Dynamic behaviour of nanometre-sized defect clusters emitted from an atomic displacement cascade in Au at 50 K

Abstract

We demonstrate the emission of nanometre-sized defect clusters from an isolated displacement cascade formed by irradiation of high-energy self-ions and their subsequent 1-D motion in Au at 50 K, using in situ electron microscopy. The small defect clusters emitted from a displacement cascade exhibited correlated back-and-forth 1-D motion along the [?1 1 0] direction and coalescence which results in their growth and reduction of their mobility. From the analysis of the random 1-D motion, the diffusivity of the small cluster was evaluated. Correlated 1-D motion and coalescence of clusters were understood via elastic interaction between small clusters. These results provide direct experimental evidence of the migration of small defect clusters and defect cascade evolution at low temperature.     

Simulating high energy cascades in metals

Abstract

The processes of radiation damage, from initial defect production to microstructure evolution, occur over a wide spectrum of time and size scales. An understanding of the fundamental aspects of these processes requires a spectrum of theoretical models, each applicable in its own time and distance scales. As elements of this multi-model approach, molecular dynamics and binary collision simulations play complementary roles in the characterization of the primary damage state of high energy collision cascades. Molecular dynamics is needed to describe the individual point defects in the primary damage state with the requisite physical reality. The binary collision approximation is needed to model the gross structure of statistically significant numbers of high energy cascades. Information provided by both models is needed for connecting the defect production in the primary damage state with the appropriate models of defect diffusion and interaction describing the microstructure evolution. Results of binary collision simulations of high energy cascade morphology are reviewed. The energy dependence of freely migrating defect fractions calculated in recent molecular dynamics simulations are compared to results obtained much earlier with a binary collision/annealing simulation approach. The favorable agreement demonstrates the viability of the multi-model approach to defect production in high energy cascades.     

Microstructural evolution in metals during helium and proton irradiations

Abstract

Recent investigations of helium-implanted and proton irradiated metals at medium temperatures (T≤100°C) have demonstrated the importance of high energy cascade effects for the microstructural evolution. They can effect the formation and the evolution of He densities in small bubbles formed by He implantation and are important also for the formation of periodic walls of defect clusters, a phenomenon observed under proton irradiations. Experimental results obtained by transmission electron microscopy and differential dilatometry for MeV irradiations of Cu and Ni are summarized and compared with observations after heavy-ion and neutron irradiations.     

The kinetics of formation and the parameters of radiation defect clusters in silicon

An approximate analytic solution of the system of equations describing the kinetics of formation and the parameters of radiation defect clusters in crystals is obtained. A model corresponding to the real parameters of Si is assumed as a basis for calculation and it is shown that two types of secondary radiation defect clusters may be realized corresponding to the congealing and spreading of the initial vacancy clusters. The cluster type depends on the incident energy of the particle which creates the effects and on the physical parameters of the crystal under irradiation. For a congealing cluster most of the initial vacancies react within the original volume of the damage cascade and for a spreading cluster the final concentration of divacancies and A-centres within the original cascade volume is much less than the initial vacancy concentration, i.e. most of the vacancies form divacancies and A-centres dispersed throughout the crystal volume.

The definition of the concept “threshold energy of cluster formation” as the minimum primarily displaced atom energy for the creation of a “congealing” vacancy cluster is proposed.

It is shown that A-centres form a belt surrounding a central divacancy cluster.     

Recent radiation damage studies and developments of the Marlowe code

Radiation damage in materials relevant to applications evolves over time scales spanning from the femtosecond – the characteristic time for an atomic collision – to decades – the aging time expected for nuclear materials. The relevant kinetic energies of atoms span from thermal motion to the MeV range.The question motivating this contribution is to identify the relationship between elementary atomic displacements triggered by irradiation and the subsequent microstructural evolution of metals in the long term. The Marlowe code, based on the binary collision approximation (BCA) is used to simulate the sequences of atomic displacements generated by energetic primary recoils and the Object Kinetic Monte Carlo code LAKIMOCA, parameterized on a range of ab initio calculations, is used to predict the subsequent long-term evolution of point defect and clusters thereof. In agreement with full Molecular Dynamics, BCA displacement cascades in body-centered cubic (BCC) Fe and a face-centered cubic (FCC) Fe\bond Ni\bond Cr alloy display recursive properties that are found useful for predictions in the long term.The case of defects evolution in W due to external irradiation with energetic H and He is also discussed. To this purpose, it was useful to extend the inelastic energy loss model available in Marlowe up to the Bethe regime. The last version of the Marlowe code (version 15) was delivered before message passing instructions softwares (such as MPI) were available but the structure of the code was designed in such a way to permit parallel executions within a distributed memory environment. This makes possible to obtain N different cascades simultaneously using N independent nodes without any communication between processors. The parallelization of the code using MPI was recently achieved by one author of this report (C.J.O.). Typically, the parallelized version of Marlowe allows simulating millions of displacement cascades using a limited number of processors (<64) within only few hours of CPU time.     

Evolution of ion-irradiated point defect concentration by cluster dynamics simulation

The relationship between ions irradiation and the induced microstructures(point defects, dislocations, clusters, etc.)could be better analyzed and explained by simulation. The mean field rate theory and cluster dynamics are used to simulate the effect of implanted Fe on the point defects concentration quantitatively. It is found that the depth distribution of point defect concentration is relatively gentle than that of damage calculated by SRIM software. Specifically, the damage rate and point defect concentration increase by 1.5 times and 0.6 times from depth of 120 nm to 825 nm, respectively. With the consideration of implanted Fe ions, which effectively act as interstitial atoms at the depth of high ion implantation rate, the vacancy concentration C_v decreases significantly after reaching the peak value, while the interstitial atom concentration C_i increases significantly after decline of the previous stage. At the peak depth of ion implantation, C_v dropped by 86%, and C_i increased by 6.2 times. Therefore, the implanted ions should be considered into the point defects concentration under high dose of heavy ion irradiation, which may help predict the concentration distribution of defect clusters, further analyzing the evolution behavior of solute precipitation.     

重离子辐照SiO2通过能量损失产生发光色心的研究

通过红外光谱和荧光发射光谱分别对600 keV、4 MeV和5 MeV Kr离子辐照的SiO2进行发光特性的研究。在低能量辐照体系中,简单色心(F2色心)的形成在损伤过程中占据主导地位,其主要诱发蓝光发射带;在高能离子辐照条件下,离子径迹上的能量密度较大,因此缺陷浓度的增大产生了一些缺陷团簇和离子径迹,形成了复杂的色心(F2+和F3+色心等)并诱发了强烈的绿光发射带和红光发射带。该实验结果与能量损失过程中统一热峰理论模型(一个综合的基于电子能损与核能损的非弹性碰撞模型和弹性碰撞模型)的模拟结果能够很好地吻合,表明在keV～MeV能区上存在电子能损过程与核能损过程的协同效应。     

A novel theory of radiation damage at high doses

Abstract

The deviations of radiation damage (in the case of metals usually monitored by the residual electrical resistivity) from proportionality to the irradiation dose have so far been analysed almost exclusively in terms of extensions of models originally developed for small doses. The present theory considers the opposite limit, i. e. the quasi-saturated state. It is argued that at high doses the Lück-Sizmann effect may result in a self-organization of clusters of vacancies and self-intersititials, forming a heterogeneous froth. Possible structures of this froth and its effect on the electrical resistivity of metals are discussed. The model is shown to account for the dependence of the “saturation resistivity” on the nature of the irradiation as well as for several other hitherto poorly explained observations. Among them are the electrical-resistivity variation induced by high-dose irradiation with heavy ions, the amorphization of certain alloys by high-dose electron irradiation, and the occurrence of ordered arrays of stacking-fault tetrahedra after in-situ irradiations in high-voltage electron microscopes.     

Time-resolved defect production and annealing during electron-beam processing of silicon

In (100)p-Si radiation damage was produced by implanting B⁺ ions with an energy of 80keV, 90keV and 1.6MeV. The specimens were annealed by scanned electronbeam irradiation (20keV, 1–2mAcm^–2). The formation, evolution and annihilation of defects during the irradiation process were investigated by employing DLTS and RBS measuring techniques. The results show a minimum of defect concentration and an efficiency of the electrical activation of B higher than 80% at an annealing time of 4.5 s. For irradiation times longer than 5 s it becomes evident, that the crystal surface acts as source of defects and contributes to an increase in defect concentration.     

Dynamical response of helium bubble motion to irradiation with high-energy self-ions in aluminum at high temperature

Brownian-type motion of helium bubbles in aluminum and its dynamical response to irradiation with 100-keV Al⁺ ions at high temperatures has been studied using in situ irradiation and transmission electron microscopy. It is found that, for most bubbles, the Brownian-type motion is retarded under irradiation, while the mobility returns when the irradiation is stopped. In contrast, under irradiation, a small number of bubbles display exceptionally rapid motion associated with the change in bubble size. These effects are discussed in terms of the dynamical interaction of helium bubbles with cascade damage formed by the high-energy self-ion irradiation.     

Evolution pattern of collision cascades in bcc V with different grain boundary structures: an atomic scale study

Abstract

In this paper, by means of atomic-scale simulations, we investigate modifications of the evolution pattern of collision cascades in bcc vanadium (V) with different grain boundary (GB) structures on picosecond (ps) timescale. In primary damage state, in agreement with previous results of bcc and fcc bi-crystals, we find that the GBs in V are biased towards interstitials. The biased absorption of interstitials over vacancies reduces the in-cascade annihilation of vacancy-interstitial pairs and leads to aggregation of more number of vacancies in the grains interiors. The sessile vacancies accumulate in the bulk and form immobile vacancy clusters; in contrast, the glissile interstitials disperse in the damage zone and mostly diffuse in the form of single self-interstitial atoms (SIAs)/di-interstitials towards the GB region. Moreover, meanwhile, as we discuss the mechanisms that reduce (or increase) the concentration of defects in bi-crystal structures on picosecond timescale, we study the energetics of defects in close vicinity of pristine GBs, as an alternative driving force that facilitates formation and accumulation of defects in the GB regions. Finally, in a prolonged irradiation, we examine stability and sink properties of the damaged GBs. The results reveal that, irrespective of GB structure, the presence of grain boundaries leads to aggregation of more number of vacancies in the grain interiors in continuous bombardment. Overall, based on the results obtained in the primary damage event and the prolonged irradiation, we conclude that the GBs in bcc V act as efficient defect sinks on the simulated time frame.     

Molecular dynamics simulations of displacement cascades in Feben 10%Cr systems

Molecular dynamics simulations of the displacement cascades in Fe-10%Cr systems are used to simulate the primary knocked-on atom events of the irradiation damage at temperatures 300, 600, and 750 K with primary knocked-on atom energies between 1 and 15 keV. The results indicate that the vacancies produced by the cascade are all in the central region of the displacement cascade. During the cascade, all recoil Fe and Cr atoms combine with each other to form Fe-Cr or Fe-Fe interstitial dumbbells as well as interstitial clusters. The number and the size of interstitial clusters increase with the energy of the primary knocked-on atom and the temperature. A few large clusters consist of a large number of Fe interstitials with a few Cr atoms, the rest are Fe-Cr clusters with small and medium sizes. The interstitial dumbbells of Fe-Fe and Fe-Cr are in the lan111ran and lan110ran series directions, respectively.     

高能重离子辐照的低活化钢硬化效应

为了探讨聚变堆候选低活化钢的抗辐照性能,在兰州重离子加速器国家实验室HIRFL的材料辐照终端,利用63 MeV的~(14)N离子和336 MeV的~(56)Fe离子在-50?C下对一种国产低活化钢进行辐照实验.借助离子梯度减能装置,使入射离子能量在0.22—6.17 MeV/u之间变化,从而在样品表面至24μm深度范围内产生0.05—0.20 dpa的原子离位损伤坪区.利用纳米压痕仪测试样品辐照前后的显微硬度,通过连续刚度测量(constant stiffness measurement)得到低活化钢硬度的深度剖面信息.使用Nix-Gao模型很好地描述了纳米压痕硬度随深度递减的现象(压痕尺寸效应,indentation size effect),从而有效避免了低能离子辐照的软基体效应(softer substrate effect).正电子湮灭寿命谱显示低活化钢在辐照之后长寿命成分增加,说明样品中产生了大量缺陷形成空位团,从而导致了材料力学性能的变化,在离子辐照剂量增加至0.2 dpa时,平均寿命τ_m增加量逐渐变慢,材料中辐照产生的缺陷趋于饱和.     

Study of defect evolution by TEM with in situ ion irradiation and coordinated modeling

The paper describes a novel transmission electron microscopy (TEM) experiment with in situ ion irradiation designed to improve and validate a computer model. TEM thin foils of molybdenum were irradiated in situ by 1?MeV Kr ions up to ～0.045 displacements per atom (dpa) at 80°C at three dose rates ?5?×?10^?6, 5?×?10^?5, and 5?×?10^?4?dpa/s – at the Argonne IVEM-Tandem Facility. The low-dose experiments produced visible defect structure in dislocation loops, allowing accurate, quantitative measurements of defect number density and size distribution. Weak beam dark-field plane-view images were used to obtain defect density and size distribution as functions of foil thickness, dose, and dose rate. Diffraction contrast electron tomography was performed to image defect clusters through the foil thickness and measure their depth distribution. A spatially dependent cluster dynamic model was developed explicitly to model the damage by 1?MeV Kr ion irradiation in an Mo thin foil with temporal and spatial dependence of defect distribution. The set of quantitative data of visible defects was used to improve and validate the computer model. It was shown that the thin foil thickness is an important variable in determining the defect distribution. This additional spatial dimension allowed direct comparison between the model and experiments of defect structures. The defect loss to the surfaces in an irradiated thin foil was modeled successfully. TEM with in situ ion irradiation of Mo thin foils was also explicitly designed to compare with neutron irradiation data of the identical material that will be used to validate the model developed for thin foils.     

利用HIRFL高能重离子束的核能材料辐照损伤研究

载能重离子与高能中子在材料中能够产生相似的级联碰撞损伤,加之重离子具有大的离位损伤截面和在材料样品中低的感生放射性,载能重离子束成为模拟先进核能装置内部结构材料辐照损伤的重要手段。HIRFL能区的重离子在结构材料中的射程一般远大于晶粒尺寸,因此能够产生材料体损伤,借助小样品技术可以获得材料力学性能变化（尤其辐照脆化）的有用信息,为探讨材料辐照损伤微结构和宏观力学性能变化的关联提供了重要条件。本文简要介绍了近年来我们基于HIRFL高能离子束开展的聚变堆候选材料辐照损伤的研究,包括低活化钢的辐照脆化行为、氧化物弥散强化（ODS）铁素体钢的结构优化对于抗辐照性能的影响、不同载能粒子辐照条件下铁素体/马氏体钢的辐照肿胀数据的关联,以及高能重离子辐照的钨材料中氢同位素的滞留行为。研究表明,结合特殊的测试技术及数据分析方法,高能重离子可作为核能结构材料辐照损伤研究及评估的有效手段。Because of the similarity in cascade damage structure in materials produced by energetic heavy ions and by fast neutrons, and the high displacement rate and low induced radioactivity of samples by heavy ions, heavy ion beam becomes an important tool to simulate radiation damage by energetic neutrons in materials in advanced nuclear energy systems. The ranges of heavy ions provided by HIRFL (Heavy Ion Research Facility in Lanzhou) are generally much larger than the mean dimensions of grains in alloys candidate to advanced nuclear reactors, and is capable of producing radiation damage in bulk scale. It therefore makes possible the evaluation of change of mechanical properties including the radiation induced embrittlement from the irradiated specimens by using miniaturized specimen techniques. In the present paper, we provide an introduction of our recent studies of radiation damage of materials candidate to future fusion reactors by utilizing heavy ion beams in HIRFL.The studies include issues as follows:ductility loss of RAFM steels causes by high-energy Ne ions, impact of oxide dispersoids on the radiation resistance of ODS ferritic steels, correlation of void swelling of ferritic/martensitic steels under different particle irradiation, and behavior of deuterium retention in tungsten under irradiation with high-energy heavy ions. The results show that high-energy heavy ions can be used as a tool to efficiently investigate or evaluate radiation damage in structure materials if combined with some special test techniques and data analysis.     

Radiation defect clusters in electron-irradiated silicon

Radiation defect formation in Czochralski-grown (pulled) and vacuum float-zone n-Si (ρ=15 to 150 ωcm) irradiated by electrons with energy E_e=2.5 to 1200 MeV has been studied. The results have been obtained from an analysis of the dose, energy and temperature dependences of the concentration n, Hall mobility μ _n , and charge-carrier lifetime τ. The experimentally observed peculiarities in the variation of n, μ _n , and τ irradiation by electrons with E10 MeV have been explained taking into account the formation of radiation defect clusters in the bulk of the crystal induced by such electrons. The correlation coefficients K_i have bsen obtained which take into consideration the “evolution” of primary displacement cascades in the location of which clusters are formed. The parameters of radiation defect clusters produced by electrons of different energies have been calculated using these coefficients.     

Optical waveguides in LiNbO3 formed by ion implantation

Abstract

Ion implantation in LiNbO₃ can be used to modify the refractive index. The change in indices, n ₀ n _e results from the damage formed by energy deposited by the (dE/dx)_nuclear collisions between the ions and the lattice and is independent of the ion species. A saturation change in index of some ?7% occurs after a deposition of 10²³ keV cm^?3 at 300K, greater changes of ?9 % occur with implants at 77K. Annealing studies indicate the optical absorption formed during irradiation is removed below 200°C whereas the index changes exist up to 400°C. For optical waveguide production a negative change in the index is not ideal as the damaged layer cannot directly act as the region of optical confinement. However the (dE/dx)_electronic term is unimportant and so we have been able to form optical waveguides by ion implantation with light energetic ions (e.g. MeV He⁺ ions) because the damaged layer is then formed beneath an unchanged high index surface layer. This retains the desirable electrooptic properties of the single crystal LiNbO₃. The experimentally observed waveguide modes are in accord with our theoretical predictions of the refractive index profiles.     

Correlation functions in the theory of atomic collision cascades: Ion location and the distribution in depth and size of damage clusters

Abstract

Simple depth distribution functions of ion bombardment damage predict the spatial extension of the cumulative damage caused by a beam of ions. Correlation functions need to be considered when more detailed information is desirable, such as the average size or depth of individual damage clusters, the average location of an ion within its damage cluster, and the fluctuations of these quantities. In this paper we establish an integral equation for the pair correlation function, coupling the individual ion range with the deposited energy. This pair correlation function determines the damage caused by all those ions that come to rest at a specific penetration depth. Solutions of the integral equation are found by standard methods. Explicit results are presented for elastic scattering governed by power cross sections. The depth distribution of damage clusters turns out to be significantly narrower than the gross damage distribution at all mass ratios except for M ₁ ? M ₂, and the size distribution appears insensitive to depth when measured perpendicular to the ion beam, but varying with depth when measured parallel. Predictions on ion location suffer from a surprizingly sensitive dependence on the scattering cross section. A note on the fluctuation of the sputtering yield by individual ions concludes the paper.     

Stored energy recovery of irradiated copper

Abstract

The stored energy released in Stage I recovery of reactor neutron irradiated copper was measured by differential thermal analysis calorimetry for three fluences up to a maximum of 3.5 × 10¹⁸ n/cm² (E>0.1 MeV) after irradiation at temperatures of less than 10 K. The stored energy dependence upon fluence, and a tendency toward saturation, were observed. Theoretical reaction rate processes were compared directly to the experimental rates of stored energy release, and the parameters associated with the theory were compared with results from previous resistivity measurements. Good agreement was found in several parameters, but major differences with previous D + E substage results lead to the conclusion that the point defect model may not describe materials experiencing severe neutron damage. Computer studies of warmup rates were made for first and second order and for correlated recovery processes as a function of defect concentration and of external power input. First and second order processes show definite distortion in their recovery rate curves for high defect concentrations; the correlated recovery process shows a much less pronounced effect.

This investigation of stored energy used several new approaches. The use of one sample in both experimental and control roles was not unique, but the use of induced radioactivity within the sample as the heating source, and the use of computer generated theoretical stored energy release curves to analyze the data were unique.     

Optical spectroscopy study of modifications induced in cerium dioxide by electron and ion irradiations

UV-visible absorption spectroscopy and Raman spectroscopy were used to study damage production in cerium dioxide epitaxial films and polycrystalline sintered samples after irradiation with electrons for three energies to span the threshold displacement energies of cerium and oxygen atoms, and 2.4-MeV Cu ions. Neither amorphization nor specific colour-centre bands were detected. Evolutions of the refractive index were derived from the interference fringes in the optical transmission spectra of epilayers after irradiation. No significant change of the refractive index occurred for the 1.0-MeV electron irradiation, whereas a maximum decrease by 28?±?8% was deduced for the 1.4-MeV and 2.5-MeV energies. These modifications are consistent with ballistic damage on the cerium sublattice for high electron energies producing Ce³⁺ ions. However, no significant change of refractive index was found for the Cu ion irradiation. This likely stems from the high rate of Frenkel pair recombination in the collision cascades induced by more energetic recoils than for the electron irradiations, combined with electronic excitations and hole capture on Ce³⁺ ions. This study reveals modifications of the electronic structure upon irradiation that could take place in other non-amorphizable oxide systems.