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  Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes

Kroll, T., Weninger, C., Alonso-Mori, R., Sokaras, D., Zhu, D., Mercadier, L., et al. (2018). Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes. Physical Review Letters, 120(13): 133203. doi:10.1103/PhysRevLett.120.133203.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0001-AB94-7 Version Permalink: http://hdl.handle.net/21.11116/0000-0004-8FD8-8
Genre: Journal Article

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PhysRevLett.120.133203.pdf (Publisher version), 848KB
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 Creators:
Kroll, T.1, 2, Author
Weninger, C.1, 3, Author              
Alonso-Mori, R.1, Author
Sokaras, D.2, Author
Zhu, D.1, Author
Mercadier, L.3, Author              
Majety, V. P.3, Author              
Marinelli, A.4, Author
Lutman, A.4, Author
Guetg, M. W.4, Author
Decker, F.-J.4, Author
Boutet, S.1, Author
Aquila, A.1, Author
Koglin, J.1, Author
Koralek, J.1, Author
DePonte, D. P.1, Author
Kern, J.1, 5, Author
Fuller, F. D.5, Author
Pastor, E.5, Author
Fransson, T.6, Author
Zhang, Y.6, AuthorYano, J.5, AuthorYachandra, V. K.5, AuthorRohringer, N.3, 7, 8, Author              Bergmann, U.1, 6, Author more..
Affiliations:
1LCLS, SLAC National Accelerator Laboratory, Menlo Park, ou_persistent22              
2SSRL, SLAC National Accelerator Laboratory, Menlo Park, ou_persistent22              
3Quantum Optics with X-Rays, Independent Research Groups, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938291              
4Accelerator Directorate, SLAC National Accelerator Laboratory, Menlo Park, ou_persistent22              
5Molecular Biophysics and Integrated Bioimaging Division, Lawrence, Berkeley National Laboratory, ou_persistent22              
6Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, ou_persistent22              
7Center for Free-Electron Laser Science, DESY, ou_persistent22              
8Department of Physics, Universität Hamburg, ou_persistent22              

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 Abstract: 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 4 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 3 orders of magnitude, pointing to the buildup of transform limited pulses of ∼1  fs duration. Driving the amplification into saturation leads to broadening and a 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.

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Language(s): eng - English
 Dates: 2017-11-162017-06-052018-03-272018-03-27
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1103/PhysRevLett.120.133203
 Degree: -

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Project name : Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02- 76SF00515. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. The SSRL Structural Molecular Biology Program (T. K.) is supported by the DOE Office of Biological and Environmental Research, and by the National Institutes of Health, National Institute of General Medical Sciences (including P41GM103393). The contents of this publication are solely the responsibility of the authors and do not necessarily represent the official views of NIGMS or NIH. A part of this work was supported by the Director, Office of Science, Office of Basic Energy Sciences (OBES), Division of Chemical Sciences, Geosciences, and Biosciences (CSGB) of the Department of Energy (DOE) (Contract No. DE-AC02- 05CH11231, J. Y. and V. K. Y.), National Institutes of Health (NIH) Grants No. GM055302 (V. K. Y.), No. GM110501 (J. Y.), the Ruth L. Kirschstein National Research Service Award (F32GM116423, F. D. F.), and the Human Frontiers Science Project Award No. RGP0063/ 2013 310 (T. F., J. Y., U. B.) and the Department of Energy, Laboratory Directed Research and Development program at SLAC National Accelerator Laboratory, under Contract No. DE-AC02-76SF00515 (U. B., Y. Z.). We would like to thank Matt Hayes and the CXI technical staff for exper- imental support and Gregory Stewart for visual art.
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Title: Physical Review Letters
  Abbreviation : Phys. Rev. Lett.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Physical Society
Pages: - Volume / Issue: 120 (13) Sequence Number: 133203 Start / End Page: - Identifier: ISSN: 0031-9007
CoNE: /journals/resource/954925433406_1