Use of the Single Particle Soot Photometer (SP2) as a pre-filter for ice nucleation measurements: effect of particle mixing state and determination of SP2 conditions to fully vaporize refractory black carbon

Abstract

Ice nucleation is a fundamental atmospheric process that impacts precipitation, cloud lifetimes, and climate. Challenges remain to identify and quantify the compositions and sources of ice-nucleating particles (INPs). Assessment of the role of black carbon (BC) as an INP is particularly important due to its anthropogenic sources and abundance at upper-tropospheric cloud levels. The role of BC as an INP, however, is unclear. This is, in part, driven by a lack of techniques that directly determine the contribution of refractory BC (rBC) to INP concentrations. One previously developed technique to measure this contribution uses the Single Particle Soot Photometer (SP2) as a pre-filter to an online ice-nucleating particle counter. In this technique, rBC particles are selectively heated to their vaporization temperature in the SP2 cavity by a 1064 nm laser. From previous work, however, it is unclear under what SP2 conditions, if any, the original rBC particles were fully vaporized. Furthermore, previous work also left questions about the effect of the SP2 laser on the ice-nucleating properties of several INP proxies and their mixtures with rBC.To answer these questions, we sampled the exhaust of an SP2 with a Scanning Mobility Particle Sizer and a Continuous Flow Diffusion Chamber. Using Aquadag® as an rBC proxy, the effect of several SP2 instrument parameters on the size distribution and physical properties of particles in rBC SP2 exhaust were explored. We found that a high SP2 laser power (930 nW∕(220 nm PSL)) is required to fully vaporize a ∼ 0.76 fg rBC particle. We also found that the exhaust particle size distribution is minimally affected by the SP2 sheath-to-sample ratio; the size of the original rBC particle, however, greatly influences the size distribution of the SP2 exhaust. The effect of the SP2 laser on the ice nucleation efficiency of Snomax®, NX-illite, and Suwannee River Fulvic Acid was studied; these particles acted as proxies for biological, illite-rich mineral dust, and brown carbon INPs, respectively. The original size distribution and ice nucleation efficiency of all non-rBC proxies were unaffected by the SP2 laser. Furthermore, the ice nucleation efficiencies of all proxies were not affected when externally mixed with rBC. These proxies, however, always show a reduction in ice-nucleating ability when internally mixed with rBC. We end this work with recommendations for users who wish to use the SP2 as a pre-filter to remove large rBC particles from an aerosol stream.