Journal of Nuclear Materials 463 (2015) 109–115

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Journal of Nuclear Materials

journal homepage: www.elsevier.com/locate/jnucmat

Hybrid simulation research on formation mechanism of tungsten

nanostructure induced by helium plasma irradiation
Atsushi M. Ito a,⇑,1, Arimichi Takayama a, Yasuhiro Oda a, Tomoyuki Tamura b, Ryo Kobayashi b,
Tatsunori Hattori b, Shuji Ogata b, Noriyasu Ohno c, Shin Kajita c, Miyuki Yajima a, Yasuyuki Noiri c,
Yoshihide Yoshimoto d, Seiki Saito e, Shuichi Takamura f, Takahiro Murashima g, Mitsutaka Miyamoto h,
Hiroaki Nakamura a,c
a
National Institute for Fusion Science, 322-6 Oroshi-cho, Toki 509-5292, Japan
b
Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555, Japan
c
Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8603, Japan
d
University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
e
Kushiro National College of Technology, Kushiro, Hokkaido 084-0916, Japan
f
Aichi Institute of Technology, 1247 Yachigusa, Yakusa-cho, Toyota 470-0392, Japan
g
Tohoku University, 6-3, Aramaki-Aza-Aoba, Aoba-Ward, Sendai 980-8578, Japan
h
Shimane University, Matsue, Shimane 690-8504, Japan

a r t i c l e i n f o a b s t r a c t

Article history: The generation of tungsten fuzzy nanostructure by exposure to helium plasma is one of the important
Available online 14 January 2015 problems for the use of tungsten material as divertor plates in nuclear fusion reactors. In the present
paper, the formation mechanisms of the helium bubble and the tungsten fuzzy nanostructure were inves-
tigated by using several simulation methods. We proposed the four-step process which is composed of
penetration step, diffusion and agglomeration step, helium bubble growth step, and fuzzy nanostructure
formation step. As the fourth step, the formation of the tungsten fuzzy nanostructure was successfully
reproduced by newly developed hybrid simulation combining between molecular dynamics and
Monte-Carlo method. The formation mechanism of tungsten fuzzy nanostructure observed by the hybrid
simulation is that concavity and convexity of the surface are enhanced by the bursting of helium bubbles
in the region around the concavity.
Ó 2015 Elsevier B.V. All rights reserved.

1. Introduction sten fuzzy nanostructure. The formation processes of the helium

The phenomenon that tungsten fuzzy nanostructure is gener-
ated by helium plasma irradiation was found from experimental
researches [1] on plasma-wall interaction for nuclear fusion reac-
tors. The tungsten fuzzy nanostructure will cause the decrease of
the mechanical property and heat conductance of the tungsten
material. These are problems in the use for divertor plates in
nuclear fusion reactors. The formation conditions of the tungsten
fuzzy nanostructure, that is, temperature, incident energy, flux,
and fluence dependencies have been researched by experimental
approaches [2–4].
The theoretical approaches mainly have been used to clarify the
mechanisms of the formation of the helium bubble and the tung-
⇑ Corresponding author.
E-mail address: ito.atsushi@nifs.ac.jp (A.M. Ito).
1
Presenting Author.
bubble and the fuzzy nanostructure are considered as multi-scale
multi-physical phenomena. To clarify the complicated phenomena,
the many kinds of elemental processes in tungsten material have
been investigated by using some kinds of simulation methods,
such as the binary collision approximation (BCA) [5,6], density
functional theory (DFT) [7–10], molecular dynamics (MD) [11–
14], and kinetic Monte-Carlo (KMC) calculations [15]. However,
the formation of the tungsten fuzzy nanostructure has not been
yet reproduced by atomic scale simulation.
In the present paper, first, we propose a four-step process to
explain the formation mechanisms of the tungsten fuzzy nano-
structure. The formation process is classified into the penetration
step, the diffusion and agglomeration step, the helium bubble
growth step, and the fuzzy nanostructure formation step. The phe-
nomena brought about by tungsten and helium atoms for the
first to third steps are analyzed by using BCA, DFT, and MD
simulation.

http://dx.doi.org/10.1016/j.jnucmat.2015.01.018
0022-3115/Ó 2015 Elsevier B.V. All rights reserved.
110 A.M. Ito et al. / Journal of Nuclear Materials 463 (2015) 109–115
Next, we developed a new hybrid simulation approach to repro-
duce the formation of tungsten fuzzy nanostructure formation. The
existing atomic scale simulation methods hardly represent the for-
mation of tungsten fuzzy nanostructure. Our hybrid simulation
which combines MD and MC simulations enables us to treat simul-
taneously two phenomena having different time scales.
2. Four-step process
The formation process of the tungsten fuzzy nanostructure is
composed of multi-scale and multi physical processes. Fig. 1 shows
major phenomena caused by irradiated helium atoms and tungsten
material. To understand the formation mechanism of the tungsten
fuzzy nanostructure, we propose a four-step process for the forma-
tion of the tungsten fuzzy nanostructure. We will introduce the
simulation analysis for the four-step process by using several sim-
ulation methods.
The first step is the penetration process. In this step, the mech-
anism of the penetration of irradiated helium ion into tungsten
surface is elucidated. In particular, the competition between the
penetration of helium atoms and the sputtering of tungsten sur-
faces should be considered. To clarify the penetration process, we
evaluated incident energy range for penetration. Helium is com-
pared with neon and argon, and hydrogen.
The upper limit of the incident energy range for penetration is
defined as the highest incident energy not to cause the sputtering
of tungsten surfaces. Namely, the upper limit is sputtering thresh-
old energy. The sputtering threshold energy can be calculated by
BCA. The sputtering threshold energies for helium, neon, argon,
and hydrogen atoms calculated by using AC8T code are 100 eV,
30 eV, 20 eV, and 700 eV, respectively (see Table 1) [6].
When the kinetic energy of the incident atom is almost same as
the potential barrier energy of the surface, the incident atom can
move from vacuum region to the interstices of the tungsten mate-
rial without creating defects. Therefore, the lower limit of the inci-
dent energy range for penetration is estimated as the potential
barrier energy of the surface. Here, we substitute the solution
energy, which is the energy difference between the state in which
the helium atom is in the vacuum region and the state in which the
helium atom is located at the interstitial tetra site in the tungsten
material, for the potential barrier energy of the surface. The
interstitial tetra site is the most stable site in the interstices in
Fig. 1. Major phenomena in the tungsten material irradiated by helium plasma.
Table 1
The solution energy Esol , the sputtering threshold energy Esp , the penetration mean
depth with the injection at the sputtering threshold energy Dsp , and the migration
barrier energy in tungsten material Emig for helium, neon, argon, and hydrogen atoms.
Element Esol (eV) Esp (eV) Dsp (Å) Emig (eV)
Helium 6.29 100 100 0.06
Neon 11.55 30 6 0.17
Argon 14.99 20 4 0.19
Hydrogen 2.47 700 1000 0.20
the tungsten material. The solution energy can be calculated with
accuracy based on DFT. The solution energies for helium, neon,
argon, and hydrogen atoms calculated by QMAS code [16] are
6.29 eV, 11.55 eV, 14.99 eV, and 2.47 eV, respectively (see Table 1)
[17]. Note that the solution energy of hydrogen atoms is negative
because it is calculated as that in the case of single atom in vac-
uum, for example, not a molecule.
The lower limit of incident energy range for penetration had
been measured by experiments [18,19] as about 6 eV. This good
agreement between the theoretical and experimental values con-
firms the validity of our calculation model.
From these estimations, it is understood that the incident
energy ranges for neon and argon are much narrower than the inci-
dent energy ranges for helium and hydrogen. Although we had
tried to generate the tungsten fuzzy nanostructure by exposure
to neon and argon plasma with low energy in the NAGDIS-II, bub-
ble and fuzzy nanostructures were not generated [20]. In this
experiment, it was necessary to keep a fairly low incident energy
to suppress the sputtering of tungsten surface. The incident energy
range for neon and argon in the experiment is comparable with
that from the present theoretical estimation.
The reason why the bubble nanostructure was not generated in
the experiment of neon and argon plasma irradiation is thought to
be that the total retained amount of neon and argon is smaller than
that of helium. To clarify this point, the penetration depths of irra-
diated atoms are considered. The penetration depths at the upper
limits of incident energies are calculated by AC8T code as 100 Å,
6 Å, 4 Å, and 1000 Å, respectively (see Table 1) [6]. From the calcu-
lation values, neon and argon penetrate into only the mono-layer
of body centered cubic lattice structure of tungsten material. This
fact expects that penetrated neon and argon promptly escape from
the tungsten surface. Hence, sufficient amounts of neon and argon
to generate bubble nanostructure are retained.
On the other hand, although a hydrogen atom has wider inci-
dent energy range for penetration and can penetrate into a deeper
site, a hydrogen atom hardly generates a bubble nanostructure.
The region is explained in the following second step.
The second step is the diffusion and agglomeration process of
helium atoms in tungsten material. In this step, also, helium is
compared with neon, argon, and hydrogen.
First, the mechanism of helium agglomeration is considered.
The agglomeration in the atomic scale is discussed as energetics
with the calculation based on DFT. Here, we employed OpenMX
code [21] in addition to QMAS code.
It was simply considered that the agglomeration of helium
occurs in a vacancy of the tungsten material. The binding energy
of n helium atoms at mono-vacancy Evac n were calculated. If the
binding energy is positive, the helium prefer clustering state to sin-
gle state, while if the binding energy is negative, the helium prefer
being isolated to clustering. In the previous work, the mono-
vacancy can trap at least nine He atoms [10].
The calculation results of the binding energies of helium, neon,
argon, and hydrogen at mono-vacancy are shown in Fig. 2. The
binding energy of helium at mono-vacancy is always positive at
least for n 6 15. Similarly, binding energies of neon and argon at
 A.M. Ito et al. / Journal of Nuclear Materials 463 (2015) 109–115 111

10 higher energy irradiation of neon and argon in keV scale created

9 He bubble nanostructure in experiments [26]. There is a possibility
H that the fuzzy nanostructures are generated by exposure to neon
8 Ne
binding energy [eV]

7 Ar and argon plasmas if sufficient retention amounts of the neon

6 and the argon are supplied.
5 On the other hand, for hydrogen, the incident energy range is
4 wide enough and the penetration depth is also deep enough. The
3 DFT indicated that both the binding energy of hydrogen atoms at
2 a vacancy and the binding energy of hydrogen atoms at an intersti-
1 tial site become negative. That is, at the low concentration of
0 hydrogen atoms, hydrogen bubbles are hardly created because
-1 the hydrogen atoms prefer being isolated in the tungsten material.
0 2 4 6 8 10 12 14 16
However, at high concentration of hydrogen atoms, hydrogen blis-
The number of trapped atoms
ters are generated because the hydrogen atoms oversaturated by
Fig. 2. The binding energies for helium, neon, argon, and hydrogen atom at a mono- plasma irradiation cannot be isolated in tungsten lattices. Thus, it
vacancy. is expected that the bursting of the helium bubble and the blister-
ing of the hydrogen bubble are caused by the different mecha-
nisms. The difference of the agglomeration of the helium and the
mono-vacancy are always positive, also. This result suggests that hydrogen had been well investigated by using not only the DFT,
the agglomeration of helium, neon, and argon are unlimited. but also MD and KMC [15].
On the other hand, the binding energy for the hydrogen atom at The third step is the helium bubble growth process. In this step,
mono-vacancy are about 1.0 eV up to n 6 6, and it becomes almost the helium bubble growth of 1 nm or greater in diameter is simu-
0.0 eV or negative for n P 7. This calculation result for hydrogen lated. Since the space and time scale of helium bubble growth is
agrees with previous researches by Kato et al. [22] and Ohsawa too large to calculate by DFT, the helium bubble growth should
et al. [23]. Consequently, this result suggests the agglomeration be calculated by using MD or MC. Here, we employed MD with
of the hydrogen atom is limited. the potential model for tungsten and helium system developed
Further, the DFT disclosed that helium, neon, and argon can by using the downfolding method [27], which can optimize poten-
agglomerate also at interstitial sites in tungsten material tial function by comparison with structure and energy data calcu-
[7,8,17,24]. From the DFT, the binding energy at an interstitial site lated by DFT. The temperature of the system was controlled by the
increases from 1.0 eV to 2.0 eV as the number of helium atoms Nosé–Poincaré thermostat method [28,29]. The tungsten material
clustering at interstitial site increases [24]. of BCC lattice structure with/without vacancies of 1.0 percent
The reason why the noble gas atoms can agglomerate at an was prepared, and helium atoms of 5.0 percent are doped at ran-
interstitial site is the decrease of electronic charge density around dom, initially.
noble gas cluster at an interstitial site [17]. If the noble gas atoms The MD results after 1.0 ns are shown in Fig. 3. The helium bub-
form a cluster at an interstitial site, the tungsten atoms around the bles of 1 nm or greater in diameter were created in the both cases
cluster are pushed out. By the expansion of tungsten, the electronic with/without initial vacancies. In this simulation, we confirmed
charge density in the region around the cluster becomes lower both helium agglomerations at vacancies and helium agglomera-
than that in the case of pure tungsten body-centered cubic (BCC) tion at interstices.
material. Because the noble gas atoms are closed-shell atom, they In this simulation condition, the size of helium bubbles in the
receive repulsion from the electronic charge in tungsten material. case without vacancies was greater than that in the case with
Therefore, the region around the cluster, in which electronic charge vacancies. To explain this difference, the diffusion of helium cluster
density is lower, is regarded as a more stable site for the next noble is considered. The migration barrier energy for helium atom to
gas atom. Thus, noble gas atoms continue to agglomerate at an escape from a mono-vacancy is equal to the biding energy of
interstitial site, also. helium at mono-vacancy, that is, 2.5 eV or greater in Fig. 2. The
Next, the diffusion of the helium, neon, argon, and hydrogen are migration barrier energy of the mono-vacancy in the tungsten
discussed. The speed of diffusion relates to the time scale of helium material is evaluated as 1.8 eV [30]. The migration barrier energy
bubble generation. The elementary diffusion processes of these for a helium cluster along with the mono-vacancy is 3.07 eV or
atoms are, in atomic scale, regarded as the migration from the greater, which depends on the size of the helium cluster. From
tetra-site to the next tetra-site via the tri-site. Neon, argon, and the comparison of these migration barrier energies, the helium
hydrogen have the same diffusion process. The migration barrier atoms trapped by the vacancy hardly diffuse. On the other hand,
energy for the diffusion process can be calculated by the DFT the migration barrier energies of helium dimer and trimer at an
[17] (shown in Table 1). As a result, the migration barrier energy interstitial site are lower than that of a single helium atom at an
of helium is one-third of that of hydrogen. The migration barrier interstitial sites [25]. Thus, the helium clusters at an interstitial site
energies of neon and argon were similar to that of hydrogen, can continue to diffuse. We suggest that the diffusion of helium
though they have a larger atomic radius. From these facts, we sug- clusters promotes the helium bubble growth.
gest that helium diffuses faster than hydrogen in tungsten The present comparison between the cases with/without
material. vacancy is one example. The ratio of the number of helium atoms
More interestingly, a recent work by the DFT revealed that the to that of vacancies is much smaller than the experimental condi-
migration energy of helium dimer, which is clustering at an inter- tion to create the tungsten fuzzy nanostructure. However, we com-
stitial site, is lower than that of the single helium atom [25]. ment that the growth process of the helium bubble in the case of
Let us discuss again why only helium could generate the bubble low energy irradiation of 100 eV or less differs from the case of
nanostructure in the previous experiments [20]. By the incident high energy irradiation of 1 keV or more, in which the vacancies
energy range in the first step, we suggest that sufficient amounts are created with helium penetration.
of neon and argon are not retained in the material. The DFT indi- In addition, the phenomenon called loop-punching can be
cated that neon and argon has the possibility of agglomeration observed in the MD with our potential model and similar system.
and the sufficient speed of diffusion similar to helium. Actually, The MD observation of the loop-punching has been reported by
112 A.M. Ito et al. / Journal of Nuclear Materials 463 (2015) 109–115
Fig. 3. The helium bubble growth calculated by the MD simulation in the case with mono-vacancies (a) and the case without vacancy (b). The blue spheres indicate helium
atoms, and the yellow and red spheres indicate the tungsten atoms whose coordination number is greater than 9 and smaller than 5, respectively. (For interpretation of the
references to color in this figure legend, the reader is referred to the web version of this article.)
Henriksson et al. [11] and Sefta et al. [13]. The point of our MD
observation is that the loop-punching is clearly confirmed as the
phenomenon that the strain of tungsten atoms around the helium
bubble is released as a dislocation loop [31].
Thus, the first to third steps have been explained by using BCA,
DFT and MD. The fourth step, in the next section, the fuzzy nano-
structure formation is reproduced by a new simulation approach.
3. Fuzzy nanostructure formation
3.1. MD–MC hybrid simulation
From the previous works, to reproduce the fuzzy nanostructure
formation is difficult if we adopt either MD or MC simulation. In
the present work, we develop the hybrid simulation between MD
and MC, which we call MD–MC hybrid simulation.
In the MD–MC hybrid simulation, the diffusion and injection of
helium are represented by MC. The deformation of tungsten mate-
rial by the strain from the helium bubble is represented by MD.
These MC and MD are repeated alternately as a hybrid simulation.
In this paper, the process of one MC phase and one MD phase is
defined as one cycle. In the MD phase, a material is composed of
atomic particles, while in the MC phase, the material is regarded
as cell data and the diffusion of helium atoms is represented by
random walk on the cells.
First, the detail of the MC phase is described. As a preprocess of
the MC phase, the information of atomic positions in the initial
state and the MD phase at the previous cycle is converted into cell
data. The simulation box is divided into small cells. Each cell has
only the flags whether the cell includes tungsten and helium atoms
in its region.
After creating cell data, the helium atom is injected into the sur-
face. The injection position coordinates in x and y directions are
determined at random. The penetration depth Din is the parameter
of this simulation. The cell placed at Din in z direction from the sur-
face of tungsten material, which depends on the injection position
and the structure varying with time development, is set to the ini-
tial cell for the following random walk of helium.
The random walk of helium is simply to repeat the movement
into the adjacent six cells. The direction of movement is deter-
mined at random. One movement is regarded as one step of the
random walk in the MC phase. If the helium moves on the cells
including tungsten atoms only, the random walk continues. The
terminating conditions of the random walk are as follows: the step
of the random walk reaches the simulation step of the MC phase
sMC , the helium comes to a cell including at least one helium atom,
the helium comes to a cell including no atom, and the helium pass
through the bottom boundary of simulation box. If the random
walk is stopped by the former two conditions, a helium atom is
doped into the last cell.
For the way to inject a helium atom, the three-dimensional
position coordinates of the helium atom are randomly determined
in the region within the last cell. After that, the four nearest neigh-
bor atoms from the doped helium atom are searched. The injected
position of the helium is set to the center of the four nearest neigh-
bor atoms. If the four nearest neighbor atoms are tungsten atoms
keeping the BCC lattice structure, the actual doped position
is tetra-site, which is the most stable position for the helium
atom.
In the MC phase, the above routine is performed N dope times
while varying the injection positions in the x and y directions. All
helium atoms are moved during the sMC steps. The doped helium
atoms in the MC phase are taken over into the initial atomic struc-
ture in the next MD phase.
In the present MD–MC hybrid simulation, the random walk of
each helium atom is performed just once in the MC phase when
the helium atom is injected. Namely, the injected helium atom
does not move in the next MC phase.
Next, the simulation condition in the MD phase is described.
The size of the simulation box is the same to the previous MC
phase. The initial atomic configuration in the current MD phase
consists of the final atomic configuration of the previous MD
phase and the helium atoms doped by the previous MC phase.
All MD phases are calculated during the sMD step. The interaction
among tungsten and helium atoms are represented in the poten-
tial model developed by using downfolding methods [27]. The
temperature of tungsten material is controlled by the Nosé–Poin-
caré thermostat [28,29]. The tungsten atoms in the bottom region
of one BCC mono-layer are fixed during the MD phase. The sim-
ulation system follows the periodic boundary condition in the x
and y direction. When atoms pass through z boundary of the sim-
ulation box, they are vanished from the simulation system. The
difference from the general MD simulations for PWI problems is
only that the injections of helium atoms are not performed in
the MD phase.
After the MD phase, the atomic configuration is converted into
the cell data for the next MC step. The time evolution of the system
is represented by repeating the above MC–MD cycle.
 A.M. Ito et al. / Journal of Nuclear Materials 463 (2015) 109–115 113

Here, the relation of physical variables in the present MD–MC
hybrid simulation is described. In the MC phase, the number of
doped helium atoms N dope is given by
Ndope ¼ /MC SsMC DtMC
where /MC is the flux of helium in the MC phase and S is the square
measure of the surface of tungsten material. The time step in the
MC phase Dt MC is derived from the diffusion coefficient D as
2 simulation box, S ¼ 3629 Å2. The size
of
a 4.32  7.85  4.31 Å3, and then
Dt MC ¼
2dD
where d is the dimension of the system, a2 is the mean square of
the sides of cell in the MC phase.
On the other hand, using the variables in the MD phase, N dope is
also given by
Ndope ¼ /MD SsMD Dt MD
where /MD is the flux of helium in the MD phase, sMD is the calcu-
lation steps in the MD phase, and Dt MD is the time step in MD phase.
From Eqs. (1) and (3), the following relation between the phys-
ical variables in the MC and MD phases can be obtained;
sion space, the size of the simulation box in the y direction was
set to thin value to save computational resources. Therefore, the
present MD–MC hybrid simulation should be called a pseudo
three-dimensional simulation.
ð1Þ
The parameters in the MD–MC hybrid simulation is set as fol-
lows: the setting temperature T set ¼ 2000 K, the mass of thermo-
stat Q ¼ N, where N is the total number of atoms except for the
fixed tungsten atoms in the bottom region. From the size of the
 cell in the MC phase is
a2 ¼ 32:95 Å2. Din ¼ 10 Å,
ð2Þ
/MC ¼1:41022 m2 s1 ;D¼1:321011 m2 s1 ; Dt MD ¼1:01016 s,
/MD ¼1:221030 m2 s1 ;sMC ¼2:0104 steps, sMD ¼1:0104 steps,
N dope ¼44:17. The total number of MD–MC cycles was 4:3103 .
3.2. Results
ð3Þ
Time evolution in the MD–MC hybrid simulation is shown in
Fig. 4.
The observed formation process of the fuzzy nanostructure is as
follows: Helium atoms formed helium bubbles. As the fluence of
helium increases, the sizes of the helium bubbles increase. The

2 helium bubbles near the tungsten surface pushed up the tungsten

a /MC
sMC ¼ /MD DtMD sMD
2dD
This relation means that the calculation steps in the MC and MD
phases are not independent, where the fluxes for the MC and MD
phase can be set as different values in this hybrid
 simulation. The
physical variables in this relation, d; S, and a2 , are determined
from the size of the simulation box. The time step in the MD phase
DtMD is determined as the adequate small value at which the atoms
can move smoothly on potential energy surface. The flux for the MC
phase /MC is set to the same value as the experimental value. The
diffusion coefficient of helium atom D is set to the measured value
from experiments or the estimated values from the theory and sim-
ulation. Hence, the control parameters in the MD–MC hybrid simu-
lation are two of sMC ; sMD , and /MD , where one of them is
automatically determined by the relation in Eq. (4).
The MD–MC hybrid simulation cannot evaluate elapsed time
because the MC and MD phase have different time scales. Here,
we should use the fluence of helium instead of elapsed time.
The simulation box has the size of 462.3  7.85  1538.6 Å3.
The initial sizes of the tungsten material in the x and y directions
are equal to the sizes of the simulation box, the initial size of the
tungsten material in the z direction is 307.1 Å, which is shorter
than the size of the simulation box in the z direction. The tungsten
material is put to the bottom in the simulation box. The h1 1 1i
surface of tungsten faces the vacuum region. In this work, though
the MD–MC hybrid simulation was calculated as a three-dimen-
atoms located above them. The pushing from the helium bubbles
ð4Þ
generates the arch structure of a tungsten surface. When the
helium bubble bursts, the break point of the arch structure is a sup-
porting point of the arch, and is not an arch crown part. The arch
structure is turned up by the helium atoms during the bursting.
Thus, the bursting creates concavity and convexity of the tung-
sten surface. Here, the next helium bubbles tend to be generated in
the region of concavity rather than convexity. Therefore, the region
of the concavity is dug through by the bursting of the helium bub-
bles. The region of convexity incorporates the tungsten arch turned
up by the bursting in the region of concavity, and then it is rein-
forced. By this process, the deformation to the concavity and con-
vexity is enhanced. We consider that the present formation process
is regarded as the early formation process of the tungsten fuzzy
nanostructure.
3.3. Discussions
Here, let us discuss the time scale of the fuzzy nanostructure
formation in the MD–MC hybrid simulation. Instead of the elapsed
time, the fluence of helium is compared with experiments. In
experiments, generally, the fluence of helium of 1024 –1025 m2 is
necessary for the generation of the tungsten fuzzy nanostructure
[32]. However, the fluence of the present MD–MC hybrid simula-
tion is only up to 4:8  1021 m2. There are thousand of gaps in
the fluence of helium.

Fig. 4. The tungsten fuzzy nanostructure formation calculated by the MD–MC hybrid simulation. The purple and blue spheres indicate tungsten and helium atoms,
respectively. (For interpretation of the references to color in this figure legend, the reader is referred to the web version of this article.)
114 A.M. Ito et al. / Journal of Nuclear Materials 463 (2015) 109–115
We consider that the gap of fluence is explained by the two
problems which are not treated in the MD–MC hybrid simulation.
One is the reflection effect of the irradiated helium by the surface.
In the present MD–MC hybrid simulation helium atoms are com-
pletely penetrated from the surface. In reality, the injected helium
atoms are reflected on the surface. For example, the reflection ratio
of the helium atoms on the flat surface calculated by the BCA is
about 20 percent. Of course, the simulation of the low energy inci-
dence by the BCA has low reliability. Furthermore the reflection
and penetration process strongly depend on the difference of the
surface structure. We should simulate the helium injection on
the bubbly and fuzzy surfaces. Although the difficulty of this sim-
ulation is how to prepare a realistic fuzzy surface structure, we will
be able to obtain the realistic fuzzy surface structure from the
result of the full three-dimensional MD–MC hybrid simulation in
the near future.
The second problem of the present MD–MC hybrid simulation,
which has the gap of fluence, is the difference of the retention ratio.
In the present MD–MC hybrid simulation, almost injected helium
atoms were retained until the bursting occurs. The reason why
the almost helium atoms were retained is that the diffusion coeffi-
cient is set to D ¼ 1:32  1011 m2 s1. However, the retention ratio
of helium atoms evaluated by the KMC simulation with the diffu-
sion coefficient of 108 m2 s1, whose code is developed in our
group, is 2.0 percent or less. The retention ratio evaluated by
KMC is in good agreement with the experimental retention ratio
of 2.0 percent measured by Lee et al. [33] The important physical
parameter in the MD–MC hybrid simulation is the ratio of the flux
and the diffusion coefficient /MC =D. However, there is a large gap in
the diffusion coefficient of helium in tungsten materials between
simulation and experiment. The diffusion coefficient of helium cal-
culated by the MD at 1400 K is on the order of 108 m2 s1 [34],
while the experimental diffusion coefficient of helium at 1400 K
is on the order of 1015 m2 s1 [32]. It is expected that the diffu-
sion coefficient of the helium in the tungsten material is influenced
by the self trapping and vacancy trapping. To resolve the gap of the
diffusion coefficient of helium, both simulation and experiment
should continue the work.
Strictly speaking, the present MD–MC hybrid simulation has
problems in completely reproducing the formation of the tungsten
fuzzy nanostructure. We here described the problems and future
works. The structure generated in the MD–MC hybrid simulation
should be compared with experiments. In particular, the problem
is whether this is the same structure or not. We consider that
the comparison by using surface fractal dimension is adequate.
Temperature dependence for the formation of bubble and fuzzy
nanostructures was observed by experiment [2]. This point should
be clarified by the simulation.
Above all, one problem of the present simulation is that the
pseudo three-dimensional system was employed. Our simulation
code GLIPS is ready to calculate full three-dimensional cases,
where much larger calculation resources will be consumed. We
will perform full three-dimensional simulation in the near future.
4. Conclusion
In the present paper, the formation process of the tungsten
fuzzy nanostructure was represented by the four-step process.
The simulation method should be selected step by step. In the first
step of helium penetration, the incident energy range for penetra-
tion was evaluated by the BCA and the DFT. In the second step of
diffusion and agglomeration of helium, the DFT showed that
helium agglomeration is unlimited, agglomeration at interstitial
site is possible, and the diffusion of helium is faster than hydrogen.
In the third step of helium bubble growth, the MD showed that the
helium agglomerations at both the vacancy and the interstices in
the tungsten material are effective for the helium bubble growth.
As the fourth step, fuzzy nanostructure formation was repre-
sented by developing the MD–MC hybrid simulation. By the MD–
MC hybrid simulation, the phenomena in the different time scales
were combined. The injection and diffusion of helium are repre-
sented by the MC simulation phase and the deformation of tung-
sten material was represented by the MD simulation phase.
The following formation mechanisms were observed by the
present MD–MC hybrid simulation. The tungsten arch structure
over the helium bubble is turned up by the bursting of the helium
bubbles. Concavity and convexity are enhanced because the burst-
ing of the next helium bubbles easily occurs in the region of the
concavity. We suggest that this process is regarded as the early for-
mation process of the tungsten fuzzy nanostructure.
Finally, we remark that the present MD–MC hybrid simulation
is in the pseudo three-dimensional system. In the near future, after
solving any problems of model and parameter settings, the tung-
sten fuzzy nanostructure will be completely reproduced by the full
three-dimensional MD–MC hybrid simulation.
Acknowledgements
We would like thank to Dr. Naoaki Yoshida, Dr. Yoshio Ueda, Dr.
Masayuki Tokitani and Dr. Heun Tae Lee for helpful discussions.
Our work was supported by the National Institute of Natural Sci-
ence (NINS) Program for Cross-Disciplinary Study, Grants-in-Aid
for Scientific Research (Nos. 23710135 and 25249132) from the
Ministry of Education, Culture, Sports, Science, and Technology,
Japan, and the National Institute for Fusion Science (NIFS) Collabo-
ration Research programs (NIFS14KNTS028 and NIFS13KNSS037).
Numerical simulations were carried out by using the Plasma Sim-
ulator at the NIFS and the HELIOS supercomputer system at Com-
putational Simulation Centre of International Fusion Energy
Research Centre (IFERC-CSC), Aomori, Japan, under the Broader
Approach collaboration between Euratom and Japan, implemented
by Fusion for Energy and JAEA.
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