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Opis: Absorbing aerosol species, such as Black (BC) and Brown (BrC) Carbon, are able to warm the atmosphere. The role of aerosols is one of the least clear aspects in the so called “Arctic Amplification” (AA) and up to now this was mostly modelled [1,2]. For this reason, we took part in four scientific cruises (AREX, Arctic-Expedition, summer 2018, 2019, 2021 and EUREC4A, 2020) in the North Atlantic, eastward and south-eastward of Barbados, aiming at the determination of the aerosol chemical composition and properties from the Tropics to the North Pole. The Heating Rate (HR) was experimentally determined at 1 minute time-resolution along different latitudes by means of an innovative methodology [3], obtained by cumulatively taking into account the aerosol optical properties, i.e. the absorption coefficients (measured by AE33 Aethalometer) and incident radiation (direct, diffuse and reflected) across the entire solar spectrum. The HR computed along AREX and in Milan (in the same period) were used to determine the energy gradient, due to the LAA induced heat storage at mid-latitudes, which contributes to AA through the atmospheric heat transport northward. Moreover, aerosol chemical composition was achieved by means of sampling via high volume sampler (ECHO-PUF Tecora) and analysis via ion chromatography, TCA08 for Total Carbon content, Aethalometer AE33 (for BC), ICP-OES for elements. A clear latitudinal behaviour in Black Carbon concentrations, with the highest values at low latitudes (e.g. average BC concentration in Gdansk up to 1507±75 ng/m3) and a progressive decrease moving northwards and away from the big Arctic settlements (Black Carbon concentrations within the 81st parallel: 5±1 ng/m3). According to the latitudinal behaviour of BC concentrations and solar radiation (decreases towards the north while the diffuse component increases), HR decreases noticeably towards the Arctic: e.g. higher in the harbor of Gdansk (0.290±0.010 K/day) followed by the Baltic Sea (0.04±0.01 K/day), the Norvegian Sea (0.010±0.010 K/day) and finally with the lowest values in the pure Arctic Ocean (0.003±0.001 K/day). Accordingly, the energy density added to the system by the aerosol, a positive forcing that differs by 2 orders of magnitude between mid-latitudes and North Pole was found: 347.3 ± 11.8 J/m3 (Milan), 244.8 ± 12.2 J/m3 (Gdansk) and 2.6 ± 0.2 J/m3 (80°N). These results highlight the presence of a great energy gradient between mid-latitudes and Arctic that can trigger a heat transport towards the Arctic. Moreover this was strengthen by the HR value for EUREC4A in Barbados that was 0.175±0.003 K/day. Finally, preliminary results from Antarctica collected onboard the Italian RV Laura Bassi cruising the Southern Ocean and the Ross Sea will be shown.     Acknoledgements: GEMMA Center, Project TECLA MIUR – Dipartimenti di Eccellenza 2023–2027. JPI EUREC4A-OA project. CAIAC (oCean Atmosphere Interactions in the Antarctic regions and Convergence latitude) PNRA project   References [1] Navarro, J. C. A. et al. (2016) Nat. Geosci. 9, 277–281. [2] Shindell, D. and Faluvegi, G. (2009) Nat. Geosci. 2, 294–300. [3] Ferrero, L. et al. (2018) Environ. Sci. Technol. 52, 3546 3555.
Ključne besede: blackcarbon, brown carbon, atmospheric heating rate, climate change
Objavljeno v RUNG: 18.03.2024; Ogledov: 2356; Prenosov: 68
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Opis: There exists a lack of aerosol absorption measurement techniques with low uncertainties and without artefacts. We have developed the two-wavelength Photothermal Aerosol Absorption Monitor (PTAAM-2λ), which measures the aerosol absorption coefficient at 532 and 1064 nm. Here we describe its design, calibration and mode of operation and evaluate its applicability, limits and uncertainties. The 532 nm channel was calibrated with ∼ 1 µmol mol−1 NO2, whereas the 1064 nm channel was calibrated using measured size distribution spectra of nigrosin particles and a Mie calculation. Since the aerosolized nigrosin used for calibration was dry, we determined the imaginary part of the refractive index of nigrosin from the absorbance measurements on solid thin film samples. The obtained refractive index differed considerably from the one determined using aqueous nigrosin solution. PTAAM-2λ has no scattering artefact and features very low uncertainties: 4 % and 6 % for the absorption coefficient at 532 and 1064 nm, respectively, and 9 % for the absorption Ångström exponent. The artefact-free nature of the measurement method allowed us to investigate the artefacts of filter photometers. Both the Aethalometer AE33 and CLAP suffer from cross-sensitivity to scattering – this scattering artefact is most pronounced for particles smaller than 70 nm. We observed a strong dependence of the filter multiple scattering parameter on the particle size in the 100–500 nm range. The results from the winter ambient campaign in Ljubljana showed similar multiple scattering parameter values for ambient aerosols and laboratory experiments. The spectral dependence of this parameter resulted in AE33 reporting the absorption Ångström exponent for different soot samples with values biased 0.23–0.35 higher than the PTAAM-2λ measurement. Photothermal interferometry is a promising method for reference aerosol absorption measurements.
Ključne besede: aerosol absorption, calibration, black carbon
Objavljeno v RUNG: 28.06.2022; Ogledov: 2735; Prenosov: 27
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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: 3546; Prenosov: 0
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Opis: We experimentally quantified the impact of cloud fraction and cloud type on the heating rate (HR) of black and brown carbon (HRBC and HRBrC). In particular, we examined in more detail the cloud effect on the HR detected in a previous study (Ferrero et al., 2018). High-time-resolution measurements of the aerosol absorption coefficient at multiple wavelengths were coupled with spectral measurements of the direct, diffuse and surface reflected irradiance and with lidar–ceilometer data during a field campaign in Milan, Po Valley (Italy). The experimental set-up allowed for a direct determination of the total HR (and its speciation: HRBC and HRBrC) in all-sky conditions (from clear-sky conditions to cloudy). The highest total HR values were found in the middle of winter (1.43 ± 0.05 K d−1), and the lowest were in spring (0.54 ± 0.02 K d−1). Overall, the HRBrC accounted for 13.7 ± 0.2 % of the total HR, with the BrC being characterized by an absorption Ångström exponent (AAE) of 3.49 ± 0.01. To investigate the role of clouds, sky conditions were classified in terms of cloudiness (fraction of the sky covered by clouds: oktas) and cloud type (stratus, St; cumulus, Cu; stratocumulus, Sc; altostratus, As; altocumulus, Ac; cirrus, Ci; and cirrocumulus–cirrostratus, Cc–Cs). During the campaign, clear-sky conditions were present 23 % of the time, with the remaining time (77 %) being characterized by cloudy conditions. The average cloudiness was 3.58 ± 0.04 oktas (highest in February at 4.56 ± 0.07 oktas and lowest in November at 2.91 ± 0.06 oktas). St clouds were mostly responsible for overcast conditions (7–8 oktas, frequency of 87 % and 96 %); Sc clouds dominated the intermediate cloudiness conditions (5–6 oktas, frequency of 47 % and 66 %); and the transition from Cc–Cs to Sc determined moderate cloudiness (3–4 oktas); finally, low cloudiness (1–2 oktas) was mostly dominated by Ci and Cu (frequency of 59 % and 40 %, respectively). HR measurements showed a constant decrease with increasing cloudiness of the atmosphere, enabling us to quantify for the first time the bias (in %) of the aerosol HR introduced by the simplified assumption of clear-sky conditions in radiative-transfer model calculations. Our results showed that the HR of light-absorbing aerosol was ∼ 20 %–30 % lower in low cloudiness (1–2 oktas) and up to 80 % lower in completely overcast conditions (i.e. 7–8 oktas) compared to clear-sky ones. This means that, in the simplified assumption of clear-sky conditions, the HR of light-absorbing aerosol can be largely overestimated (by 50 % in low cloudiness, 1–2 oktas, and up to 500 % in completely overcast conditions, 7–8 oktas). The impact of different cloud types on the HR was also investigated. Cirrus clouds were found to have a modest impact, decreasing the HRBC and HRBrC by −5 % at most. Cumulus clouds decreased the HRBC and HRBrC by −31 ± 12 % and −26 ± 7 %, respectively; cirrocumulus–cirrostratus clouds decreased the HRBC and HRBrC by −60 ± 8 % and −54 ± 4 %, which was comparable to the impact of altocumulus (−60 ± 6 % and −46 ± 4 %). A higher impact on the HRBC and HRBrC suppression was found for stratocumulus (−63 ± 6 % and −58 ± 4 %, respectively) and altostratus (−78 ± 5 % and −73 ± 4 %, respectively). The highest impact was associated with stratus, suppressing the HRBC and HRBrC by −85 ± 5 % and −83 ± 3 %, respectively. The presence of clouds caused a decrease of both the HRBC and HRBrC (normalized to the absorption coefficient of the respective species) of −11.8 ± 1.2 % and −12.6 ± 1.4 % per okta. This study highlights the need to take into account the role of both cloudiness and different cloud types when estimating the HR caused by both BC and BrC and in turn decrease the uncertainties associated with the quantification of their impact on the climate.
Ključne besede: black carbon, brown carbon, cloud, atmospheric heating rate, climate change
Objavljeno v RUNG: 29.03.2021; Ogledov: 3873; Prenosov: 0
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Ključne besede: aerosol absorption, method intercomparison
Objavljeno v RUNG: 17.07.2019; Ogledov: 5066; Prenosov: 0
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