Analysis on the temperature-dependent Raman spectra measured between 27–450 °C range in relation to various Ge compositional ratios of Cu2Sn1−xGexS3 thin-film alloys, which were prepared by closed-tube sulfurization technique, was carried out in detail. By XRD and Raman analyses, linear transformation of the lattice parameters for Cu2Sn1−xGexS3 thin-film alloys with respect to the Ge composition was confirmed to be obeying the Vegard’s law. By AC Hall effect measurement, reducing of carrier mobility was observed in the Cu2Sn1−xGexS3 thin-film alloys with higher Ge content. By the temperature dependent Raman spectroscopy analysis, it is observed that the red shifting of Raman vibration energy due to the thermal expansion is resembled to that of the temperature dependency of energy bandgap of semiconductors. Anisotropic thermal dilatation behavior was observed in the Cu2Sn1−xGexS3 thin-film alloy independent of its Ge composition.

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