Guang-Hong Lu

Investigating behaviours of hydrogen in a tungsten grain boundary by first principles: from dissolution and diffusion to a trapping mechanism

We have investigated the dissolution, segregation and diffusion of hydrogen (H) in a tungsten (W) grain boundary (GB) using a first-principles method in order to understand the GB trapping mechanism of H. Optimal charge density plays an essential role in such a GB trapping mechanism. Dissolution and segregation of H are directly associated with the optimal charge density, which can be reflected by the H solution and segregation energy sequence for the different interstitial sites. To occupy the optimal-charge-density site, H can be easily trapped by the W GB with the solution and segregation energy of −0.23 eV and −1.11 eV, respectively. Kinetically, such a trapping is easier to realize due to the much lower diffusion barrier of 0.13–0.16 eV from the bulk to the GB in comparison with the segregation energy, suggesting that it is quite difficult for the trapped H to escape out of the GB. However, the GB can hold no more than 2 H atoms because the isosurface of optimal charge density almost disappears with the second H atom in, leading to the conclusion that H2 molecule and thus H bubble cannot form in the W GB. Taking into account the lower vacancy formation energy in the GB as compared with the bulk, we propose that the experimentally observed H bubble formation in the W GB should be via a vacancy trapping mechanism.

A review of modelling and simulation of hydrogen behaviour in tungsten at different scales

Tungsten (W) is considered to be one of the most promising plasma-facing materials (PFMs) for next-step fusion energy systems. However, as a PFM, W will be subjected to extremely high fluxes of low-energy hydrogen (H) isotopes, leading to retention of H isotopes and blistering in W, which will degrade the thermal and mechanical properties of W. Modelling and simulation are indispensable to understand the behaviour of H isotopes including dissolution, diffusion, accumulation and bubble formation, which can contribute directly to the design, preparation and application of W as a PFM under a fusion environment. This paper reviews the recent findings regarding the behaviour of H in W obtained via modelling and simulation at different scales.

First-principles study of He effects in a bcc Fe grain boundary: site preference, segregation and theoretical tensile strength

We perform a first-principles calculation to investigate the effects of He in an Fe Σ5(310)/[001] grain boundary (GB) with the SIESTA code, for which the reliability of the pseudopotential and the basis set are systematically tested. We calculate the formation and segregation energies for different substitutional and interstitial cases in order to determine the site preference and the segregation properties of He in the Fe GB. It is demonstrated that the He segregation either breaks (substitution) or weakens (interstitial) the surrounding interfacial Fe-Fe bonds, leading to the GB tensile strength reduction.

Theoretical strength and charge redistribution of fcc Ni in tension and shear

We employ a first-principles total-energy method to investigate the theoretical tensile and shear strengths of fcc Ni systematically. The theoretical tensile strengths are shown to be 36.1, 10.5 and 34.1 GPa in the [001], [110] and [111] directions, respectively. We indicate that [110] is the weakest direction due to the formation of an instable bct ‘phase’ in the tensile process. The theoretical shear strengths are, respectively, 5.1 and 15.8 GPa in the ‘easy’ and ‘hard’ directions in the {111}� 112� slip system, and 6.4 GPa in the {111}� 110� slip system. Both the tensile and the shear strengths are consistent with either experimental or theoretical values. The different shear strengths in the ‘easy’ and ‘hard’ directions originate from the different charge redistribution under the shear strain. The shear strain along the ‘easy’ direction of [112] results in a charge distributed in the � 001� which forms a directional bond, while the strain along the ‘hard’ direction of [112] makes the charge extend to the whole {111} interlayers. (Some figures in this article are in colour only in the electronic version)

Towards theoretical connection between tensile strength of a grain boundary and segregated impurity concentration: Helium in iron as an example

A theoretical method is proposed to investigate the tensile strength dependence on the impurity concentration in metals using a first-principles method in combination with the classical thermodynamics models. In the present study, helium (He) in an iron (Fe) grain boundary (GB) is taken as an example. The theoretical tensile strength of an FeΣ5(310)/[001] GB with different amounts of He impurity is determined using first-principles computational tensile tests (FPCTT) and the He concentration is derived depending on the solution energy and temperature using thermodynamics models. Thus, the dependence of the tensile strength of an Fe GB on He concentration is established, and a critical He concentration is defined using the amount of the tensile strength reduction compared with that of a clean GB. Such a method is expected to be quite useful in predicting the impurity-induced degradation of the mechanical properties of metals.

Dissolution, diffusion and permeation behavior of hydrogen in vanadium: a first-principles investigation.

Employing a first-principles method, we have studied the stability, diffusivity, and permeation properties of hydrogen (H) and its isotopes in bcc vanadium (V). A single H atom is found to favor the tetrahedral interstitial site (TIS) in V. The charge density distribution exhibits a strong interaction between H and its neighbor V atoms. Analysis of DOS and Bader charge reveals that the occupation number of H-induced low energy states is directly associated with the stability of H in V. Further, H is shown to diffuse between the neighboring TISs with a diffusion barrier of 0.07 eV. Diffusion coefficients and permeabilities of H isotopes in V are estimated with empirical theory. At a typical temperature of 800 K, the diffusion coefficient and the permeability of H are 2.48 × 10(-4) cm(2) s(-1) and 2.19 × 10(-9) mol m(-1) s(-1) Pa(- 1/2), respectively.

First-principles study of the effects of segregated Ga on an Al grain boundary

The effects of different amounts of segregated Ga (substitutional) on an Al grain boundary have been investigated by using a first-principles pseudopotential method. The segregated Ga is found to draw charge from the surrounding Al due to the electronegativity difference between Ga and Al, leading to a charge density reduction between Ga and Al as well as along the Al grain boundary. Such an effect can be enhanced by increasing the Ga segregation amount. With further Ga segregated, in addition to the charge-drawing effect that occurs in the Al–Ga interface, a heterogeneous α-Ga-like phase can form in the grain boundary, which greatly alters the boundary structure. These effects are suggested to be responsible for Ga-induced Al intergranular embrittlement.

Dissolution and diffusion properties of carbon in tungsten

We have investigated the structure, solution and diffusion behavior of carbon (C) in tungsten (W) based on first-principles calculations. The single C atom is energetically favorable sitting at the octahedral interstitial site (OIS) with a solution energy of 0.78 eV in W. Double C atoms tend to be paired up at the two neighboring OISs along the (210) direction with a distance of ∼ 3.57 Å and a binding energy of + 0.50 eV. This suggests that a positive attractive interaction between C atoms exists, which might lead to a local higher concentration of C in W and form carbide. Kinetically, the C and vacancy diffusion co-efficients as a function of temperature have been determined, and are 1.32 × 10(-19) m(2) s(-1) and 3.11 × 10(-23) m(2) s(-1) at a typical temperature of 600 K, respectively.

Structure and stability of He and He–vacancy clusters at a Σ5(310)/[001] grain boundary in bcc Fe from first-principles

We have studied the atomic structure and energetic stability of helium (He) and He-vacancy clusters in an iron (Fe) Σ5(310)/[001] grain boundary (GB) using a first-principles method. The He and He-vacancy clusters in the Fe GB are shown to exhibit high-symmetry structures. The equilibrium He-He distance in the clusters is ~1.70 Å, much smaller than 2.80 Å in the vacuum or 2.94 Å in a face centred cubic (fcc) crystal, indicating the attractive interaction between the He atoms due to the presence of Fe. The charge density surrounding He is demonstrated to decrease with an increasing number of He atoms in the clusters, leading to a positive binding energy of a He atom to the clusters. This suggests He and He-vacancy clusters can energetically trap more He atoms, which is responsible for the growth of the He-related clusters (He and He-vacancy clusters) and thus the He bubbles in the GB. The binding energy of an interstitial He atom to the He-related clusters is found generally lower in the GB than in a bcc crystal. Besides, the binding strengths of small He clusters to the GB and to a vacancy in a bcc matrix are compared, and the latter shows greater trapping strength to an interstitial He and a He(2) cluster. The magnetism of the Fe atoms near the GB as well as its variation caused by the He-related clusters is also investigated. The local magnetic moment variation of the Fe atoms in the system is enhanced to a different extent, depending on the size of the He-related clusters.

Deuterium occupation of vacancy-type defects in argon-damaged tungsten exposed to high flux and low energy deuterium plasma

Doppler broadening spectroscopy in the positron annihilation technique (DBS-PA) has been employed to investigate the defect properties in argon-damaged tungsten exposed to low-energy and high flux deuterium plasma. Argon ion irradiations with energy 500 keV are performed for tungsten samples with various levels of damage. The remarkable increment of the S parameter in DBS-PA indicates the introduction of vacancy-type defects in argon irradiated tungsten. An increase of ion fluence results in a continuous increase of the S parameter until saturation. Unexpectedly, a much higher fluence leads to a decrease of the S parameter in the near surface, and the (S,W) slope changes greatly. This should be associated with the formation of argon-vacancy complexes in the near surface produced by the excessive implanted argon ions. With deuterium plasma exposure, a significant decrease of the S parameter occurs in the pre-irradiated tungsten, suggesting the sharp reduction of the number and density of the vacancy-type defects. The thermal desorption spectroscopy results demonstrate that the argon-damaged tungsten, compared to the pristine one, exhibits an enhanced low-temperature desorption peak and an additional and broad high-temperature desorption peak, which indicates that deuterium atoms are trapped in both low-energy and high-energy sites. All these observations directly indicate the deuterium occupation of irradiation-induced vacancy defects in damaged tungsten, which is responsible for the remarkable increase of the deuterium retention in comparison with the pristine one.