The impact of cloudiness and cloud type on the atmospheric heating rate of black and brown carbon in the Po Valley

oleh: L. Ferrero, L. Ferrero, A. Gregorič, A. Gregorič, G. Močnik, G. Močnik, M. Rigler, S. Cogliati, S. Cogliati, F. Barnaba, L. Di Liberto, G. P. Gobbi, N. Losi, N. Losi, E. Bolzacchini, E. Bolzacchini

Format: Article
Diterbitkan: Copernicus Publications 2021-03-01

Deskripsi

<p>We experimentally quantified the impact of cloud fraction and cloud type on the heating rate (HR) of black and brown carbon (<span class="inline-formula">HR<sub>BC</sub></span> and <span class="inline-formula">HR<sub>BrC</sub></span>). 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: <span class="inline-formula">HR<sub>BC</sub></span> and <span class="inline-formula">HR<sub>BrC</sub></span>) in all-sky conditions (from clear-sky conditions to cloudy). The highest total HR values were found in the middle of winter (1.43 <span class="inline-formula">±</span> 0.05 <span class="inline-formula">K d<sup>−1</sup></span>), and the lowest were in spring (0.54 <span class="inline-formula">±</span> 0.02 <span class="inline-formula">K d<sup>−1</sup></span>). Overall, the <span class="inline-formula">HR<sub>BrC</sub></span> accounted for 13.7 <span class="inline-formula">±</span> 0.2 % of the total HR, with the BrC being characterized by an absorption Ångström exponent (AAE) of 3.49 <span class="inline-formula">±</span> 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 <span class="inline-formula">±</span> 0.04 oktas (highest in February at 4.56 <span class="inline-formula">±</span> 0.07 oktas and lowest in November at 2.91 <span class="inline-formula">±</span> 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).</p> <p>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 <span class="inline-formula">∼</span> 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,<span id="page4870"/> 1–2 oktas, and up to 500 % in completely overcast conditions, 7–8 oktas).</p> <p>The impact of different cloud types on the HR was also investigated. Cirrus clouds were found to have a modest impact, decreasing the <span class="inline-formula">HR<sub>BC</sub></span> and <span class="inline-formula">HR<sub>BrC</sub></span> by <span class="inline-formula">−</span>5 % at most. Cumulus clouds decreased the <span class="inline-formula">HR<sub>BC</sub></span> and <span class="inline-formula">HR<sub>BrC</sub></span> by <span class="inline-formula">−</span>31 <span class="inline-formula">±</span> 12 % and <span class="inline-formula">−</span>26 <span class="inline-formula">±</span> 7 %, respectively; cirrocumulus–cirrostratus clouds decreased the <span class="inline-formula">HR<sub>BC</sub></span> and <span class="inline-formula">HR<sub>BrC</sub></span> by <span class="inline-formula">−</span>60 <span class="inline-formula">±</span> 8 % and <span class="inline-formula">−</span>54 <span class="inline-formula">±</span> 4 %, which was comparable to the impact of altocumulus (<span class="inline-formula">−</span>60 <span class="inline-formula">±</span> 6 % and <span class="inline-formula">−</span>46 <span class="inline-formula">±</span> 4 %). A higher impact on the <span class="inline-formula">HR<sub>BC</sub></span> and <span class="inline-formula">HR<sub>BrC</sub></span> suppression was found for stratocumulus (<span class="inline-formula">−</span>63 <span class="inline-formula">±</span> 6 % and <span class="inline-formula">−</span>58 <span class="inline-formula">±</span> 4 %, respectively) and altostratus (<span class="inline-formula">−</span>78 <span class="inline-formula">±</span> 5 % and <span class="inline-formula">−</span>73 <span class="inline-formula">±</span> 4 %, respectively). The highest impact was associated with stratus, suppressing the <span class="inline-formula">HR<sub>BC</sub></span> and <span class="inline-formula">HR<sub>BrC</sub></span> by <span class="inline-formula">−</span>85 <span class="inline-formula">±</span> 5 % and <span class="inline-formula">−</span>83 <span class="inline-formula">±</span> 3 %, respectively. The presence of clouds caused a decrease of both the <span class="inline-formula">HR<sub>BC</sub></span> and <span class="inline-formula">HR<sub>BrC</sub></span> (normalized to the absorption coefficient of the respective species) of <span class="inline-formula">−</span>11.8 <span class="inline-formula">±</span> 1.2 % and <span class="inline-formula">−</span>12.6 <span class="inline-formula">±</span> 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.</p>