This study provides molecular insights into the light absorption properties of biomass burning (BB) brown carbon (BrC) through the chemical characterization of tar condensates generated from heated wood pellets at oxidative and pyrolysis conditions. Both liquid tar condensates separated into "darker oily" and "lighter aqueous" immiscible phases. The molecular composition of these samples was investigated using reversed-phase liquid chromatography coupled with a photodiode array detector and a high-resolution mass spectrometer. The results revealed two sets of BrC chromophores: (1) common to all four samples and (2) specific to the "oily" fractions. The common BrC chromophores consist of polar, monoaromatic species. The oil-specific BrC chromophores include less-polar and nonpolar polyaromatic compounds. The most-light-absorbing pyrolysis oily phase (PO) was aerosolized and size-separated using a cascade impactor to compare the composition and optical properties of the bulk versus the aerosolized BrC. The mass absorption coefficient (MAC300-500 nm) of aerosolized PO increased compared to that of the bulk, due to gas-phase partitioning of more volatile and less absorbing chromophores. The optical properties of the aerosolized PO were consistent with previously reported ambient BB BrC measurements. These results suggest the darkening of atmospheric BrC following non-reactive evaporation that transforms the optical properties and composition of aged BrC aerosols.