Rethinking the distinction between black and brown carbon

Aerosol radiative properties contribute large uncertainty to modeling of the earth's radiative budget. Black carbon (BC) aerosols originate from combustion processes and substantially contribute to warming and uncertainty - ongoing efforts are focused on reducing their anthropogenic emissions even as their emissions from biomass burning sources, such as wildfire, may increase in the future. Quantifying the radiative effect of BC is challenging, in part due to its association with other light absorbing materials including Brown carbon organic aerosol (BrC) that absorbs primarily blue and ultraviolet light while BC absorbs broadly across the visible. Conventionally BrC is thought of a low volatility spherical particles, distinguishing it from BC, which has a distinctive agglomerate morphology and is refractory at high temperatures. However, the separation of BC and BrC is often operationally defined and dependent on the measurement method. Using measurements of aerosol morphology, mass, absorption, and refractory BC mass content we were able to identify a light absorbing contribution from biomass burning aerosol that does not correspond to either BC or BrC as conventionally defined. Our measurements were collected from realistic biomass burning fires at the Missoula Fire Sciences Laboratory as part of the NOAA FIREX project (2016) and from extensive natural wildfire sampled aloft during NASA SEAC4RS field study (2013). We coin the term Dark Brown Carbon (DBrC) to describe this material, which absorbs broadly across the visible and survives thermal denuding at 250°C but does not incandesce in laser induced incandesce (LII) measurements. DBrC may be an intermediate burning stage product between polycyclic aromatic hydrocarbons (PAHs) and the mature soot. DBrC deserves further study to quantify its abundance and aging in ambient biomass burning plumes, and its relationship to tar balls. Our findings show that more than half of the light absorption in biomass burning smoke could be potentially contributed to DBC, which may provide an explanation for some of the persistent inconsistencies in measurements of BC from biomass burning by different methods.