Abstract
Recently, the application of two-dimensional (2D) piezoelectric materials has been seriously hindered because most of them possess only in-plane piezoelectricity but lack out-of-plane piezoelectricity. In this work, using first-principles calculation, by atomic substitution of penta-graphene (PG) with tiny out-of-plane piezoelectricity, we design and predict stable 2D X-PG (X = Si or Ge) semiconductors with excellent in-plane and out-of-plane piezoelectricity and extremely high in-plane hole mobility. Among them, Ge-PG exhibits better performance in all aspects with an in-plane strain piezoelectric coefficient d(11) = 8.43 pm/V, an out-of-plane strain piezoelectric coefficient d(33) = -3.63 pm/V, and in-plane hole mobility μ(h) = 57.33 × 10(3) cm(2) V(-1) s(-1). By doping Si and Ge atoms, the negative Poisson's ratio of PG approaches zero and reaches a positive value, which is due to the gradual weakening of the structure's mechanical strength. The bandgaps of Si-PG (0.78 eV) and Ge-PG (0.89 eV) are much smaller than that of PG (2.20 eV), by 2.82 and 2.47 times, respectively. This indicates that the substitution of X atoms can regulate the bandgap of PG. Importantly, the physical mechanism of the out-of-plane piezoelectricity of these monolayers is revealed. The super-dipole-moment effect proposed in the previous work is proved to exist in PG and X-PG, i.e., it is proved that their out-of-plane piezoelectric stress coefficient e(33) increases with the super-dipole-moment. The e(33)-induced polarization direction is also consistent with the super-dipole-moment direction. X-PG is predicted to have prominent potential for nanodevices applied as electromechanical coupling systems: wearable, ultra-thin devices; high-speed electronic transmission devices; and so on.