File Name : figs1.tif Caption : wdx line scans averaged to proof the homogeneity of different czgse grains in a specific sample. File Name : figs2.tif Caption : refined xrd pattern of an off-stoichiometric g-f-type czgse sample containing znse as secondary phase. File Name : figs3.tif Caption : unit cell volumes of off-stoichiometric czgse powder samples versus cu/(zn+ge). File Name : figs4.tif Caption : refined neutron diffraction pattern of an off-stoichiometric, single-phase f-i-type czgse sample. File Name : figs5.tif Caption : total point defect concentration in dependence of the cation ratios. File Name : figs6.tif Caption : evolution of the stoichiometric coefficients of cu, zn, and ge with changing cu/(zn+ge). File Name : figs7.tif Caption : tauc plot of the diffuse reflectance data to deduce bandgap energies of czgse with different compositions.