Materials used in commercial D-T fusion reactors will be exposed to irradiation and a mixture of helium and hydrogen plasma. Modeling the microstructural evolution of such materials requires the use of large-scale molecular dynamics simulations. The focus of this study is to develop a fast EAM potential for the interactions among the three elements (W, H, and He), fitted to accurately reproduce both the ab initio formation energies and relaxation volumes of small defect clusters containing light gases within tungsten. The potential enables the study of tungsten under irradiation and in the presence of light gases. To demonstrate the utility of the potential, we construct a thermodynamically motivated model for predicting the energetics of light-gas-filled voids. The model is then validated through molecular dynamics simulations with our new potential.
The changing thermal conductivity of an irradiated material is among the principal design considerations for any nuclear reactor, but at present few models are capable of predicting these changes starting from an arbitrary atomistic model. Here we present a simple model for computing the thermal diffusivity of tungsten, based on the conductivity of the perfect crystal and resistivity per Frenkel pair, and dividing a simulation into perfect and athermal regions statistically. This is applied to highly irradiated microstructures simulated with Molecular Dynamics. A comparison to experiment shows…
Elastic interactions play an important role in controlling irradiation damage evolution, but remain largely unexplored experimentally. Using transmission electron microscopy (TEM) and high-resolution on-axis transmission Kikuchi diffraction (HR-TKD), we correlate the evolution of irradiation-induced damage structures and the associated lattice strains in self-ion irradiated pure tungsten. TEM reveals different dislocation loop structures as a function of sample thickness, suggesting that free surfaces limit the formation of extended defect structures found in thicker samples. HR-TKD strain ana…
Helium-ion-induced swelling and blistering of single-crystal tungsten is investigated using a Helium Ion Microscope for site-specific dose-controlled irradiation (at 25 keV) with analysis by Helium Ion Microscopy, Atomic Force Microscopy and Transmission Electron Microscopy (cross-sectioning by Focused Ion Beam milling). Our measurements show that the blister cavity forms at the depth of the helium peak and that nanobubbles coalesce to form nanocracks within the envelope of the ion stopping range, causing swelling of the blister shell. These results provide the first direct experimental eviden…
Hydrogen isotopes are retained in materials for fusion power applications, changing both hydrogen embrittlement and tritium inventory as the microstructure undergoes irradiation damage. But modelling of highly damaged materials - exposed to over 0.1 displacements per atom (dpa) - where asymptotic saturation is observed, for example tungsten facing the plasma in a fusion tokamak reactor, is difficult because a highly damaged microstructure cannot be treated as weakly interacting isolated defect traps. In this paper we develop computational techniques to find the defect content in highly irradia…
The different point defects formed by two hydrogen atoms or two helium atoms in tungsten were investigated through first-principles calculation. The energetically favorable site for a hydrogen atom is tetrahedral interstitial site while substitutional site is the most preferred site for a helium atom. The formation energies of two hydrogen or helium atoms are determined by their positions, and there are not a multiple of a single atom's. After relaxation, two adjacent hydrogen atoms are away from each other while helium atoms are close to. The reasons for the interaction between two hydrogen o…
Using _in situ_ transmission electron microscopy (TEM), we have observed nanometre scale dislocation loops formed when an ultra-high-purity tungsten foil is irradiated with a very low fluence of self-ions. Analysis of the TEM images has revealed the largest loops to be predominantly of prismatic 1/2<111> type and of vacancy character. The formation of such dislocation loops is surprising since isolated loops are expected to be highly mobile, and should escape from the foil. In this work we show that the observed size and number density of loops can be explained by the fact that the loops are _…
Tungsten is the main candidate material for plasma-facing armour components in future fusion reactors. Bombardment with energetic fusion neutrons causes collision cascade damage and defect formation. Interaction of defects with helium, produced by transmutation and injected from the plasma, modifies defect retention and behaviour. Here we investigate the residual lattice strains caused by different doses of helium-ion-implantation into tungsten and tungsten-rhenium alloys. Energy and depth-resolved synchrotron X-ray micro-diffraction uniquely permits the measurement of lattice strain with sub-…
Understanding how properties of materials change due to nuclear transmutations is a major challenge for the design of structural components for a fusion power plant. In this study, by combining a first-principles matrix Hamiltonian approach with thermodynamic integration we investigate quasi-steady state configurations of multi-component alloys, containing defects, over a broad range of temperature and composition. The model enables simulating transmutation-induced segregation effects in materials, including tungsten where the phenomenon is strongly pronounced. Finite-temperature analysis show…
Damage dose dependence of deuterium retention in high-temperature self-ion irradiated tungsten
Max Planck Institute for Plasma Physics（马克斯·普朗克等离子体物理研究所）；Karlsruhe Institute of Technology (KIT), Institute for Applied Materials - Applied Materials Physics（卡尔斯鲁厄理工学院应用材料研究所）
The formation of helium cavities in coarse-grained materials produces hardening proportional to the number density and size of the cavities and due to the interaction of dislocations with intragranular helium defects. In nanostructured metals containing a high density of interfacial sinks, preferential cavity formation on the grain boundaries instead produces softening and often attributed to enhanced interfacial plasticity. Employing two grades of ultrafine-grained tungsten, we explore this effect using targeted implantation studies to map cavity evolution as a function of the irradiation con…
Reflection and implantation of low energy helium (He) ions by tungsten (W) substrate are studied using molecular dynamics (MD) simulations. Motivated by the ITER divertor design, our study considers a range of W substrate temperatures (300 K, 1000 K, 1500 K), a range of He atom incidence energies ($\le$100 eV) and a range of angles of incidence ($0^{\circ}$-$75^{\circ}$) with respect to substrate normal. The MD simulations quantify the reflection and implantation function, the integrated moments such as the particle/energy reflection coefficients and average implantation depths. Distributions …
Molecular dynamics simulations were performed to study the dependence of migration behaviours of single helium atoms near tungsten surfaces on the surface orientation and temperature. For W{100} and W{110} surfaces, He atoms can quickly escape out near the surface without accumulation even at a temperature of 400 K. The behaviours of helium atoms can be well-described by the theory of continuous diffusion of particles in a semi-infinite medium. For a W{111} surface, the situation is complex. Different types of trap mutations occur within the neighbouring region of the W{111} surface. The trap …
Understanding defect production and evolution under irradiation is a long-standing multi-scale problem. Conventionally, experimental examination of irradiation-induced defects (IIDs) has mainly relied on transmission electron microscopy (TEM), which offers high spatial resolution but requires destructive sample preparation. Furthermore, limited field of view and low strain sensitivity make multi-scale characterisation and quantitative strain measurements difficult. Here we explore the potential of using advanced techniques in the scanning electron microscope (SEM) to non-destructively probe ir…
Using X-ray micro-diffraction and surface acoustic wave spectroscopy, we measure lattice swelling and elastic modulus changes in a W-1%Re alloy after implantation with 3110 appm of helium. A fraction of a percent observed lattice expansion gives rise to an order of magnitude larger reduction in the surface acoustic wave velocity. A multiscale elasticity, molecular dynamics, and density functional theory model is applied to the interpretation of observations. The measured lattice swelling is consistent with the relaxation volume of self-interstitial and helium-filled vacancy defects that domina…
Object kinetic Monte Carlo simulations were performed to study the impact of varying dose rate and grain size up to a dose of 1.0 dpa in pure, polycrystalline tungsten, subjected to a neutron irradiation having a PKA spectrum corresponding to the High Flux Isotope Reactor. The present study models defect cluster accumulation in tungsten, but does not consider the impact of transmutation or pre-existing defects beyond the grain boundary sinks, with varying grain size. With increasing dose rate, the vacancy cluster density increases, while the number density of vacancies decreases. Accordingly, …
Predicting the dramatic changes in material properties caused by irradiation damage is key for the design of future nuclear fission and fusion reactors. Self-ion implantation is an attractive tool for mimicking the effects of neutron irradiation. However, the damaged layer of implanted samples is only few microns thick, making it difficult to estimate macroscopic properties. Here we address this challenge using a combination of experimental and modelling techniques. We concentrate on self-ion-implanted tungsten, the front-runner for fusion armour components and a prototypical bcc material. To …
Decoupling Strain-Rate Sensitivity and Deformation Length Scale Effects in Neutron-Irradiated Tungsten: A Coupled Nano-Indentation, HR-EBSD and Crystal Plasticity Study
Indian Institute of Science（印度科学学院）；University of Oxford（牛津大学）；UK Atomic Energy Authority（英国原子能管理局）
Tungsten is the main candidate material for plasma-facing armour components in future fusion reactors. In-service, fusion neutron irradiation creates lattice defects through collision cascades. Helium, injected from plasma, aggravates damage by increasing defect retention. Both can be mimicked using helium-ion-implantation. In a recent study on 3000 appm helium-implanted tungsten (W-3000He), we hypothesized helium-induced irradiation hardening, followed by softening during deformation. The hypothesis was founded on observations of large increase in hardness, substantial pile-up and slip-step f…
The production of energy through nuclear fusion poses serious challenges related to the stability and performance of materials in extreme conditions. In particular, the constant bombardment of the walls of the reactor with high doses of He ions is known to lead to deleterous changes in their microstructures. These changes follow from the aggregation of He into bubbles that can grow and blister, potentially leading to the contamination of the plasma, or to the degradation of their mechanical properties. We computationally study the behavior of small clusters of He atoms in W in conditions relev…
Based on the in-detail tracking of the movements of atoms in a large number of molecular dynamics simulation boxes, we find that the diffusion of H and He atoms in single-crystal W is composed of non-Markovian jumps. The waiting time distribution of the triggering of jumps is not the usually recognized exponential distribution, but a temperature-dependent power-law distribution. The power-law distribution of the waiting time may lead to clear ergodicity-breaking diffusion, a phenomenon that has formerly been reported to only occur in complex systems such as living biological cells or soft matt…
Despite well documented first-principles theoretical determination of the low migration energy (0.06 eV) of a single He in tungsten, fully quantum mechanical calculations on the migration of a He pair still present a challenge due to the complexity of its trajectory. By identifying the six most stable configurations of the He pair in W and decomposing its motion into rotational, translational, and rotational-translational routines, we are able to determine its migration barrier and trajectory. Our density functional theory calculations demonstrate a He pair has three modes of motion: a close o…
Under low energy and high flux/fluence irradiation of helium (He) atoms, the formation and bursting of He bubbles on tungsten (W) surfaces play important roles in the morphological evolution of component surfaces and impurity production in fusion reactors. Microscopically, the bursting of He bubbles is a stochastic process, and He bubbles have statistically average lifetimes. In the present paper, a molecular dynamics-based method was developed to extract, for the first time, the lifetime of He bubbles near tungsten surfaces. It was found that He bubble bursting can be treated as an activated …
Graph neural network prediction of temperature-dependent hydrogen diffusion and thermal conductivity tensors of tungsten containing helium bubbles and grain boundaries
Graduate School of Science and Engineering, Yamagata University（山形大学理工学研究科）；National Institute for Fusion Science（国立研究開発法人核融合科学研究所）
Molecular dynamics (MD) simulations were performed to study the cumulative bombardments of low-energy (60-200 eV) helium (He) atoms on tungsten (W) surfaces. The behaviour of He and the response of the W surface were investigated. The He incident energy and tungsten temperature play important roles on the formation and growth of He clusters. The temperature can promote the coalescence of He clusters and increase the size of the He clusters. A stratification phenomenon of the He depth distribution has been observed. The rupture of the He clusters and, at the same time, the escape and re-deposit…
Mechanism of Oxygen Reduction via Chemical Affinity in NiO/SiO2 Interfaces Irradiated with keV Energy Hydrogen and Helium Ions for Heterostructure Fabrication
Combining spatially resolved X-ray Laue diffraction with atomic-scale simulations, we observe how ion-irradiated tungsten undergoes a series of non-linear structural transformations with increasing irradiation exposure. Nanoscale defect-induced deformations accumulating above 0.02 displacements per atom (dpa) lead to highly fluctuating strains at ~0.1 dpa, collapsing into a driven quasi-steady structural state above ~1 dpa. The driven asymptotic state is characterized by finely dispersed vacancy defects coexisting with an extended dislocation network, and exhibits positive volumetric swelling …
Properties of point defects resulting from the incorporation of inert-gas atoms in bcc tungsten are investigated systematically using first-principles density functional theory (DFT) calculations. The most stable configuration for the interstitial neon, argon, krypton and xenon atoms is the tetrahedral site, similarly to what was found earlier for helium in W. The calculated formation energies for single inert-gas atoms at interstitial sites as well as at substitutional sites are much larger for Ne, Ar, Kr and Xe than for He. While the variation of the energy of insertion of inert-gas defects …
Defect microstructures formed in ion-irradiated metals, for example iron or tungsten, often exhibit patterns of spatially ordered nano-scale dislocation loops. We show that such ordered dislocation loop structures may form spontaneously as a result of Brownian motion of loops, biased by the angular-dependent elastic interaction between the loops. Patterns of spatially ordered loops form once the local density of loops produced by ion irradiation exceeds a critical threshold value.
Ti3SiC2 is a potential structural material for nuclear reactor applications. However, He irradiation effects in this material are not well understood, especially at high temperatures. Here, we compare the effects of He irradiation in Ti3SiC2 at room temperature (RT) and at 750 °C. Irradiation at 750 °C was found to lead to extremely elongated He bubbles that are concentrated in the nano-laminate layers of Ti3SiC2, whereas the overall crystal structure of the material remained intact. In contrast, at RT, the layered structure was significantly damaged and highly disordered after irradiation. Ou…
A novel computational treatment of dense, stiff, coupled reaction rate equations is introduced to study the nucleation, growth, and possible coalescence of cavities during neutron irradiation of metals. Radiation damage is modeled by the creation of Frenkel pair defects and helium impurity atoms. A multi-dimensional cluster size distribution function allows independent evolution of the vacancy and helium content of cavities, distinguishing voids and bubbles. A model with sessile cavities and no cluster-cluster coalescence can result in a bimodal final cavity size distribution with coexistence …
The economical lifetime of the divertor is a key concern for realizing nuclear fusion reactors that may solve the world's energy problem. A main risk is thermo-mechanical failure of the plasma-facing tungsten monoblocks, as a consequence of irradiation hardening induced by neutron displacement cascades. Lifetime extensions that could be carried out without prolonged maintenance periods are desired. In this work, the effects of potential treatments for extending the lifetime of an operational reactor are explored. The proposed treatments make use of cyclic recrystallization processes that can o…
The purpose of this short contribution is to report on the development of a Spectral Neighbor Analysis Potential (SNAP) for tungsten. We have focused on the characterization of elastic and defect properties of the pure material in order to support molecular dynamics simulations of plasma-facing materials in fusion reactors. A parallel genetic algorithm approach was used to efficiently search for fitting parameters optimized against a large number of objective functions. In addition, we have shown that this many-body tungsten potential can be used in conjunction with a simple helium pair potent…
We carry out generalized-ensemble molecular dynamics simulations of the formation of small Helium (He) clusters in bulk Tungsten (W), a process of practical relevance for fusion energy production. We calculate formation free energies of small Helium clusters at temperatures up to the melting point of W, encompassing the whole range of interest for fusion-energy production. From this, parameters like cluster break-up or formation rates can be calculated, which help to refine models of microstructure evolution in He-irradiated Tungsten.
Ab initio calculations have been performed to clarify the primary behaviors of He atoms in vanadium and to generate the database for the development of the interatomic potential for V-He system within the framework of the"s-band"model.The calculated formation energies of the tetrahedral,octahedral and substitutional He defects,as well as those for He2,He3 and He2V clusters are reasonable when compared with relevant experimental results and ab initio calculations under the same conditions.The applicability of the present V-He potential for atomistic simulations to investigate the moving,cluster…
A recently developed reduced activation ferritic/martensitic steel MNHS was irradiated with 200keV He ions to a fluence of 1E21ions/m^2 at 450 celsius degree and 1E20ions/m^2 at 300 celsius degree and 450 celsius degree, respectively. The irradiation hardening of the steel was investigated by nanoindentation measurements combined with transmission electron microscopy (TEM) analysis. Dispersed barrier-hardening (DBH) model was applied to predict the hardness increments based on TEM analysis. The predicted hardness increments are consistent with the values obtained by nanoindentation tests. It i…
Precise and scalable defect engineering of 2D nanomaterials is acutely sought-after in contemporary materials science. Here we present defect engineering in monolayer graphene and molybdenum disulfide (MoS$_2$) by irradiation with noble gas ions at 30 keV. Two ion species of different masses were used in a gas field ion source microscope: helium (He$^+$) and neon (Ne$^+$). A detailed study of the introduced defect sizes and resulting inter-defect distance with escalating ion dose was performed using Raman spectroscopy. Expanding on existing models, we found that the average defect size is cons…
Here, we report a study on the radiation resistance enhancement of Gd2Zr2O7 nanograin ceramics, in which amorphization, cell volume expansion and multi-stage helium (He) bubble formation are investigated and discussed. Gd2Zr2O7 ceramics with a series of grain sizes (55-221 nm) were synthesized and irradiated by 190 keV He ion beam up to a fluence of 5x10^17 ions/cm2. Both the degree of post irradiation cell volume expansion and the amorphization fraction appear to be size dependent. As the average grain size evolves from 55 to 221 nm, the degree of post irradiation cell volume expansion increa…
The experimental research on the irradiation of the functional design materials by the Helium ions in the linear accelerator is conducted. The experimental measurements techniques and data on the irradiation of the functional design materials by the Helium ions with the energy up to 4 MeV, including the detailed scheme of experimental measurements setup, are presented. The new design of accelerating structure of the IH-type such as POS-4, using the method of alternate-phase focusing with the step-by-step change of the synchronous phase along the focusing periods in a linear accelerator, is dev…
