A First-Principles Study on Electronic, Thermodynamic, and Dielectric Properties of Monolayer Ca(OH)2 and Mg(OH)2

Abstract

We perform first-principles calculations to explore electronic, thermodynamic, and dielectric properties of two-dimensional (2D) layered, alkaline-earth hydroxides Ca(OH) 2 and Mg(OH) 2 .We calculate the lattice parameters, exfoliation energies, and phonon spectra of monolayers and also investigate the thermal properties of these monolayers such as Helmholtz free energy, heat capacity at constant volume, and entropy as a function of temperature. We employ Density Functional Perturbation Theory (DFPT) to calculate the in-plane and out-of-plane static dielectric constant of the bulk and monolayer samples. We compute the bandgap and electron affinity values using the HSE06 functional and estimate the leakage current density of transistors with monolayer Ca(OH) 2 and Mg(OH) 2 as dielectrics when combined with HfS 2 and WS 2 , respectively. Our results show that bilayer Mg(OH) 2 (EOT ∼ 0.60 nm) with a lower solubility in water, offers higher out-of-plane dielectric constants and lower leakage currents than bilayer Ca(OH) 2 (EOT ∼ 0.56 nm). Additionally, the out-of-plane dielectric constant, leakage current, and EOT of Mg(OH) 2 outperform bilayer h-BN. We verify the applicability of Anderson's rule, and conclude that bilayers of Ca(OH) 2 and Mg(OH) 2 respectively paired with lattice-matched