Broadband Dielectric Response of Group-II Metal Oxide Monolayers: From Ionic to Electronic Polarization

The dielectric response provides an integral description of polarization mechanisms across frequency ranges and constitutes a key physical basis for understanding ferroelectric behavior. Here, we systematically investigate the broadband dielectric response of Group-II metal oxide (BeO, MgO, CaO, ZnO, and CdO) monolayers using first-principles calculation. In the low-frequency regime, ionic polarization governs the dielectric response. A distinctive feature is the LO–TO degeneracy at the Γ point accompanied by a V-shaped nonanalytic LO phonon dispersion. d-state hybridization increases with the metal atomic number, resulting in higher Born effective charge, which works together with phonon softening, reduced mass and unit cell area to significantly strengthen the ionic dielectric contribution. The quasiparticle band gap decreases with the metal atomic number, driving redshifts of the dielectric function and wide band optical response from the deep-ultraviolet to the near-infrared. Particularly, CdO exhibits the strongest electronic polarization, with an optical dielectric constant of 2.68 and a static refractive index of 1.64. This work establishes a complete dielectric spectrum from ionic to electronic polarization, providing theoretical guidance for polarization engineering and design of two-dimensional ferroelectric devices.