In this paper, we present some results of mathematical modeling of the conditions for solving the inverse problem on determination of optical parameters of atmospheric layers from the data of measurements of hemispherical spectral flux of radiation at different levels in the atmosphere. The iteration process used in the paper for solving the inverse problem is shown to be convergent even for rather rough zero-o–rder approximation. It is also shown that the proposed algorithm can be successfully used for processing of the data of real experiments.