A First-Principles Time-Dependent Density Functional Theory Framework for Spin 
and Time-Resolved Angular-Resolved Photoelectron Spectroscopy in Periodic 
Systems

de Giovannini, U.; Hübener, H.; Rubio, A.

doi:10.1021/acs.jctc.6b00897

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A First-Principles Time-Dependent Density Functional Theory Framework for Spin and Time-Resolved Angular-Resolved Photoelectron Spectroscopy in Periodic Systems

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Rubio, A.
Nano-Bio Spectroscopy Group, University of the Basque Country UPV/EHU;
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science and Department of Physics, University of Hamburg;

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https://dx.doi.org/10.1021/acs.jctc.6b00897
(Publisher version)

https://arxiv.org/abs/1609.03092
(Preprint)

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1609.03092.pdf
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Citation

de Giovannini, U., Hübener, H., & Rubio, A. (2017). A First-Principles Time-Dependent Density Functional Theory Framework for Spin and Time-Resolved Angular-Resolved Photoelectron Spectroscopy in Periodic Systems. Journal of Chemical Theory and Computation, 13(1), 265-273. doi:10.1021/acs.jctc.6b00897.

Cite as: https://hdl.handle.net/21.11116/0000-0001-7E9A-5

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 analyzing surface. The resulting approach, that we named t-SURFFP, allows us 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, monolayer, and bilayer WSe2, and hexagonal BN (hBN) under different laser configurations.