Fast and accurate ARPES simulations from first-principles within a plane-wave framework

The role of angle-resolved photoemission spectroscopy (ARPES) has evolved beyond the conventional mapping of band structures and Fermi surfaces to a versatile tool for unveiling the topological character of electronic wave functions such as Berry curvature [1], orbital texture [2], and other hidden quantum features, positioning ARPES as a key technique in the exploration of quantum materials. However, their manifestation in ARPES spectra is still obscure due to interference effects [2,3] inherent to the photoemission process. Therefore, it is essential to simulate them with a high accuracy first-principles approach, capturing not only the underlying electronic structure but also the intricate mechanisms affecting the photo-electron states. In our formalism, these mechanisms are well captured by describing those states as the solution of the Kohn-Sham equation subject to the ARPES boundary conditions. This methodology is computationally efficient and advances the standard plane-wave-based density-functional theory implementations, allowing a streamlined yet robust framework for ARPES simulation. We benchmark our method against all-electron calculations and experimental dataset on graphene and WSe₂. Our results achieve a remarkable agreement, confirming the predictive power and versatility of our techniques.

[1] M. Schüler et al. Sci. Adv. 6, eaay2730(2020).

[2] Y. Yen et al. Nat. Phys. 20, 1912–1918 (2024).

[3] I. Sidilkover et al. Phys. Rev. Research 7, 033027.