TY - JOUR
AU - Kroll, Thomas
AU - Weninger, Clemens
AU - Alonso-Mori, Roberto
AU - Sokaras, Dimosthenis
AU - Zhu, Diling
AU - Mercadier, Laurent
AU - Majety, Vinay P.
AU - Marinelli, Agostino
AU - Lutman, Alberto
AU - Guetg, Marc W.
AU - Decker, Franz-Josef
AU - Boutet, Sébastien
AU - Aquila, Andy
AU - Koglin, Jason
AU - Koralek, Jake
AU - DePonte, Daniel P.
AU - Kern, Jan
AU - Fuller, Franklin D.
AU - Pastor, Ernest
AU - Fransson, Thomas
AU - Zhang, Yu
AU - Yano, Junko
AU - Yachandra, Vittal K.
AU - Rohringer, Nina
AU - Bergmann, Uwe
TI - Stimulated X-Ray Emission Spectroscopy in Transition Metal Complexes
JO - Physical review letters
VL - 120
IS - 13
SN - 1079-7114
CY - College Park, Md.
PB - APS
M1 - PUBDB-2019-00874
SP - 133203
PY - 2018
AB - 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<sup>20</sup> W/cm<sup>2</sup> 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.
LB - PUB:(DE-HGF)16
C6 - pmid:29694162
UR - <Go to ISI:>//WOS:000428394800008
DO - DOI:10.1103/PhysRevLett.120.133203
UR - https://bib-pubdb1.desy.de/record/419010
ER -