All-electron full-potential implementation of real-time TDDFT in exciting

Abstract

Abstract Linearized augmented planewaves combined with local-orbitals (LAPW + lo) are arguably the most precise basis set to represent Kohn–Sham states. When employed within real-time time-dependent density functional theory (RT-TDDFT), they promise ultimate precision achievable for exploring the evolution of electronic excitations. In this work, we present an implementation of RT-TDDFT in the full-potential LAPW + lo code exciting. We benchmark our results against those obtained by linear-response TDDFT with exciting and by RT-TDDFT calculations with the Octopus code, finding a satisfactory level of agreement. To illustrate possible applications of our implementation, we have chosen three examples: the dynamic behavior of excitations in MoS2 induced by a laser pulse, the third harmonic generation in silicon, and a pump–probe experiment in diamond. Besides, we provide further benchmark results.