Superior Limit of Light-Absorption Improvement in Two-Dimensional Haeckelite GaN-ZnO by Nonadiabatic Molecular Dynamics Simulation

Abstract

A weak internal electrostatic field is usually required to improve optical performance; however, this is not the case in two-dimensional haeckelite (8|4) GaN-ZnO that has physical properties that are better than those of their binary counterparts. By performing nonadiabatic molecular dynamics simulations, we ascribe the superior limit of improvement of light absorption to the convergence of the electron-hole recombination time when the thickness of the 8|4 phase exceeds a critical value, which arises from the competition between nonadiabatic coupling and quantum decoherence. We show that nonadiabatic coupling continuously becomes weaker because of the reduced nucleus velocity with an increase in thickness. We further demonstrate that the quantum decoherence is first accelerated and then decelerated because of the thickness-dependent electron-phonon coupling controlled by the peculiar in-plane A' and A″ phonon modes. Our study clarifies the issue with regard to light absorption, which provides useful guidance for improving our understanding of the optical properties in two-dimensional polar semiconductors.