Eur. Phys. J. B (2018) 91: 126
https://doi.org/10.1140/epjb/e2018-90108-7

Regular Article

First-principles simulations for attosecond photoelectron spectroscopy based on time-dependent density functional theory^★

¹ Max Planck Institute for the Structure and Dynamics of Matter and Center for Free-Electron Laser Science, Luruper Chaussee 149, 22761 Hamburg, Germany
² Center for Computational Quantum Physics (CCQ), The Flatiron Institute, 162 Fifth Avenue, New York, NY 10010, USA
³ Nano-Bio Spectroscopy Group, Departamento de Fisica de Materiales, Universidad del País Vasco UPV/EHU, 20018 San Sebastián, Spain

^a e-mail: umberto.degiovannini@gmail.com

Received: 1 March 2018
Received in final form: 9 April 2018
Published online: 22 June 2018

Abstract

We develop a first-principles simulation method for attosecond time-resolved photoelectron spectroscopy. This method enables us to directly simulate the whole experimental processes, including excitation, emission and detection on equal footing. To examine the performance of the method, we use it to compute the reconstruction of attosecond beating by interference of two-photon transitions (RABBITT) experiments of gas-phase Argon. The computed RABBITT photoionization delay is in very good agreement with recent experimental results from [Klünder et al., Phys. Rev. Lett. 106, 143002 (2011)] and [Guénot et al., Phys. Rev. A 85, 053424 (2012)]. This indicates the significance of a fully-consistent theoretical treatment of the whole measurement process to properly describe experimental observables in attosecond photoelectron spectroscopy. The present framework opens the path to unravel the microscopic processes underlying RABBITT spectra in more complex materials and nanostructures.