Abstract. The summer of 2015 was an extreme forest fire year in the Pacific Northwest. Our sample site at the Mt. Bachelor Observatory (MBO, 2.7 km a.s.l.) in central Oregon observed biomass burning (BB) events more than 50 % of the time during August. In this paper we characterize the aerosol physical and optical properties of 19 aged BB events during August 2015. Six of the 19 events were influenced by Siberian fires originating near Lake Baikal that were transported to MBO over 4–10 days. The remainder of the events resulted from wildfires in Northern California and Southwestern Oregon with transport times to MBO ranging from 3 to 35 h. Fine particulate matter (PM1), carbon monoxide (CO), aerosol light scattering coefficients (σscat), aerosol light absorption coefficients (σabs), and aerosol number size distributions were measured throughout the campaign. We found that the Siberian events had a significantly higher Δσabs∕ΔCO enhancement ratio, higher mass absorption efficiency (MAE; Δσabs∕ΔPM1), lower single scattering albedo (ω), and lower absorption Ångström exponent (AAE) when compared with the regional events. We suggest that the observed Siberian events represent that portion of the plume that has hotter flaming fire conditions and thus enabled strong pyroconvective lofting and long-range transport to MBO. The Siberian events observed at MBO therefore represent a selected portion of the original plume that would then have preferentially higher black carbon emissions and thus an enhancement in absorption. The lower AAE values in the Siberian events compared to regional events indicate a lack of brown carbon (BrC) production by the Siberian fires or a loss of BrC during transport. We found that mass scattering efficiencies (MSE) for the BB events ranged from 2.50 to 4.76 m2 g−1. We measured aerosol size distributions with a scanning mobility particle sizer (SMPS). Number size distributions ranged from unimodal to bimodal and had geometric mean diameters (Dpm) ranging from 138 to 229 nm and geometric standard deviations (σg) ranging from 1.53 to 1.89. We found MSEs for BB events to be positively correlated with the geometric mean of the aerosol size distributions (R2 = 0.73), which agrees with Mie theory. We did not find any dependence on event size distribution to transport time or fire source location.

Abstract. Biomass-burning aerosols have a significant effect on global and regional aerosol climate forcings. To model the magnitude of these effects accurately requires knowledge of the size distribution of the emitted and evolving aerosol particles. Current biomass-burning inventories do not include size distributions, and global and regional models generally assume a fixed size distribution from all biomass-burning emissions. However, biomass-burning size distributions evolve in the plume due to coagulation and net organic aerosol (OA) evaporation or formation, and the plume processes occur on spacial scales smaller than global/regional-model grid boxes. The extent of this size-distribution evolution is dependent on a variety of factors relating to the emission source and atmospheric conditions. Therefore, accurately accounting for biomass-burning aerosol size in global models requires an effective aerosol size distribution that accounts for this sub-grid evolution and can be derived from available emission-inventory and meteorological parameters. In this paper, we perform a detailed investigation of the effects of coagulation on the aerosol size distribution in biomass-burning plumes. We compare the effect of coagulation to that of OA evaporation and formation. We develop coagulation-only parameterizations for effective biomass-burning size distributions using the SAM-TOMAS large-eddy simulation plume model. For the most-sophisticated parameterization, we use the Gaussian Emulation Machine for Sensitivity Analysis (GEM-SA) to build a parameterization of the aged size distribution based on the SAM-TOMAS output and seven inputs: emission median dry diameter, emission distribution modal width, mass emissions flux, fire area, mean boundary-layer wind speed, plume mixing depth, and time/distance since emission. This parameterization was tested against an independent set of SAM-TOMAS simulations and yields R2 values of 0.83 and 0.89 for Dpm and modal width, respectively. The size distribution is particularly sensitive to the mass emissions flux, fire area, wind speed, and time, and we provide simplified fits of the aged size distribution to just these input variables. The simplified fits were tested against 11 aged biomass-burning size distributions observed at the Mt. Bachelor Observatory in August 2015. The simple fits captured over half of the variability in observed Dpm and modal width even though the freshly emitted Dpm and modal widths were unknown. These fits may be used in global and regional aerosol models. Finally, we show that coagulation generally leads to greater changes in the particle size distribution than OA evaporation/formation does, using estimates of OA production/loss from the literature.

Abstract. Even though the Arctic is remote, aerosol properties observed there are strongly influenced by anthropogenic emissions from outside the Arctic. This is particularly true for the so-called Arctic haze season (January through April). In summer (June through September), when atmospheric transport patterns change, and precipitation is more frequent, local Arctic sources, i.e., natural sources of aerosols and precursors, play an important role. Over the last few decades, significant reductions in anthropogenic emissions have taken place. At the same time a large body of literature shows evidence that the Arctic is undergoing fundamental environmental changes due to climate forcing, leading to enhanced emissions by natural processes that may impact aerosol properties. In this study, we analyze 9 aerosol chemical species and 4 particle optical properties from 10 Arctic observatories (Alert, Kevo, Pallas, Summit, Thule, Tiksi, Barrow/Utqiaġvik, Villum, and Gruvebadet and Zeppelin Observatory – both at Ny-Ålesund Research Station) to understand changes in anthropogenic and natural aerosol contributions. Variables include equivalent black carbon, particulate sulfate, nitrate, ammonium, methanesulfonic acid, sodium, iron, calcium and potassium, as well as scattering and absorption coefficients, single scattering albedo and scattering Ångström exponent. First, annual cycles are investigated, which despite anthropogenic emission reductions still show the Arctic haze phenomenon. Second, long-term trends are studied using the Mann–Kendall Theil–Sen slope method. We find in total 41 significant trends over full station records, i.e., spanning more than a decade, compared to 26 significant decadal trends. The majority of significantly declining trends is from anthropogenic tracers and occurred during the haze period, driven by emission changes between 1990 and 2000. For the summer period, no uniform picture of trends has emerged. Twenty-six percent of trends, i.e., 19 out of 73, are significant, and of those 5 are positive and 14 are negative. Negative trends include not only anthropogenic tracers such as equivalent black carbon at Kevo, but also natural indicators such as methanesulfonic acid and non-sea-salt calcium at Alert. Positive trends are observed for sulfate at Gruvebadet. No clear evidence of a significant change in the natural aerosol contribution can be observed yet. However, testing the sensitivity of the Mann–Kendall Theil–Sen method, we find that monotonic changes of around 5 % yr−1 in an aerosol property are needed to detect a significant trend within one decade. This highlights that long-term efforts well beyond a decade are needed to capture smaller changes. It is particularly important to understand the ongoing natural changes in the Arctic, where interannual variability can be high, such as with forest fire emissions and their influence on the aerosol population. To investigate the climate-change-induced influence on the aerosol population and the resulting climate feedback, long-term observations of tracers more specific to natural sources are needed, as well as of particle microphysical properties such as size distributions, which can be used to identify changes in particle populations which are not well captured by mass-oriented methods such as bulk chemical composition.

Concentrations of atmospheric black carbon, [BC], were determined from filter samples collected weekly at Kevo, Finland (69°45′N, 27°02′E), from 1964 to 2010 using optical and thermal optical methods. The data provide the longest record of directly measured [BC] 1976-1977, 1985-1987, and 1999. During such periods, nickel concentrations were well correlated with [BC]. This suggests that emissions from extensive ore smelting on the Kola Peninsula were significant contributors of particulate matter observed at Kevo. Simulations of [BC] at Kevo using the OsloCTM3 model using different emission inventories and meteorological data sets were performed. Modeled concentrations were lower than observed by a factor of 4. The results indicated that circulation changes can explain year to year variability, but the downward trend in the observations is mostly explained by emissions. Emission inventories in Europe, Russia, and the former Soviet Union are poorly constrained and appear to need revision in order to match observed trends in BC atmospheric concentrations.

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Forty‐seven years of week‐long total suspended particle samples from Kevo Finland were analyzed for methane sulfonic acid (MSA) and sulfate. Kevo is located 350 km north of the Arctic Circle. MSA and non‐sea‐salt sulfate (NSS‐SO4) showed clear seasonal trends. MSA peaks from May to July, coinciding with warmer waters and increased biogenic activity in the surrounding seas. NSS‐SO4 peaks in March with a minimum during the summer, the typical pattern for Arctic haze. MSA concentrations were found to be positively correlated (p < 0.001) with sea surface temperature anomalies in the surrounding seas. MSA showed a trend of 0.405 ng/m3/yr (0.680%/yr) for June and July. NSS‐SO4 concentrations at Kevo declined dramatically in the early 1990s, probably as a result of the collapse of the Soviet Union. The decline has continued since the mid‐1990s.

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In this study we evaluate the recently upgraded aethalometer (AE33) and the newly released tricolor absorption photometer (TAP) with respect to their response to wildfire aerosol plumes during their deployment at the Mount Bachelor Observatory (MBO; 2763 m a.s.l.) in central Oregon, USA, during the summer of 2016. While both instruments use similar methodology (i.e., light extinction through an aerosol-laden filter), each has a unique set of correction schemes to address artifacts originating from filter loading, scattering from captured aerosol particles, and multiple scattering effects of the filter fibers. We also utilize a Single Particle Soot Photometer (SP2) to determine refractory black carbon (rBC) in these air masses. In addition to comparing the AE33 filter-loading correction methodology to previously published aethalometer correction schemes, we also compare the AE33 to the correction schemes used for the TAP and evaluate the degree to which the different correction factors influence the derived absorption Å ngström exponents (AAE) and mass absorption cross sections (MACs). We find that while the different correction factors for either the AE33 or TAP do exert an influence on the derived MACs, AAEs exhibit the most sensitivity to the correction schemes. Our study finds that using the AE33 manufacturer's recommended settings results in aerosol light absorption coefficients that are 3.4 to 4 times greater than the aerosol light absorption coefficients reported by the TAP. We calculated a correction factor (C f ) of 4.35 for the AE33 by normalizing the AE33 to match the TAP. The uncorrected AE33 also gives equivalent black carbon (eBC) values that are approximately 2 times the rBC measured by the SP2 instrument. We also find that biomass burning aerosols result in significant MAC enhancements, particularly at lower wavelengths, which is attributable to brown carbon (BrC).