Group III (In/Ga)-V (P/As)-VI (S/Se) Monolayers: A New Class of Auxetic Semiconductors with Highly Anisotropic Electronic/Optical/Mechanical/Thermal Properties

We present a theoretical design of a class of 2D semiconducting materials, namely, group III (In/Ga)-V (P/As)-VI (S/Se) monolayers, whose global-minimum structures are predicted based on the particle swarm optimization method. Electronic structure calculations suggest that all group III-V-VI monolayers exhibit quasi-direct semiconducting characteristics with desirable band gaps ranging from 1.76 to 2.86 eV (HSE06 functional). Moreover, most group III-V-VI monolayers possess highly anisotropic carrier mobilities with large anisotropic ratios (3.4-6 for electrons, 2.2-25 for holes). G₀W₀+BSE calculations suggest that these monolayers show high optical anisotropy and relatively large exciton binding energies (0.33-0.75 eV), comparable to that (0.5 eV) of MoS₂ monolayer. In particular, the GaPS monolayer manifests strikingly anisotropic I-V curves with a large ON/OFF ratio of ∼10⁵ (10⁶ for the GaPS bilayer) and anisotropic lattice thermal conductivity. Furthermore, the GaPS monolayer is predicted to exhibit both in-plane and out-of-plane negative Poisson ratios (NPRs) and prominent anisotropic Young moduli. © 2024 American Chemical Society.