Unique phenomena of tungsten associated with fusion reactor: uncertainties of stable hydrogen configuration tapped in tungsten vacancy

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1 Unique phenomena of tungsten associated with fusion reactor: uncertainties of stable hydrogen configuration tapped in tungsten vacancy Kyushu University Kazuhito Ohsawa Technical Meeting of the International Code Centre Network Simulation of Plasma-Material Interaction Experiments IAEA Vienna, July 2015 Out line 1. Introduction of unique phenomena of W as an example 2. Abnormal configuration in W mono-vacancy application of random sampling 3. Zero point energy calculations

2 Back Ground of this work ITER divertor In fusion reactor (ITER), divertor armor is exposed to extremely large fluence of plasma particle, isotopes D, T, heluium (e), and heat flux. In order to protect the sever irradiation, tungsten (W) is considered as a plausible candidate for plasma facing materials in fusion reactor. Advantage of tungsten as plasma facing materials 1. ighest melting point of all the pure metals Low hydrogen solubility +1.1eV par 3. Low sputtering erosion 4. igh thermal conductivity 5. Low induced radioactivity, compared with molybdenum (Mo)

3 Some unique properties of tungsten are observed by the studies of fusion reactor materials. Why do unique phenomena happen in tungsten associated with fusion reactor? Of course, fusion reactor is an innovative technology. Plasma e e e e Schematic view of and e irradiation to W specimen e e W specimen and e compulsorily introduced in W 1. Negative formation energy of di-vacancy in tungsten 2. e 2 migrates more quickly than a single e atom at T < 400K 3. Fibreform tungsten covering surface by e irradiarion 4. Abnormal configuration in W nomo-vacancy 5. etc.

4 1. Negative formation energy of di-vacancy in tungsten 2. e 2 migrates more quickly than a single e atom at T < 400K Y.L. Zhou et. al. J. Nucl. Mater. 446 (2014) 49 Fe L. Ventelon et. al. J. Nucl. Mater. 425 (2012) 16

5 3. Fibreform tungsten covering surface by e irradiation 4. Abnormal confuguration in W mono-vacancy W K. Ohsawa et. al. Phys. Rev. B 82 (2010) Phys. Rev. B 85 (2012) S. Kajita et. al. Nucl. Fusion 49 (2009) Nucl. Fusion 49 (2009) I would like to talk about this topic.

6 Main subject Abnormal stable configuration of atoms in W mono-vacancy ow many hydrogen atoms are accommodated in a vacancy in tungsten and other bcc transition metals? What is abnormal stable configuration of ydrogen in vacancy?

7 Ionic compound hydrogen storage type Δ<0 anti hydrgen storage type Δ>0 I II III IV V VI VII covalent compound Li Be B C N O F Ne Group V, VI, and Fe Na Mg Al Si P S Cl Ar III IV V VI VII VIII IX X XI XII K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr 0 e 5 Rb Sr Y Zr Nb Mo Tc Ru Rh Pb Ag Cd In Sn Sb Te I Xe 6 Cs Ba La f Ta W Re Os Ir Pt Au g Tl Pb Bi Po At Rn 7 Fr Ra Ac BCC metal BCC metal La Ce Pr Nd Pm Sm Eu Gd Tb Dy o Er Tm Tb Lu Ac Th Pa U Np Pu Am Cm Bk

8 Simulation method First-principle calculation Vienna ab-initio simulation package (VASP) Perdew-Burke-Ernzerhof (PBE) potential Super cell size 3x3x3 (54) bcc lattice For W, 5x5x5 (432) lattice is also used Plane wave cau-off energy is 350 ev Atomic relaxation are iterated until a break condition is satisfied (0.003eV/A ) Initial atom position Electronic relaxation no Break condition yes Finish Ionic relaxation relaxation process

9 Review of ydrogen in BCC metals Interstitial atom prefers in bulk BCC metals. Metal Metal Tetrahedral interstitial site () Octahedral interstitial site (O-site) is more favorable for than O-site. W 0.380eV Mo 0.265eV Fe 0.131eV Nb 0.271

10 normal stable configuration of atoms in mono-vacancy in bcc transition metals O-site vacancy Usually, a maximum of 6 atoms are trapped. This was established theory but we decided to investigate stable configuration more carefully 6 6 s regular tetrahedral configuration

11 Initial atom positions for ionic relaxation atoms are located inner surface of vacancy. O-site Initial distribution S 2 Initial configuration for atoms are randomly generated within a area. Usually, S 1 =0.4d, S 2 =0.2d The purpose of meeting is uncertainty quantification. This is an application of the random sampling. S 1 d About 30 % initial configurations arrive at true ground-state structure. Many Initial atom position relaxation not finish stable meta-stable

12 <010> direction (d ) Results of application of random generate initial configuration (a) Stable configurations of multiple atoms in W mono-vacancy single atom in monovacancy W A single atom is located close to O-site on inner surface of a monovacancy. But d O-site 1 {001} <100> direction (d ) stable positions of projected onto the {001} plane

13 <010> direction (d ) W W W 4 atom in monovacancy d d d ground state eV degenerate eV planar structure eV O-site 1 {001} <100> direction (d )

14 <010> direction (d ) 6 atom in monovacancy W W d d degenerate ground state eV degenerate ground state eV O-site -0.2 {001} <100> direction (d ) W d regular octahedral structure unstable Stable positions for are gradually shifted toward the eV

15 <010> direction (d ) 12 atom in monovacancy W d ground state eV Repulsive interaction of O-site {001} <100> direction (d )

16 Finally, we would like to answer the first question. The total binding energy of multiple atoms to metal vacancy e k T V E M V k E M E M E M n-1 n-1 k n-1 n

17 (ev) Short summary of the simulations Group 5 transition metals (V, Nb, Ta) and Cr and Fe A maximum of atoms trapped in mono-vacancy is 6. Normal stable configuration of the multiple atom. W and Mo vacancy can accommodate a maximum of 12 atoms. configurations are abnormal. New question Why are so many trapped in W and Mo vacancy? at release large energy when trapped in vacancy molecule (in vacuum) at 0.328eV V Nb Ta in vacancy 1.015eV Cr Mo W in vacancy Fe W and Mo have large vacancy. lattice constant W 3.16A Mo 3.15A Cr 2.88A Fe 2.85A

18 What is relation of our woks and uncertainty quantification? Main purpose of this meeting is uncertainty quantification (UQ) activities. Initial positions of atoms are determined by assuming a random distribution. This is an important application of random sampling. In the present works, we determine the parameter S 1 and S 2 appropriately. But if we perform more complicated simulations, we have to do same optimization of the method. O-site Initial distribution S 2 S 1 d

19 Application: zero point energy calculation 2 D 3 T 4 e MeV n 14.06MeV Abnormal configurations are applied to calculations of zero point energy. We can calculate vibration energy from abnormal configuration. Ground state Saddle point = unstable Schematic view of vibration

20 Summary and conclusion 1. The abnormal atom configurations are found in W and Mo mono-vacancy by first-principle calculations. 2. A maximum of 12 atoms can be accommodated in the vacancy. 3. The abnormal configurations can be applied to calculations of zero point energy. W or Mo 12 bcc metals 4. configurations in mono-vacancy of other bcc transition metal (V, Nb, Ta, Cr, Fe) are normal ones. 5. A maximum of 6 atoms are accommodated in it, which are good agreement with established theory. 6

21 References Negative formation energy for di-vacancy C.S. Becquart and C. Domain Nucl. Instr. Meth. In Phys. Res. B 255 (2007) L. Ventelon, F. Willaime, C.-C. Fu, M. eran, I. Ginoux J. Nucl. Mater. 425 (2012) e 2 migration Y.L. Zhou, J. Wang, Q. ou, A.. Deng J. Nucl. Mater. 446 (2014) Namometre-sized fibreform tungsten S. Kajita, W. Sakaguchi, N. Ohno, N. Yoshida, T. Saeki Nucl. Fusion 49 (2009) Abnormal configuration in W mono-vacancy K. Ohsawa, J. Goto, M. Yamakami, M. Yamaguchi, M. Yagi Phys. Rev. B 82 (2010) K. Ohsawa, K. Eguchi,. Watanabe, M. Yamaguchi, M. Yagi Phys. Rev. B 85 (2012) K. Ohsawa, F. Nakamori, Y. atano, M. Yamaguchi J. Nucl. Mater. 458 (2015)

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