Strain Effect on Rashba Splitting and Phonon Scattering to Improve Thermoelectric Performance of 2D Heterobilayer MoTe$_{2}$/PtS$_{2}$

Abstract: Rashba spin-orbit coupling significantly modifies the electronic band structure in two-dimensional (2D) van der Waals (vdW) heterobilayers, which may enhance their thermoelectric (TE) properties. In this study, we use first-principles calculations and Boltzmann transport theory to explore the strain effect on the TE performance of the 2D vdW heterobilayer MoTe${2}$/PtS${2}$. A strong Rashba spin-splitting is observed in the valence band, resulting in an increase in the Seebeck coefficient for p-type. The lattice thermal conductivity of MoTe${2}$/PtS${2}$ is remarkably low about of 0.6 Wm$^{-1}$K$^{-1}$ at $T = 300$ K due to large anharmonic scattering. Furthermore, biaxial strain enhances the power factor (PF) by introducing band convergence. At a strain of 2\%, the optimal PF for the n-type material reaches 170 $\mu$W/cmK$^{2}$, indicating approximately 84.78\% increase compared to the unstrained state (92 $\mu$W/cmK$^{2}$). Given the low lattice thermal conductivity, the optimized figure of merit $ZT$ achieves up to 0.88 at 900 K for n-type. Our findings indicate that MoTe${2}$/PtS${2}$ is a highly promising candidate for 2D heterobilayer TE materials, owing to its strong Rashba splitting and significant anharmonicity.