Examining real-time TDDFT non-equilibrium simulations for the calculation of electronic stopping power

Abstract

In ion irradiation processes, electronic stopping power describes the energy transfer rate from the irradiating ion to the target material's electrons. Due to the scarcity and significant uncertainties in experimental electronic stopping power data for materials beyond simple solids, there has been growing interest in the use of first-principles theory for calculating electronic stopping power. In recent years, advances in high-performance computing have opened the door to fully first-principles nonequilibrium simulations based on real-time time-dependent density functional theory (RT-TDDFT). While it has been demonstrated that the RT-TDDFT approach is capable of predicting electronic stopping power for a wide range of condensed matter systems, there has yet to be an exhaustive examination of the physical and numerical approximations involved and their effects on the calculated stopping power. We discuss the results of such a study for crystalline silicon with protons as irradiating ions. We examine the influences of key approximations in RT-TDDFT nonequilibrium simulations on the calculated electronic stopping power, including approximations related to basis sets, finite size effects, exchange-correlation approximation, pseudopotentials, and more. Finally, we propose a simple and efficient correction scheme to account for the contribution from core-electron excitations to the stopping power, as it was found to be significant for large proton velocities.

arXiv comment10 pages, 10 figures, and supplemental material

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• Electron energy loss spectroscopy of bulk gold with ultrasoft pseudopotentials and the Liouville-Lanczos method
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• Electronic stopping and proton dynamics in InP, GaP, and In${}_{0.5}$Ga${}_{0.5}$P from first principles
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• Ion Type Dependence of DNA Electronic Excitation in Water under Proton, alpha-particle, and Carbon Ion Irradiation: A First-Principles Simulation Study
• Floquet theory for the electronic stopping of projectiles in solids
• Assessing the electronic excitation spectra of chromium, palladium and samarium from their stopping quantities
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• Valence and core excitons in solids from velocity-gauge real-time TDDFT with range-separated hybrid functionals: An LCAO approach