Lippmann-Schwinger Approach for Accurate Photoelectron Wave Functions and Angle-Resolved Photoemission Spectra from First Principles

We present a conceptually simple and technically straightforward method for calculating photoelectron wave functions that is easily integrable with standard wave-function-based density-functional-theory packages. Our method is based on the Lippmann-Schwinger equation, naturally incorporating the boundary condition that the final photoelectron state must satisfy. The calculated results are in good agreement with the measured photon-energy and polarization dependence of the angle-resolved photoemission spectroscopy (ARPES) of graphene, the photon-energy-dependent evolution of the so-called dark corridor arising from the pseudospin, and WSe_{2}, the circular dichroism reflecting the hidden orbital polarization. Our Letter opens doors to do-it-yourself simulations of ARPES with standard density-functional-theory packages, of crucial importance in the era of "quantum materials," whose key experimental tool is ARPES.