Search

The amount of ice present in clouds can affect cloud lifetime, precipitation and radiative properties (1,2). The formation of ice in clouds is facilitated by the presence of airborne ice-nucleating particles (1,2). Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice (3-11). Sea-spray aerosol contains large amounts of organic material that is ejected into the atmosphere during bubble bursting at the organically enriched sea-air interface or sea surface microlayer (12-19). Here we show that organic material in the sea surface microlayer nucleates ice under conditions relevant for mixed-phase cloud and high-altitude ice cloud formation. The ice-nucleating material is probably biogenic and less than approximately 0.2 micrometres in size. We find that exudates separated from cells of the marine diatom Thalassiosira pseudonananucleate ice, and propose that organic material associated with phytoplankton cell exudates is a likely candidate for the observed ice-nucleating ability of the microlayer samples. Global model simulations of marine organic aerosol, in combination with our measurements, suggest that marine organic material maybe an important source of ice-nucleating particles in remote marine environments such as the Southern Ocean, North Pacific Ocean and North Atlantic Ocean., Atmospheric ice-nucleating particles (INPs) allow ice to nucleate heterogeneously at higher temperatures or lower relative humidity than is typical for homogeneous ice nucleation. Heterogeneous ice nucleation proceeds via different pathways [...]

Four correction models with differing forms were developed on a training dataset of 32 PurpleAir–Federal Equivalent Method (FEM) hourly fine particulate matter (PM 2.5) observation colocation sites across North America (NA). These were evaluated in comparison with four existing models from external sources using the data from 15 additional NA colocation sites. Colocation sites were determined automatically based on proximity and a novel quality control process. The Canadian Air Quality Health Index Plus (AQHI +) system was used to make comparisons across the range of concentrations common to NA, as well as to provide operational and health-related context to the evaluations. The model found to perform the best was our Model 2, PM2.5-corrected=PM2.5-cf-1/(1+0.24/(100/RH%-1)), where RH is limited to the range [30%,70%] , which is based on the RH growth model developed by Crilley et al. (2018). Corrected concentrations from this model in the moderate to high range, the range most impactful to human health, outperformed all other models in most comparisons. Model 7 (Barkjohn et al., 2021) was a close runner-up and excelled in the low-concentration range (most common to NA). The correction models do not perform the same at different locations, and thus we recommend testing several models at nearby colocation sites and utilizing that which performs best if possible. If no nearby colocation site is available, we recommend using our Model 2. This study provides a robust framework for the evaluation of low-cost PM 2.5 sensor correction models and presents an optimized correction model for North American PurpleAir (PA) sensors. [ABSTRACT FROM AUTHOR]

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 0.2µm, approximately 1 in 106 particles acted as an INP at -25°C, while at diameters of around 8µm, 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. [ABSTRACT FROM AUTHOR]

The nocturnal nitrogen oxides, which include the nitrate radical (NO3), dinitrogen pentoxide (N2O5), and its uptake product on chloride containing aerosol, nitryl chloride (ClNO2), can have profound impacts on the lifetime of NOx ( =  NO + NO2), radical budgets, and next-day photochemical ozone (O3) production, yet their abundances and chemistry are only sparsely constrained by ambient air measurements.Here, we present a measurement data set collected at a routine monitoring site near the Abbotsford International Airport (YXX) located approximately 30 km from the Pacific Ocean in the Lower Fraser Valley (LFV) on the west coast of British Columbia. Measurements were made from 20 July to 4 August 2012 and included mixing ratios of ClNO2, N2O5, NO, NO2, total odd nitrogen (NOy), O3, photolysis frequencies, and size distribution and composition of non-refractory submicron aerosol (PM1).At night, O3 was rapidly and often completely removed by dry deposition and by titration with NO of anthropogenic origin and unsaturated biogenic hydrocarbons in a shallow nocturnal inversion surface layer. The low nocturnal O3 mixing ratios and presence of strong chemical sinks for NO3 limited the extent of nocturnal nitrogen oxide chemistry at ground level. Consequently, mixing ratios of N2O5 and ClNO2 were low ( <  30 and  <  100 parts-per-trillion by volume (pptv) and median nocturnal peak values of 7.8 and 7.9 pptv, respectively). Mixing ratios of ClNO2 frequently peaked 1–2 h after sunrise rationalized by more efficient formation of ClNO2 in the nocturnal residual layer aloft than at the surface and the breakup of the nocturnal boundary layer structure in the morning. When quantifiable, production of ClNO2 from N2O5 was efficient and likely occurred predominantly on unquantified supermicron-sized or refractory sea-salt-derived aerosol. After sunrise, production of Cl radicals from photolysis of ClNO2 was negligible compared to production of OH from the reaction of O(1D) + H2O except for a short period after sunrise. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The nocturnal nitrogen oxides, which include the nitrate radical (NO3), dinitrogen pentoxide (N2O5), and its uptake product on chloride containing aerosol, nitryl chloride (ClNO2), can have profound impacts on the lifetime of NOx (= NO + NO2), radical budgets, and next-day photochemical ozone (O3) production, yet their abundances and chemistry are only sparsely constrained by ambient air measurements. Here, we present a measurement data set collected at a routine monitoring site near the Abbotsford International Airport (YXX) located approximately 30 km from the Pacific Ocean in the Lower Fraser Valley (LFV) on the West coast of British Columbia. Measurements were made from July 20 to August 4, 2012, and included mixing ratios of ClNO2, N2O5, NO, NO2, total odd nitrogen (NOy), O3, photolysis frequencies, and size distribution and composition of non-refractory submicron aerosol. At night, O3 was rapidly and often completely removed by dry deposition and by titration with NO of anthropogenic origin and unsaturated biogenic hydrocarbons in a shallow nocturnal inversion surface layer. The low nocturnal O3 mixing ratios and presence of strong chemical sinks for NO3 limited the extent of nocturnal nitrogen oxide chemistry at ground level. Consequently, mixing ratios of N2O5 and ClNO2 were low (< 30 and < 100 parts-per-trillion by volume (pptv) and median nocturnal peak values of 7.8 pptv and 7.9 pptv, respectively). Mixing ratios of ClNO2 frequently peaked 1-2 hours after sunrise rationalized by more efficient formation of ClNO2 in the nocturnal residual layer aloft than at the surface and the breakup of the nocturnal boundary layer structure in the morning. When quantifiable, production of ClNO2 from N2O5 was efficient and likely occurred predominantly on unquantified supermicron sized or refractory sea salt derived aerosol. After sunrise, production of Cl radicals from photolysis of ClNO2 was negligible compared to production of OH from the reaction of O(1D) + H2O except for a short period after sunrise. [ABSTRACT FROM AUTHOR]