钚因放射性衰变而出现自辐照老化效应。钚中氦行为是理解钚自辐照老化效应的一个基础和前提。运用分子动力学模拟技术,计算研究了钚中缺陷行为、氦与缺陷的相互作用、氦泡的初始形核过程、氦泡的长大过程以及氦泡对钚材料宏观性能的影...钚因放射性衰变而出现自辐照老化效应。钚中氦行为是理解钚自辐照老化效应的一个基础和前提。运用分子动力学模拟技术,计算研究了钚中缺陷行为、氦与缺陷的相互作用、氦泡的初始形核过程、氦泡的长大过程以及氦泡对钚材料宏观性能的影响等。其中,钚-钚、钚-氦和氦-氦相互作用势分别采用修正嵌入原子多体势(modified embedded atom method,MEAM)、Morse对势和Lennard-Jones对势。主要的计算结果表明,氦原子与空位的结合能较大,在钚的自辐照过程中,两者易于结合并形成氦-空位团簇,成为氦泡的前驱体;氦泡可通过冲出位错环的机制而长大;氦泡的压力在GPa量级,且氦泡引起的基体膨胀很小。展开更多
The hydrogen storage alloys are selected as tritium s torage and boost materials. The alloy’s lattice swells and compresses in the hyd rogen ab /desorption cycle, and the wall stress is induced as a result of ununi f...The hydrogen storage alloys are selected as tritium s torage and boost materials. The alloy’s lattice swells and compresses in the hyd rogen ab /desorption cycle, and the wall stress is induced as a result of ununi form deformation. The pulverization of the bulk material leads to self compacti on and concentration of stress. The relationships of wall stress of hydrogen sto rage bed with cycle number of hydrogen ab /desorption, capacity of hydrogen sto rage, packing fraction and thickness of the wall are studied using strain gauges . In the paper, the relationship of wall stress and capacity of hydrogen storage is mainly discussed.展开更多
Pu can be loaded with H forming complicated continuous solid solutions and compounds,and causing remarkable electronic and structural changes.Full potential linearized augmented plane wave methods combined with Hubbar...Pu can be loaded with H forming complicated continuous solid solutions and compounds,and causing remarkable electronic and structural changes.Full potential linearized augmented plane wave methods combined with Hubbard parameter U and the spin-orbit effects are employed to investigate the electronic and structural properties of stoichiometric and non-stoichiometric face-centered cubic Pu hydrides（PuHx,x=2,2.25,2.5,2.75,3）.The decreasing trend with increasing x of the calculated lattice parameters is in reasonable agreement with the experimental findings.A comparative analysis of the electronic-structure results for a series of PuH x compositions reveals that the lattice contraction results from the associated effects of the enhanced chemical bonding and the size effects involving the interstitial atoms.We find that the size effects are the driving force for the abnormal lattice contraction.展开更多
钚因放射性衰变而出现自辐照老化效应，氦行为和氦泡行为是这种老化效应的集中体现，也是理解这种老化效应的重要途径。运用分子动力学模拟技术，研究了氦泡的释放过程。钚-钚、钚-氦和氦-氦相互作用势分别采用嵌入原子多体势（Embedded...钚因放射性衰变而出现自辐照老化效应，氦行为和氦泡行为是这种老化效应的集中体现，也是理解这种老化效应的重要途径。运用分子动力学模拟技术，研究了氦泡的释放过程。钚-钚、钚-氦和氦-氦相互作用势分别采用嵌入原子多体势（Embedded Atom Method，EAM）、Morse对势和Lennard．Jones对势，计算体系采用表面平板模型。研究结果表明：距离表面一定距离的氦泡中的氦原子发生释放，释放过程受距离表面的距离、温度、氦泡大小以及氦原子密度等因素的影响；展开更多
A modified analytic embedded atom method （MAEAM） potential is constructed for fcc 5-Pu. Molecular dynamics （MD） simulations with the potential are performed to investigate the interactions between two symmetrical ...A modified analytic embedded atom method （MAEAM） potential is constructed for fcc 5-Pu. Molecular dynamics （MD） simulations with the potential are performed to investigate the interactions between two symmetrical tilt grain boundaries （GBs） and point defects such as He atom, vacancy and self-interstitial atom （SIA） in Pu. The calculated results show that point defect formation energies are on average lower than those in the lattice but variations from site to site along the GBs are very remarkable. Both substitutional and interstitial He atoms are trapped at GBs. Interstitial He atom is more strongly bound at the GB core than the substitutional He atom. The binding energy of SIA at GB core is higher than those of He atom and vacancy. GB core can bind many He atoms and SIAs due mainly to the fact that it contains many vacancies. Compared with He atom and SIA, the vacancy far from GB core is difficult to diffuse into the core. The GBs can act as sinks and sources of He atoms and SIAs, which may be a reason for the swelling of Pu after a period of self-irradiation because of the higher concentration of vacancy in the bulk.展开更多
We perform first-principles calculations to investigate the structural, magnetic, electronic, and mechanical properties of face-centered cubic （fcc） Pull2 and fcc Pull3 using the full potential linearized augmented ...We perform first-principles calculations to investigate the structural, magnetic, electronic, and mechanical properties of face-centered cubic （fcc） Pull2 and fcc Pull3 using the full potential linearized augmented plane wave method （FP- LAPW） with the generalized gradient approximation （GGA） and the local spin density approximation （LSDA） taking account of both relativistic and strong correlation effects. The optimized lattice constant a0 = 5.371 A for fcc Pull2 and a0 = 5.343 A for fcc PuH3 calculated in the GGA ＋ sp （spin polarization） ＋ U （Hubbard parameter） ＋ SO （spin-orbit coupling） scheme are in good agreement with the experimental data. The ground state of fcc PuH3 is found to be slightly ferromagnetic. Our results indicate that fcc PuH2 is a metal while fcc PuH3 is a semiconductor with a band gap about 0.35 eV. We note that the SO and the strong correlation between localized Pu 5f electrons are responsible for the band gap of fcc PuH3. The bonds for PuH2 have mainly covalent character while there are covalent bonds in addition to apparent ionicity bonds for PuH3. We also predict the elastic constants of fcc PuH2 and fcc PuH3, which were not observed in the previous experiments.展开更多
Density functional theory（DFT） calculations are performed to investigate the reactivity of Th atom toward ethane C–C bond activation.A comprehensive description of the reaction mechanisms leading to two different r...Density functional theory（DFT） calculations are performed to investigate the reactivity of Th atom toward ethane C–C bond activation.A comprehensive description of the reaction mechanisms leading to two different reaction products is presented.We report a complete exploration of the potential energy surfaces by taking into consideration different spin states.In addition,the intermediate and transition states along the reaction paths are characterized.Total,partial,and overlap population density of state diagrams and analyses are also presented.Furthermore,the natures of the chemical bonding of intermediate and transition states are studied by using topological method combined with electron localization function（ELF） and Mayer bond order.Infrared spectrum（IR） is obtained and further discussed based on the optimized geometries.展开更多
The electronic structure, magnetic states, chemical bonding, and thermodynamic properties of β-US2 are investigated by using first-principles calculation through the density functional theory（DFT） ＋U approach. The...The electronic structure, magnetic states, chemical bonding, and thermodynamic properties of β-US2 are investigated by using first-principles calculation through the density functional theory（DFT） ＋U approach. The obtained band structure exhibits a direct band gap semiconductor at Γ point with a band gap of 0.9 e V for β-US2, which is in good agreement with the recent experimental data. The charge-density differences, the Bader charge analysis, and the Born effective charges suggest that the U–S bonds of the β-US2 have a mixture of covalent and ionic characters, but the ionic character is stronger than covalent character. The Raman-active, infrared-active, and silent modes at the Γ point are further assigned and discussed. The obtained optical-mode frequencies indicate that the three apparent LO–TO（longitudinal optical–transverse optical） splittings occur in B1 u, B2 u, and B3 umodes, respectively. Furthermore, the Helmholtz free energy ？F, the specific heat ？E, vibrational entropy S, and constant volume CVare studied over a range from 0 K-100 K. We expect that our work can provide some valuable information for further experimental investigation of the dielectric properties and the infrared reflectivity spectrum of uranium chalcogenide.展开更多
文摘钚因放射性衰变而出现自辐照老化效应。钚中氦行为是理解钚自辐照老化效应的一个基础和前提。运用分子动力学模拟技术,计算研究了钚中缺陷行为、氦与缺陷的相互作用、氦泡的初始形核过程、氦泡的长大过程以及氦泡对钚材料宏观性能的影响等。其中,钚-钚、钚-氦和氦-氦相互作用势分别采用修正嵌入原子多体势(modified embedded atom method,MEAM)、Morse对势和Lennard-Jones对势。主要的计算结果表明,氦原子与空位的结合能较大,在钚的自辐照过程中,两者易于结合并形成氦-空位团簇,成为氦泡的前驱体;氦泡可通过冲出位错环的机制而长大;氦泡的压力在GPa量级,且氦泡引起的基体膨胀很小。
文摘The hydrogen storage alloys are selected as tritium s torage and boost materials. The alloy’s lattice swells and compresses in the hyd rogen ab /desorption cycle, and the wall stress is induced as a result of ununi form deformation. The pulverization of the bulk material leads to self compacti on and concentration of stress. The relationships of wall stress of hydrogen sto rage bed with cycle number of hydrogen ab /desorption, capacity of hydrogen sto rage, packing fraction and thickness of the wall are studied using strain gauges . In the paper, the relationship of wall stress and capacity of hydrogen storage is mainly discussed.
基金Project supported by the National Natural Science Foundation of China (Grant No. 20971114)
文摘Pu can be loaded with H forming complicated continuous solid solutions and compounds,and causing remarkable electronic and structural changes.Full potential linearized augmented plane wave methods combined with Hubbard parameter U and the spin-orbit effects are employed to investigate the electronic and structural properties of stoichiometric and non-stoichiometric face-centered cubic Pu hydrides（PuHx,x=2,2.25,2.5,2.75,3）.The decreasing trend with increasing x of the calculated lattice parameters is in reasonable agreement with the experimental findings.A comparative analysis of the electronic-structure results for a series of PuH x compositions reveals that the lattice contraction results from the associated effects of the enhanced chemical bonding and the size effects involving the interstitial atoms.We find that the size effects are the driving force for the abnormal lattice contraction.
文摘钚因放射性衰变而出现自辐照老化效应，氦行为和氦泡行为是这种老化效应的集中体现，也是理解这种老化效应的重要途径。运用分子动力学模拟技术，研究了氦泡的释放过程。钚-钚、钚-氦和氦-氦相互作用势分别采用嵌入原子多体势（Embedded Atom Method，EAM）、Morse对势和Lennard．Jones对势，计算体系采用表面平板模型。研究结果表明：距离表面一定距离的氦泡中的氦原子发生释放，释放过程受距离表面的距离、温度、氦泡大小以及氦原子密度等因素的影响；
基金supported by the National Natural Science Foundation of China (Grant No.20801007)the Science and Technology Foundation of China Academy of Engineering Physics (Grant No.2009A0301019)
文摘A modified analytic embedded atom method （MAEAM） potential is constructed for fcc 5-Pu. Molecular dynamics （MD） simulations with the potential are performed to investigate the interactions between two symmetrical tilt grain boundaries （GBs） and point defects such as He atom, vacancy and self-interstitial atom （SIA） in Pu. The calculated results show that point defect formation energies are on average lower than those in the lattice but variations from site to site along the GBs are very remarkable. Both substitutional and interstitial He atoms are trapped at GBs. Interstitial He atom is more strongly bound at the GB core than the substitutional He atom. The binding energy of SIA at GB core is higher than those of He atom and vacancy. GB core can bind many He atoms and SIAs due mainly to the fact that it contains many vacancies. Compared with He atom and SIA, the vacancy far from GB core is difficult to diffuse into the core. The GBs can act as sinks and sources of He atoms and SIAs, which may be a reason for the swelling of Pu after a period of self-irradiation because of the higher concentration of vacancy in the bulk.
基金Project supported by the National Natural Science Foundation of China (Grant No. 20971114)
文摘We perform first-principles calculations to investigate the structural, magnetic, electronic, and mechanical properties of face-centered cubic （fcc） Pull2 and fcc Pull3 using the full potential linearized augmented plane wave method （FP- LAPW） with the generalized gradient approximation （GGA） and the local spin density approximation （LSDA） taking account of both relativistic and strong correlation effects. The optimized lattice constant a0 = 5.371 A for fcc Pull2 and a0 = 5.343 A for fcc PuH3 calculated in the GGA ＋ sp （spin polarization） ＋ U （Hubbard parameter） ＋ SO （spin-orbit coupling） scheme are in good agreement with the experimental data. The ground state of fcc PuH3 is found to be slightly ferromagnetic. Our results indicate that fcc PuH2 is a metal while fcc PuH3 is a semiconductor with a band gap about 0.35 eV. We note that the SO and the strong correlation between localized Pu 5f electrons are responsible for the band gap of fcc PuH3. The bonds for PuH2 have mainly covalent character while there are covalent bonds in addition to apparent ionicity bonds for PuH3. We also predict the elastic constants of fcc PuH2 and fcc PuH3, which were not observed in the previous experiments.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.21371160,21401173,and 11364023)
文摘Density functional theory（DFT） calculations are performed to investigate the reactivity of Th atom toward ethane C–C bond activation.A comprehensive description of the reaction mechanisms leading to two different reaction products is presented.We report a complete exploration of the potential energy surfaces by taking into consideration different spin states.In addition,the intermediate and transition states along the reaction paths are characterized.Total,partial,and overlap population density of state diagrams and analyses are also presented.Furthermore,the natures of the chemical bonding of intermediate and transition states are studied by using topological method combined with electron localization function（ELF） and Mayer bond order.Infrared spectrum（IR） is obtained and further discussed based on the optimized geometries.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.21371160 and 21401173)
文摘The electronic structure, magnetic states, chemical bonding, and thermodynamic properties of β-US2 are investigated by using first-principles calculation through the density functional theory（DFT） ＋U approach. The obtained band structure exhibits a direct band gap semiconductor at Γ point with a band gap of 0.9 e V for β-US2, which is in good agreement with the recent experimental data. The charge-density differences, the Bader charge analysis, and the Born effective charges suggest that the U–S bonds of the β-US2 have a mixture of covalent and ionic characters, but the ionic character is stronger than covalent character. The Raman-active, infrared-active, and silent modes at the Γ point are further assigned and discussed. The obtained optical-mode frequencies indicate that the three apparent LO–TO（longitudinal optical–transverse optical） splittings occur in B1 u, B2 u, and B3 umodes, respectively. Furthermore, the Helmholtz free energy ？F, the specific heat ？E, vibrational entropy S, and constant volume CVare studied over a range from 0 K-100 K. We expect that our work can provide some valuable information for further experimental investigation of the dielectric properties and the infrared reflectivity spectrum of uranium chalcogenide.
