Abstract
Abstract. There is evidence that black carbon (BC) particles may affect cirrus formation and, hence, global climate by acting as potential ice nucleating particles (INPs) in the troposphere. Nevertheless, the ice nucleation (IN) ability of bare BC and BC coated with secondary organic aerosol (SOA) material remains uncertain. We have systematically examined the IN ability of 100–400 nm size-selected BC particles with different morphologies and different SOA coatings representative of anthropogenic (toluene and n-dodecane) and biogenic (β-caryophyllene) sources in the cirrus regime (−46 to −38 ∘C). Several BC proxies were selected to represent different particle morphologies and oxidation levels. Atmospheric aging was further replicated with the exposure of SOA-coated BC to OH. The results demonstrate that the 400 nm hydrophobic BC types nucleate ice only at or near the homogeneous freezing threshold. Ice formation at cirrus temperatures below homogeneous freezing thresholds, as opposed to purely homogeneous freezing, was observed to occur for some BC types between 100 and 200 nm within the investigated temperature range. More fractal BC particles did not consistently act as superior INPs over more spherical ones. SOA coating generated by oxidizing β-caryophyllene with O3 did not seem to affect BC IN ability, probably due to an SOA-phase state transition. However, SOA coatings generated from OH oxidation of various organic species did exhibit higher IN-onset supersaturation ratio with respect to ice (SSi), compared with bare BC particles, with the toluene-SOA coating showing an increase in SSi of 0.1–0.15 while still below the homogeneous freezing threshold. Slightly oxidized toluene SOA coating seemed to have a stronger deactivation effect on BC IN ability than highly oxidized toluene SOA, which might be caused by oligomer formation and the phase state transition of toluene SOA under different oxidation levels. n-dodecane and β-caryophyllene-derived SOA-coated BC only froze in the homogeneous regime. We attribute the inhibition of IN ability to the filling of the pores on the BC surface by the SOA material coating. OH exposure levels of n-dodecane and β-caryophyllene SOA coating experiments, from an equivalent atmospheric exposure time from 10 to 90 d, did not render significant differences in the IN potential. Our study of selected BC types and sizes suggests that increases in diameter, compactness, and/or surface oxidation of BC particles lead to more efficient IN via the pore condensation freezing (PCF) pathway, and that coatings of common SOA materials can inhibit the formation of ice.
Highlights
Cirrus clouds affect the global energy balance predominantly by more effectively trapping long-wave terrestrial radiation than reflecting solar energy (e.g., Kärcher et al, 2007; Heymsfield et al, 2017; Kärcher, 2018)
Our results suggest that less oxidized secondary organic aerosol (SOA), with 200 to 4000 times the typical tropospheric SOA (Tsigaridis and Kanakidou, 2003; Heald et al, 2008; Hodzic et al, 2016) mass loading in the PAM chamber (∼ 2000 to 4000 μg m−3), is more likely to condense on seed particles and form fully coated black carbon (BC) particles, moving ice nucleation (IN)-onset supersaturation with respect to ice (SSi) to the homogeneous regime, while β-caryophyllene SOA oxidized by O3 does not alter the SSi of the soot particles
The IN ability of size-selected (100–400 nm) BC particles with different morphologies and surface chemistry and BC particles coated with toluene, n-dodecane, and βcaryophyllene-derived SOA has been systematically investigated in the cirrus temperature regime (−46 to −38 ◦C)
Summary
Cirrus clouds affect the global energy balance predominantly by more effectively trapping long-wave terrestrial radiation than reflecting solar energy (e.g., Kärcher et al, 2007; Heymsfield et al, 2017; Kärcher, 2018). Ozone (Friedman et al, 2011) and hydroxyl (OH) radical (Chou et al, 2013; Kulkarni et al, 2016) oxidation can change surface functional groups of BC particles and enhance hydrophilicity, but no distinguishable BC IN activity change has been observed Despite these previous efforts, the influence of particle morphology, chemistry, and aging, as well as the microphysical mechanism behind BC IN ability, remains ambiguous. Our results help to clarify the effects of physicochemical properties and SOA formation on BC IN ability and on cirrus formation in the upper troposphere
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