Abstract

Abstract. The high variability of aerosol particle concentrations, sizes and chemical composition makes their description challenging in atmospheric models. Aerosol–cloud interaction studies are usually focused on the activation of accumulation mode particles as cloud condensation nuclei (CCN). However, under specific conditions Aitken mode particles can also contribute to the number concentration of cloud droplets (Nd), leading to large uncertainties in predicted cloud properties on a global scale. We perform sensitivity studies with an adiabatic cloud parcel model to constrain conditions under which Aitken mode particles contribute to Nd. The simulations cover wide ranges of aerosol properties, such as total particle number concentration, hygroscopicity (κ) and mode diameters for accumulation and Aitken mode particles. Building upon the previously suggested concept of updraft (w)- and aerosol-limited regimes of cloud droplet formation, we show that activation of Aitken mode particles does not occur in w-limited regimes of accumulation mode particles. The transitional range between the regimes is broadened when Aitken mode particles contribute to Nd, as aerosol limitation requires much higher w than for aerosol size distributions with accumulation mode particles only. In the transitional regime, Nd is similarly dependent on w and κ. Therefore, we analyze the sensitivity of Nd to κ, ξ(κ), as a function of w to identify the value combinations above which Aitken mode particles can affect Nd. As ξ(κ) shows a minimum when the smallest activated particle size is in the range of the “Hoppel minimum” (0.06 µm ≤ Dmin ≤0.08 µm), the corresponding (w–κ) pairs can be considered a threshold level above which Aitken mode particles have significant impact on Nd. This threshold is largely determined by the number concentration of accumulation mode particles and by the Aitken mode diameter. Our analysis of these thresholds results in a simple parametric framework and criterion to identify aerosol and updraft conditions under which Aitken mode particles are expected to affect aerosol–cloud interactions. Our results confirm that Aitken mode particles likely do not contribute to Nd in polluted air masses (urban, biomass burning) at moderate updraft velocities (w≤3 m s−1) but may be important in deep convective clouds. Under clean conditions, such as in the Amazon, the Arctic and remote ocean regions, hygroscopic Aitken mode particles can act as CCN at updrafts of w<1 m s−1.

Highlights

  • The representation of aerosol–cloud interactions in atmospheric models is challenging due to the high variability of aerosol particle loading, properties and processes on small temporal and spatial scales

  • We perform simulations with an adiabatic parcel model to systematically explore the parameter ranges of aerosol properties (Na, Na: ξ (Na),Ait/Na,acc, κ, Dg,Ait, Dg,acc) and of w to identify aerosol and cloud conditions under which Aitken mode particles contribute to Nd. (All parameters are defined Table A1 in the Appendix.) Our analysis results in a framework that can be used to assess under which aerosol and cloud conditions detailed information on Aitken mode particles is needed to describe their potential role in aerosol–cloud interactions

  • Our sensitivity studies have shown that for bimodal (Aitken and accumulation mode) aerosol size distribution (ASD), the w–κ combinations resulting in ξ(κ) minimum values can be used as a criterion of conditions under which Aitken mode particles contribute to Nd

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Summary

Introduction

The representation of aerosol–cloud interactions in atmospheric models is challenging due to the high variability of aerosol particle loading, properties and processes on small temporal and spatial scales. Based on an intercomparison of 16 global models, it was concluded that Aitken mode particles do not significantly contribute to CCN in clouds with maximum supersaturations Smax = 0.2 % (Fanourgakis et al, 2019) Based on another global model study, Lee et al (2013) compared the influence of 28 parameters characterizing aerosol emissions, processes and size distributions on the CCN number concentration at S = 0.3 %. They identified the width of the Aitken mode as the second most important parameter after the dry deposition of accumulation mode particles.

Model description
Initialization
Results and discussion
Updraft and hygroscopicity regimes of Aitken mode CCN activation
Summary and conclusions
Full Text
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