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024 7 _ |a 10.1103/PhysRevLett.120.133203
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024 7 _ |a 0031-9007
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024 7 _ |a 1079-7114
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024 7 _ |a 1092-0145
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024 7 _ |a 10.3204/PUBDB-2019-00874
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100 1 _ |a Kroll, Thomas
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245 _ _ |a Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes
260 _ _ |a College Park, Md.
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520 _ _ |a 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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700 1 _ |a Alonso-Mori, Roberto
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700 1 _ |a Sokaras, Dimosthenis
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