Abstract
Abstract. A significant fraction of atmospheric particles that serve as cloud condensation nuclei (CCN) are thought to originate from the condensational growth of new particle formation (NPF) from the gas phase. Here, 7 years of continuous aerosol and meteorological measurements (June 2008 to May 2015) at a remote background site of the eastern Mediterranean were recorded and analyzed to assess the impact of NPF (of 162 episodes identified) on CCN and cloud droplet number concentration (CDNC) formation in the region. A new metric is introduced to quantitatively determine the initiation and duration of the influence of NPF on the CCN spectrum. NPF days were found to increase CCN concentrations (from 0.10 % to 1.00 % supersaturation) between 29 % and 77 %. Enhanced CCN concentrations from NPF are mostly observed, as expected, under low preexisting particle concentrations and occur in the afternoon, relatively later in the winter and autumn than in the summer. Potential impacts of NPF on cloud formation were quantified by introducing the observed aerosol size distributions and chemical composition into an established cloud droplet parameterization. We find that the supersaturations that develop are very low (ranging between 0.03 % and 0.27 %) for typical boundary layer dynamics (σw ∼0.3 m s−1) and NPF is found to enhance CDNC by a modest 13 %. This considerable contrast between CCN and CDNC response is in part from the different supersaturation levels considered, but also because supersaturation drops from increasing CCN because of water vapor competition effects during the process of droplet formation. The low cloud supersaturation further delays the appearance of NPF impacts on CDNC to clouds formed in the late evening and nighttime – which has important implications for the extent and types of indirect effects induced by NPF events. An analysis based on CCN concentrations using prescribed supersaturation can provide very different, even misleading, conclusions and should therefore be avoided. The proposed approach here offers a simple, yet highly effective way for a more realistic impact assessment of NPF events on cloud formation.
Highlights
Cloud condensation nuclei (CCN) and cloud droplet formation constitute the direct microphysical link between aerosols and clouds
Its contribution to the total estimated PM1 mass was found to be on the order of 38 ± 10 % using the bulk PM10 24 h quartz fiber filters, and its contribution to the total PM1 mass was calculated to be 44 ± 12 % using the ACSM data, indicating that the relative abundance of sulfate and organics dictates to a high extent the hygroscopic and cloud-activating properties of submicron particles over Finokalia
The aerosol particle number size distributions along with chemical composition and meteorological parameters were studied at a remote background site in the eastern Mediterranean over a 7-year period in order to quantify how regional new particle formation (NPF) events modulate the concentration of aerosol, cloud condensation nuclei (CCN), droplet number and maximum supersaturation developed in clouds of the region
Summary
Cloud condensation nuclei (CCN) and cloud droplet formation constitute the direct microphysical link between aerosols and clouds. Quantifying how changes in aerosols affect global clouds, precipitation, and climate is limited by the large number of processes and scales that need to be captured in models New particle formation (NPF), the process during which new particles are formed directly from the gas phase, is thought to significantly shape the distribution of CCN throughout the atmosphere (Pierce and Adams, 2007; Westervelt et al, 2013; Gordon et al, 2017). Initially too small (1–2 nm; Kerminen et al, 2012) to act as CCN, particles from NPF can grow to sufficient size and hygroscopicity over a period of a few hours to days and eventually act as efficient CCN
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