57Fe Mössbauer isomer shift of pure iron and iron oxides at high pressure—An experimental and theoretical study

Desmarais, Jacques K.; Bi, Wenli; Zhao, Jiyong; Hu, Michael Y.; Alp, Esen; Tse, John S.

doi:10.1063/5.0048141

Title: 57Fe Mössbauer isomer shift of pure iron and iron oxides at high pressure—An experimental and theoretical study

Journal Article · Tue Jun 01 00:00:00 EDT 2021 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0048141· OSTI ID:1830019

^[1]; Bi, Wenli ^[2]; Zhao, Jiyong ^[3];

^[3]; Alp, Esen ^[3];

^[4]

Univ. of Saskatchewan, Saskatoon, SK (Canada); Université de Pau et des Pays de l’Adour (France); Univ. of Torino (Italy)
Univ. of Birmingham (United Kingdom)
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Univ. of Saskatchewan, Saskatoon, SK (Canada)

The 57Fe isomer shift (IS) of pure iron has been measured up to 100 GPa using synchrotron Mössbauer spectroscopy in the time domain. Apart from the expected discontinuity due to the α→ε structural and spin transitions, the IS decreases monotonically with increasing pressure. The absolute shifts were reproduced without semi-empirical calibrations by periodic density functional calculations employing extensive localized basis sets with several common density functionals. However, the best numerical agreement is obtained with the B1WC hybrid functional. Extension of the calculations to 350 GPa, a pressure corresponding to the Earth’s inner core, predicted the IS range of 0.00 to -0.85 mm/s, covering the span from Fe(0) to Fe(VI) compounds measured at ambient pressure. The calculations also reproduced the pressure trend from polymorphs of prototypical iron oxide minerals, FeO and Fe2O3. Analysis of the electronic structure shows a strong donation of electrons from oxygen to iron at high pressure. The assignment of formal oxidation to the Fe atom becomes ambiguous under this condition.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science and Engineering Research Council of Canada

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1830019

Journal Information:: Journal of Chemical Physics, Vol. 154, Issue 21; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: 57Fe Mössbauer isomer shift of pure iron and iron oxides at high pressure—An experimental and theoretical study

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