001     580279
005     20231107210735.0
024 7 _ |a 10.3204/PUBDB-2023-01185
|2 datacite_doi
037 _ _ |a PUBDB-2023-01185
041 _ _ |a English
088 _ _ |a DESY-THESIS-2023-004
|2 DESY
100 1 _ |a Engel, Robin
|0 P:(DE-H253)PIP1021933
|b 0
|e Corresponding author
|g male
245 _ _ |a From Linear to Non-Linear X-ray Spectroscopy on Materials using SASE-FELs
|f 2018-07-15 - 2023-02-28
260 _ _ |a Hamburg
|c 2023
|b Verlag Deutsches Elektronen-Synchrotron DESY
300 _ _ |a 193
336 7 _ |a Output Types/Dissertation
|2 DataCite
336 7 _ |a Book
|0 PUB:(DE-HGF)3
|2 PUB:(DE-HGF)
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336 7 _ |a DISSERTATION
|2 ORCID
336 7 _ |a PHDTHESIS
|2 BibTeX
336 7 _ |a Thesis
|0 2
|2 EndNote
336 7 _ |a Dissertation / PhD Thesis
|b phd
|m phd
|0 PUB:(DE-HGF)11
|s 1699359880_341808
|2 PUB:(DE-HGF)
336 7 _ |a doctoralThesis
|2 DRIVER
490 0 _ |a DESY-THESIS
502 _ _ |a Dissertation, Universität Hamburg, 2023
|c Universität Hamburg
|b Dissertation
|d 2023
|o 2023-02-28
520 _ _ |a The key feature of X-ray Free Electron Lasers (XFELs) is their capability to generate ultrashort and at least partially coherent X-ray pulses with extreme intensity. This capability holds the promise to revolutionize X-ray physics in a way similar to how lasers have revolutionized optics, as the non-linear and coherent interactions known from theoptical regime combined with the properties of X-ray radiation could enable techniques with unprecedented analyzing power. This thesis summarizes several contributions tothe development from linear to non-linear X-ray spectroscopies at XFELs. To begin with, I address the technical challenge of normalizing the spectral intensity fluctuationsof XFEL-radiation by presenting several versions of the split-beam normalization scheme. Versions suitable for both monochromatic and broadband measurements, either in transmission through liquids or metal films or in reflection from bulk-supported samples are demonstrated and their capabilities and performance are compared. Moving to non-parametric high-fluence studies, we present a non-linear absorption study at the nickel L3-edge using a monochromatic split-beam normalization scheme. We interpret the fluence-dependent spectral changes by characterizing the evolution of the electronic system during interaction with the X-ray pulse using a rate model that quantifiesthe photon absorption and electronic scattering processes. Further, we show a similar non-linear absorption experiment that utilizes a broadband split-beam normalization scheme. While we observe a comparable evolution ofthe electronic system, the broadband incident radiation leads to a strong contribution of stimulated inelastic scattering that is up to six orders of magnitude stronger than the spontaneous contribution that is exploited in conventional Resonant Inelastic X-rayScattering (RIXS). Finally, we demonstrate sum and difference frequency generation between core-resonant XFEL-photons with two infrared photons for the first time. The observed photon-energy dependence of the third-order non-linear susceptibility suggests an enhancement through coupling between the 1s2p and 1s2s excited states, thus demonstratinga key capability of wave-mixing spectroscopy methods. In summary, the presented work contributes to the development of non-linear X-rayspectroscopy on various fronts, but further developments will be needed to bring X-ray wave-mixing techniques into their preconceived position to deliver unprecedented insights into molecular and solid-state dynamics.
536 _ _ |a 632 - Materials – Quantum, Complex and Functional Materials (POF4-632)
|0 G:(DE-HGF)POF4-632
|c POF4-632
|f POF IV
|x 0
536 _ _ |a 6G2 - FLASH (DESY) (POF4-6G2)
|0 G:(DE-HGF)POF4-6G2
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536 _ _ |a PHGS, VH-GS-500 - PIER Helmholtz Graduate School (2015_IFV-VH-GS-500)
|0 G:(DE-HGF)2015_IFV-VH-GS-500
|c 2015_IFV-VH-GS-500
|x 2
693 _ _ |a FLASH
|f FLASH Beamline PG2
|1 EXP:(DE-H253)FLASH-20150101
|0 EXP:(DE-H253)F-PG2-20150101
|6 EXP:(DE-H253)F-PG2-20150101
|x 0
693 _ _ |a XFEL
|e SCS: Spectroscopy & Coherent Scattering
|f SASE3
|1 EXP:(DE-H253)XFEL-20150101
|0 EXP:(DE-H253)XFEL-SCS-20150101
|5 EXP:(DE-H253)XFEL-SCS-20150101
|6 EXP:(DE-H253)XFEL-SASE3-20150101
|x 1
693 _ _ |a FLASH
|e Facility (machine) FLASH
|1 EXP:(DE-H253)FLASH-20150101
|0 EXP:(DE-H253)FLASH(machine)-20150101
|5 EXP:(DE-H253)FLASH(machine)-20150101
|x 2
700 1 _ |a Beye, Martin
|0 P:(DE-H253)PIP1005334
|b 1
|e Thesis advisor
700 1 _ |a Huse, Nils
|0 P:(DE-H253)PIP1010773
|b 2
|e Thesis advisor
856 4 _ |u https://bib-pubdb1.desy.de/record/580279/files/desy-thesis-23-004.title.pdf
|y OpenAccess
856 4 _ |u https://bib-pubdb1.desy.de/record/580279/files/thesis.pdf
|y OpenAccess
856 4 _ |u https://bib-pubdb1.desy.de/record/580279/files/desy-thesis-23-004.title.pdf?subformat=pdfa
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|y OpenAccess
856 4 _ |u https://bib-pubdb1.desy.de/record/580279/files/thesis.pdf?subformat=pdfa
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|y OpenAccess
909 C O |o oai:bib-pubdb1.desy.de:580279
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910 1 _ |a Deutsches Elektronen-Synchrotron
|0 I:(DE-588b)2008985-5
|k DESY
|b 0
|6 P:(DE-H253)PIP1021933
910 1 _ |a European XFEL
|0 I:(DE-588)1043621512
|k XFEL.EU
|b 0
|6 P:(DE-H253)PIP1021933
910 1 _ |a Deutsches Elektronen-Synchrotron
|0 I:(DE-588b)2008985-5
|k DESY
|b 1
|6 P:(DE-H253)PIP1005334
910 1 _ |a European XFEL
|0 I:(DE-588)1043621512
|k XFEL.EU
|b 1
|6 P:(DE-H253)PIP1005334
910 1 _ |a Centre for Free-Electron Laser Science
|0 I:(DE-H253)_CFEL-20120731
|k CFEL
|b 2
|6 P:(DE-H253)PIP1010773
910 1 _ |a External Institute
|0 I:(DE-HGF)0
|k Extern
|b 2
|6 P:(DE-H253)PIP1010773
913 1 _ |a DE-HGF
|b Forschungsbereich Materie
|l Von Materie zu Materialien und Leben
|1 G:(DE-HGF)POF4-630
|0 G:(DE-HGF)POF4-632
|3 G:(DE-HGF)POF4
|2 G:(DE-HGF)POF4-600
|4 G:(DE-HGF)POF
|v Materials – Quantum, Complex and Functional Materials
|x 0
913 1 _ |a DE-HGF
|b Forschungsbereich Materie
|l Großgeräte: Materie
|1 G:(DE-HGF)POF4-6G0
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914 1 _ |y 2023
915 _ _ |a OpenAccess
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920 1 _ |0 I:(DE-H253)FS-FLASH-20140814
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980 _ _ |a phd
980 _ _ |a VDB
980 _ _ |a book
980 _ _ |a I:(DE-H253)FS-FLASH-20140814
980 _ _ |a UNRESTRICTED
980 1 _ |a FullTexts


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