Size-dependent mass absorption cross-section of soot particles from various sources

TL;DR

This study demonstrates that the mass absorption cross-section of soot particles varies with size, increasing until a plateau, and suggests that soot graphitization degree is the likely factor influencing this size dependence.

Contribution

It provides the first comprehensive size-dependent MAC measurements across various soot sources and evaluates different hypotheses, identifying soot graphitization as the probable cause.

Findings

MAC increases with aggregate size until a plateau at 4-30 fg mass

Smallest particles have 50-80% lower MAC than largest ones

Modeling suggests soot graphitization degree influences MAC size dependence

Abstract

The mass absorption cross-section (MAC) of combustion-generated soot is used in pollution and emissions measurements to quantify the mass concentration of soot and in atmospheric modelling to predict the radiative effects of soot on climate. Previous work has suggested that the MAC of soot particles may change with their size, due to (1) internal scattering among monomers in the soot aggregate, (2) the correlation of soot primary-particle diameter with aggregate size, (3) quantum confinement effects, or (4) a size-dependent degree of soot graphitization. Here, we report a size-dependent MAC for ex-situ soot sampled from two commercially available diffusion-flame soot generators, one aviation turbine engine, and one diesel generator. We also incorporate literature data. We show that the MAC increases with aggregate size until a plateau is reached at single particle masses between 4 and 30 fg (approximately 300-650 nm soot mobility diameter). The smallest particles may have MACs 50% to 80% smaller than the largest, depending on the source, while the largest particles have MACs within the range reported by previous measurements on polydisperse samples. Moreover, we show that models of hypotheses (1), (2), and (3) do not describe our measurement results, leaving hypothesis (4) as the only remaining candidate.