In this study a photoacoustic spectrometer (PA), a laser-induced incandescence instrument system (LII) and an Aerosol Mass Spectrometer were operated in parallel for in-situ measurements of black carbon (BC) light absorption enhancement. Results of a thermodenuder experiment using ambient particles in Toronto are presented first to show that LII measurements of BC are not influenced by the presence of non-refractory material thus providing true atmospheric BC mass concentrations. In contrast, the PA response is enhanced when the non-refractory material is internally mixed with the BC particles. Through concurrent measurements using the LII and PA the specific absorption cross-section (SAC) can be quantified with high time resolution (1 min). Comparisons of ambient PA and LII measurements from four different locations (suburban Toronto; a street canyon with diesel bus traffic in Ottawa; adjacent to a commuter highway in Ottawa and; regional background air in and around Windsor, Ontario), show that different impacts from emission sources and/or atmospheric processes result in different particle light absorption enhancements and hence variations in the SAC. The diversity of measurements obtained, including those with the thermodenuder, demonstrated that it is possible to identify measurements where the presence of externally-mixed non-refractory particles obscures direct observation of the effect of coating material on the SAC, thus allowing this effect to be measured with more confidence. Depending upon the time and location of measurement (urban, rural, close to and within a lake breeze frontal zone), 30 min average SAC varies between 9 ± 2 and 43 ± 4 m2 g−1. Causes of this variation, which were determined through the use of meteorological and gaseous measurements (CO, SO2, O3), include the particle emission source, airmass source region, the degree of atmospheric processing. Observations from this study also show that the active surface area of the BC aggregate, which is measured by the LII as the PPS, is an important parameter for inferring the degree of particle collapse of a BC particle. In addition, PPS could be a useful measurement for indicating the importance of recently emitted BC (e.g. from gasoline or diesel engines) relative to the total measured BC in the atmosphere.