Experimental and computational approaches to study the high temperature thermoelectric properties of novel...

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 ofa=b=c= 4.445 Å. The measured values of Seebeck coefficient (S) shows the non-monotonic behaviour in the studied temperature range with the value of ∼-81μV K^-1at room temperature. The |S| first increases till 560 K (∼-93μV K^-1) and then decreases up to 800 K (∼-84μV K^-1) indicating the dominating n-type behaviour in the full temperature range. The electrical conductivity,σ(thermal conductivity,κ) shows the monotonic decreasing (increasing) behaviour with the values of∼5.2×105(12.1 W m^-1 K^-1) and∼3.6×105(14.2 W m^-1 K^-1) Ω^-1 m^-1at 300 K and 800 K, respectively. Theκexhibits the temperature dependency as,κ∝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 ofσaround 450 K are due to the contribution of thermally generated charge carriers from the hole pockets. The temperature dependent relaxation time (τ) is computed by comparing the experimentalσwith calculatedσ/τand it shows temperature dependency of 1/T^0.35. Further this value ofτis used to calculate the temperature dependent electronic part of thermal conductivity (κ_e) and it gives a fairly good match with the experiment. Present study suggests that electronic band-structure obtained from DFT provides a reasonably good estimate of the transport coefficients of CoSi in the high temperature region of 300-800 K.