“…Over the years of implementation of the combinatorial approach for the research of thin films, a variety of different techniques have been employed to provide the most complete analysis of graded samples. In the case of thin‐film chalcogenides PV technologies, these have been mainly limited to some conventional techniques that provide information about the main physicochemical properties of these materials, including X‐ray fluorescence (XRF), [ 73,75,84,94 ] energy‐dispersive X‐ray spectroscopy (EDS), [ 66,74,86,97 ] X‐ray diffraction (XRD), [ 73,78,81,94 ] optical spectroscopy, [ 78,84,97,98 ] and photoluminescence (PL) spectroscopy (see Figure ). [ 72,81,86,99 ] In the last years strong attention has also been given to Raman spectroscopy, [ 73,74,86,95 ] which has shown high potential for the detection and control of secondary phase formation, crystalline quality, structural/compositional polymorphs, etc.…”