Strong Interlayer Coupling In Two-Dimensional Pbse With High Thermoelectric Performance

It was generally believed that weak van der Waals interactions exist between neighboring layers in the two-dimensional group-IV chalcogenides. Using PbSe as a prototypal example, we find additional strong coupling between the Pb-Pb layers, as evidenced by detailed analysis of the differential charge density plot. The coupling is covalent-like and can be fine-tuned to obviously reduce the phonon thermal conductivity but slightly change the electronic transport of PbSe layer. As a consequence, a maximum ZT value of 2.5 can be realized at 900 K for the p-type system. Our work also offers an effective and feasible design strategy to enhance the thermoelectric performance of similar layered structures.