Prediction of enhanced thermoelectric performance in two-dimensional black phosphorus nanosheets

Abstract Because of the unique layered structure, black phosphorus (BP) provides a possibility of relatively independent control in electrical and thermal conductivity for thermoelectrical applications. It is therefore of great interest to realize high-performance BP-based thermoelectrics as flexible non-toxic and ultralight devices in spite of the low energy conversion efficiency and structural instability of the bulk BP. In this work, we systematically study the thermoelectric properties for the two-dimensional BP from mono-layer up to quad-layer by first-principles calculations and Boltzmann transport theory. It can be concluded from the calculations that the thermoelectric performance of BP nanosheets can be effectively optimized by tuning the layer thickness. We reveal that the maximum ZT values at 300 and 500 K can reach up to 0.45 and 0.90 in p-type bi-layer BP along armchair direction, respectively, around 5 times higher than that of the bulk at room temperature. The high performance in bi-layer BP is mainly attributed to its highly anisotropic and degenerate carrier pockets. Accordingly, we further propose that the formation of BP/h-BN heterostructure can enhance ZT up to 1.2 at 500 K, which facilitates the real application of thin BP for flexible and eco-friendly thermoelectrics.