The problem of simultaneous physical retrieval of surface emissivity, skin temperature, and temperature, water-vapor, and ozone atmospheric profiles from high-spectral-resolution observations in the infrared is formulated according to an inverse problem with multiple regularization parameters. A methodology has been set up, which seeks an effective solution to the inverse problem in a generalized L-curve criterion framework. The a priori information for the surface emissivity is obtained on the basis of laboratory data alone, and that for the atmospheric parameters by climatology or weather forecasts. To ensure that we deal with a problem of fewer unknowns than observations, the dimensionality of the emissivity is reduced through expansion in Fourier series. The main objective of this study is to demonstrate the simultaneous retrieval of emissivity, skin temperature, and atmospheric parameters with a two-dimensional L-curve criterion. The procedure has been demonstrated with spectra observed from the infrared atmospheric sounder interferometer, flying onboard the European Meteorological Operational satellite. To check the quality and reliability of the methodology, we have used spectra recorded over regions characterized by known or stable emissivity. These include sea surface, for which effective emissivity models are known, and arid lands (Sahara and Namib Deserts) that are known to exhibit the characteristic spectral signature of quartz-rich sand.