Experimental and computational approaches to study the high temperature thermoelectric properties of novel topological semimetal CoSi

TL;DR

This study combines experimental measurements and DFT calculations to analyze the thermoelectric properties of CoSi from 300 to 800 K, revealing temperature-dependent behavior of Seebeck coefficient, conductivity, and thermal conductivity.

Contribution

It provides a comprehensive experimental and theoretical analysis of CoSi's thermoelectric properties at high temperatures, highlighting the role of electronic band structure and charge carriers.

Findings

Seebeck coefficient shows non-monotonic temperature dependence.

Electrical conductivity decreases with temperature, thermal conductivity increases.

DFT-based models accurately estimate transport coefficients at high temperatures.

Abstract

Here, we study the thermoelectric properties of topological semimetal CoSi in the temperature range $300-800$ K by using combined experimental and density functional theory (DFT) based methods. CoSi is synthesized using arc melting technique and the Rietveld refinement gives the lattice parameters of a = b = c = 4.445 {\AA}. The measured values of Seebeck coefficient (S) shows the non-monotonic behaviour in the studied temperature range with the value of $\sim-$81 $\mu$V/K at room temperature. The $|S|$ first increases till 560 K ($\sim-$93 $\mu$V/K) and then decreases up to 800 K ($\sim-$84 $\mu$V/K) indicating the dominating n-type behaviour in the full temperature range. The electrical conductivity, $\sigma$ (thermal conductivity, $\kappa$) shows the monotonic decreasing (increasing) behaviour with the values of $\sim$5.2$\times 10^{5}$ (12.1 W/m-K) and $\sim$3.6$\times 10^{5}$ (14.2 W/m-K) $\Omega^{-1}m^{-1}$ at 300 K and 800 K, respectively. The $\kappa$ exhibits the temperature dependency as, $\kappa \propto T^{0.16}$. The DFT based Boltzmann transport theory is used to understand these behaviour. The multi-band electron and hole pockets appear to be mainly responsible for deciding the temperature dependent transport behaviour. Specifically, the decrease in the $|S|$ above 560 K and change in the slope of $\sigma$ around 450 K are due to the contribution of thermally generated charge carriers from the hole pockets. The temperature dependent relaxation time is computed which shows temperature dependency of $1/T^{0.35}$. Present study suggests that electronic band-structure obtained from DFT provides reasonably good estimate of the transport coefficients of CoSi in the high temperature region of $300-800$ K.