A statistical technique is developed for inferring the optimum values of the ground albedo and the effective imaginary term of the complex refractive index of atmospheric particulates. The procedure compares measurements of the ratio of the hemispheric diffuse to directly transmitted solar flux density at the earth's surface with radiative transfer computations of the same as suggested by Herman et al. (1975). A detailed study is presented which shows the extent to which the ratio of diffuse to direct solar radiation is sensitive to many of the radiative transfer parameters. Results indicate that the optical depth and size distribution of atmospheric aerosol particles are the two parameters which uniquely specify the radiation field to the point where ground albedo and index of absorption can be inferred. Varying the real part of the complex refractive index of atmospheric particulates as well as their vertical distribution is found to have a negligible effect on the diffuse-direct ratio. The statistical procedure utilizes a semi-analytic gradient search method from least-squares theory and includes a detailed error analysis.