Ultralow thermal conductivity of W-Janus bilayers (WXY: X, Y = S, Se, and Te) for thermoelectric devices

Abstract

Lattice thermal conductivity (κ) in tungsten dichalcogenide Janus (WXY, where X, Y = S, Se, and Te) monolayers and heterostructures (HSs) have been investigated using ab initio DFT simulations. Tungsten-based Janus monolayers show semiconducting behavior with the bandgap in the semiconducting range for WSSe (1.70 eV), WSTe (1.26 eV), and WSeTe (1.34 eV). When Janus monolayers are stacked to form HSs with weak van der Waals (vdW) interactions, the bandgap reduces to 0.19 eV, 0.40 eV, and 0.24 eV, respectively, for WSeTe/WSTe, WSSe/WSTe, and WSSe/WSeTe HSs. Thermal vibrational characteristics of Janus monolayers are modified when these are stacked in 2D HSs with the introduction of interlayer hybrid phonon modes. Large longitudinal-transverse optical (LO-TO) splitting is noticed at the Brillouin zone-center (Γ-point): 135 cm⁻¹, 140 cm⁻¹, and 150 cm⁻¹ for WSeTe/WSTe, WSSe/WSeTe and WSSe/WSTe HSs, respectively. Thermal conductivity calculations show ultra-low κ values for WSeTe/WSTe (0.01 W m⁻¹ K⁻¹), WSSe/WSTe (0.02 W m⁻¹ K⁻¹) and WSSe/WSeTe HS (0.004 W m⁻¹ K⁻¹) at 300 K. The results can be attributed to the hybrid phonon modes with frequencies very close to acoustic modes at the gamma point, low Debye temperature (θ_D) and specific heat capacity. Our results highlight the possible applications of these HSs in designing thermoelectric interfaces at the nanoscale.