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000419010 1001_ $$0P:(DE-H253)PIP1010158$$aKroll, Thomas$$b0$$eCorresponding author
000419010 245__ $$aStimulated X-Ray Emission Spectroscopy in Transition Metal Complexes
000419010 260__ $$aCollege Park, Md.$$bAPS$$c2018
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000419010 520__ $$aWe report the observation and analysis of the gain curve of amplified $Kα$ x-ray emission from solutions of Mn(II) and Mn(VII) complexes using an x-ray free electron laser to create the $1s$ core-hole population inversion. We find spectra at amplification levels extending over 4 orders of magnitude until saturation. We observe bandwidths below the Mn 1s core-hole lifetime broadening in the onset of the stimulated emission. In the exponential amplification regime the resolution corrected spectral width of ∼1.7  eV FWHM is constant over 3 orders of magnitude, pointing to the buildup of transform limited pulses of ∼1  fs duration. Driving the amplification into saturation leads to broadening and a shift of the line. Importantly, the chemical sensitivity of the stimulated x-ray emission to the Mn oxidation state is preserved at power densities of $∼10^{20}$  $W/cm^2$ for the incoming x-ray pulses. Differences in signal sensitivity and spectral information compared to conventional (spontaneous) x-ray emission spectroscopy are discussed. Our findings build a baseline for nonlinear x-ray spectroscopy for a wide range of transition metal complexes in inorganic chemistry, catalysis, and materials science. 
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000419010 7001_ $$aWeninger, Clemens$$b1
000419010 7001_ $$aAlonso-Mori, Roberto$$b2
000419010 7001_ $$aSokaras, Dimosthenis$$b3
000419010 7001_ $$aZhu, Diling$$b4
000419010 7001_ $$aMercadier, Laurent$$b5
000419010 7001_ $$0P:(DE-H253)PIP1032833$$aMajety, Vinay P.$$b6
000419010 7001_ $$aMarinelli, Agostino$$b7
000419010 7001_ $$aLutman, Alberto$$b8
000419010 7001_ $$aGuetg, Marc W.$$b9
000419010 7001_ $$aDecker, Franz-Josef$$b10
000419010 7001_ $$aBoutet, Sébastien$$b11
000419010 7001_ $$aAquila, Andy$$b12
000419010 7001_ $$aKoglin, Jason$$b13
000419010 7001_ $$aKoralek, Jake$$b14
000419010 7001_ $$0P:(DE-H253)PIP1008249$$aDePonte, Daniel P.$$b15$$udesy
000419010 7001_ $$aKern, Jan$$b16
000419010 7001_ $$aFuller, Franklin D.$$b17
000419010 7001_ $$aPastor, Ernest$$b18
000419010 7001_ $$aFransson, Thomas$$b19
000419010 7001_ $$aZhang, Yu$$b20
000419010 7001_ $$aYano, Junko$$b21
000419010 7001_ $$aYachandra, Vittal K.$$b22
000419010 7001_ $$0P:(DE-H253)PIP1010949$$aRohringer, Nina$$b23$$udesy
000419010 7001_ $$aBergmann, Uwe$$b24
000419010 773__ $$0PERI:(DE-600)1472655-5$$a10.1103/PhysRevLett.120.133203$$gVol. 120, no. 13, p. 133203$$n13$$p133203$$tPhysical review letters$$v120$$x1079-7114$$y2018
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