Title: Temperature dependence of the radiation tolerance of nanocrystalline pyrochlores A₂Ti₂O₇ (A = Gd, Ho and Lu)

Abstract

A potentially enhanced radiation resistance of nanocrystalline materials, as a consequence of the high density of interfaces and surfaces, has attracted much attention both to understand the fundamental role of these defect sinks and to develop them for high-radiation environments. Here, irradiation response of nanocrystalline A₂Ti₂O₇ (A = Gd, Ho and Lu) pyrochlore powders with grain sizes of 20–30 nm was investigated by 1-MeV Kr²⁺ ion bombardment. In situ transmission electron microscopy (TEM) revealed that the critical amorphization fluence for each nanocrystalline compound at room temperature was greater than that for their coarse-grained counterparts, indicating an enhanced amorphization resistance. The effect of temperature on the irradiation response of one of these compounds, nanocrystalline Lu₂Ti₂O₇, was further examined by performing ion irradiation at an elevated temperature range of 480–600 K. The critical amorphization temperature (T_c) was found to be noticeably higher in nanocrystalline Lu₂Ti₂O₇ (610 K) than its coarse-grained counterpart (480 K), revealing that nanocrystalline Lu₂Ti₂O₇ is less resistant to amorphization compared to its coarse-grained phase under high temperatures. We interpret these results with the aid of atomistic simulations. Molecular statics calculations find that cation antisite defects are less energetically costly to form near surfaces than in the bulk, suggesting thatmore » the nanocrystalline form of these materials is generally less susceptible to amorphization than coarse-grained counterparts at low temperatures where defect kinetics are negligible. In contrast, at high temperatures, the annealing efficiency of antisite defects by cation interstitials is significantly reduced due to the sink properties of the surfaces in the nanocrystalline pyrochlore, which contributes to the observed higher amorphization temperature in the nano-grained phase than in coarse-grained counterpart. Altogether, these results provide new insight into the behavior of nanocrystalline materials under irradiation.« less

Authors:

Wen, J. ^[1]; Sun, C. ^[2]; Dholabhai, P. P. ^[2]; Xia, Y. ^[3]; Tang, M. ^[2]; Chen, D. ^[2]; Yang, D. Y. ^[3]; Li, Y. H. ^[3]; Uberuaga, B. P. ^[2]; Wang, Y. Q.  ^[2]

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+ Show Author Affiliations

1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Lanzhou Univ., Gansu (China)
2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
3. Lanzhou Univ., Gansu (China)

Publication Date:

Mon Mar 21 00:00:00 EDT 2016

Research Org.:

Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Org.:

USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1255267

Alternate Identifier(s):

OSTI ID: 1329963

Report Number(s):

LA-UR-16-20128
Journal ID: ISSN 1359-6454

Grant/Contract Number:  

AC52-06NA25396; 2013LANL8400; AC04-94AL85000; AC02-06CH11357

Resource Type:

Accepted Manuscript

Journal Name:

Acta Materialia

Additional Journal Information:

Journal Volume: 110; Journal Issue: C; Journal ID: ISSN 1359-6454

Publisher:

Elsevier

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE