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Residential biomass combustion significantly contributes to light-absorbing carbonaceous aerosols in the atmosphere, impacting the earth's radiative balance at regional and global levels. This study investigates the contribution of brown carbon (BrC) to the total particulate light absorption in the wavelength range of 370–950 nm (BrC 370–950) and the particulate absorption Ångström exponents (AAE 470/950) in 15 different European residential combustion appliances using a variety of wood-based fuels. BrC 370–950 was estimated to be from 1 % to 21 % for wood log stoves and 10 % for a fully automatized residential pellet boiler. Correlations between the ratio of organic to elemental carbon (OC / EC) and BrC 370–950 indicated that a one-unit increase in OC / EC corresponded to approximately a 14 % increase in BrC 370–950. Additionally, BrC 370–950 was clearly influenced by the fuel moisture content and the combustion efficiency, while the effect of the combustion appliance type was less prominent. AAE 470/950 of wood log combustion aerosols ranged from 1.06 to 1.61. By examining the correlation between AAE 470/950 and OC / EC, an AAE 470/950 close to unity was found for pure black carbon (BC) particles originating from residential wood combustion. This supports the common assumption used to differentiate light absorption caused by BC and BrC. Moreover, diesel aerosols exhibited an AAE 470/950 of 1.02, with BrC contributing only 0.66 % to the total absorption, aligning with the assumption employed in source apportionment. These findings provide important data to assess the BrC from residential wood combustion with different emission characteristics and confirm that BrC can be a major contributor to particulate UV and near-UV light absorption for northern European wood stove emissions with relatively high OC / EC ratios. [ABSTRACT FROM AUTHOR]

Residential biomass combustion significantly contributes to light-absorbing carbonaceous aerosols in the atmosphere, impacting the Earth's radiative balance at regional and global levels. This study investigates the contribution of brown carbon to the total particulate light absorption in the wavelength range of 370 to 950 nm (BrC370-950)and the particulate absorption Ångström exponents (AAE470/950) in 15 different European residential combustion appliances using a variety of wood-based fuels. BrC370-950 was estimated to be from 1 % to 21 % for wood log stoves and was primarily influenced by fuel moisture content and minimally affected by combustion appliance type. The BrC370-950 contribution was 10 % for a fully automatized residential pellet boiler. Correlations between the ratio of organic to elemental carbon (OC/EC) and BrC indicated that a one unit increase in OC/EC corresponded to approximately a 14 % increase in BrC370-950. Additionally, BrC370-950 increased with decreasing combustion efficiency. AAE470/950 of wood log combustion aerosols ranged from 1.06 to 1.61. By examining the correlation between AAE470/950 and OC/EC, an AAE470/950 close to unity was found for pure black carbon (BC) particles originating from residential wood combustion. This supports the common assumption used to differentiate light absorption caused by BC and BrC. Moreover, diesel aerosols exhibited an AAE470/950 of 1.02, with BrC370-950 contributing only 0.66 % to the total absorption, aligning with the assumption employed in source apportionment. These findings provide important data to assess the BrC370-950 of RWC emissions with different emission characteristics and confirm that BrC can be a major contributor to particulate UV and near-UV light absorption for Northern European wood stove emissions with relatively high OC/EC ratios. [ABSTRACT FROM AUTHOR]

Aerosol light absorption was measured during a 1-month field campaign in June–July 2019 at the Pallas Global Atmospheric Watch (GAW) station in northern Finland. Very low aerosol concentrations prevailed during the campaign, which posed a challenge for the instruments' detection capabilities. The campaign provided a real-world test for different absorption measurement techniques supporting the goals of the European Metrology Programme for Innovation and Research (EMPIR) Black Carbon (BC) project in developing aerosol absorption standard and reference methods. In this study we compare the results from five filter-based absorption techniques – aethalometer models AE31 and AE33, a particle soot absorption photometer (PSAP), a multi-angle absorption photometer (MAAP), and a continuous soot monitoring system (COSMOS) – and from one indirect technique called extinction minus scattering (EMS). The ability of the filter-based techniques was shown to be adequate to measure aerosol light absorption coefficients down to around 0.01 Mm-1 levels when data were averaged to 1–2 h. The hourly averaged atmospheric absorption measured by the reference MAAP was 0.09 Mm-1 (at a wavelength of 637 nm). When data were averaged for >1 h, the filter-based methods agreed to around 40 %. COSMOS systematically measured the lowest absorption coefficient values, which was expected due to the sample pre-treatment in the COSMOS inlet. PSAP showed the best linear correlation with MAAP (slope=0.95 , R2=0.78), followed by AE31 (slope=0.93). A scattering correction applied to PSAP data improved the data accuracy despite the added noise. However, at very high scattering values the correction led to an underestimation of the absorption. The AE31 data had the highest noise and the correlation with MAAP was the lowest (R2=0.65). Statistically the best linear correlations with MAAP were obtained for AE33 and COSMOS (R2 close to 1), but the biases at around the zero values led to slopes clearly below 1. The sample pre-treatment in the COSMOS instrument resulted in the lowest fitted slope. In contrast to the filter-based techniques, the indirect EMS method was not adequate to measure the low absorption values found at the Pallas site. The lowest absorption at which the EMS signal could be distinguished from the noise was >0.1 Mm-1 at 1–2 h averaging times. The mass absorption cross section (MAC) value measured at a range 0–0.3 Mm-1 was calculated using the MAAP and a single particle soot photometer (SP2), resulting in a MAC value of 16.0±5.7 m2g-1. Overall, our results demonstrate the challenges encountered in the aerosol absorption measurements in pristine environments and provide some useful guidelines for instrument selection and measurement practices. We highlight the need for a calibrated transfer standard for better inter-comparability of the absorption results. [ABSTRACT FROM AUTHOR]

The Aethalometer model has been used widely for estimating the contributions of fossil fuel emissions and biomass burning to equivalent black carbon (eBC). The calculation is based on measured absorption Ångström exponents (αabs). The interpretation of αabs is ambiguous since it is well known that it not only depends on the dominant absorber but also on the size and internal structure of the particles, core size, and shell thickness. In this work the uncertainties of the Aethalometer-model-derived apparent fractions of absorption by eBC from fossil fuel and biomass burning are evaluated with a core–shell Mie model. Biomass-burning fractions (BB(%)) were calculated for pure and coated single BC particles for lognormal unimodal and bimodal size distributions of BC cores coated with ammonium sulfate, a scattering-only material. BB(%) was very seldom 0 % even though BC was the only absorbing material in the simulations. The shape of size distribution plays an important role. Narrow size distributions result in higher αabs and BB(%) values than wide size distributions. The sensitivity of αabs and BB(%) to variations in shell volume fractions is the highest for accumulation-mode particles. This is important because that is where the largest aerosol mass is. For the interpretation of absorption Ångström exponents it would be very good to measure BC size distributions and shell thicknesses together with the wavelength dependency of absorption. [ABSTRACT FROM AUTHOR]

The Aethalometer model has been used widely for estimating the contributions of fossil fuel emissions and biomass burning to equivalent black carbon (eBC). The calculation is based on measured absorption Ångström exponents (aabs). The interpretation of aabs is ambiguous since it is well-known that it not only depends on the dominant absorber but also on the size and internal structure of the particles, core size and shell thickness. In this work the uncertainties of the Aethalometer-model-derived apparent fractions of absorption by eBC from fossil fuel and biomass burning are evaluated with a core-shell Mie model. Biomass-burning fractions (BB(%)) were calculated for pure and coated single BC particles, for lognormal unimodal and bimodal size distributions of BC cores coated with ammonium sulfate, a scattering-only material. BB(%) was very seldom 0% even though BC was the only absorbing material in the simulations. The shape of size distribution plays an important role. Narrow size distributions result in higher aabs and BB(%) values than wide size distributions. The sensitivity of aabs and BB(%) to variations in shell volume fractions is the highest for accumulation mode particles. This is important because that is where the largest aerosol mass is. For the interpretation of absorption Ångström exponents it would be very good to measure BC size distributions and shell thicknesses together with the wavelength dependency of absorption. [ABSTRACT FROM AUTHOR]

The Arctic absorbing aerosols have a high potential to accelerate global warming. Accurate and sensitive measurements of their concentrations, variability and atmospheric mixing are needed. Filter-based aerosol light absorption measurement methods are the most widely applied in the Arctic. Those will be the focus of this study. Aerosol light absorption was measured during one month field campaign in June–July 2019 at the Pallas Global AtmosphericWatch (GAW) station in northern Finland. The campaign provided a real-world test for different absorption measurement techniques supporting the goals of the EMPIR BC metrology project in developing aerosol absorption standard and reference methods. Very low aerosol concentrations prevailed during the campaign which imposed a challenge for the instruments detection. In this study we compare the results from five filter-based absorption techniques: Aethalometer models AE31 and AE33, Particle Soot Absorption Photometer (PSAP), Multi Angle Absorption Photometer (MAAP) and Continuous Soot Monitoring System (COSMOS), and from one indirect method called Extinction Minus Scattering (EMS). The sensitivity of the filter-based techniques was adequate to measure aerosol light absorption coefficients down to around 0.05 Mm-1 levels. The average value measured during the campaign using MAAP was 0.09 Mm-1 (at wavelength of 637 nm). When data were averaged for >1h, an agreement of around 20% was obtained between instruments. COSMOS measured systematically the lowest absorption coefficient values, which was expected due to the sample pre-treatment in COSMOS inlet. PSAP showed the best linear correlation with MAAP (R2 = 0.85), followed by AE33 and COSMOS (R2 = 0.84). The noisy data from AE31 resulted in a slightly lower, yet a significant, correlation with MAAP (R2 = 0.46). In contrast to the filter-based techniques, the sensitivity of the indirect EMS method to measure aerosol absorption was not adequate at such low concentrations levels. An absorption coefficient on the order of >1 Mm-1 was estimated as the lowest limit, to reliably distinguish the signal from the noise. Throughout the campaign the aerosol was highly scattering with an average single-scattering albedo of 0.97. Two different air-mass origins could be identified: the north-east and from the north-west. The north-eastern air masses contained higher fraction of thickly coated light absorbing particles than the westerly air masses. Aerosol scattering, absorption and the particle coating thickness increased on the last ten days of the campaign during the north-eastern air flow. The simultaneous changes in aerosol source region, mixing state, concentration and particle optical size were reflected in the instruments' response in a complex way. The observed decrease in aerosol size suggested additional activation of secondary particle formation mechanisms. The results demonstrate the challenges encountered in the Arctic absorbing aerosol measurements. The applicability and uncertainties of different techniques are discussed and new knowledge on the absorbing aerosol characteristics in summer Arctic air masses reference to the source region is provided. [ABSTRACT FROM AUTHOR]

The deposition of light-absorbing aerosol (LAA) onto snow initiates processes that lead to increased snowmelt. Measurements of LAA, such as black carbon (BC) and mineral dust, have been observed globally to darken snow. Several measurement techniques of LAA in snow collect the particulates on filters for analysis. Here we investigate micro-quartz filters' optical response to BC experiments in which the particles are initially suspended in air or in a liquid. With particle soot absorption photometers (PSAPs) we observed a 20 % scattering enhancement for quartz filters compared to the standard PSAP Pallflex filters. The multiple-scattering correction factor (Cref) of the quartz filters for airborne soot aerosol is estimated to be ∼3.4. In the next stage correction factors were determined for BC particles mixed in water and also for BC particles both mixed in water and further treated in an ultrasonic bath. Comparison of BC collected from airborne particles with BC mixed in water filters indicated a higher mass absorption cross section by approximately a factor of 2 for the liquid-based filters, which is probably due to the BC particles penetrating deeper in the filter matrix. The ultrasonic bath increased absorption still further, roughly by a factor of 1.5, compared to only mixing in water. Application of the correction functions to earlier published field data from the Himalaya and Finnish Lapland yielded mass absorption coefficient (MAC) values of ∼7 –10 m 2 g -1 at λ=550 nm, which is in the range of the published MAC of airborne BC aerosol. [ABSTRACT FROM AUTHOR]

Black carbon is emitted from the incomplete combustion of carbonaceous fuels and will detrimentally affect air quality, climate and human health. In this study, equivalent black carbon (eBC) concentrations were measured by using an aethalometer (AE33) at three different locations in the Helsinki metropolitan area, Finland from October 2015 to May 2017. One sampling site was located in an urban street canyon (SC, sampling period 18 months) and two of the sampling sites were located in suburban detached house (DH) areas (DH1, 13 months and DH2, 5 months). Based on the campaign averages, the eBC concentration levels were higher at the street canyon site (1690 ± 1520 ng/m 3 ) than at the residential detached house areas (DH1 = 880 ± 1500 ng/m 3 and DH2 = 1040 ± 2130 ng/m 3 ). The contribution of eBC from fossil fuel (BC FF ) and wood burning (BC WB ) were estimated based on the spectral dependence of light absorption of different sources. The spectral behavior is described using absorption Ångström exponent (α) values for both fossil fuel (α FF ) and wood burning (α WB ) that were determined using concurrent wood burning tracer (levoglucosan) measurements. Based on the source apportionment, the contribution of BC WB to eBC was clearly higher at the detached house area sites DH1 (41 ± 14%) and DH2 (46 ± 15%) than at the urban street canyon site (15 ± 14%). A distinct seasonal dependency was observed in the eBC concentration levels at the detached house areas. The highest concentrations were detected during the cold seasons due to residential wood combustion. On the opposite, at the SC site, the concentration levels of eBC were rather constant throughout the campaign, being dominated by the BC FF emissions from close-by vehicular traffic. Substantial temporal and spatial variability in eBC concentrations and sources were observed within the Helsinki metropolitan area. eBC is shown to be closely tied to the characteristics of the measurement site, season, meteorological conditions and the time of the day. [ABSTRACT FROM AUTHOR]

While more and more studies are being conducted on carbonaceous fractions—organic carbon (OC) and elemental carbon (EC)—in urban areas, there are still too few studies about these species and their effects in polar areas due to their very low concentrations; further, studies in the literature report only data from intensive campaigns, limited in time. We present here for the first time EC–OC concentration long-time data records from the sea-level sampling site of Ny-Ålesund, in the High Arctic (5 years), and from Dome C, in the East Antarctic Plateau (1 year). Regarding the Arctic, the median (and the interquartile range (IQR)) mass concentrations for the years 2011–2015 are 352 (IQR: 283–475) ng/m3 for OC and 4.8 (IQR: 4.6–17.4) ng/m3 for EC, which is responsible for only 3% of total carbon (TC). From both the concentration data sets and the variation of the average monthly concentrations, the influence of the Arctic haze on EC and OC concentrations is evident. Summer may be interested by high concentration episodes mainly due to long-range transport (e.g., from wide wildfires in the Northern Hemisphere, as happened in 2015). The average ratio of EC/OC for the summer period is 0.05, ranging from 0.02 to 0.10, and indicates a clean environment with prevailing biogenic (or biomass burning) sources, as well as aged, highly oxidized aerosol from long-range transport. Contribution from ship emission is not evident, but this result may be due to the sampling time resolution. In Antarctica, a 1 year-around data set from December 2016 to February 2018 is shown, which does not present a clear seasonal trend. The OC median (and IQR) value is 78 (64–106) ng/m3; for EC, it is 0.9 (0.6–2.4) ng/m3, weighing for 3% on TC values. The EC/OC ratio mean value is 0.20, with a range of 0.06–0.35. Due to the low EC and OC concentrations in polar areas, correction for the blank is far more important than in campaigns carried out in other regions, largely affecting uncertainties in measured concentrations. Through the years, we have thus developed a new sampling strategy that is presented here for the first time: samplers were modified in order to collect a larger amount of particulates on a small surface, enhancing the capability of the analytical method since the thermo-optical analyzer is sensitive to carbonaceous aerosol areal density. Further, we have recently coupled such modified samplers with a sampling strategy that makes a more reliable blank correction of every single sample possible. [ABSTRACT FROM AUTHOR]

Atmospheric aerosols have a significant effect on earth's radiative budget, particularly on regional scales. This paper presents a ~6 year, in situ, ground level aerosol scattering and absorption dataset, measured at a background site strategically positioned to enable differentiation of the effect of anthropogenic, population density and open biomass burning activities on a regional scale. Relatively well-defined seasonal and diurnal patterns were observed for all the aerosol optical properties, i.e. scattering coefficient (σ SP), absorption coefficient (σ AP), single scattering albedo (ω 0) and Ångström exponent of scattering (α SP). These patterns were explained by considering southern African specific sources and metrological conditions. Using a receptor modelling method (auto-generated source maps) it was found that air masses that had higher σ SP , σ AP and ω 0 , and lower α SP , if compared with the relatively clean background, passed over source regions with significant industrial or other anthropogenic activities, higher population density, re-circulation of polluted air masses and higher open biomass burning frequency. To quantify differences, four source regions were defined, i.e. Karoo, Kalahari, anti-cyclonic recirculation pattern and the industrial hub of South Africa. Air masses that had passed over the Karoo source region represented the cleanest regional background conditions, while air masses that had passed either over the industrial hub and/or the anti-cyclonic recirculation pattern represented the most significant anthropogenically impacted, as indicated by the aerosol optical properties. The ω 0 medians of air masses that had passed over the Karoo (0.80–0.86) were 9, 12 and 7% lower than in air masses that had passed over source regions with the highest ω 0 median, in the warmest/wettest, coldest, and driest, peak open biomass burning periods, respectively. • A six-year, ground level aerosol optical property dataset is presented. • Well-defined seasonal and diurnal patterns were evident for the optical properties. • Auto-generated source maps were used to explain results within a regional context. • Air masses passing over the Karoo region represented the most natural background. • Anthropogenic influences were evident in air masses passing over all other regions. [ABSTRACT FROM AUTHOR]