A first principles TDDFT framework for spin and time-resolved ARPES in periodic systems

TL;DR

This paper introduces a first-principles TDDFT-based framework, t-SURFFP, for simulating spin, time, and angle-resolved photoelectron spectroscopy in various low-dimensional periodic systems under arbitrary laser fields.

Contribution

The paper develops the t-SURFFP method, extending the t-SURFF approach to periodic systems for comprehensive ARPES simulations from first principles.

Findings

Successfully applied to graphene, WSe₂, and BN systems.

Capable of simulating pump-probe and various laser configurations.

Provides detailed photoelectron spectra for low-dimensional materials.

Abstract

We present a novel theoretical approach to simulate spin, time and angular-resolved photoelectron spectroscopy (ARPES) from first principles that is applicable to surfaces, thin films, few layer systems, and low-dimensional nanostructures. The method is based on a general formulation in the framework of time-dependent density functional theory (TDDFT) to describe the real time-evolution of electrons escaping from a surface under the effect of any external (arbitrary) laser field. By extending the so called t-SURFF method to periodic systems one can calculate the final photoelectron spectrum by collecting the flux of the ionization current trough an analysing surface. The resulting approach, that we named t-SURFFP, allows to describe a wide range of irradiation conditions without any assumption on the dynamics of the ionization process allowing for pump-probe simulations on an equal footing. To illustrate the wide scope of applicability of the method we present applications to graphene, mono- and bi-layer WSe$_2$, and hexagonal BN under different laser configurations.