<i>Penta</i>‐PdPSe: A New 2D Pentagonal Material with Highly In‐Plane Optical, Electronic, and Optoelectronic Anisotropy

Due to their low-symmetry lattice characteristics and intrinsic in-plane anisotropy, 2D pentagonal materials, a new class of 2D materials composed entirely of pentagonal atomic rings, are attracting increasing research attention. However, the existence of these 2D materials has not been proven experimentally until the recent discovery of PdSe₂ . Herein, penta-PdPSe, a new 2D pentagonal material with a novel low-symmetry puckered pentagonal structure, is introduced to the 2D family. Interestingly, a peculiar polyanion of [SePPSe]^4- is discovered in this material, which is the biggest polyanion in 2D materials yet discovered. Strong intrinsic in-plane anisotropic behavior endows penta-PdPSe with highly anisotropic optical, electronic, and optoelectronic properties. Impressively, few-layer penta-PdPSe-based phototransistor not only achieves excellent electronic performances, a moderate electron mobility of 21.37 cm² V^-1 s^-1 and a high on/off ratio of up to 10⁸ , but it also has a high photoresponsivity of ≈5.07 × 10³ A W^-1 at 635 nm, which is ascribed to the photogating effect. More importantly, penta-PdPSe also exhibits a large anisotropic conductance (σ_max /σ_max = 3.85) and responsivity (R_max /R_min = 6.17 at 808 nm), superior to most 2D anisotropic materials. These findings make penta-PdPSe an ideal material for the design of next-generation anisotropic devices.