using Cloud-Top-Phase Observations
- 2021
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In: Geophysical Research Letters. - 1944-8007 .- 0094-8276. ; 48:11
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Journal article (peer-reviewed)abstract
- Despite advances in our understanding of ice-nucleating particles, the effect of cloud glaciation on the Earth's radiation balance has remained poorly constrained. Particularly, dust ice nuclei are believed to enhance cloud glaciation in the Northern Hemisphere. We used satellite observations of the hemispheric and seasonal contrast in cloud top phase to assess the dust-driven droplet freezing in a climate model. The required freezing efficiency for dust ice nuclei suggests that climate models glaciate too few clouds through immersion droplet freezing. After tuning, the model leads to more realistic cloud-top-phase contrasts and a dust-driven glaciation effect of 0.14 ± 0.13 W m−2 between 30°N and 60°N. Observations of cloud-top-phase contrasts provide a strong constraint for ice formation in mixed-phase clouds and may provide a weak constraint for the associated impact on radiation and precipitation. Future studies should therefore consider both the mean-state cloud-phase partitioning and cloud-phase contrasts to achieve a more accurate simulation of dust-driven cloud glaciation.
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| 7. |
- Wagner, Robert, et al.
(author)
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Heterogeneous ice nucleation ability of aerosol particles generated from Arctic sea surface microlayer and surface seawater samples at cirrus temperatures
- 2021
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In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:18, s. 13903-13930
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Journal article (peer-reviewed)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 235K 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 x 10(10) m(-2) at an ice saturation ratio of 1.3. Much smaller densities in the range of 10(8)-10(9) 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.
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