Radiation-induced disorder in compressed lanthanide zirconates

Park, Sulgiye; Tracy, Cameron L.; Zhang, Fuxiang; Park, Changyong; Trautmann, Christina; Tkachev, Sergey N.; Lang, Maik; Mao, Wendy L.; Ewing, Rodney C.

doi:10.1039/c7cp08664d

Title: Radiation-induced disorder in compressed lanthanide zirconates

Journal Article · 11 February 2018 · Physical Chemistry Chemical Physics. PCCP

DOI: https://doi.org/10.1039/c7cp08664d · OSTI ID:1460680

^[1]; Tracy, Cameron L. ^[1]; Zhang, Fuxiang ^[2];

^[3];

^[4]; Tkachev, Sergey N. ^[5]; Lang, Maik ^[6]; Mao, Wendy L. ^[7]; Ewing, Rodney C. ^[1]

Stanford Univ., CA (United States). Dept. of Geological Sciences
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Carnegie Inst. of Washington, Argonne, IL (United States). Geophysical Lab., High Pressure Collaborative Access Team (HPCAT)
GSI-Helmholtz Centre for Heavy Ion Research, Darmstadt (Germany); Technical Univ. of Darmstadt (Germany)
Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Nuclear Engineering
Stanford Univ., CA (United States). Dept. of Geological Sciences; SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

For this study, the effects of swift heavy ion irradiation-induced disordering on the behavior of lanthanide zirconate compounds (Ln₂Zr₂O₇ where Ln = Sm, Er, or Nd) at high pressures are investigated. After irradiation with 2.2 GeV ¹⁹⁷Au ions, the initial ordered pyrochlore structure (Fm$$\bar{3}$$m) transformed to a defect-fluorite structure (Fm$$\bar{3}$$m) in Sm₂Zr₂O₇ and Nd₂Zr₂O₇. For irradiated Er₂Zr₂O₇, which has a defect-fluorite structure, ion irradiation induces local disordering by introducing Frenkel defects despite retention of the initial structure. When subjected to high pressures (>29 GPa) in the absence of irradiation, all of these compounds transform to a cotunnite-like (Pnma) phase, followed by sluggish amorphization with further compression. However, if these compounds are irradiated prior to compression, the high pressure cotunnite-like phase is not formed. Rather, they transform directly from their post-irradiation defect-fluorite structure to an amorphous structure upon compression (>25 GPa). Defects and disordering induced by swift heavy ion irradiation alter the transformation pathways by raising the energetic barriers for the transformation to the high pressure cotunnite-like phase, rendering it inaccessible. As a result, the high pressure stability field of the amorphous phase is expanded to lower pressures when irradiation is coupled with compression. The responses of materials in the lanthanide zirconate system to irradiation and compression, both individually and in tandem, are strongly influenced by the specific lanthanide composition, which governs the defect energetics at extreme conditions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: Carnegie Inst. of Science, Carnegie/DOE Alliance Center (CDAC); National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; Univ. of Notre Dame

Grant/Contract Number:: AC02-76SF00515; FC03-03NA00144; FG02-99ER45775; NA0001974; SC0001089

OSTI ID:: 1460680

Journal Information:: Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 9 Vol. 20; ISSN 1463-9076; ISSN PPCPFQ

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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