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This overview article provides insight into how to apply Raman spectroscopy in combination with a confocal, optical microscope setup on polycrystalline material systems, in order to obtain quantitative information on phase distribution, grain sizes, crystal orientations and microstrain. Although the present work uses Cu(In,Ga)(S,Se)₂ absorber layers in corresponding thin-film solar cells as a model system to demonstrate the capabilities of Raman microspectroscopy, the approaches discussed may be applied to any organic or inorganic, polycrystalline materials system.