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

Abstract

Here, 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 ~1 fs 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 ~10 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) and 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:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23); USDOE Laboratory Directed Research and Development (LDRD) Program; National Institutes of Health (NIH)
OSTI Identifier:
1421553
Alternate Identifier(s):
OSTI ID: 1429943; OSTI ID: 1465454
Grant/Contract Number:  
AC02-76SF00515; AC02-05CH11231; GM055302; GM110501; F32GM116423; RGP0063/2013 310
Resource 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)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Kroll, Thomas, Weninger, Clemens, Alonso-Mori, Roberto, Sokaras, Dimosthenis, Zhu, Diling, Mercadier, Laurent, Majety, Vinay P., Marinelli, Agostino, Lutman, Alberto, Guetg, Marc, Decker, Franz-Josef, Boutet, Sebastien, Aquila, Andy, Koglin, Jason, Koralek, Jake, DePonte, Daniel P., Kern, Jan, Fuller, Franklin D., Pastor, Ernest, Fransson, Thomas, Zhang, Yu, Yano, Junko, Yachandra, Vittal K., Rohringer, Nina, and Bergmann, Uwe. Stimulated x-ray emission spectroscopy in transition metal complexes. United States: N. p., 2018. Web. doi:10.1103/PhysRevLett.120.133203.
Kroll, Thomas, Weninger, Clemens, Alonso-Mori, Roberto, Sokaras, Dimosthenis, Zhu, Diling, Mercadier, Laurent, Majety, Vinay P., Marinelli, Agostino, Lutman, Alberto, Guetg, Marc, Decker, Franz-Josef, Boutet, Sebastien, Aquila, Andy, Koglin, Jason, Koralek, Jake, DePonte, Daniel P., Kern, Jan, Fuller, Franklin D., Pastor, Ernest, Fransson, Thomas, Zhang, Yu, Yano, Junko, Yachandra, Vittal K., Rohringer, Nina, & Bergmann, Uwe. Stimulated x-ray emission spectroscopy in transition metal complexes. United States. doi:10.1103/PhysRevLett.120.133203.
Kroll, Thomas, Weninger, Clemens, Alonso-Mori, Roberto, Sokaras, Dimosthenis, Zhu, Diling, Mercadier, Laurent, Majety, Vinay P., Marinelli, Agostino, Lutman, Alberto, Guetg, Marc, Decker, Franz-Josef, Boutet, Sebastien, Aquila, Andy, Koglin, Jason, Koralek, Jake, DePonte, Daniel P., Kern, Jan, Fuller, Franklin D., Pastor, Ernest, Fransson, Thomas, Zhang, Yu, Yano, Junko, Yachandra, Vittal K., Rohringer, Nina, and Bergmann, Uwe. Tue . "Stimulated x-ray emission spectroscopy in transition metal complexes". United States. doi:10.1103/PhysRevLett.120.133203. https://www.osti.gov/servlets/purl/1421553.
@article{osti_1421553,
title = {Stimulated x-ray emission spectroscopy in transition metal complexes},
author = {Kroll, Thomas and Weninger, Clemens and Alonso-Mori, Roberto and Sokaras, Dimosthenis and Zhu, Diling and Mercadier, Laurent and Majety, Vinay P. and Marinelli, Agostino and Lutman, Alberto and Guetg, Marc and Decker, Franz-Josef and Boutet, Sebastien and Aquila, Andy and Koglin, Jason and Koralek, Jake and DePonte, Daniel P. and Kern, Jan and Fuller, Franklin D. and Pastor, Ernest and Fransson, Thomas and Zhang, Yu and Yano, Junko and Yachandra, Vittal K. and Rohringer, Nina and Bergmann, Uwe},
abstractNote = {Here, 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 ~1 fs 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 ~1020~W/cm2 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.},
doi = {10.1103/PhysRevLett.120.133203},
journal = {Physical Review Letters},
number = 13,
volume = 120,
place = {United States},
year = {2018},
month = {3}
}

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    Works referencing / citing this record:

    Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes
    text, January 2018

    • Kroll, Thomas; Weninger, Clemens; Alonso-Mori, Roberto
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-00874

    Spectral Control of an X-Ray L -Edge Transition via a Thin-Film Cavity
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    Spectral Control of an X-Ray L -Edge Transition via a Thin-Film Cavity
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    Evidence of Extreme Ultraviolet Superfluorescence in Xenon
    journal, July 2019