Transition-metal dichalcogenide MoSe2, two-dimensional
(2D) materials with a hexagonal lattice, are promising candidates
for direct energy conversion due to their excellent thermoelectric
properties. Twist and interlayer van der Waals (vdW) force modulation
have attracted considerable attention as effective approaches to reduce
thermal conductivity and hence improve thermoelectric performance.
However, the underlying mechanism analysis of the twist-angle-dependent
thermal conductivity remains incomprehensive, and there has been few
research on the joint effects of twist and interlayer coupling strength.
In this study, the heat transfer of monolayer and bilayer MoSe2 was systematically investigated by nonequilibrium molecular
dynamics and density functional theory. The results indicated that
in the presence of twist angles, the calculated thermal conductivities
of monolayer and bilayer MoSe2 both exhibit “W-shaped”,
achieving a maximum decrease of 56.6%. For bilayer MoSe2, the thermal conductivities corresponding to different twist angles
all decrease monotonically with increasing vdW interaction strength,
and structures with twist angles larger than 5° show greater
sensitivity to the variation of vdW forces. Twist induces the increase
of the lattice constant of bilayer MoSe2, leading to the
reduction of the Brillouin zone and the emergence of folded phonon
modes. The characteristics that dominate heat transfer, heat capacity,
phonon group velocity, and phonon lifetime, display divergent tendencies,
with heat capacity increasing with lattice constant while phonon group
velocity and phonon lifetime do the reverse. This would provide an
effective guide to further elucidate the thermal characteristics and
to enhance the efficiency in thermoelectric energy conversion applications
of 2D nanothermoelectric materials.