Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes
| Autor: | Sébastien Boutet, Ernest Pastor, Franz-Josef Decker, Agostino Marinelli, Alberto Lutman, Diling Zhu, Roberto Alonso-Mori, Clemens Weninger, Marc W. Guetg, Nina Rohringer, Thomas Kroll, Vittal K. Yachandra, Junko Yano, Jake Koralek, Jason E. Koglin, Yu Zhang, Jan Kern, Daniel P. DePonte, Vinay P. Majety, Thomas Fransson, Franklin D. Fuller, Dimosthenis Sokaras, Laurent Mercadier, Andrew Aquila, Uwe Bergmann |
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| Rok vydání: | 2018 |
| Předmět: |
General Physics
Materials science Astrophysics::High Energy Astrophysical Phenomena General Physics and Astronomy 02 engineering and technology Population inversion 01 natural sciences Article Spectral line Mathematical Sciences law.invention Engineering law 0103 physical sciences Spectral width ddc:530 Emission spectrum Stimulated emission 010306 general physics Spectroscopy 021001 nanoscience & nanotechnology Laser Orders of magnitude (time) Physical Sciences Atomic physics 0210 nano-technology |
| Zdroj: | Physical review letters, vol 120, iss 13 Physical Review Letters Physical review letters 120(13), 133203 (2018). doi:10.1103/PhysRevLett.120.133203 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). doi: 10.1103/PhysRevLett.120.133203. Lawrence Berkeley National Laboratory: Retrieved from: http://www.escholarship.org/uc/item/8rg0n3np |
| DOI: | 10.1103/PhysRevLett.120.133203 |
| Popis: | Physical review letters 120(13), 133203 (2018). doi:10.1103/PhysRevLett.120.133203 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. Published by APS, College Park, Md. |
| Databáze: | OpenAIRE |
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