Aitken mode particles as CCN in aerosol- and updraft-sensitive regimes of cloud droplet formation

摘要

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 ( N d ), 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 N d . 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 N d , as aerosol limitation requires much higher w than for aerosol size distributions with accumulation mode particles only. In the transitional regime, N d is similarly dependent on w and κ . Therefore, we analyze the sensitivity of N d to κ , ξ ( κ ) , as a function of w to identify the value combinations above which Aitken mode particles can affect N d . As ξ ( κ ) shows a minimum when the smallest activated particle size is in the range of the “Hoppel minimum” (0.06? μ m? ≤ ? D min ? ≤0.08 ? μ m), the corresponding ( w – κ ) pairs can be considered a threshold level above which Aitken mode particles have significant impact on N d . 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 N d 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 .