TY - JOUR
T1 - Bulk and surface diffusion of neodymium in alpha-uranium
T2 - Ab initio calculations and kinetic Monte Carlo simulations
AU - Jiang, Chao
AU - Aagesen, Larry K.
AU - Andersson, David
AU - Matthews, Christopher
AU - Badry, Fergany
N1 - Funding Information:
This work was fully sponsored by the U.S. Department of Energy, Office of Nuclear Energy, Nuclear Energy Advanced Modeling and Simulation (NEAMS) Program at Idaho National Laboratory operated by Battelle Energy Alliance (BEA) under DOE-NE Idaho Operations Office Contract DE-AC07–05ID14517. Los Alamos National Laboratory, an affirmative action/equal opportunity employer, is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under Contract No. 89233218CNA000001. The authors thank Benjamin Beeler from North Carolina State University for helpful discussions. All DFT calculations are performed using the FALCON supercomputer at Idaho National Laboratory.
Funding Information:
This work was fully sponsored by the U.S. Department of Energy, Office of Nuclear Energy, Nuclear Energy Advanced Modeling and Simulation (NEAMS) Program at Idaho National Laboratory operated by Battelle Energy Alliance (BEA) under DOE-NE Idaho Operations Office Contract DE-AC07?05ID14517. Los Alamos National Laboratory, an affirmative action/equal opportunity employer, is operated by Triad National Security, LLC, for the National Nuclear Security Administration of the U.S. Department of Energy under Contract No. 89233218CNA000001. The authors thank Benjamin Beeler from North Carolina State University for helpful discussions. All DFT calculations are performed using the FALCON supercomputer at Idaho National Laboratory.
Publisher Copyright:
© 2021
PY - 2021/12/15
Y1 - 2021/12/15
N2 - A fundamental understanding of lanthanide transport in metallic fuels is critical for high fidelity modeling of the fuel-cladding chemical interaction (FCCI) phenomenon, which can lead to the formation of brittle intermetallic compounds and premature failure of the cladding. Here we report a combined ab initio density functional theory (DFT) and kinetic Monte Carlo (KMC) study of the bulk diffusivity of Nd in α-U, fully taking into account the effect of radiation enhanced diffusion. The vacancy mechanism is considered to be the dominant mechanism for the bulk diffusion of Nd since a Nd interstitial is found to be intrinsically unstable in α-U. The surface diffusivity of a Nd adatom on α-U (001) surface has been further predicted using KMC simulations parameterized by DFT calculations. The present study suggests that Nd transport via the surface diffusion mechanism can be many orders of magnitude faster than bulk diffusion. Furthermore, the results from the present lower length scale study can be used to inform mesoscale phase-field simulations to determine the effective diffusion coefficient of Nd through α-U with a porous microstructure.
AB - A fundamental understanding of lanthanide transport in metallic fuels is critical for high fidelity modeling of the fuel-cladding chemical interaction (FCCI) phenomenon, which can lead to the formation of brittle intermetallic compounds and premature failure of the cladding. Here we report a combined ab initio density functional theory (DFT) and kinetic Monte Carlo (KMC) study of the bulk diffusivity of Nd in α-U, fully taking into account the effect of radiation enhanced diffusion. The vacancy mechanism is considered to be the dominant mechanism for the bulk diffusion of Nd since a Nd interstitial is found to be intrinsically unstable in α-U. The surface diffusivity of a Nd adatom on α-U (001) surface has been further predicted using KMC simulations parameterized by DFT calculations. The present study suggests that Nd transport via the surface diffusion mechanism can be many orders of magnitude faster than bulk diffusion. Furthermore, the results from the present lower length scale study can be used to inform mesoscale phase-field simulations to determine the effective diffusion coefficient of Nd through α-U with a porous microstructure.
KW - Diffusion
KW - Fuel-cladding chemical interaction
KW - Kinetic Monte Carlo
KW - Lanthanide
UR - http://www.scopus.com/inward/record.url?scp=85115775009&partnerID=8YFLogxK
UR - https://www.mendeley.com/catalogue/540fb436-a4fa-3ed5-8245-a62a3a2ea4eb/
U2 - 10.1016/j.jnucmat.2021.153307
DO - 10.1016/j.jnucmat.2021.153307
M3 - Article
AN - SCOPUS:85115775009
SN - 0022-3115
VL - 557
JO - Journal of Nuclear Materials
JF - Journal of Nuclear Materials
M1 - 153307
ER -