In the central Arctic Ocean the formation of clouds and their properties are sensitive to the availability of cloud condensation nuclei (CCN). The vapors responsible for new particle formation (NPF), potentially leading to CCN, have remained unidentified since the first aerosol measurements in 1991. Here, we report that all the observed NPF events from the Arctic Ocean 2018 expedition are driven by iodic acid with little contribution from sulfuric acid. Iodic acid largely explains the growth of ultrafine particles (UFP) in most events. The iodic acid concentration increases significantly from summer towards autumn, possibly linked to the ocean freeze-up and a seasonal rise in ozone. This leads to a one order of magnitude higher UFP concentration in autumn. Measurements of cloud residuals suggest that particles smaller than 30 nm in diameter can activate as CCN. Therefore, iodine NPF has the potential to influence cloud properties over the Arctic Ocean.
Surfactants account for minor fractions of total organic carbon in the ocean but can significantly influence the production of primary marine aerosol particles (PMA) at the sea surface via modulation of bubble surface tension. During September and October 2016, model PMA (mPMA) were produced from seawater by bursting bubbles at two biologically productive and two oligotrophic stations in the western North Atlantic Ocean. Total concentrations of surfactants extracted from mPMA and seawater were quantified and characterized via measurements of surface tension isotherms and critical micelle concentrations (CMCs). Surfactant CMCs in biologically productive seawater were lower than those in the oligotrophic seawater suggesting that surfactant mixtures in the two regions were chemically distinct. mPMA surfactants were enriched in all regions relative to those in the associated seawater. Surface tension isotherms indicate that mPMA surfactants were weaker than corresponding seawater surfactants. mPMA from biologically productive seawater contained higher concentrations of surfactants than those produced from oligotrophic seawater, supporting the hypothesis that seawater surfactant properties modulate mPMA surfactant concentrations. Diel variability in concentrations of seawater and mPMA surfactants in some regions is consistent with biological and/or photochemical processing. This work demonstrates direct links between surfactants in mPMA and those in the associated seawater.
Marine refractory dissolved organic carbon is emitted to the atmosphere in primary marine aerosol.
The Arctic is warming faster than any other environment on the planet (Manabe & Wetherald, 1975;Serreze & Barry, 2011). The accelerated warming-Arctic amplification-leads to other changes, such as sea ice decline, glacier melt, permafrost thaw, and changes in the composition of the biological communities in the Arctic Ocean (e.g., AMAP, 2015). Aerosol particles can affect Arctic climate directly, through interactions with radiation (e.g., AMAP, 2015), and indirectly, through interactions with clouds (Albrecht, 1989;Mauritsen et al., 2011;Twomey, 1977). Our limited understanding of the feedback mechanisms and local processes related to clouds and aerosol-cloud interactions in the Arctic contributes significantly to the uncertainty in projections of future Arctic climate (IPCC, 2013). The large differences between polar night and day in terms of, for example, radiation, sea ice, cloud type and phase (liquid, mixed-phase, or ice), and atmospheric circulation result in large seasonal variations not only in aerosol particle abundance and composition but also in their impact on clouds (e.g., Willis et al., 2018). These conditions make the Arctic environment particularly challenging to represent in large-scale climate models (e.g.,
Abstract. The interior of western Canada, up to and including the Arctic, has experienced rapid change in its climate, hydrology, cryosphere, and ecosystems, and this is expected to continue. Although there is general consensus that warming will occur in the future, many critical issues remain. In this first of two articles, attention is placed on atmospheric-related issues that range from large scales down to individual precipitation events. Each of these is considered in terms of expected change organized by season and utilizing mainly “business-as-usual” climate scenario information. Large-scale atmospheric circulations affecting this region are projected to shift differently in each season, with conditions that are conducive to the development of hydroclimate extremes in the domain becoming substantially more intense and frequent after the mid-century. When coupled with warming temperatures, changes in the large-scale atmospheric drivers lead to enhancements of numerous water-related and temperature-related extremes. These include winter snowstorms, freezing rain, drought, forest fires, as well as atmospheric forcing of spring floods, although not necessarily summer convection. Collective insights of these atmospheric findings are summarized in a consistent, connected physical framework.
During September–October 2016, a marine aerosol generator configured with forced‐air Venturis was deployed at two biologically productive and two oligotrophic regions of the western North Atlantic Ocean to investigate factors that modulate primary marine aerosol (PMA) production. The generator produced representative bubble size distributions with Hinze scales (0.32 to 0.95 mm radii) and void fractions (0.011 to 0.019 Lair Lsw‐1) that overlapped those of plumes produced in the surface ocean by breaking wind waves. Hinze scales and void fractions of bubble plumes varied among seawater hydrographic regions, whereas corresponding peaks and widths of bubble size distributions did not, suggesting that variability in seawater surfactants drove variability in plume dynamics. Peaks in size‐resolved number production efficiencies for model PMA (mPMA) emitted via bubble bursting in the generator were within a narrow range (0.059 to 0.069 μm geometric mean diameter) over wide ranges in subsurface bubble characteristics, suggesting that subsurface bubble size distributions were not the primary controlling factors as was suggested by previous work. Total mass production efficiencies for mPMA decreased with increasing air detrainment rates, supporting the hypothesis that surface bubble rafts attenuate mPMA mass production. Total mass and Na+ production efficiencies for mPMA from biologically productive seawater were significantly greater than those from oligotrophic seawater. Corresponding mPMA number distributions peaked at smaller sizes during daytime, suggesting that short‐lived surfactants of biological and/or photochemical origin modulated diel variability in marine aerosol production.
In this study, a series of fog events that occurred near Halifax, Canada, during 20 June to 31 July 2016 are investigated using the Weather Research and Forecasting Model Version 3.8.1 (WRF), in comparison with in situ and satellite remotely sensed observations from the Moderate Resolution Imaging Spectroradiometer. We evaluate five planetary boundary layer (PBL) schemes available in WRF. Results show that these five PBL schemes lead to overestimates in liquid water content, especially the nonlocal schemes, and that they are biased early, in terms of the predicting the onset of fog, and late, in terms of fog dissipation, although their spatial patterns of fog are in good agreement with those suggested by Moderate Resolution Imaging Spectroradiometer imagery. The Kunkel equation is used to calculate visibility, based on WRF modeling of liquid water content. Comparisons with observed visibility show that this methodology sometimes fails to predict fog dissipation. We present a modification of this formulation for visibility that shows improved agreement with observations and more accurate fog dissipation. Continued improvements in the PBL scheme and visibility parameterization are needed for more accurate fog prediction.
Predictions of cloud droplet activation in the late summertime (September) central Arctic Ocean are made using κ -Köhler theory with novel observations of the aerosol chemical composition from a high-resolution time-of-flight chemical ionization mass spectrometer with a filter inlet for gases and aerosols (FIGAERO-CIMS) and an aerosol mass spectrometer (AMS), deployed during the Arctic Ocean 2018 expedition onboard the Swedish icebreaker Oden . We find that the hygroscopicity parameter κ of the total aerosol is 0.39 ± 0.19 (mean ± std). The predicted activation diameter of ∼25 to 130 nm particles is overestimated by 5%, leading to an underestimation of the cloud condensation nuclei (CCN) number concentration by 4–8%. From this, we conclude that the aerosol in the High Arctic late summer is acidic and therefore highly cloud active, with a substantial CCN contribution from Aitken mode particles. Variability in the predicted activation diameter is addressed mainly as a result of uncertainties in the aerosol size distribution measurements. The organic κ was on average 0.13, close to the commonly assumed κ of 0.1, and therefore did not significantly influence the predictions. These conclusions are supported by laboratory experiments of the activation potential of seven organic compounds selected as representative of the measured aerosol.
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