Enhanced Thermoelectric Performance in Black Phosphorene via Tunable Interlayer Twist

Twist-angle two-dimensional (2D) systems are attractive in their exotic and tunable properties by the formation of the moiré superlattices, allowing easy access to manipulating intrinsic electrical and thermal properties. Here, the angle-dependent thermoelectric properties of twisted bilayer black phosphorene (tbBP) by first-principles calculations are reported. The simulations show that significantly enhanced Seebeck coefficient and power factor can be achieved in p-type tbBP due to merging of the multi-valley electronic states and flat moiré bands. Moreover, the twisted layers bring in a strong anharmonic phonon scattering and thus very low lattice thermal conductivity of 4.51 W m^-1  K^-1 at 300 K. Consequently, a maximal ZT value can be achieved in p-type 10.11° tbBP along the armchair direction up to 0.57 and 1.06 at 300 and 500 K, respectively. The room-temperature ZT value along the zigzag direction is also significantly increased by almost 40 times compared to pristine BP when the twist angle is close to 70.68°. This work demonstrates a platform to manipulate thermoelectric performance in 2D materials by creating moiré patterns, leading tbBP as a promising eco-friendly candidate for thermoelectric applications.