Applied Radiation and Isotopes 64 (2006) 11301135

A low-level activation technique for monitoring thermonuclear fusion

plasma conditions
Joe l Gasparro
a
, Mikael Hult
a,
, Georges Bonheure
b
, Peter N. Johnston
c
a
EC-JRC-IRMM, Institute for Reference Materials and Measurements, Retieseweg 111, B-2440 Geel, Belgium
b
Laboratory for Plasma Physics, Association Euratom-Belgian State, Royal Military Academy, Avenue de la Renaissance, 30,
Kunstherlevinglaan, B-1000 Brussels, Belgium
c
Applied Physics, Royal Melbourne Institute of Technology, GPO Box 2476V, Melbourne 3001, Australia
Abstract
Optimisation of the connement and sustainability of a thermonuclear plasma requires methods to monitor processes in the plasma. In
this work three materials were used as activation targets (Ti, MgF
2
and a TiVAl compound). They were placed inside the joint European
Torus (JET) vacuum chamber. Certain gamma-ray emitting radionuclides (
7
Be,
54
Mn,
56
Co,
57
Co,
58
Co and
46
Sc) were measured using
ultra low-level gamma-ray spectrometry in an underground laboratory 12 months after activation. They were found to arise from
neutron activation of bulk sample material and surface contaminants sputtered from other Tokamak parts. Decision thresholds for some
activation products were determined in order to aid in giving upper bounds for the ux of charged particles.
r 2006 Elsevier Ltd. All rights reserved.
Keywords: Ultra low-level gamma-ray spectrometry; Thermonuclear fusion; Underground laboratory; Charged particles; Activation
1. Introduction
The work on understanding and controlling thermo-
nuclear plasma has made considerable progress over the
past 40 years (Tuong Hoang and Jacquinot, 2004). In order
to further improve the containment of the thermonuclear
plasma it is important to have more and better information
on the characteristics of the plasma. Of particular interest
is the measurement of the neutron energy distribution as
well as the measurement of the leakage of charged
particles. In order to improve computer codes describing
the plasma, improved knowledge of the particle uxes and
leakage is needed. The approach by Bonheure and co-
workers (Bonheure et al., 2003) was to insert an activation
probe into the vacuum chamber. The main idea is that
charged particles leaking from the plasma would interact
with the target material and activate it. The activation
products would later be measured using e.g. gamma-ray
spectrometry. The charged particle activation cross sec-
tions are normally much lower than e.g. the capture cross
sections of thermal neutrons. This means that the resulting
activities are very low. Having in mind that the samples are
fairly small one can conclude that the measurements of the
long lived gamma-ray emitting reaction products (half-life
longer than a few days) are best performed using ultra low-
level gamma-ray spectrometry (ULGS) (Hult et al., 2006).
Activated high purity samples with very low impurity levels
are highly suited for ULGS. The reason for this is that the
background from the sample itself can be very low since
there is no contribution from primordial radionuclides or
other impurities.
2. Materials and methods
2.1. Samples and samples activation
There are quite severe restrictions to which materials can
be placed inside the JET vacuum chamber. The materials
have to be able to withstand 300 1C, a strong magnetic
eld, high vacuum and not be fragile or brittle. The sample
probe that was inserted into the JET vacuum chamber was
30 cm long, made from BN (boron nitride) and had a
hexagonal cross section. On each of the six sides there were
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doi:10.1016/j.apradiso.2006.02.009

Corresponding author. Tel.: +32 14 571 269; fax: +32 14 584 273.
E-mail address: mikael.hult@cec.eu.int (M. Hult).
three materials: (i) pure Ti placed near the tip of the probe;
(ii) MgF
2
placed just above the Ti and; (iii) an alloy of Ti
(90% by mass), Al (6%) and V (4%) (hereafter referred to
as TiVAl) placed just above the MgF
2
. All samples were
1 mm thick and had a width of 10 mm. The height of the
TiVAl samples were 30 mm, whilst the other two types of
samples were only 10 mm in height. Since the probe was
inserted above the plasma and sticking down from the
ceiling so to say, the pure Ti samples were nearest to the
plasma and the TiVAl samples furthest away. The activities
induced in the same material but at different sides would
give information on the angular distributions of particle
uxes.
The probe was inserted in a position close to the plasma
edge. The activation took place between February 10, 2004
and February 17, 2004, for a total of 49 JET He-plasma
pulses. The probe was measured on a HPGe-detector at
JET 48 h after the activation stopped. The probe was
disassembled and each piece was cleaned and checked for
contamination before being shipped to Belgium. At IRMM
additional smear tests were performed to check for tritium-
contamination. The tritium levels that were found
(o100 Bq per sample) were permissible for a measurement
in HADES. The samples were again cleaned using
isopropanol and then placed in a Teon sample container
with an O-ring seal in order to avoid further transport of
tritium.
2.2. Gamma-ray measurements in an underground
laboratory
All the samples except two MgF
2
samples (F-2 and
F-3) have been measured using ultra low-level gamma-
ray spectrometry in the underground laboratory HADES,
which is located at the Belgian nuclear centre SCKCEN
(StudieCentrum voor Kernenergie Centre dEtude de
le nergie Nucle aire) in Mol, 225 m below ground level
(500 m water equivalent) in the middle of a 100 m thick clay
layer (Hult et al., 2003). All samples were measured
between March 19 and May 18 in 2004 and each sample
was measured for a period of time ranging from 6 to 14
days. Three underground HPGe-detectors were employed
for these measurements, Ge-2, Ge-4 and Ge-5 (Hult
et al., 2000, 2003) with relative efciencies of 8%, 106%
and 50%, respectively. All three detectors have thin
deadlayers (o1 mm) and are shielded with 1520 cm of
low-background lead lined with 515 cm of electrolytic
copper. The sample volumes were ushed with nitrogen gas
boiling off the liquid nitrogen Dewars.
3. Results
3.1. Uncertainties and reference date
The uncertainties are expressed as combined standard
uncertainties, following the Guide to the Expression of
Uncertainty in Measurement (ISO/IEC/OIML/BIPM,
1995). They are given in brackets after the measurement
value and the last digit(s) of their numerical value
correspond(s) to the last digit(s) of the quoted result.
Table 1 gives the uncertainty budget for some selected
radionuclides and samples in this work. The main
contribution to the uncertainty budget comes (as often is
the case in low-level measurements) from counting
statistics. There is also a signicant contribution from
uncertainties due to geometry because of the short distance
between the sample and the detector. All the results were
compared to the decision thresholds using a 0:05 (ISO,
2000). The reference time for all activities reported here is
2004-02-17 14:00 (UTC +2), which corresponds to the end
of the fusion experiment during which the samples were
activated.
3.2. Efciency calculations
The full energy peak (FEP) efciencies were calculated
using the EGS4 Monte Carlo code (Nelson et al., 1985).
The code uses models of detectors and samples. The
models of the detectors were based on radiography of the
detectors when cooled with liquid nitrogen. The radio-
graphs gave the exact placement of the crystal in the
cryostat. The deadlayers (top, side and bottom) were
determined by adjusting their thicknesses in the computer
model until a match between the Monte Carlo calculated
efciencies and experimental efciencies measured using
calibration point sources was obtained. For the radio-
nuclides with cascading gamma-rays (
22
Na,
46
Sc,
48
V,
56
Co
and
57
Co), the coincidence summing was also calculated
using EGS4. For this it was necessary to enter the complete
decay scheme into the code. The complete decay scheme
was obtained from Nucle ide (Be et al., 1999; DAMRI/
LPRI, 1998) for
48
V and from table of isotopes (Firestone,
1996) for the other radionuclides.
3.3. Measurements results
Fig. 1 shows a part of the spectrum from sample Ti-6.
The sample was measured for 8.2 days on detector Ge-4.
ARTICLE IN PRESS
Table 1
Uncertainty budget for surface activity of two radionuclides detected on
the MgF
2
sample sitting in the 901 position
Uncertainty contribution Relative uncertainty (%)
7
Be
56
Co
Counting statistics 50.1 99.3
Gamma-ray emission probability 0.5 o0.1
Correction for decay during cooling o0.1 o0.1
Correction for decay during measurement o0.1 o0.1
Efciencyfrom counting statistics o0.1 o0.1
Efciencyfrom electron and photon transport 9.0 0.1
Efciencyfrom geometry 20.2 0.3
Efciencyprecision of calibration sources 20.2 0.3
Total 100 100
J. Gasparro et al. / Applied Radiation and Isotopes 64 (2006) 11301135 1131
It is clear that the small peaks in this spectrum with low
count rates (6 d
1
for the
56
Co peak at 847 keV for
example) could not have been measured above ground
using a conventional gamma-ray spectrometry set-up.
Table 2 shows a list of all the radionuclides that were
detected and the reactions that could have led to the
production. Special attention was given to
22
Na in MgF
2
-
samples as well as
48
V in Ti-samples and TiVAl-samples as
they could potentially be produced by
19
F(a,n)
22
Na and
48
Ti(p,n)
48
V respectively. The two radionuclides were not
observed and they are thus not indicated in Table 2. The
decision thresholds were 0.3 mBq for
22
Na in MgF
2
-
samples and 5.5 mBq for
48
V in TiVAl-samples for a
measurement time of 7 days following a cooling time (the
time from the end of the activation inside the JET vacuum
chamber to the start of the gamma-ray spectrometry
measurement) of 60 days.
Several of the radionuclides that were detected (e.g.
56
Co
and
57
Co) cannot have been produced by activation of the
samples since the impurity levels of e.g. Ni and Fe were too
low for that. They must have been produced in other parts
of the Tokamak and transported to the sample position
where they were deposited on or implanted in the samples.
It is thus not correct to assume a homogeneous distribution
of these radionuclides in the complete sample volume. Also
radionuclide production due to charged particle interaction
only takes place in the outer few micrometers of the
sample. In order to study FEP efciency as a function of
the depth distribution of these radionuclides simulations
using EGS4 were performed for all samples and gamma-
rays. Fig. 2 shows, for a Ti-sample, the FEP efciency for a
1312 keV gamma-ray as a function of the depth to which a
homogeneous distribution in the sample extends. It is clear
from Fig. 2 that the change in FEP efciency is relatively
small so it is not necessary to know the exact distribution
or extent of the distribution. For this study it was decided
to use the efciency obtained from a homogeneous
distribution in the whole sample for the radionuclides
produced in the sample. For the radionuclides that were
deposited or implanted it was decided to use the efciency
obtained from assuming a homogeneous distribution
extending to a depth of 50 mm.
Table 3 shows all the results that were obtained for the
radionuclides where at least one gamma-ray line was
observed in one sample. Chromium-51 is mentioned in the
table although it was never above decision threshold. The
reason it is mentioned in the table is that in several samples
there were indications of this peak. It could be produced in
the
48
Ti(a,n)
51
Cr and
51
V(p,n)
51
Cr reaction but also from
some other more or less likely reaction channels. The thick
target yield for the (a,n)- reaction is very low and the Cr-
impurity level in the samples is also very low. It is most
likely that the
51
Cr was another neutron activation product
that was sputtered off the Tokamak wall and deposited or
implanted in the samples. The decision threshold for
51
Cr
in a Ti-sample measured for 14 days on Ge-4 is 5 mBq in
case of a cooling time of 34 days.
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56
Co
46
Sc
56
Co
46
Sc
0
20
40
60
80
100
120
140
160
180
200
0 200 400 600 800 1000 1200 1400 1600 1800 2000
Energy (keV)
N
u
m
b
e
r

o
f

c
o
u
n
t
s
0
10
20
30
40
800 820 840 860 880 900
57
Co
7
Be
58
Co
54
Mn
57
Co
7
Be
58
Co
54
Mn
Fig. 1. A gamma-ray spectrum of sample Ti-6 showing the different
radionuclides observed after 76.9 days cooling time and 8.2 days
measurement time. (Energy calibration: 0.344 keV/channel).
Table 2
List of radionuclides that were detected using gamma-ray spectrometry
Radionuclide Half-life Production reaction Activity location Measurement location
24
Na 15 h
24
Mg(n,p);
27
Al(n,a) Bulk JET
44m
Sc 2.4 d
46
Ti(d,a) Bulk JET
47
Sc 3.35 d
47
Ti(n,p)
a
;
48
Ti(n,d);
51
V(n,na)
b
Bulk JET
48
Sc 1.82 d
48
Ti(n,p) Bulk JET
46
Sc 83.8 d
46
Ti(n,p)
a
;
47
Ti(n,d) Bulk HADES
51
Cr 27.7 d
48
Ti(a,n);
50
Cr(n,g),
52
Cr(n,2n);
52
Cr(g,n),
51
V(p,n);
54
Fe(n,a) Bulk or surface HADES
7
Be 53.3 d
10
B(p,a)
a
;
10
B(d,na);
7
Li(p,n)
b
,
6
Li(d,n)
b
Surface HADES
56
Co 77.7 d
58
Ni(d,a);
56
Fe(p,n);
56
Fe(d,2n) Surface HADES
57
Co 271.77 d
56
Fe(d,n);
56
Fe(p,g);
58
Ni(n,d) Surface HADES
58
Co 70.916 d
58
Ni(n,p) Surface HADES
54
Mn 312.2 d
51
V(a,n);
54
Fe(n,p)
a
Bulk or surface
a
HADES
Column 4 gives information on how the radionuclide was distributed in the sample. The short-lived radionuclides were measured at JET shortly after
activation, whilst the long-lived ones were measured in HADES by IRMM.
a
The reaction that gives the major contribution to the produced radionuclide.
b
Reaction that can be neglected due to either low cross section, low abundance of the isotope to be activated near to the target or low particle ux at the
important energy in question.
J. Gasparro et al. / Applied Radiation and Isotopes 64 (2006) 11301135 1132
Beryllium-7 was produced by protons and deuterons
impinging on the boron nitride samples holder.
7
Be in itself
is interesting since it should give direct information on the
charged particle ux. In this case it is difcult to make
conclusions since the
7
Be was sputtered away from the
holder and deposited on all samples.
The distribution of neutrons is different from heavy
sputtered ions and charged light particles. The deposited
heavy ions (e.g.
56
Co) are to some extent also useful as their
angular distribution as well as the vertical distribution
gives information on plasma conditions. Figs. 3 and 4 show
the angular and vertical distribution of
7
Be and
56
Co,
respectively. Their distribution is the same as for
57
Co,
58
Co and
54
Mn (in Ti-samples), which is characterised by
(i) the highest surface activity is near the tip of the probe
and at 301, (ii) The lowest surface activity is on the TiVAl
samples and in the 2701 position, (iii) There are minima at
901 and 2701. The
54
Mn in the Ti sample is due to deposited
ions. It is not detected in the MgF
2
samples and one would
thus expect no detectable surface contamination of
54
Mn
on the TiVAl samples since it is located further away from
the plasma. It is thus possible that the
54
Mn that was
detected in the TiVAl samples comes entirely from
activation by alpha-particles. Scandium 46 is not found
on the MgF
2
samples which is an indication that it is solely
produced by neutron activation of the bulk of the target
material. The distribution of the massic activity of
46
Sc is
shown in Fig. 5. Also here the highest activity was found at
301 near the tip and the activity is lower further away from
the tip (in the TiVAl samples). The angular distribution of
46
Sc is different from the deposited ions (Figs. 3 and 4) and
also different for the Ti and TiVAl samples. This reects the
fact that the neutrons are not affected by the magnetic eld.
4. Discussion
The data indicate that neutrons with energy higher than
2.45 MeV (DD fusion neutrons) were present, which
implies that the heating of the plasma was efcient and
accelerated ions in the MeV range. From the detection of
7
Be, it was possible to conrm losses of protons and
deuterons from the plasma. The loss rate of alpha particles
from the plasma was too low to be detected.
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0.0360
0.0365
0.0370
0.0375
0.0380
0.0385
1 10 100 1000
Depth (m)
E
f
f
i
c
i
e
n
c
y
Fig. 2. Full energy peak efciency for the 1312 keV gamma-ray line in a
TiVAl-sample as a function of the depth in the sample to which the
activity distribution extends.
Table 3
Massic and surface activities for the radionuclides observed in HADES
Sample Massic activity (mBq/g) Surface deposited activity (mBq/cm
2
) Sample orientation (1)
46
Sc
51
Cr
a 54
Mn
7
Be
56
Co
57
Co
58
Co (1)
F-1 220(20)
b
1.0(5) 1.3(2) 90
F-4 22(6) 0.21(10) 270
F-5 210(20)
b
2.0(7) 0.83(17) 330
F-6 310(30)
b
1.6(8) 1.3(2) 30
Ti-1 25(3) 0.53(18) 230(20)
b
1.3(4) 1.34(18) 0.8(2) 90
Ti-2 22(3) o38 1.0(3) 620(50)
b
3.6(8) 2.2(3) 1.2(4) 150
Ti-3 22(4) o0.7 330(40)
b
2.2(10) 1.4(2) o1.3 210
Ti-4 25(3) o12 o0.35 34(5) o0.2 o0.6 270
Ti-5 21(3) o0.7 410(40)
b
o1.3 1.2(2) o1.2 330
Ti-6 29(3) 1.1(3) 610(50)
b
4.8(10) 3.3(4) 1.7(5) 30
V-1 18.3(16) 0.22(6) 103(9) 0.44(14) 0.59(7) 0.33(9) 90
V-2 18.4(18) 0.23(9) 155(13) 0.9(3) 0.70(9) 0.53(17) 150
V-3 17.5(18) 0.27(9) 73(7) 0.5(2) 0.70(9) 0.40(18) 210
V-4 15.1(14) 12.1(15) 0.11(3) 0.21(8) 270
V-5 15.9(17) o14 o0.15 36(4) 0.8(3) 0.26(7) 330
V-6 16.3(17) o0.2 120(11) 0.4(2) 0.54(9) 30
The decision threshold is only indicated for those samples where a peak was seen. Chromium-51 was thus observed in three samples, but the activity was
below decision threshold. F refers to the MgF
2
samples, Ti to the Ti-samples and V to the TiVAl compound.
a
The whole mass of the sample was used in this calculation. Although this is unrealistic assumption it gives at least a guideline value.
b
Rounding interval 10.
J. Gasparro et al. / Applied Radiation and Isotopes 64 (2006) 11301135 1133
Unlike charged particles, neutrons do not feel the
magnetic eld. Scandium-46 (Fig. 5) is mainly produced
by neutron activation and the neutron eld is expected to
be relatively isotropic at the position of the probe. This is
what is seen within uncertainties in Fig. 5, while Figs. 3 and
4 show activation indicating a much less isotropic particle
distribution. The design of the probe with samples facing
six different directions helps to identify reactions induced
by charged particles vs. neutrons.
This activation technique was applied in the JET
Tokamak for the rst time. The number of radionuclides
that could be measured using ULGS makes it interesting to
develop this techniques further. It could be advantageous
to use other materials and reactions than those used here,
but there are severe restrictions on what can be used inside
the Tokamak. The most plausible way of increasing the
yield of certain radionuclides is probably to use enriched
samples. Boron-10 is an interesting candidate for
such a target but then the sample holder must not be
made from BN. It would also be advantageous to use
bigger samples in order to obtain higher activities. There
are also ongoing developments to reduce the detection
limits obtainable in HADES further by introducing
coincidence techniques and more Ge-detectors. It is
possible that this activation technique could prove even
more valuable for better understanding the plasma
characteristics in larger scale facilities like ITER, where it
is likely that the ux of charged particles would be so high
that more reactions are possible to study using under-
ground measurements.
Acknowledgements
The HADES crew of SCKCEN in Mol, Belgium, is
gratefully acknowledged for their work. We thank Timos
Altzitzoglou (IRMM) for measuring the tritium on the
samples using liquid scintillation counting.
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0
100
200
300
400
500
600
700
800
Ti Ti
MgF
2
A
c
t
i
v
i
t
y

(
m
B
q
/
c
m
2
)
0 50 100 150 200 250 300 350
Sample orientation ()
TiVAl
Fig. 3. The angular distribution of the surface activity of
7
Be. Note that
the Ti-samples being closest to the plasma display the highest activity,
whilst the TiVAl samples being furthest away have the lowest activity. The
lines connecting the points (for Ti and TiVAl samples) are provided to
guide the eye.
0
5
10
15
20
25
30
35
0 50 150 200 250 300 350
A
c
t
i
v
i
t
y

(
m
B
q
/
g
)
100
Sample orientation ()
TiVAl
Ti
Fig. 5. The angular distribution of the massic activity of
46
Sc. The lines
connecting the points are provided to guide the eye.
0
1
2
3
4
5
6
7
0 50 100 150 200 250 300 350
A
c
t
i
v
i
t
y

(
m
B
q
/
c
m
2
)
Sample orientation ()
TiVAl
MgF
2
Ti
Ti TiVAl
Decision threshold
Fig. 4. The angular distribution of the surface activity of
56
Co. The lines
connecting the points (for Ti and TiVAl samples) are provided to guide the
eye and there is no line to connect to a decision threshold.
J. Gasparro et al. / Applied Radiation and Isotopes 64 (2006) 11301135 1134
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