Langevin dynamics/Monte Carlo simulations method for calculating nanoscale dielectric functions of materials

Abstract

We have developed a simulational methodology for calculating the nanoscale frequency-dependent complex dielectric function of a wide range of materials using a combination of Langevin dynamics and Metropolis Monte Carlo methods. The premise of such a scheme is to use the atomistic structure of materials and designate appropriate interatomic interactions as well as internal field couplings to accommodate correlated materials. We validate our model by recreating the dielectric functions of well-studied representative materials including insulator ${\text{SiO}}_{2}$ thin film that has phonon resonances in the midinfrared, and semiconductor monolayer ${\text{MoS}}_{2}$ that exhibits strong excitonic resonances in the visible frequency range. To further showcase the capability of the model in calculating nanoscale dielectric modulation of complex materials, we simulate the dielectric response of ${\text{SmNiO}}_{3}$, a correlated perovskite oxide, with respect to differing levels of hydrogenation, oxygen vacancy formation, and external fields. This is accomplished by inserting and tracking the movement of dopants at the nanoscale using Metropolis Monte Carlo methods that explicitly include interactions with each other as well as external fields. Simulated nanoscale dielectric spectra agree very well with high-resolution near-field experimental measurements based on scattering type scanning near-field microscopy. We find that this modeling scheme carries a broad utility in describing and predicting the nanoscale dielectric behavior of a broad range of materials exposed to changing local environments.