Accurate and efficient simulation of photoemission spectroscopy via Kohn-Sham scattering states
Abstract
We introduce an efficient first-principles framework for simulating angle-resolved photoemission spectroscopy (ARPES) based on the direct computation of photoelectron states as solutions of the Kohn-Sham equation with scattering boundary conditions. While the one-step theory of photoemission has a long and successful history, existing implementations are often tied to specialized electronic-structure formalisms. Our approach is formally equivalent to the Lippmann-Schwinger formulation, and it is directly compatible with standard plane-wave and real-space density functional theory codes, enabling seamless integration with advanced exchange-correlation functionals and modern electronic-structure workflows. By providing explicit photoelectron wave functions, the method allows for a transparent analysis of matrix-element effects, multiple scattering, and experimental geometry. We demonstrate the accuracy and predictive power of the framework through circular-dichroism ARPES simulations for monolayer graphene and bulk 2H-WSe2, achieving excellent agreement with experimental data over a wide photon-energy range. Our results establish a robust and accessible route toward quantitative ARPES modeling, opening the door to systematic studies of orbital textures, many-body effects, and nonequilibrium phenomena within widely used ab initio platforms.
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BibTeX
@misc{parusa2026accurate,
title = {{Accurate and efficient simulation of photoemission spectroscopy via Kohn-Sham scattering states}},
author = {Gian Parusa and Sotirios Fragkos and Samuel Beaulieu and Michael Schüler},
howpublished = {HAL},
year = {2026},
month = nov,
doi = {10.48550/arxiv.2601.12490},
url = {https://hal.science/hal-05780785v1},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Accurate and efficient simulation of photoemission spectroscopy via Kohn-Sham scattering states
AU - Gian Parusa
AU - Sotirios Fragkos
AU - Samuel Beaulieu
AU - Michael Schüler
PY - 2026
DA - 2026/11/05
PB - HAL
DO - 10.48550/arxiv.2601.12490
UR - https://hal.science/hal-05780785v1
AB - We introduce an efficient first-principles framework for simulating angle-resolved photoemission spectroscopy (ARPES) based on the direct computation of photoelectron states as solutions of the Kohn-Sham equation with scattering boundary conditions. While the one-step theory of photoemission has a long and successful history, existing implementations are often tied to specialized electronic-structure formalisms. Our approach is formally equivalent to the Lippmann-Schwinger formulation, and it is directly compatible with standard plane-wave and real-space density functional theory codes, enabling seamless integration with advanced exchange-correlation functionals and modern electronic-structure workflows. By providing explicit photoelectron wave functions, the method allows for a transparent analysis of matrix-element effects, multiple scattering, and experimental geometry. We demonstrate the accuracy and predictive power of the framework through circular-dichroism ARPES simulations for monolayer graphene and bulk 2H-WSe_2, achieving excellent agreement with experimental data over a wide photon-energy range. Our results establish a robust and accessible route toward quantitative ARPES modeling, opening the door to systematic studies of orbital textures, many-body effects, and nonequilibrium phenomena within widely used ab initio platforms.
ER -