Decoherence in Attosecond Photoionization

Stefan Pabst, Loren Greenman, Phay J. Ho, David A. Mazziotti, and Robin Santra

Phys. Rev. Lett. 106, 053003 – Published 2 February 2011

Abstract

The creation of superpositions of hole states via single-photon ionization using attosecond extreme-ultraviolet pulses is studied with the time-dependent configuration-interaction singles (TDCIS) method. Specifically, the degree of coherence between hole states in atomic xenon is investigated. We find that interchannel coupling not only affects the hole populations, but it also enhances the entanglement between the photoelectron and the remaining ion, thereby reducing the coherence within the ion. As a consequence, even if the spectral bandwidth of the ionizing pulse exceeds the energy splittings among the hole states involved, perfectly coherent hole wave packets cannot be formed. For sufficiently large spectral bandwidth, the coherence can only be increased by increasing the mean photon energy.

Received 15 October 2010

DOI:https://doi.org/10.1103/PhysRevLett.106.053003

Authors & Affiliations

Stefan Pabst^1,2, Loren Greenman³, Phay J. Ho⁴, David A. Mazziotti³, and Robin Santra^1,2,*

¹Center for Free-Electron Laser Science, DESY, Notkestrasse 85, 22607 Hamburg, Germany
²Department of Physics, University of Hamburg, Jungiusstrasse 9, 20355 Hamburg, Germany
³Department of Chemistry and The James Franck Institute, The University of Chicago, Chicago, Illinois 60637, USA
⁴Argonne National Laboratory, Argonne, Illinois 60439, USA