11. Molecular and physical characteristics of aerosol at a remote free troposphere site : implications for atmospheric agingSimeon K. Schum, Bo Zhang, Katja Džepina, Paulo Fialho, Claudio Mazzoleni, Lynn R. Mazzoleni, 2018, izvirni znanstveni članek Opis: Aerosol properties are transformed by atmospheric processes during long-range transport and play a key role in the Earth’s radiative balance. To understand the molecular and physical characteristics of free tropospheric aerosol, we studied samples collected at the Pico Mountain Observatory in the North Atlantic. The observatory is located in the marine free troposphere at 2225m above sea level, on Pico Island in the Azores archipelago. The site is ideal for the study of long-range-transported free tropospheric aerosol with minimal local influence. Three aerosol samples with elevated organic carbon concentrations were selected for detailed analysis. FLEXPART retroplumes indicated that two
of the samples were influenced by North American wildfire
emissions transported in the free troposphere and one by
North American outflow mainly transported within the marine
boundary layer. Ultrahigh-resolution Fourier transform
ion cyclotron resonance mass spectrometry was used to determine
the detailed molecular composition of the samples.
Thousands of molecular formulas were assigned to each of
the individual samples. On average ~60% of the molecular
formulas contained only carbon, hydrogen, and oxygen
atoms (CHO), ~ 30% contained nitrogen (CHNO), and
~ 10% contained sulfur (CHOS). The molecular formula
compositions of the two wildfire-influenced aerosol samples
transported mainly in the free troposphere had relatively low
average O=C ratios (0:48 ± 0:13 and 0:45 ± 0:11) despite the
7–10 days of transport time according to FLEXPART. In contrast,
the molecular composition of the North American outflow
transported mainly in the boundary layer had a higher
average O=C ratio (0:57 ± 0:17) with 3 days of transport time.
To better understand the difference between free tropospheric
transport and boundary layer transport, the meteorological
conditions along the FLEXPART simulated transport pathways
were extracted from the Global Forecast System analysis
for the model grids. We used the extracted meteorological
conditions and the observed molecular chemistry to predict
the relative-humidity-dependent glass transition temperatures
(Tg) of the aerosol components. Comparisons of the
Tg to the ambient temperature indicated that a majority of
the organic aerosol components transported in the free troposphere were more viscous and therefore less susceptible to
oxidation than the organic aerosol components transported
in the boundary layer. Although the number of observations
is limited, the results suggest that biomass burning organic
aerosol injected into the free troposphere is more persistent
than organic aerosol in the boundary layer having broader
implications for aerosol aging.
Ključne besede: secondary organic aerosols, brown carbon, particle dispersion model, ultrahigh-resolution FT-ICR MS, Pico Mountain Observatory
Objavljeno v RUNG: 10.04.2021; Ogledov: 3642; Prenosov: 0
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12. The impact of cloudiness and cloud type on the atmospheric heating rate of black and brown carbon in the Po ValleyLuca Ferrero, Asta Gregorič, Griša Močnik, Martin Rigler, Sergio Cogliati, Francesca Barnaba, Luca Di Liberto, Gian Paolo Gobbi, Niccolò Losi, Ezio Bolzacchini, 2021, izvirni znanstveni članek 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: 3659; Prenosov: 0
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13. Substantial brown carbon emissions from wintertime residential wood burning over FranceYunjiang Zhang, Alexandre Albinet, Jean-Eudes Petit, Véronique Jacob, Florie Chevrier, Gregory Gille, Sabrina Pontet, Eve Chrétien, Marta Dominik-Sègue, Gilles Levigoureux, Griša Močnik, Valérie Gros, Jean-Luc Jaffrezo, Olivier Favez, 2020, izvirni znanstveni članek Opis: Brown carbon (BrC) is known to absorb light at subvisible wavelengths but its optical properties and sources are still poorly documented, leading to large uncertainties in climate studies. Here, we show its major wintertime contribution to total aerosol absorption at 370 nm (18–42%) at 9 different French sites. Moreover, an excellent correlation with levoglucosan (r2 = 0.9 and slope = 22.2 at 370 nm), suggesting important contribution of wood burning emissions to ambient BrC aerosols in France. At all sites, BrC peaks were mainly observed during late evening, linking to local intense residential wood burning during this time period. Furthermore, the geographic origin analysis also highlighted the high potential contribution of local and/or small-regional emissions to BrC. Focusing on the Paris region, twice higher BrC mass absorption efficiency value was obtained for less oxidized biomass burning organic aerosols (BBOA) compared to more oxidized BBOA (e.g., about 4.9 ± 0.2 vs. 2.0 ± 0.1 m2 g−1, respectively, at 370 nm). Finally, the BBOA direct radiative effect was found to be 40% higher when these two BBOA fractions are treated as light-absorbing species, compared to the non-absorbing BBOA scenario.
Ključne besede: Brown carbon, Multi sites, Residential wood burning, Mass absorption efficiency, France
Objavljeno v RUNG: 20.07.2020; Ogledov: 4503; Prenosov: 0
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