UTTAC-78, 2009

UTTAC
ANNUAL REPORT 2008

TANDEM ACCELERATOR COMPLEX
Research Facility Center for Science and Technology
University of Tsukuba

http://www.tac.tsukuba.ac.jp/

UTTACANNUAL REPORT 2008
April 1, 2008 – March 31, 2009

UTTAC-78 2009

Executive Editor: Hiroshi Kudo
Editors: Yoshihiro Yamato, Daiichiro Sekiba, Kimikazu Sasa, Tetsuro Komatsubara

UTTAC is a series of issues, which include annual reports of
Tandem Accelerator Complex, Research Facility Center
for Science and Technology, University of Tsukuba.
The issues may also include irregular reports written by English.
Copyright © 2009 by Tandem Accelerator Complex, Research Facility Center
for Science and Technology, University of Tsukuba and individual contributors.
All reports are written on authors’ responsibility and thus the editors are not liable
for the contents of the report.

Tandem Accelerator Complex, Research Facility Center for Science and Technology,
University of Tsukuba
Tennodai 1-1-1, Tsukuba, Ibaraki 305-8577, Japan
http://www.tac.tsukuba.ac.jp/
annual@tac.tsukuba.ac.jp

PREFACE
This annual report covers researches carried out at University of Tsukuba Tandem
Accelerator Complex (UTTAC) during the fiscal year 2008 (1 April 2008 ∼ 31 March 2009).
The topics include not only accelerator-based researches using the 12UD Pelletron and 1 MV
Tandetron accelerators, but also closely related researches to UTTAC.
August 15, 2009
Editors-i-CONTENTS

1. ACCELERATOR AND EXPERIMENTAL FACILITIES
1.1

Accelerator operation 2008 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .

1

1.2

Status of the Tsukuba AMS system (2008) . . . . . . . . . . . . . . . . . . . . . . . . .

6

1.3

Development of tilted electrode gas ionization chamber with high-rate . . . . . . . . . . .

8

2. NUCLEAR PHYSICS
2.1

Measurement of nuclear magnetic moment of unstable nuclei 40 Sc . . . . . . . . . . . . . 11

2.2

Study of nuclear synthesis on 26 Al by gamma ray spectroscopy II . . . . . . . . . . . . . 13

3. MATERIALS AND CLUSTER SCIENCE
3.1

RBS study on Mg4 NiHx system . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15

3.2

Temperature dependence of hyperfine fields in spinel type Fe3 O4 nano-particles . . . . . . 16

3.3

Fabrication of aligned pairs of gold nanowires in SiO2 films by ion irradiation . . . . . . . 18

3.4

RBS of Pt and Cu nano-clusters on HOPG . . . . . . . . . . . . . . . . . . . . . . . . . 20

4. ACCELERATOR MASS SPECTROMETRY
4.1

Measurement of cosmogenic 36 Cl in the Dome Fuji ice core, Antarctica: Preliminary
results for the Last Glacial Maximum and early Holocene . . . . . . . . . . . . . . . . . . 21

4.2

Measurement of 36 Cl in groundwater samples from Satsuma-Iwojima . . . . . . . . . . . 23

4.3

Quantifying long-term limestone denudation using cosmogenic 36 Cl: an application toformative rate of a doline in the Akiyoshi karst, Japan . . . . . . . . . . . . . . . . . . . . 25

4.4

Production rates of 36 Cl for target elements in chondritic meteorites . . . . . . . . . . . . 27

4.5

Chemical procedure for sulfur reduction for 36 Cl-AMS of soil samples . . . . . . . . . . 29

5. INTERDISCIPLINARY RESEARCH
5.1

Nucleation rate of nano-particles in N2 /H2 O/SO2 by 20 MeV protons . . . . . . . . . . . 31

5.2

Open Advanced Facilities Initiative for Innovation (strategic use by industry) at UTTAC . 32

5.3

Micro-PIXE analyses of fluid inclusions in quartz from miarolitic cavities at the Kofu
granite, Japan . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33

6. LIST OF PUBLICATIONS
6.1

Journals . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37

6.2

International conferences . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 41

7. THESES43

8. SEMINARS

44

9. SYMPOSIUM

45

10. LIST OF PERSONEL

46- iii -

1.
ACCELERATOR AND EXPERIMENTAL FACILITIES1.1

Accelerator operation 2008

K. Sasa, S. Ishii, H. Kimura, H. Oshima, Y. Tajima, T. Takahashi, Y. Yamato,
T. Komatsubara, D. Sekiba and H. Kudo.
The total service time of the UTTAC multi-tandem accelerator facilities was 145 days (3,480 hours)in the fiscal year 2008. 24.8 % (864 hours) of the total service time was used by industrial users, under the
project "Open Advanced Facilities Initiative for Innovation (strategic use by industry)", which was
supported financially by the Ministry of Education, Culture, Sports, Science and Technology since 2007.
The 12UD Pelletron tandem accelerator
The operating time and the experimental beam time of the 12UD Pelletron tandem accelerator were1605.5 and 1177.4 hours, respectively, during the fiscal year 2008. Fig.1 shows the accelerator operation
hours per month. Fig.2 shows the beam time histogram with respect to the terminal voltage. Fig.3
represents the percentage of the operation hours for the three ion sources and ion species.
180

Machine operation hours

160
140
120
100
80
60
40
20
0

2008
Apr

May

Jun

Jul

Aug

Sep

Oct

Nov

Dec

2009
Jan

Feb

Mar

Fig.1. Accelerator operation hours per month for the 12UD Pelletron tandem accelerator in 2008.

11 MV
10 MV

Terminal voltage

9 MV
8 MV
7 MV
6 MV
5 MV
4 MV
3 MV
2 MV
1 MV
0

100

200

300

400

500

600

Beam hours

700

800

900

Fig.2. Beam time histogram as a function of the terminal voltage for the 12UD Pelletron
tandem accelerator in 2008.

1

1
H
15.2 %AMS
Ion Source

SputterIon Source
12

C
3.8
16

O
1.5

36

Cl
38.8

79

Br
4.2

197

Au
4.7

35

Cl
2.9

3
He
18.9

32

Si
0.2

28

Si
0.3

2
H
0.7

1
H
7.8

4

He
0.9

Polarized
Ion Source

Fig.3. Percentage of the operation hours for the three ion sources and ion species in 2008.
Accelerator Innovation
Heavy Ion Science
8.7
RBS
0.5
Detector 1.4
development
3.8
Nano Science(Heavy Ion
Irradiation)
7.6

Accelerator
Mass
Spectrometry(AMS)
42.3 %

AtomicPhysics
8.3
NuclearPhysics
27.4

Fig.4. Percentage of the experimental beam time for the running research fields in 2008.
In 2008, 56 research programs were carried out using the 12UD Pelletron tandem accelerator. Totally,
556 researchers used the 12UD Pelletron tandem accelerator. Fig.4 shows the percentage of theexperimental beam time for the running research fields with the 12UD Pelletron tandem accelerator.
The scheduled maintenance in the spring of 2009 was started on March 4. We replaced old corona
needles with a divided resistor system during this period. Fig. 5 shows a photograph of the divided resisterat the first unit. We adjusted the voltage gradient at the first unit in order to focus the ion beams on theterminal stripper position. At the first unit, a first accelerating tube was set to one third gradient. On theother hand, a 2nd accelerating tube was set to half gradient. The divided resister system allows theterminal voltage to vary from 1 to 11 MV without shorting column units. The divided resister system is2also expected to improve the stability of the terminal voltage. Fig. 6 shows the relationships between the
charging current and the terminal voltage for corona needles and the divided resistor system. There areappreciable differences in the gradient of the terminal voltage generation. In the case of the divided
resister system, the terminal voltage is proportional to the charging current.

Ion beam
0.37 GFirst unit
1/3 gradient

4/6
gap short
3/6
gap shortstringer

0.55 G

1/2 gradientstringer

gap full
1.1 G

Fig.5. A photograph of the divided resister system at the first unit of the 12UD Pelletron
tandem accelerator.

Fig. 6. The relationships between the charging current and the terminal voltage
for corona needles and the divided resistor system.

3

Fig. 7 shows the proton beam transmission for various terminal voltages without shorting column
units. The beam transmissions were measured between the object point on the injection magnet (FC-2) andthe analyzer magnet (FC-5), under the condition of the injected proton current of 100 nA. The SF6 gas
recovery system was also repaired during the scheduled maintenance. We replaced a vacuum pumping
system for SF6 gas.

Fig.7. Proton beam transmission for various terminal voltages without shorting column units.

4The 1MV Tandetron accelerator
The operating time and the experimental beam time of the 1MV Tandetron accelerator were 485.2
and 273.0 hours, respectively, during the total service time. In 2008, 41 research programs were carriedout using the 1 MV Tandetron accelerator. Totally, 216 researchers used the 1MV Tandetron accelerator.
Fig. 8 shows the percentage of accelerated ions for the 1MV Tandetron accelerator. Fig. 9 shows thepercentage of the experimental beam time for the running research fields. The 1MV Tandetron accelerator
was mainly used for trace-element analysis with Particle Induced X-ray Emission (PIXE), Rutherford
Backscattering Spectroscopy (RBS), Elastic Recoil Detection Analysis (ERDA) and Cluster physics. In
2008, a new RBS/ERDA system was installed in the C beam line (15 -course).

Ccluster
13.0

He
22.6

H
64.4 %

Fig.8. Percentage of accelerated ions for the 1 MV Tandetron accelerator in 2008.

RBS・
ERDA
22.6 %
Innovation
52.0

Cluster
Physics
12.3
PIXE
12.1
Education
1.0

Fig.9. Percentage of the experimental beam time for the running research fields
with the 1 MV Tandetron accelerator in 2008.

5

1.2

Status of the Tsukuba AMS system (2008)

K. Sasa, T. Takahashi, Y. Tosaki, K. Sueki, M. Tamari, T. Amano, T. Oki, Y. Yamato, Y. Nagashima, K.
Bessho 1, H. Matsumura1, N. Kinoshita1 and Y. Matsushi 2
We present the current status and research programs of a multinuclide accelerator mass
spectrometry (AMS) system on the 12UD Pelletron tandem accelerator at the University of Tsukuba(Tsukuba AMS system) in 2008. The Tsukuba AMS system can measure environmental levels of
long-lived radioisotopes of 14C, 26Al, 36Cl and 129I by employing a molecular pilot beam. We measured 365
samples in 2008, including samples for earth and environmental sciences and nuclear safety research.
Total operation of AMS facility was 56 days in 2008.
Table 1 Research programs and the number of samples by the Tsukuba AMS system in 2008.
AMS research programs

Target material

Organization

Number36

Cl-AMS36
Cl in the Dome Fuji ice core,
Antarctic ice core
Antarctica
36
Cl in the radiation shield at
Concreteaccelerator facilities
Bomb-produced 36Cl as a tracer inHydrological samples
groundwater(ground water, rain water)
36
In-situ Cl for denudation rates of karst
Limestone
landform
36

Cl in meteorite

Development of the chemical
procedure for sulfur reduction
Environmental monitoring for nuclear
facilities by AMS
36
Cl interlaboratory comparisons36
Cl exposure dating for Tiankeng
limestone samples

Meteorite

Univ. of Tsukuba

76

KEK

15

Univ. of Tsukuba

83

The Univ. of Tokyo 51
Tokyo Metro. Univ. 25

Environmental samples (soil) Univ. of Tsukuba

91

Environmental samples

Univ. of Tsukuba

9Standard samples

Univ. of Tsukuba 11
CIAE,
2
Guangxi University

Limestone

32

Si-AMS
32

Si-AMS research and development

SiO2

Univ. of Tsukuba

2

Performance of the Tsukuba AMS system
The performance of 36Cl-AMS was enhanced by improving the AMS technique and system,
including modifying the sample preparation technique [1], upgrading the ion source and installing a newdata acquisition system. Beam currents of 35Cl– and 37Cl– could be measured by the offset Faraday cupswith the beam-current monitoring system [2]. A typical beam current for 35Cl– was up to 20 µA. 36Cl14+
1
2

Radiation Science Center, High Energy Accelerator Research Organization
Micro Analysis Laboratory, Tandem Accelerator, The University of Tokyo6

with an energy of 100 MeV is detected by the gas ∆E – SSD E detector. The standard deviation offluctuations is typically ± 2%, and the machine background level for the 36Cl/Cl ratio is lower than 1 ×
10–15 with a halite sample, as shown in Figure 1(b) [2]. The AMS system achieved complete
discrimination between 36Cl and 36S up to a counting rate of ~5 kHz.

(1003 counts)

400
36Cl standard

36Cl/Cl=1.60×10−12

300

102

Halite sample

36Cl/Cl < 1 × 10−15

300

300
400
Eres in channels

10

36S14+

1800 sec
35Cl current: 11492 µC (6.5 µA)

300

104

36S
36Cl

(b)

400

36S14+

300 sec
35Cl current: 1929 µC (6.5 µA)

103

Counts∆E in channels

(a)

500

36Cl14+

Counts∆E in channels

500

400
Eres in channels

103
102
10

300
400
Eres in channels

300

400
Eres in channels

Fig. 1 (a) 36Cl spectrum of a standard sample for 36Cl/Cl = 1.60 × 10–12. (b) 36Cl spectrum of a halite
sample for the system background check. Total of three counts of 36Cl are detected for 30-min
measurement. The background level is less than 36Cl/Cl = 1 × 10–15.

Acknowledgements
This work was supported in part by Grants-in-Aid for Scientific Research Programs of the
Ministry of Education, Culture, Sports, Science and Technology, Japan (Grant-in-Aid Nos. 18360043,
19201003, 19300304, and 21310004) and the Promotion of Collaborative Research Programs in
Universities, KEK.
References[1] Y. Tosaki et al., Nucl. Instr. and Meth. B 259 (2007) 479.
[2] K. Sasa et al., Nucl. Instrum. Methods Phys. Res. B, 2009, in press.

7

1.3

Development of tilted electrode gas ionization chamber with high-rate

K.Ogawa, A.Ozawa, Y.Yasuda, K.Hara, T.Moriguchi, Y.Ito, H.Ooishi, Y.Ishibashi
We have been developing tilted electrode gas ionization chambers (TEGIC) as energy-loss detectors for
RI beams. Detection of energy-loss is indispensable for particle identification. It is known that energy
resolution of the detectors becomes worse at high counting-rate. Thus, we develop TEGIC, which can beused at the high counting-rate (~106 cps). A cross-sectional view of TEGIC is shown in Fig.1, where its
electrodes are tilted by 60  from the beam axis. In the previous experiment, rate dependences of energy
resolution have been measured with two different gases; P-10 and Ar-CF4 [1].

In this measurement,

6

energy resolution with P-10 becomes worse in the high-rate (~10 cps), on the other hand, energy
resolution with Ar-CF4 is almost constant for the counting rate.

Recently, tilted-angle dependences ofenergy resolution were investigated. The results show that there was no difference in the energy resolution
between 60  and 90  tilted-angles with the 103 cps counting-rate [2]. Thus, in the present experiment,
we investigate the tilted-angle dependences of energy resolution in the high-rate and try to confirm thedifference of the energy resolution with two gases.

Fig.1 A cross-sectional view of TEGIC.
The experiment was carried out at the 12UD Pelletron tandem accelerator. Ion beam of 12C nucleus was
accelerated up to 60MeV. The 12C beam, which was scattered elastically by a gold 2µm target to adjust thebeam intensity, was irradiated to TEGIC. The beam intensity was increased to 106 cps. TEGIC wasoperated using P-10 and Ar-CF4 with about 130 Torr. Counting-rate dependences of the energy resolution
with different tilted-angles are shown in Fig.2. In the high counting-rate (more than 105 cps), energy
resolution becomes worse in two different tilted-angles. Counting-rate dependences of the energy
resolution with different gases are shown in Fig. 3. Here, the energy resolutions in the two gases become
worse in the high counting-rate similarly. The present results are not consistent with the previous ones.
Further analysis is in progress.

8

50 deg.
90 deg.

14

Energy-resolution [%]

12
10
8
6
4
2
1000

10000
100000Count-rate [cps]1e+006

Fig.2 Counting-rate dependences of the energy resolution with two different tilted-angles (50 deg. and 90
deg. ). The diamond shape is 50 deg. Line is 90 deg.
Ar-CF4P-10

14Energy-resolution [%]

12
10
8
6
4
2
1000

10000
100000Count-rate [cps]1e+006

Fig.3 Counting-rate dependences of the energy resolution with two different gases (P-10 and Ar-CF4). The
diamond shape is Ar-CF4 gas. Line is P-10 gas.

References[1] K.Kimura, et.,al., Nuclear Instromental & Methods in Physical Resarch A 538(2005)608-614.
[2] Y.Yasuno, University of Tsukuba, Master thesis (2006).

9

10

2.
NUCLEAR PHYSICS

2.1 Measurement of nuclear magnetic moment of unstable nucleus 40Sc
Y.Ishibashi, A.Ozawa, Y.Tagishi, M.Iijima, Y.Ito, H.Ooishi, K.Ogawa, T.Moriguchi, Y.Yasuda,
T.Nagatomo1 and K.Matsuta2
The unstable nucleus 40Sc (half life T1/2=182 ms) is located near stable nucleus 40Ca, which is a doubly
closed shell nucleus. Thus, its nuclear structure is interesting. However, the nuclear magnetic moment (µ)
of 40Sc has never been measured. Since µ is sensitive to the configuration mixing in the nucleus, westarted to measure 40Sc.
Polarized 40Sc nucleus was produced at UTTAC by using 40Ca(p,n)40Sc (Q=-15.105 MeV) reaction. A
20 MeV polarized proton beam (P=88%) from the tandem accelerator irradiated a CaF2 crystal target witha thickness of 3 mm. The intensity of polarized proton beam was ~3 nA. Fig.1 shows setup around thetarget. The polarized proton beam was transported to the beam line of F-course in the first experimentalroom and was stopped in CaF2 crystal. Primary beam was chopped by a beam chopper., which was locatedat the entrance of the F-course. The beam chopper is a rotatable Cu cylinder with windows, as shown in
Fig. 2, and controls the primary beam with on : off=1:2.
To measure µ of 40Sc, we applied the β-NMR method [1]. The experimental setup for β-NMR isshown in Fig.1. To keep nuclear polarization of 40Sc inside the stopper, a static magnetic field (~2.5 kG)
was applied. A Helmholtz-type coil surrounded by the stopper produced a radio-frequency (RF) magnetic
field (~1.8 MHz, ~5 G) to perform NMR. The detectors located in up and down of the stopper counted thenumber of β-rays emitted from the stopped 40Sc. To search for the µ of 40Sc, we measured up and down
ratio of β-rays while changing the frequency of RF.
Magnet Pole
High-frequency

Plastic Scintillator

magnetic field(~5G)

Static magnetic

Polarized Proton Beam

field(~2.5kG)

Energy:20MeV

Cu(1mmt)

Intensity:~3.0nA

Fig.2. Beam chopper.

Chamber
Stopper(CaF2:3mmt)

RF CoilFig.1. Experimental setup around the target. Two plastic scintillators were used to detect β-rays. Cu
absorber located between the detectors and the chamber to cutlow energy β-rays.
We observed β-rays for 600 ms after the beam was stopped. Fig.3 (a) shows an observed typical time
spectrum of the β-rays.
1
2

RIKEN, Wako, Saitama 351-0198, Japan
Department of Physics, Osaka University, Toyonaka, Osaka 560-0043, Japan11

In Fig.3 (a), typical time spectrum for the β-rays is shown. Here, component of 40Sc is clearly seen in thefirst 120 ms. However, background is dominant in the last 120 ms. Observed NMR spectra for 40Sc isshown in Fig. 3 (b), where we extracted asymmetry changes observed in the last 120 ms from those in thefirst 120 ms. We measured NMR spectra with three different RF widths (160 kHz, 300 kHz, and 500 kHz).
To search for the magnetic moment, we averaged results with the different RF widths in the corresponding
magnetic moment in Fig. 3 (b), thus, the spectrum shown in Fig.3 (c) was obtained. We may see someasymmetry change near the |µ |=5.1 µN. To confirm this, further investigation is needed. Observed nuclear
polarization is very small in the present measurements, so it is necessary to increase asymmetry change.
We will apply higher static magnetic field and decrease background of β-rays in the future measurements.
Fig.3. (a) Typical time spectrum of β-rays. The(a)time spectrum of 40Sc is clearly visible in the first
120 ms. (b) NMR spectrum for the first 120 ms.
where experimental data in the last 120 ms are
subtracted. (c) NMR spectrum weighted average ofeach magnetic moment in (b).

(b)

(c)

µ [µN]µ [µN]

References[1] C.P. Slichter , Principles of magnetic resonance, 3rd enlarged and updated ed.

12

2.2

Study of nuclear synthesis of 26Al by gamma ray spectroscopy II

T. Komatsubara, A. Ozawa, K. Hara, T. Moriguchi, Y. Ito, H. Satake, H. Ooishi, Y. Ishibashi, T. Shizuma*,
T. Hayakawa*, S. Kubono#, S. Hayakawa#, D.N. Binh#, D. Kahl#, A. Chen% and J. Chen%* JAEA#

CNS, Tokyo University%

McMaster University, CANADA

Since observation of 1.809-MeV gamma rays by satellite gamma ray telescope has been reported[1], theastrophysical study of 26Al is very important for nuclear synthesis. The nucleus 26Al can be created by25

Mg(p,γ) reaction. However there is bypass reaction sequence 25Al(p,γ)26Si(β,ν)26mAl(β,ν) which emits no

gamma ray of 1.809 MeV. The excited states of 26Si, key nucleus, have been studied by reaction
mechanism[2-5] and gamma ray spectroscopy[6]. In our previous study, one new level is found above
proton threshold at 5886-keV in the 26Si[7]. For the determination of spin of the observed state,
gamma-ray angular correlation measurements were carried out.
In order to investigate level structure in 26Si, in-beam gamma ray spectroscopy was performed at UTTAC.
The excited states of the 26Si were populated by the nuclear reaction 24Mg(3He,n)26Si. The 3He beam of 10
MeV was irradiated on a natural Mg target. Gamma-gamma coincidence measurements were performedby using Ge detectors. Relative efficiencies of the Ge detectors are 140% and 70% at 1333-keV.
For the determination of spins, ratios of directional angular correlation of gamma-rays from oriented
states (DCO ratios)[8] have been evaluated. The larger Ge detector was located at 135 degree with respect
to the beam axis, while other was at 90 degree. For the values of 90-90 degree correlation, gamma-gamma
coincidence data taken in the last year were re-analyzed.
As the results of the DCO measurement, the ratios are shown as closed circles in Fig. 1 as a function of
the gamma ray energy. The gate gamma ray is 1797-keV 2+ → 0+ transition. In this figure, theoretical
expectation values are also shown as open triangles. In this calculation initial distribution of magnetic
sub-state is assumed by following distribution;

P ( m) =

e

−

J

m2
2σ 2

∑e

−

x2
2σ 2

.

x =− J

where the σ is assumed to be 2.0 J. Mixing ratios are also assumed to be zero.
For the gamma rays of 989- and 1960-keV transitions, measured values of DCO ratio agree with thecalculation within the errors where those are 2→2→0 and 3→2→0 transitions, respectively. For the1537-keV, small value of the DCO ratio is rather consistent with the calculation of 0→2→0 transition.

13

References[1] R. Diehl, H. Halloin, K. Kretschmer, G.G. Lichti, V. Schönfelder, A.W. Strong, A. Kienlin, W. Wang, P.
Jean, J. Knödlseder, J.P. Roques, G. Weidenspointner, S. Schanne, D.H. Hartmann, C. Winkler, C.
Wunderer, Nature 439 (2006) 45.
[2] D.W. Bardayan, J.C. Blackmon, A.E. Champagne, A.K. Dummer, T. Davinson, U. Greife, D. Hill, C.
Iliadis, B.A. Johnson, R.L. Kozub, C.S. Lee, M.S. Smith, P.J. Woods, Phys. Rev. C 65 (2002) 032801(R).
[3] J.A. Caggiano, W.B. Smith, R. Lewis, P.D. Parker, D.W. Visser, J.P. Greene, K.E. Rehm, D.W.
Bardayan, A.E. Champagne, Phys. Rev. C 65 (2002) 055801.
[4] Y. Parpottas, S. M. Grimes, S. Al-Quraishi, C.R. Brune, T.N. Massey, J.E. Oldendick, A. Salas, T.
Wheeler, Phys. Rev. C 70 (2004) 065805.
[5] P.N. Replowski, L.T. Baby, I. Wiedenhöver, S.E. Dekat, E. Diffenderfer, D.L. Gay, O. Grubor-Urosevic,
P. H öflich, R.A. Kaye, N. Keeley, A. Rojas, A. Volya, Phys. Rev. C 79 (2009) 032801(R).
[6] D. Seweryniak, P.J. Woods, M.P. Carpenter, T. Davinson, R.V.F. Janssens, D.G. Jenkins, T. Lauritsen,
C.J. Lister, J. Shergur, S. Sinha, A. Woehr, Phys. Rev. C 75 (2007) 062801(R).
[7] T. Komatsubara, K. Ebisu, T. Kawamata, A. Ozawa, K. Hara, T. Moriguchi, Y. Hashizume, T. Shizuma,
T. Hayakawa, S. Kubono, UTTAC Annual Report 2007, UTTAC-77 (2008) pp15-16.
[8] K.S. Krane, R.M. Steffen, R.M. Wheeler, Nuclear Data Tables, 11, (1973) 351.

Fig.1 DCO ratios for 26Si.

143.
MATERIALS AND CLUSTER SCIENCE

3.1

RBS study on Mg4NiHx system

D. Sekiba, S. Abe, M. Horikoshi, H. Kudo
Mg2Ni has been studied by many techniques because this alloy shows good absorption ability forhydrogen. Hydrogen storing alloys are important from the viewpoint of the sustainable energy. On the other
hand, many hydrogen storing alloys, which consist of Mg, show a remarkable property that metal-insulatortransition due to the hydrogenation. This transition is reversible for the hydrogenation and dehydrogenation.
Mg2Ni and Mg2NiH4 are reflective and transparent for the visible light, so that this material is calledswitchable mirror. Apart from the Mg2Ni, other Mg-based alloys such as Mg-Co, Mg-Ti, Mg-Fe show asimilar phenomenon.
A problem to be solved for the practical use of the Mg-Ni switchable mirror is the poor switching
durability. To elucidate the mechanism of degradation of the device, we constructed a new small chamber inwhich the Mg-Ni thin film is hydrogenated and dehydrogenated automatically by computer-controlled gas
inlet system. The samples were prepared by DC magnetron sputtering. We made Mg4Ni, referring the reportby Yoshimura et al. [1], on Si and glass substrate with the film thickness of 40 nm and 5 nm thick Pd cap
layer. We made a comparative study of RBS (Rutherford back scattering) on the both as-deposited andretrograded sample by 120 times switching. 1.6 MeV 4He was used as an incident beam, and the scatteredions were collected at the angle of 150 degree with respect to the incident direction.
Figure 1 shows RBS spectra obtained. The three peak features at ~ 0.6 MeV, ~ 0.8 MeV and ~ 1.2
MeV are attributed to oxygen, Mg and Ni, respectively. We can see that the Ni peak shifts toward the lower
energy, while the leading edges of Mg peaks are coincident between the as-deposited and retrogradedsamples. The O peak is observed only on the retrograded sample. By the analysis of these data we found outthat Mg4Ni showed a phase separation to the stoicheiometric Mg2Ni and Mg layers. The segregated Mg
layer below the Pd cap layer might construct stable hydride and oxide and play a role of blocking layer forthe hydrogen permeation.

Fig. 1: RBS spectra taken on the
as-deposited and retrograded samples.
1.6 MeV 4He2+ ion was used as anincident beam and scattered ions werecollected at the angle of 150 degreewith respect to the beam incident
direction.

References[1] K. Yoshimura, Y. Yamada, M. Okada, Appl. Phys. Lett. 81 (2002) 4709.

15

3.2

Temperature dependence of hyperfine fields in spinel type Fe3 O4nano-particles

M. Minagawa, H. Yanagihara, E. Kita and M. Kishimoto1
Magnetic hyperthermia has been a new therapy for small and spread cancerous tumors, because it
dose not need surgical operations. Using nano-sized magnetic particles and selective adhesion basedon the antigen-antibody reaction between the particles and cancer tumors, effective application of heat
power on the particular cells can be achieved. Particles are necessary to move in the human bodies,then sizes of the magnetic particles are limited to be small less than several tens of nano-meters. A
few mechanisms of heating with magnetic fine particles are considered, such as relaxation heating insuperparamagnetic(SPM) states (Neel mechanism), ferromagnetic hysteresis loss heating and frictionalmotion of magnetic particles.[1] Most of researches are using SPM particles in which particle aggregationof particles is small. Very large specific loss power (SLP) has been expected in the narrow distributionof particle sizes and, in other words, there are severe conditions in size and distribution of magnetic
nanoparticles and driving frequency. If ferromagnetic nanoparticles can be used for hyperthermia, there ismuch less limitation for tuning of operation conditions.
We have been testing the ability of ferromagnetic nano-particles with rather higher coercive force as a
hyperthermia material[2]. To understand the relation between coercive force and heating ability, magnetic
states of nano particles are an important issue. We performed Mössbauer study to understand the influenceof thermal fluctuation on the ferromagnetic state of nano-particles.

Fig. 1. Sample holder part of Mössbauer measurement oven. Temperature range from room temperature
to 200◦ C can be achieved. The heater is made of a type E fine sheath thermocouple. A Pt resistancethermometer is set into the housing.

Cobalt-contained iron oxide particles with spinel structure, (Co)Fe3−δ O4 , were produced by heating
the co-precipitants containing Co2+ , Fe2+ and Fe3+ ions.[2] Spinel structures were confirmed with X1 Hitachi Maxell, Ltd.

16

ray diffraction patterns. The coercive forces (HC ) from 50 Oe to 240 Oe were obtained by changing thecontent of Co ions from 2 ∼ 7 at% of total Fe ions. Sizes of nano-particles were ranged between 10
and 20 nm. Sample ATH1 (pure Fe oxide with HC of 50 Oe) and ATH4 (Co doped Fe oxide with HC of
160 Oe) were used for Mössbauer measurements. To perform high temperature measurements between
room temperature and 200◦ C, a new sample oven was built(see Fig. 1). The sample temperature wasmeasured with a Pt thermometer. Data were analyzed with a commercially available software, MossWinn
3.0. Distribution in hyperfine field(Hhf ) was taken into account carried out in the analysis.
ATH4

140 °C

80 °C

(a)
-10

200 °C

Transmission (arb.)

Transmission (arb.)

200 °C

140 °C

80 °C

RT

(b)
-5

0

5

10

-10

Velocity (mm/s)

-5

0

5

10

Velocity (mm/sec)

Fig. 2. Mössbauer spectrum of the samples ATH1 and ATH4 at the temperature range between room
temperature and 200 ◦ C. Solid lines display results of numerical fitting.

Mössbauer spectra for ATH1 and ATH4 samples are show in Figs. 2 (a) and (b), respectively. At room
temperature, ferromagnetic sextets with slightly spread hyperfine fields were observed in both samples
and no trace of SPM contribution was found. Elevating sample temperature, the spectra for the ATH1
above 140 ◦ C composed of a major ferromagnetic sextet and a doublet which is originated from an SPM
state. This result suggests that ATH1 has two magnetic phase above 140 ◦ C and the ferromagnetic state in
ATH1 is relatively weak. ON the other hand, feromagnetism in the ATH4 sample is stable even at 200 ◦ C.
Higher heat generation has been proved by applying AC high magnetic field test for ATH4 samples thanthe ATH1 sample.
This work is a part of a cooperative research carrying out with digestive surgery group in Universityof Tsukuba and AIST.

References[1] for example, see R. Hergt and W. Andrä, Magnetism in Medicine Wiley-VCH, Weinheim 2007, p.
550.
[2] Eiji Kita, H. Yanagihara, S. Hashimoto, K. Yamada, T. Oda, M. Kishimoto, and A. Tasaki, IEEE Trans
Magn., vol. 42 pp. 3566-3568, 2008.

17

3.3

Fabrication of aligned pairs of gold nanowires in SiO2 films by ion
irradiation

Koichi Awazu, 1 Xiaomin Wang,1 Tetsuro Komatsubara
Introduction
It has been found that anisotropic metal colloids can be fabricated in a controllable manner by irradiationof core-shell colloidal particles by swift ions of megaelectron volt (MeV) energy, where each colloidal
particle has a Au core surrounded by a silica shell. [1] However, it has been pointed out that the process of
Au elongation could be very complicated. For example, the uncontrolled nucleation and growth processes
results in broad spatial and size distribution of the nanoparticles during ion irradiation.[2] Heinig andcoworkers [3] reported that the mean size of Au nanoparticles in SiO2 theoretically increases withincreasing implantation temperature, a process known as Ostwald ripening, but that inverse Ostwald
ripening occurs below a certain critical temperature. To avoid these kinds of complicated matters, we usedelectron-beam lithography to fabricate Au nanoparticles of a constant diameter spaced a constant relatively
large distance apart in a SiO2 matrix, and we examined the dependence of the elongation of thenanoparticles on their initial size and on the fluence and flux of the ion beam.
Experimental procedure
To form the substrate, a 2- m-thick layer of amorphous SiO2 (a-SiO2) was fabricated by surface oxidationof a silicon wafer with water vapor at 1000 C. The a-SiO2 substrate was spin-coated with a 50-nm-thicklayer of ZEP520-type resist, and the coating layer was cured at 180 °C for 3 min. Nanoscale patterns weredrawn in a 200 × 200 μm region of the resist by electron-beam lithography. Subsequent development
produced pairs of nanoscale holes in the resist on the a-SiO2 substrate. The substrate was then mounted inan evaporator and a 0.5-nm-thickCr layer was applied to aid adhesion of a subsequently deposited
40-nm-thick layer of Au. Next, the resist was removed by treatment with acetone to leave an array of pairsof Au nanodisks on the a-SiO2 substrate. The Au nanodisk pairs were then embedded in a-SiO2 bydepositing a second layer of silica by sputtering from a silica target in an Ar atmosphere. The thickness ofthe top layer of a-SiO2 was 200 nm. The final assemblies were irradiated with 110-MeV Br10+ ionsproduced by the 12-unit double Pelletron tandem accelerator at University of Tsukuba. The beam current
was changed from 10 nA to 60 nA to examine the effect of the flux density. Flux density was calculated
from the beam current, where a beam current of 100 nA corresponded to (2.8

0.3)

1011 cm–2 s–1. The

direction of propagation of the ion beam was perpendicular to the upper surface of the a-SiO2.
Cross-sections of the pristine and irradiated samples were examined by transmission electric microscopy(TEM).
Results and Discussion
We examined the dependence of elongation of Au nanodisks on the flux density of the ion beam at aconstant fluence. Figures (a)– (d) show Au nanoparticles embedded in SiO2 before irradiation (Fig. (a))

18and after irradiation with 110-MeV Br10+ ions at flux densities of 3s–1 [Fig. (c)], and 1.61010 cm–2 s–1 [Fig. (b)], 6

1011 cm–2 s–1 [Fig. (d)] at a constant fluence of 21014 cm–2. The aspect ratio of

the nanorods increased markedly with increasing flux density up to a flux density of 61010 cm–2 s–1 inthe direction of propagation of the ion beam. The aspect ratio reached 20 at a flux density of 6
s–1. At a flux density of 1.6

1010 cm–2

1010 cm–2

1011 cm–2 s–1, however, the positions, as well as the lengths, of Au nanodisks

pairs were changed (Fig. (d)).
Summary
We successfully avoided Ostwald ripening by fabricating Au nanoparticles pairs with a constant separationof 60 nm. By this technique, the mechanism of elongation of Au nanoparticles was considerably simplified.
Au nanodisks of diameter 40 nm were elongated in a manner dependent on flux density of ion irradiation.
We assume that both the 40-nm-diameter Au nanoparticles and surrounding a-SiO2 were melted during ion
bombardment.

Figures. Bright-field and cross-sectional TEM(a)micrographs. The flux density dependence of
500nm
(b)

Au elongation was examined at a constant

500nm

fluence of 2 × 1014 cm–2. (a)–(c); Au

Ion propagation

nanodisks of 40 nm in diameter. Specimens(c)were created with focused ion beam. (a);500nm

before irradiation of 110-MeV Br10+ ion. (b),(c), and (d); flux density of 3 × 1010 cm–2 s–1,
500nm

6 × 1010 cm–2 s–1, 1.6 × 1011 cm–2 s–1,(d)respectively. The direction of ion propagation
direction is shown by the arrow.

500nm

References[1] Roorda S, Dillen T V, Polman A, Graf C, Blaaderen A V and Kooi B J 2004 Adv. Mater. 16 235[2] Rizza G,Ramjauny Y,Gasoin T, Vieille L and Henry S, 2007 Phys. Rev. B 76 245414[3] Heinig K H, Müller T, Schmidt B, Strobel M and Möller W 2003 Appl. Phys. A 77 17

19

3.4

RBS of Pt and Cu nano-clusters on HOPG

T. Kondo, T. Suzuki, J. P. Oh, D. Sekiba, H. Kudo and J. Nakamura
Understanding the interface interaction between metal nano-clusters and the surfaces ofgraphite-related material is indispensable for many industrial applications such as catalysis. It has beenfound that Pt monolayer clusters, with a width of 2-3 nm, on a highly oriented pyrolytic graphite (HOPG)
surface promote catalytic activity for the H2-D2 exchange reaction [1]. The origin of this enhancement has
been attributed to the interface interaction between the Pt atoms and the graphite surface which leads to ashift in the d-band center of the Pt away from the Fermi level. This result suggests that even for the inert
metal atoms for the H2-D2 exchange reaction such as Cu, the promoted catalytic activity may appear byforming monolayer cluster on the graphite surface through the interface interaction. In this work, we haveinvestigated the catalytic activity of Cu/HOPG as well as Pt/HOPG in terms of H2-D2 exchange reaction.
Fig. 1a shows typical RBS spectra for HOPG, Pt/HOPG and Cu/HOPG. There is no peak originatingfrom contaminants such as O2 or other metal atoms, suggesting that the Pt or Cu atoms are successively
deposited on HOPG without any contamination. Based on the spectra, the absolute amount of Pt or Cu on
HOPG is estimated. The catalytic activities km of Pt/HOPG and Cu/HOPG for the H2-D2 exchange reaction
measured in the high-pressure reactor-cell at 400 K under 24 Torr condition (H2:D2 = 1:1) are summarized
in Fig. 1b as a function of the absolute coverage of Cu or Pt on HOPG.. The catalytic activity of Cu/HOPG
is found to be 1-2 orders of magnitude smaller than that of Pt/HOPG. Similar low catalytic activity has
also been reported for Cu films on HOPG [2]. Thus the Cu atoms deposited on HOPG in this work may
form larger and thicker domains instead to form monolayer clusters with a width of 2-3 nm. By changing
the deposition condition of Cu and measuring the morphology of Cu cluster by scanning tunnelingmicroscopy, we will investigate the catalytic activity of Cu/HOPG more in detail.
18(a)
Carbon17

Ei = 1.6 MeV

HOPG
Pt
Cu
0.4

0.8
1.2
Energy (MeV)

Pt/HOPG

10

16

Cu/HOPG

10

15

10

Cu/HOPG
1.6(b)

Pt/HOPG
km [molecules/s]

He ion intensity [arb. units]

10

Background

14

2.0

10

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

CuCcoverage [ML]Fig. 1: (a) RBS spectra taken on the HOPG, Cu/HOPG and Pt/HOPG. 1.6 MeV 4He2+ ion was used
as an incident beam and scatted ions were collected at the angle of 150 degree with respect to thebeam incident direction. (b) km of Cu/HOPG and Pt/HOPG for the H2-D2 exchange reaction.
References[1] T. Kondo, K. Izumi, K. Watahiki, Y. Iwasaki, T. Suzuki, J. Nakamura, J. Phys. Chem. C 112 (2008) 15607.
[2] Johansson et al., J. Chem. Phys. 128 (2008) 034706.

20

4.
ACCELERATOR MASS SPECTROMETRY

4.1

Measurement of cosmogenic 36Cl in the Dome Fuji ice core, Antarctica:
Preliminary results for the Last Glacial Maximum and early Holocene

K. Sasa, Y. Matsushi3, Y. Tosaki, M. Tamari, T. Takahashi, K. Sueki, T. Amano, T. Oki, Y. Nagashima, H.
Matsumura1, N. Kinoshita1, K. Bessho 1, K. Horiuchi2, H. Matsuzaki3, Y. Shibata4, M. Hirabayashi5 and H.
Motoyama5
We report the results of trial measurements of 36Cl concentrations for ~150 g-size of ice persample, with the aim of enabling routine analysis during planned high-resolution multi-nuclide research aspart of the second deep-ice-core project at Dome Fuji Station (DF2) in Antarctica (77°19'01'' S, 39°42'12''
E; 3810 m above sea level) [1]. Samples analyzed were taken from those parts of the DF2 ice core
corresponding to the Last Glacial Maximum (LGM) and early Holocene. We also present preliminary
calculations of the depositional flux of cosmogenic 36Cl for these periods, as an initial result from inland
Antarctica.
Ten samples, obtained as ice chips produced from core trimmings for measurements of electricalconductivity, were analyzed for 36Cl concentrations. These samples were obtained from 540 m, 490 m, and
340–320 m below the surface of the ice sheet, corresponding to ages of 22, 18, and 11–10 kyr according to
the DFO-2006 age scale, respectively [2]. Each sample comprised 0.5 m in core length (110–180 g inweight), corresponding to a temporal resolution of approximately 30–40 years.
successfully conducted with at least ~100 counts of total
full-processing chemistry blank yielded 0.6 × 10

–14

36

Cl-AMS was36

Cl detection for the ice samples. The

36

of Cl/Cl. The 36Cl/Cl values for the ice samples range

from 2 × 10–14 to 16 × 10–14 after subtraction of the background observed in the chemistry blank. The
original chlorine concentrations in the LGM samples range from 210 to 260 ppb, corresponding to lessthan 5% of the carrier amount. The overall uncertainty in the measurements was ~10% for the Holocene
samples with a larger carrier amount, and up to ~6% for the LGM samples. The 36Cl concentrations in theice samples range from 6 × 103 to 8 × 103 atoms g–1 for the early Holocene, and from 14 × 103 to 17 × 103
atoms g–1 for the LGM. The differences in concentrations between the two periods reflect contrasting rates
of snow accumulation during glacial and interglacial periods. The annual net amount of snow
accumulation can be estimated empirically from the δ18O value of ice [3], which is about−60‰ for the
LGM and −54‰ for the early Holocene [4], corresponding to snow accumulation rates of ~1.8 and ~4.3 g
cm–2 yr–1, respectively [3]. These rates differ by a factor of ~2.4; accordingly, the contrasting 36Cl
concentrations between the LGM and early Holocene are well explained by the dilution of nuclide fallout
by snow deposition. The apparent depositional fluxes of 36Cl onto the ice sheet were calculated from thenuclide concentrations multiplied by the snow accumulation rates. The calculated 36Cl fluxes are nearly1Radiation Science Center, High Energy Accelerator Research Organization
Hirosaki University
3
Micro Analysis Laboratory, Tandem Accelerator, The University of Tokyo
4
National Institute for Environmental Studies
5
National Institute of Polar Research2

21

identical for the LGM and early Holocene (uncorrected for post-depositional 36Cl radioactive decay),
being approximately 2.5–3.5 × 104 atoms cm–2 yr–1 (Fig. 1). These values are similar to the prospective
nuclide flux at ~80 °S (~4–5 × 104 atoms cm–2 yr–1), estimated from the latitudinal dependence of nuclide
fallout [5] and the global mean production rate of 36Cl [6, 7]. This similarity demonstrates the reliability of
our measurements and the integrity of the 36Cl record in the DF2 ice core. The 36Cl flux at Greenland overthe past 100 kyr was 5–10 × 104 atoms cm–2 yr–1 [8], which is 2–3 times higher than our values (Fig. 1).
The reason for this discrepancy is currently unclear, but it probably reflects the different post-depositional
behavior of chloride [9], and/or contrasting transport processes of the nuclide related to the characteristic
4
3
2

36Cl conc. (103 atoms g−1)

20
1536Cl flux (104 atoms cm−2 yr−1)

tropospheric circulation regimes in the Northern and Southern Hemispheres.

10
5
0
10-11
Holocene18

22

Age (ka)

LGM

Fig. 1 Comparison of 36Cl concentrations (gray bars) and depositional fluxes (open boxes) for theLast Glacial Maximum (LGM) and early Holocene at Dome Fuji Station, Antarctica. Error bars
indicate ±1σ analytical uncertainty. Horizontal dashed lines represent averages for each period.
Acknowledgements
This work is supported in part by the Grants-in-Aid for Scientific Research Program of the Ministry of
Education, Culture, Sports, Science and Technology, Japan.
References[1] H. Motoyama, Scientific Drilling 5, (2007) 41–43.
[2] K. Kawamura et al., Nature 448 (2007) 912.
[3] K. Satow et al., Polar Meteorol. Glaciol., 13 (1999) 43-52.
[4] O. Watanabe, J. Jouzel, S. Johnsen, F. Parrenin, H. Shoji, N. Yoshida, Nature 422 (2003) 509.
[5] D. Lal, B. Peters, in: K. Sitte (Ed.), Handbuch der Physik, Vol. 46/2, Springer, Berlin, 1967, p. 551.
[6] J. Masarik, J. Beer, J. Geophys. Res. 104/D10 (1999) 12099.
[7] D. Huggle et al., Planet. Space Sci. 44 (1996) 147.
[8] S. Baumgartner et al., J. Geophys. Res. 102/C12 (1997) 26659.

[9] R.J. Delmas et al., Tellus 56B (2004) 492.

22

4.2

Measurement of 36Cl in groundwater samples from Satsuma-Iwojima

Y. Tosaki, K. Sasa, T. Takahashi, Y. Matsushi 1, M. Tamari, T. Amano, K. Kazahaya 2, M. Yasuhara2, H.A.
Takahashi2, N. Morikawa2, M. Ohwada2 and K. Asai 3
Introduction
Chlorine-36 is an informative environmental tracer for determining the sources of chloride [1]. In
order to distinguish one from other chloride sources, this application generally requires highly sensitive
36

Cl/Cl measurements, typically down to the order of 10−15. This work therefore attempts to detect such

low level 36Cl/Cl in groundwater, and tests the applicability of our AMS (accelerator mass spectrometry)system. The eventual goal of this study is to investigate whether the application of 36Cl can contribute to
the understanding of groundwater systems under the influence of seawater and volcanic activity.
Study area and methods
Satsuma-Iwojima was selected as the study area, which is a volcanic island located at ~50 km south of
Kyushu, southwestern Japan. This island constitutes the northwestern margin of the Kikai caldera formed
after a large-scale eruption approximately 7,300 years ago [2,3]. The main largest aquifer exists in the
middle of the island, exclusively offering drinkable groundwater [4]. During 28–29 November 2007,
samples were collected from 9 wells within the main aquifer (samples Nos. 1–9) and 4 coastal hot springs
around the island (Nos. 10–13).
Chloride concentrations were determined by ion chromatography at the Geological Survey of Japan.
The 36Cl/Cl ratios of the samples were measured with the AMS system at UTTAC. The sample volume for
AMS ranged between 0.5 mL and 50 mL, corresponding to ~2 mg of Cl. Silver chloride (AgCl) was
directly precipitated from each sample by using the standard method [5]. The background for the entire
processes was evaluated with a process blank (halite sample), which gave a 36Cl/Cl ratio of (1.3 ± 0.6) ×
10−15. The measured ratios were normalized to a 36Cl standard (36Cl/Cl = 1.60 × 10−12 [6]) and corrected
for the background.
Results and discussion
Table 1 presents 36Cl/Cl ratios and Cl− concentrations in the samples. The obtained ratios were in therange of 1–6 × 10−15. These low ratios might be attributed to the low meteoric 36Cl/Cl ratios due to theclose proximity of the sea. After recharge, there would be additional influences in aquifers by magmaticcomponents and seawater. Figure 1 depicts the relationship between 36Cl/Cl ratios and Cl− concentrations.
As an overall trend, the 36Cl/Cl ratios decrease with increasing Cl− concentration. Since the 36Cl/Cl ratios
in seawater and magmatic water are both expected to be very low (~1 × 10−15 or less) [7], the mixing of
the Cl− from these components with meteoric water could have resulted in isotopic dilution effects. This
1

Micro Analysis Laboratory, Tandem accelerator, The University of Tokyo.
Geological Survey of Japan, National Institute of Advanced Industrial Science and Technology
3
Geo-Science Laboratory Co. Ltd.
2

23

reasonable trend supports the fundamental validity of the data presented here.
Figure 1 also shows several data points deviating from the mixing trend. Possible explanations include
the difference in contribution of bomb-produced 36Cl input (when the groundwater was recharged), which
would be related to groundwater residence times. At present, however, we do not have enough data forfurther interpretation. When other geochemical and isotopic parameters are available, we will move on toa detailed discussion on the relationship between the 36Cl data and the groundwater system.
References[1] F.M. Phillips, in: P.G. Cook, A.L. Herczeg (Eds.), Environmental Tracers in Subsurface Hydrology,
Kluwer, Boston, 2000, p. 299.
[2] K. Ono, T. Soya, T. Hosono, Geology of Satsuma-Io-Jima District, Geological Survey of Japan,
Tsukuba, 1982 (in Japanese with English Abstract).
[3] H. Kitagawa, H. Fukuzawa, T. Nakamura, M. Okamura, K. Takemura, A. Hayashida, Y. Yasuda,
Radiocarbon, 37 (1995) 371.
[4] K. Kazahaya, H. Shinohara, G. Saito, Programme and abstracts, the Volcanological Society of Japan,
1994-2 (1994) 218 (in Japanese).
[5] Y. Tosaki, N. Tase, G. Massmann, Y. Nagashima, R. Seki, T. Takahashi, K. Sasa, K. Sueki, T.
Matsuhiro, T. Miura, K. Bessho, H. Matsumura, M. He, Nucl. Instr. and Meth. B 259 (2007) 479.
[6] P. Sharma, P.W. Kubik, U. Fehn, H.E. Gove, K. Nishiizumi, D. Elmore, Nucl. Instr. and Meth. B 52
(1990) 410.
[7] G.T. Snyder, U. Fehn, F. Goff, Earth Planet. Space 54 (2002) 265.

Table 1Chloride concentrations and 36Cl/Cl ratios in Satsuma-

10

Iwojima samples
Cl− (mg/L)

36

Cl/Cl (10−15)

SIJW_07_001
SIJW_07_002
SIJW_07_003
SIJW_07_004
SIJW_07_005
SIJW_07_006
SIJW_07_007
SIJW_07_008
SIJW_07_009
SIJW_07_010
SIJW_07_011
SIJW_07_012
SIJW_07_013

141
112
75.9
106
40.3
327
139
105
375
9978
1999
10066
1331

6.0 ± 1.2
3.4 ± 1.2
4.5 ± 1.1
3.8 ± 1.1
6.2 ± 1.0
2.4 ± 0.9
5.4 ± 1.1
3.7 ± 1.1
0.9 ± 0.8
3.9 ± 1.0
2.5 ± 0.9
1.0 ± 0.8
1.4 ± 0.88Cl/Cl (10−15)

Sample ID

6
4

36

No.
1
2
3
4
5
6
7
8
9
10
11
12
13

2
0

0

0.01

0.02

0.03

1/Cl− (L/mg)

Fig. 1. 36Cl/Cl ratios in the samples, plottedagainst reciprocal Cl− concentrations.

24

4.3

Quantifying long-term limestone denudation using cosmogenic 36Cl:
an application to formative rate of a doline in the Akiyoshi karst, Japan

Y. Matsushi1, K. Sasa, K. Sueki, T. Takahashi, T. Hattanji and Y. Matsukura
Introduction
Determination of denudation rates of land surfaces poses a fundamental issue in understanding
landscape evolution over long timescales. Recent advances in the methodology using in situ-produced
cosmogenic nuclides have brought innovation to strategies for quantifying denudation. Cosmogenic 36Cl in
calcite offers such a tool for carbonate rocks, providing an indicator of long-term physical and chemical
mass loss from eroding surfaces [1]. Procedures for measuring cosmogenic 36Cl and original Cl in rocks
have already been developed at the University of Tsukuba Tandem Accelerator Complex (UTTAC) [2].
This paper reports an application of this method for a doline in the Akiyoshi karst composed of Mesozoic
metamorphosed limestone, southeast Japan.
Samples and measurements
A small doline was selected (N34°15'35", E131°18'36", ~320 m a.s.l.) on the Akiyoshi-karst tableland.
The doline exhibits a typical amphitheater-shaped depression with ~150 m in diameter and ~17 m inrelative height. A north-south oriented cross section was surveyed, for which rock outcrops are available
for sampling as many bare limestone pinnacles expose markedly along this direction. Samples werecorrected at nine locations from the topmost ~5 cm of the pinnacles standing 50–140 cm high from its

Large

36

Erosionrate

Cl conc. (105 atoms g−1)base. The nine sampling sites cover across the entire profile of the cross section (Fig. 1).

Small

2

Cosmogenic 36Cl

4
6
8
N

9

7

45 °N

6

1
40

10 m

Akiyoshi
karst

5

2
4
3

35

30

130 °E135

8 S

500 kmTopography: Rock outcrops

20 m
Vertical : Horizontal = 2 : 1

1~9: Sampling sites

Fig. 1. Cosmogenic 36Cl concentrations in limestone surfaces along a cross sectional profile of a doline in
the Akiyoshi karst, Japan. Preliminary calculation indicates the denudation rates ranging from ~90 to ~25
mm kyr−1, corresponding to the nuclide concentrations from 2 × 105 to 8 × 105 atoms g−1, respectively.

1

Micro Analysis Laboratory, Tandem accelerator, The University of Tokyo (E-mail: matsushi@n.t.u-tokyo.ac.jp).

25Samples were prepared by a standard procedure for 36Cl accelerator mass spectrometry (AMS) [2,3],
and for Cl measurements by isotope dilution using a 99 atom%-enriched 35Cl carrier from Aldrich Co.
[2,4]. Simultaneous measurements of 36Cl and Cl were carried out with the Tsukuba AMS System at
UTTAC [5], by using an AMS-standard with the known 36Cl/Cl ratio of 1.60 × 10−12 [6]. Concentration of
Ca and abundances of other neutron absorption nuclei were determined for one of the nine samples (fromsite 1) by prompt gamma-ray analysis (PGA) with JRR-3M nuclear reactor at the Japan Atomic Energy
Agency (JAEA).
Nuclide concentrations and denudation rates
Concentrations of 36Cl in the samples range from 2 × 105 to 8 × 105 atoms g−1, tending higher at upperparts, and lowest at bottoms of the slopes (Fig. 1). This tendency indicates that denudation rates are fastest
at the center of the depression, and hence the doline has not reached a morphometric steady-state but isin-the process to be deepened.
Denudation rates of the limestone surfaces were calculated from the 36Cl concentrations and nuclide
production rates in calcite. The 36Cl production rates were scaled preliminary through the calibrated
spallogenic and muogenic nuclide production systematics [1,3,7], by using the latitude and elevation at thesites, and the measured chemical composition of the limestone: [Ca] = 39.2%, [Fe] = 0.2%, [Cl] = 4–9
ppm, [B] = ~0.4 ppm, [Sm] = ~0.3 ppm and [Gd] = ~0.3 ppm, with bulk density of 2.7 g cm−3. The
calculated denudation rates range from ~25 mm kyr−1 for the maximum 36Cl concentration at the site 8 to
~90 mm kyr−1 for the minimum at the site 4, indicating 3−4 times higher rates at the bottom than at ridgesof the doline.
The difference between the denudation rates is ~65 mm kyr−1, and thereby the time needed for theformation of the relative height between the bottom and ridges (~17 m) is calculated to be about 260 kyr.
During this duration, the doline experiences surface lowering of ~23 m at the center of the depression, and~6.5 m even at the ridge with the lowest denudation. The difference in denudation rates may be attributed
to nonuniform water supply, providing that the conditions of subsoil CO2 and temperature are not muchvaried along the slopes. We are planning hydrological monitoring, including subsoil moisture contents aswell as soil-air CO2 concentrations and temperatures at the side slope of this doline, to explain
mechanisms controlling the denudation rates of limestone surfaces linked to dynamic evolution of karst
landforms.
References[1] J.O.H. Stone et al., Geochim. Cosmochim. Acta 62 (1998) 433.
[2] Y. Matsushi et al., Nucl. Instr. and Meth. B in press.
[3] J.O. Stone et al., Geochim. Cosmochim. Acta 60 (1996) 679.
[4] D. Desilets et al., Chem. Geol. 233 (2006) 185.
[5] K. Sasa et al., Nucl. Instr. and Meth. B in press.
[6] P. Sharma et al., Nucl. Instr. and Meth. B 52 (1990) 410.
[7] J.O. Stone, J. Geophys. Res. 105 B10 (2000) 23753.

26

4.4

Production rates of 36Cl for target elements in chondritic meteorites

Y. Hamanaka 1, Y. Oura1, M. Ebihara1, K. Sasa, Y. Nagashima, T. Takahashi, Y. Tosaki, Y. Matsushi,
M. Tamari, T. Amano, K. Sueki, K. Bessho 2, N. Kinoshita2
Stable and radioactive cosmogenic nuclides, which are produced by nuclear reactions with high-energy
cosmic rays during their flights in the space, provide important cosmochemical information. For example,
several cosmogenic nuclides having different half life were determined simultaneously to be clear aboutcomplex cosmic-ray irradiation history [1].

36

Cl is a one of the cosmogenic radionuclides and produced

by several nuclear reactions such as proton and neutron induced spallation reactions (main target elements:
K, Ca, Ti, Cr, Mn, Fe, and Ni) and neutron capture reaction (target nuclide: 35Cl). Cross sections of thosereactions are depended on particle energies characteristically. Thus it is suggested that additional
information must be obtained from 36Cl production rates normalized by a weight of target element (indpm/kg) for individual target element. Therefore, we tried to determine production rates of 36Cl in two
chondritic meteorites in 2006 [2]. Further elemental production rates of 36Cl were determined in anothertwo meteorites in this study.
Two fragments of Gold Basin (L4 chondrite) and a fragment of Gao (H5 chondrite) were used in thissturdy. From powdered whole-rock samples, five phases with different elemental compositions wereseparated by both physical and chemical treatments. Chemical compositions of target elements for bulk
and five separated phases samples were determined nondestructively by neutron induced prompt
gamma-ray activation analysis (PGA) and instrumental neutron activation analysis. For analysis of 36Cl byaccelerator mass spectrometry (AMS), AgCl precipitates were prepared for each powder samples by achemical process. 36Cl/Cl ratios were determined by AMS at the Tandem Accelerator Complex, Universityof Tsukuba.
In Table 1, 36Cl concentrations in separated phases of 3 fragments are shown. For all 3 fragments,
silicate phases dissolved in nitric acid had highest 36Cl concentration among bulk and 5 separated phases.
These phases had also highest Cl concentrations and variations of Cl concentration among 6 phases ineach fragment were significant in comparison with other target element concentrations except Co and Ni.
Thus, experimentally, contribution of Cl to 36Cl production in chondrites was proved qualitatively. Welten
et al. [2] determined some cosmogenic nuclides including 36Cl in 15 fragments of Gold Basin meteorite
and estimated depth of those fragments in the pre-atmospheric meteoroid. According to the correlation
between 36Cl concentration and estimated depth, depths of fragment 1 and 2 in the meteoroid are estimatedto be about 90 cm and 120 cm, respectively.
Production rates of 36Cl for element groups, which are classified based on excitation function of proton
induced spallation reaction, were calculated from 36Cl concentrations and elemental abundances in bulk
and separated phases, and shown in Table 2. It is noted that values in Table 2 are preliminary because Cl
concentrations determined by PGA have a large uncertainty. Additional analysis of Cl by radiochemical
1
2

Graduate School of Science and Engineering, Tokyo Metropolitan University
Radiation Science Center, High Energy Accelerator Research Organization27

photon activation analysis (RPAA) is planed to determine accurately. For Gold Basin meteorites,
production rates for all element groups except Cl in fragment 1 are higher than those in fragment 2 anddifferences between fragments are varied according to element group. And the ratio of production rate for(K + Ca) to one for (Fe + Co + Ni + Mn) in fragment 2 is smaller than in fragment 1. As describing above,
fragment 2 was estimated to be originated from deeper position in a meteoroid than fragment 1, whichmeans that fragment 2 was irradiated by protons and/or secondary neutrons with smaller energy thanfragment 1. Considering a feature of excitation functions on proton induced spallation reaction (withincrease of production rate for Ca and Fe, a ratio of them decreases), the ratio of production rate infragment 2 should be larger than in fragment 1. Calculated production rate for (K + Ca) in fragment 2 isguess to be too small. Relation of production rates between fragment 1 of Gold Basin and Gao seems to bereasonable. In contrast, production rates for Cl are similar among 3 fragments. Welten et al. [3] showedthat concentrations of 36Cl and 41Ca produced by neutron capture in Gold Basin were dependent on depth.
Therefore, after determining Cl concentration by RPAA, production rates will be calculated again, andfurther determination of 36Cl in many fragments of Gold Basin is required.

Table 136

Cl concentrations (dpm/kg) in separated phases.
Gold BasinGaophasesfragment 1
fragment 2
bulk
10.9 ± 0.2
7.06 ± 0.14
9.95 ± 0.18
silicate
11.4 ± 0.2
5.47 ± 0.11
10.3 ± 0.2
metal2.49 ± 0.07
1.33 ± 0.04
7.46 ± 0.15
insoluble in nitric acid
2.01 ± 0.06
1.23 ± 0.04
4.80 ± 0.13
soluble in nitric acid -1
46.8 ± 0.7
22.5 ± 0.3
25.3 ± 0.6
soluble in nitric acid -2
0.96 ± 0.03
0.74 ± 0.03
3.52 ± 0.08
Table 2 Production rates of 36Cl in dpm/kgTarget.
Gold Basintarget element groupfragment 1
fragment 2
K + Ca50
14
Ti + Cr
27
20
Fe + Co + Ni + Mn
2.1
0.88
Cl
25
28
(K + Ca) / (Fe + Co + Ni + Mn)
23
16

Gao
88
71
7.6
28
12

References[1] M. Honda, K. Nishiizumi, M. Imamura, N. Takaoka, O. Nitoh, K. Horie, and K. Komura, Earth Planet.
Sci. Lett. 57 (1982) 101.
[2] Y. Oura, S. Yamazaki, M. Ebihara, Y. Tosaki, K. Sasa, Y. Nagashima, T. Takahashi, Y. Tosaki, Y.
Matsushi, M. Tamari, K. Sueki, H. Matsumura, K. Bessho, and T. Miura, UTTAC Annural Report 2006
(2007) 39.
[3] K. C. Welten, M. W. Caffee, I. Leya, J. Masarik, K. Nishiizumi, and R. Wieler, Meteorit. Planet. Sci.
38 (2003) 157.

28

4.5

Chemical procedure for sulfur reduction for 36Cl-AMS of soil
samplesM. Tamari, K. Sueki, K. Sasa, T. Takahashi, Y. Tosaki, Y. Matsushi, T. Oki, T. Amano, Y.
Nagashima, N. Kinoshita, H. Matsumura, K. Bessho
Introduction
Chlorine-36 is mainly measured through accelerator mass spectrometry (AMS), but 36S, an
isobar of 36Cl, interferes with the measurement. In surface soil, sulfur is mainly present as organic
sulfur [1]. When extract is added to the soil, not only an inorganic substance but also a part oforganic substance is extracted and the usual method of removing sulfate ions from samples—theBaSO4 precipitation method—is ineffective in removing extractable organic sulfur. We developed
new leaching procedures for removing the organic sulfur from the soil.
The sample for measurement of the isotope ratio (36Cl/Cl) in all chlorine can be obtained byburning and collecting whole soil as pre-treatment. By the measurement from inorganic chlorine
and organic chlorine, an inorganic substance was extracted from the soil at first, and it is attainedby making residue burning and taking out chlorine. A method is established that an inorganic
substance without sulfur is taken out from the soil and is measured by accelerator mass
spectrometry (AMS).
Examination of leaching procedure for soil
Two kinds of soil were used in this study. One was surface soil collected at the University ofTsukuba (Tsukuba soil), and was applied to examine the degree of interference of 36S after
different leaching processes. Another was uncultivated surface soil collected at Tokai-mura (Tokaisoil), and was applied to examine the 36Cl/Cl ratios after different leaching processes.
The leaching conditions for Cl are shown in Figure 1. Soil was dried up at 120°C, and wassieved to eliminate >2 mm-size particles. Extractant (ultrapure water, 0.01 M HNO3 or 0.8 M
HNO3 with 1.5-5 times the weight of the dried soil) was added to the soil. Then, in Tsukuba E, F
and Tokai L, 30% H2O2 was used to decompose the organic matter in soil (ratios of H2O2 to driedsoil: 15 ml/100 g, 170 ml/100 g, and 100 ml/100 g, respectively). Supernatant was separated fromthe soil by centrifugation. In Tokai I and K, 1-1.5 g of activated carbon (Calgon Mitsubishi
Chemical Corporation) was added to the supernatant in order to remove extractable organic
matters without decomposition. The organic matter in the solution was decomposed with 30%
H2O2 (10-30 ml) in each procedure except Tsukuba A, C, E and F. After leaching from soils, theAgCl samples for AMS-target made from the obtained solutions at ordinary treatment.

29

Figure 1. Leaching procedures for soil samples. (AC and Sup. mean activated carbon and supernatant.)(See [2] for more on Tsukuba C.)

Results and discussion

Table 1 Results of 36S-assay and 36Cl-AMS for soil samples

The results of 36S-assay and 36Cl-AMS are
shown in Table 1, as well as those of the standard
samples (36Cl/Cl = 1.000×10−11 [11]). The 36S-assay
36

Sample36S/35Cl

×102(counts/µC)

36S
×103
(cps)

36Cl/Cl
×10−13(atoms/atoms)

Tsukuba A*

-

> 6.6

-

shows the counts per second of S in the detector

Tsukuba B

2.2

1.4

1.07 ± 0.11

and the degree of interference of 36S indicated by

Tsukuba C

4.1

2.0

2.92 ± 0.50

Tsukuba D

0.5

0.4

0.94 ± 0.05

were counted because of large interference from 36S.

Tsukuba E

13.2

6.6

1.28 ± 0.20

Tsukuba F

0.5

0.4

1.08 ± 0.06

In the same extractant the addition of H2O2 to theTokai G

2.2

1.2

149 ± 4

sample (Tsukuba B, D) reduced the interference

Tokai H1.1

0.6

125 ± 1036

S/35Cl ratio. In Tsukuba A, neither 36Cl nor 36S

from 36S to lesser than that for the samples without

Tokai I0.3

0.2

145 ± 3

Tokai J1.7

0.2

129 ± 11

H2O2 (Tsukuba A, C). In Tsukuba E and F, theTokai K0.9

0.6

144 ± 15

extractant and H2O2 added directly in the soils, but

Tokai L2.0

1.0

79 ± 3STD†

0.07-1.6

0.06-1.4

in Tsukuba E in which too little H2O2 was used sothat the decomposition reaction was only half100

* Detection did not work because of a large interference of 36S.
† Standard for 36Cl-AMS (36Cl/Cl = 1.000×10−11)

completed, there was large 36S interference. The result was shown that the interference from 36S
reduced Tsukuba D and F by using diluted HNO3 as extractant, and H2O2 sequentially.
We examined the differences in the 36Cl/Cl ratios among the different leaching procedures in
Tokai soil, which had a 36Cl/Cl ratio of order 10−11. Within system error, the 36Cl/Cl ratios were
almost the same except for Tokai L, and that for Tokai L was about half of the others. However,
the ratios for Tokai H (J) seem slightly lower than for Tokai I (K). This suggests that the 36Cl/Cl
ratio for Tokai L became lower than those of the others due to the decomposition of the organic
chlorine. In other words, the 36Cl/Cl ratio for organic chlorine seems to be lower than that for
inorganic chlorine in Tokai soil.
References[1] G.E. Likens et al., Biogeochemistry 60 (2002) 235.
[2] R. Seki et al., Nucl. Instr. and Meth. B 259 (2007) 486.

30

5.
INTERDISCIPLINARY RESEARCH

5.1

Nucleation rate of nano-particles in N2/H2O/SO2 by 20 MeV protons

S. Tomita, M. Fujieda, M. Matsuoka, K. Terada, K. Sasa, H. Kudo
Formation mechanism of nano-particles in gas mixture of N2/H2O/SO2 at atmospheric pressure attract
attentions, because this might explain a possible correlation between the Earth's total low-altitude cloud
cover and galactic cosmic ray flux [1]. Under proton irradiation, H2SO4 is formed by oxidation reaction of
SO2 with OH radicals which produced by the energetic protons. The H2SO4 plays an important role innucleation process, and produces nano-partiles with diameter of about 8 nm.
In this report, we report nano-particle formation rate as a function of proton beam intensity. The
experiments were performed with a tandem accelerator (12UD Pelletron) at University of Tsukuba. The
size distribution of nano-particle was obtained by measuring the electrical mobility of charged particle
with a differential mobility analyzer. The density of produced nanoparticles was then obtained byintegrating the area under the spectrum. Figure 1 shows a typical result obtained for the sample gas 0.2
ppm SO2, 80% relative humidity. It is clearly seen that the droplet yield is proportional to the square rootof beam intensity. Since almost all of the ions produced by the proton beam is recombined and become
neutral, the resulted ion density becomes proportional to the square root of proton beam intensity.
Therefore, one can say that the droplet yield is proportional to the ion density generated by proton beam.
This shows possible importance of ions for the nucleation process. As written above, H2SO4 is important
for the nucleation process. Thus, ions might play important role in the oxidation mechanism or the

Droplet density (arb. unit)

nucleation process. Further investigations are planned to ensure the possibilities.
10
9
8
7
6
5
4
3
2

1
0.01

0.1

1

Beam intensity (nA)
Fig.1. Densities of generated water droplet as a function of proton beam intensities. The
sample gas was N2/H2O/SO2, with relative humidity of 80% and SO2 concentration of 0.2 ppm.
Solid line shows power of 0.5.
References[1] N.D. Marsh, and H. Svensmark, Phys. Rev. Lett. 85, 5004 (2000).

31

5.2

Open Advanced Facilities Initiative for Innovation (strategic use byindustry) at UTTAC

H. Kudo, Y. Tagishi, H. Naramoto, S. Mihara, T. Oki
In the fiscal years 2007-2008, UTTAC provided 20-25% of the available machine time for industrial
researches programmed by ~10 industries, which were supported by the Open Advanced Facilities
Initiative for Innovation conducted by The Japanese Ministry of Education, Culture, Sports, Science andTechnology (MEXT) [1]. The background of this program includes new mission required currently foruniversities in Japan, i.e., social contribution, in addition to the main mission of education andfundamental research.
The researches include ion beam analysis of materials, ion beam fabrications, ion irradiation
experiments, and material analysis using radioisotopes. The list of the research programs are shown in
Table 1, which were reviewed and accepted by the steering committee organized for the initiative. The
research results for the finished programs have been or are to be published in the home page of MEXT [2].
Table 1. List of the research programs
Research title： Industry

FY2007

FY2008FY2009FY2010Development of radiation detector for use on satellite: Meisei
Electric + JAXA
[Test exp.] Study of durability test for public-use semiconductor
devices using low-LET particle beams: Mitsubishi Electric + Ryoei
Technica
Development of high sensitivity sensors using nano perforation
with swift heavy ion irradiation: Emerging Technologies Corporation

finished
finished

Analysis of hydrogen in thin films： Optical instrument maker
Preliminary search for a raremetal deposit related withradioisoropes: Developer of mineral resources

finished[Test exp.] Analysis of impurities in semiconductor crystals: R&D
Association for Future Electron Devices

finished

Characterization of nonorganic films by high-energy ion beams:
general beverage makerMossbauer study of electron states of nanoparticles: Generalelectric maker
PIXE analysis of impurities in SiC: R&D Association for FutureElectron Devices

finished

Hydrogen analysis in electronic devices: Electronic device maker
Study of characterization technique for public-use semiconductor
devices using low-LET particle beams: Mitsubishi Electric + Ryoei
Technica

References[1] This report was published on June 15, 2009 (Vol. 5, No. 6) in the online journal, “Journal of IndustryAcademia-Government Collaboration” http://sangakukan.jp/journal/index.html, published (in Japanese)monthly by Japan Science and Technology Agency (JST).
[2] http://kyoyonavi.mext.go.jp/report/search

32

5.3

Micro-PIXE analyses of fluid inclusions in quartz from miarolitic
cavities at the Kofu granite, Japan

M. Kurosawa, S. Ishii and K. Sasa
Introduction
Fluid released from granitic magma during solidification plays a key role in many geologicalevents related to hydrothermal process. Compositions of the granite-derived fluid are commonly
approximated by the H2O–CO2–NaCl system, and the fluid also has wide varieties of other elemental
species and concentration range [1]. Thus, it is essential to formation of various metal-ore deposits,hydrothermal alteration, and chemistries of deep groundwater inside and around granite bodies [1]. A partof the fluid is normally trapped as fluid inclusions in the solidified granite and surrounding rocks.
Chemical analyses of the inclusions, therefore, provide abundant information about chemistries andbehaviors of the fluid. Fluid inclusions in minerals from miarolitic cavities inside granite are particularly
important to investigate an original composition of fluids released during solidification of the granite.
Because miarolitic cavities are commonly formed by entrapment of fluid segregated by vesiculation of
granite magma during the final stage of crystallization of the granite. Hence, fluid inclusions of quartz
crystals in miarolitic cavities from granites at the continental area have been analyzed by particle-induced
X-ray emission (PIXE) and laser ablation-inductively coupled plasma-mass spectrometry [2-5]. The
analytical results for the island-arc granite, however, are very scarce. For these reasons, we describe
micro-PIXE analyses of single fluid inclusions in quartz crystals from miarolitic cavities at the Kofu
granite, Japan.
SampleMiarolitic cavities are common in biotite granite of
the Miocene Kofu granite body near Kurobera district, Kofu,

Fluid inclusions

Yamanashi Prefecture. Localities of four cavities used in thisstudy are very close, a distance of less than 3 km. These
cavities are a few to tens cm in diameter, consists of smoky
quartz, microcline, albite, muscovite, and a small amount ofschorl. They are sometimes accompanied by small amounts
of topaz, zinnwaldite, beryl, monazite-(Ce), and cassiterite.
Smoky euhedral quartz crystals were collected from thesemiarolitic cavities for the inclusion analyses. Fluid inclusions
in the quartz samples are two-phase inclusions, 70–120 m insize (Fig. 1). The homogenization temperatures range fromabout 380 to 280 C and have a peak around 350 C. Measured
inclusions were an ellipsoidal or negative-crystal shape, andthe inclusion depths were less than 10 m.

33

Fig.1. Photomicrograph of fluidinclusions in quartz crystal from amiarolitic cavity at the Kofu granite,
Japan. Large bubbles are present in
the inclusions. Scale bar is a 100 m.

Experimental

Proton beam

X-ray
45

inclusion depth

matrix
o

l

X

t

Y
Z

1MV Tandetron. A 1.0 to 5.0 nA beam of 1.92-MeV
proton was focused to a 100 x 100

m spot on thesample using slits and magnetic lenses. The beamincidence was normal to the sample surface, and the(x,y,z)w

The PIXE analyses were performed at the

Fluid
inclusion

Fig.2. Schematic geometry for PIXE analysis
of fluid inclusion.

X-ray measurement take-off angle was 45˚[6]. The
characteristic X-rays excited by the incident beam werecollected by the Si(Li) X-ray-energy detector (GreshamCo.) with a nominal resolution of 153 eV at 5.9 keV. A
55- m-thick Mylar film was used to attenuate theintense X-rays from the predominant light elements andto prevent the entry into the detector of protons scatteredfrom samples. The total charge was determined by integrating the target currents, and all samples wereanalyzed to the integrated charges of 0.5 to 5.0 C. Analytical points were chosen based on opticalviewing using a CCD camera mounted on the microscope [6]. Quantification was performed based on themodel of Kurosawa et al. [7,8]. Intensities of X-rays generated from fluid inclusions are decreased by theattenuation of energy of the incident protons and the absorption of the X-rays by a quartz matrix and thefluid, because fluid inclusions are buried in the matrix (Fig. 2). In this model, the decrease of total X-ray
intensities from a whole fluid-inclusion are calculated by considering sizes and depth of fluid inclusion,
the major element composition, the densities of the matrix and the fluid, their proton-stopping powers, the
X-ray production cross sections, and the X-ray absorption coefficients. Finally, element concentrations arecalculated based on X-ray intensities corrected for the decrease and the detector sensitivity determined foreach element. A shape of the fluid inclusion is assumed as an ellipsoidal equal to the size of the measured
fluid inclusion. The inclusion sizes were determined with an optical microscope. The inclusion depths
were exactly determined by measuring an intensity ratio of Cl K and Cl K . In the calculations,contributions of X-rays from impurities in the matrix and bubbles in the fluid inclusion were also
corrected [7,8]. By using the calculation model, almost trace elements in fluid inclusions at levels of a few
to several thousands ppm can be determined with the total analytical error of 11- 40 % [7].
Results and Discussion
PIXE spectra of a fluid inclusion in the miarolitic cavities consisted of K X-ray peaks from Cl, K,
Ca, Mn, Fe, Cu, Zn, Ge, Br, and Rb, and of L X-ray peaks from Pb and Ba (Fig. 3). Most of inclusions in
the miarolitic cavities demonstrated the similar X-ray spectra. The element concentrations determined
were several tens to hundreds of wt. ppm for Mn, Fe, Cu, Zn, Rb, Ge, Ba, and Pb. For the inclusions,calculated salinities range from about 8 to 17 wt.% NaCl equivalent: they were calculated based on theassumption that all the chlorine contents are originated from NaCl components. The fluid inclusions of the
miarolitic cavities are divided into two types: low-content type with tens of ppm for the most34

transition-metal elements and high-content
types with hundreds of ppm for those.

10

4

10

3

Si

Cl

K

cavities

basically

contained

inclusions of the one type, both type ofinclusions were rarely observed in the same
crystals of the particular cavity. Compositions
of

all

the

inclusions

showedIntensity (cts)Although a quartz crystal in the single
miarolitic

Fluid inclusions(PIXE: 1.92 MeV)

Ca

Mn
Fe
Ba
Zn

10

2

Cu
Ge

positive10

correlations between Mn and Fe, Zn and Fe,

5and Zn concentrations. The interelement

the compositional difference in both types of

Rb

Sr

10

15

Energy (keV)

ratios (e.g., Mn/Fe and Ge/Zn) of the bothlevel well within the analytical error. Thus,Br

1

Zn and Cu, Ge and Zn, Ba and Zn, and Pb

type of inclusions are nearly constant at aPb

Fig.3. PIXE spectrum of fluid inclusion in quartz
crystal from miarolitic cavity at the Kofu granite,
Japan.

inclusions could not be due to inflow ofdifferent magmatic fluids but due to dilution of magmatic fluids by meteoritic waters during formation of
the miarolitic cavities. Fluid inclusions in single quartz crystals from miarolitic cavities at the continental
area have often demonstrated extreme variations in elemental concentration, ranging over several orders ofmagnitude [2-5]. These variations suggest chemical diversity of magmatic fluids during granite
solidification. Lack of the extreme variations for the present samples indicates that an original fluid
generated during the granite solidification could be formed by relatively simple processes, unmixing of
fluids from granitic magma and the dilution by meteoritic water. Further chemical variation of the fluid
would be caused by secondary processes during and after transport of the fluid inside the granite body.
References[1] E. Roedder, Rev. Mineral., 14, "Fluid Inclusions" (1984)[2] A. Audétat et al., Science, 279 (1998) 2091.
[3] A. Audétat et al., Econ. Geol., 95 (2000) 1563.
[4] V. S. Kamenetsky et al., Geology, 30 (2002), 459.
[5] V. S. Kamenetsky et al., Chem. Geol., 210 (2004), 73.
[6] M. Kurosawa et al., Nucl. Instr. and Meth. B142 (1998), 599.
[7] M. Kurosawa et al., Geochim. Cosmochim. Acta, 67 (2003), 4337.
[8] M. Kurosawa et al., Nucl. Instr. and Meth. B266 (2008), 3633.

35

36

6. LIST OF PUBLICATIONS
The publications listed here are those released in the fiscal year 2008 by all the workers listed on p.46.

6.1 Journals
NUCLEAR PHYSICS
1. T. Yamaguchi, T. Suzuki, T. Ohnishi, F. Becker, M. Fukuda, H. Geissel, M. Hosoi, R. Janik,
K. Kimura, T. Kuboki, S. Mandel, M. Matsuo, G. Münzenberg, S. Nakajima, T. Ohtsubo, A.
Ozawa, A. Prochazka, M. Shindo, B. Sitár, P. Strmeň, T. Suda, K. Sümmerer, K. Sugawara,
I. Szarka, M. Takechi, A. Takisawa, K. Tanaka, and M. Yamagami, Nuclear matter radii ofneutron-deficient Kr isotopes, Physical Review C 77, 034315 (2008).
2. Tetsuya Ohnichi, Toshiyuki Kubo , Kensuke Kusaka, Atsushi Yoshida, Koichi Yoshida, Naoki
Fukuda, Masao Ohtake, Yoshiyuki Yagagisawa, Hiroyuki Takeda, Daisuke Kameda, Yoshitaka
Yamaguchi, Nori Aoi, Ken- ichiro Yoneda, Hideaki Otsu, Satoshi Takeuchi, Takashi Sugimoto,
Yosuke Kondo, Heiko Scheit, Yasuyuki Gono, Hiroyoshi Sakurai, Tohru Motobayashi, Hiroshi Suzuki, Taro Nakao, Hitomi Kimura, Yutaka Mizoi, Masafumi Matsushita, Kazuo Ieki,
Takamasa Kuboki, Takayuki Yamaguchi, Takeshi Suzuki, Akira Ozawa, Tetsuaki Moriguchi,
Yusuke Yasuda, Takashi Nakamura, Takashi Nannichi, Tomoyuki Shimamura, Yoshiaki Nakayama,
Hans Geissel, Helmut Weick, Jerry A. Nolen, Oleg B. Tarasov, Anthony S. Nettleton, Daniel
P. Bazin, Bradley M. Sherrill, David J. Morrissey, and Wolfgang Mittig, Identification of New
Isotopes 125 Pd and 126 Pd Produced by In-Flight Fission of 345 MeV/nucleon 238 U: First Results from the RIKEN RI Beam Factory, Journal of the Physical Society of Japan, Vol. 77, No.
8, August, (2008) 083201.
3. Y.Yamaguchi, A.Ozawa, A.Goto, I.Arai, T.Fujinawa, N.Fukunishi, T.Kikuchi, T.Ohnishi, T.Ohtsubo,
H.Sakurai, T.Suzuki, M.Wakasugi, T.Yamaguchi, Y.Yasuda, Y.Yano, Rare-RI ring project at
RIKEN RI beam factory, Nuclear Instruments and Methods in Physics Research B 266, 45754578 (2008).
4. S.Nakajima, T.Kuboki, M.Yoshitake, Y.Hashizume, M.Kanazawa, A.Kitagawa, K.Kobayashi,
T.Moriguchi, T.Ohtsubo, A.Ozawa, S.Sato, T.Suzuki, Y.Yamaguchi, Y.Yasuda. T.Yamaguchi,
Development of a time-of-flight detector for the Rare-RI Ring project at RIKEN, Nuclear Instruments and Methods in Physics Research B 266, 4621-4624 (2008).
5. B.Sun, R.Knöbel, Yu.A.Litvinov, H.Geissel, J.Meng, K.Beckert, F.Bosch, D.Boutin, C.Brandau,
L.Chen, I.J.Cullen, C.Dimopoulou, B.Fabian, M.Hausmann, C.Kozhuharov, S.A.Litvinov, M.Mazzocco,
F.Montes, G.Münzenberg, A.Musumarra, S.Nakajima, C.Nociforo, F.Nolden, T.Ohtsubo, A.Ozawa,
Z.Patyk, W.R.Plaβ , C.Scheidenberger, M.Steck, T.Suzuki, P.M.Walker, H.Weick, N.Winckler,
M.Winkler, T.Yamaguchi, Nuclear structure studies of short-lived neutron-rich nuclei with the37novel large-scale isochronous mass spectrometry at the FRS-ESR facility, Nuclear Physics A
812 (2008) 1-12
6. A.Ozawa, D.Q.Fang, M.Fukuda, N.Iwasa, T.Izumikawa, H.Jeppesen, R.Kanungo, R.Koyama,
T.Ohnishi, T.Ohtsubo, W.Shinozaki, T.Suda, T.Suzuki, M.Takahashi, I.Tanihata, C.Wu, Y.Yamaguchi,
Measurement of the reaction cross section of 18C and observations of fragments from 17 C and
18 C at 80 AMeV, Physical Review C 78, 054313 (2008).

7. C.B. Moon, C.S. Lee, M. Oshima, Y. Toh, J. Goto, Y. Hatsukawa, A. Kimura, M. Koizumi, A.
Osa, T. Komatsubara, K. Miyakawa, Multi-quasiparticle states in odd-odd I-118, Journal of the
Korean Physical Society, Vol. 53, No. 4, October (2008) 1844-1847
8. T. Shizuma, T. Hayakawa, H. Ohgaki, H. Toyokawa, T. Komatsubara, N. Kikuzawa, A. Tamii,
H. Nakada, Fine structure of the magnetic-dipole-strength distribution in Pb-208, Phys. Rev. C
78, 061303, Dec (2008)

MATERIALS AND CLUSTER SCIENCE

9. Eiji Kita, H. Yanagihara, S. Hashimoto, K. Yamada, T. Oda, M. Kishimoto, and A. Tasaki,
Hysteresis Power-Loss Heating of Ferromagnetic Nanoparticles Designed for Magnetic Thermoablation, IEEE Trans MAG, MAG44 No.11 part2, pp. 4452-4455 (2008).
10. Takahiro Kondo, Ken-ichi Izumi, Kenji Watahiki, Yosuke Iwasaki, Tetsuya Suzuki and Junji
Nakamura, Promoted catalytic activity of a Platinum monolayer cluster on Graphite, Journal of
Physical Chemistry C, Vol. 112, 15607-15610, 2008
11. JunePyo Oh, Takahiro Kondo, Daigo Hatake and Junji Nakamura, Elastic and inelastic scattering components in the angular intensity distribution of He scattered from graphite, Surface
Science, Vol. 603, 894-899, 2009
12. H. Sano M. Miyaoka, T. Iimori, D. Sekiba, K. Nakatsuji, W. Wolf, R. Podloucky, N. Kawamura, G. Mizutani, F. Komori, Enhancement of optical second harmonic generation bynitrogen
adsorption on Cu(001), Appl. Surf. Sci.255, (2008) 3289-3293.
13. Kan Nakatsuji, Yoshihide Yoshimoto, Daiichiro Sekiba, Shunsuke Doi, Takushi Iimori, Kazuma
Yagyu, Yasumasa Takagi, Shin-ya Ohno, Hideharu Miyaoka, Masamichi Yamada, Fumio Komori, Kenta Amemiya, Daiju Matsumura, and Toshiaki Ohta, Electron correlation effects in Co
nanoscale islands on a nitrogen-covered Cu(001) surface, Phys. Rev. B 77 (2008) 235436-1-8.
14. Kan Nakatsuji, Takushi Iimori, Yasumasa Takagi, Daiichiro Sekiba, Shunsuke Doi, Masamichi
Yamada, Taichi Okuda, Ayumi Harasawa, Toyohiko Kinoshita, Fumio Komori, Surface restructuring process on a Ag/Ge(0 0 1) surface studied by photoelectron spectroscopy, Applied
Surface Science, 254 (2008) 7638-7641.

38

15. D. Sekiba, H. Yonemura, T. Nebiki, M. Wilde, S. Ogura, H. Yamashita, M. Matsumoto, J.
Kasagi, Y. Iwamura, T. Itoh, H. Matsuzaki, T. Narusawa, K. Fukutani, Development of microbeam NRA for 3D-mapping of hydrogen distribution in solids: Application of tapered glass
capillary to 6 MeV 15N ion, Nuclear Instruments and Methods in Physics Research Section B:
Beam Interactions with Materials and Atoms, Volume 266 (2008) 4027-4036.
16. T. Nebiki, D. Sekiba, H. Yonemura, M. Wilde, S. Ogura, H. Yamashita, M. Matsumoto, K.
Fukutani, T. Okano, J. Kasagi, Y. Iwamura, T. Itoh, S. Kuribayashi, H. Matsuzaki, T. Narusawa, Taper angle dependence of the focusing effect of high energy heavy ion beams by glass
capillaries, Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, 266 (2008) 1324-1327.
17. D. Sekiba, Y. Yoshimoto, K. Nakatsuji, F. Komori, Lattice strain and related phenomena on
Metal Surfaces (in Japanese), Journal of the Vacuum Society of Japan, 51 (2008) 285.
18. A. Uedono, C. Shaogiang, S. Jongwon, K. Ito, H. Nakamori, N. Honda, S. Tomita, K. Akimoto,H. Kudo, and S. Ishibashi, Vacancy-type defects in Er-doped GaN studied by a monoenergetic
positron beam, J. Appl. Phys. 103, (2008) 104505 (1-5)
19. Masataka Ohkubo, Masahiro Ukibe, Yiner Chen, Shigetomo Shiki, Yuki Sato, Shigeo Tomita,
Shigeo Hayakawa, Superconducting Solid-State Particle Spectrometers for Atoms and Macromolecules of 3-20 keV, J. Low. Temp. Phys. 151, (2008) 760-765
20. S. Shiki, M. Ukibe, Y. Sato, S. Tomita, S. Hayakawa, M. Ohkubo, Kinetic-energy-sensitive
mass spectrometry for separation of different ions with the same m/z value, J. Mass Spectro.
43, (2008) 1686-1691
21. S. Shiki, M. Ukibe, R. Maeda, M. Ohkubo, Y. Sato, S. Tomita, Energy resolution improvement of superconducting tunnel junction particle detectors with infrared-blocking filters, Nucl.
Instrum. and Methods A-595, (2008) 391-394

ACCELERATOR MASS SPECTROMETRY

22. M. Hoshi, S. Endo, K. Tanaka, M. Ishikawa, T. Straume, K. Komura, W. Rühm, E. Nolte, T.
Huber, Y. Nagashima, R. Seki, K. Sasa, K. Sueki, H. Fukushima, S. D. Egbert and T. Imanaka,
Intercomparison study on 152 Eu gamma ray and 36 Cl AMS measurements for development of
the new Hiroshima-Nagasaki Atomic Bomb Dosimetry System 2002 (DS02), Radiation andEnvironmental Biophysics, 47 (2008) 313-322.

INTERDISCIPLINARY RESEARCH

39

23. S.C.B. Gopinath, K. Awazu, M. Fujimaki, K. Sugimoto, Y. Ohki, T. Komatsubara, J. Tominaga,
K.C. Gupta, P.K.R. Kumar, Influence of nanometric holes on the sensitivity of a waveguidemode sensor: Label-free nanosensor for the analysis of RNA aptamer-ligand interactions, Analytical Chemistry, Vol. 80, Sep (2008), 6602-6609
24. M. Fujimaki, C. Rockstuhl, X.M. Wang, K. Awazu, J. Tominaga, Y. Koganezawa, Y. Ohki,
T. Komatsubara, Silica-based monolithic sensing plates for waveguide-mode sensors, Optics
Express, Vol. 16, 6408-6416, Apr (2008)
25. T. Komatsubara, K. Sasa, H. Ohshima, H. Kimura, Y. Tajima, T. Takahashi, S. Ishii, Y. Yamato,
M. Kurosawa, Hydrogen analysis for granite using proton-proton elastic recoil coincidence
spectrometry, Radiation and Environmental Biophysics 47 (2008) 337-342
26. K. Awazu, X. Wang, M. Fujimaki, J. Tominaga, H. Aiba, Y. Ohki, T. Komatsubara, Elongationof gold nanoparticles in silica glass by irradiation with swift heavy ions, Phys. Rev. B 78,
054102 (2008)
27. I. Sugai, Y. Takeda, M. Oyaizu, H. Kawakami, K.Sasa, S. Ishii, K. Shima, First results of target
preparation by the HIVIPP method in pressures higher than one bar, Nuclear Instruments andMethods in Physics Research A, 590 (2008) 83-90.
28. Masanori Kurosawa, Satoshi Ishii and Kimikazu Sasa, Quantitative PIXE analyses of single
fluid inclusions in quartz crystals with a 1.92-MeV tandetron, Nuclear Instruments and Methods
in Physics Research B, 266 (2008) 3633-3642.
29. Seung-Jun Yu, Yoshimichi Ohki, Makoto Fujimaki, Koichi Awazu, Junji Tominaga, Kimikazu
Sasa and Tetsuro Komatsubara, Reduction in Polarization Dependent Loss of a Planar Lightwave Circuit by Ion-implantation-induced Birefringence, Nuclear Instruments and Methods inPhysics Research B, 266 (2008) 4762-4765.

40

6.2 International conferences

1. Junji Nakamura, Takahiro Kondo, Ken-ichi Izumi, Kenji Watahiki, Yosuke Iwasaki, June Pyo
Oh, Daiichiro Sekiba, Hiroshi Kudo, Catalytic property and morphology of Pt clusters on thegraphite surface, The 5th International Symposium on Surface Science and Nanotechnology(ISSS-5), Waseda (Tokyo) 9-13, November, 2008.
2. D. Sekiba, H. Yonemura, Y. Kitaoka, M. Matsumoto, Y. Iwamura, T. Itoh, H. Matsuzaki, T.
Narusawa, K. Fukutani, In-situ NRA measurement of hydrogen uptake in palladium foil, 4th
Vacuum and Surface Sciences Conference of Asia and Australia, Matsue (Japan) 28-31 October, 2008.
3. Takahiro Kondo, Kenji Watahiki, June Pyo Oh, Ken-ichi Izumi, Yosuke Iwasaki, Daiichiro
Sekiba, Hiroshi Kudo and Junji Nakamura, Catalytic Activity and Morphology of Pt Clusters on
the Graphite Surface, American Vacuum Society (AVS) 55th International Symposium, Boston(United States) 19-24, October, 2008.
4. June Pyo Oh, Takahiro Kondo, Yoshiyuki Suda, Daiichiro Sekiba, Hiroshi Kudo and Junji
Nakamura, Significant Reduction in Adsorption Energy of CO on Platinum Nanoparticles on
Graphite, American Vacuum Society (AVS) 55th International Symposium, Boston (UnitedStates) 19-24, October, 2008.
5. Takahiro Kondo, Ken-ichi Izumi, Kenji Watahiki, June Pyo Oh, Daiichiro Sekiba, Hiroshi Kudo
and Junji Nakamura, Catalytic property and morphology of Pt clusters on the graphite surface,
25th European Conference on Surface Science, Liverpool (United Kingdom) 8-12, July, 2008.
6. Takahiro Kondo, Ken-ichi Izumi, Kenji Watahiki, June Pyo Oh, Daiichiro Sekiba, Hiroshi Kudo
and Junji Nakamura, Promoted Catalytic Activity of a Platinum Monolayer Cluster on Graphite,
Pre-Symposium of 14th International Congress on Catalysis (ICC 14), Kyoto (Japan) 8-12,
July, 2008.
7. Norikazu Kinoshita, Hiroshi Matsumura, Kotaro Bessho, Akihiro Toyoda, Kazuyoshi Masumoto, Yuki Matsushi, Kimikazu Sasa, Tsutomu Takahashi, Shozo Mihara, Toshiyuki Oki,
Masumi Matsumura, Yuki Tosaki, Keisuke Sueki, Michiko Tamari, Yasuo Nagashima, Depth
profile of radioactivity induced in the thick concrete shield in EP-1 beam line at the 12-GeV
proton synchrotron facility, KEK. The 11th International Conference on Radiation Shielding(ICRS-11), April 13-18, 2008, Callaway Gardens, Pine Mountain, Georgia, USA.
8. Yuki TOSAKI, Norio TASE, Kimikazu SASA, Tsutomu TAKAHASHI, Yasuo NAGASHIMA,
Estimation of groundwater residence time using bomb-produced 36 Cl: a case study on springwaters from Mt. Fuji, Japan, the 36th the International Association of Hydrogeologists (IAH)
Congress 2008, ”Integrating groundwater science and human well-being, 26 Oct. - 1 Nov.
2008, Toyama, Japan.

41

9. Kimikazu Sasa, Yuki Matsushi, Yuki Tosaki, Michiko Tamari, Tsutomu Takahashi, Keisuke
Sueki, Shozo Mihara, Toshiyuki Oki, Yasuo Nagashima, Hiroshi Matsumura, Norikazu Kinoshita, Kotaro Bessho, Kazuho Horiuchi, Hiroyuki Matsuzaki, Yasuyuki Shibata, Motohiro
Hirabayashi and Hideaki Motoyama, Cosmogenic nuclide 36 Cl measurements in the Dome
Fuji ice core, Antarctica, The 11th International Conference on Accelerator Mass Spectrometry (AMS11), Rome, Italy, 14th to 19th September, 2008.
10. Kimikazu Sasa, Tsutomu Takahashi, Yuki Tosaki, Michiko Tamari, Keisuke Sueki, Toshiyuki
Oki, Shozo Mihara, Yoshihiro Yamato, Yasuo Nagashima, Hiroshi Matsumura, Kotaro Bessho,
Norikazu Kinoshita, Yuki Matsushi, Status and research programs of the multi-nuclide AMS
system at the University of Tsukuba The 11th International Conference on Accelerator Mass
Spectrometry (AMS11), Rome, Italy, 14th to 19th September, 2008.
11. Yuki Matsushi, Kimikazu Sasa, Tsutomu Takahashi, Keisuke Sueki, Yasuo Nagashima, Yukinori Matsukura, Chlorine-36 in calcite: denudation rates of karst landform in Japan, The 11th
International Conference on Accelerator Mass Spectrometry (AMS11), Rome, Italy, 14th to19th September, 2008.
12. Yuki Tosaki, Gudrun Massmann, Norio Tase, Kimikazu Sasa, Tsutomu Takahashi, Yuki Matsushi, Michiko Tamari, Yasuo Nagashima, Kotaro Bessho, Hiroshi Matsumura, Distribution of
36 Cl in groundwater: an attempt to estimate local fallout of bomb-produced 36 Cl, The 11th In-

ternational Conference on Accelerator Mass Spectrometry (AMS11), Rome, Italy, 14th to 19th
September, 2008.
13. Michiko Tamari, Keisuke Sueki, Yuki Tosaki, Yuki Matsushi, Toshiyuki Oki, Shozo Mihara,
Norikazu Kinoshita, Hiroshi Matsumura, Kotaro Bessho, Tsutomu Takahashi, Kimikazu Sasa,
Yasuo Nagashima, Chemical procedure of sulfur reduction for 36 Cl-AMS: A case of soil samples, The 11th International Conference on Accelerator Mass Spectrometry (AMS11), Rome,
Italy, 14th to 19th September, 2008.
14. Silke Merchel, Wolfram Bremser, Vasily Alfimov, Maurice Arnold, Georges Aumatre, Lucilla Benedetti, Didier L. Bourl‘es, Régis Braucher, Marc Caffee, Marcus Christl, L.Keith Fifield, Robert C. Finkel1, Stewart P.H.T. Freeman, Aarón Ruiz Gómez, Peter W. Kubik, Dylan H. Rood, Kimikazu Sasa, Peter Steier, Steve G. Tims, Anton Wallner, Klaus M. Wilcken,
and Sheng Xu, Be-10 and Cl-36 interlaboratory comparisons, Annual Meeting of the DPG(DPG=German Physical Society) and DPG Spring Meeting of the Section AMOP, Hamburg,
Germany from 2nd - 6th of March 2009.

42

7. THESES

Ph. D. Theses
Yuki Tosaki

Estimation of groundwater residence time using bomb-produced chlorine-36

M. Sc. Theses
Michiko Tamari

Analysis of long-life radionuclide Cl-36 in the soil by AMS

Mitsuteru Fujieda

Formation of condensation nuclei under proton irradiation

Masakuni Murakami

Precise measurement of energy losses of fast carbon clusters

Yuki Sato

Development of electrostatic ion beam trap43

8. SEMINARS
Title and Speaker

Date
2009
Jan

28

Study of Physics Performance of Transition Radiation Detector and D/B Mesons
Identification Capability at LHC-ALICE Experiment
M. Sano (Univ. of Tsukuba)
Determinations of Reaction Plane and Back-to-Back Jet Axis at LHC- ALICE Experiment
D. Sakata (Univ. of Tsukuba)

Mar

18

ANSTO AMS Facility and recent applications
Quan Hua (ANSTO)

Mar

26

LHCf experiments and high energy cosmic rays
T. Sako (Univ. of Nagoya)

Mar

26

Ions in the atmosphere - a link between the Sun and Earth’s climate?
Jens Olaf Pepke Pedersen (National Space Institute, Danish Technical University)

44

9.

SYMPOSIUM
Annual meeting of UTTAC users
Ion-beam based interdisciplinary studies
16 March, 2009
Laboratory of Advanced Research B 0110
1. Opening : H. Kudo (Uinv. of Tsukuba)
2. Fabrication of ZnO nanoparticles by ion implantation and thermal oxidation : H. Amekura(NIMS)
3. Sharpening of gold nanoparticles in SiO2 by bombardment of ion beam and the mechanism K.
Awazu (AIST)
4. RBS study on degradation mechanism of swichable mirrors : D. Sekiba (Univ. of Tsukuba)
5. In situ observation of hydrogen by nuclear reaction analysis : K. Fukutani (Tokyo Univ.)
6. Applications of AMS for geoenvironmental science and Antarctic ice core : K. Sasa (Univ. of
Tsukuba)
7. Analysis of radionuclide Cl-36 in the soil by AMS : K. Sueki (Univ. of Tsukuba)
8. Trace element analyses of fluid inclusions in quartz crystals from Tsushima granite with shallower emplacement level : M. Kurosawa (Univ. of Tsukuba)
9. Droplet formation in N2 /H2 O/SO2 by proton beam irradiation : S. Tomita (Univ. of Tsukuba)

10. Application of NMR using unstable nuclei to the study of nuclear moments and material science: M. Mihara (Osaka Univ.)
11. Physics of unstable nuclei in UTTAC : A. Ozawa (Univ. of Tsukuba)
12. Study of nucleosynthesis by gamma-ray spectroscopy : T. Komatsubara (Univ. of Tsukuba)

45

10. LIST OF PERSONNEL
Tandem Accelerator Complex
H. KudoT. Komatsubara
K. Sasa
D. Sekiba
S. Ishii
H. Kimura
H. Oshima
Y. Tajima
T. Takahashi
Y. Yamato
Y. Tagishi
H. Naramoto
S. Mihara
T. OkiM. MoroDirector, Professor
Assistant Professor
Assistant Professor
Assistant Professor
Mechanical Engineer
Computer Engineer
Electric Engineer
Mechanical Engineer
Electric Engineer
Electric Engineer
Research Coordinator
Research Coordinator
Research Fellow
Research Fellow
Administrative Stuff

Steering Committee
H. KudoA. Ozawa

Y. Miake
T. Komatsubara

T. Sakae
K. Sasa

K. Matsukura
D. Sekiba

K. Murakami

T. Komatsubara

M. Onoda

A. Ozawa

K. Sasa

E. Kita
H. Yanagihara

H. KudoT. Suemasu

Research Members 1
Inst. of Physics
I. Arai
Y. YasudaInst. of Applied Physics
S. AokiK. Akimoto
S. Tomita
A. UedonoInst. of Materials Science
T. Kondo

J. Nakamura

Inst. of Engineering Mechanics and Systems
K. Matsuuchi
Inst. of Geoscience
M. Kurosawa

N. TaseY. Tosaki

1 The ”research members” include the authors and coauthors within 5 years back from this fiscal year, as well as themembers of research projects runnning at UTTAC.

46

Inst. of Chemistry
K. Sueki

Graduate students
Doctoral Programs of Pure and Applied Science
M. Iijima
Y. Ikeda
K. MikiR. Tanabe
K. Watanabe
K. Yamaguchi

T. Moriguchi

M. Shimomura

Master’s Programs of Pure and Applied Science
M. Fujieda
E. Hamada
M. Horikoshi
M. Kajigaya
M. Kimura
M. Matsuoka
H. Nakamori
K. Ogawa
A. Oonishi
Y. SatoK. Shiba
N. Shiobara
H. Yokoyama

T. Ikuyama
M. Minakawa
D. Sakata
M. TamariY. ItoM. Murakami
M. SanoT. Todoroki

T. Kayano
T. Takeuchi

N. Kurihara
K. Terada

Undergraduates
S. AbeH. Ooishi
T. Watanabe

T. Amano
H. SatakeY. Ishibashi
Y. Sekine47

Scientific Guests and Fellows
K. Awazu
M. Fujimaki
S.J. Yu
K. Sugimoto
K. Nomura
A. Maeda
S. Fujii
T. KatoK. SatoY. Matsushi
H. Muramatsu
K. Bessho
K. Masumoto
N. Kinoshita
T. Miura
T. Hayakawa
T. Shizuma
H. Matsumoto
T. Komiyama
Y. Sasaki
Y. Terakado
M. Nakazawa
M. Kusakabe
M. Tomitaka
H. Yamaguchi
T. Ooyanagi
Y. Ohura
H. Hashizume
Y. Hamanaka
S. Kubono
S. Hayakawa
D. Kahl
D.N. Binh
A. ChenJ. ChenK. HaraAIST
AIST
Waseda Univ.
Waseda Univ.
Waseda Univ.
Waseda Univ.
Waseda Univ.
Waseda Univ.
Waseda Univ.
Tokyo Univ.
KEK
KEK
KEK
KEK
KEK
JAEA
JAEA
JAXA
JAXA
JAXA
Meisei Denki
Meisei Denki
Meisei Denki
Meisei Denki
AIST
AIST
Tokyo Metropolitan Univ.
Tokyo Metropolitan Univ.
Tokyo Metropolitan Univ.
CNS
CNS
CNS
CNS
McMaster Univ.
McMaster Univ.
RIKEN

48