Stimulated x-ray emission spectroscopy in transition metal complexes

Kroll, Thomas; Weninger, Clemens; Alonso-Mori, Roberto; Sokaras, Dimosthenis; Zhu, Diling; Mercadier, Laurent; Majety, Vinay P.; Marinelli, Agostino; Lutman, Alberto; Guetg, Marc; Decker, Franz-Josef; Boutet, Sebastien; Aquila, Andy; Koglin, Jason; Koralek, Jake; DePonte, Daniel P.; Kern, Jan; Fuller, Franklin D.; Pastor, Ernest; Fransson, Thomas; Zhang, Yu; Yano, Junko; Yachandra, Vittal K.; Rohringer, Nina; Bergmann, Uwe

doi:10.1103/PhysRevLett.120.133203

Title: Stimulated x-ray emission spectroscopy in transition metal complexes

Journal Article · Tue Mar 27 00:00:00 EDT 2018 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.120.133203· OSTI ID:1421553

Kroll, Thomas ^[1]; Weninger, Clemens ^[2]; Alonso-Mori, Roberto ^[3]; Sokaras, Dimosthenis ^[4]; Zhu, Diling ^[3]; Mercadier, Laurent ^[5]; Majety, Vinay P. ^[5]; Marinelli, Agostino ^[6]; Lutman, Alberto ^[6]; Guetg, Marc ^[6]; Decker, Franz-Josef ^[6]; Boutet, Sebastien ^[3]; Aquila, Andy ^[3]; Koglin, Jason ^[3]; Koralek, Jake ^[3]; DePonte, Daniel P. ^[3]; Kern, Jan ^[7]; Fuller, Franklin D. ^[8]; Pastor, Ernest ^[8]; Fransson, Thomas ^[9] more »

SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS) and Stanford Synchrotron Radiation Lightsource (SSRL)
Max Planck Inst. for the Structure and Dynamics of Matter, Hamburg (Germany); SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Max Planck Inst. for the Structure and Dynamics of Matter, Hamburg (Germany)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Accelerator Directorate
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Biophysics and Integrated Bioimaging Division
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Biophysics and Integrated Bioimaging Division
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
Max Planck Inst. for the Structure and Dynamics of Matter, Hamburg (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg, Hamburg (Germany)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS); SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)

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 ~10²⁰ W/cm² 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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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; USDOE Office of Science (SC), Biological and Environmental Research (BER); USDOE Laboratory Directed Research and Development (LDRD) Program; National Institutes of Health (NIH)

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; GM055302; GM110501; F32GM116423; RGP0063/2013 310

OSTI ID:: 1421553

Alternate ID(s):: OSTI ID: 1429943; OSTI ID: 1465454

Journal Information:: Physical Review Letters, Vol. 120, Issue 13; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 38 works

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Amplified spontaneous emission in the extreme ultraviolet by expanding xenon clusters Benediktovitch, Andrei; Mercadier, Laurent; Peyrusse, Olivier Physical Review A, Vol. 101, Issue 6 https://doi.org/10.1103/physreva.101.063412	journal	June 2020
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Amplified spontaneous emission in the extreme ultraviolet by expanding xenon clusters Benediktovitch, Andrei; Mercadier, Laurent; Peyrusse, Olivier Deutsches Elektronen-Synchrotron, DESY, Hamburg https://doi.org/10.3204/pubdb-2020-02451	text	January 2020
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