1. |
- Engel, Robin Y., et al.
(author)
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Electron population dynamics in resonant non-linear x-ray absorption in nickel at a free-electron laser
- 2023
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In: Structural Dynamics. - : American Institute of Physics (AIP). - 2329-7778. ; 10:5
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Journal article (peer-reviewed)abstract
- Free-electron lasers provide bright, ultrashort, and monochromatic x-ray pulses, enabling novel spectroscopic measurements not only with femtosecond temporal resolution: The high fluence of their x-ray pulses can also easily enter the regime of the non-linear x-ray-matter interaction. Entering this regime necessitates a rigorous analysis and reliable prediction of the relevant non-linear processes for future experiment designs. Here, we show non-linear changes in the L-3-edge absorption of metallic nickel thin films, measured with fluences up to 60 J/cm(2). We present a simple but predictive rate model that quantitatively describes spectral changes based on the evolution of electronic populations within the pulse duration. Despite its simplicity, the model reaches good agreement with experimental results over more than three orders of magnitude in fluence, while providing a straightforward understanding of the interplay of physical processes driving the non-linear changes. Our findings provide important insights for the design and evaluation of future high-fluence free-electron laser experiments and contribute to the understanding of non-linear electron dynamics in x-ray absorption processes in solids at the femtosecond timescale.
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2. |
- Huttmann, Felix, et al.
(author)
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Europium Cyclooctatetraene Nanowire Carpets : A Low-Dimensional, Organometallic, and Ferromagnetic Insulator
- 2019
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In: The Journal of Physical Chemistry Letters. - : American Chemical Society (ACS). - 1948-7185. ; 10:5, s. 911-917
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Journal article (peer-reviewed)abstract
- We investigate the magnetic and electronic properties of europium cyclooctatetraene (EuCot) nanowires by means of low-temperature X-ray magnetic circular dichroism (XMCD) and scanning tunneling microscopy (STM) and spectroscopy (STS). The EuCot nanowires are prepared in situ on a graphene surface. STS measurements identify EuCot as an insulator with a minority band gap of 2.3 eV. By means of Eu M5,4 edge XMCD, orbital and spin magnetic moments of (-0.1 ± 0.3)μB and (+7.0 ± 0.6)μB, respectively, were determined. Field-dependent measurements of the XMCD signal at the Eu M5 edge show hysteresis for grazing X-ray incidence at 5 K, thus confirming EuCot as a ferromagnetic material. Our density functional theory calculations reproduce the experimentally observed minority band gap. Modeling the experimental results theoretically, we find that the effective interatomic exchange interaction between Eu atoms is on the order of millielectronvolts, that magnetocrystalline anisotropy energy is roughly half as big, and that dipolar energy is approximately ten times lower.
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3. |
- La Torre, Enrico, et al.
(author)
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Local probe of irradiation-induced structural changes and orbital magnetism in Fe60Al40 thin films via an order-disorder phase transition
- 2018
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In: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 98:2
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Journal article (peer-reviewed)abstract
- Hard x-ray absorption and magnetic circular dichroism spectroscopy have been applied to study the consequential changes of the local environment around Fe atoms and their orbital polarizations in 40 nm thick Fe60Al40 thin films along the order-disorder (B2 -> A2) phase transition initiated by 20-keV Ne+ ion irradiation with fluences of (0.75-6) x 10(14) ions cm(-2). The analysis of the extended x-ray absorption fine structure spectra measured at the Fe K edge at room temperature revealed an increased number of Fe-Fe nearest neighbors from 3.47(7) to 5.0(1) and similar to 1% of volume expansion through the transition. The visualization of the Fe and Al nearest-neighbor rearrangement in the first coordination shell of Fe absorbers via the transition was carried out by wavelet transformations. The obtained changes in Fe coordination are evidently reflected in the x-ray magnetic circular dichroism spectra which show an increased orbital magnetic moment of Fe atoms and a pronounced magnetic multielectronic excitations peak at similar to 60 eV above the edge. The amplitudes of both peaks demonstrated similar dependencies on the irradiation fluence. The results of self-consistent density functional calculations on relaxed Fe60Al40 model structures for the ordered (B2) and the disordered (A2) phases are consistent with the experimental findings and point to the formation of Fe-rich regions in the films studied.
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4. |
- Lojewski, Tobias, et al.
(author)
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The interplay of local electron correlations and ultrafast spin dynamics in fcc Ni
- 2023
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In: Materials Research Letters. - : Taylor & Francis. - 2166-3831. ; 11:8, s. 655-661
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Journal article (peer-reviewed)abstract
- The complex electronic structure of metallic ferromagnets is determined by a balance between exchange interaction, electron hopping leading to band formation, and local Coulomb repulsion. By combining high energy and temporal resolution in femtosecond time-resolved X-ray absorption spectroscopy with ab initio time-dependent density functional theory we analyze the electronic structure in fcc Ni on the time scale of these interactions in a pump-probe experiment. We distinguish transient broadening and energy shifts in the absorption spectra, which we demonstrate to be captured by electron repopulation respectively correlation-induced modifications of the electronic structure, requiring to take the local Coulomb interaction into account.
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