Pu-Ga合金中氦泡聚集行为的分子动力学模拟

在钚(Pu)材料中加入少量其他金属元素,如铝(Al)、镓(Ga)、铟(In)、铈(Ce)等,能实现Pu合金材料在室温条件下稳定。本文采用分子动力学(MD)方法及修正的嵌入原子势(MEAM),在300K下对Pu-Ga合金中的氦泡聚集行为进行了模拟,合金中Ga的含量(原子分数)分别为0%、2%和5%。通过计算和分析,得到不同Ga含量下,随氦原子数目增长Pu-Ga合金中氦泡半径和压强的变化趋势,以及由氦泡引起的体积膨胀,研究结果对于理解钚自辐照过程中的氦效应的内在机制具有一定的参考价值。     

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。     

金属铁和镍中氦缺陷性质的理论研究

采用投影缀加波赝势和广义梯度近似方法分别计算了体心立方结构金属铁和面心立方结构镍中3种氦缺陷形成能及态密度分布。计算结果表明,以上两种金属的置换氦缺陷最稳定,其次是四面体间隙氦缺陷,八面体间隙氦缺陷最不稳定。分析表明,金属铁和镍中氦缺陷稳定性并不是由缺陷的弹性畸变决定的,而是由缺陷氦原子与其最邻近金属原子之间的电子相互作用决定的。     

充氚不锈钢中氦行为的PAL和TEM研究

对充氚和未充氚的抗氢-2(HR-2)不锈钢样品进行退火处理,利用正电子湮没寿命谱(PAL)以及透射电镜(TEM)等技术探讨不锈钢中氦和微缺陷的相互作用。未充氚样品中,退火温度对缺陷态的影响主要表现为偏聚物在晶界的析出。充氚样品实验中,退火温度小于300℃时,充氚不锈钢中的He原子主要通过自捕获机制在晶内缺陷处聚集成泡;热处理温度为300～600℃时,充氚不锈钢中的He原子主要通过热迁移的方式迁移至晶界导致晶界宽化,但晶界处无明显的He泡形成;热处理温度大于600℃时,热平衡空位开始发挥作用,与聚集在晶内缺陷处的He原子结合形成He泡,且随退火温度的升高,He泡有明显聚合长大的现象。     

α-铁中氦缺陷对氢原子的俘获

体心立方结构的金属铁(α-铁)是聚变反应堆重要的候选结构材料,受氢和氦原子的辐照后可能会发生力学性能的退化。了解氢和氦原子在铁中的聚集行为是反应堆聚变材料研究的重点。本文采用密度泛函理论计算了α-铁中HeHn集团的稳定性,揭示了替代位氦缺陷俘获氢原子的过程和机制,结果表明,1个氦原子最多可俘获4个氢原子,被俘获的氢原子占据氦原子周围的八面体间隙位,且氢原子倾向于彼此聚拢。对氢原子俘获能的计算表明,氢原子足量时,HeH4是α-铁中主要的氢氦集团构型,反之则以HeH2为主。     

第一性原理拟合氦钛两体作用势

分子动力学研究氦钛两体相互作用涉及3种体系势能函数的表述。文章讨论其中氦氦相互作用势及氦钛相互作用势,分析不同势能函数形式描述氦与金属作用势的区别。Lennard-Jones势较好描述分子晶体特别是惰性固体之间的作用势,在金属钛与氦原子之间的相互作用时,在小于平衡位置的条件下,Born-Mayer势的排斥势太强,未较好反映实际氦钛原子作用,而采用量子化学第一性原理的方法,并结合相关的实验参数拟合氦钛两体相互作用势在近程作用上存在明显的优势。     

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...     

质子辐照钼退火行为的正电子寿命谱学研究

室温下用3.2MeV质子对多晶纯钼样品进行了辐照,用正电子寿命测量技术研究了辐照损伤及晶格缺陷在293～1138K温区内的退火行为,得出了许多有关空位团生长以及氢-缺陷相互作用的信息。辐照后在Mo中产生2～3个空位的聚集体,其浓度随辐照剂量增加而增加。从所测得正电子寿命、强度参数的变化获知高温退火后空位团的增长行为以及氢原对空位团长大的影响。     

质子辐照钼退火行为的正电子寿命谱学研究

室温下用3.2MeV质子对多晶纯钼样品进行了辐照,用正电子寿命测量技术研究了辐照损伤及晶格缺陷在293～1138K温区内的退火行为,得出了许多有关空位团生长以及氢-缺陷相互作用的信息。辐照后在Mo中产生2～3个空位的聚集体,其浓度随辐照剂量增加而增加。从所测得正电子寿命、强度参数的变化获知高温退火后空位团的增长行为以及氢原对空位团长大的影响。     

氦离子辐照对镍基合金硬度的影响

在室温下对镍基合金进行了氦离子辐照,利用纳米压痕仪测试了微观硬度,利用慢正电子多普勒展宽谱(Doppler Broadening Spectrum,DBS)和透射电子显微镜(Transmission Electron Microscope,TEM)分析了微观缺陷,利用离子束分析弹性反冲探测(Elastic Recoil Detection,ERD)技术测量了氦的浓度深度分布。结果显示合金样品的硬度随剂量而增大,退火后合金样品硬度增量有所减小,并观测到氦泡生成。合金硬化的主要原因是由于氦离子辐照产生了1-7 nm的缺陷团簇,而退火后不稳定缺陷的回复及氦-空位复合体数量的减少造成了硬化强度减弱。     

Self-radiation damage in plutonium and uranium mixed dioxide

In plutonium compounds, the lattice parameter increases due to self-radiation damage by α-decay of plutonium isotopes. The lattice parameter change and its thermal recovery in plutonium and uranium mixed dioxide (MOX) were studied. The lattice parameter for samples of MOX powders and pellets that had been left in the air for up to 32 years was measured. The lattice parameter increased and was saturated at about 0.29%. The change in lattice parameter was formulated as a function of self-radiation dose. Three stages in the thermal recovery of the damage were observed in temperature ranges of below 673 K, 673-1073 K and above 1073 K. The activation energies in each recovery stage were estimated to be 0.12, 0.73 and 1.2 eV, respectively, and the corresponding mechanism for each stage was considered to be the recovery of the anion Frenkel defect, the cation Frenkel defect and a defect connected with helium, respectively.     

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.     

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。     

Atomistic simulation of helium bubble nucleation in palladium

A palladium crystal has been constructed with 11808 atoms. 55 helium atoms occupied the octahedral position of palladium crystal are introduced and retained in a spherical region. Molecular dynamic simulations are performed in a constant temperature and constant volume ensemble (NVT) with temperature controlled by Nose-Hoover thermostat. The interactions between palladium atoms are described with modified analytic embedded atom method (MAEAM), the interactions between palladium atom and helium atom are in the form of Morse potential, and the interactions between helium atoms are in the form of L-J potential function. With the analysis of the radial distribution function (RDF) and microstructure, it reveals that some of helium atoms form a series of clusters with different size, and the nucleation core is random at low temperature, and which is the embryo of helium bubble. Increasing temperature can accelerate the process of bubble nucleation, and the clusters will aggregate and coalesce into a bigger one in which there are no palladium atoms, and it is considered as a helium bubble.     

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.     

三烷基(混合)氧膦的结构分析及其对镎、钚的萃取

本文用红外光谱和核磁共振谱研究了TRPO的组成及萃取结构,证明了萃取是由膦酰基上氧原子的孤对电子配位引起的,萃取络合物为配位络合物。研究了 TRPO萃取水和硝酸的平衡常数及络合物结构形式。还用~(238)Np示踪和α液体闪烁测量研究了TRPO-煤油-硝酸体系中各种价态的镎、钚萃取和反萃取情况。     

钛中氦泡融合的分子动力学模拟

本文采用分子动力学方法模拟了金属钛中氦泡的融合,分析了氦泡融合对金属微结构的影响,对比了氦泡在金属块体内部与接近金属表面处融合的异同。研究表明:在金属块体内部,两氦泡的融合会在其周围诱发很多缺陷且范围逐渐扩大;直径均为1.77nm的两氦泡的融合会在二者周围形成位错环,位错环内金属原子的排列与基底的一致;两氦泡发生融合后由哑铃状向椭球形演化。在接近金属表面处,由氦泡融合诱发的缺陷易于向金属表面移动,氦泡周围的金属易于向晶体结构恢复;两氦泡发生融合后由哑铃状向半球形演化。     

Pu-H2相互作用的反应机理及电子密度分析

通过量子力学中密度泛函理论的相关方法和相对论有效原子实模型(RECP),应用Gaussian09程序对钚与氢气的相互作用进行了计算和分析。计算得到了钚与氢气的详细微观反应机理：Pu+H2→FC→TS→PuH2,优化了沿反应路径的特殊结构（能量极小点及过渡态）,并通过能量分析画出了势能剖面图。基于优化的几何结构,通过多种拓扑分析方法分析了反应路径中所有特殊结构的电子密度相关性质,如自旋密度分析、Mulliken自旋布居分析、电子定域泛函理论分析,得到了电子密度在反应过程中的详细变化。     

氢氦在钨中的影响的第一性原理研究

采用PBE形式的广义梯度近似(GGA)的第一性原理计算方法研究了氢或氦在钨中产生点缺陷的形成能以及缺陷形成后对钨的弹性的影响;采用同样的方法研究了空位和自间隙原子这两种缺陷。经计算发现:氢氦掺杂在钨的晶体结构中会引起晶体体积的变化,其变化结果跟掺杂的位置有关,在四面体或八面体处的掺杂会使晶体体积增加,替位掺杂会引起晶体体积减小;从形成能来看,氢掺杂在钨中最占优的位置是四面体处,而氦最占优的则是替位掺杂。在几种缺陷中,形成能最小的是氢的四面体掺杂,形成能最大的则是钨的自间隙原子形成;钨中若含有氢或氦的点缺陷,晶体的体弹模量和剪切模量会发生改变,当钨中含有氢替位或自间隙原子时晶体会向塑性改变,含有其他点缺陷时晶体会沿着脆性方向转变。但总体来说带有缺陷的钨仍然具有延展性。值得注意的是,氢或氦在钨中会引起晶体的各向异性,其具体结果与缺陷所处位置相关,只有缺陷属于替位时才不会发生各向异性。本文的研究工作可为第一壁材料的开发提供理论参考。