Nuclear Engineering and Technology 55 (2023) 2984e2996

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Nuclear Engineering and Technology

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Original Article

Measurement of the applicability of various experimental materials in

a medically relevant reactor neutron source Part One: Material
characteristics acting as a carrier for boron compounds during neutron
irradiation
Ezddin Hutli a, b, *, Peter Zagyvai a, b
a
Centre for Energy Research, Budapest, Hungary
b
Institute of Nuclear Techniques, Budapest University of Technology and Economics, Budapest, Hungary

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

Article history: A 100 kW thermal power pool-type light water reactor and Pu(Be) as a fast neutron source were used to
Received 11 August 2022 determine the appropriate carrier for irradiating boron-containing samples with neutron beams. The
Received in revised form tested materials (carriers) were subjected to neutron beams in the reactor's tangential channel. The
23 March 2023
geometrical arrangement of experimental facilities relative to the neutron beam trajectory, as well as the
Accepted 25 April 2023
Available online 20 June 2023
effect of sample thickness on the count rate, were investigated. The majority of the detectable charged
particles emitted by the neutron beam's interaction with tested materials and the detector's detecting
layer are protons (recoiled hydrogen) and particles generated in nuclear reactions (protons and alpha
Keywords:
Reactor
particles), respectively. Stopping and Range of Ions in Matter (SRIM) software was used to do theoretical
Boron calculations for the range of expected released particles in various materials, including human tissue. The
Neutron results of measurement and calculation are in good agreement. According to experiments and theoretical
Alpha calculations, the number of protons emitted by tissue-like materials may commit a dose comparable to
Proton that of boron capture reactions. Furthermore, the range of protons is significantly larger than that of
Dose alpha particles, which most probably changes dose distribution in healthy cells surrounding the tumor,
which is undesirable in the BNCT approach.
© 2023 Korean Nuclear Society, Published by Elsevier Korea LLC. This is an open access article under the
CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

1. Introduction protocol due to the harmful effect predicted in re-irradiated normal

tissues. In the photon or particle radiation approach, the normal
Radiation therapy is commonly used in cancer treatment. One of cells surrounding the tumor are given a therapeutic dose of more
the important techniques in this discipline is energetic gamma than 60 Gy [2e4]. The BNCT method can achieve a significant dose
irradiation (teletherapy). Irradiation is also done with charged gradient between normal and malignant cells, allowing a curative
particles such as protons and 12C ions (brachytherapy). The disad- dose to be delivered to the local tumor while normal cells and
vantage of these irradiation approaches is that the irradiation beam tissues are almost completely preserved. According to this, the
energy is deposited on the trajectory prior to the tumor cells. Even BNCT is considered a noninvasive cancer treatment. It is extremely
for charged particles, the effect is less pronounced than for gamma effective against cancers of the head and neck, the brain, and the
rays but still significant. This effect is much less pronounced in skin [5e13]. BNCT is a tumor therapy capture reaction based on
boron neutron capture therapies (BNCT) because the target region boron neutron capture that combines nuclear physics, chemistry,
is defined by the presence and distribution of 10B in the injected biology, medicine, and other disciplines [3,13,14]. When a thermal
medication [1]. neutron is captured by a10B atom, an alpha (4He2þ) particle and a
Re-irradiation is avoided in the radiation cancer treatment rebound lithium nucleus are produced (7Li). The average LET is high
for both of them (7Li's LET y 162 keV/mm and 4He's LET y 196 keV/
mm in “average” human tissue) so these particles' kinetic energy is
dissipated over a short distance (10 mm). Because a single human
* Corresponding author. Centre for Energy Research, Budapest, Hungary. cell is approximately 10 mm in size, the boron neutron capture
E-mail address: [email protected] (E. Hutli).

https://doi.org/10.1016/j.net.2023.04.037
1738-5733/© 2023 Korean Nuclear Society, Published by Elsevier Korea LLC. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/
licenses/by-nc-nd/4.0/).
E. Hutli and P. Zagyvai Nuclear Engineering and Technology 55 (2023) 2984e2996

process occurs within a single cell. In theory, 10B can be selectively 2. Experiments and discussion
accumulated in tumor cells; thus, BNCT kills tumor cells with two
heavy particles (4He and 7Li) having sufficient kinetic energy while 2.1. Conditions of the experiments
protecting normal tissue [15].
Two important alternative reactions may occur during the BNCT, The nuclear reactor of the Technical University of Budapest is a
yielding high LET radiations resulting in a high relative biological swimming-pool-type reactor. The maximum power is 100 kW and
effectiveness (RBE): 14N(n,p)14C and 1H(n,n')1H. The RBE of each the maximum thermal neutron flux in the active core is 2.7xl012 n/
such radiation must be considered. RBEs of these radiations are cm2s. There are five horizontal beam tubes (channels), which
easily found because hydrogen and nitrogen are inherently ho- mainly serve experimental purposes. Four of the horizontal chan-
mogeneously distributed in both tumor and normal tissue. Because nels terminate at the edges of the core radially, while channel No.5
achieving a homogeneous microscopic distribution is difficult, the is tangentially connected to the core. A large irradiation tunnel is
treatment technique and dose calculation use the averaged also part of the irradiation facilities; this tunnel is modified to be
macroscopic value of 10B concentration in a tissue. The effective RBE suitable for BNCT technique [28e30]. Fig. 1 presents the horizontal
of the 10B(n, a)7Li reaction is determined by the 10B-containing section view of the Training Reactor at the middle plane of the core
drug's microscopic distribution. As a consequence, the effective (from the MCNP model of the reactor) [31].
RBE, also known as compound biological effectiveness (CBE), varies The main purpose of the experiments and measurements is to
depending on the boron compound, target tissue, and endpoints investigate the high-LET charged particles produced both in
(An endpoint is a clinical trial outcome that is statistically analyzed different materials which will be used later as carriers for boron
to help determine the efficacy and safety of the therapy under compounds during neutron irradiation, and in tissue-like
investigation). Because of their nature, these quantities can only be hydrogen-containing materials in circumstances (i.e., in a neutron
determined by tests. In terms of neutron physics, the reaction 10B(n, field) similar to that of the BNCT irradiations. During the experi-
a)7Li belongs to the thermal energy region of BNCT [6,16]. ments, we also wanted to study the detection characteristics of the
Thermal neutron flux and tumor boron content were defined to applied alpha-detector and the behavior of the detector in the
be the most important parameters influencing BNCT efficiency. For neutron field.
BNCT to be effective, the tumor must have a high concentration of Horizontal channel No.5 was chosen for the tests conducted in
boron in comparison to surrounding tissue. It was discovered that a the context of this work for a variety of reasons. On the one hand,
sufficient amount of 10B (20e50 mg of 10B/g of tumor or 109 atoms/ because of the above-mentioned geometrical layout, this channel
cell) should be delivered to the tumor [17,18]. Therefore, the has the largest thermal to fast neutron flux ratio, which is advan-
selectivity of boron drug accumulation in the tumor is an important tageous given the nuclear reaction under investigation (10B(n, a)
7
factor. The Positron Emission Tomography PET technique is Li) has a 1=w cross-section versus energy function. (see Section
commonly used to quantify the accumulation and concentration of 2.5). However, when measuring procedures are considered, the
boron drugs, in which the boron gent can be labeled with a gamma radiation dose rate at the exit of this tube is the lowest
positron-emitting nuclide such as 18F and submitted to PET when compared to the other channels (this can partly be attributed
[19e21]. to the fact that a bismuth filter of approximately 128 mm thickness
During treatment processes, the change in boron concentration is built into the outer part of the channel). Channel #5 has the
with time following boron agent delivery should be addressed; this
change is dependent on tumor and normal tissue metabolism. This
information is only available through the PET imaging method, PET
is frequently required for the precision and safety paramount for
radiation use [1,13,22e26].
In terms of neutron physics, the reaction 10B(n, a)7Li belongs to
the thermal energy region of BNCT.
Many institutions worldwide are now working on clinically
focused projects. The majority of these efforts are aimed at clini-
cally implementing neutron capture therapy. Major projects are
currently going on in the United States, Japan, Australia, and
Europe. In Europe, the European Union launched a collaborative
research project, the center of which is in Petten in the Netherlands
[27].
In this paper, the usefulness of various experimental materials in
research using a medically important reactor neutron source is
demonstrated. Neutrons are measured by detecting a-particles
generated from boron target nuclei. The operating voltage, effi-
ciency, and sensitivity to other predicted emitted particles of the
ZnS(Ag)-detector were measured, and the change of the sensitivity
along the detecting layer was investigated. The reactor channel was
utilized to investigate detector and sample location in relation to
the neutron beam origin and trajectory, sample thickness, and
sample type. The investigation also included measurements with a
portable fast neutron source. In addition, the investigation covers
calculating the range of predicted emitted particles in various
materials, including human tissues (bone and muscle).

Fig. 1. The horizontal section view of the Training Reactor at the middle plane of the
core (from the MCNP model of the reactor) [31].

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biggest diameter when compared to the other channels, which is absorbers or an electronic circuit) a-particles in the case of
also helpful because it is equivalent to the diameter of the detecting measuring protons and protons in the case of measuring
surface of the nuclear detector to be used as described later. a-particles.
The measured parameters of the BNCT irradiation tunnel, and Because we'll be dealing with a wide range of nuclear radiations
tangential channel#5 in the NTI-BME reactor at 100 kW reactor in our experiment, including fast and thermal neutrons, gamma
power are presented in Table 1 and Table 2 respectively: (the un- radiation, and heavy particles (alpha, protons), ZnS(Ag) is the ideal
certainty of the data is in all cases less than 10%) [28,29]. detector for the majority of them. Because silver activated zinc
For safety reason, the reactor power was limited to 1 kW in this sulfide has a better scintillation efficiency than other scintillation
work, and the thermal and fast neutron fluxes (fth ; ff ) were 1.1E5 detectors, the detector ZnS(Ag) was chosen for this experiment. It is
and 1.5E4 cm2s1, respectively. The thermal to fast neutron flux only available as a polycrystalline powder [32,33]. Due to the multi-
ratio (fth =ff ) was approximately 7.33. In the following part of our crystalline layer's opacity to its own luminescence, thicknesses
study, we will work on the boron compounds used in BNCT. To greater than roughly 25 mg/cm2 are rendered worthless. Its
obtain quantifiable results from work with such a low thermal to application is confined to small screens that are used to detect a
fast neutron ratio, the mass of the boron compounds that will be -particles or other heavy ions. a-particle monitors primarily use
irradiated with neutron beam should be increased to increase the ZnS(Ag) [33e35].
possibility of thermal reactions (10B(n, a)7Li), also the irradiation ZnS(Ag) can be used to detect thermal neutrons if a lithium
time should be considered. compound enriched in 6Li is introduced. When the a-particle and
The reactor power was chosen to meet the following Triton from the 6Li(n,a)3H reaction interact with the ZnS(Ag),
requirements. scintillations are produced. Another application for ZnS(Ag) is fast
neutron detection. A fast neutron detector was created by incor-
 The time required for the various experiments should be porating ZnS(Ag) into a pure hydrogenous compound. A recoiling
reasonably short and enough to have a measurable finding; proton generated by a neutron-proton scattering interaction is
 The neutron plus gamma dose rate around the measuring site being used to detect the neutrons. The energy of the protons will
should be acceptably low, i.e. within the limits regulated by range from zero to that of the incoming neutrons [33,36e38].
radiation protection laws, with a relatively easily movable The key challenges for this type of detector include having a
shielding arrangement. relatively low background, i.e., approximately 103 counts/s. The
lack of understanding about the response and background sources
According to early measurements, the reactor output of 1 kW of these types of detectors appears to be the main reason of the
appeared to be adequate for both of the aforementioned needs. difficulty experienced in identifying the appropriate measurement
Because the boron samples that will be irradiated later will be settings. It was assumed that the background is derived from nat-
placed on the surface of carriers, the thermal neutron flux is more ural sources (mainly radon) and that cosmic, beta, or gamma rays
appropriate for these experiments than the epithermal flux. In have no contribution because their efficiency is extremely low [38].
clinical applications, the modulation of the neutron beam energy The measurements were made at the second level of underground
spectrum is determined by the location of the tumor in the body in the nuclear reactor building at NTI BME also the measurement
and its depth; special filters made of specific materials are used for setup was surrounded by big blocks (shield materials) to reduce the
optimization. contribution of these types of radiations (due to radon gas particles
A pure thermal neutron beam is only useful for tumors close to in the ambient air) to the alpha background. In addition, the
the skin's surface, while epithermal neutrons are required for deep a-source used the measurements has a strong activity.
tumor treatment. More information on how to modulate the Table 3 shows the properties of Saint-Gobain commercial
neutron beam energy spectrum to the epithermal neutron energy ZnS(Ag) powder which was used in this study (Conventional
region when implementing BNCT with the output neutron beam of ZnS(Ag) Alpha Detector).
the used reactor (NTI-BME reactor) is presented in the publication To operate scintillation detector systems, the scintillation de-
[28,29]. tector requires a high voltage. The voltage depends on the type of
Because the experiments were conducted some time ago, we photomultiplier tube that is used in the system and may vary from
were unable to manage the procedure with appropriate phantoms about 500 V to about 3000 V [39].
so we needed to rely on approximate methods. In fact, we did not The operating voltage of the ZnS(Ag) alpha detector was
conduct any experiments on patients. Our goal was to test the determined by measuring the detector's count rate as a function of
boron compounds in various forms. high voltage to achieve the best working conditions. The setting
was performed using a flat disc a-source (6986 Bq), the detecting
2.2. Detection system characterization and measurements system configuration is presented in Fig. 2. The results of the
measurements are depicted in Fig. 3. The composition of the
2.2.1. Determination of the operating voltage a-source is presented in Table 4.
To be confident in the results, a detector should be used that is The detector electronics are made up of two user-adjustable
theoretically insensitive to all other radiation components except components: the high voltage applied to the photomultiplier tube
the one being measured, or that can be easily eliminated (via (PMT) and the low level discriminator (LLD), which is used to
eliminate electronic noise. The high voltage and LLD optimization
Table 1 are useful for achieving the best counting conditions. The charac-
Measured parameters at 100 kW reactor power (NTI-BME) in the irradiation tunnel
teristic curve was determined by measuring the alpha source in a
[28,29].
ZnS(Ag) scintillation alpha detector and increasing the voltage from
Measured parameters at 100 kW Value 1050 to 1450 V in 50 V steps, while increasing the LLD in all cases to
Thermal neutron flux rate fth ðE < 0:5 eV Þ 1.23E9 cm2s1 optimize.
Epithermal neutron flux rate fepi ðE ¼ 0:5 eV  1 MeVÞ 7.07E7 cm2s1 Based on previous experience with this type of detector, the
Fast neutron flux rate ff ðE > 1 MeVÞ 7.03E3 cm2s1 measurement began with 1050V.
g dose rate 1.3 Gy/h
For each voltage/LLD combination, the counting time was
fth =ff ðE > 1 MeVÞ ⁓175
10 min. The region of minimum slope of the curve is referred to as
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Table 2
Characteristics of the irradiation field at the 5th horizontal tangential channel at a reactor power of 100 kW [28].

D_g (cGy/min)
ð1=EÞ
Position fth (cm2s1) fepi (cm2s1)[0.5eV-500 keV] ff (cm2s1)[E > 1MeV]

At the outlet of the port (original leakage spectrum) 4.36 Eþ07 4.17 Eþ07 0.93 Eþ07 87
Behind filter I (193 mm; graphite-bismuth combination) 4.05 Eþ06 2.11 Eþ06 0.59 Eþ06 0.15
Behind filter II (128 mm; bismuth) 1.08 Eþ07 7.76 Eþ06 1.48 Eþ06 0.22
Behind filter Ill (103 mm; bismuth) 1.50 Eþ07 1.29 Eþ7 2.24 Eþ06 0.52

Table 3 the plateau. The slope is expressed as a percentage increase in

The properties of ZnS(Ag) powder [36]. counting rate for every 50 V increase in applied voltage:
Property Value
100ðR2  R1 Þ=R1
Cleavage plane Polycrystalline %=100V ¼  100
Density (g/cm3) 4.09 V2  V1
Wavelength of emission max. (nm) 450
Lower wavelength cut off (nm) 330
Refractive index at emission max. 2.36 100ð60277:257562:8Þ
57562:8
Photoelectron yield [% of NaI(Tl)] 130 % = 100V ¼  100 ¼ 4:7155%
Scintillation decay times (ns) 110 1350  1250

where R1 and V1 are the count rate and voltage at the begin of the
plateau and R2 and V2 at the end of the plateau. A good tube should
have a slope not greater than 5e10% per 100 V. The advantage of
this plateau is that the instrument's sensitivity is fairly independent
of small changes in the high voltage. It is recommended not to use
too high a voltage in a PMT because the phototube's lifetime may be
slightly longer at a lower voltage. At the same time, the operating
voltage should be set above the plateau's threshold voltage to
ensure that the detecting system performs well. Based on the re-
sults in Fig. 3, the detector's operating voltage was set to 1300 V,
which is in the middle of the flat plateau of the high voltage vs.
count rate curve, following general practice as described in details
in the literatures [40e42].

2.2.2. Measurement of detector efficiency

Fig. 2. Schematic diagram of the detecting system setup. The detector's efficiency had to be determined because the
measured count rates would later be converted to dose rate values.
Natural radiations contribute insignificantly to the alpha back-
ground in this measurement due to the procedures described
above. The absolute detection efficiency of the detector was
determined in this study without the presence of beta and gamma
interference (only Am-241 has an intensive gamma transition at
59.5 keV, its photonic yield is 36%, accompanied with low energy
internal conversion electrons and X-rays).
For determining the a-counting efficiency in the given mea-
surement geometry an a-source of known activity was used. The
composition of the a-source is given in Table 4.
The efficiency of a detector is given by equation (1) below,
assuming that the a-emission yield of the standard radionuclides is
1:

Count rate
ε¼ (1)
Activity of isotope
Fig. 3. The count rate as a function of the applied detector's operating voltage.
Where the activity of isotope is the activity at the date of mea-
surement. Therefore, the activity of the source at the date of the
Table 4 efficiency determination has to be calculated. As it can be seen from
Composition and characteristic data of the a-emitting isotopes of the calibrating Table 4 the half-life of 239Pu and 241Am is very long compared with
source.
the time elapsed between the calibration of the isotope and the
Isotope Activity on (November 01, 2014) Half-life main a-energy [keV] date of measurement. Accordingly, the change in their activity can
239
Pu 3034 Bq 2.4  104 y 5160 be neglected. However, the change in the activity of 244Cm cannot
241
Am 2449 Bq 432 y 5490 be neglected and has to be calculated using the following formula:
244
Cm 1917 Bq 18.1 y 5800
A ¼ Ao elt (2)

Where A is the activity of the source at the time of measurement, Ao

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is the activity of the source at the time of calibration, and l is the

decay constant.
After performing the calculation, for the activity of 244Cm we
obtain:

A ¼ 1503 Bq

The total activity of the isotopes:

A ¼ 6986 Bq

and thus, the efficiency (ε)of the detector is

97547±312 ðcpsÞ
ε¼ x100 ¼ 23±0:5%
6986 Bq
It must be noted here that this detector efficiency is only valid
strictly for a- particles with the same energy as those emitted by
the calibrating source (E z 5 MeV). If the energy of the incident
Fig. 4. Arrangement of neutron source on the detector.
particle is significantly lower, the detecting efficiency will become
lower as well as a result of its absorption in the layers between the
source and the sensitive volume of the detector. According to the Table 5
literature, the detection efficiencies of various commercially man- Results of different neutron source placements.
ufactured ZnS(Ag) alpha detectors range from 33 to 44% with flat Source placement count rate (cpm)
point-like sources like that applied in the experiment [43,44].
1 15394 ± 124
However, due to the detector's efficiency, it can operate under
2 13425 ± 116
normal neutron beam conditions, producing count-rates that can 3 13036 ± 114
be processed by the electronic counting chain without information 4 12651 ± 113
loss. 5 14696 ± 121
6 12844 ± 113
The standard deviation of the count rate was calculated using
the rules of probability theory to analyze the results. The signals
measured by the nuclear detector are known to follow the Poisson-
distribution laws. As a consequence, in subsequent measurements, to be examined in the course of further planned experiments were
this relationship is used to calculate the standard deviation corre- not expected to be known an average neutron sensitivity was
sponding to the measured count rate value. calculated by taking the arithmetic mean of the arrangements
presented here. This inhomogeneity had a significant negative ef-
fect on the precision of our further measurements with this de-
2.2.3. Investigation of b-sensitivity of the detector
tector that we were not able to replace. The non-uniformity of the
To study the response of the detector to b- particles (energetic
large detector was not an issue to investigate further, we only
electrons) and make sure that the particles detected in the later
stated its existence. So the investigation on the charged particle
measurements are not electrons, an experiment had to be per-
equilibrium thickness was not separated from this simple state-
formed. In this experiment three b-sources (90Sr/90Y) with a total
ment. Based on these measurements, we can conclude that the
activity exceeding 600 kBq were put on top of the detector,
inhomogeneity of the detecting layer could limit measurement
immediately on the closing surface. The count rate of the detector
precision. The interactions between the nuclei of the detector's
was measured along with a background measurement. Since there
material components and the fast neutrons entering the detector
was no significant difference between the two measurements (in 3
reflect the processes that result in scintillation events in the de-
times 1 min measuring time for both, the measured counts were 0)
tector crystal, which then counted in the detection system's elec-
it can be stated with certainty that the detector cannot detect
tronic system as they are presented in Table 5.
b-particles. This is acceptable since the detector's light conversion
ZnS with Ag impurities serves as the detecting layer. Because of
efficiency is rather low for fast electrons, which may be advanta-
the small amount of Ag, its fast neutron interactions can be ignored.
geous for detecting heavy ionizing particles in a relatively intense
Fast neutron interactions with zinc and sulphur yield protons and
g-ray background.
a-particles, depending on the neutron energy, isotope fraction and
the cross-section. Because the detector window's cover foil is made
2.2.4. Investigation of the uniformity of distribution of ZnS(Ag) of aluminum, fast neutron interactions that create protons and
detecting layer and its response to fast neutron irradiation a-particles there should also be considered. Also there is possibility
Utilizing a Pu(Be) neutron source that emits fast neutrons and of (n,n’) interaction (inelastic scattering) in the detecting layer and
12
C atoms as reaction products with 5.7 MeV Q-value, it is possible the produced neutrons that may interact again with detecting
to study the responses generated by neutrons in the ZnS(Ag) de- material and enhance the count rate.
tector. As the source was significantly smaller than the sensitive The results are in good agreement with the technical specifi-
surface of the detector, the assumed inhomogeneity of the detect- cations of the detector. The specifications state that the thickness of
ing layer in the detector had an influence on the accuracy of the the detecting layer is between 15 and 20 mg/cm2. Therefore, it can
results. At various locations, the neutron source was positioned be concluded that as the thickness of the detecting layer changes,
directly on the surface of the detector window, with nothing in the counting sensitivity also changes. Taking into consideration
between, as shown in Fig. 4. The count rate was measured at each that the fast neutrons have high penetrability for material, it can
location (point) and the results are shown in Table 5. Since the easily be understood that by placing the neutron source (which can,
accurate locations of the neutron-generating “spots” of the samples
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for the moment, be considered as a point source) at different points polyethylene foil-covered detector was just detectable here, the
on the detecting layer the count rate changes with the changes in difference between the uncovered detector and the polyethylene
the layer's thickness. Fig. 5(a and b) is adapted from literature [33]. foil-covered detector was much larger, with the polyethylene count
It shows the relation between the characteristics of the detecting rate being more than double that of the “sole” detector count rate.
layer, its sensitivity and the detecting efficiency. Fig. 5(a) demon- The reason behind this increase in the count rate is that poly-
strates the relationship between the ZnS(Ag) sensor pulse height ethylene (characterized with the chemical formula (CH2)n) has a
spectrum (counts) and the ZnS(Ag) sensor layer thicknesses. The high hydrogen content, the detector detects recoil particles from
ZnS(Ag) sensor of 41.99 m m thickness shows the best a-particle the polyethylene, specifically recoil protons caused by elastic (n,p)
detection efficiency as seen in Fig. 5(b), more information on the scattering. By the way this method is suitable for detecting fast
effects of detecting layer on the sensitivity of the detector can be neutrons (fast neutrons do not have a large cross-section for ab-
found in the literature [33]. sorption), allowing fast neutron detection without the use of a
moderator. The nuclei of hydrogen and helium are light enough for
this purpose.
2.3. Reactor channel-neutron irradiation experiments The results of the two setups (Fig. 6(a and b) and Fig. 7(a and b))
should be compared to understand the effect of the arrangements.
2.3.1. Investigation of the geometrical arrangement of experiment When the results of two experiments using the setups shown in
facilities on the count rate Figs. 6(a) and Fig. 7(b) are compared, the influence of the distance
The neutron flux was directly irradiated the detector, with just between the detector and the neutron source (reactor channel
air between the channel and the detector, to investigate the inter- output) is clearly obvious. The count rate was lowered by extending
action between the detection and the neutron beam, and two the travel distance of the neutron beam. This is because of beam
setups are used to investigate the effect of the detector's position scattering in the air.
with respect to the neutron irradiation channel on the count rate, as We now assume that the direction of the outgoing particles is
illustrated in Fig. 6 (a,b). The reactor operating power was limited to similar to that of the incident neutrons, this assumption is verifi-
1 kW, and the thermal and fast neutron flounces(fth ;ff ) were 1.1E5 able. It was investigated with the help of another experimental
and 1.5E4 cm2s1, respectively. The results for the two experi- arrangements depicted in Fig. 8(a,b) in which the distance between
ments are given in Table 6. In these experiments the distance (d) the detector and the channel output was kept constant at d ¼ 15 cm
between the channel edge and detector window (d) is kept fixed; while the detector was moved down with 10 cm under the lower
d ¼ 25 cm. edge of the channel to avoid interaction between the neutron beam
Comparing the results of the two arrangements one can see that and the detector (the distance between the detector window and
the difference is practically “just” significant. It is probably because the channel center “neutron beam center” is 22.5 cm).
in the case of the first experiment the different parts of the Table 8 shows the results for the two arrangements. The results
detecting surface are at different distances from the channel in of the two experiments are practically the same. The sensitive layer
addition to the probable divergence of the neutron beam with of the detector is practically out of the beam in this experiments. As
traveling distance; as a consequence, the reaction probability in this a result, if the particles are emitted “backward,” the difference
arrangement is less in Case 1. One should also note that the ex- between the two results must reflect this feature of the interaction.
periments were all performed in ambient atmosphere so the The low count rate obtained in these setups (Fig. 8(a,b)) in
scattering of particles in the air molecules could also play a role in comparison to prior configurations (Fig. 6(a,b) and Fig. 7(a,b)) is due
diminishing the angular correlations. to the detector's location with respect to the neutron beam
An experiment was carried out to investigate the direction of the trajectory.
particles that will be emitted from the hydrogenous materials
covering the detector surface as a result of neutron irradiation. As
shown in Fig. 7 (a,b), the setup is identical to the previous experi- 2.3.2. Investigation of the effect of sample-to-detector distance
ment (Fig. 6(a)). With this arrangement, the number of neutrons To determine the influence of the distance between the reactor
that may penetrate the converting material (polyethylene foil) and channel output and the detector on the count rate, the attenuation
incident on the detector making reaction with its detecting layer of the neutron beam was investigated first, then the attenuation of
can be reduced. the emitted particles and neutron beam together was investigated.
The results are shown in Table 7. Here the distance d is 15 cm. This investigation is suitable to ensure that the detected particles
The difference between the uncovered detector and the (emitted particles) are protons. Two series of measurements were

Fig. 5. (a) The spectrum of 241Am pulse height with respect to ZnS(Ag) layer thickness, and (b) The detection efficiency of ZnS(Ag) sensors with six different layer thicknesses [33].

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Fig. 6. Detector arranged (a) parallel, and (b)coaxial with the neutron beam.

Table 6 Table 7
Results of the detector arranged parallel and perpendicular to the Results of detector face arranged parallel to the neutron beam
neutron beam. direction.

Experiment No. Count rate (cpm) Experiment No. Count rate (cpm)

1(Fig. 6(a)) 3820.0 ± 61.9 1(Fig. 7(a)) 5198.3 ± 72.1

2(Fig. 6(b)) 4170.0 ± 64.6 2(Fig. 7(b)) 4743.3 ± 68.9

carried out: in the first, the detector was placed at various distances beam source and the detector; the boron compound will be
in front of the channel. The detector was facing the canal in its distributed and glued over the carrier surface. Because this carrier
middle as in Fig. 6(b), with only air (no convertor) between them. In must be as thin as possible to avoid attenuation of the emitted
the second series, a sheet of paper was taped to the channel outlet, particles from the tested boron compounds, we must also deter-
and the detector was placed at various distances once more. Fig. 9 mine the emitted particles from the carrier materials themselves
show the measurement results. For the 25 cm baseline measure- under neutron irradiation to see their contribution to the count
ment, the two series of measured values are normalized to each rate. As a consequence, before the carrier can be used, its charac-
other. teristics must be determined. A series of experiments and mea-
The following conclusions can be drawn from the results shown surements were performed, and various proposed carriers were
in the figure: When the two curves representing the detector tested. The thickness of various particle emitting material samples
response to neutron and neutron plus charged particle radiation are (carrier materials) and the observed count rate are investigated.
compared, the range of charged particles in the air is found to be The materials investigated were aluminum foil, paper, polyethylene
between 5 and 15 cm. These values will later be compared to foil, and sticking foil. The results are shown in Figs. 10e13.
theoretically calculated range values to determine the type of the The following conclusions can be drawn from these findings.
emitted particles (counted particles).
 In Fig. 10: Changing the thickness of aluminum has no effect.
There are two possible explanations for this phenomenon:
2.3.3. Investigation of the effect of sample thickness either none or only a small number of detectable particles leave
To irradiate the boron compounds with the neutron beam, we
need a carrier material to hold the compound between the neutron

Fig. 7. Detector face arranged parallel to the neutron beam (a) with foil and (b)without foil sample.

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Fig. 8. Detector face arranged parallel to the neutron beam (a) with inclined foil sample (b) without foil sample.

Table 8
The results of a detector window aligned parallel to the neutron
beam's direction.

Experiment No. Count rate (cpm)

1 503.7 ± 22.4
2 511.3 ± 22.6

Fig. 11. Influence of the thickness of polyethylene foil sample on the count rate.

Fig. 9. Influence of the detector distance on the count rate.

Fig. 12. Influence of the number of sticker foils on the count rate.

the Al foil as a result of neutron irradiation, or almost all of them

are self-attenuated inside the material.
 In Fig. 11: Although the thickness of the polyethylene foils has no
effect on the measured count rate, the point on the right side of
the graph corresponds to a much thicker polyethylene plate, the
Fig. 10. Influence of the thickness of aluminum foil sample on the count rate. material composition of which can also differ from the others.

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The analysis of the results shown in Table 9 reveals that.

 The interaction between the detector's detecting layer and fast

neutrons is dominant (protons and a-particles are emitted);
 The fast neutrons emitted by the Pu(Be) source produce the
same type of particle emission from paper and polyethylene as
the neutron beam from the horizontal channel of the applied
reactor. The emitted particles are recoil protons (hydrogen), the
big difference in the count rate from paper and that from
polyethylene is likely due to the polyethylene has higher
hydrogen content than the paper (the nominal paper thickness
was triple of the polyethylene thickness, further work is needed
for this point).
 In the case of the aluminum foil, the fast neutrons emitted by
the Pu(Be) source produce protons and a-particles according to
Fig. 13. Influence of the thickness of the paper layer on the count rate. the reactions (27Al(n, p)27Mg and 27Al(n, a)24Na) respectively.

3. Calculation of the range of protons and a-particles in

 Figs. 12 and 13 show that the relationship between the thickness various types of matter
of sticking foils and the count rate, as well as the thickness of
paper sheets and the count rate, is approximately linearly pro- The previous sections described various types of experiments,
portional in the represented range. the results of which should be validated by theoretical calculations.
During the experiments, some charged particles were assumed to
Taking into account all the above observations, one can conclude be emitted from hydrogenous material. Obviously, protons were
that the material composition and quality do have a significant thought to be these particles. This assumption is supported by
effect on the number of particles emitted from the given sample. theoretically calculated range graphs for protons and a-particles. To
However, the relationship between the amount (thickness) of the determine the ions’ range in matter the Stopping and Range of Ions
given material and the caused particle emission is not so straight- in Matter (SRIM) software was used. SRIM is a software package
forward. In the case of paper and sticker foil, the effect seems to be that deals with the stopping and range of ions in matter, as well as
quite significant, but in the case of polyethylene foil, the signifi- ion-matter interactions. SRIM is well-known in the ion implanta-
cance of the effect could not be confirmed. tion research and technology community, and it is also widely used
in other areas of radiation material science. The core of SRIM is a
2.4. Experiments with fast neutron source (Pu(Be) neutron source) program called Transport of Ions in Matter (TRIM). TRIM is Monte
Carlo computer program that calculates the interactions of ener-
To investigate the scenario when only fast neutrons irradiated getic ions with amorphous targets. TRIM is a computer program
the carriers, some experiments and measurements were carried written based on J.P. Biersack and J.F. Ziegler work [45,46].
out using alpha neutron source. The used alpha neutron source is a
Pu(Be) Source, it has an activity of 83.3 GBq and can emit 4- 3.1. The motion of charged particles in air
5.4  104 (n/s)/GBq, with an average neutron energy of 4.2e5 MeV,
while the maximum energy is 11 MeV. The source was placed on First, the range of protons and a-particles were calculated in air
the detector face, while different carriers (aluminum foil (standard as function of their energies. The results of these calculations are
household), paper (a sheet of A4 paper), and polyethylene foil shown in Fig. 15 and Fig. 16, respectively.
(standard household)) were sandwiched between it and the de- The results show that there is a significant particle energy vs.
tector (Fig. 14). The thicknesses of the tested carriers were not traveling range correlation, which followed an empirical rational
equal. Table 9 shows the results of the experiments. dependence, with a good correlation coefficient (R2 ¼ 0.99). The
type of correlations varies according to the charged particles and
the traveling medium. Many trend line (regression line) options
were tested in order to obtain the best line that includes the largest
number of points on the curve; the indicator is R2. R-squared is a
statistical measure that indicates how close the data is to the fitted
regression line. The equation that represents the accepted trend
line as a correlation between the parameters (variables). The cor-
relations are depicted in the graphs. The distinction between the
correlations is logical because the interaction between charge
particle and medium is dependent on both of their properties.
When these figures are compared to the results obtained earlier

Table 9
Results of neutron source measurements.

The material between neutron source and detector Count rate (cpm)

Uncovered detector 13770 ± 117

Al foil (thickness is 0.01 mm) 6671.3 ± 81.7
Paper (thickness is 0.1 mm) 7823.0 ± 88.4
Polyethylene (thickness is 0.03 mm) 10498 ± 102.5
Fig. 14. Arrangement of neutron source and sample on the detector.

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Fig. 15. Proton range in air as a function of energy.

Fig. 17. Proton range in Aluminum as a function of energy.

Fig. 16. a-particle range in air as a function of energy.

Fig. 18. a-particle range in Aluminum as a function of energy.

(see Figs. 9e13), the following conclusions can be drawn.

neutron interactions are of particular interest here. As a result, the
range of protons in polyethylene must be computed and compared
1. Because the experimental results show a range of several cen-
to experimental data. Fig. 19 and Fig. 20 show the theoretical range
timeters in air, the particles studied are almost certainly
curves for protons and a-particles.
protons.
Before proceeding with the actual comparison, it should be
2. Using Fig. 15, it is possible to conclude that the energy of the
noted that the thickness to which the count rate can increase must
emitted protons must be between 1 and 2 MeV. It is self-evident,
be approximately the same as the theoretically calculated range. In
given that the most likely fast neutron energy in the neutron
other words, increasing the thickness of the sample further (once
beam from the NTI-BME reactor (tangential channel 5) at 1 kW
the thickness approximately equal to the particle range is reached)
reactor power is around 2 MeV
will not increase the number of particles emitted from the sample
because particles created at a specific location are themselves

3.2. The motion of charged particles in aluminum (attenuation in

foils)

The range of protons and a-particles in aluminum was again

calculated for various energies. Fig. 17 and Fig. 18 show the results
of the calculations.
By comparing Figs. 17 and 18 to the results shown in Fig. 9, one
can conclude that the experimentally measured range of protons is
approximately the same as the theoretically predicted range, i.e. 5
to 10 m m in aluminum (that corresponds to 1.5e2 MeV incident a
energy).

3.3. The motion of charged particles in polyethylene (self-

attenuation in foils)

The results obtained for the relationship between the thickness

of polyethylene foils and the count rate due to particle emission by Fig. 19. Proton range in polyethylene as a function of energy.

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3.4. The motion of charged particles in human tissues

The microscopic neutron capture cross-section of the target

nuclides and the nature of the reaction products are two important
factors in determining which element to use for neutron capture
therapy (NCT). The first is connected with the ability of the nuclei
used in NCT to absorb neutrons, while the second is connected with
determining the effectiveness of radiation in killing cancer cells.
According to the data, 10B is a qualified candidate for NCT. As
mentioned in the introduction the neutron capture process occurs
when the non-radioactive target 10B is irradiated with low-energy
(0.025 eV) thermal neutrons or higher-energy (0.5 eV) epithermal
neutrons, resulting in a reaction depending on the position of tu-
mor [47]. Thermal neutrons (0.025 eV) are absorbed by the non-
radioactive isotope 10B atoms which then split into an a particle
Fig. 20. Alpha-particle range in polyethylene as a function of energy. (4He) and a recoiled lithium nucleus (7Li). There are two schemes
for this reaction; 4He and ground state 7Li with 6.3% reaction yield
(total energy of 2.79 MeV), or excited state 7Li (93.7% reaction yield,
total particle kinetic energy of 2.31 MeV) plus a 0.48 MeV prompt
gamma photon that is generated in the process of returning from
the excited state to the ground state. Resultant is the high Linear
Energy Transfer (LET) alpha particle and 7Li ion [48].
Because boron neutron capture therapy is based on the 10B(n, a)
7
Li reaction, the energy of the thermal neutron (0.025eV) and
capture cross section of 3836 b are considered in the calculations.
The range of the produced a-particles in tissues (bone and muscle)
must be assessed. Because 14N(n,p)14C reactions can also occur
during neutron irradiation, the range of protons in tissues should
also be determined. For this “competing” reaction with neutron
energy <0.5 eV the neutron capture cross section is 1.75 b. The total
kinetic energy released in this reaction is Etr ¼ 0.62 MeV, it is shared
by the proton (0.58 MeV) and the 14C nucleus (0.04 MeV) which is a
low-energy b-emitter [47,49].
Fig. 21. Proton range in in bone and muscle tissue as a function of energy. Fig. 21 and Fig. 22 depicted the calculation results. They show
that the range of protons is roughly 10 times that of the a-particles.
The range of a 2 MeV a-particle is less than 10 mm which is
stopped by the sample material if the location is sufficiently far roughly equal to the cell width (the size of a single cell is about
from the emission surface (self-absorption). 10 mm), which is ideal for BNCT, but a proton with the same energy
When the obtained results are compared to Figs. 9, Fig.10, Fig.11, travels further, which is not advantageous. This is why, in order to
Figs. 12 and 13, we can conclude that the measurement represented achieve good BNCT results, a high-quality neutron source and bo-
by Fig. 11 is in good agreement with the polyethylene calculations. ron agent must be used (good accumulation of boron in tumor
However, the range of protons in paper and sticker foil appears to area).
be
longer than that in polyethylene, which could be attributed to 4. Conclusions
the fact that paper and sticker foils have lower densities in terms of
hydrogen atoms. In this study, channel#5 of the NTI-BME 100 kW pool-type light
water reactor and a portable neutron source (Pu(Be)) were
employed to irradiate the examined materials.
The operating characteristics of the applied ZnS(Ag)-detector
were effectively determined using appropriate radiation sources.
Experiments, measurements and approximate calculations
were performed to identify a specific material that would serve as a
carrier for the boron compounds for irradiations via the reactor
irradiation channel. Various common materials were investigated
(aluminum foil, typing paper, polyethylene foil, and sticking foil) in
order to define the types of particles that reached the sensitive
volume of the detector.
To compare, the carrier materials were tested “alone” without
boron compounds to see how they contributed to the measured
count rates when the boron compounds were irradiated. It was
confirmed that the detector's count rate was caused by two pro-
cesses within the measurement uncertainty: the interaction be-
tween the detector and the neutron beam, and the particles
released by the carrier materials.
Fig. 22. Alpha-particle range in bone and muscle tissue as a function of energy. The attenuation and self-attenuation of neutron-induced
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E. Hutli and P. Zagyvai Nuclear Engineering and Technology 55 (2023) 2984e2996

particles emitted by various materials were investigated. Different S.H. Jiang, C.W. Chang, C.S. Liu, S.J. Wang, P.Y. Chu, S.H. Yen, Fractionated BNCT
for locally recurrent head and neck cancer: experience from a phase I/II
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 The identified particles are most likely protons (recoil protons); [12] R.F. Barth, M.G. Vicente, O.K. Harling, W.S. Kiger, K.J. Riley, P.J. Binns,
 The recoil protons can be detected very effectively, even with F.M. Wagner, M. Suzuki, T. Aihara, I. Kato, S. Kawabata, Current status of boron
neutron capture therapy of high-grade gliomas and recurrent head and neck
the aid of such a simple measurement technique. cancer, Radiat. Oncol. 7 (2012) 146e167, https://doi.org/10.1186/1748-717X-
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basis and advances in clinical application of boron neutron capture therapy,
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commit a dose comparable to that of boron capture reactions. E. Boggio, J. Longhino, M. Pisarev, G. Juvenal, M.A. Dagrosa, Experimental
 The range of the protons is significantly more extensive than studies for the personalized application of boron neutron capture therapy to
that of the a-particles, this most probably modifies the dose the treatment of cutaneous melanoma, Therapeutic Radiology and Oncology 5
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of cancer: current status and future prospects, Clin. Cancer Res. 11 (2005)
financial interests or personal relationships that could have 3987e4002, https://doi.org/10.1158/1078-0432.ccr-05-0035.
appeared to influence the work reported in this paper. [19] F.Y. Yang, H.E. Wang, G.L. Lin, M.C. Teng, H.H. Lin, T.T. Wong, R.S. Liu, Micro-
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[20] K. Hanaoka, T. Watabe, S. Naka, Y. Kanai, H. Ikeda, G. Horitsugi, H. Kato,
The first author would like to express his deepest appreciation
K. Isohashi, E. Shimosegawa, J. Hatazawa, FBPA PET in boron neutron capture
to the NTI-BME training reactor staff for their outstanding assis- therapy for cancer: prediction of 10B concentration in the tumor and normal
tance. His appreciation also goes to Dr. L. Duffek, SOTE Department tissue in a rat xenograft model, EJNMMI Res. 4 (2014) 70e79.
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