Bilayer MSe 2 (M = Zr, Hf) as promising two-dimensional thermoelectric materials: a first-principles study.

Motivated by the experimental synthesis of two-dimensional MSe 2 (M = Zr, Hf) thin films, we set out to investigate the electronic, thermal, and thermoelectric transport properties of 1T-phase MSe 2 (M = Zr, Hf) bilayers on the basis of first-principles calculations and Boltzmann transport theory. Both bilayer ZrSe 2 and HfSe 2 are indirect band gap semiconductors possessing degenerate conduction bands and stair-like-shaped DOS, which provide a high n-doped power factor. In combination with the low lattice thermal conductivity that originated from the low phonon frequency of acoustic modes and the coupling of acoustic modes with optical modes, the maximum figure of merits ZT at room temperature for n-type doping are predicted as 1.84 and 3.83 for ZrSe 2 and HfSe 2 bilayers, respectively. Our results suggest that bilayer conformation of ZrSe 2 and HfSe 2 are promising thermoelectric materials with superior performance to their bulk counterparts.