Monolayer SnP3: an excellent p-type thermoelectric material.

Monolayer SnP3 is a novel two-dimensional (2D) semiconductor material with high carrier mobility and large optical absorption coefficient, implying its potential applications in the photovoltaic and thermoelectric (TE) fields. Herein, we report on the TE properties of monolayer SnP3 utilizing first principles density functional theory (DFT) together with semiclassical Boltzmann transport theory. Results indicate that it exhibits a low lattice thermal conductivity of ∼4.97 W m-1 K-1 at room temperature, mainly originating from its small average acoustic group velocity (∼1.18 km s-1), large Grüneisen parameters (∼7.09), strong dipole-dipole interactions, and strong phonon-phonon scattering. A large in-plane charge transfer is observed, which results in a non-ignorable bipolar effect on the lattice thermal conductivity. The exhibited mixed mode between in-plane and out-of-plane vibrations enhances the complexity of the phonon phase space, which enhances the possibility of phonon scattering processes and results in suppression of thermal conductivity. A highly twofold degeneracy appearing at the K point gives a high Seebeck coefficient. Our calculated figure of merit (ZT) for optimal p-type doping at 500 K can approach 3.46 along the armchair direction, which is better than the theoretical value of 1.94 reported in the well-known TE material SnSe. Our studies here shed light on monolayer SnP3 in use as a TE material and supply insights to further optimize the TE properties in similar systems.