Results of investigations of Cr overlayers on Fe surfaces by magnetic linear dichroism in the angular distribution and spin-resolved core level photoemission are analyzed within the framework of a new model approach. It includes a special algorithm for modelling epitaxial growth of overlayers with different roughness together with self-consistent calculations of the magnetic moment distribution within a Periodic Anderson Model. On this basis the value of the magnetic dichroism and the spin polarization in photoemission as functions of the Cr coverage can be modelled also for rough surfaces. The comparison of experimental spectra and theoretical coverage dependencies obtained for the different surface roughnesses leads to conclusions about the microscopic structure of Cr overlayers.