Abstract. Number concentrations of ice-nucleating particles (NINP) in the Arctic were derived from ground-based filter samples. Examined samples had been collected in Alert (Nunavut, northern Canadian archipelago on Ellesmere Island), Utqiaġvik, formerly known as Barrow (Alaska), Ny-Ålesund (Svalbard), and at the Villum Research Station (VRS; northern Greenland). For the former two stations, examined filters span a full yearly cycle. For VRS, 10 weekly samples, mostly from different months of one year, were included. Samples from Ny-Ålesund were collected during the months from March until September of one year. At all four stations, highest concentrations were found in the summer months from roughly June to September. For those stations with sufficient data coverage, an annual cycle can be seen. The spectra of NINP observed at the highest temperatures, i.e., those obtained for summer months, showed the presence of INPs that nucleate ice up to −5 ∘C. Although the nature of these highly ice-active INPs could not be determined in this study, it often has been described in the literature that ice activity observed at such high temperatures originates from the presence of ice-active material of biogenic origin. Spectra observed at the lowest temperatures, i.e., those derived for winter months, were on the lower end of the respective values from the literature on Arctic INPs or INPs from midlatitude continental sites, to which a comparison is presented herein. An analysis concerning the origin of INPs that were ice active at high temperatures was carried out using back trajectories and satellite information. Both terrestrial locations in the Arctic and the adjacent sea were found to be possible source areas for highly active INPs.

Isotopes pinpoint strong seasonal variations in black carbon sources with consistent patterns at sites around the Arctic.

Long‐term measurements of the light absorption coefficient (babs) obtained with a particle soot absorption photometer (PSAP), babs (PSAP), have been previously reported for Barrow, Alaska, and Ny‐Ålesund, Spitsbergen, in the Arctic. However, the effects on babs of other aerosol chemical species coexisting with black carbon (BC) have not been critically evaluated. Furthermore, different mass absorption cross section (MAC) values have been used to convert babs to BC mass concentration (MBC = babs/MAC). We used a continuous soot monitoring system (COSMOS), which uses a heated inlet to remove volatile aerosol compounds, to measure babs (babs (COSMOS)) at these sites during 2012–2015. Field measurements and laboratory experiments have suggested that babs (COSMOS) is affected by about 9% on average by sea‐salt aerosols. MBC values derived by COSMOS (MBC (COSMOS)) using a MAC value obtained by our previous studies agreed to within 9% with elemental carbon concentrations at Barrow measured over 11 months. babs (PSAP) was higher than babs (COSMOS), by 22% at Barrow (PM1) and by 43% at Ny‐Ålesund (PM10), presumably due to the contribution of volatile aerosol species to babs (PSAP). Using babs (COSMOS) as a reference, we derived MBC (PSAP) from babs (PSAP) measured since 1998. We also established the seasonal variations of MBC at these sites. Seasonally averaged MBC (PSAP) decreased at a rate of about 0.55 ± 0.30 ng m−3 yr−1. We also compared MBC (COSMOS) and scaled MBC (PSAP) values with previously reported data and evaluated the degree of inconsistency in the previous data.

Abstract. Loss of sea ice is opening the Arctic to increasing development involving oil and gas extraction and shipping. Given the significant impacts of absorbing aerosol and secondary aerosol precursors emitted within the rapidly warming Arctic region, it is necessary to characterize local anthropogenic aerosol sources and compare to natural conditions. From August to September 2015 in Utqiaġvik (Barrow), AK, the chemical composition of individual atmospheric particles was measured by computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (0.13-4 µm projected area diameter) and real-time single-particle mass spectrometry (0.2-1.5 µm vacuum aerodynamic diameter). During periods influenced by the Arctic Ocean (70 % of the study), our results show that fresh sea spray aerosol contributed ∼ 20 %, by number, of particles between 0.13 and 0.4 µm, 40-70 % between 0.4 and 1 µm, and 80-100 % between 1 and 4 µm particles. In contrast, for periods influenced by emissions from Prudhoe Bay (10 % of the study), the third largest oil field in North America, there was a strong influence from submicron (0.13-1 µm) combustion-derived particles (20-50 % organic carbon, by number; 5-10 % soot by number). While sea spray aerosol still comprised a large fraction of particles (90 % by number from 1 to 4 µm) detected under Prudhoe Bay influence, these particles were internally mixed with sulfate and nitrate indicative of aging processes during transport. In addition, the overall mode of the particle size number distribution shifted from 76 nm during Arctic Ocean influence to 27 nm during Prudhoe Bay influence, with particle concentrations increasing from 130 to 920 cm −3 due to transported particle emissions from the oil fields. The increased contributions of carbonaceous combustion products and partially aged sea spray aerosol should be considered in future Arctic atmospheric composition and climate simulations.

To quantify the contributions of fossil and biomass sources to the wintertime Arctic aerosol burden source apportionment is reported for elemental (EC) and organic carbon (OC) fractions of six PM10 samples collected during a wintertime (2012-2013) campaign in Barrow, AK. Radiocarbon apportionment of EC indicates that fossil sources contribute an average of 68 ± 9% (0.01-0.07 μg m(-3)) in midwinter decreasing to 49 ± 6% (0.02 μg m(-3)) in late winter. The mean contribution of fossil sources to OC for the campaign was stable at 38 ± 8% (0.04-0.32 μg m(-3)). Samples were also analyzed for organic tracers, including levoglucosan, for use in a chemical mass balance (CMB) source apportionment model. The CMB model was able to apportion 24-53% and 99% of the OC and EC burdens, respectively, during the campaign, with fossil OC contributions ranging from 25 to 74% (0.02-0.09 μg m(-3)) and fossil EC contributions ranging from 73 to 94% (0.03-0.07 μg m(-3)). Back trajectories identified two major wintertime source regions to Barrow: the Russian and North American Arctic. Atmospheric lifetimes of levoglucosan, ranging from 50 to 320 h, revealed variability in wintertime atmospheric processing of this biomass burning tracer. This study allows for unambiguous apportionment of EC to fossil fuel and biomass combustion sources and intercomparison with CMB modeling.

Marine aerosol plays a vital role in cloud-aerosol interactions during summer in the Arctic. The recent rise in temperature and decrease in sea ice extent have the potential to impact marine biogenic sources. Compounds like methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO 4 2−), oxidation products of dimethyl sulfide (DMS) emitted by marine primary producers, are likely to increase in concentration. Long-term studies are vital to understand these changes in marine sulfur aerosol and potential interactions with Arctic climate. Samples were collected over three summers at two coastal sites on the North Slope of Alaska (Utqiaġvik and Oliktok Point). MSA concentrations followed previously reported seasonal trends, with evidence of high marine primary productivity influencing both sites. When added to an additional data set collected at Utqiaġvik, an increase in MSA concentration of + 2.5% per year and an increase in nss-SO 4 2− of + 2.1% per year are observed for the summer season over the 20-year record (1998-2017). This study identifies ambient air temperature as a strong factor for MSA, likely related to a combination of interrelated factors including warmer sea surface temperature, reduced sea ice, and temperature-dependent chemical reactions. Analysis of individual particles at Oliktok Point, within the North Slope of Alaska oil fields, showed evidence of condensation of MSA onto anthropogenic particles, highlighting the connection between marine and oil field emissions and secondary organic aerosol. This study shows the continued importance of understanding MSA in the Arctic while highlighting the need for further research into its seasonal relationship with organic carbon. Plain Language Summary Particles in the Earth's atmosphere play an important role in affecting the planet's climate. Understanding the compounds that make up these aerosol particles is especially important in the Arctic where dramatic changes in temperature and sea ice extent are being observed. Aerosol resulting from biological activity in marine regions is expected to increase in concentration and therefore have greater effects on climate. Methanesulfonic acid is one such compound that can be utilized to understand the impact of marine aerosol sources. Aerosol samples were collected over three summers at two sites on the North Slope of Alaska: Utqiaġvik and Oliktok Point. The samples were analyzed for a wide range of compounds including methanesulfonic acid. The results were combined with 16 years of data from the National Oceanic and Atmospheric Administration. Concentrations of methanesulfonic acid are increasing at a rate of 2.5% per year. Methanesulfonic acid was strongly related to temperature at Oliktok Point, where most marine aerosol is from the Beaufort Sea. At Utqiaġvik, strong relationships were found between methanesulfonic acid and temperature during years when intense Arctic cyclones occurred.

Urban trees could represent important short- and long-term landscape sinks for elemental carbon (EC). Therefore, we quantified foliar EC accumulation by two widespread oak tree speciesQuercus stellata (post oak) and Quercus virginiana (live oak)as well as leaf litterfall EC flux to soil from April 2017 to March 2018 in the City of Denton, Texas, within the Dallas-Fort Worth metropolitan area. Post oak trees accumulated 1.9-fold more EC (299 ± 45 mg EC m–2 canopy yr–1) compared to live oak trees (160 ± 31 mg EC m–2 canopy yr–1). However, in the fall, these oak species converged in their EC accumulation rates, with ∼70% of annual accumulation occurring during fall and on leaf surfaces. The flux of EC to the ground via leaf litterfall mirrored leaf-fall patterns, with post oaks and live oaks delivering ∼60% of annual leaf litterfall EC in fall and early spring, respectively. We estimate that post oak and live oak trees in this urban ecosystem potentially accumulate 3.5 t EC yr–1, equivalent to ∼32% of annual vehicular EC emissions from the city. Thus, city trees are significant sinks for EC and represent potential avenues for climate and air quality mitigation in urban areas.

Long‐term data on organic aerosol concentration and optical properties are needed in the Arctic to improve characterization of radiative forcing by atmospheric aerosols. This study presents the seasonal trends (summer 2012 to summer 2013) of organic carbon (OC) and water‐soluble organic carbon (WSOC) along with optical properties of light‐absorbing OC from a yearlong sampling campaign in Utqiaġvik, AK. Ambient OC concentrations for the year range from 0.008 ± 0.002 μg m−3 to 0.95 ± 0.06 μg m−3 with peaks in late summer, early fall, and late winter. On average, WSOC accounted for 57 ± 11% of the total OC burden throughout the sampling campaign, which is consistent with previous WSOC values. In order to understand the potential radiative impacts of light‐absorbing OC, the light absorption properties of WSOC were determined. Seasonal averaging revealed that the highest average mass absorption efficiency value of 1.54 ± 0.75 m2 g−1 was in the fall, with an annual range of 0.70 ± 0.44 to 1.54 ± 0.75 m2 g−1. To quantify the contributions of fossil and contemporary carbon sources to OC, radiocarbon abundance measurements were performed. For OC, fossil contributions were the greatest for select samples in the fall at 61.4 ± 9.8%, with contemporary contributions dominating OC in the spring and summer (68.9 ± 9.8% and 64.8 ± 9.8%, respectively). Back trajectories identified five major source regions to Utqiaġvik throughout the year, with a marine influence from the Arctic Ocean potentially present in all seasons. All these results point to impact from primary and secondary sources of OC in the Arctic.