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.
Highlights
The quaternary semiconductor Cu2ZnSnS4 has received considerable attention in recent years due to its potential use as a solar absorber [1,2]
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
Summary
The quaternary semiconductor Cu2ZnSnS4 has received considerable attention in recent years due to its potential use as a solar absorber [1,2]. The possibility for using this environmentally friendly material in thermoelectric applications has emerged recently [4,5,6]. The current record for the thermoelectric figure of merit ZT = 1.6 has been achieved for Na-doped Cu2ZnSnS4 single crystals at 800 K [4], a rather promising and competitive value [7]. A critical component for determining the thermoelectric performance of a semiconducting material such as Cu2ZnSnS4 is the inherent anharmonic phonon–phonon interactions, which influence the lattice thermal conductivity. The latter is inversely proportional to ZT, such that an enhancement of ZT can be realized via the reduction in the lattice thermal conductivity contribution. The understanding of these anharmonic processes may lead to the optimization of the respective thermoelectric efficiency
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