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000580279 005__ 20231107210735.0
000580279 0247_ $$2datacite_doi$$a10.3204/PUBDB-2023-01185
000580279 037__ $$aPUBDB-2023-01185
000580279 041__ $$aEnglish
000580279 088__ $$2DESY$$aDESY-THESIS-2023-004
000580279 1001_ $$0P:(DE-H253)PIP1021933$$aEngel, Robin$$b0$$eCorresponding author$$gmale
000580279 245__ $$aFrom Linear to Non-Linear X-ray Spectroscopy on Materials using SASE-FELs$$f2018-07-15 - 2023-02-28
000580279 260__ $$aHamburg$$bVerlag Deutsches Elektronen-Synchrotron DESY$$c2023
000580279 300__ $$a193
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000580279 502__ $$aDissertation, Universität Hamburg, 2023$$bDissertation$$cUniversität Hamburg$$d2023$$o2023-02-28
000580279 520__ $$aThe 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.
000580279 536__ $$0G:(DE-HGF)POF4-632$$a632 - Materials – Quantum, Complex and Functional Materials (POF4-632)$$cPOF4-632$$fPOF IV$$x0
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000580279 536__ $$0G:(DE-HGF)2015_IFV-VH-GS-500$$aPHGS, VH-GS-500 - PIER Helmholtz Graduate School (2015_IFV-VH-GS-500)$$c2015_IFV-VH-GS-500$$x2
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000580279 693__ $$0EXP:(DE-H253)XFEL-SCS-20150101$$1EXP:(DE-H253)XFEL-20150101$$5EXP:(DE-H253)XFEL-SCS-20150101$$6EXP:(DE-H253)XFEL-SASE3-20150101$$aXFEL$$eSCS: Spectroscopy & Coherent Scattering$$fSASE3$$x1
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000580279 7001_ $$0P:(DE-H253)PIP1005334$$aBeye, Martin$$b1$$eThesis advisor
000580279 7001_ $$0P:(DE-H253)PIP1010773$$aHuse, Nils$$b2$$eThesis advisor
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000580279 9101_ $$0I:(DE-H253)_CFEL-20120731$$6P:(DE-H253)PIP1010773$$aCentre for Free-Electron Laser Science$$b2$$kCFEL
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000580279 9131_ $$0G:(DE-HGF)POF4-6G2$$1G:(DE-HGF)POF4-6G0$$2G:(DE-HGF)POF4-600$$3G:(DE-HGF)POF4$$4G:(DE-HGF)POF$$aDE-HGF$$bForschungsbereich Materie$$lGroßgeräte: Materie$$vFLASH (DESY)$$x1
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