skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Femtosecond electronic structure response to high intensity XFEL pulses probed by iron X-ray emission spectroscopy

Journal Article · · Scientific Reports
 [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1];  [3];  [1];  [1];  [4];  [4];  [5];  [1];  [6];  [7];  [1];  [1] more »;  [1] « less
  1. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  2. Univ. Rennes (France)
  3. Paul Scherrer Institute (PSI), Villigen (Switzerland)
  4. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  5. European XFEL, Schenefeld (Germany)
  6. ShanghaiTech University (China)
  7. Beijing Normal University (China)

We report the time-resolved femtosecond evolution of the K-shell X-ray emission spectra of iron during high intensity illumination of X-rays in a micron-sized focused hard X-ray free electron laser (XFEL) beam. Detailed pulse length dependent measurements revealed that rapid spectral energy shift and broadening started within the first 10 fs of the X-ray illumination at intensity levels between 1017 and 1018 W cm-2. We attribute these spectral changes to the rapid evolution of high-density photoelectron mediated secondary collisional ionization processes upon the absorption of the incident XFEL radiation. These fast electronic processes, occurring at timescales well within the typical XFEL pulse durations (i.e., tens of fs), set the boundary conditions of the pulse intensity and sample parameters where the widely-accepted ‘probe-before-destroy’ measurement strategy can be adopted for electronic-structure related XFEL experiments.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Contributing Organization:
SLAC National Accelerator Laboratory, Menlo Park, CA-94025, USA. Univ Rennes, CNRS, IPR (Institut de Physique de Rennes) - UMR 6251, F-35000 Rennes. France. SwissFEL, Paul Scherrer Institute, 5232 Villigen, Switzerland Deutsches Elektronen-Synchrotron DESY, Notkestraße 85, 22607 Hamburg, Germany. European XFEL, Holzkoppel 4, 22869 Schenefeld, Germany High Pressure for Science & Technology Advanced Research, Shanghai 201203, China Department of Physics and Applied Optics Beijing Area Major Laboratory, Center for Advanced Quantum Studies, Beijing Normal University, Beijing 100875, China
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1671331
Alternate ID(s):
OSTI ID: 1769046
Journal Information:
Scientific Reports, Vol. 10, Issue 1; ISSN 2045-2322
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (27)

Single mimivirus particles intercepted and imaged with an X-ray laser journal February 2011
Multiplet effects in X-ray spectroscopy journal January 2005
Femtosecond x-ray pulse temporal characterization in free-electron lasers using a transverse deflector journal December 2011
Room temperature femtosecond X-ray diffraction of photosystem II microcrystals journal June 2012
Imaging single cells in a beam of live cyanobacteria with an X-ray laser journal February 2015
Tracking excited-state charge and spin dynamics in iron coordination complexes journal May 2014
High-Resolution Protein Structure Determination by Serial Femtosecond Crystallography journal May 2012
A multi-crystal wavelength dispersive x-ray spectrometer journal July 2012
Femtosecond X-ray protein nanocrystallography journal February 2011
Metalloprotein entatic control of ligand-metal bonds quantified by ultrafast x-ray spectroscopy journal June 2017
Impact of hollow-atom formation on coherent x-ray scattering at high intensity journal March 2011
High resolution 1s core hole X-ray spectroscopy in 3d transition metal complexes—electronic and structural information journal January 2005
Taking snapshots of photosynthetic water oxidation using femtosecond X-ray diffraction and spectroscopy journal July 2014
Femtosecond X-Ray Pulse Characterization in Free-Electron Lasers Using a Cross-Correlation Technique journal December 2012
Indications of radiation damage in ferredoxin microcrystals using high-intensity X-FEL beams journal February 2015
A hard x-ray transmissive single-shot spectrometer for FEL sources conference October 2012
Full spatial characterization of a nanofocused x-ray free-electron laser beam by ptychographic imaging journal April 2013
Simultaneous Femtosecond X-ray Spectroscopy and Diffraction of Photosystem II at Room Temperature journal February 2013
The X-ray Pump–Probe instrument at the Linac Coherent Light Source journal April 2015
X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis journal December 2018
Potential for biomolecular imaging with femtosecond X-ray pulses journal August 2000
Energy-dispersive X-ray emission spectroscopy using an X-ray free-electron laser in a shot-by-shot mode journal November 2012
Inception of electronic damage of matter by photon-driven post-ionization mechanisms journal March 2019
Femtosecond diffractive imaging of biological cells journal September 2010
Observation of K Hypersatellites and KL Satellites in the X-Ray Spectrum of Doubly K -Ionized Gallium journal September 1971
Focus characterization at an X-ray free-electron laser by coherent scattering and speckle analysis journal April 2015
Photon-in photon-out hard X-ray spectroscopy at the Linac Coherent Light Source journal April 2015

Cited By (4)

Probing Transient Valence Orbital Changes with Picosecond Valence-to-Core X-ray Emission Spectroscopy journal January 2017
Vibrational wavepacket dynamics in Fe carbene photosensitizer determined with femtosecond X-ray emission and scattering journal January 2020
A versatile experimental system for tracking ultrafast chemical reactions with X-ray free-electron lasers journal September 2019
Communication: The electronic structure of matter probed with a single femtosecond hard x-ray pulse text January 2014

Figures / Tables (4)