This report accounts for the occurrence of the temperature‐induced variation in the phonon properties and the spatial variation in the Raman spectra for the spray‐deposited Zn0.98Mn0.02S thin films. The study of the temperature dependence of the Raman line position, line width, and the phonon lifetime using the theoretical models that consider the thermal expansion and three‐ and four‐phonon anharmonic effects is the novelty of this work. The lifetime of the LO phonon in Zn0.98Mn0.02S thin film was as low as 0.234 ps, indicating material suitability for optical limiting applications. The intensity ratio I2LO/I1LO ranges within 0.5 at most of the (x, y) positions in the Raman mapping data, indicating the nanocrystalline nature of Zn0.98Mn0.02S.
Anharmonic properties of the longitudinal optical (LO) phonon mode of Mg-doped ZnS (Zn0.96 Mg0.04S) are investigated using the Balkanski and Klemens models on the temperature-dependent Raman spectra. The variation in the position of the Raman line, peak width, and phonon lifetime with temperature were fitted using three and four phonon decay mechanisms. The values of the anharmonic fitting parameters indicated low anharmonicity. A lifetime of ~0.17 ps at 90 K indicated a fast phonon decay. Also, the thin film is analyzed to evaluate its surface characteristics using Raman mapping that showed chemical homogeneity over a large area of the film. Further, we analyzed spatial variations of Raman line intensity, peak area, line width, and line position of LO phonon mode. Raman analysis helped in understanding the phonon-phonon interaction mechanism in Zn0.96 Mg0.04S thin films.
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