Journal Article

PUBDB-2019-00874

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes

Kroll, T. (Corresponding author)Extern* ; Weninger, C. ; Alonso-Mori, R. ; Sokaras, D. ; Zhu, D. ; Mercadier, L. ; Majety, V. P.CFEL* ; Marinelli, A. ; Lutman, A. ; Guetg, M. W. ; Decker, F.-J. ; Boutet, S. ; Aquila, A. ; Koglin, J. ; Koralek, J. ; DePonte, D. P.XFEL.EU*DESY* ; Kern, J. ; Fuller, F. D. ; Pastor, E. ; Fransson, T. ; Zhang, Y. ; Yano, J. ; Yachandra, V. K. ; Rohringer, N.CFEL*DESY* ; Bergmann, U.

2018
APS College Park, Md.

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Please use a persistent id in citations: doi:10.1103/PhysRevLett.120.133203  doi:10.3204/PUBDB-2019-00874

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 $∼10^{20}$  $W/cm^2$ 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.

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Contributing Institute(s):

1. Theoretical ultrafast X-ray science (FS-TUX)
2. European XFEL Projekt Team (Eur.XFEL)
3. MPSD (CFEL-QOX)

Research Program(s):

1. 6211 - Extreme States of Matter: From Cold Ions to Hot Plasmas (POF3-621) (POF3-621)

Experiment(s):

1. No specific instrument

Appears in the scientific report 2018

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Database coverage:
; ; ; Clarivate Analytics Master Journal List ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; IF >= 5 ; JCR ; NCBI Molecular Biology Database ; Nationallizenz ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Web of Science Core Collection

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