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Ramifications of optical pumping on the interpretation of time-resolved photoemission experiments on graphene

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Date
04/2015
Author
Ulstrup, Søren
Johannsen, Jens Christian
Cilento, Federico
Crepaldi, Alberto
Miwa, Jill A.
Zacchigna, Michele
Cacho, Cephise
Chapman, Richard T.
Springate, Emma
Fromm, Felix
Raidel, Christian
Seyller, Thomas
King, Phil D.C.
Parmigiani, Fulvio
Grioni, Marco
Hofmann, Philip
Funder
The Royal Society
EPSRC
Grant ID
UF120096
EP/I031014/1
Keywords
Hot Electrons
Graphene
Time- and Angle-Resolved Photoemission
Space Charge
QC Physics
NDAS
Metadata
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Abstract
Abstract In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES) experiments the presence of the pump pulse adds a new level of complexity to the photoemission process in comparison to conventional ARPES. This is evidenced by pump-induced vacuum space-charge effects and surface photovoltages, as well as multiple pump excitations due to internal reflections in the sample-substrate system. These processes can severely affect a correct interpretation of the data by masking the out-of-equilibrium electron dynamics intrinsic to the sample. In this study, we show that such effects indeed influence TR-ARPES data of graphene on a silicon carbide (SiC) substrate. In particular, we find a time- and laser fluence-dependent spectral shift and broadening of the acquired spectra, and unambiguously show the presence of a double pump excitation. The dynamics of these effects is slower than the electron dynamics in the graphene sample, thereby permitting us to deconvolve the signals in the time domain. Our results demonstrate that complex pump-related processes should always be considered in the experimental setup and data analysis.
Citation
Ulstrup , S , Johannsen , J C , Cilento , F , Crepaldi , A , Miwa , J A , Zacchigna , M , Cacho , C , Chapman , R T , Springate , E , Fromm , F , Raidel , C , Seyller , T , King , P D C , Parmigiani , F , Grioni , M & Hofmann , P 2015 , ' Ramifications of optical pumping on the interpretation of time-resolved photoemission experiments on graphene ' , Journal of Electron Spectroscopy and Related Phenomena , vol. 200 , pp. 340–346 . https://doi.org/10.1016/j.elspec.2015.04.010
Publication
Journal of Electron Spectroscopy and Related Phenomena
Status
Peer reviewed
DOI
https://doi.org/10.1016/j.elspec.2015.04.010
ISSN
0368-2048
Type
Journal article
Rights
Copyright © 2015 Published by Elsevier B.V. This is the author’s version of a work that was accepted for publication in Journal of Electron Spectroscopy and Related Phenomena. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Journal of Electron Spectroscopy and Related Phenomena, DOI: https://dx.doi.org/10.1016/j.elspec.2015.04.010
Description
The authors acknowledge financial support from the VILLUM foundation, The Danish Council for Independent Research / Technology and Production Sciences, the Swiss National Science Foundation (NSF), EPSRC, The Royal Society and the Italian Ministry of University and Research (Grants No. FIRBRBAP045JF2 and No. FIRB-RBAP06AWK3). Access to the Artemis Facility was funded by STFC. Work in Chemnitz was supported by the European Union through the project ConceptGraphene, and by the German Research Foundation in the framework of the SPP 1459 Graphene.
Collections
  • University of St Andrews Research
URI
http://hdl.handle.net/10023/8670

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