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Ključne besede: total carbon, black carbon, brown carbon
Objavljeno v RUNG: 17.11.2021; Ogledov: 1912; Prenosov: 51
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Ključne besede: Aethalometer, Adriatic sea, Black carbon, Source apportionment, Levoglucosan, LOTOS-EURO
Objavljeno v RUNG: 17.11.2021; Ogledov: 1829; Prenosov: 8
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Opis: Providing reliable observations of aerosol particles' absorption properties at spatial and temporal resolutions suited to climate models is of utter importance to better understand the effects that atmospheric particles have on climate. Nowadays, one of the instruments most widely used in international monitoring networks for in situ surface measurements of light absorption properties of atmospheric aerosol particles is the multi-wavelength dual-spot Aethalometer, AE33. The AE33 derives the absorption coefficients of aerosol particles at seven different wavelengths from the measurements of the optical attenuation of light through a filter where particles are continuously collected. An accurate determination of the absorption coefficients from the AE33 instrument relies on the quantification of the non-linear processes related to the sample collection on the filter. The multiple-scattering correction factor (C), which depends on the filter tape used and on the optical properties of the collected particles, is the parameter with both the greatest uncertainty and the greatest impact on the absorption coefficients derived from the AE33 measurements. Here we present an in-depth analysis of the AE33 multiple-scattering correction factor C and its wavelength dependence for two different and widely used filter tapes, namely the old, and most referenced, TFE-coated glass, or M8020, filter tape and the currently, and most widely used, M8060 filter tape. For performing this analysis, we compared the attenuation measurements from AE33 with the absorption coefficients measured with different filter-based techniques. On-line co-located multi-angle absorption photometer (MAAP) measurements and off-line PP_UniMI polar photometer measurements were employed as reference absorption measurements for this work. To this aim, we used data from three different measurement stations located in the north-east of Spain, namely an urban background station (Barcelona, BCN), a regional background station (Montseny, MSY) and a mountaintop station (Montsec d'Ares, MSA). The median C values (at 637 nm) measured at the three stations ranged between 2.29 (at BCN and MSY, lowest 5th percentile of 1.97 and highest 95th percentile of 2.68) and 2.51 (at MSA, lowest 5th percentile of 2.06 and highest 95th percentile of 3.06). The analysis of the cross-sensitivity to scattering, for the two filter tapes considered here, revealed a large increase in the C factor when the single-scattering albedo (SSA) of the collected particles was above a given threshold, up to a 3-fold increase above the average C values. The SSA threshold appeared to be site dependent and ranged between 0.90 to 0.95 for the stations considered in the study. The results of the cross-sensitivity to scattering displayed a fitted constant multiple-scattering parameter, Cf, of 2.21 and 1.96, and a cross-sensitivity factor, ms, of 1.8 % and 3.4 % for the MSY and MSA stations, respectively, for the TFE-coated glass filter tape. For the M8060 filter tape, Cf values of 2.50, 1.96 and 1.82 and ms values of 1.6 %, 3.0 % and 4.9 % for the BCN, MSY and MSA stations, respectively, were obtained. SSA variations also influenced the spectral dependence of C, which showed an increase with wavelength when SSA was above the site-dependent threshold. Below the SSA threshold, no statistically significant dependence of C on the wavelength was observed. For the measurement stations considered here, the wavelength dependence of C was to some extent driven by the presence of dust particles during Saharan dust outbreaks that had the potential to increase the SSA above the average values. At the mountaintop station, an omission of the wavelength dependence of the C factor led to an underestimation of the absorption Ångström exponent (AAE) by up to 12 %. Differences in the absorption coefficient determined from AE33 measurements at BCN, MSY and MSA of around 35 %–40 % can be expected when using the site-dependent experimentally obtained C value instead of the nominal C value. Due to the fundamental role that the SSA of the particles collected on the filter tape has in the multiple-scattering parameter C, we present a methodology that allows the recognition of the conditions upon which the use of a constant and wavelength-independent C is feasible.
Ključne besede: black carbon, aerosol absorption, filter photometer, artifact
Objavljeno v RUNG: 01.10.2021; Ogledov: 1989; Prenosov: 0
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Opis: Accurate and temporally consistent measurements of light absorbing aerosol (LAA) heating rate (HR) and of its source apportionment (fossil-fuel, FF; biomass-burning, BB) and speciation (black and brown Carbon; BC, BrC) are needed to evaluate LAA short-term climate forcing. For this purpose, wavelength- and time-dependent accurate LAA absorption coefficients are required. HR was experimentally determined and apportioned (sources/species) in the EMEP/ACTRIS/COLOSSAL-2018 winter campaign in Milan (urban-background site). Two Aethalometers (AE31/AE33) were installed together with a MAAP, CPC, OPC, a low volume sampler (PM2.5) and radiation instruments. AE31/AE33 multiple-scattering correction factors (C) were determined using two reference systems for the absorption coefficient: 1) 5-wavelength PP_UniMI with low time resolution (12 h, applied to PM2.5 samples); 2) timely-resolved MAAP data at a single wavelength. Using wavelength- and time-independent C values for the AE31 and AE33 obtained with the same reference device, the total HR showed a consistency (i.e. reproducibility) with average values comparable at 95% probability. However, if different reference devices/approaches are used, i.e. MAAP is chosen as reference instead of a PP_UniMI, the HR can be overestimated by 23-30% factor (by both AE31/AE33). This became more evident focusing on HR apportionment: AE33 data (corrected by a wavelength- and time-independent C) showed higher HRFF (+24±1%) and higher HRBC (+10±1%) than that of AE31. Conversely, HRBB and HRBrC were -28±1% and -29±1% lower for AE33 compared to AE31. These inconsistencies were overcome by introducing a wavelength-dependent Cλ for both AE31 and AE33, or using multi-wavelength apportionment methods, highlighting the need for further studies on the influence of wavelength corrections for HR determination. Finally, the temporally-resolved determination of C resulted in a diurnal cycle of the HR not statistically different whatever the source- speciation- apportionment used.
Ključne besede: climate change, heating rate, black carbon, light absorbing aerosols
Objavljeno v RUNG: 09.06.2021; Ogledov: 2135; Prenosov: 0
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Opis: Aerosolized black carbon is monitored worldwide to quantify its impact on air quality and climate. Given its importance, measurements of black carbon mass concentrations must be conducted with instruments operating in quality-checked and ensured conditions to generate data which are reliable and comparable temporally and geographically. In this study, we report the results from the largest characterization and intercomparison of filter-based absorption photometers, the Aethalometer model AE33, belonging to several European monitoring networks. Under controlled laboratory conditions, a total of 23 instruments measured mass concentrations of black carbon from three well-characterized aerosol sources: synthetic soot, nigrosin particles, and ambient air from the urban background of Leipzig, Germany. The objective was to investigate the individual performance of the instruments and their comparability; we analyzed the response of the instruments to the different aerosol sources and the impact caused by the use of obsolete filter materials and the application of maintenance activities. Differences in the instrument-to-instrument variabilities from equivalent black carbon (eBC) concentrations reported at 880 nm were determined before maintenance activities (for soot measurements, average deviation from total least square regression was −2.0 % and the range −16 % to 7 %; for nigrosin measurements, average deviation was 0.4 % and the range −15 % to 17 %), and after they were carried out (for soot measurements, average deviation was −1.0 % and the range −14 % to 8 %; for nigrosin measurements, the average deviation was 0.5 % and the range −12 % to 15 %). The deviations are in most of the cases explained by the type of filter material employed by the instruments, the total particle load on the filter, and the flow calibration. The results of this intercomparison activity show that relatively small unit-to-unit variability of AE33-based particle light absorbing measurements is possible with well-maintained instruments. It is crucial to follow the guidelines for maintenance activities and the use of the proper filter tape in the AE33 to ensure high quality and comparable black carbon (BC) measurements among international observational networks.
Ključne besede: black carbon, aerosol, absorption, filter absorption photometer, aethaloemter
Objavljeno v RUNG: 03.05.2021; Ogledov: 2073; Prenosov: 0
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