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Title: Radiation-induced disorder in compressed lanthanide zirconates

Abstract

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.

Authors:
ORCiD logo [1];  [1];  [2]; ORCiD logo [3]; ORCiD logo [4];  [5];  [6];  [7];  [1]
  1. Stanford Univ., CA (United States). Dept. of Geological Sciences
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  3. Carnegie Inst. of Washington, Argonne, IL (United States). Geophysical Lab., High Pressure Collaborative Access Team (HPCAT)
  4. GSI-Helmholtz Centre for Heavy Ion Research, Darmstadt (Germany); Technical Univ. of Darmstadt (Germany)
  5. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources (CARS)
  6. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Nuclear Engineering
  7. 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)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA); SLAC National Accelerator Lab., Menlo Park, CA (United States); Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
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, IN (United States). EFRC Materials Science of Actinides (MSA); National Science Foundation (NSF); Carnegie Inst. of Science, Washington, DC (United States). Carnegie/DOE Alliance Center (CDAC)
OSTI Identifier:
1460680
Grant/Contract Number:  
AC02-76SF00515; NA0001974; FG02-99ER45775; SC0001089; AC02-06CH1135; FC03-03NA00144
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 20; Journal Issue: 9; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY

Citation Formats

Park, Sulgiye, Tracy, Cameron L., Zhang, Fuxiang, Park, Changyong, Trautmann, Christina, Tkachev, Sergey N., Lang, Maik, Mao, Wendy L., and Ewing, Rodney C. Radiation-induced disorder in compressed lanthanide zirconates. United States: N. p., 2018. Web. doi:10.1039/c7cp08664d.
Park, Sulgiye, Tracy, Cameron L., Zhang, Fuxiang, Park, Changyong, Trautmann, Christina, Tkachev, Sergey N., Lang, Maik, Mao, Wendy L., & Ewing, Rodney C. Radiation-induced disorder in compressed lanthanide zirconates. United States. doi:10.1039/c7cp08664d.
Park, Sulgiye, Tracy, Cameron L., Zhang, Fuxiang, Park, Changyong, Trautmann, Christina, Tkachev, Sergey N., Lang, Maik, Mao, Wendy L., and Ewing, Rodney C. Mon . "Radiation-induced disorder in compressed lanthanide zirconates". United States. doi:10.1039/c7cp08664d. https://www.osti.gov/servlets/purl/1460680.
@article{osti_1460680,
title = {Radiation-induced disorder in compressed lanthanide zirconates},
author = {Park, Sulgiye and Tracy, Cameron L. and Zhang, Fuxiang and Park, Changyong and Trautmann, Christina and Tkachev, Sergey N. and Lang, Maik and Mao, Wendy L. and Ewing, Rodney C.},
abstractNote = {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.},
doi = {10.1039/c7cp08664d},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 9,
volume = 20,
place = {United States},
year = {2018},
month = {2}
}

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Fig. 1 Fig. 1 : Shows the pyrochlore structure and its relation to this disordered, defect-fluorite structure.

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