Marine and coastal fog forms mainly from the cooling of warm and moist air advected over a colder sea surface. Atlantic Canada is one of the foggiest regions of the world due to the strong temperature contrast between the two oceanic currents in the vicinity. Recurring periods of low visibility notably disrupt off-shore operations and marine traffic, but also land and air transportation. On longer time-scales, marine fog variability also has a significant impact on the global radiative budget. Clouds, including fog, are the greatest source of uncertainty in the current climate projections because of their complex feedback mechanisms. Meteorological records indicate a significant negative trend in the occurrence of foggy conditions over the past six decades at most airports in Atlantic Canada, with large internal variability, including interannual and interdecadal variations. Using the airport observations, reanalysis data and climate model outputs, we investigated the various variabilities on the trend, at interannual and interdecadal scales, and attempted to address what caused these changes in fog frequency. Our results show that the strength and position of the North Atlantic Subtropical High as well as the sea-surface temperature of the cold and warm waters near Atlantic Canada were highly correlated with fog occurrence. We applied the derived fog indices on climate model outputs and projected the fog trends and variability in the different future climate scenarios. The results from this study will be compared with those obtained from other methods and the implications will be discussed.

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.

The physical and chemical properties of aerosol particles are important for the formation of cloud droplets and ice crystals. This is especially true for pristine regions such as the Arctic, where particle number concentrations are often very low. Observations from these regions are still sparse due to the technical challenges involved. Here, we present recent results of detailed in-situ observations of aerosols and clouds performed on board the Swedish icebreaker Oden over the central Arctic Ocean in 2018. We show that Aitken-mode particles, i.e. particles below 70 nm diameter, contribute significantly to cloud-forming particles (here termed cloud residuals), especially towards autumn with the start of the freeze-up of the sea ice. These cloud-forming Aitken-mode particles coincided with air that spent more time over the ice, while accumulation-mode dominated cloud residuals showed more of an oceanic influence, as shown using air back trajectory analysis. At the same time, the Aitken-mode dominated cloud residuals were associated with changes in the average chemical composition of the accumulation mode showing an increased organic contribution, in contrast to the accumulation-mode dominated cloud residuals, which showed an increased sulfate contribution. The Hoppel-minima in both whole-air and cloud residual size distributions was almost unchanged, suggesting only little addition of aerosol mass due to aqueous-phase cloud processing. Our highly detailed observations of aerosol-cloud interactions over the central Arctic Ocean close to the North Pole provide valuable insights into the properties and the origin of particles that are relevant for cloud formation in this remote region of our planet. This work is currently in review at the Journal of Geophysical Research (JGR).

Detailed knowledge of the physical and chemical properties and sources of particles that form clouds is especially important in pristine areas like the Arctic, where particle concentrations are often low and observations are sparse. Here, we present in situ cloud and aerosol measurements from the central Arctic Ocean in August–September 2018 combined with air parcel source analysis. We provide direct experimental evidence that Aitken mode particles (particles with diameters ≲70 nm) significantly contribute to cloud condensation nuclei (CCN) or cloud droplet residuals, especially after the freeze‐up of the sea ice in the transition toward fall. These Aitken mode particles were associated with air that spent more time over the pack ice, while size distributions dominated by accumulation mode particles (particles with diameters ≳70 nm) showed a stronger contribution of oceanic air and slightly different source regions. This was accompanied by changes in the average chemical composition of the accumulation mode aerosol with an increased relative contribution of organic material toward fall. Addition of aerosol mass due to aqueous‐phase chemistry during in‐cloud processing was probably small over the pack ice given the fact that we observed very similar particle size distributions in both the whole‐air and cloud droplet residual data. These aerosol–cloud interaction observations provide valuable insight into the origin and physical and chemical properties of CCN over the pristine central Arctic Ocean.

Fog has a wide range of impacts that can include transportation disruptions and climate effects. Despite being a common phenomenon, models struggle to incorporate fog microphysical properties which can affect the visibility, formation and dissipation of fog. Results are presented from a fog microphysics study conducted in June and July of 2016 near Halifax, on the eastern coast of Canada, where droplet and aerosol size distributions were measured, as well as fog droplet residuals using a ground-based counterflow virtual impactor. In the ten distinct events that were analyzed, fog never formed when the dew-point temperature was lower than the sea-surface temperature, suggesting that advection fog was primarily observed. During fog events, the concentration of particles larger than 500 nm in diameter was observed to decrease up to 90%, suggesting that nucleation scavenging was an important loss process during fog. Maximum droplet concentration was correlated (r = 0.61) to the total pre-fog aerosol concentration, despite a large (423 nm) estimated activation diameter. From our measurements, the peak supersaturation (SS) was estimated to range from 0.015-0.046%, including uncertainties due to chemical composition, which is lower than previous estimates for continental fog, including mountain sites, and would be consistent with advection fog as well as the presence of sea salt aerosol. Using basic assumptions, we estimate that for each added aerosol per cm(3) in the air mass, the maximum fog droplet concentration increases by 0.011 per cm(3) and the fog albedo increases by (0.55-3.8) x 10(-4). This in-situ dataset will help evaluate models to ultimately improve fog forecasts for coastal areas and further our understanding of aerosol-cloud interactions.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

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.

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.

Breaking waves produce bubble plumes that burst at the sea surface, injecting primary marine aerosol (PMA) highly enriched with marine organic carbon (OC) into the atmosphere. It is widely assumed that this OC is modern, produced by present-day biological activity, even though nearly all marine OC is thousands of years old, produced by biological activity long ago. We used natural abundance radiocarbon (14C) measurements to show that 19 to 40% of the OC associated with freshly produced PMA was refractory dissolved OC (RDOC). Globally, this process removes 2 to 20 Tg of RDOC from the oceans annually, comparable to other RDOC losses. This process represents a major removal pathway for old OC from the sea, with important implications for oceanic and atmospheric biogeochemistry, the global carbon cycle, and climate.

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 L air L sw ‐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.

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.