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

Journal Of Chemical Theory And Computation 13 (1), 265 - 273 (2017)

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

Umberto De Giovannini, Hannes Hübener, Angel Rubio

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 WSe2, and hexagonal BN under different laser configurations.

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Doi
http://dx.doi.org/ 10.1021/acs.jctc.6b00897
arxiv
http://arxiv.org/abs/arXiv:1609.03092v1

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