Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation

Tracy, Cameron L.; Shamblin, Jacob; Park, Sulgiye; Zhang, Fuxiang; Trautmann, Christina; Lang, Maik; Ewing, Rodney C.

doi:10.1103/PhysRevB.94.064102

Title: Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation

Abstract

A₂Sn₂O₇ (A = Nd, SM, Gd, Er, Yb, and Y) materials with the pyrochlore structure were irradiated with 2.2 GeV Au ions to systematically investigate disordering of this system in response to dense electronic excitation. Structural modifications were characterized, over multiple length scales, by transmission electron microscopy, x-ray diffraction, and Raman spectroscopy. Transformations to amorphous and disordered phases were observed, with disordering dominating the structural response of materials with small A -site cation ionic radii. Both the disordered and amorphous phases were found to possess weberite-type local ordering, differing only in that the disordered phase exhibits a long-range, modulated arrangement of weberite-type structural units into an average defect-fluorite structure, while the amorphous phase remains fully aperiodic. Comparison with the behavior of titanate and zirconate pyrochlores showed minimal influence of the high covalency of the Sn-O bond on this phase behavior. Finally, an analytical model of damage accumulation was developed to account for simultaneous amorphization and recrystallization of the disordered phase during irradiation.

Authors:

Tracy, Cameron L. ^[1]; Shamblin, Jacob ^[2]; Park, Sulgiye ^[1]; Zhang, Fuxiang ^[3]; Trautmann, Christina ^[4]; Lang, Maik ^[2]; Ewing, Rodney C. ^[1]

Stanford Univ., CA (United States)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
GSI Helmholtzzentrum für Schwerionenforschung, Darmstadt (Germany); Technische Univ., Darmstadt (Germany)

Publication Date:: Wed Aug 03 00:00:00 EDT 2016

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Materials Science of Actinides (MSA)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:: 1387936

Alternate Identifier(s):: OSTI ID: 1295980

Grant/Contract Number:: SC0001089; DMR-1332208

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 94; Journal Issue: 6; Related Information: MSA partners with University of Notre Dame (lead); University of California, Davis; Florida State University; George Washington University; University of Michigan; University of Minnesota; Oak Ridge National Laboratory; Oregon state University; Rensselaer Polytechnic Institute; Savannah River National Laboratory; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 73 NUCLEAR PHYSICS AND RADIATION PHYSICS; nuclear (including radiation effects); materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly)

Citation Formats


                    Tracy, Cameron L., Shamblin, Jacob, Park, Sulgiye, Zhang, Fuxiang, Trautmann, Christina, Lang, Maik, and Ewing, Rodney C. Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation.  United States: N. p., 2016. 
Web.  doi:10.1103/PhysRevB.94.064102.

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                    Tracy, Cameron L., Shamblin, Jacob, Park, Sulgiye, Zhang, Fuxiang, Trautmann, Christina, Lang, Maik, & Ewing, Rodney C. Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation.  United States.  https://doi.org/10.1103/PhysRevB.94.064102

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                    Tracy, Cameron L., Shamblin, Jacob, Park, Sulgiye, Zhang, Fuxiang, Trautmann, Christina, Lang, Maik, and Ewing, Rodney C. Wed .  
"Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation".  United States.  https://doi.org/10.1103/PhysRevB.94.064102.  https://www.osti.gov/servlets/purl/1387936.

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@article{osti_1387936,

  title        = {Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation},

  author       = {Tracy, Cameron L. and Shamblin, Jacob and Park, Sulgiye and Zhang, Fuxiang and Trautmann, Christina and Lang, Maik and Ewing, Rodney C.},

  abstractNote = {A2Sn2O7 (A = Nd, SM, Gd, Er, Yb, and Y) materials with the pyrochlore structure were irradiated with 2.2 GeV Au ions to systematically investigate disordering of this system in response to dense electronic excitation. Structural modifications were characterized, over multiple length scales, by transmission electron microscopy, x-ray diffraction, and Raman spectroscopy. Transformations to amorphous and disordered phases were observed, with disordering dominating the structural response of materials with small A -site cation ionic radii. Both the disordered and amorphous phases were found to possess weberite-type local ordering, differing only in that the disordered phase exhibits a long-range, modulated arrangement of weberite-type structural units into an average defect-fluorite structure, while the amorphous phase remains fully aperiodic. Comparison with the behavior of titanate and zirconate pyrochlores showed minimal influence of the high covalency of the Sn-O bond on this phase behavior. Finally, an analytical model of damage accumulation was developed to account for simultaneous amorphization and recrystallization of the disordered phase during irradiation.},

  doi          = {10.1103/PhysRevB.94.064102},

  journal      = {Physical Review B},

  number       = 6,

  volume       = 94,

  place        = {United States},

  year         = {Wed Aug 03 00:00:00 EDT 2016},

  month        = {Wed Aug 03 00:00:00 EDT 2016}

}

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Response of Gd₂Ti₂O₇ and La₂Ti₂O₇ to swift-heavy ion irradiation and annealing

Journal Article Park, Sulgiye ; Lang, Maik ; Tracy, Cameron L. ; ... - Acta Materialia

Swift heavy ion (2 GeV ¹⁸¹Ta) irradiation-induced amorphization and temperature-induced recrystallization of cubic pyrochlore Gd₂Ti₂O₇ (Fd3¯m) are compared with the response of a compositionally-similar material with a monoclinic-layered perovskite-type structure, La₂Ti₂O₇ (P2₁). The averaged electronic energy loss, dE/dx, was 37 keV/nm and 35 keV/nm in Gd₂Ti₂O₇ and La₂Ti₂O₇, respectively. Systematic analysis of the structural modifications was completed using transmission electron microscopy, synchrotron X-ray diffraction, Raman spectroscopy, and small-angle X-ray scattering. Increasing ion-induced amorphization with increasing ion fluence was evident in the X-ray diffraction patterns of both compositions by a reduction in the intensity of the diffraction maxima concurrent with themore »« less
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https://doi.org/10.1016/j.actamat.2015.04.010

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Nuclear Waste Disposal--Pyrochlore (A,B,O(7)): Nuclear Waste Form for the Immobilization of Plutonium and ''Minor'' Actinides

Journal Article Ewing, Rodney C ; Weber, William J ; Lian, J - Journal of Applied Physics

During the past half-century, the nuclear fuel cycle has generated approximately 1,400 metric tons of plutonium and substantial quantities of the ''minor'' actinides, such as Np, Am and Cm. The successful disposition of these actinides has an important impact on the strategy for developing advanced nuclear fuel cycles, weapons proliferation and the geologic disposal of high-level radioactive waste. During the last decade, there has been substantial interest in the use of the isometric pyrochlore structure-type, A,B,O, for the immobilization of actinides. Most of the interest has focused on titanate-pyrochlore because of its chemical durability; however, these compositions experience a radiation-inducedmore »« less
https://doi.org/10.1063/1.1707213

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Title: Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation

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Connection between oxygen-ion conductivity of pyrochlore fuel-cell materials and structural change with composition and temperature journal, April 2000

Radiation damage effects in the perovskite Ca Ti O 3 and resistance of materials to amorphization journal, October 2004

Raman and x-ray absorption spectroscopy study of the phase evolution induced by mechanical milling and thermal treatments in R 2 Ti 2 O 7 pyrochlores journal, September 2011

Response of Gd2Ti2O7 and La2Ti2O7 to swift-heavy ion irradiation and annealing journal, July 2015

X-Ray Determination of the Structure of Glass journal, December 1934

Review of A2B2O7 pyrochlore response to irradiation and pressure journal, October 2010

Understanding resistance to amorphization by radiation damage journal, November 2004

X-ray line broadening from filed aluminium and wolfram journal, January 1953

Solid-density plasma nanochannel generated by a fast single ion in condensed matter journal, March 2009

Modelling the effects of electronic excitations in ionic-covalent materials journal, April 2012

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides journal, September 1976

Complex ceramic structures. I. Weberites journal, May 2009

Ion implantation in semiconductors—Part II: Damage production and annealing journal, January 1972

Rare-earth titanates and stannates of pyrochlore structure; vibrational spectra and force fields journal, April 1983

Effect of composition on the behavior of pyrochlores irradiated with swift heavy ions journal, February 2012

Phase transformations induced by high electronic excitation in ion-irradiated Gd2(ZrxTi1−x)2O7 pyrochlores journal, November 2010

Etude de la transformation ordre-desordre de la structure fluorite a la structure pyrochlore pour des phases (1−x) ZrO2  x Ln2O3 journal, November 1974

First-principles calculation of defect-formation energies in the Y 2 ( Ti , Sn , Zr ) 2 O 7 pyrochlore journal, August 2004

Criteria for bombardment-induced structural changes in non-metallic solids journal, January 1975

Characterization of ion-induced radiation effects in nuclear materials using synchrotron x-ray techniques journal, May 2015

Structural response of titanate pyrochlores to swift heavy ion irradiation journal, September 2016

Incorporation of uranium in pyrochlore oxides and pressure-induced phase transitions journal, November 2014

Study by Raman spectroscopy of order-disorder phenomena occurring in some binary oxides with fluorite-related structures journal, August 1976

Low-Thermal-Conductivity Rare-Earth Zirconates for Potential Thermal-Barrier-Coating Applications journal, December 2002

Defect formation and accumulation in CeO2 irradiated with swift heavy ions journal, November 2013

SRIM – The stopping and range of ions in matter (2010) journal, June 2010

Irradiation damage in Gd 2 Ti 2 O 7 single crystals: Ballistic versus ionization processes journal, August 2011

Structural modifications of Gd 2 Zr 2- x Ti x O 7 pyrochlore induced by swift heavy ions: Disordering and amorphization journal, April 2009

Making tracks: electronic excitation roles in forming swift heavy ion tracks journal, November 2009

First-principles study of structural, elastic, and bonding properties of pyrochlores journal, August 2005

Radiation Tolerance of Complex Oxides journal, August 2000

Structure change of pyrochlore Sm2Ti2O7 at high pressures journal, May 2005

Crystal structure of fluorite-related Ln3SbO7 (Ln=La–Dy) ceramics studied by synchrotron X-ray diffraction and Raman scattering journal, July 2013

Raman spectra of oxides with the fluorite structure journal, August 1973

La3TaO7 derivatives with Weberite structure type: Possible electrolytes for solid oxide fuel cells and high temperature electrolysers journal, November 2010

A lattice dynamical investigation of the Raman and the infrared frequencies of the cubic A2Sn2O7 pyrochlores journal, November 2001

Structural modifications in pyrochlores caused by ions in the electronic stopping regime journal, October 2008

First-principles prediction of disordering tendencies in pyrochlore oxides journal, March 2009

Pressure-Induced Disordering and Anomalous Lattice Expansion in La 2 Zr 2 O 7 Pyrochlore journal, June 2010

Simulation of defects and defect processes in fluorite and fluorite related oxides: Implications for radiation tolerance journal, February 2007

Probing disorder in isometric pyrochlore and related complex oxides journal, February 2016

Optimum pyrochlore compositions for low thermal conductivity journal, February 2004

Frustration under pressure: Exotic magnetism in new pyrochlore oxides journal, April 2015

Yttrium pyrogermanate, Y 2 Ge 2 O 7 journal, September 2007

Magnetic pyrochlore oxides journal, January 2010

Ion Irradiation of Ternary Pyrochlore Oxides journal, July 2009

Models and mechanisms of irradiation-induced amorphization in ceramics journal, May 2000

Phenomenological model for the formation of heterogeneous tracks in pyrochlores irradiated with swift heavy ions journal, January 2012

Atomic scale simulations of pyrochlore oxides with a tight-binding variable-charge model: implications for radiation tolerance journal, January 2014

Nature of the chemical bond and prediction of radiation tolerance in pyrochlore and defect fluorite compounds journal, April 2007

Effect of Structure and Thermodynamic Stability on the Response of Lanthanide Stannate Pyrochlores to Ion Beam Irradiation journal, February 2006

Nanoscale phase transitions under extreme conditions within an ion track journal, July 2010

Electron and Nuclear Densities of a Pyrochlore, Y 2 Sn 2 O 7 Studied by the Maximum Entropy Method journal, January 1999

Oxide pyrochlores — A review journal, January 1983

Krypton ion irradiation-induced amorphization and nano-crystal formation in pyrochlore Lu 2 Ti 2 O 7 at room temperature journal, December 2015

Short-Range Atomic Ordering in Amorphous Ion-Tracks in Pyrochlores journal, August 2015

Local Structure of Rare Earth Niobates (RE 3 NbO 7 , RE = Y, Er, Yb, Lu) for Proton Conduction Applications ▴ journal, November 2012

Nuclear waste disposal—pyrochlore (A2B2O7): Nuclear waste form for the immobilization of plutonium and “minor” actinides journal, June 2004

A model for the formation of amorphous Si by ion bombardment journal, January 1970

Spectroscopic Investigations of the Structural Phase Transition in Gd 2 (Ti 1 - y Zr y ) 2 O 7 Pyrochlores journal, May 2002

Fluorite-related phases Ln3MO7, Ln = rare earth, Y or Sc, M = Nb, Sb, or Ta journal, January 1979

Ion-irradiation-induced amorphization of La 2 Zr 2 O 7 pyrochlore journal, August 2002

Synchrotron X-ray diffraction and Raman spectroscopy of Ln3NbO7 (Ln=La, Pr, Nd, Sm-Lu) ceramics obtained by molten-salt synthesis journal, January 2014

Single-ion tracks in Gd 2 Zr 2 − x Ti x O 7 pyrochlores irradiated with swift heavy ions journal, June 2009

Swift heavy ion track formation in Gd2Zr2−Ti O7 pyrochlore: Effect of electronic energy loss journal, October 2014

Two-dimensional detector software: From real detector to idealised image or two-theta scan journal, January 1996

How the nature of the chemical bond governs resistance to amorphization by radiation damage journal, May 2005

Connection between oxygen-ion conductivity of pyrochlore fuel-cell materials and structural change with composition and temperature
journal, April 2000

Radiation damage effects in the perovskite $Ca Ti O_{3}$ and resistance of materials to amorphization
journal, October 2004

Raman and x-ray absorption spectroscopy study of the phase evolution induced by mechanical milling and thermal treatments in $R$ $_{2}$ Ti $_{2}$ O $_{7}$ pyrochlores
journal, September 2011

Response of Gd2Ti2O7 and La2Ti2O7 to swift-heavy ion irradiation and annealing
journal, July 2015

X-Ray Determination of the Structure of Glass
journal, December 1934

Review of A2B2O7 pyrochlore response to irradiation and pressure
journal, October 2010

Understanding resistance to amorphization by radiation damage
journal, November 2004

X-ray line broadening from filed aluminium and wolfram
journal, January 1953

Solid-density plasma nanochannel generated by a fast single ion in condensed matter
journal, March 2009

Modelling the effects of electronic excitations in ionic-covalent materials
journal, April 2012

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

Complex ceramic structures. I. Weberites
journal, May 2009

Ion implantation in semiconductors—Part II: Damage production and annealing
journal, January 1972

Rare-earth titanates and stannates of pyrochlore structure; vibrational spectra and force fields
journal, April 1983

Effect of composition on the behavior of pyrochlores irradiated with swift heavy ions
journal, February 2012

Phase transformations induced by high electronic excitation in ion-irradiated Gd2(ZrxTi1−x)2O7 pyrochlores
journal, November 2010

Etude de la transformation ordre-desordre de la structure fluorite a la structure pyrochlore pour des phases (1−x) ZrO2  x Ln2O3
journal, November 1974

First-principles calculation of defect-formation energies in the $Y_{2} {(Ti, Sn, Zr)}_{2} O_{7}$ pyrochlore
journal, August 2004

Criteria for bombardment-induced structural changes in non-metallic solids
journal, January 1975

Characterization of ion-induced radiation effects in nuclear materials using synchrotron x-ray techniques
journal, May 2015

Structural response of titanate pyrochlores to swift heavy ion irradiation
journal, September 2016

Incorporation of uranium in pyrochlore oxides and pressure-induced phase transitions
journal, November 2014

Study by Raman spectroscopy of order-disorder phenomena occurring in some binary oxides with fluorite-related structures
journal, August 1976

Low-Thermal-Conductivity Rare-Earth Zirconates for Potential Thermal-Barrier-Coating Applications
journal, December 2002

Defect formation and accumulation in CeO2 irradiated with swift heavy ions
journal, November 2013

SRIM – The stopping and range of ions in matter (2010)
journal, June 2010

Irradiation damage in Gd $_{2}$ Ti $_{2}$ O $_{7}$ single crystals: Ballistic versus ionization processes
journal, August 2011

Structural modifications of Gd ₂ Zr _{2- x} Ti _x O ₇ pyrochlore induced by swift heavy ions: Disordering and amorphization
journal, April 2009

Making tracks: electronic excitation roles in forming swift heavy ion tracks
journal, November 2009

First-principles study of structural, elastic, and bonding properties of pyrochlores
journal, August 2005

Radiation Tolerance of Complex Oxides
journal, August 2000

Structure change of pyrochlore Sm2Ti2O7 at high pressures
journal, May 2005

Crystal structure of fluorite-related Ln3SbO7 (Ln=La–Dy) ceramics studied by synchrotron X-ray diffraction and Raman scattering
journal, July 2013

Raman spectra of oxides with the fluorite structure
journal, August 1973

La3TaO7 derivatives with Weberite structure type: Possible electrolytes for solid oxide fuel cells and high temperature electrolysers
journal, November 2010

A lattice dynamical investigation of the Raman and the infrared frequencies of the cubic A2Sn2O7 pyrochlores
journal, November 2001

Structural modifications in pyrochlores caused by ions in the electronic stopping regime
journal, October 2008

First-principles prediction of disordering tendencies in pyrochlore oxides
journal, March 2009

Pressure-Induced Disordering and Anomalous Lattice Expansion in ${La}_{2} {Zr}_{2} O_{7}$ Pyrochlore
journal, June 2010

Simulation of defects and defect processes in fluorite and fluorite related oxides: Implications for radiation tolerance
journal, February 2007

Probing disorder in isometric pyrochlore and related complex oxides
journal, February 2016

Optimum pyrochlore compositions for low thermal conductivity
journal, February 2004

Frustration under pressure: Exotic magnetism in new pyrochlore oxides
journal, April 2015

Yttrium pyrogermanate, Y ₂ Ge ₂ O ₇
journal, September 2007

Magnetic pyrochlore oxides
journal, January 2010

Ion Irradiation of Ternary Pyrochlore Oxides
journal, July 2009

Models and mechanisms of irradiation-induced amorphization in ceramics
journal, May 2000

Phenomenological model for the formation of heterogeneous tracks in pyrochlores irradiated with swift heavy ions
journal, January 2012

Atomic scale simulations of pyrochlore oxides with a tight-binding variable-charge model: implications for radiation tolerance
journal, January 2014

Nature of the chemical bond and prediction of radiation tolerance in pyrochlore and defect fluorite compounds
journal, April 2007

Effect of Structure and Thermodynamic Stability on the Response of Lanthanide Stannate Pyrochlores to Ion Beam Irradiation
journal, February 2006

Nanoscale phase transitions under extreme conditions within an ion track
journal, July 2010

Electron and Nuclear Densities of a Pyrochlore, Y ₂ Sn ₂ O ₇ Studied by the Maximum Entropy Method
journal, January 1999

Oxide pyrochlores — A review
journal, January 1983

Krypton ion irradiation-induced amorphization and nano-crystal formation in pyrochlore Lu ₂ Ti ₂ O ₇ at room temperature
journal, December 2015

Short-Range Atomic Ordering in Amorphous Ion-Tracks in Pyrochlores
journal, August 2015

Local Structure of Rare Earth Niobates (RE ₃ NbO ₇ , RE = Y, Er, Yb, Lu) for Proton Conduction Applications ^▴
journal, November 2012

Nuclear waste disposal—pyrochlore (A2B2O7): Nuclear waste form for the immobilization of plutonium and “minor” actinides
journal, June 2004

A model for the formation of amorphous Si by ion bombardment
journal, January 1970

Spectroscopic Investigations of the Structural Phase Transition in Gd ₂ (Ti ₁ _- _y Zr _y ) ₂ O ₇ Pyrochlores
journal, May 2002

Fluorite-related phases Ln3MO7, Ln = rare earth, Y or Sc, M = Nb, Sb, or Ta
journal, January 1979

Ion-irradiation-induced amorphization of ${La}_{2} {Zr}_{2} O_{7}$ pyrochlore
journal, August 2002

Synchrotron X-ray diffraction and Raman spectroscopy of Ln3NbO7 (Ln=La, Pr, Nd, Sm-Lu) ceramics obtained by molten-salt synthesis
journal, January 2014

Single-ion tracks in ${Gd}_{2} {Zr}_{2 - x} {Ti}_{x} O_{7}$ pyrochlores irradiated with swift heavy ions
journal, June 2009

Swift heavy ion track formation in Gd2Zr2−Ti O7 pyrochlore: Effect of electronic energy loss
journal, October 2014

Two-dimensional detector software: From real detector to idealised image or two-theta scan
journal, January 1996

How the nature of the chemical bond governs resistance to amorphization by radiation damage
journal, May 2005