Aerosol Indirect Effects on Glaciated Clouds. Part II: Sensitivity Tests Using Solute Aerosols

Sensitivity tests were performed on a midlatitude continental case using a state-of-the-art aerosol–cloud model to determine the salient mechanisms of aerosol indirect effects (AIE) from solute aerosols. The simulations showed that increased solute aerosols doubled cloud-droplet number concentrations and hence reduced cloud particle sizes by about 20% and consequently inhibited warm rain processes, thus enhancing the chances of homogeneous freezing of cloud droplets and aerosols. Cloud fractions and their optical thicknesses increased quite substantially with increasing solute aerosols. Although liquid mixing ratios were boosted, there was, however, a substantial reduction of ice mixing ratios in the upper troposphere, owing to the increase in snow production aloft. The predicted total aerosol indirect effect was equal to −9.46 ± 1.4 W m−2. The AIEs of glaciated clouds (−6.33 ± 0.95 W m−2) were greater than those of water-only clouds (−3.13 ± 0.47 W m−2) by a factor of two in this continental case. The higher radiative importance of glaciated clouds compared with water-only clouds emerged from their larger collective spatial extent and their existence above water-only clouds. In addition to the traditional AIEs (glaciation, riming and thermodynamic), the new AIEs sedimentation, aggregation and coalescence were identified

Aerosol indirect effects on glaciated clouds. Part I: Model description

Various improvements were made to a state-of-the-art aerosol–cloud model and comparison of the model results with observations from field campaigns was performed. The strength of this aerosol–cloud model is in its ability to explicitly resolve all the known modes of heterogeneous cloud droplet activation and ice crystal nucleation. The model links cloud particle activation with the aerosol loading and chemistry of seven different aerosol species. These improvements to the model resulted in more accurate prediction especially of droplet and ice crystal number concentrations in the upper troposphere and enabled the model to directly sift the aerosol indirect effects based on the chemistry and concentration of the aerosols. In addition, continental and maritime cases were simulated for the purpose of validating the aerosol–cloud model and for investigating the critical microphysical and dynamical mechanisms of aerosol indirect effects from anthropogenic solute and solid aerosols, focusing mainly on glaciated clouds. The simulations showed that increased solute aerosols reduced cloud particle sizes by about 5 μm and inhibited warm rain processes. Cloud fractions and their optical thicknesses were increased quite substantially in both cases. Although liquid mixing ratios were boosted, there was however a substantial reduction of ice mixing ratios in the upper troposphere owing to the increase in snow production aloft. These results are detailed in the subsequent parts of this study

The relevance of nanoscale biological fragments for ice nucleation in clouds

Most studies of the role of biological entities as atmospheric ice-nucleating particles have focused on relatively rare supermicron particles such as bacterial cells, fungal spores and pollen grains. However, it is not clear that there are sufficient numbers of these particles in the atmosphere to strongly influence clouds. Here we show that the ice-nucleating activity of a fungus from the ubiquitous genus Fusarium is related to the presence of nanometre-scale particles which are far more numerous, and therefore potentially far more important for cloud glaciation than whole intact spores or hyphae. In addition, we quantify the ice-nucleating activity of nano-ice nucleating particles (nano-INPs) washed off pollen and also show that nano-INPs are present in a soil sample. Based on these results, we suggest that there is a reservoir of biological nano-INPs present in the environment which may, for example, become aerosolised in association with fertile soil dust particles

Contributions of biogenic material to the atmospheric ice-nucleating particle population in North Western Europe

A minute fraction of atmospheric particles exert a disproportionate effect on the phase of mixed-phase clouds by acting as ice-nucleating particles (INPs). To understand the effects of these particles on weather and climate, both now and into the future, we must first develop a quantitative understanding of the major INP sources worldwide. Previous work has demonstrated that aerosols such as desert dusts are globally important INPs, but the role of biogenic INPs is unclear, with conflicting evidence for their importance. Here, we show that at a temperate site all INPs active above −18 °C at concentrations >0.1 L−1 are destroyed on heating, consistent with these INPs being of biological origin. Furthermore, we show that a global model of desert dust INPs dramatically underestimates the measured INP concentrations, but is consistent with the thermally-stable component. Notably, the heat sensitive INPs are active at temperatures where shallow cloud layers in Northern Europe are frequently observed to glaciate. Hence, we suggest that biogenic material is important for primary ice production in this region. The prevalence of heat sensitive, most likely biogenic, INPs in this region highlights that, as a community, we need to quantify the sources and transport of these particles as well as determine their atmospheric abundance across the globe and at cloud altitudes

Secondary ice production during the break-up of freezing water drops on impact with ice particles

We provide the first dedicated laboratory study of collisions of supercooled water drops with ice particles as a secondary ice production mechanism. We experimentally investigated collisions of supercooled water drops (∼ 5 mm in diameter) with ice particles of a similar size (∼ 6 mm in diameter) placed on a glass slide at temperatures 12 ∘C. Our results showed that secondary drops were generated during both the spreading and retraction phase of the supercooled water drop impact. The secondary drops generated during the spreading phase were emitted too fast to quantify. However, quantification of the secondary drops generated during the retraction phase with diameters >0.1 mm showed that 5–10 secondary drops formed per collision, with approximately 30 % of the secondary drops freezing over a temperature range between −4 and −12 ∘C. Our results suggest that this secondary ice production mechanism may be significant for ice formation in atmospheric clouds containing large supercooled drops and ice particles