In-situ TEM observation of the evolution of helium bubbles in Mo during He+ irradiation and post-irradiation annealing

The evolution of helium bubbles in purity Mo was investigated by in-situ transmission electron microscopy (TEM) during 30 keV He⁺ irradiation (at 673 K and 1173 K) and post-irradiation annealing (after 30 keV He⁺ irradiation with the fluence of 5.74×10¹⁶ He⁺/cm² at 673 K). Both He⁺ irradiation and subsequently annealing induced the initiation, aggregation, and growth of helium bubbles. Temperature had a significant effect on the initiation and evolution of helium bubbles. The higher the irradiation temperature was, the larger the bubble size at the same irradiation fluence would be. At 1173 K irradiation, helium bubbles nucleated and grew preferentially at grain boundaries and showed super large size, which would induce the formation of microcracks. At the same time, the geometry of helium bubbles changed from sphericity to polyhedron. The polyhedral bubbles preferred to grow in the shape bounded by {100} planes. After statistical analysis of the characteristic parameters of helium bubbles, the functions between the average size, number density of helium bubbles, swelling rate and irradiation damage were obtained. Meanwhile, an empirical formula for calculating the size of helium bubbles during the annealing was also provided.     

超临界水冷堆燃料包壳材料的辐照损伤研究进展

超临界水冷堆（SCWR）是第四代核电站的主力堆型之一,高温、高压、超临界水环境下的辐照损伤问题是其燃料包壳材料面临的最大挑战。SCWR燃料包壳候选材料主要包括锆合金、奥氏体不锈钢、铁素体/马氏体不锈钢、镍基合金、ODS合金五大类,奥氏体不锈钢是最有希望的候选材料。介绍了近年来在这个领域国际上的主要研究进展。作者所在团队也对多种SCWR的候选材料进行了辐照损伤研究,包括:镍基合金C-276和718、铁素体/马氏体钢P92、奥氏体不锈钢AL-6XN和HR3C。对AL-6XN的氢离子辐照实验发现,辐照产生的缺陷主要是间隙型位错环,伯格斯矢量为1/3<111>,在较高剂量（5～7 dpa）辐照下,出现空洞肿胀。在氢滞留的影响下,位错环有着独特的演化规律,总结提出了位错环的四阶段演化过程。The Supercritical Water-cooled Reactor (SCWR) is one of the prior Generation IV advanced reactors. Irradiation damage is one of the key issues of fuel cladding materials which will suffer serious environment, such as high temperature, high pressure, high irradiation and supercritical water. The candidate materials contain zirconium alloys, austenitic stainless steels, ferritic/martensitic stainless steels, Ni-base alloys and ODS alloys. Austenitic stainless steels are the most promising materials. This paper summarized the international researches on irradiation effects in fuel cladding materials for SCWR. The group of authors also has done many researches in this field, including nickel-base alloy C-276 and 718, ferritic/martensitic steel P92 and austenitic stainless steel AL-6XN and HR3C. In AL-6XN austenitic stainless steels irradiated by hydrogen ions, dislocation loops were the dominant irradiation defects. At higher irradiation dose (5～7 dpa), the voids were found. All the dislocation loops were confirmed to be 1/3<111> interstitial type dislocation loops, and four evolution stages of dislocation loops with hydrogen retention were suggested.     

Effect of helium concentration on irradiation damage of Fe-ion irradiated SIMP steel at 300℃ and 450℃

SIMP steel is newly developed fully martensitic steel for lead-cooled fast reactors and accelerator-driven systems.It is important to evaluate its radiation resistance via high flux neutron irradiation, where dense He atoms can be formed via(n, α) transmutation reaction. Co-irradiation with Fe and He ions, instead of neutron, was performed. Specimens were irradiated with 6.4-Me V Fe ions to the damage dose of 5 dpa at a depth of 600 nm. Three different helium injection ratios of 60-appm He/dpa(dpa: displacements per atom), 200-appm He/dpa and 600-appm He/dpa at a depth of 600 nm,were performed. Two different irradiation temperatures of 300℃ and 450℃ were carried out. The effect of helium concentration on the microstructure of Fe-irradiated SIMP steel was investigated. Microstructural damage was observed using transmission electron microscopy. The formed dislocation loops and bubbles depended on the helium injection ratio and irradiation temperature. Lots of dislocation loops and helium bubbles were homogeneously distributed at 300℃, but not at 450℃. The causes of observed effects are discussed.     

冲击加载下铝中氦泡和孔洞的塑性变形特征研究

通过分子动力学模拟研究了在相同冲击加载强度下单晶铝中氦泡和孔洞的塑性变形特征,结果发现氦泡和孔洞的塌缩是由发射剪切型位错环引起的,而没有观测到棱锥型位错环发射. 氦泡和孔洞周围的位错优先成核位置基本一致,但是氦泡周围发射的位错环数目比孔洞多,位错环发射速度明显比孔洞快. 且氦泡和孔洞被冲击波先扫过部分比后扫过部分发射位错困难. 通过滑移面上的分解应力分析发现,氦泡和孔洞周围塑性特征的差别是由于氦泡内压引起最大分解应力分布改变造成的. 氦泡和孔洞被冲击波先后扫过部分塑性不对称是因为冲击波扫过时引起形状变化, 关键词： 分子动力学 冲击波 氦泡 孔洞     

氦离子低温预辐照对不锈钢中氦泡生长抑制作用的Monte Carlo模拟研究

实验中已发现氦离子低温预辐照不锈钢材料能有效抑制高温辐照阶段的氦泡生长,但这一结果一直缺少理论解释.基于持续注入粒子的三维格子气模型,采用Monte Carlo模拟方法研究了不同温度模式对氦泡生长行为的影响.研究发现,计算结果能很好地再现氦离子低温预注入抑制高温氦泡生长的实验现象,其原理为低温预注入时材料中形成了较高数密度的小氦泡,由于氦泡数量较多从而限制了氦泡平均尺寸的增大.     

氦、氘对纯铁辐照缺陷的影响

在核聚变堆的辐照环境中, 核嬗变产物氢、氦对结构材料的抗辐照性能将产生很大的影响. 本实验采用离子注入和电子辐照模拟研究了氦和氘对具有体心立方结构的纯铁的影响. 采用离子加速器在室温分别对纯铁注入氦离子和氘离子, 经500℃时效1 h后在高压电镜下进行电子辐照.结果表明: 室温注氦和室温注氘的纯铁在500℃时效后分别形成间隙型位错环和空位型位错环. 在电子辐照下, 间隙型位错环吸收间隙原子而不断长大, 而空位型位错环吸收间隙原子不断缩小. 通过计算位错环的变化速率发现, 空位型位错环比间隙型位错环吸收了更多的间隙原子, 即室温注氘纯铁的位错偏压比室温注氦纯铁的偏压参量大, 这意味着相同实验条件下空位型位错环对辐照肿胀的贡献大于间隙型位错环对辐照肿胀的贡献. 利用氦-空位复合体和氘-空位复合体的结构, 分析了注氦和注氘后在纯铁中形成不同类型位错环的原因. 关键词： 氦 氘 辐照损伤 位错环     

Synergistic effects in hydrogen-helium bubbles

The detrimental effects of hydrogen and helium on structural materials undergoing irradiation are well documented, if not well understood. There is experimental evidence to suggest that a synergistic effect between the two elements exists, which results in increased damage when both are present. This situation is expected in the next generation of fusion and fission reactors, so a fundamental understanding of these synergistic interactions is needed to predict materials performance. We perform atomistic simulations of hydrogen and helium bubbles in body-centered cubic iron to determine the mechanism behind this effect. We first develop an interatomic potential suitable for describing the interactions between hydrogen and helium. Through analysis of the energetics and structure of these bubbles, we explain the observed synergy as a consequence of bubble growth through helium induced loop punching, aided by the presence of hydrogen, instead of as a direct interaction between hydrogen and helium. The hydrogen benefits from an increased area of free surface on which to bind.     

Evolution of gas-filled nanocracks in crystalline solids

In this work, the evolution of gas-filled cracks under gas implantation and subsequent annealing is studied on the basis of an elastic continuum approach. The observed growth limitation of He-filled nanocracks in SiC is attributed to their stabilization by the formation of circular dislocation dipoles. The formation and Ostwald ripening of bubble-loop complexes at elevated temperatures is modeled in terms of gas atom exchange between such complexes coupled with local matrix atom exchange between bubbles and loops of the same complex. The scaling laws derived for the time dependence of bubble and loop sizes are found to be in good agreement with experimental data.     

Evolution of dislocation loops in austenitic stainless steels implanted with high concentration of hydrogen

Abstract

It has been found that under certain conditions, hydrogen retention would be strongly enhanced in irradiated austenitic stainless steels. To investigate the effect of the retained hydrogen on the defect microstructure, AL-6XN stainless steel specimens were irradiated with low energy (100 keV) H₂⁺ so that high concentration of hydrogen was injected into the specimens while considerable displacement damage dose (up to 7 dpa) was also achieved. Irradiation induced dislocation loops and voids were characterised by transmission electron microscopy. For specimens irradiated to 7 dpa at 290 °C, dislocation loops with high number density were found and the void swelling was observed. At 380 °C, most of dislocation loops were unfaulted and tangled at 7 dpa, and the void swellings were observed at 5 dpa and above. Combining the data from low dose in previous work to high dose, four stages of dislocation loops evolution with hydrogen retention were suggested. Finally, molecular dynamics simulation was made to elucidate the division of large dislocation loops under irradiation.     

MOSFET 辐照诱生界面陷阱形成过程的1/f噪声研究

基于界面陷阱形成的氢离子运动两步模型和反应过程的热力学平衡假设，推导了金属-氧化物-半导体-场效应晶体管(MOSFET)经历电离辐照后氧化层空穴俘获与界面陷阱形成间关系的表达式.利用初始1/f噪声功率谱幅值与氧化层空穴俘获之间的联系，建立了辐照前的1/f噪声幅值与辐照诱生界面陷阱数量之间的半经验公式，并通过实验予以验证.研究结果表明，由于辐照诱生的氧化层内陷阱通过与分子氢作用而直接参与到界面陷阱的建立过程中，从而使界面陷阱生成数量正比于这种陷阱增加的数量，因此辐照前的1/f噪声功率谱幅值正比于辐照诱生的界面陷阱数量.研究结果为1/f噪声用作MOSFET辐照损伤机理研究的新工具，对其抗辐照性能进行无损评估提供了理论依据与数学模型. 关键词： 辐照效应 界面陷阱 1/f噪声 氧化层空穴俘获     

He 离子注入引起的高纯钨硬化

完成了不同注量或温度下100 keV 的He 离子注入高纯钨的实验,并利用纳米压痕技术测量了材料的微观力学性能。所有注入样品的纳米硬度值都高于未注入样品的纳米硬度值。对于室温注入样品,随着注量的增加,样品抗弹性变形能力下降;当注量不高于5x1017 ions/cm2 时,钨的纳米硬度峰值随着注量的增加而增加;注量为1x1018 ions/cm2 的钨样品的纳米硬度峰值反而降低。高温注入样品的抗弹性变形能力优于室温注入样品的抗弹性变形能力;随着注入温度的增加,样品的平均纳米硬度值和弹性模量略有下降。分析讨论了He 注入钨硬化和抗弹性形变能力降低的可能原因。Tungsten has been selected as divertor materials in fusion reactors because of its high thermal conductivity,high melting point, low expansion coefficient and high threshold energy for sputtering etc. The paper presents the hardening behaviour of high pure tungsten by 100 keV He+ with different fluences from 5x1016 ions/cm2 to 1x1018ions/cm2 at room temperature, and with fluence of 1x1018 ions/cm2 at higher temperatures (400, 600 and 800 °C). The microscopic mechanical properties of these samples were investigated by nano-indentation technology. The results show that all of the implanted samples harden obviously. The reason for hardening may be that defects of interstitial dislocation loops or dense helium bubbles etc induced by helium implantation obstacle the movement of dislocation. The peak nanohardness of the samples increased with the fluences increasing when the fluence is not more than 5x1017 ions/cm2, while the nano-hardness value of the implanted sample with the fluence of 1x1018 ions/cm2 decreases and the nano-hardness changes little in the region of 50 nm to 200 nm from surface. For all the implanted samples with 1x1018 ions/cm2 at higher temperatures, their nano-hardness values are similar, but show a trend of decrease with increasing temperature.The reason may be the decrease of the defects’ density during implantation at higher temperatures. In addition, the capability of resisting deformation for the implanted tungsten reduces with increasing fluence and increases a little at higher temperatures.     

两种国产低活化的铁素体/马氏体钢的He离子辐照硬化研究

低活化的铁素体/马氏体钢（RAFM）以其高导热率、低热膨胀率、高抗辐照肿胀能力成为未来核聚变堆重要的候选结构材料,在聚变堆高能中子辐照环境由于（n,α）核反应产生的高浓度He在材料中的积累对于材料微观结构和宏观性能的影响是关系这类材料服役寿命的重要问题。本工作研究了面向聚变反应堆应用的两种国产低活化钢（CLF、CNS）的辐照硬化效应,利用中国科学院近代物理研究所320 kV高压实验平台提供的4He离子束进行辐照实验,辐照剂量6×10-3,6×10-2,6×10-1 dpa （辐照损伤/原子平均离位）,对应注He浓度分别为100,1 000,10 000 appm （氦离子浓度/百万分之一）。采用多能注入方法,在样品表面至1微米深度形成He浓度和离位损伤的坪区分布。利用纳米压痕仪对参比样品和注入He的样品进行了连续刚度测试。基于NIX-GAO模型对纳米硬度数据进行分析,获得了注入He的区域样品纳米硬度的数据。研究表明,注入He区域的纳米硬度与辐照损伤水平之间存在着1/2次幂函数的关系。未辐照CLF钢比CNS钢的纳米硬度略低,随着辐照剂量的增加,CLF钢呈现的辐照硬化现象更明显。Reduced activation ferritic/martensitic steels (RAFM) are important candidate materials for future fusion nuclear reactors because of their high thermal conductivity, low thermal expansion rate and high resistance to irradiation swelling performance. The influence of high concentration helium produced by nuclear reaction (n,α) on the micro-structure and macro-properties is an important issue limiting the service lifetime of the materials. In the present work, helium implantation to three different doses (100, 1 000, 10 000 appm helium, corresponding to 6×10-3, 6×10-2, 6×10-1 dpa) was carried out to investigate irradiation hardening of two RAFM Steels. Multi-energy He ion-beams at 320 kV high-voltage platform were used to get a damage plateau from surface to 1 μm depth in specimens. The continuous-stiffness test by a Nano-indentor G2000 was carried out Data of nano-hardness were analyzed based on Nix-Gao model. It is shown that there is a 1/2-power law relationship between the hardening and the irradiation damage level. Before helium implantation, the hardness of the CLF steel is slightly lower than that of the CNS steel. However, with the increase of helium-implantation dose, the hardening is more obvious in CLF steel. Further investigation of microstructures is needed to get a deeper understanding of the hardening mechanism.     

高He通量注入条件下F/M和ODS钢中纳米微结构对He泡形核和长大的影响

利用LEAF装置提供的2 MeV的He离子,在500和600 °C分别对新型F/M钢-SIMP钢和ODS钢(MA956和Eurofer-ODS钢)注入1×1017 ions/cm2的高通量He离子,借助透射电子显微镜,表征了辐照后三种材料的肿胀行为,验证了各材料中纳米微结构(晶界,析出相和纳米氧化物)对辐照后He泡成核和长大的影响。结果表明,基于材料中晶界和析出相对He泡生长的抑制作用,温度为500 °C时,SIMP和Eurofer-ODS钢表现出较高的抗辐照肿胀性能,而MA956中纳米界面He泡成核和长大作用不明显,表现出较差的抗辐照肿胀性能;此外,温度为600 °C时,Eurofer-ODS钢由于其晶界和氧化物界面的较强作用,表现出较好的抗辐照肿胀性能。总体来说,在高He通量注入条件下,材料中纳米结构的存在会抑制He泡长大的过程,但不同材料中纳米结构对He影响作用不同。     

Effect of simultaneous helium implantation on the microstructure evolution of Inconel X-750 superalloy during dual-beam irradiation

This study focuses on investigation into the effect of helium implantation on microstructure evolution in Inconel X-750 superalloy during dual-beam (Ni⁺/He⁺) irradiation. The 1 MeV Ni⁺ ions with the damage rate of 10^?3 dpa/s as well as 15 keV He⁺ ions using rate of 200 appm/dpa were simultaneously employed to irradiate specimens at 400 °C to different doses. Microstructure characterization has been conducted using high-resolution analytical transmission electron microscopy (TEM). The TEM results show that simultaneous helium injection has significant influence on irradiation-induced microstructural changes. The disordering of γ′ (Ni₃ (Al, Ti)) precipitates shows noticeable delay in dose level compared to mono heavy ion irradiation, which is attributed to the effect of helium on promoting the dynamic reordering process. In contrast to previous studies on single-beam ion irradiation, in which no cavities were reported even at high doses, very small (2–5 nm) cavities were detected after irradiation to 5 dpa, which proved that helium plays crucial role in cavity formation. TEM characterization also indicates that the helium implantation affects the development of dislocation loops during irradiation. Large 1/3 〈1?1?1〉 Frank loops in the size of 10–20 nm developed during irradiation at 400 °C, whereas similar big loops detected at higher irradiation temperature (500 °C) during sole ion irradiation. This implies that the effect of helium on trapping the vacancies can help to develop the interstitial Frank loops at lower irradiation temperatures.     

氢离子辐照纯钒中形成的位错环

钒合金作为聚变堆候选材料, 其辐照损伤行为一直是关注的重点. 研究辐照时形成的位错环的性质, 其意义在于揭示纯钒中辐照空洞的长大机理. 这种机理表现为不同类型位错环对点缺陷吸收的偏压不同, 从而影响金属的辐照肿胀. 本文利用加速器对纯钒薄膜样品进行氢离子辐照, 然后, 利用透射电镜的inside-outside方法分析氢离子辐照所形成的位错环的类型. 结果表明, 在氢离子辐照纯钒中没有发现柏氏矢量b=<110>的位错环, 只有柏氏矢量b=1/2<111>和b=<110>的位错环, 这两种位错环的惯性面处于{110}-{112}之间. 能确定性质的位错环全部为间隙型位错环, 未发现空位型位错环.     

Evolution of helium bubbles in nickel-based alloy by post-implantation annealing

Nickel-based alloys have been considered as candidate structural materials used in generation IV nuclear reactors serving at high temperatures. In the present study, alloy 617 was irradiated with 180-keV helium ions to a fluence of 3.6×10¹⁷ ions/cm² at room temperature. Throughout the cross-section transmission electron microscopy (TEM) image, numerous over-pressurized helium bubbles in spherical shape are observed with the actual concentration profile a little deeper than the SRIM predicted result. Post-implantation annealing was conducted at 700 ℃ for 2 h to investigate the bubble evolution. The long-range migration of helium bubbles occurred during the annealing process, which makes the bubbles of the peak region transform into a faceted shape as well. Then the coarsening mechanism of helium bubbles at different depths is discussed and related to the migration and coalescence (MC) mechanism. With the diffusion of nickel atoms slowed down by the alloy elements, the migration and coalescence of bubbles are suppressed in alloy 617, leading to a better helium irradiation resistance.     

Superior tolerance of Ag/Ni multilayers against Kr ion irradiation: an in situ study

Monolithic Ag and Ni films and Ag/Ni multilayers with individual layer thickness of 5 and 50?nm were subjected to in situ Kr ion irradiation at room temperature to 1 displacement-per-atom (a fluence of 2?×?10¹⁴?ions/cm²). Monolithic Ag has high density of small loops (4?nm in diameter), whereas Ni has fewer but much greater loops (exceeding 20?nm). In comparison, dislocation loops, ～4?nm in diameter, were the major defects in the irradiated Ag/Ni 50?nm film, while the loops were barely observed in the Ag/Ni 5?nm film. At 0.2?dpa (0.4?×?10¹⁴?ions/cm), defect density in both monolithic Ag and Ni saturated at 1.6 and 0.2?×?10²³/m³, compared with 0.8?×?10²³/m³ in Ag/Ni 50?nm multilayer at a saturation fluence of ～1?dpa (2?×?10¹⁴?ions/cm²). Direct observations of frequent loop absorption by layer interfaces suggest that these interfaces are efficient defect sinks. Ag/Ni 5?nm multilayer showed a superior morphological stability against radiation compared to Ag/Ni 50?nm film.     

Helium effects on the microstructural evolution of reactor irradiated ferritic and austenitic steels

Abstract

Microstructural evolution in neutron irradiated austenitic stainless steels and Cr-Mo ferritic steels is reviewed. Important highlights are: (1) there is a strong correlation between precipitation and void evolution in austenitic steels; (2) helium affects precipitate evolution in austenitic steels, but observations indicate no effect on precipitation in ferritic steels; (3) helium has a pronounced effect on the cavity evolution of the two steel types. Helium effects are explained in terms of the interrelationship between microstructural evolution and point-defect annihilation processes. In stainless steel, three relative regimes of microstructural behavior for different helium generation rate-displacement rate ratios are recognized: (1) “low” He/dpa ratio, where helium effects on the radiation-induced microstructural evolution are negligible or develop slowly, (2) “medium” He/dpa ratio, where helium effects strongly enhance the microstructural changes, and (3) “high” He/dpa ratio, where helium effects are limited to the early development of a high density of fine bubbles which interfere with other radiation-induced microstructural changes, but allow enhanced thermal microstructural evolution to take place instead. The extensive data on austenitic steels fall within these regimes. Ferritic steels are known to be highly resistant to void swelling without helium. It is suggested that enhanced cavity formation due to helium in ferritic steels makes higher swelling a potential concern for fusion reactor applications.     

Helium-hydrogen synergistic effects on swelling in in-situ multiple-ion beams irradiated steels

The development of reliable fusion energy is one of the most important challenges in this century. The accelerated degradation of structural materials in fusion reactors caused by neutron irradiation would cause severe problems. Due to the lack of suitable fusion neutron testing facilities, we have to rely on ion irradiation experiments to test candidate materials in fusion reactors. Moreover, fusion neutron irradiation effects are accompanied by the simultaneous transmutation production of helium and hydrogen. One important method to study the He-H synergistic effects in materials is multiple simultaneous ion beams (MSIB) irradiation that has been studied for decades. To date, there is no convincing conclusion on these He-H synergistic effects among these experiments. Recently, a multiple ion beam in-situ transmission electron microscopy (TEM) analysis facility was developed in Xiamen University (XIAMEN facility), which is the first triple beam system and the only in-running in-situ irradiation facility with TEM in China. In this work, we conducted the first high-temperature triple simultaneous ion beams irradiation experiment with TEM observation using the XIAMEN facility. The responses to in-situ triple-ion beams irradiation in austenitic steel 304L SS and ferritic/martensitic steel CLF-1 were studied and compared with the results in dual- and single-ion beam(s) irradiated steels. Synergistic effects were observed in MSIB irradiated steels. Helium was found to be critical for cavity formation, while hydrogen has strong synergistic effect on increasing swelling.     

基于辐照前1/f噪声的金属-氧化物-半导体场效应晶体管潜在缺陷退化模型

基于金属-氧化物-半导体-场效应管(MOSFET)辐射损伤的微观机理,推导出了MOSFET经历辐照之后氧化层空穴俘获与阈值电压漂移之间关系的表达式.又根据MOSFET中1/f噪声产生的微观机理,建立了辐照之前MOSFET的1/f噪声功率谱幅值与阈值电压漂移量之间的定量关系,并通过实验予以验证.结果表明,辐照之前的1/f噪声功率谱幅值与辐照之后的阈值电压漂移量存在正比例关系,阈值电压漂移量可以反映出MOSFET内部的潜在缺陷的退化程度,因此,该模型有助于利用1/f噪声参量来表征MOSFET内部潜在缺陷的数量和严重程度.