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This content will become publicly available on March 27, 2019

Title: Stimulated x-ray emission spectroscopy in transition metal complexes

We report the observation and analysis of the gain curve of amplified Kα X-ray emission from solutions of Mn(II) and Mn(VII) complexes using an X-ray free electron laser to create the 1s core-hole population inversion. We find spectra at amplification levels extending over four orders of magnitude until saturation. We observe bandwidths below the Mn 1s core-hole lifetime broadening in the onset of the stimulated emission. In the exponential amplification regime the resolution corrected spectral width of ~1.7 eV FWHM is constant over three orders of magnitude, pointing to the build-up of transform limited pulses of ~1fs duration. Driving the amplification into saturation leads to broadening and shift of the line. Importantly, the chemical sensitivity of the stimulated X-ray emission to the Mn oxidation state is preserved at power densities of $$\sim10 20$$~W/cm 2 for the incoming X-ray pulses. Differences in signal sensitivity and spectral information compared to conventional (spontaneous) X-ray emission spectroscopy are discussed. Our findings build a baseline for nonlinear X-ray spectroscopy for a wide range of transition metal complexes in inorganic chemistry, catalysis and materials science.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [3] ;  [5] ;  [5] ;  [6] ;  [6] ;  [6] ;  [6] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [7] ;  [8] ;  [8] ;  [9] more »;  [9] ;  [8] ;  [8] ;  [10] ;  [11] « less
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  2. Max Planck Inst. for the Structure and Dynamics of Matter, Hamburg (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  5. Max Planck Inst. for the Structure and Dynamics of Matter, Hamburg (Germany)
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Accelerator Directorate
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Biophysics and Integrated Bioimaging Division
  8. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Biophysics and Integrated Bioimaging Division
  9. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  10. Max Planck Inst. for the Structure and Dynamics of Matter, Hamburg (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg, Hamburg (Germany)
  11. SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
Publication Date:
Grant/Contract Number:
AC02-76SF00515; AC02-05CH11231; GM055302; GM110501
Type:
Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 120; Journal Issue: 13; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Institutes of Health (NIH); USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS
OSTI Identifier:
1421553
Alternate Identifier(s):
OSTI ID: 1429943