Spatial Variability in Black Carbon Mixing State Observed During The Multi-City NASA DISCOVER-AQ Field Campaign

Abstract:

Light absorbing carbonaceous aerosols are known to be an important climatic driver with a global radiative forcing of about half (IPCC, 2013) to two-thirds (Bond et al., 2013) that of the dominant greenhouse gas, carbon dioxide. While the mass absorption coefficient of pure black carbon (BC) is fairly well known, observational evidence suggests that BC rapidly mixes with other aerosol chemical components within hours of emission (Moffet and Prather, 2009; Moteki et al., 2007). These other components may include predominantly scattering organic, sulfate, and nitrate species, as well as light-absorbing, so-called “brown carbon” (BrC). It has been suggested that the presence of these BC-mixed components may induce mixing-state-dependent lensing effects that could potentially double the BC direct radiative forcing (Jacobson, 2001). The key to better understanding how BC-rich aerosols are distributed in the atmosphere is to examine an unbiased set of measurements covering broad spatial and temporal coverage; however, many past airborne field campaigns have specifically targeted source plumes or other scientifically-relevant emissions sources. The recent NASA DISCOVER-AQ campaign is unique in that approximately the same flight pattern was performed over a month-long period in each of four different U.S. metropolitan areas, ensuring an unbiased, or at least less biased, data set with both wide horizontal and vertical (surface to 5 km altitude) coverage.

We present a statistical analysis of BC-rich particle mixing state measured during DISCOVER-AQ by a DMT Single Particle Soot Photometer (SP2). The SP2 measures the BC mass distribution via laser incandescence, and the non-BC coating thickness is inferred from the light scattering signal of particles greater than 200 nm in diameter (Gao et al., 2007; Moteki and Kondo, 2008). The SP2-derived size distributions are compared to optical scattering size distributions measured by an UHSAS in order determine 1) the externally mixed fraction of particles containing BC across the optically-active region of the size distribution (200-1000 nm) and 2) the internally mixed volume fraction of BC relative to the total particle volume assuming spherical particles. Vertical profiles of these variables are discussed in the context of remotely sensing aerosol mixing state.