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Title: Parallel Broadband Femtosecond Reflection Spectroscopy at a Soft X-Ray Free-Electron Laser

Journal Article · · Applied Sciences
DOI:https://doi.org/10.3390/app10196947· OSTI ID:1852384
ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [2]; ORCiD logo [2];  [2]; ORCiD logo [1];  [5];  [6];  [6];  [5];  [7];  [3]; ORCiD logo [1]
  1. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany). Dept. of Physics
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  3. Uppsala Univ. (Sweden). Dept. of Physics and Astronomy
  4. Uppsala Univ. (Sweden). Dept. of Physics and Astronomy; Univ. of California, San Diego, CA (United States). Center for Memory and Recording Research
  5. Paul Scherrer Inst. (PSI), Villigen (Switzerland)
  6. Max-Planck Institut für Mikrostrukturphysik, Halle (Germany)
  7. Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Berlin (Germany)

X-ray absorption spectroscopy (XAS) and the directly linked X-ray reflectivity near absorption edges yield a wealth of specific information on the electronic structure around the resonantly addressed element. Observing the dynamic response of complex materials to optical excitations in pump–probe experiments requires high sensitivity to small changes in the spectra which in turn necessitates the brilliance of free electron laser (FEL) pulses. However, due to the fluctuating spectral content of pulses generated by self-amplified spontaneous emission (SASE), FEL experiments often struggle to reach the full sensitivity and time-resolution that FELs can in principle enable. Here, we implement a setup which solves two common challenges in this type of spectroscopy using FELs: First, we achieve a high spectral resolution by using a spectrometer downstream of the sample instead of a monochromator upstream of the sample. Thus, the full FEL bandwidth contributes to the measurement at the same time, and the FEL pulse duration is not elongated by a monochromator. Second, the FEL beam is divided into identical copies by a transmission grating beam splitter so that two spectra from separate spots on the sample (or from the sample and known reference) can be recorded in-parallel with the same spectrometer, enabling a spectrally resolved intensity normalization of pulse fluctuations in pump–probe scenarios. We analyze the capabilities of this setup around the oxygen K- and nickel L-edges recorded with third harmonic radiation of the free electron laser in Hamburg (FLASH), demonstrating the capability for pump–probe measurements with sensitivity to reflectivity changes on the per mill level.

Research Organization:
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Helmholtz Association; Swedish Research Council (VR); European Research Council (ERC)
Grant/Contract Number:
SC0017643; VH-NG-1105; 2017-06711; 2018-0498; 701647
OSTI ID:
1852384
Journal Information:
Applied Sciences, Vol. 10, Issue 19; ISSN 2076-3417
Publisher:
MDPICopyright Statement
Country of Publication:
United States
Language:
English

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