First principle study of the behavior of helium in plutonium dioxide

Charge states of point defects in plutonium oxide: A first-principles study

“…(Color online) Defect transition levels of V O , I O , V Pu , and I Pu in PuO 2 . Numbers next to the color bars correspond to the most favorable charge state of the defects.FPs are in agreement with other theoretical results ranging from 3.9∼9.78 eV[34,[57][58][59][60][61].And the formation energy of 3.45 eV for the oxygen FP with two doubly charged point defects is by far the closest result to the experimental data of 2.72∼2.92 eV[62]. This fact indicates that point defects in plutonium dioxide should be charged.…”

First-Principles Energetics of Some Nonmetallic Impurity Atoms in Plutonium Dioxide

“…formation energy of O and Pu vacancies in Pu 4 O 8 are calculated to be 3.98 eV and 14.10 eV,respectively, which is in reasonable agreement with other theoretical results [24][25][26]. Note that the formation energy of a Pu vacancy in Pu 4 O 8 is much larger than in metallic Pu.…”

“…However, previous studies have demonstrated that E i X is still the dominant term even when the above dependences are considered. 26 For the sake of brevity, we discuss here the solution energies of only the most widely studied RG atoms based on incorporation energy.…”

“…In any case, the influence of octahedral interstitial He atoms on the electronic structure of the actinide dioxide hosts was shown to be insignificant. Recently, Tian et al 26 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 5 the very limited theoretical reports on He-atom behavior in PuO 2 , it is worth noting that increasingly more theoretical results have emerged on the electronic structure of Pu for the purpose of understanding many peculiar properties of this most complex element, whose 5f electrons lie at the critical point of the itineration → localization transition. Among these properties, the electronic structure of PuO 2 has been calculated with various different methods such as standard DFT, DFT + U, hybrid DFT, and dynamical mean field theory (DMFT).…”

First-principles DFT +U calculations on the energetics of Ga in Pu, Pu2O3 and PuO2

“…To our knowledge, the behaviors of point defects and impurities in Pu-based materials have only rarely been reported. Limited theoretical reports on the topic have focused only on the defect formation energy of Ga in d-Pu, and rare gases such as He and Xe in PuO 2 [20][21][22][23][24][25][26]. For Ga in PuO 2 and Pu 2 O 3 , no any theoretical report is available; one scarcity can be attributed to the difficulty in the computational efficiency of Pu 2 O 3 containing 80 atoms per unit cell which is a very large computational system from the point view of electronic structure calculations.…”