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The influence of x-ray pulse length on space-charge effects in optical pump/x-ray probe photoemission

  • Pump-probe photoelectron spectroscopy (PES) is a versatile tool to investigate the dynamics of transient states of excited matter. Vacuum space-charge effects can mask these dynamics and complicate the interpretation of electron spectra. Here we report on space-charge effects in Au 4f photoemission from a polycrystalline gold surface, excited with moderately intense 90 ps (FWHM) soft x-ray probe pulses, under the influence of the Coulomb forces exerted by a pump electron cloud, which was produced by intense 40 fs laser pulses. The experimentally observed kinetic energy shift and spectral broadening of the Au 4f lines, measured with highly-efficient time-of-flight spectroscopy, are in good agreement with simulations utilizing a mean-field model of the electrostatic pump electron potential. This confirms that the line broadening is predominantly caused by variations in the take-off time of the probe electrons without appreciable influence of local scattering events. Our findings might be of general interest for pump-probe PES withPump-probe photoelectron spectroscopy (PES) is a versatile tool to investigate the dynamics of transient states of excited matter. Vacuum space-charge effects can mask these dynamics and complicate the interpretation of electron spectra. Here we report on space-charge effects in Au 4f photoemission from a polycrystalline gold surface, excited with moderately intense 90 ps (FWHM) soft x-ray probe pulses, under the influence of the Coulomb forces exerted by a pump electron cloud, which was produced by intense 40 fs laser pulses. The experimentally observed kinetic energy shift and spectral broadening of the Au 4f lines, measured with highly-efficient time-of-flight spectroscopy, are in good agreement with simulations utilizing a mean-field model of the electrostatic pump electron potential. This confirms that the line broadening is predominantly caused by variations in the take-off time of the probe electrons without appreciable influence of local scattering events. Our findings might be of general interest for pump-probe PES with picosecond-pulse-length sources.show moreshow less

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Metadaten
Author details:Danilo KühnGND, Erika Giangrisostomi, Raphael Martin JayORCiDGND, Florian SorgenfreiORCiDGND, Alexander FöhlischORCiDGND
DOI:https://doi.org/10.1088/1367-2630/ab2f5c
ISSN:1367-2630
Title of parent work (English):New journal of physics : the open-access journal for physics
Publisher:IOP Publ. Ltd.
Place of publishing:Bristol
Publication type:Article
Language:English
Date of first publication:2019/07/23
Publication year:2019
Release date:2020/12/16
Tag:ARTOF; electron spectroscopy; mean-field model; pump-probe; space-charge effects; x-ray photoemission
Volume:21
Number of pages:12
Funding institution:FLAG-ERA-Graphene-Basic Research 2 2017 in project LaMeS DFG [400335214]; ERCEuropean Research Council (ERC) [669531]
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie
DDC classification:5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik
Peer review:Referiert
Publishing method:Open Access / Gold Open-Access
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License (English):License LogoCreative Commons - Namensnennung 3.0 Unported
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