Laboratory studies of ice nucleation onto bare and internally mixed soot–sulfuric acid particles

Abstract

Abstract. Soot particles are potential candidates for ice-nucleating particles in cirrus cloud formation, which is known to exert a net-warming effect on climate. Bare soot particles, generally hydrophobic and fractal ones, mainly exist near emission sources. Coated or internally mixed soot particles are more abundant in the atmosphere and have a higher probability of impacting cloud formation and climate. However, the ice nucleation ability of coated soot particles is not as well understood as that of freshly produced soot particles. In this laboratory study, two samples, a propane flame soot and a commercial carbon black, were used as atmospheric soot surrogates and coated with varying wt % of sulfuric acid (H2SO4). The ratio of coating material mass to the mass of bare soot particles was controlled and progressively increased from less than 5 wt % to over 100 wt %. Both bare and coated soot particle ice nucleation activities were investigated with a continuous-flow diffusion chamber operated at mixed-phase and cirrus cloud conditions. The mobility diameter and mass distribution of size-selected soot particles with/without H2SO4 coating were measured by a scanning mobility particle sizer and a centrifugal particle mass analyser running in parallel. The mixing state and morphology of soot particles were characterized by scanning electron microscopy and transmission electron microscopy. In addition, the evidence of the presence of H2SO4 on a coated soot particle surface is shown by energy-dispersive X-ray spectroscopy. Our study demonstrates that H2SO4 coatings suppress the ice nucleation activity of soot particles to varying degrees depending on the coating thickness, but in a non-linear fashion. Thin coatings causing pore filling in the soot aggregate inhibits pore condensation and freezing. Thick coatings promote particle ice activation via droplet homogeneous freezing. Overall, our findings reveal that H2SO4 coatings will suppress soot particle ice nucleation abilities in the cirrus cloud regime, having implications for the fate of soot particles with respect to cloud formation in the upper troposphere.