Double Half-Heusler Alloys X$_2$Ni$_2$InSb (X= Zr/Hf) with promising Thermoelectric Performance: Role of varying structural phases

Abstract: Double half-heusler alloys are the new class of compounds which can be seen as transmuted version of two single half-heusler with higher flexibility of tuning their properties. Here, we report a detailed study of thermoelectric (TE) properties of two double half-heusler (HH) alloys X$_2$Ni$_2$InSb (X=Hf/Zr), using first-principles calculation. These alloys exhibit a rich phase diagram with the possibility of tetragonal, cubic and solid solution phase at different temperature range. As such, a comparative study of TE properties of all these phases is performed. The ordered phases show quite favorable electronic transport as compared to the disordered ones in both compounds. Lattice thermal conductivity of double HH alloys is lower than their ternary counter-part, making them most promising for TE application. Simulated band gap, obtained using hybrid functional, of ordered phases of Hf$_2$Ni$_2$InSb and Zr$_2$Ni$_2$InSb lie in the range 0.24-0.4 eV and 0.17-0.59 eV respectively, while for disordered phase, it is 0.05- 0.06 eV. Hf$_2$Ni$_2$InSb shows a reasonably high ZT value of $\sim$ 2.19, while Zr$_2$Ni$_2$InSb yields 2.46 at high temperature for n-type conduction in tetragonal phase. The ZT value for p-type conduction is also quite promising ($\sim$ 1.35 and $\sim$ 2.19 for Hf- and Zr-based compounds). In both the compounds, electronic transport (Seebeck and electrical conductivity) plays the dominant role for the high ZT-value. Keeping in mind the promising TE performance, we propose immediate attention from experimentalists to synthesize and cross validate our findings for these new candidate materials.