氷結晶成長実験（Ice Crystal 2）供試体開発と実験運用 Development

27B06
氷結晶成長実験（Ice Crystal 2）供試体開発と実験運用
○田丸晴香，吉崎泉（JAXA），島岡太郎（JSF），曽根武彦（JAMSS），古川義純，中坪俊一（ILTS），
真木孝雄，赤羽隆之（オリンパス株式会社），友部俊之（株式会社 IHI エアロスペース）
Development and Operation of the Ice Crystal 2 Experiment in ISS-KIBO
Haruka TAMARU, Izumi YOSHIZAKI (JAXA), Taro SHIMAOKA (JSF), Takehiko SONE (JAMSS),
Yoshinori FURUKAWA, Shunichi NAKATSUBO (ILTS), Takao MAKI,
Takayuki AKAHANE (Olympus Corporation), Toshiyuki TOMOBE (IHI AEROSPACE Co., Ltd.)
1. Introduction
JAXA selected the scientific experiment titled “Crystal
growth mechanisms associated with the macromolecules
adsorbed at a growing interface –Microgravity effect for selfoscillatory growth– (Ice Crystal 2)” in February 2008. The
purpose of this experiment is to shed light on the self-oscillation
mechanism of growth phenomena in supercooled water with
antifreeze glyco protein (AFGP).
In order to clarify this mechanism, we developed the
experiment facility called “Ice Cell 2”. It was launched by
HTV4 in August 2013, and attached on the Solution Crystal
Observation Facility (SCOF) located in the Japanese
Experiment Module “KIBO”. Fig. 1 and 2 show the external
and internal appearance of Ice Cell 2. This paper describes the
specifications of Ice Cell 2 and introduces its operational status.
Nucleation Cell and Growth Cell. Both cells are filled with
sample solution and temperature is controlled by Peltier devices.
In this experiment, at first, a crystal nucleus is created by
rapidly cooling the Nucleation Cell. After that, through the glass
capillary, the crystal nucleus grows into the Growth Cell, which
is set at the predetermined degrees of supercooling. Then, its
crystal surface and growth rate are observed and measured with
Optical systems.
In order to satisfy these specifications, we improved the
cooling performance and optimally designed the optical path.
Table 1 shows the specifications of Ice Cell 2.
Table 1
Specifications of Ice Cell 2
Items
Size
Sample
Growth
Cell
H2O + AFGP
Internal Shape
Spherical
Temperature
Control
-3~25 deg. C
Position Control
Internal Shape
Nucleation
Cell
Fig. 1
External appearance of Ice Cell 2
Observation
Unit
Specifications
250 x 250 x 215 mm
Translation drive
Capillary
Temperature
Control
-20~25 deg. C
Position Control
Rotary drive
Mc Interference microscope
Inside Ice Cell 2
Phase contrast microscope
Azimuth observation camera
3. Operation on Orbit
Fig. 2
Internal structure of Ice Cell 2
2. Specifications
Ice Cell 2 is roughly divided into the Observation Unit and
Specimen Cell Unit. Specimen Cell Unit is composed of
Ice Crystal 2 experiment is carried out at night in the ISS with
less disturbance from astronauts. The timing of nucleation and
growth rate are different for each temperature condition.
Therefore, it is necessary to quickly send commands from the
ground for the operation of the observation systems.
In late August, this experiment was started, but there is a
problem on the Nucleation Cell temperature control. Currently
JAXA is troubleshooting on ground and on orbit. It is expected
that Ice Crystal 2 experiment will be resumed in near future.
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27B07
ISS－KIBO で実施されている Ice Crysatal 2 実験の概要
○古川義純，佐崎元，長嶋剣，麻川明俊，Dmitry Vorontsov，中坪俊一（ILTS），
吉崎泉，田丸晴香（JAXA），島岡太郎（JSF），曽根武彦（JAMSS）
Outline of Ice Crystal 2 experiments on ISS-KIBO
Yoshinori FUUKAWA, Gen SAZAKI, Ken NAGASHIMA, Harutoshi ASAKAWA Dmitry VORONTSOV,
Shunichi NAKATSUBO (Hokkaido Univ,), Izumi YOSHIZAKI, Haruka TAMARU (JAXA),
Taro SHIMAOKA (JSF), Takehiko SONE (JAMSS)
1. Introduction
Ice crystal growth in the supercooled water is an important
subject relating to the crystal growth and pattern formation
mechanisms. The first experiment for ice crystal growth was
carried out on ISS-KIBO in the period from December 2008 to
March 2009 and we successfully obtained an excellent dataset
for ice crystal growth in the pure D2O water. Ice Crystal 2
experiment was planned to observe the ice crystal growth in the
supercooled aqueous solution of antifreeze glycoprotein
(AFGP). Laboratory experiments show that the ice crystal
growth is strongly modified by the effect of AFGP molecules
(1,2). .Especially, the growth patterns are drastically modified to
hexagonal plate, faceted dendrite or needle crystal, depending
on the AFGP concentration and the supercooling temperature.
Growth rates of basal and prism planes are also changed as the
function of AFGP concentration.
composed of the growth cell and the Michelson-type
interferometer combined with the phase contrast microscope.
Using this apparatus we can observe the pattern formation
process of ice single crystal and precisely measure the growth
rates of two basal planes and the growth rate of dendrite tip
separately as a function of growth time.
Fig. 2 shows the 3D illustration of growth cell, which is
composed of a spherical growth chamber (40mm in diameter)
and a glass capillary. The capillary can be rotated around its
axis to adjust the direction of ice crystal for the optical axis.
Capillary
Spherical
growth chamber
Fig.2 Cross-sectional illustration of ice growth chamber
AFGP solution
3. Present status of ISS-KIBO experiments
Fig. 1 An ice crystal grown in the supercooled solution of
AFGP. Faceted dendrite and the step migration are observed.
These modifications can occur by the adsorption of AFGP on
the interfaces between ice and water. Namely, the drastic
change for the ice crystal growth occurs by the modification of
growth kinetics by the adsorbed AFGP molecules.
The purpose of Ice Crystal 2 experiments is to clarify the ice
crystal growth mechanism affected by the AFGP molecules and
to detect the self oscillation of growth velocities. Final goal of
this experiment is to clarify the growth mechanism controlled by
the additives such as the biological macromolecules.
The ice crystal 2 cell was launched by JAXA HTV-4 in
August 2013 from Tanegashima Space Center. The experiment
was started from 26 August 2013. A trouble, however,
occurred shortly after the beginning of experiments.
Consequently, the experiments are the experiment is on hiatus at
the present time (26 September 2013). But we would like to
give a presentation to introduce the concept of our space
experiment.
References
1)
2)
2. Apparatus
A new apparatus was developed for this experiment. It is
− 29 −
Furukawa, Y., N. Inohara and E. Yokoyama, J. Cryst.
Growth, 275, (2005)167-174.
Zepeda, S., E. Yokoyama, Y. Uda, C. Katagiri and Y.
Furukawa, Cryst. Growth Des., 8, (2008)3666-3672.
27B08
ISS きぼう船内実験室利用テーマ「Soret-Facet」
○鈴木進補，森雄飛，橋本栄尭（早稲田大学），稲富裕光（JAXA），正木匡彦（芝浦工業大学），
渡邉匡人，水野章敏（学習院大学），上野一郎（東京理科大学），山根岳志（富山大学），
伊丹俊夫（北海道大学），勝田真登（JAXA）
Experiments Aboard the ISS-JEM “Soret-Facet”
○S.Suzuki, Y.MORI, Y.HASHIMOTO (Waseda Univ.), Y.INATOMI (JAXA), T.MASAKI (Shibaura Inst. Tech.),
M.WATANABE, A.MIZUNO (Gakushuin Univ.), I.UENO (Tokyo Univ. Sci.), T.YAMANE (Toyama Univ.),
T.ITAMI (Hokkaido Univ.), M.KATSUTA (JAXA)
1. Introduction
When a temperature gradient is given in a binary liquid of AB, component A moves to the lower temperature side and B
moves vice versa (Fig.1(a)). On the other hand, mass transport
is induced to opposite side by concentration gradient. The mass
transports in the both ways balances at the stationary state. This
phenomenon of mass transport caused by temperature gradient
is called Soret effect. The knowledge of Soret effect in liquid is
necessary to solve scientific and industrial problems, such as,
crystal growth, geophysics, and so on. The parameter to
describe the stationary state of the mass transports is Soret
coefficient ST as following equation.
(1)
1
C
ST  
two lasers of wavelengths of 532 and 780 nm.
A temperature gradient is set by heating the ends of the cell
(Fig.1(b)). The average temperature of the melt is ranging from
25 to 55°C including the supercooled liquid region. Then the
interference fringes should shift because of refractive index
change. We can calculate the temperature and concentration
distribution by measuring the moving distance of fringes.
C0 ( 1 - C0 ) T
Here, C0 and C/T are the average concentration and the ratio
between the concentration and temperature gradients at the
stationary state, respectively.
Although thermodynamic approach is necessary to clarify the
mechanism of Soret effect, there are not enough data to discuss
it because of the difficulty of measurements. Convective flow
must be eliminated, and the temperature and concentration
distribution must be measured accurately. Although
measurements of ST were carried out under g conditions , the
1)
conventional measurements were conducted by interferometer
with one wavelength, with which only the concentration
distribution can be measured.
This research group is preparing for measurements of ST in
melt under convection-free conditions in Kibo/ ISS to elucidate
the mechanism of Soret effect. The temperature and
concentration distributions are measured individually by a twowavelength interferometer to improve the accuracy. We
introduce the plan of the experiments “Soret-Facet” in JEM
(Kibo) and analysis of the results in this presentation.
Fig.1 Mass transport induced by temperature and concentration
gradient (a) and temperature program (b)
3. Mechanism of Soret Effect
The relationship between –CT and C0/T2 is obtained from
the measurements. If the relationship is linear, the validity of
Onsager reciprocal relation can be verified.
A linear relationship between the concentration gradient and
the temperature gradient at each average temperature of solution
is expected. The inclination of the relationship is proportional to
ST. The temperature dependence of ST is compared with that of
the Gibbs free energy of the solution by calorimeters and the
relationship between them is described. Furthermore, the
thermodynamic properties for mass transport in supercooled
liquid below the melting temperature is discussed.
References
2. Experimental
1)
The ssamples are salol tertial-butyl alcohol alloys melt (3 and
5 mol%) in FACET-cell cartridges, which were used in the
experiments FACET2) and already exist in Kibo. The solutions
in FACET-cell cartridges are set in Crystallization Observation
Facility (SCOF) having a Mach-Zehnder interferometer with
V. Shevtsova, T. Lyubimova, Z. Saghir, D. Melnikov, Y.
Gaponenko, V. Sechenyh, J.C. Legros and A. Mialdun: J. Phys.:
Conf. Ser. 327 (2011) 012031.
2)
− 30 −
Y. Inatomi, I. Yoshizaki, K. Sakata, T. Shimaoka, T. Sone, T.
Tomobe, S. Adachi, S. Yoda and Y. Yoshimura: Defect and
Diffusion Forum, 323-325 (2012), 533-537.
27B09
微小重力下における TLZ 法による均一組成 SiGe 結晶育成の研究（その１）
○木下恭一，荒井康智，稲富裕光（宇宙航空研究開発機構），塚田隆夫（東北大学大学院工学研究科），
宮田浩旭，田中涼太（（株）エイ・イー・エス）
Rapid Report of the Growth of Homogeneous SiGe Crystals by the TLZ Method in Microgravity
Kyoichi KINOSHITA, Yasutomo ARAI, Yuko INATOMI (Japan Aerospace Exploration Agency),
Takao TSUKADA (Dept. Chem. Eng. Tohoku Univ.), Hiroaki MIYATA, Ryota TANAKA (AES Co. Ltd.)
1. Introduction
The first microgravity experiment on SiGe crystal growth by
the traveling liquidus-zone (TLZ) method using a gradient
heating furnace (GHF) aboard the “Kibo” in the International
Space Station was performed in March, 2013. Objective of a
series of 4 experiments is to study the TLZ growth mechanism
by suppressing convection in a melt in microgravity. In the first
experiment, growth conditions for growing homogeneous
Si0.5Ge0.5 crystals were investigated.
2. Experiment
A 10 mm diameter Si1-xGex (x ~ 0.5) crystal was grown by the
TLZ methods. Orientation of the Si seed was <100>. The zone
former Ge was polycrystalline. After removing the surface
contamination and the oxide layer by etching in an acid solution,
a 30 mm long Si seed, a 20 mm long Ge zone forming material
and a 57 mm long Si feed were put into a boron nitride (BN)
crucible with a carbon spring for avoiding free melt surface. The
crucible was vacuum sealed in a quartz ampoule at about 1×
10 Pa. The ampoule wrapped by ZrO2 cloth was then inserted
into a metal cartridge. The assembled metal cartridges were
heated in the GHF. Growth conditions are as follows,
in the molten zone that plays a role of averaging the zone
temperature. The melt back length of the Si seed 0.4 mm is
much shorter than that of the terrestrial experiment 2 mm.
Figure 2 shows Ge concentration profiles along the center
axis (□), and right and left peripheral axes (△,◇) which are 4
mm away from the center line. It should be noted that Ge
concentration is almost constant for the whole of the crystal:
48.5±1.5 at%. One origin of the concentration deviation from
the expected Si0.5Ge0.5 is the growth rate increase due to
temperature gradient increase; The programmed heater
temperatures gradually deviate from the expected growth
temperatures. Another origin is temperature increase by the
cartridge surface emissivity change. Since composition is
directly related to the solidus temperature in the phase diagram,
the concentration variation can be compensated by temperature
change. In the second experiment, heater temperatures were
adjusted based on the concentration profile of the first
experiment. The second experiment was conducted in July and
the cartridge will be returned to the earth by Soyuz 35 in Nov,
2013.
Melt (quenched)
Feed
Seed
temperature gradient: 8℃/cm, heater translation rate 0.1 mm/h,
Grown crystal
freezing interface temperature: 1107 ℃ , experiment period:
10 mm
123.8 h. The microgravity level was almost 10-5G during
experiment, but the crew exercises generated about 10-3G in a
few tens of seconds.
The sample cartridge was returned by Space-X 2 vehicle in
March. No missing part, large voids and major cracks was
detected in a cross section of the grown crystal. No free surface
of the melt would be existed during the experiment. The
concentration profiles were measured for the whole of the
crystal by an EPMA. Two dimensional Ge concentration map is
shown in Fig. 1. From this figure growth length was observed to
be 17.2 mm although 15 mm crystal length was expected. The
difference in the growth length was considered that the
temperature gradient was different from that of the terrestrial
experiments. Based on the 1D TLZ model equation, temperature
gradient of 9oC/cm was suggested. This temperature gradient
increase would be caused by suppression of convective mixing
− 31 −
Ge concentration（at.%）
3. Results and discussion
Fig. 1
Freezing
Int.
Dissolving Int.
2D Ge concentration map.
100
90
80
70
60
Grown crystal
系列1
Peripheral
50
Melt
(quenched)
40
30
20
10
Seed
0
20
30
40
50
Length（mm）
Fig. 2
Axial Ge concentration profiles.
60
Center
系列2
Peripheral
系列3
27B10
ISS における Alloy Semiconductor プロジェクトの現状
○稲富裕光，阪田薫穂（JAXA），早川泰弘（静岡大学），石川毅彦（JAXA），Mukannan Arivanandhan，
Govindasamy Rajesh，小山忠信，百瀬与志美，田中昭（静岡大学），小澤哲夫静（岡理工科大学），
岡野泰則（大阪大学），高柳昌弘，上垣内茂樹（JAXA）
Current Status of Alloy Semiconductor Crystal Growth Project in ISS
○Yuko INATOMI, Kaoruho SAKATA (JAXA), Yasuhiro HAYAKAWA (Shizuoka Univ.), Takehiko ISHIKAWA
(JAXA), Mukannan ARIVANANDHAN, Govindasamy RAJESH, Tadanobu KOYAMA, Yoshimi MOMOSE,
Akira TANAKA (Shizuoka Univ.), Tetsuo OZAWA (Shizuoka Inst. Sci. Tech.), Yasunori OKANO (Osaka Univ.),
Masahiro TAKAYANAGI, Shigeki KAMIGAICHI (JAXA)
1. Introduction
High quality homogeneous ternary alloy semiconductor
crystals are required for the fabrication of optoelectronic devices,
since wavelength and lattice constant are controlled by adjusting
the composition of the constituents. However, it is very difficult
to grow high quality homogeneous single crystals due to the
following factors: 1) segregation phenomenon, 2) temperature
and concentration fluctuations caused by convection, and 3)
growth kinetics at the growth interface. Since the heat and mass
transport in the liquid phase are affected by buoyancy
convection, the dissolution and growth processes are strongly
influenced by gravity.
The purpose of “Alloy Semiconductor” crystal growth project
is to make clear the factors for crystal growth of a high-quality
bulk alloy semiconductor by investigating (1) solute transport in
liquid and (2) surface orientation dependence of growth kinetics
under microgravity and terrestrial conditions. If the
homogeneous and high-quality bulk crystal with desired
composition can be grown based on the results of the space
experiment, the knowledge to grow suitable thin layers on the
crystal will be achieved for fabrication of the optoelectronic
devices. The temperature gradient furnace Gradient Heating
Furnace (GHF) onboard “Kibo” is used for the growth of an
InxGa1-xSb bulk crystal, whose melting point is lower than
712°C. Since no in situ observation facility for semiconductor
crystal growth has been installed in ISS at this point, a thermalpulse technique is periodically applied to make impurity
striations in a grown crystal as time markers artificially. The
present paper describes the current status of the space
experiment project.
in order to make the contrast of the striations to be sharp. The
striations in the grown crystal were observed by chemical
etching as shown in Fig. 1. The composition of the grown
crystals was determined by means of Electron Probe MicroAnalysis (EPMA). Figure 2 shows the measurement result of
concentration distribution of In, Ga and Sb in the grown crystal
by EPMA. By measurement of the concentration gradient
around the striation, the local temperature gradient can be
calculated using the InSb-GaSb pseudo-binary phase diagram.
The first growth experiment of “Alloy Semiconductor” on
orbit was performed on June, 2013. The current status of the
space experiment project will be reported in the presentation.
6th pulse
5th pulse
4th pulse
3rd pulse
2nd pulse
GaSb seed
Interface
1 mm
Fig. 1 Impurity striations in grown crystal as time markers.
Narrow blue lines correspond to the striations.
2. Experimental
The InxGa1-xSb crystals were grown by the temperature
gradient method on earth with the same configuration as the
flight model. During the crystal growth, thermal pulses were
introduced to yield dopant striations in the grown crystal by
changing the heater temperature as a delta-function of time. The
growth rate can be obtained from the ratio of the striation
distance divided by the period of the thermal pulse. It is
necessary to adjust height and width of the temperature change
Fig. 2 Concentration distribution of In, Ga and Sb in grown
crystal.
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