Measurements of aerosol optical properties over the atmospheric column (aerosol optical thickness, spectral angular sky radiance (sky brightness), and downwelling hemispheric flux) have been used to derive climate-relevant aerosol parameters such as the phase function, the broadband single-scattering albedo, and the refractive index. These parameters are needed to estimate the direct short-wave radiative forcing by aerosols and to validate aerosol models in the satellite retrieval algorithms. Values of the broadband single-scattering albedo obtained in this study range between ω0 = 0.98 (marine aerosols) and 0.90 (continental pollution aerosols). The columnar ambient broadband refractive index is found to be m = 1.39 ¿ 0.044 - i (<0.003) for marine conditions and m = 1.48 ¿ 0.058 - i (0.01 ¿ 0.003) for polluted continental aerosols. Nonsphericity is shown to be important in the case of marine aerosols. Moreover, aerosol nonsphericity gives an additional contribution to the negative short-wave radiative forcing of marine aerosols under clear-sky conditions, which can be estimated as being 30 up to 50% of the radiative forcing estimated for spherical marine aerosols. In the case of continental polluted aerosols the optical properties can be represented by spherical particles, and no additional shape effect has to be considered. However, the aerosol absorption leads to an increase of about 40% of the radiative forcing estimated for nonabsorbing aerosol of the same size distribution.