ALBERT

Description: Despite the potential importance of black carbon (BC) for radiative forcing of the Arctic atmosphere, vertically resolved measurements of the particle light scattering coefficient (σsp) and light absorption coefficient (σap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80∘ N. Here, relationships among vertically distributed aerosol optical properties (σap, σsp and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9 and 83.4∘ N from near the surface to 500 hPa. Airborne data collected during April 2015 are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the Goddard Earth Observing System (GEOS) model, GEOS-Chem, coupled with the TwO-Moment Aerosol Sectional (TOMAS) model (collectively GEOS-Chem–TOMAS; Kodros et al., 2018) to further our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for σsp less than 15 Mm−1, which represent 98 % of the observed σsp, because the single scattering albedo (SSA) has a tendency to be lower at lower σsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g−1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (13.6 and 9.1 m2 g−1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC, the presence of small amounts of dust and/or possible differences in BC microphysics and morphologies between the observations and model. In comparing the observations and simulations, we present σap and SSA, as measured, and σap∕2 and the corresponding SSA to encompass the lower modelled MAC that is more consistent with accepted MAC values. Median values of the measured σap, rBC and the organic component of particles all increase by a factor of 1.8±0.1, going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics and σap agree with the near-surface measurements but do not reproduce the higher values observed between 900 and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Model-observation discrepancies may be mostly due to the modelled ejection of biomass burning particles only into the boundary layer at the sources. For the assumption of the observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of σsp

Description: Atmospheric aerosol particles that can nucleate ice are referred to as ice-nucleating particles (INPs). Recent studies have confirmed that aerosol particles emitted by the oceans can act as INPs. This very relevant information can be included in climate and weather models to predict the formation of ice in clouds, given that most of them do not consider oceans as a source of INPs. Very few studies that sample INPs have been carried out in tropical latitudes, and there is a need to evaluate their availability to understand the potential role that marine aerosol may play in the hydrological cycle of tropical regions. This study presents results from the first measurements obtained during a field campaign conducted in the tropical village of Sisal, located on the coast of the Gulf of Mexico of the Yucatan Peninsula in Mexico in January–February 2017, and one of the few data sets currently available at such latitudes (i.e., 21∘ N). Aerosol particles sampled in Sisal are shown to be very efficient INPs in the immersion freezing mode, with onset freezing temperatures in some cases as high as −3 ∘C, similarly to the onset temperature from Pseudomonas syringae. The results show that the INP concentration in Sisal was higher than at other locations sampled with the same type of INP counter. Air masses arriving in Sisal after the passage of cold fronts have surprisingly higher INP concentrations than the campaign average, despite their lower total aerosol concentration. The high concentrations of INPs at warmer ice nucleation temperatures (T〉-15 ∘C) and the supermicron size of the INPs suggest that biological particles may have been a significant contributor to the INP population in Sisal during this study. However, our observations also suggest that at temperatures ranging between −20 and −30 ∘C mineral dust particles are the likely source of the measured INPs.

Description: Despite the importance of ice-nucleating particles (INPs) for climate and precipitation, our understanding of these particles is far from complete. Here, we investigated INPs at three coastal marine sites in Canada, two at mid-latitude (Amphitrite Point and Labrador Sea) and one in the Arctic (Lancaster Sound). For Amphitrite Point, 23 sets of samples were analyzed, and for Labrador Sea and Lancaster Sound, one set of samples was analyzed for each location. At all three sites, the ice-nucleating ability on a per number basis (expressed as the fraction of aerosol particles acting as an INP) was strongly dependent on the particle size. For example, at diameters of around 0.2 µm, approximately 1 in 106 particles acted as an INP at −25 ∘C, while at diameters of around 8 µm, approximately 1 in 10 particles acted as an INP at −25 ∘C. The ice-nucleating ability on a per surface-area basis (expressed as the surface active site density, ns) was also dependent on the particle size, with larger particles being more efficient at nucleating ice. The ns values of supermicron particles at Amphitrite Point and Labrador Sea were larger than previously measured ns values of sea spray aerosols, suggesting that sea spray aerosols were not a major contributor to the supermicron INP population at these two sites. Consistent with this observation, a global model of INP concentrations under-predicted the INP concentrations when assuming only marine organics as INPs. On the other hand, assuming only K-feldspar as INPs, the same model was able to reproduce the measurements at a freezing temperature of −25 ∘C, but under-predicted INP concentrations at −15 ∘C, suggesting that the model is missing a source of INPs active at a freezing temperature of −15 ∘C.

Description: Motivated by the need to predict how the Arctic atmosphere will change in a warming world, this article summarizes recent advances made by the research consortium NETCARE (Network on Climate and Aerosols: Addressing Key Uncertainties in Remote Canadian Environments) that contribute to our fundamental understanding of Arctic aerosol particles as they relate to climate forcing. The overall goal of NETCARE research has been to use an interdisciplinary approach encompassing extensive field observations and a range of chemical transport, earth system, and biogeochemical models. Several major findings and advances have emerged from NETCARE since its formation in 2013. (1) Unexpectedly high summertime dimethyl sulfide (DMS) levels were identified in ocean water (up to 75 nM) and the overlying atmosphere (up to 1 ppbv) in the Canadian Arctic Archipelago (CAA). Furthermore, melt ponds, which are widely prevalent, were identified as an important DMS source (with DMS concentrations of up to 6 nM and a potential contribution to atmospheric DMS of 20 % in the study area). (2) Evidence of widespread particle nucleation and growth in the marine boundary layer was found in the CAA in the summertime, with these events observed on 41 % of days in a 2016 cruise. As well, at Alert, Nunavut, particles that are newly formed and grown under conditions of minimal anthropogenic influence during the months of July and August are estimated to contribute 20 % to 80 % of the 30–50 nm particle number density. DMS-oxidation-driven nucleation is facilitated by the presence of atmospheric ammonia arising from seabird-colony emissions, and potentially also from coastal regions, tundra, and biomass burning. Via accumulation of secondary organic aerosol (SOA), a significant fraction of the new particles grow to sizes that are active in cloud droplet formation. Although the gaseous precursors to Arctic marine SOA remain poorly defined, the measured levels of common continental SOA precursors (isoprene and monoterpenes) were low, whereas elevated mixing ratios of oxygenated volatile organic compounds (OVOCs) were inferred to arise via processes involving the sea surface microlayer. (3) The variability in the vertical distribution of black carbon (BC) under both springtime Arctic haze and more pristine summertime aerosol conditions was observed. Measured particle size distributions and mixing states were used to constrain, for the first time, calculations of aerosol–climate interactions under Arctic conditions. Aircraft- and ground-based measurements were used to better establish the BC source regions that supply the Arctic via long-range transport mechanisms, with evidence for a dominant springtime contribution from eastern and southern Asia to the middle troposphere, and a major contribution from northern Asia to the surface. (4) Measurements of ice nucleating particles (INPs) in the Arctic indicate that a major source of these particles is mineral dust, likely derived from local sources in the summer and long-range transport in the spring. In addition, INPs are abundant in the sea surface microlayer in the Arctic, and possibly play a role in ice nucleation in the atmosphere when mineral dust concentrations are low. (5) Amongst multiple aerosol components, BC was observed to have the smallest effective deposition velocities to high Arctic snow (0.03 cm s−1).

Description: Modelling studies suggest that the climate and the hydrological cycle are sensitive to the concentrations of ice-nucleating particles (INPs). However, the concentrations, composition, and sources of INPs in the atmosphere remain uncertain. Here, we report daily concentrations of INPs in the immersion freezing mode and tracers of mineral dust (Al, Fe, Ti, and Mn), sea spray aerosol (Na+ and Cl−), and anthropogenic aerosol (Zn, Pb, NO3-, NH4+, and non-sea-salt SO42-) at Alert, Canada, during a 3-week campaign in March 2016. In total, 16 daily measurements of INPs are reported. The average INP concentrations measured in the immersion freezing mode were 0.005±0.002, 0.020±0.004, and 0.186±0.040 L−1 at −15, −20, and −25 ∘C, respectively. These concentrations are within the range of concentrations measured previously in the Arctic at ground level or sea level. Mineral dust tracers all correlated with INPs at −25 ∘C (correlation coefficient, R, ranged from 0.70 to 0.76), suggesting that mineral dust was a major contributor to the INP population at −25 ∘C. Particle dispersion modelling suggests that the source of the mineral dust may have been long-range transport from the Gobi Desert. Sea spray tracers were anti-correlated with INPs at −25 ∘C (R=-0.56). In addition, INP concentrations at −25 ∘C divided by mass concentrations of aluminum were anti-correlated with sea spray tracers (R=-0.51 and −0.55 for Na+ and Cl−, respectively), suggesting that the components of sea spray aerosol suppressed the ice-nucleating ability of mineral dust in the immersion freezing mode. Correlations between INPs and anthropogenic aerosol tracers were not statistically significant. These results will improve our understanding of INPs in the Arctic during spring.

Description: Ice nucleating particles (INPs) in the Arctic can influence climate and precipitation in the region; yet our understanding of the concentrations and sources of INPs in this region remain uncertain. In the following, we (1) measured concentrations of INPs in the immersion mode in the Canadian Arctic marine boundary layer during summer 2014 on board the CCGS Amundsen, (2) determined ratios of surface areas of mineral dust aerosol to sea spray aerosol, and (3) investigated the source region of the INPs using particle dispersion modelling. Average concentrations of INPs at −15, −20, and −25 ∘C were 0.005, 0.044, and 0.154 L−1, respectively. These concentrations fall within the range of INP concentrations measured in other marine environments. For the samples investigated the ratio of mineral dust surface area to sea spray surface area ranged from 0.03 to 0.09. Based on these ratios and the ice active surface site densities of mineral dust and sea spray aerosol determined in previous laboratory studies, our results suggest that mineral dust is a more important contributor to the INP population than sea spray aerosol for the samples analysed. Based on particle dispersion modelling, the highest concentrations of INPs were often associated with lower-latitude source regions such as the Hudson Bay area, eastern Greenland, or north-western continental Canada. On the other hand, the lowest concentrations were often associated with regions further north of the sampling sites and over Baffin Bay. A weak correlation was observed between INP concentrations and the time the air mass spent over bare land, and a weak negative correlation was observed between INP concentrations and the time the air mass spent over ice and open water. These combined results suggest that mineral dust from local sources is an important contributor to the INP population in the Canadian Arctic marine boundary layer during summer 2014.

Description: Despite the potential importance of black carbon (BC) to radiative forcing of the Arctic atmosphere, vertically-resolved measurements of the particle light scattering coefficient (Bsp) and light absorption coefficient (Bap) in the springtime Arctic atmosphere are infrequent, especially measurements at latitudes at or above 80oN. Here, relationships among vertically-distributed aerosol optical properties Bap, Bsp, and single scattering albedo or SSA), particle microphysics and particle chemistry are examined for a region of the Canadian archipelago between 79.9oN and 83.4oN from near the surface to 500 hPa. Airborne data collected during April, 2015, are combined with ground-based observations from the observatory at Alert, Nunavut and simulations from the GEOS-Chem-TOMAS model (Kodros et al., 2018) to increase our knowledge of the effects of BC on light absorption in the Arctic troposphere. The results are constrained for Bsp less than 15 Mm-1, which represent 98% of the observed Bsp, because the single scattering albedo (SSA) has a tendency to be lower at lower Bsp, resulting in a larger relative contribution to Arctic warming. At 18.4 m2 g-1, the average BC mass absorption coefficient (MAC) from the combined airborne and Alert observations is substantially higher than the two averaged modelled MAC values (9.5 m2 g-1 and 7.0 m2 g-1) for two different internal mixing assumptions, the latter of which is based on previous observations. The higher observed MAC value may be explained by an underestimation of BC and possible differences in BC microphysics and morphologies between the observations and model. We present Bap and SSA based on the assumption that Bap is overestimated in the observations in addition to the assumption that the higher MAC is explained. Median values of the measured Bap, rBC and organic component of particles all increase by a factor of 1.8±0.1 going from near-surface to 750 hPa, and values higher than the surface persist to 600 hPa. Modelled BC, organics, and Bap agree with the near-surface measurements, but do not reproduce the higher values observed between 900 hPa and 600 hPa. The differences between modelled and observed optical properties follow the same trend as the differences between the modelled and observed concentrations of the carbonaceous components (black and organic). Some discrepancies in the model may be due to the use of a relatively low imaginary refractive index of BC as well as by the ejection of biomass burning particles only into the boundary layer at sources. For the assumption of the higher observed MAC value, the SSA range between 0.88 and 0.94, which is significantly lower than other recent estimates for the Arctic, in part reflecting the constraint of Bsp 〈15 Mm-1. The large uncertainties in measuring optical properties and BC as well as the large differences between measured and modelled values, here and in the literature, argue for improved measurements of BC and light absorption by BC as well as more vertical profiles of aerosol chemistry, microphysics, and other optical properties in the Arctic.

Description: Despite the importance of ice-nucleating particles (INPs) for climate and precipitation, our understanding of these particles is far from complete. Here, we investigated INPs at three coastal marine sites in Canada, two at mid-latitude (Amphitrite Point and Labrador Sea), and one in the Arctic (Lancaster Sound). At all three sites, the ice-nucleating efficiency on a per number basis (expressed as the fraction of aerosol particles acting as an INP) was strongly dependent on the size. For example, at diameters of around 0.2 µm, approximately 1 in 106 particles acted as an INP at −25 ºC, while at diameters of around 8 µm, approximately 1 in 10 particles acted as an INP at −25 ºC. The ice-nucleating efficiency on a per surface area basis (expressed as the surface active site density, ns) was also dependent on the size, with larger particles being more efficient at nucleating ice. The ns values of supermicron particles at Amphitrite Point and Labrador Sea were larger than previously measured ns values of sea spray aerosol, suggesting that sea spray aerosol was not a major contributor to the supermicron INP population at these two sites. Consistent with this observation, a global model of INP concentrations under-predicted the INP concentrations when assuming only marine organics as INPs. On the other hand, assuming only K-feldspar as INPs, the same model was able to reproduce the measurements at a freezing temperature of −25 ºC, but under-predicted INP concentrations at −15 ºC, suggesting that the model is missing a source of INPs active at a freezing temperature of −15 ºC.

Description: Ice nucleating particles (INPs) in the Arctic can influence climate and precipitation in the region; yet our understanding of the concentrations and sources of INPs in this region remain uncertain. In the following we (1) measured concentrations of INPs in the Canadian Arctic marine boundary layer during summer 2014 on board the CCGS Amundsen, (2) determined ratios of surface areas of mineral dust aerosol to sea spray aerosol, and (3) investigated the source region of the INPs using particle dispersion modelling. Average concentrations of INPs at −15, −20 and −25°C were 0.005, 0.044, and 0.154L−1, respectively. These concentrations fall within the range of INP concentrations measured in other marine environments. For the samples investigated the ratio of mineral dust surface area to sea spray surface area ranged from 0.03 to 0.09. Based on these ratios and the ice active surface site densities of mineral dust and sea spray aerosol determined in previous laboratory studies, our results suggest that mineral dust is a more important contributor to the INP population than sea spray aerosol for the samples analysed. Based on particle dispersion modelling, the highest concentrations of INPs were often associated with lower latitude source regions such as the Hudson Bay area, eastern Greenland, or northwestern continental Canada. On the other hand, the lowest concentrations were often associated with regions further north of the sampling sites and over Baffin Bay. A weak correlation was observed between INP concentrations and the time the air mass spent over bare land, and a weak negative correlation was observed between INP concentrations and the time the air mass spent over ice and open water. These combined results suggest that mineral dust from local sources is an important contributor to the INP population in the Canadian Arctic marine boundary layer during summer 2014.

Description: Modelling studies suggest that the climate and the hydrological cycle are sensitive to the concentrations of ice-nucleating particles (INPs). However, the concentrations, composition, and sources of INPs in the atmosphere remain uncertain. Here we report daily concentrations of INPs and tracers of mineral dust (Al, Fe, Ti, and Mn), sea spray aerosol (Na+ and Cl−), and anthropogenic aerosol (Zn, Pb, NO3−, NH4+, and non-sea-salt SO42−) at Alert, Canada during a three-week campaign in March 2016. The average INP concentrations measured in the immersion freezing mode were approximately 0.005±0.002L−1, 0.020±0.004L−1, and 0.186±0.040L−1 at −15ºC, −20ºC, and −25ºC, respectively. These concentrations are within the range of concentrations measured previously in the Arctic at ground level or sea level. Mineral dust tracers all correlated with INPs at −25ºC (correlation coefficient, R, ranged from 0.70 to 0.76), suggesting that mineral dust was a major contributor to the INP population. Particle dispersion modelling suggests that the source of the mineral dust may have been the long-range transported dust from the Gobi desert. Sea spray tracers were anti-correlated with INPs at −25ºC (R=−0.56). In addition, INP concentrations at −25ºC divided by mass concentrations of aluminum were anti-correlated with sea spray tracers (R=−0.51 and −0.55 for Na+ and Cl−, respectively), suggesting that the components of sea spray aerosol suppressed the ice-nucleating ability of mineral dust in the immersion freezing mode. Correlations between INPs and anthropogenic aerosol tracers were not statistically significant. These results will improve our understanding of INPs in the Arctic during spring.