RESUMO
Recent years have shown that secondary ice production (SIP) is ubiquitous, affecting all clouds from polar to tropical regions. SIP is not described well in models and may explain biases in warm mixed-phase cloud ice content and structure. Through modeling constrained by in-situ observations and its synergy with radar we show that SIP in orographic clouds exert a profound impact on the vertical distribution of hydrometeors and precipitation, especially in seeder-feeder cloud configurations. The mesoscale model simulations coupled with a radar simulator strongly support that enhanced aggregation and SIP through ice-ice collisions contribute to observed spectral bimodalities, skewing the Doppler spectra toward the slower-falling side at temperatures within the dendritic growth layer, ranging from -20 °C to -10 °C. This unique signature provides an opportunity to infer long-term SIP occurrences from the global cloud radar data archive, particularly for this underexplored temperature regime.
RESUMO
Aviation soot can affect contrail and cirrus cloud formation and impact climate. A product of incomplete combustion, soot particles, are fractal and hydrophobic aggregates comprising carbonaceous spheres with complex physicochemical properties. In the cirrus cloud regime, the surface wettability and pore abundance of soot particles are important determinants for their ice nucleation ability via pore condensation and freezing. In the atmosphere, soot particles can undergo various ageing processes which modify their surface chemistry and porosity, thus acting as ice nucleating particles with varying abilities as a function of ageing. In this study, size-selected soot particles were treated by thermal denuding at 573 K in a pure nitrogen (N2) or synthetic air (N2 + O2) flow and then exposed to varying relative humidity conditions at a fixed temperature in the range from 218 to 243 K, to investigate the role of volatile content in the ice nucleation ability. Both organic-lean and organic-rich propane (C3H8) flame soot particles, as well as two types of commercially available carbon black soot particles with high and low surface wettability, were tested. The size and mass distribution of soot aerosol were monitored during the ice nucleation experiments. Bulk soot samples also prepared in pure N2 or synthetic air environments at 573 K were characterised by thermogravimetric analysis, Fourier transform infrared spectroscopy and dynamic vapour sorption measurements, to reveal the relation between denuding volatile content, associated soot particle property modifications and the ice nucleation ability. Our study shows that thermal denuding induces a change in soot particle porosity playing a dominant role in regulating its ice nucleation via the pore condensation and freezing mechanism. The enrichment in mesopore (2-50 nm) availability may enhance soot ice nucleation. The presence of O2 in the thermal denuding process may introduce new active sites on soot particles for water interaction and increase soot surface wettability. However, these active sites only facilitate soot ice nucleation when mesopore structures are available. We conclude that a change in volatile content modifies both morphological properties and surface chemistry for soot particles, but porosity change plays the dominant role in regulating soot particle ice nucleation ability.
