Ultralow In-Plane Thermal Conductivity in 2D Magnetic Mosaic Superlattices for Enhanced Thermoelectric Performance

Lowering thermal conductivity via introducing heterointerfaces of heterophase fillings (HPFs) is a common strategy for optimizing thermoelectric performance, but it is always accompanied by deterioration of electrical conductivity. Here we report an ordered magnetic HPF system in a CoSe2–SnSe mosaic heterostructure superlattice synthesized by van der Waals confined epitaxial growth (vdWCEG), which realizes a maximized filling amount to decrease in-plane thermal conductivity of SnSe layers and maintain the intact in-plane carrier transport path. The in-plane thermal conductivity of CoSe2–SnSe superlattice reaches the lowest range among SnSe-based materials with a value of 0.27 W m–1 K–1 at 850 K, which can be attributed to abundant interfaces between CoSe2 nanocrystals and SnSe layers. Moreover, the CoSe2 nanocrystals show superparamagnetic behavior, by which the rotation of magnetic domains provides additional phonon scattering to further decrease in-plane thermal conductivity. By combination with the preserved in-plane electrical conductivity of SnSe layers, an enhanced in-plane ZT value of 0.62 is achieved at 850 K. This vdWCEG approach can also be generally applied to fabricate various other two-dimensional (2D) mosaic heterostructures, providing an avenue for artificial 2D heterostructures with desired functionalities.