Abstract
The ultrafast synthesis of ε-Fe3N1+x in a diamond-anvil cell (DAC) from Fe and N2 under pressure was observed using serial exposures of an X-ray free electron laser (XFEL). When the sample at 5 GPa was irradiated by a pulse train separated by 443 ns, the estimated sample temperature at the delay time was above 1400 K, confirmed by in situ transformation of α- to γ-iron. Ultimately, the Fe and N2 reacted uniformly throughout the beam path to form Fe3N1.33, as deduced from its established equation of state (EOS). We thus demonstrate that the activation energy provided by intense X-ray exposures in an XFEL can be coupled with the source time structure to enable exploration of the time-dependence of reactions under high-pressure conditions.
| Original language | English |
|---|---|
| Pages (from-to) | 3246–3252 |
| Number of pages | 7 |
| Journal | Journal of Physical Chemistry Letters |
| Volume | 12 |
| Issue number | 12 |
| Early online date | 25 Mar 2021 |
| DOIs | |
| Publication status | Published - 01 Apr 2021 |
| Externally published | Yes |
Bibliographical note
Funding Information:We thank H. Sinn for experimental assistance and T. Tschentscher and S. Pascarelli for fruitful discussions. This work was supported by the Leader Researcher program (NRF-2018R1A3B1052042) of the Korean Ministry of Science, ICT and Planning (MSIP). We also thank the supports by NRF-2019K1A3A7A09033395 and NRF-NRF-2016K1A4A3914691 grants of the MSIP. We acknowledge European XFEL in Schenefeld, Germany, for provision of X-ray free-electron laser beamtime at Scientific Instrument HED (High Energy Density Science) and thank the staff for their assistance. The authors are indebted to the Helmholtz International Beamline for Extreme Fields (HIBEF) user consortium for the provision of instrumentation and staff that enabled this experiment. We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRA III (beamline P02.2). The research leading to this result has been supported by the project CALIPSOplus under the Grant Agreement 730872 from the EU Framework Program for Research and Innovation HORIZON 2020. Part of this work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344 and by the US Department of Energy through the Los Alamos National Laboratory, operated by Triad National Security, LLC, for the National Nuclear Security Administration (Contract No. 89233218CNA000001). Research presented in this Letter was supported by the Department of Energy, Laboratory Directed Research and Development program at Los Alamos National Laboratory under Project Number 20190643DR and at SLAC National Accelerator Laboratory, under contract DE-AC02-76SF00515. Support is acknowledged from the Panofsky Fellowship at SLAC (awarded to EEM); the DOE Office of Fusion Energy Science funding number FWP100182 (MF and EEM); EPSRC Grants EP/P024513/1 (RSM) and EP/R02927X/1 (E.J.P. and M.I.M.); the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation Programme for Grant Agreement Nos. 670787 (G.F., M.A.B., and G.M.) and 864877 (H.M.). K.A., K.G., R.H., Z.K., H.P.L., and R.R. thank the DFG for support within the Research Unit FOR 2440. S.M. and J.C. acknowledge support from the I-SITE ULNE project MetalCore (R-ERCGEN-19-006-MERKEL). C.S.Y. acknowledges DOE-NNSA (DE-NA0003342), NSF (DMR-1701360), and ARO (W911NF-17-1-0468).
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ASJC Scopus subject areas
- General Materials Science
- Physical and Theoretical Chemistry