Monte Carlo simulations of measured electron energy-loss spectra of diamond and graphite: role of dielectric-response models

TL;DR

This study compares Monte Carlo simulations of electron energy-loss spectra in diamond and graphite using different dielectric response models, highlighting the importance of ab initio methods for accurate material characterization.

Contribution

It demonstrates that ab initio dielectric functions improve agreement with experimental spectra over semi-classical models, especially for insulators and semiconductors at finite momentum transfers.

Findings

Ab initio dielectric functions match experimental spectra better.

Semi-classical models are less accurate beyond the optical limit.

Energy loss function behavior significantly affects inelastic mean free path and stopping power.

Abstract

In this work we compare Monte Carlo (MC) simulations of electron transport properties with reflection electron energy loss measurements in diamond and graphite films. We assess the impact of different approximations of the dielectric response on the observables of interest for the characterization of carbon-based materials. We calculate the frequency-dependent dielectric response and energy loss function of these materials in two ways: a full ab initio approach, in which we carry out time-dependent density functional simulations in linear response for different momentum transfers, and a semi-classical model, based on the Drude--Lorentz extension to finite momenta of the optical dielectric function. Ab initio calculated dielectric functions lead to a better agreement with electron energy loss measured spectra with respect the widely used Drude-Lorentz model. This discrepancy is particularly evident for insulators and semiconductors beyond the optical limit ($\mathbf{q} \neq 0$), where single particle excitations become relevant. Furthermore, we show that the behaviour of the energy loss function at different accuracy levels has a dramatic effect on other physical observables, such as the inelastic mean free path and the stopping power in the low energy regime ($< 100$ eV) and thus on the accuracy of MC simulations.