This work describes a technique for the real-time determination of aerosol sources using high temporal resolution measurements to determine rapid changes in particle size distribution in accumulation and coarse modes, along with measurements of spectrally resolved light absorption measurements in the near-UV to near-IR range. The paper presents relevant real-time applications, including emergency surveillance during accidental events and the rapid identification of long-range transport of secondary particles, desert dust, and smoke. The documented approach is transferable to air quality networks involved in aerosol mass source apportionment as it relies on optical instruments commonly employed by regulatory government agencies.