Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution

Daniel J. Higley (), Alex H. Reid, Zhao Chen, Loïc Le Guyader, Olav Hellwig, Alberto A. Lutman, Tianmin Liu, Padraic Shafer, Tyler Chase, Georgi L. Dakovski, Ankush Mitra, Edwin Yuan, Justine Schlappa, Hermann A. Dürr, William F. Schlotter and Joachim Stöhr ()
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Daniel J. Higley: SLAC National Accelerator Laboratory
Alex H. Reid: SLAC National Accelerator Laboratory
Zhao Chen: SLAC National Accelerator Laboratory
Loïc Le Guyader: SLAC National Accelerator Laboratory
Olav Hellwig: HGST a Western Digital Company
Alberto A. Lutman: SLAC National Accelerator Laboratory
Tianmin Liu: SLAC National Accelerator Laboratory
Padraic Shafer: Lawrence Berkeley National Laboratory
Tyler Chase: SLAC National Accelerator Laboratory
Georgi L. Dakovski: SLAC National Accelerator Laboratory
Ankush Mitra: SLAC National Accelerator Laboratory
Edwin Yuan: SLAC National Accelerator Laboratory
Justine Schlappa: European X-Ray Free-Electron Laser Facility GmbH
Hermann A. Dürr: SLAC National Accelerator Laboratory
William F. Schlotter: SLAC National Accelerator Laboratory
Joachim Stöhr: SLAC National Accelerator Laboratory

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: Abstract Resonant X-ray absorption, where an X-ray photon excites a core electron into an unoccupied valence state, is an essential process in many standard X-ray spectroscopies. With increasing X-ray intensity, the X-ray absorption strength is expected to become nonlinear. Here, we report the onset of such a nonlinearity in the resonant X-ray absorption of magnetic Co/Pd multilayers near the Co L$${}_{3}$$3 edge. The nonlinearity is directly observed through the change of the absorption spectrum, which is modified in less than 40 fs within 2 eV of its threshold. This is interpreted as a redistribution of valence electrons near the Fermi level. For our magnetic sample this also involves mixing of majority and minority spins, due to sample demagnetization. Our findings reveal that nonlinear X-ray responses of materials may already occur at relatively low intensities, where the macroscopic sample is not destroyed, providing insight into ultrafast charge and spin dynamics.

Date: 2019
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DOI: 10.1038/s41467-019-13272-5

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