Abstract
This paper presents a study of the spectral and temperature dependences of the Ag6+x(P1−xGex)S5I (x = 0.25; 0.5; 0.75) single crystals optical properties. The refractive index (n) and extinction coefficient (k) were investigated by the spectral ellipsometry method. The spectral dependences of the n and k are characterized by the presence of anomalies in the region of the optical absorption edge. The temperature (77–300 K) behavior of the optical absorption edge was studied by optical spectroscopy. The spectral dependences of the absorption coefficient have an exponential form and obey to Urbach’s rule. The corresponding values of pseudogap Eg*, steepness parameter σ, and electron–phonon interaction parameter σ0 are calculated. An increase in temperature causes a decrease in the Eg* values and a monotonic increase in the parameter σ. The compositional dependences of EU and σ0 are characterized by a presence of extreme point for Ag6.75(P0.25Ge0.75)S5I composition. Using Dow–Redfield theory, the mechanism of electron–phonon interaction (EPI) is described. Urbach’s total energy was divided into contributions of temperature-independent (EU)X,C and temperature-dependent (EU)T types of disorder using the Einstein model. It is established that in general, the heterovalent substitution P5+ → Ge4+ leads to a weakening of the EPI in solid solutions. The exception is the Ag6.75(P0.25Ge0.75)S5I composition, for which there is a slight increase in EPI. Peculiarities of EU and σ0 changes in Ag6+x(P1−xGex)S5I solid solutions were explained using structural descriptors. It was established that decrease in the volume of [(PGe)S4] tetrahedron, for Ag6.75(P0.25Ge0.75)S5I solid solution, is one of the factors enhancing the EPI.
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All data generated or analyzed during this study are included in this published article. The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request.
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Pogodin, A.I., Pop, M.M., Shender, I.O. et al. Effect of structural site disorder on the optical properties of Ag6+x(P1−xGex)S5I solid solutions. J Mater Sci: Mater Electron 33, 21874–21889 (2022). https://doi.org/10.1007/s10854-022-08974-4
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DOI: https://doi.org/10.1007/s10854-022-08974-4