Home > Publications database > From Linear to Non-Linear X-ray Spectroscopy on Materials using SASE-FELs > print |
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) |m book |
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 |c POF4-6G2 |f POF IV |x 1 |
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 |
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856 | 4 | _ | |u https://bib-pubdb1.desy.de/record/580279/files/thesis.pdf?subformat=pdfa |x pdfa |y OpenAccess |
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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 |0 G:(DE-HGF)POF4-6G2 |3 G:(DE-HGF)POF4 |2 G:(DE-HGF)POF4-600 |4 G:(DE-HGF)POF |v FLASH (DESY) |x 1 |
914 | 1 | _ | |y 2023 |
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