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

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 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.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [3];  [4]; ORCiD logo [2];  [1]; ORCiD logo [5];  [1];  [2];  [6];  [1];  [7];  [8];  [2];  [2]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States); European X-Ray Free-Electron Laser Facility GmbH, Schenefeld (Germany)
  4. HGST a Western Digital Company, San Jose, CA (United States); Chemnitz Univ. of Technology (Germany); Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Warwick (United Kingdom)
  7. European X-ray Free-Electron Laser (XFEL), Hamburg (Germany)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States); Uppsala Univ. (Sweden)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); VolkswagenStiftung
OSTI Identifier:
1580988
Alternate Identifier(s):
OSTI ID: 1571824
Grant/Contract Number:  
AC02-76SF00515; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; Ultrafast; Femtosecond; Electronic dynamics; Magnetic dynamics; Nonlinear X-ray science; X-ray absorption spectroscopy

Citation Formats

Higley, Daniel J., Reid, Alex H., Chen, Zhao, Guyader, Loïc Le, Hellwig, Olav, Lutman, Alberto A., Liu, Tianmin, Shafer, Padraic, Chase, Tyler, Dakovski, Georgi L., Mitra, Ankush, Yuan, Edwin, Schlappa, Justine, Dürr, Hermann A., Schlotter, William F., and Stöhr, Joachim. Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution. United States: N. p., 2019. Web. doi:10.1038/s41467-019-13272-5.
Higley, Daniel J., Reid, Alex H., Chen, Zhao, Guyader, Loïc Le, Hellwig, Olav, Lutman, Alberto A., Liu, Tianmin, Shafer, Padraic, Chase, Tyler, Dakovski, Georgi L., Mitra, Ankush, Yuan, Edwin, Schlappa, Justine, Dürr, Hermann A., Schlotter, William F., & Stöhr, Joachim. Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution. United States. doi:10.1038/s41467-019-13272-5.
Higley, Daniel J., Reid, Alex H., Chen, Zhao, Guyader, Loïc Le, Hellwig, Olav, Lutman, Alberto A., Liu, Tianmin, Shafer, Padraic, Chase, Tyler, Dakovski, Georgi L., Mitra, Ankush, Yuan, Edwin, Schlappa, Justine, Dürr, Hermann A., Schlotter, William F., and Stöhr, Joachim. Thu . "Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution". United States. doi:10.1038/s41467-019-13272-5. https://www.osti.gov/servlets/purl/1580988.
@article{osti_1580988,
title = {Femtosecond X-ray induced changes of the electronic and magnetic response of solids from electron redistribution},
author = {Higley, Daniel J. and Reid, Alex H. and Chen, Zhao and Guyader, Loïc Le and Hellwig, Olav and Lutman, Alberto A. and Liu, Tianmin and Shafer, Padraic and Chase, Tyler and Dakovski, Georgi L. and Mitra, Ankush and Yuan, Edwin and Schlappa, Justine and Dürr, Hermann A. and Schlotter, William F. and Stöhr, Joachim},
abstractNote = {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 L3 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.},
doi = {10.1038/s41467-019-13272-5},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {2019},
month = {11}
}

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