Anharmonic Effects in Ordered Kesterite-Type Cu2ZnSnS4

Abstract

We performed an in-depth investigation and analysis of the effect of temperature on the Raman-active A-modes of bulk kesterite-type Cu2ZnSnS4 within the 300–460 K temperature range. We acquired the individual contributions to each Raman mode, namely, the thermal expansion and anharmonic interactions terms responsible for the Raman shift and broadening with temperature. Our results indicate that the Raman shift with temperature is dominated by the thermal expansion term, whereas the broadening is mainly governed by three-phonon damping processes in this material. Considering relevant results from the literature, it appears that dimensionality is a key factor in regulating the dominant phonon decay mechanism.

Thermal conductivity and phonon anharmonicity of chemical vapor transport grown and mineral–FeS2single crystals: An optothermal Raman study

“…The model proposed by Klemens [ 33 ] and extended by Balkanski et al [ 32 ] (Balkanski–Klemens) together with thermal expansion contribution (or quasiharmonicity) allows us to determine the scattering mechanism of the studied Raman active mode. Unconstrained fitting of the model may converge to positive anharmonic constants (referred as phonon upconversion [ 37,38 ] ), due to the possibility of more than one local minima within the parameter space. In order to examine this, a full temperature‐dependent parameter scan of the Balkanski–Klemens model is performed for both A g and E g modes, which is shown in Figures S5 and S6 and Table S2.…”