Atmospheric aerosols play an important part in the Earth's energy budget by scattering and absorbing incoming solar and outgoing terrestrial radiation. To quantify the effective radiative forcing due to aerosol-radiation interactions, researchers must obtain a detailed understanding of the spectrally dependent intensive and extensive optical properties of different aerosol types. Our new approach retrieves the optical coefficients and the single-scattering albedo of the total aerosol population over 300 to 650 nm wavelength, using extinction measurements from a broadband cavity-enhanced spectrometer at 315 to 345 nm and 390 to 420 nm, extinction and absorption measurements at 404 nm from a photoacoustic cell coupled to a cavity ring-down spectrometer, and scattering measurements from a three-wavelength integrating nephelometer. By combining these measurements with aerosol size distribution data, we retrieved the time-and wavelength-dependent effective complex refractive index of the aerosols. Retrieval simulations and laboratory measurements of brown carbon proxies showed low absolute errors and good agreement with expected and reported values. Finally, we implemented this new broadband method to achieve continuous spectral-and time-dependent monitoring of ambient aerosol population, including, for the first time, extinction measurements using cavity-enhanced spectrometry in the 315 to 345 nm UV range, in which significant light absorption may occur.