DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: A Novel Dual-Step Nucleation Pathway in Crystalline Solids under Neutron Irradiation

Abstract

Innovations in nanostructuring of inorganic crystalline solids are often limited by prerequisite critical nucleation energy and solute supersaturation for formation of a phase. This research provides direct evidence supporting the viability of an unconventional irradiation-induced nanostructuring process, via transmission electron microscopy, that circumvents these preconditions. Using polymorphic silicon carbide (SiC) as a prototype, a surprising two-step nucleation route is demonstrated through which nanoscale distribution of the second phase is achieved by reaction of solutes with neutron irradiation-induced precursors. In the first step, nanoscale α–SiC precipitates in a β–SiC matrix unexpectedly nucleate heterogeneously at structural defects. This occurs at significantly lower temperatures compared with the usual β→α transition temperature. Subsequently, α–SiC precipitate acts as a surrogate template for its structural and compositional transition into a fission product precipitate, palladium silicide. These discoveries provide a modern view of irradiation engineering in polymorphic ceramics for advanced applications.

Authors:
ORCiD logo [1];  [1];  [1]
  1. Idaho National Lab. (INL), Idaho Falls, ID (United States)
Publication Date:
Research Org.:
Idaho National Laboratory (INL), Idaho Falls, ID (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
Contributing Org.:
EMN-HyMARC
OSTI Identifier:
1469359
Report Number(s):
INL/JOU-17-42957-Rev000
Journal ID: ISSN 2045-2322; PII: 18548
Grant/Contract Number:  
AC07-05ID14517
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Meher, Subhashish, van Rooyen, Isabella J., and Lillo, Thomas M. A Novel Dual-Step Nucleation Pathway in Crystalline Solids under Neutron Irradiation. United States: N. p., 2018. Web. doi:10.1038/s41598-017-18548-8.
Meher, Subhashish, van Rooyen, Isabella J., & Lillo, Thomas M. A Novel Dual-Step Nucleation Pathway in Crystalline Solids under Neutron Irradiation. United States. https://doi.org/10.1038/s41598-017-18548-8
Meher, Subhashish, van Rooyen, Isabella J., and Lillo, Thomas M. Mon . "A Novel Dual-Step Nucleation Pathway in Crystalline Solids under Neutron Irradiation". United States. https://doi.org/10.1038/s41598-017-18548-8. https://www.osti.gov/servlets/purl/1469359.
@article{osti_1469359,
title = {A Novel Dual-Step Nucleation Pathway in Crystalline Solids under Neutron Irradiation},
author = {Meher, Subhashish and van Rooyen, Isabella J. and Lillo, Thomas M.},
abstractNote = {Innovations in nanostructuring of inorganic crystalline solids are often limited by prerequisite critical nucleation energy and solute supersaturation for formation of a phase. This research provides direct evidence supporting the viability of an unconventional irradiation-induced nanostructuring process, via transmission electron microscopy, that circumvents these preconditions. Using polymorphic silicon carbide (SiC) as a prototype, a surprising two-step nucleation route is demonstrated through which nanoscale distribution of the second phase is achieved by reaction of solutes with neutron irradiation-induced precursors. In the first step, nanoscale α–SiC precipitates in a β–SiC matrix unexpectedly nucleate heterogeneously at structural defects. This occurs at significantly lower temperatures compared with the usual β→α transition temperature. Subsequently, α–SiC precipitate acts as a surrogate template for its structural and compositional transition into a fission product precipitate, palladium silicide. These discoveries provide a modern view of irradiation engineering in polymorphic ceramics for advanced applications.},
doi = {10.1038/s41598-017-18548-8},
journal = {Scientific Reports},
number = 1,
volume = 8,
place = {United States},
year = {Mon Jan 08 00:00:00 EST 2018},
month = {Mon Jan 08 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Phase Transformations in Metals and Alloys
journal, August 1973


Handbook of SiC properties for fuel performance modeling
journal, September 2007


Ab initio study of the adsorption, migration, clustering, and reaction of palladium on the surface of silicon carbide
journal, March 2011


Palladium transport in SiC
journal, March 2012


Properties of zirconium carbide for nuclear fuel applications
journal, October 2013


Data Compilation for AGR-1 Baseline Coated Particle Composite LEU01-46T
report, April 2006

  • Hunn, John D.; Lowden, Richard Andrew
  • ORNL/TM-2006/019
  • DOI: 10.2172/974594

Identification of silver and palladium in irradiated TRISO coated particles of the AGR-1 experiment
journal, March 2014


The role of Pd in the transport of Ag in SiC
journal, January 2013


Irradiation-induced β to α SiC transformation at low temperature
journal, April 2017


A silicon carbide room-temperature single-photon source
journal, November 2013

  • Castelletto, S.; Johnson, B. C.; Ivády, V.
  • Nature Materials, Vol. 13, Issue 2
  • DOI: 10.1038/nmat3806

Associations of Pd, U and Ag in the SiC layer of neutron-irradiated TRISO fuel
journal, May 2015


Photoinduced Conversion of Silver Nanospheres to Nanoprisms
journal, November 2001


Palladium interaction with silicon carbide
journal, July 2015


Nanostructured ceramics: a review of their potential
journal, January 2001

  • Cain, Markys; Morrell, Roger
  • Applied Organometallic Chemistry, Vol. 15, Issue 5
  • DOI: 10.1002/aoc.153

Nanostructured ceramics: a review of their potential
journal, January 2001

  • Cain, Markys; Morrell, Roger
  • Applied Organometallic Chemistry, Vol. 15, Issue 5
  • DOI: 10.1002/aoc.153

The polymorphic transformations of zirconia
journal, May 1988


A silicon carbide room-temperature single-photon source
journal, November 2013

  • Castelletto, S.; Johnson, B. C.; Ivády, V.
  • Nature Materials, Vol. 13, Issue 2
  • DOI: 10.1038/nmat3806

A Review of Classical and Nonclassical Nucleation Theories
journal, October 2016

  • Karthika, S.; Radhakrishnan, T. K.; Kalaichelvi, P.
  • Crystal Growth & Design, Vol. 16, Issue 11
  • DOI: 10.1021/acs.cgd.6b00794

Interface reactions between Pd thin films and SiC by thermal annealing and SHI irradiation
journal, March 2016

  • Njoroge, E. G.; Theron, C. C.; Skuratov, V. A.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 371
  • DOI: 10.1016/j.nimb.2015.10.014

Irradiation-induced β to α SiC transformation at low temperature
journal, April 2017


The formation of discrete precipitate dispersions on mobile interphase boundaries in iron-base alloys
journal, June 1983


Properties of zirconium carbide for nuclear fuel applications
journal, October 2013


Ultrahigh-Quality Silicon Carbide Single Crystals.
journal, November 2004

  • Nakamura, Daisuke; Gunjishima, Itaru; Yamaguchi, Satoshi
  • ChemInform, Vol. 35, Issue 44
  • DOI: 10.1002/chin.200444243

Light ion irradiation-induced phase transformation in the monoclinic polymorph of zirconia
journal, November 2008


Associations of Pd, U and Ag in the SiC layer of neutron-irradiated TRISO fuel
journal, May 2015


First-principles study of the Pd–Si system and Pd(0 0 1)/SiC(0 0 1) hetero-structure
journal, November 2014


First-principles study of the Pd–Si system and Pd(0 0 1)/SiC(0 0 1) hetero-structure
journal, November 2014


A DFT investigation of the interactions of Pd, Ag, Sn, and Cs with silicon carbide
journal, June 2014

  • Rabone, Jeremy; Kovács, Attila
  • International Journal of Quantum Chemistry, Vol. 114, Issue 22
  • DOI: 10.1002/qua.24720

Ionization-induced annealing of pre-existing defects in silicon carbide
journal, August 2015

  • Zhang, Yanwen; Sachan, Ritesh; Pakarinen, Olli H.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9049

Ultrahigh-quality silicon carbide single crystals
journal, August 2004

  • Nakamura, Daisuke; Gunjishima, Itaru; Yamaguchi, Satoshi
  • Nature, Vol. 430, Issue 7003
  • DOI: 10.1038/nature02810

Electron irradiation-induced phase transformation in α-FeSi[sub 2]
journal, January 2008

  • Naito, Muneyuki; Ishimaru, Manabu; Valdez, James A.
  • Journal of Applied Physics, Vol. 104, Issue 7
  • DOI: 10.1063/1.2986142

Polytypic transformations in silicon carbide
journal, January 1983


Polytypic transformations in silicon carbide
journal, January 1983


Irradiation‐induced phase transformation in type 304 stainless steel
journal, December 1982

  • Hayashi, N.; Takahashi, T.
  • Applied Physics Letters, Vol. 41, Issue 11
  • DOI: 10.1063/1.93379

A Review of Classical and Nonclassical Nucleation Theories
journal, October 2016

  • Karthika, S.; Radhakrishnan, T. K.; Kalaichelvi, P.
  • Crystal Growth & Design, Vol. 16, Issue 11
  • DOI: 10.1021/acs.cgd.6b00794

Microstructural defects in SiC neutron irradiated at very high temperatures
journal, December 2008


Fission products silver, palladium, and cadmium identification in neutron-irradiated SiC TRISO particles using a Cs-Corrected HRTEM
journal, August 2016


Ultrahigh-Quality Silicon Carbide Single Crystals.
journal, November 2004

  • Nakamura, Daisuke; Gunjishima, Itaru; Yamaguchi, Satoshi
  • ChemInform, Vol. 35, Issue 44
  • DOI: 10.1002/chin.200444243

Microstructural defects in SiC neutron irradiated at very high temperatures
journal, December 2008


Irradiation‐induced phase transformation in type 304 stainless steel
journal, December 1982

  • Hayashi, N.; Takahashi, T.
  • Applied Physics Letters, Vol. 41, Issue 11
  • DOI: 10.1063/1.93379

The role of Pd in the transport of Ag in SiC
journal, January 2013


Polytype control of spin qubits in silicon carbide
journal, May 2013

  • Falk, Abram L.; Buckley, Bob B.; Calusine, Greg
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2854

Photoinduced Conversion of Silver Nanospheres to Nanoprisms
journal, November 2001


Identification of silver and palladium in irradiated TRISO coated particles of the AGR-1 experiment
journal, March 2014


Electron irradiation-induced phase transformation in α-FeSi[sub 2]
journal, January 2008

  • Naito, Muneyuki; Ishimaru, Manabu; Valdez, James A.
  • Journal of Applied Physics, Vol. 104, Issue 7
  • DOI: 10.1063/1.2986142

Fission products silver, palladium, and cadmium identification in neutron-irradiated SiC TRISO particles using a Cs-Corrected HRTEM
journal, August 2016


The polymorphic transformations of zirconia
journal, May 1988


Polytype control of spin qubits in silicon carbide
journal, May 2013

  • Falk, Abram L.; Buckley, Bob B.; Calusine, Greg
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2854