钚自辐照老化过程中氦效应理论研究进展

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（modifiedembeddedatommethod,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。     

First-principles approach to the properties of point defects and small helium-vacancy clusters in palladium

First-principles calculations based on density functional theory (DFT) have been performed to study the properties of interstitial helium atoms, the vacancy, substitutional, and small helium-vacancy clusters He_mV_n (m, n = 0-4) in palladium. The result indicates that the vacancy has the strongest ability of capturing helium atoms and the octahedral interstitial configuration is more stable than the tetrahedral one, while the energy difference between them is very small. In the palladium crystal, helium atom will migrate from one octahedral interstitial site to another one through the O-T-O path. The formation energies and binding energies of an interstitial helium atom and an isolated vacancy to the helium-vacancy clusters are also determined in palladium. It is found that the formation energies increase with the increasing of helium atoms and the binding energies mainly depend on the helium to vacancy ratio of the clusters rather than the cluster size.     

Ab initio study of Kr in hcp Ti: Diffusion, formation and stability of small Kr-vacancy clusters

Ab initio electronic structure calculations have been performed to study the formation and migration of Kr impurities, and the stability of small Kr-vacancy clusters for clusters with up to four vacancies and four Kr atoms, in hcp Ti. Both the substitutional and the interstitial configurations of Kr are found to be stable. The octahedral configuration is however found to be more stable than the tetrahedral. Interstitial Kr atoms are shown to have attractive interactions and a low migration barrier, suggesting that, at low temperature, Kr bubble formation is possible, even in the absence of vacancies. We also find vacancy clusters to be stable. The binding energies of an interstitial Kr atom and a vacancy to a Kr-vacancy cluster are obtained from the calculated formation energies of the clusters. The stability of small-vacancy clusters is found to be dependent on Kr-vacancy ratio. The trends of the calculated binding energies are discussed in terms of providing further insights on the behaviour of Kr in implanted Ti.     

Study on C-W interactions by molecular dynamics simulations

By means of molecular dynamics simulations using bond-order potential (BOP), we have investigated the interactions between carbon (C) atoms and bcc tungsten (W). At finite temperature (T = 300 K) with incident energy of C atoms ranging from 0.5 to 100 eV at normal incidence, the projected range distribution as a function of incident energy and the average depth have been depicted. The properties of vacancy, vacancy migration, interstitial and substitutional C atoms in W have been determined. The most stable configuration for an interstitial C atom in W is in octahedral position and the lattice distortion around the C atom in octahedral interstitial configuration occurs along 〈1 0 0〉 and 〈1 1 0〉 directions. The mutual interaction between a vacancy and near interstitial C atom is also studied.     

Trapping of helium atoms in aluminum

Using molecular dynamic simulation, the effect of vacancy clusters on the interstitial helium atoms was studied in the early stages of helium bubble formation in the vessel of fission reactor, aluminum. The simulation shows, that there is a slight propensity of helium interstitial clustering without initial vacancies in aluminum. When vacancy cluster was introduced, the behavior of interstitial helium atoms was strongly dependent on the ratio of vacancy to helium. The interstitial helium atoms will be attracted in the center of the vacancy cluster when the ratio of vacancy to helium is much larger than 1, and when the ratio approaches 1, the helium will recombine with the vacancies, and, form in substitutions. In the case of the ratio of vacancy to helium less than 1, some aluminum interstitials will be created. The result shows, that the vacancy cluster plays a role of a nucleation center for helium atoms to accelerate the helium bubble growth.     

Molecular dynamics simulation of helium-vacancy interaction in plutonium

The formation energies of small He_nV_m clusters (n and m denote the number of He atoms and vacancy, respectively) in Pu have been calculated with molecular dynamics (MD) simulations using the embedded atom method (EAM) potential, the Mores potential and the Lennard-Jones potential for describing the interactions of Pu-Pu, Pu-He and He-He, respectively. The binding energies of an interstitial He atom, an isolated vacancy and a self-interstitial Pu atom to a He_nV_m cluster are also obtained from the calculated formation energies of the clusters. All the binding energies mainly depend on the He-vacancy ratio (n/m) of clusters rather than the clusters size. With the increase of the n/m ratio, the binding energies of a He atom and a Pu atom to a He_nV_m cluster decrease with the ratio, and the binding energy of a vacancy to a He_nV_m cluster increases. He atoms act as a catalyst for the formation of He_nV_m clusters.     

Atomistic simulations of the elastic properties of helium bubble embedded aluminum

The helium bubble has significant consequence to the mechanical properties of irradiated materials. The influence of embedded helium bubble to the elastic properties of aluminum has been investigated by molecular dynamics (MD) simulations. The interaction between aluminum atoms and the interaction between helium atoms are described by an embedded-atom-method (EAM) many-body potential and a pair potential, respectively. Another pair potential, which is parameterized based on ab initio calculation, is used to describe the interaction between aluminum and helium atoms, and its validation under pressure up to 10 GPa is reasonable demonstrated by the electron density calculation. For the composite system consisting of 62,500 aluminum atoms and one helium bubble with various diameters, its elastic constants are calculated properly by stress-strain relation rather than by energy-strain relation. The results show that elastic constants c₁₁, c₁₂ and c₄₄ decrease with increasing of the volume of the helium bubble, and remain almost invariable with the internal pressure of the helium bubble. The main reason is under high-pressure the helium is softer than aluminum, and the soft effect overwhelms the hard effect of internal pressure of helium bubble.     

Positron lifetime calculations of defects in fusion irradiated beryllium

Numerical quantum-mechanical positron lifetime calculations were performed for mono-vacancies, di-vacancies, tri-vacancies and small nano-voids containing helium and hydrogen in neutron irradiated beryllium. Helium and hydrogen atoms in the sample after the irradiation are considered as atoms forming interstitial O-type loops. Spherical clusters of vacancies are included in the calculations as a reference. It was found that the presence of He and H atoms significantly changes the positron lifetime in irradiated beryllium. A correlation between the positron lifetime and mutual position of vacancies in nano-voids and interstitial loops was established.     

The interaction of defects in titanium: A molecular dynamics study

Behaviors and properties of helium in titanium were explored by molecular dynamics (MD) simulation in this study. The influence of He number, vacancy number and He density (ratio of helium to vacancy) on the thermal stability of HenVm clusters (where n and m denote the number of He atoms and vacancies) were investigated. Meanwhile, interactions among He atoms, SIA atoms and vacancies were discussed. The results demonstrate that the binding energies of an interstitial helium atom primarily depend on He and vacancy numbers rather than the helium-to-vacancy ratio (n/m). It is different from the previous report of other researchers. The binding energies of an isolated vacancy and a self-interstitial titanium atom depend on both the number of helium atoms and the helium-to-vacancy ratio (n/m) of clusters. The thermal stability of clusters is decided by the competitive processes among thermal emissions of vacancy, SIA and helium atom.     

Molecular Statics Simulation of Hydrogen Defect Interaction in Tungsten

Hydrogen(H) defect interactions have been investigated by molecular statics simulations in tungsten(W),including H-H interactions and interactions between H and W selfinterstitial atoms.The interactions between H and small H-vacancy clusters are also demonstrated;the binding energies of an H,a vacancy and a self-interstitial W to an H-vacancy cluster depend on the H-to-vacancy ratio.We conclude that H bubble formation needs a high concentration of H in W for the H bubble nucleation and growth,which are also governed by the H-to-vacancy ratio of the cluster.The vacancy first combines with H atoms and a cluster forms,then the H-vacancy cluster goes through the whole process of vacancy capture,H capture,and vacancy capture again,and as a result the H-vacancy cluster grows larger and larger.Finally,the H bubble forms.     

Double resonant neutralization in hyperthermal energy alkali ion scattering at clean metal surfaces

Resonant neutralization of hyperthermal Na⁺ ions impinging on clean surfaces is studied, focussing on long lived electronic interactions involving the projectile and a target atom. Specific trajectories are considered where the incident particle undergoes multiple collisions within the first surface layers, interacting simultaneously with several target atoms, which leads to single emission of a surface atom that can resonantly exchange charge with both the solid and the projectile. The system is described via a semi-empirical, one-electron potential that includes the effect of a plane metal surface, with projected band gap, the projectile, whose charge state will be eventually investigated, and the substrate atom. On this basis, a model Hamiltonian of the Anderson-Newns type is constructed and the calculated neutralization probability is compared with the angle resolved neutral fraction measured by Keller et al. [C.A. Keller, C.A. DiRubio, G.A. Kimmel, B.H. Cooper, Phys. Rev. Lett. 75 (1995) 1654].     

氦离子辐照烧结碳化硅损伤效应研究

利用中国科学院近代物理研究所320 kV高压平台提供的氦离子辐照烧结碳化硅,辐照温度从室温到1 000 ℃,辐照注量为1015~1017 cm-2。辐照完成后,进行退火处理,然后开展透射电子显微镜、拉曼光谱、纳米硬度和热导率测试。研究发现,烧结碳化硅中氦泡形核阈值注量低于单晶碳化硅。同时,氦泡形貌和尺寸与辐照温度、退火温度有关。另外,对辐照产生的晶格缺陷、元素偏析进行了研究。结果表明,辐照产生了大量的缺陷团簇,同时氦泡生长也会发射间隙子,在氦泡周围形成间隙型位错环。在晶界处,容易发生碳原子聚集。辐照导致材料先发生硬化而后发生软化,且热导率降低。     

体心立方钨和铁中氦泡生长机制模拟研究进展

体心立方金属钨和铁作为核聚变反应堆的第一壁面向等离子体材料和第一壁结构材料处于高剂量的中子辐照环境中。辐照过程产生的氦原子易在金属内聚集形成氦泡,对材料微观结构和宏观力学性能产生极大影响。本文通过综合分析文献中关于通过第一性原理、分子动力学和蒙特卡罗方法对氦泡形核和生长机制,比较了不同模拟条件下氦泡的演化机制。分析表明,晶界、位错、空位等内部缺陷和温度等外部条件都对氦泡的形核及其生长机制有影响。在此基础上提出了下一步研究方向和思路。     

含氦Ti膜的透射电镜研究

在氦气和氩气混合气氛中用磁控溅射法制备含氦Ti膜。应用透射电镜观察不同氦气和氩气流量比对Ti膜微观结构及氦泡形貌和分布的影响,并研究退火温度对氦泡聚集和长大行为的影响。研究观测到,Ti膜中氦泡的尺寸随氦流量的增加而增大,氦泡的密度随氦流量改变出现一最大值;温度低于0.5 Tm时,He泡以泡迁移和合并机制(MC)长大;温度高于0.5 Tm时,He从小泡离解,被大泡吸收,以OR机制长大,氦泡尺寸明显增加。     

Helium solubility and behaviour in uranium dioxide

A set of devices was developed in order to infuse UO₂ disks with helium, at high temperature and pressure, to measure the helium infused quantity and from these data to calculate the helium solubility in the UO₂ matrix. Samples of UO₂ single crystal and UO₂ polycrystal were infused at a temperature of 1473 and 1743 K in a helium atmosphere ranging between 50 and 100 MPa. These samples were then annealed and the helium released was measured with a mass spectrometer. From the obtained spectra it was possible to give an interpretation of the helium release mechanism and to calculate its solubility in the UO₂ lattice in these specific thermodynamic conditions. Additionally to the helium solubility measurement from infused samples, a 37 years old sample of ²³⁸PuO₂, retrieved from an old ²⁴²Cm radioisotope thermoelectric generator (RTG), containing radiogenic helium, was also measured to widen perspectives of this kind of measurements to damaged sample more representative of spent fuel.     

含空洞双晶α-Fe中He团簇的分子动力学研究

本文利用分子动力学方法和Gao等最近发现的Fe-He势函数研究了α-Fe倾侧晶界在300 K下弛豫与单轴拉伸下He团簇的演变过程及材料内部空洞缺陷对He团簇的影响,并分析对比了拉伸过程中晶界的应力 应变曲线。结果显示：对比两种空洞位置,在弛豫过程中He原子更易在晶界面上的空洞中聚集发生He团簇;在拉伸加载阶段,晶界面空洞与晶界面相交处和基体内部空洞与晶界相切位置易产生微裂纹,成为断裂初始点。对比应力-应变曲线可知,其基体内部含有空洞时的双晶模型断裂应力及断裂应变最小。     

金属氚化物中氦泡生长显微机制研究现状与发展趋势

氚是核聚变反应的关键核燃料,金属氚化物是国防领域及核聚变能源领域中的重要功能材料。氚衰变产生的氦原子及其演化过程严重影响金属氚化物的宏观性能,氦泡的形成与驻留又会影响金属氚化物的贮氚性能,金属氚化物中氦泡生长机制的研究是备受关注的重要科学问题。受限于氚的放射性和缺乏对氚与氦等轻元素原子的显微分析技术,氦泡生长模型的研究长期处于唯象理论阶段。近年来,随着电子显微分析技术的进步,提出了更加准确分析氦泡信息的新技术,氦泡生长显微机制研究取得了新的突破。本文将首先简要介绍金属氚化物中氦泡生长机制的主要理论与成果,然后介绍电子显微分析技术的发展及研究成果,最后针对氦泡生长显微机制的研究趋势做出展望。     

Dispersion coefficients for interactions between positronium and light atoms with pure Coulomb and screened Coulomb potentials

The Van der Waals two-body dispersion coefficients for interactions between the positronium (Ps) atom and light atoms have been investigated using highly correlated exponential basis functions in the framework of both pure Coulomb and screened Coulomb potentials. The C₆, C₈ and C₁₀ coefficients for Ps-Ps and Ps-H interactions, and the C₆ coefficients for Ps-He interactions for both the screened and unscreened cases, are reported.     

Energetics and self-diffusion behavior of Zr atomic clusters on a Zr(0 0 0 1) surface

Using a molecular dynamics method and a modified analytic embedded atom potential, the energetic and the self-diffusion dynamics of Zr atomic clusters up to eight atoms on α-Zr(0 0 0 1) surface have been studied. The simulation temperature ranges from 300 to 1100 K and the simulation time varies from 20 to 40 ns. It’s found that the heptamer and trimer are more stable comparing to other neighboring non-compact clusters. The diffusion coefficients of clusters are derived from the mean square displacement of cluster’s mass-center and the present diffusion coefficients for clusters exhibit an Arrhenius behavior. The Arrhenius relation of the single adatom can be divided into two parts in different temperature range because of their different diffusion mechanisms. The migration energies of clusters increase with increasing the number of atoms in cluster. The differences of the prefactors also come from the diverse diffusion mechanisms. On the facet of 60 nm, the heptamer can be the nuclei in the crystal growth below 370 K.     

A description of stress driven bubble growth of helium implanted tungsten

Low energy (<100 keV) helium implantation of tungsten has been shown to result in the formation of unusual surface morphologies over a large temperature range (700-2100 °C). Simulation of these macroscopic phenomena requires a multiscale approach to modeling helium transport in both space and time. We present here a multiscale helium transport model by coupling spatially-resolved kinetic rate theory (KRT) with kinetic Monte Carlo (KMC) simulation to model helium bubble nucleation and growth. The KRT-based HEROS Code establishes defect concentrations as well as stable helium bubble nuclei as a function of implantation parameters and position from the implanted surface and the KMC-based Mc-HEROS Code models the growth of helium bubbles due to migration and coalescence. Temperature- and stress-gradients can act as driving forces, resulting in biased bubble migration. The Mc-HEROS Code was modified to simulate the impact of stress gradients on bubble migration and coalescence. In this work, we report on bubble growth and gas release of helium implanted tungsten W/O stress gradients. First, surface pore densities and size distributions are compared with available experimental results for stress-free helium implantation conditions. Next, the impact of stress gradients on helium bubble evolution is simulated. The influence of stress fields on bubble and surface pore evolution are compared with stress-free simulations. It is shown that near surface stress gradients accelerate helium bubbles towards the free surface, but do not increasing average bubble diameters significantly.