The Journal of Physical Chemistry Letters, 12, 3246-3252 , (2021) [doi: 10.1021/acs.jpclett.1c00150 ]
X‑ray Free Electron Laser-Induced Synthesis of ε‑Iron Nitride at High Pressures
H. Hwang, T. Kim, H. Cynn, T. Vogt, R. J. Husband, K. Appel, C. Baehtz, O. B. Ball, M. A. Baron, R. Briggs, M. Bykov, E. Bykova, V. Cerantola, J. Chantel, A. L. Coleman, D. Dattlebaum, L. E. Dresselhaus-Marais, J. H. Eggert, L. Ehm, W. J. Evans, G. Fiquet, M. Frost, K. Glazyrin, A. F. Goncharov, Z. Jenei, J. Kim, Z. Konôpková, J. Mainberger, M. Makita, H. Marquardt, E. E. McBride, J. D. McHardy, S. Merkel, G. Morard, E. F. O’Bannon, III, C. Otzen, E. J. Pace, A. Pelka, C. M. Pépin, J. S. Pigott, V. B. Prakapenka, C. Prescher, R. Redmer, S. Speziale, G. Spiekermann, C. Strohm, B. T. Sturtevant, N. Velisavljevic, M. Wilke, C.-S. Yoo, U. Zastrau, H.-P. Liermann, M. I. McMahon, R. S. McWilliams, and Y. Lee
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.
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