van Thanh, VuongVuongvan ThanhTUAN HUNG NGUYEN2025-09-242025-09-242025https://www.scopus.com/inward/record.uri?eid=2-s2.0-105009515324&doi=10.1021%2Facsaem.5c01254&partnerID=40&md5=d62a2e6aa67375f9b39d40abfc5668dbhttps://scholars.lib.ntu.edu.tw/handle/123456789/732280Rashba 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 effect of strain on the TE performance of 2D vdW heterobilayer MoTe<inf>2</inf>/PtS<inf>2</inf>. A strong Rashba spin-splitting is observed in the valence band, resulting in an increase in the Seebeck coefficient for the p-type. The lattice thermal conductivity of MoTe<inf>2</inf>/PtS<inf>2</inf> is remarkably low, about 0.6 W m-1 K-1 at 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 μW/cmK2, indicating an approximately 84.78% increase compared to the unstrained state (92 μW/cmK2). Given the low lattice thermal conductivity, the optimized figure of merit ZT achieves up to 0.88 at 900 K for the n-type. Our findings indicate that MoTe<inf>2</inf>/PtS<inf>2</inf> is a highly promising candidate for 2D heterobilayer TE materials owing to its strong Rashba splitting and significant anharmonicity.2d Van Der Waals Heterobilayer Mote2/pts2AnharmonicityBand ConvergenceDensity Functional TheoryRashba Spin?orbit CouplingThermoelectricityCrystal LatticesMolybdenum CompoundsStatistical MechanicsTellurium CompoundsThermal ConductivityThermoelectricityAnharmonicitiesBand ConvergenceDensity-functional-theoryLattice Thermal ConductivityRashba Spin-orbit CouplingSplittingsThermoelectric PerformanceTwo-dimensionalTwo-dimensional Van Der Waal Heterobilayer Mote2/pts2Van Der WaalDensity Functional Theoryjournal article10.1021/acsaem.5c012542-s2.0-105009515324