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Applications of Neutron Generators

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DOI: 10.1007/978-1-4419-0720-2_32

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Chapter 10

Applications of Neutron Generators

J. Csikai, R. Dóczi

Department of Experimental Physics, University of Debrecen, Debrecen, Hungary

Abstract: Miscellaneous applications of low-voltage neutron generators providing 3 MeV and 14 MeV
neutrons via the D-D and D-T reactions, respectively, are reviewed. New experimental
methods are reported, and emerging applications in the areas of prompt and delayed neutron
activation analysis, fast neutron imaging and profiling, irradiation effects, fast neutron
radiobiology, and shielding design are highlighted.

1. INTRODUCTION

In this chapter some applications of low voltage ( 150-200 kV) neutron generators
using 3 MeV and 14 MeV neutrons, produced via the 2H(d,n)3He (D-D) and 3H(d,n)4He
(D-T) reactions, respectively, are discussed. Principles of operation and output charac-
teristics of neutron generators have been described elsewhere (Csikai 1987, 1989, IAEA
1996, 2000). The nuclear methods based on small neutron generators have a great
importance in the development of such new technologies as process and quality-control
systems, exploration of natural resources, detection of illicit traffic materials, trans-
mutation of nuclear waste, fusion reactor neutronics, irradiation effects on biological
and industrial samples, which can be directly utilized in other sciences, in the economy
and society.

2. ACTIVATION ANALYSIS WITH 14 MeV AND 3 MeV

NEUTRONS

Recently, neutron activation analysis (NAA) has been improved by application of

separated isotopes as targets, quick radiochemical separations, corrections for flux
perturbation in the case of bulky samples, high-resolution detectors (Ge(Li), HPGe,
LEGe, Si(Li), Si-avalanche, etc.—for a summary of the properties of LEGe and other
364 Chapter 10

types of Ge detectors see Figure 9 in Chapter 1, Volume 5, on ‘Radiation Detection’)

and better data acquisition as well as processing systems, in addition to the use of high-
efficiency detectors (Bi4Ge3O12, GSO, CsI, PbWO4, BaF2, CdTe, etc.) (Proctor et al.
1999, Dokhale et al. 2001, Hlavac 2001). A typical example of the advantages of high-
resolution gamma spectrometry in elemental analysis is the determination of Si in Al
alloys. (The problems of trace element determination by INNA in aluminum matrix are
touched upon in various parts of Chapter 8 on ‘Activation Analysis’.) The intensity ratio
of the 1.73 MeV and 1.78 MeV gamma lines produced in 27Al(n,)24Na and
27
Al(n,)28Al, 28Si(n,p)28Al reactions, respectively, depends strongly on the Si content in
the Al matrix (see FIGURE 1). Another example showing the importance of high
efficiency gamma-detectors is related to the detection of illicit traffic materials (drugs,
explosives) via the determination of carbon and oxygen, using the respective 4.44 MeV
and 6.13 MeV gamma rays from the (n,n’) reactions.

FIGURE 1. Gamma-ray spectrum of Al and Al + Si mixture. Note that on adding just 1% of Si to Al, the peak
ratio 24Na/28Al changes from about 2/1 to about 1/4.

There are two important new fields of application of fast neutrons in elemental
analysis: determination of chemical compounds by measuring the atomic ratios of the
composite elements and the correlations between them, and studies of the interaction of
secondary energetic charged particles (p, , t, d) with their chemical environment
(hot atom chemistry) and the role of secondary reactions in activation analysis of light
Applications of Neutron Generators 365

elements such as Li, Be, B, and C. Considerable progress has been made in the
knowledge of decay data for radioactive products (IAEA 2002) and the possible
interfering reactions and gamma lines from fast neutron reactions, as presented in
Appendix 3 of this Volume.
The activation expression related to the decay of a single state should be extended to
a more general case in which ground and isomeric states are produced and the ground
state activity is used for the analysis. Such a typical case is the 58Ni(n,p) reaction in
which the 58m+gCo isomeric pair is produced and the activation analysis is based on the
decay of 58gCo. Some decay modes of the radioactive atoms are demonstrated in
FIGURE 2.

FIGURE 2. Typical decay modes involving metastable (m) and ground (g) states.

If the final nucleus has an isomeric state, which can also populate the ground state
via an isomeric transition IT with a branching ratio , then the differential equations for
the two states are as follows

dN m dN g
 Φ m n   m N m and  Φ g n   g N g    m N m (1)
dt dt

where , n, g, m, g and m are the neutron flux density, the number of atoms to be
determined in the sample, decay constants of the nuclei produced in ground and
metastable states, and the corresponding cross sections, respectively.
If the activity is measured via the decay of ground state atoms as a function of
cooling time, tc the Ng(tc) function is given by

 ( m    g )    
N g (tc )  Φn   m   (1  e   t )e   t   m   (1  e   t )e  
g i g c m i mtc
 (2)

 g m  g  m  g 

366 Chapter 10

where tc and ti are the cooling time and the irradiation time, respectively.
For example, in the case of 58mCo  = 1 and the ground state decays by a 810 keV
gamma-line. By measuring the peak area of this line as a function of cooling time the
m/g ratio can be deduced. It follows from Eq. (2) that the intensity function Ig(tc) is
given by the following expression

 g t c
I g (t c )  Φ n ( Ae  Be   t )
m c
(3)

i.e. the measured intensity is approximated by the sum of two exponential functions.
The pre-exponential constants, A and B, contain the m and g values as unknown
parameters. In the knowledge of the isomeric cross sections, the decay parameters, the
irradiation and measuring conditions the number of atoms of a given element, n can be
determined. In some cases  g <<  m and tc is high then Ig(tc) is given by a single
exponential function, i.e. by the first term in Eq. (3).
Investigations on the sensitivity, accuracy, interfering reactions and gamma-lines
lead to the conclusion that neutron activation analysis based on small accelerators
requires the use of thermal, resonance and fast neutrons depending on the element to be
determined in different matrices. In this case the D-D and D-T targets are surrounded
with hydrogenous moderators. Thermal (TNAA) and epithermal (ENAA) or resonance
neutron activation analysis as well as the capture gamma-ray techniques are favored
over the fast neutron (FNAA) method for the following elements: Dy, Eu, In, Mn, Lu,
Au, V; U, Th, Rb, Sr, Mo, Sb, Cs, Ba, Ta, Tb; H, Be, B, N, O, S, Ni, Cd, Gd, Eu.
It should be noted, however, that the method to be chosen for NAA depends also on the
type of the detector. The RNAA is favored over TNAA for example for Ni, Zn, Rb, Sr,
Sb, Cs, Tb, Ta, Th and Mo, Ba, Gd, Tm, Yb, Hf, U if a GeLi, HPGe and a Low Energy
Photon (LEP) detector is used, respectively.
Though there are less interfering reactions and gamma-lines for the reactions
induced by the 3 MeV D-D neutrons as compared to the 14 MeV D-T neutron reactions,
the latter is recommended for NAA because of the much higher neutron yield and the
availability of the multi-elemental analysis via the many open reaction channels.
The specific activity expected from the principal reactions at En = 14.5 MeV was
calculated using the recommended nuclear data (Bődy and Csikai 1987). The specific
activity in Bq/g was calculated for the reactions of maximum yield of each element,
assuming a reasonable flux  = 109 cm–2 s–1 and irradiation time ti = 1 h. Nuclear
processes proposed for the determination of each element together with the possible
interfering reactions are summarized in Appendix 3 of this Volume.
Recently, large efforts have been carried out for the determination of the thermal
neutron flux perturbation factor in the case of bulky samples of unknown composition
(Csikai et al. 2002b). The flux perturbation factor, F is defined by the following relation
F  Φ Φ0  , where Φ and Φ0  denote the average thermal neutron fluxes in the
sample and in a moderator material of similar volume, respectively. It was found that
the flux distribution  (x) both in thin (Buczkó and Borbély 1978) and bulk (Csikai
et al. 2002b) absorbing samples can be described by the following expression
Applications of Neutron Generators 367

2 1
Φ ( x)  (a x  b x  c) (4)

where x is the distance from the surface of the sample while a, b and c are fitting
parameters. According to Eq. (4) for the determination of the  (x) function it is
sufficient to measure the flux value only in three positions, e.g. at x = 0, x = d/2 and
x = d for a sample of thickness d. In the knowledge of the  (x) function the average
neutron flux is given by
d
1
d 0
Φ  Φ ( x) dx . (5)

The unperturbed flux density Φ0  must be measured in the same positions using
activation detector foils and replacing the sample with the moderator material.
The spatial distribution of the thermal neutron flux around a point source changes
significantly for hydrogenous moderators which prevents the use of TNAA for bulky
samples. In the case of graphite moderator the thermal neutron flux distribution changes
only slightly, assuring an almost constant flux density for irradiation of bulky samples
whose size is on the order of 10×10×10 cm3.
The semi-log plot of F as a function of thickness d is linear both for graphite and for
hydrogenous moderators, i.e. the following simple equation

Φ
F  F0 e  K d (6)
Φ0 

can be used for the determination of the flux perturbation factor for both thin and bulky
absorbing samples of unknown compositions if K is determined by experiment.

After determining F the corrected activity  A0  at the end of irradiation time ti is

given by
 A
 A0    Φ0  n (1  e   t ) i
(7)
F

where  A is the activity of the sample produced by the average activating flux, Φ. It
should be noted that the correction for the flux perturbation can be neglected neither for
bulky nor for thin samples if they contain absorbing elements. For the elemental
analysis of thin absorbing samples hydrogenous moderators are recommended. For
bulky samples, however, the graphite moderator is better. The attenuation of 3 MeV and
14 MeV neutrons in different samples is discussed in Appendix 3 of this Volume.
In practice, the  (E) function in a given point inside the sample is determined by
the unfolding method using a set of activation threshold detector foils. The most
commonly used dosimetry reactions are also summarized in Appendix 3. With the
368 Chapter 10

knowledge of the  (E) and  (E) functions the differential and spectrum-averaged
reaction rates, R(E) =  (E) (E) for any element can be determined. A method based on
the combination of physical integration and activation threshold detectors was
developed by Csikai et al. (1988) to determine the volume-averaged activity produced
by neutron-induced reactions.

3. PROMPT RADIATION ANALYSIS

In addition to NAA, neutrons are widely used in prompt radiation analysis for the
determination of concentration and spatial distribution of elements in different matrices.
For example, a track-etched detector (LR-115, Makrofol KG, CR 39, mica) placed on
the polished surface of a sample is irradiated with fast or thermal neutrons then etched
with a suitable chemical to deduce the concentration profiles from the track
distributions. This method can also be used for the detection of suspended and dissolved
U, Th and Pu in water by (n,f) reactions; N in polymers by the 14N(n,p)14C reaction; B
and Li in semiconductors or glasses by the 10B(n,)7Li and 6Li(n,)3H reactions,
respectively. For the detection of fission fragments the use of mica is recommended.

3.1 Neutron methods

Neutron absorption, moderation and reflection methods are also widely used in
elemental analysis of bulk samples, especially for the determination of hydrogen and
moisture content. A systematic study had shown that the relative number of excess
neutrons  = (I − I0) / I0, measured with (I ) and without (I0) a reflector (see FIGURE 3),
depends linearly on the hydrogen content of liquid, powder and solid samples up to
about 1 cm thickness, i.e.
  s H   (T ) (8)

where H is the hydrogen content in wt.%, s is the slope of the -H calibration function
and  (T) is the matrix effect (Buczkó et al. 1975). For the determination of the relation
expressed by Eq. (8) for the given source-sample-detector geometry a combination of
reflector with thin polyethylene (PE, composition: CnH2n+2) layers was recommended
(Csikai et al. 2002a).
Applications of Neutron Generators 369

FIGURE 3. Neutron reflection arrangement.

The concept of the reflection cross section of thermal neutrons  as a microscopic

parameter for the characterization of the reflection property of substances has been
introduced (Csikai and Buczkó 1999). The relation between ,  and the surface
density of atoms is given by
n 
  Nd   (9)
S

where n is the total number of atoms in the sample, N the number of atoms per cm3, S
the surface of the sample in cm2, and d is the thickness of the sample in cm. The
quantity Nd = m NA /(M S) is obtained from the mass of the sample (m) and the molar
mass of the element (M), where NA is the Avogadro constant (see Appendix 2 in
Volume 1). If the reflector consists of molecules the following formula can be used

nmolec  vi  i
nmolec  molec
  i
(10)
S S

where nmolec is the total number of molecules in the sample and vi is the number of
atoms of type i with cross section i in the molecule. The cross-correlation between the
 values deduced from the  molec data obtained for different compounds has proved
370 Chapter 10

that the reflection cross sections are additive. For a mixture of elements the averaged
molar mass of the elements should be used, i.e.

m i
M   i
(11)
m
i Mi
i

where mi and Mi are the mass and molar mass, respectively, of the element of type i in
the target. The values of cross sections for elements, organic and inorganic compounds
as well as for different combinations of metal layers are given by Csikai and Buczkó
(1999), Király and Csikai (2000), and Csikai et al. (2002a). These data are useful for
different applications of neutrons, like quality control of organic and inorganic
compounds; bulk hydrogen analysis; atomic H/C ratio for the detection of illicit drugs,
explosives and qualification of fossil fuels; assay of nuclear materials in solutions
(Mohapatra and Reddy 2001); validation of neutron data libraries (NEA 1994). For
example, it follows from the relation that the measured cross sections for hydrogenous
materials, such as crude oil, coal, illicit drugs, normalized to the number of carbon
atoms present in the molecule as a function of the H/C atomic ratio exhibit a straight
line (Jonah 2001). The calibration equation can also be determined from the excess
counts  = s(nH/nC) + 0 measured for different hydrocarbons.
It is worth noting that the determination of hydrogen in bulk materials has great
importance in many areas (NEA 2001), e.g. hydrogen in metals and alloys causes
structural weakness in the components of heavy-duty systems (aircraft, engines,
missiles, pipelines of nuclear and chemical plants). Metal hydrides are applied in
various fields of science and technology (electricity, propulsion, battery, food, nuclear
fusion, etc.).
Both pulsed-neutron backscattering combined with time-of-flight (TOF; see later)
measurements and the elastic scattering of neutrons can be used for the detection of
light elements. Scattering signatures measured for multi-element samples were analyzed
to determine atom fractions for H, C, N, O and other elements in different objects by
using a combination of TOF and pulse height measurement (Buffler et al. 2001). Simple
backscattering spectrometry is based on the fact that the broad spectra of neutrons from
Pu-Be, 252Cf and 9Be(d,n) sources can cover a large energy interval (1.5-10 MeV) of the
elastic scattering cross sections (EL) of light elements like C, N and O as the major
constituents of a number of organic and inorganic compounds. Therefore, the spectral
yields of backscattered neutrons are affected by the structures present in the EL(En)
functions. The measured spectral yields and the calculated energy dependence of the
reaction rate, R(En) indicate the different structures in the EL(En) functions for C, N, O
(Csikai and ElAgib 1999). An improved neutron backscattering technique based on the
combination of a  1.5 ns wide pulsed beam of 550 keV and the TOF technique at 150°
scattering angle was applied for the detection of C, N and O from different samples
(Aoki et al. 2000).
Applications of Neutron Generators 371

3.2 Gamma-ray methods

Recently the neutron induced prompt gamma emission method (also called prompt
gamma neutron activation analysis or PGNAA) is widely used in on-line bulk elemental
analysis, especially for the identification of explosives and illicit drugs. This method is
not restricted to the use of prompt gammas emitted in radiative capture or (n,γ) reaction
of slowed-down neutrons, but is extended to the fast-neutron (n,xγ) reactions with
x = (n, p, ), in which characteristic gamma rays are also produced. Among the (n,x)
type reactions the inelastic neutron scattering (n,n’γ) is the most common in elemental
analysis. The (n,γ) and (n,xγ) reactions are quite complementary to each other. For
example, the (n,γ) cross section is low for Li, Be, B, C, N, O and also for Na, Mg, Al,
Si, while the (n,xγ) reaction yields are very high and the produced gamma rays specific
to these elements. Therefore, prompt gamma rays produced in thermal, epithermal and
fast neutron interactions are all used for the elemental analysis of bulk media
(Watterson et al. 1995). A typical example is the inspection of waste containers by
irradiation with low-energy neutrons. The prompt gamma rays emitted in the de-
excitation of fission fragments of actinide materials are measured with an array of
HPGe detectors. The actinide isotopes are identified by observing selected gamma rays
emitted from the fragments in pair-wise coincidence (Smiths and Micklich 2000).
Pulsed 14 MeV neutron generators with neutron pulse width in the s and ns regions
have also been developed for analysis of bulk media and for borehole logging (Clayton
and Wormald 1983, Schweitzer et al. 1988). The high penetrability of fast neutrons and
energetic gamma rays renders the multi-elemental analysis of bulk (m >> 1 kg,
V >>1 dm3) samples possible. In addition to the identification of explosives and illicit
drugs by the detection of the 4.44 MeV and 6.13 MeV gamma rays emitted in the
12
C(n,n’γ) and 16O(n,n’γ) reactions, respectively (Gozani 1994, Vourvopoulos 1994,
Viesti et al. 1999), the on-line analysis is applied for example at coal mines, coal
preparation plants, and coal-fired power plants. Concentrations of H, C, O and N give
information on caloric value, S on environmental pollution, Cl on corrosion of boiler,
Al, Si, Ca and Fe on ash content.
The combination of the sealed tube accelerator with the associated alpha-particle
method (APM), illustrated in FIGURE 4, has great importance in the analysis of bulk
samples, verification of chemical and nuclear weapons, in-vivo analysis of human body
element contents, and three-dimensional elemental analysis in solids. The time spectrum
measured by the APM suggests that about 90% of the gamma rays of interest for prompt
gamma-ray analysis are emitted from the 12 cm thick surface layer of solids in less than
10 ns after the neutrons hit the sample. Considering the attenuation of neutrons and
gammas in the sample the PGNAA technique can give representative information on a
few 10 kg of the samples. Some recommended reactions for bulk-media assay by
prompt gamma-ray analysis using thermal and fast neutrons are summarized in
Apendix 3 of this Volume.
372 Chapter 10

FIGURE 4. Combination of the sealed tube accelerator and the associated alpha-particle method (APM).

Among the gamma-ray methods pulsed fast-thermal neutron analysis (PFTNA)

plays an important role. The PFTNA method (Gozani 1994, Vourvopoulos 1994) is
based on 14 MeV neutrons with 10 s pulse duration and 10 kHz frequency produced
by a sealed tube D-T generator. The gated signals from the gamma rays emitted during
and between the neutron bursts are routed separately into two channel regions of an
MCA. The 4.44 MeV and 6.13 MeV gamma rays are recorded in the prompt region
while the 2.23 MeV gamma rays from the H(n,) reaction induced by the neutrons
thermalized in the sample volume are measured between the pulses. Two devices based
on this method, namely PELAN (Pulsed Elemental Analysis with Neutrons) for the
detection of explosives and NELIS (pallet inspection system) for the observation of
illicit drugs are promising. Advantages and limitations of this technique are discussed in
detail in a recent publication (Dokhale et al. 2001).

3.3 Specific applications

The prompt and delayed gamma rays produced in 14 MeV neutron bombardment of
rocks were published by Przewlocki et al. (1984). In the case of such complex samples
a number of interfering reactions and gamma-lines are produced. Separation between
different elements can be improved by the combination of the D-D and D-T reactions.
For example, the (n,n’) reaction cannot be performed by the 3 MeV D-D neutrons on
12
C and 16O. The use of associated particle timing based on the D-D reaction has been
demonstrated for elemental analysis of bulk samples such as the human body (Evans
et al. 1997). The nanosecond timing of a HPGe detector rendered it possible to identify
the spatial origin of the measured gamma rays. The major elements in most rock types
are Si, O, Al, Fe, Mg, Ca, Na, K, Ti and P. Concentrations of these elements in the well-
known terrestrial rocks vary from 1 to 4 orders of magnitude, therefore, careful
Applications of Neutron Generators 373

investigations are needed to develop the most suitable methods for the elemental
analysis of minerals, standard geological materials, lunar soil samples, processing
solutions or slurries and ocean bottom cores (Csikai 1992).
TABLE 1. Typical applications of neutrons in elemental analysis.

Field Elements (matrices)

N, O, F (alloys);
O (refractory and nonferrous metals);
Metallurgy
Al, Si, P, Mg (cast iron, Al, Si-compounds);
Al, Si, K (tungsten)
N, O, P, Al, Cl (explosives and propellants);
N, O, Na, P (organic compounds and polymers);
Chemistry
Cl, I (emulsions);
N, P, K (fertilizers)

Electronics N, O, Si, Al, Ti, P, Zn, Cr, Fe, Y, Zr, Eu, Ba, Dy (oxides, circuit boards, thin films)

N, Na, P, Cl, Ca (whole body);

N (proteins, fossil bones);
Biology N, O, P, Ca (mixed feeds);
N, O, K, Cl, Ca, Fe (plants);
F, Na, Si, S, Ca, Fe, Ti, Sr, Ba, Hg, Pb (air-dust, fly ash)
O, Al, Si, Fe (lunar rocks);
H, O, Na, S, Cl, V, Mn, Ni (crude oils);
Geology/mining/ U, Th (rocks);
space sciences O, Mg, Al, Si, Fe (sea cores);
H, O, Al, Si (zeolites);
H, C, O, Al, Si, Fe (coals)

The conventional neutron methods are the neutron-epithermal neutron, neutron-

thermal neutron and the neutron-gamma procedures. In all three cases, rocks are
bombarded by fast neutrons and either epithermal or thermal neutrons or gamma rays
from radiative capture are registered. Both pulsed and stationary neutron sources are
applied to these measurements (Berg and Jacobs 1983, Morris et al. 1983, Tittle et al.
1985, Demény et al. 1988, Mills et al. 1991). The pulsed time-of-flight (TOF) prompt
gamma-ray analysis has been successfully applied by a number of authors, especially to
the measurements of light elements (Sawa 1993, Brown et al. 1994, Gozani 1994,
Vilaithong et al. 2000).
Nuclear techniques based on neutrons from radionuclidic (252Cf, Pu-Be, Am-Be) or
small accelerator sources are successfully used in elemental analysis of bulk samples
including the detection of illicit traffic materials in airline luggage (suitcases, briefcases,
small boxes) by identifying H, C, N, O, Cl as major elements of these objects (Dokhale
and Hussein 1997, Evans et al. 1999, Csikai et al. 2001). The atom fractions of these
elements, in particular the C/O, C/H and C/N ratios are quite different for drugs
(cocaine C17H21NO4, morphine C17H19NO3, heroine C21H23NO5) and explosives
374 Chapter 10

(nitroglycerin C3H5N3O9, TNT C7H5N3O6, RDX C3H6N6O6) as compared to other

materials (sugar C12H22O11, alcohol C2H6O, melamine C3H6N6). Recently, a
comprehensive review on the possible use of neutron methods for the detection and
identification of explosives and drugs has been published (Cinausero and Viesti 2000).
There are many more new fields in the utilization of neutrons produced mainly by
small D-D and D-T accelerators (IAEA 2000). Some typical fields of activation and
prompt radiation analysis are summarized in TABLE 1.

4. NEUTRON IMAGING AND PROFILING SYSTEMS

The various applications of neutron radiography (reactor technology; rocket and

missile technology; medical and biological investigations; inspection of plastic coating,
gaskets, and turbines) have been extended for many new fields during the last three
decades. The main advantages of neutron radiography (NR) are the ability of revealing
many low-density media (water, oil, plastic) inside dense materials such as steel, Pb, Zr,
U; high penetrability; high sensitivity for certain elements (H, B); discrimination
between elements of similar atomic weight and physical density; discrimination
between different isotopes of the same element (10B, 11B, 113Cd, 114Cd); and applicability
for highly radioactive objects, e.g., fuel elements (Csikai 1987). It is impossible to cover
all the new applications in a short review, therefore some results on the neutron depth
profiling and imaging systems are intended to be discussed.
The nanosecond pulsed beam with time gating at the detector and the associated
particle method (APM) render the three dimensional (3D) elemental analysis of solids
possible (Overley 1987, Rynes et al. 1999). The APM is based mainly on the D-D and
D-T reactions by the detection of 3He and 4He particles, respectively, emitted at  180°
to the neutron direction. The 4-5 cm/ns travel time of the neutrons allows the imaging of
the interrogated volume along the direction of the ns pulsed neutrons with a spatial
resolution of  5 cm. Some 2D-3D fast neutron imaging principles and techniques are
summarized by Gozani (1994), Mikerov et al. (1998, 2001), Chen and Lanza (2001),
while typical thermal neutron radiography systems are demonstrated by Balaskó et al.
(1988, 2001) and Shaikh et al. (1998, 2001).
Fast neutron resonance radiography (NRR) used by Chen and Lanza (2001) for
elemental mapping is based on a hydrogen-rich plastic scintillator to detect the transmit-
ted neutrons of 2 MeV to 6 MeV energy. Different energies of neutrons were obtained
by rotating the object detector assembly around a D-D source based on a 5 MV Van de
Graaff accelerator. Monoenergetic neutrons in the 1.5 MeV and 2.5 MeV ranges could
also be obtained from the 7Li(p,n)7Be reaction with a 10 m thin Li target. Light from
the scintillator is recorded by a charge coupled device (CCD) camera to form a
radiographic image. (Editors’ note: Charge coupled devices are silicon chips containing
a matrix of potential wells that can trap electrons released by radiation. Since the size of
the potential wells is only a few m, they have good spatial resolution, a useful feature
for electronic imaging.) The structures in the energy dependence of the total cross
sections, T(En), below 6 MeV render the distinction between light elements possible.
Applications of Neutron Generators 375

The 2D images were formed using a 1 cm thick BC-430 plastic scintillator lens-coupled
system with a cooled CCD camera which used a 1242×1152 pixel CCD.
Recently, investigations on the realization and prospects of real time fast neutron
radiography with a portable sealed tube D-T neutron generator with a yield up to
1010 s−1 and a luminescent CCD detector were published (Mikerov et al. 2001). The
major components of the detector are shown in FIGURE 5: fast neutron screen prepared
from hydrogenous polymer mixed with powder luminophor (Gd2O2S:Tb), image
intensifier, CCD matrix and fast lens system. Efficiency of disperse fast neutron screens
and the effects of X-ray emission, scattered neutrons and geometry of measurements on
the quality of the image are also described.

FIGURE 5. Fast neutron luminescent CCD-detector on the basis. 1 - CCD-matrix, 2 - lens system, 3 - mirror,
4 - luminescent screen, 5 - sample, 6 - image intensifier.

Dynamic neutron radiography (DNR) measurements were performed (Balaskó et al.

2001) at the thermal channel of the 10 MW Budapest Research Reactor with a
collimator ratio L/D = 170. The 108 cm–2 s–1 thermal neutron flux at the sample position
of a beam with diameter of 150 mm and the 40 ms imaging cycle rendered the medium
speed movements up to about 2.4 m/s possible. The light from an NE 426 converter
screen was detected by a high sensitivity video camera. The neutron images of
 200 m resolution were displayed on a monitor and stored by an S-VHS recorder.
This neutron imaging system provides a unique possibility to visualize various
hydrogen-containing materials inside closed objects. A similar electronic imaging
system based on a commercially available image intensifier tube and a low-cost CCD
camera has been used (Shaikh et al. 2001) for visualization and analysis of water/air,
water/vapor two-phase flow inside metallic pipes under high temperature and pressure
conditions. Most of the cladding metals such as aluminum or steel are transparent to
neutrons while hydrogenous materials such as water are relatively opaque which makes
neutrons a unique tool for visualizing the flow pattern. The fully automated neutron
radiography system (DIANE) based on a sealed tube neutron generator is commercially
available (Cluzeau et al. 1994). The necessary exposure fluence is about 1012/m2 which
376 Chapter 10

can be produced at a 3 m source-object distance within 1 min by an intense neutron

generator of 5×1012/s output rate.

FIGURE 6. Schematic view of the experimental setup and principle of NERD used for depth profiling.

Associated particle timing based on D-D neutrons was applied successfully (Evans
and Mutamba 2002) for imaging an aluminum box. A combination of a Si detector for
charged particles and an NaI(Tl) scintillator for induced gamma rays yielded a time
resolution of 0.4 ns assuring a spatial resolution of better than 1 cm.
Knowledge of the concentration and spatial distribution of hydrogen in solids is
required in many fields of science and technology. Therefore the development of such a
hydrogen depth profiling method by which over 100 m depth can be analyzed is
indispensable. The drawback of elastic recoil detection and resonant nuclear reaction
methods is that the depth is limited to several m and serious radiation damage may
occur. However, a fast neutron beam as a probe via the H(n,p) reaction is non-
destructive and can extend the depth to be analyzed beyond 100 m. The energy
distribution of recoiled protons is related to the depth profile of hydrogen. A fast
neutron profiling method is based on the combination of an imaging plate (IP) and a
polyethylene film as a converter. An experimental setup for the depth profiling is shown
in FIGURE 6. Using an appropriate neutron energy in the 5-15 MeV interval and a
converter thickness close to the proton range fairly clear images could be obtained
(Miura et al. 2000, Sanami et al. 2000).
Applications of Neutron Generators 377

5. FAST NEUTRON IRRADIATION EFFECTS IN SOLIDS

Recently, both steady-state and pulsed fast neutron generators have been applied to
the investigation of radiation damage of metals, alloys, semiconductors and high Tc
ceramics and to nuclear heating of superconductors by prompt reaction products and
long-lived radioisotopes. Of the wide range of applications a few typical examples are
discussed in this review (Csikai 1995).
The irradiation of solids with fast neutrons results in the displacement of atoms from
their lattice sites; the resultant interstitials and vacancies can cause various radiation
damage phenomena. In addition, the determination of H and He gas production as well
as the neutron multiplication by 14 MeV-neutron-induced (n,p), (n,) and (n,2n)
reactions, respectively, in the construction materials of fusion reactors is very important.
Studies on the tritium breeding and outgassing efficiency for different blanket materials
are also important tasks.
Some physical parameters related to the radiation effects which can be studied with
small neutron generators are as follows.
Determination of the average range of recoil atoms by measuring the activities (A)
of catcher foils placed on the surface of a sample of thickness d. (Note that r is used for
the range of recoil atoms instead of the usual notation of R. The reason for this is that
the latter could be confused with the reaction rate which is also denoted by R.) The
mean projected range r  of recoil atoms in forward and backward directions are given
by the ratios of the released to the produced radioactive atoms i.e.  rf   ( Af / At )d and
 rb   ( Ab / At )d , where At = Asample + Acathcer while the mean range r  is obtained
from  r   [( Af  Ab ) / At ]d . The mean range of recoil atoms is between 10 and 1000 nm
in 14 MeV-neutron-induced reactions. Both the mean range and the value of d are
customarily given in mg/cm2. These data are also important for the elemental analysis of
thin layers at which the released atoms should be taken into account. Therefore, for the
elemental analysis of thin layers by neutron-induced reactions the knowledge of
the r  vs. d function is required.
For the investigations on the release of foreign and lattice atoms by diffusion or
evaporation from metals and alloys the activated sample is placed into a vacuum
chamber and the released radioactive atoms are collected by catcher foils. The activity
of these foils is measured as a function of time at different sample temperatures. Data
on the release of alloying elements from metallic compounds and alloys are required not
only by solid state physics but also by high-tech industry and fusion technology.
The diffusion coefficients of tracers and the displacement of lattice atoms and their
activation energies can also be measured (Sudár et al. 1977). Using fast neutrons
radioactive tracers can be produced homogeneously in extended samples. For example,
the measurement of the diffusion coefficient of the 24Na produced in 27Al(n,) reaction
for different alloys has a great practical importance, because a number of alloys used in
reactor technology contain aluminum (e.g. the reactor fuel can).
Production rates of total hydrogen and total helium are important parameters in the
evolution of the microstructure during the irradiation of solids, especially for fission and
fusion reactor construction materials. These data can be measured by using a vacuum
378 Chapter 10

furnace equipment connected to a mass spectrometer for the detection of H and He

gases produced in an irradiated bulk sample.
The production rate and the outgassing efficiency of tritium for different Li, Be, B
compounds and alloys used as blanket or structural materials (e.g. lithium-vanadium,
lead-lithium and ceramic breeder, TiBe12) can be determined for fusion neutrons by
using small neutron generators, even for the EURATOM Fusion Project (Gasparotto
2002). Data for the outgassing efficiency as a function of heating time and temperature
for different samples are required. In addition, the behavior of hydrogen in metals can
also be investigated by using deuterium and tritium as tracers. Studies on deuterium and
tritium as substitutes for hydrogen in solids are of considerable interest to a better
understanding of the depth profile, trapping, reflection and diffusion of hydrogen
implanted into different samples like metals, semiconductors, metallic glasses, or high
Tc ceramics. For deuterium the retention kinetics, concentration profile and the
saturation yield can be determined via the 2H(d,p) and 2H(d,n) reactions (Csikai et al.
1997).
Studies of the effect of 14 MeV neutron irradiation on semiconductor electronic
components have an essential role because many electronic instruments are used in
intense fast neutron fields. Radiation effects can be observed at a fast neutron fluence in
the order of 1010/cm2 at 20°C. Changes in the main characteristics of electronic circuits
depend strongly on the type of semiconductor components. For example, definite
changes were observed in the operating characteristics of Si(Li) detectors, diodes,
transistors and integrated circuits after the irradiation with 14 MeV neutrons up to
 1013/cm2 fluence. Further investigations are needed to study the effect of self-recovery
of the irradiated Si(Li) detectors and integrated circuits.
Irradiations of optical components (laser glasses, fiber optics) to measure any effects
of 14 MeV neutrons on light transmission or the index of refraction was carried out in
the last decades (Heikkinen 1989). Studies on the effect of fast neutrons on electro-
optical components are also required.
On-line and off-line investigations are in progress to study the effects of fast
neutrons in solids using fluences in the range  1018/cm2 - 1015/cm2. Samples and
physical properties to be studied are as follows: metals and alloys (mechanical,
microstructure, electrical resistivity); superconductors (critical current, temperature and
field); insulators (electrical and mechanical properties).
In recent years various types of high Tc superconducting ceramics have been
developed. Studies of the effects of fast neutrons on the physical parameters of high Tc
superconductors are of interest both for basic research and applications. In the case of
multiphase YBa2Cu3O7 and Tl2CaBa2Cu2O8 ceramics a fluence of about 1014/cm2 can
cause a definite change in the physical parameters (Bódi et al. 1994), e.g. both the
specific resistance R/R293 and the microwave absorption of the sample decrease
significantly. A systematic investigation on the oxygen content of high Tc ceramics is
also required. This can be measured with high accuracy by the detection of the
6.13 MeV gamma line produced in the 16O(n,p)16N reaction.
Applications of Neutron Generators 379

6. RADIOBIOLOGY WITH FAST NEUTRONS

Neutrons are of interest for cancer therapy because they produce protons and other
densely ionizing particles (alphas, recoil nuclei) in tissue. The use of fast neutrons in
cancer radiotherapy was stimulated by three radiobiological findings: the oxygen
enhancement ratio (OER); the sensitivity of cells at different phases of the cell cycle;
the contribution of sublethal damage to cell reproductive death. Neutrons have
advantages to treat those types of tumors which contain anoxic cells. The variation in
radio sensitivity of cells in different phases is less for neutrons than for X-rays.
The relative biological effectiveness (RBE) of neutrons is generally higher in tumors
than in normal tissues. Taking into account the cross sections at 14 MeV and
abundances of H, C, N and O in tissues, about 65% of the absorbed dose is due to
neutron-proton elastic scattering. Therefore, the absorbed dose is proportional to the H
content of the organs, i.e., it is about 15% higher in fat tissue than in muscle ones, while
it is much lower in bones.
The radiation therapy in practice requires from the neutron source a high dose rate,
good depth dose, well defined horizontal and vertical beams movable around the
patient, and a variable beam size up to about 20×20 cm2. In addition, an average neutron
yield of 4×1012/s, as well as 125 cm specified source-screen distance (SSD), and 2 cm
maximum source diameter are needed for cancer therapy. A typical treatment schedule
for malignant diseases involves two fractions per week, modal tumor doses of
1.2-1.3 Gy per fraction and total doses in the range of 14-21 Gy.
In order to estimate the induced activity, the neutron dose value and the effect of
interfering reactions, the distributions of thermal, epithermal and fast neutron flux
densities should be determined in a bulk media or a phantom. The most commonly used
dosimetry reactions are given in Appendix 3 in this Volume. In the case of a phantom
the combination of the activation detectors and the physical integration methods is
recommended for the determination of the volume averaged dose equivalent rates and
through it the total dose absorbed by a given organ (Csikai et al. 1988).

7. NEUTRON ATTENUATION AND SHIELDING

Neutron moderators, filters, absorbers and shielding are used in many devices and
facilities of experimental nuclear and high-energy particle physics and in nuclear
technology as well. Extended neutron transporting media are considered in some large-
scale projects like on-line analysis of bulky geological samples, such as coal and
minerals (Watterson 2000), bulk hydrogen analysis using neutrons (IAEA 1998, 2001),
design of blankets of fusion reactors, development of accelerator-driven transmutation
of nuclear waste (NEA 2002, Reimer 2002), checking of neutron transport calculations
for shielding, effects of nuclear weapons, etc.
380 Chapter 10

FIGURE 7. Setup geometries for leakage spectra measurements (1.2 ≤ En ≤ 15 MeV).

The characterization of the transport and the estimation of the radiation-induced

damage and activation inside the medium require the knowledge of the expected
neutron spectrum at each point of interest or of the average value over a large volume of
the materials to be investigated. The above bulky units are typically planned on the
basis of detailed Monte Carlo transport calculations using cross sections taken from
different libraries. The consistency of the data used in the calculations can be checked
experimentally by leakage spectrum measurements using simple geometries and known
spectra of primary neutrons.
Applications of Neutron Generators 381

FIGURE 8. Measured and calculated leakage spectra of 2H(d,n) source neutrons for Al slabs at Ed = 9.4 MeV.

The leakage spectra of neutrons depend on the integrated density of the elements
present between the neutron source and the detector, and on the interaction cross
sections. A Pulse Height Response Spectrometer (PHRS) based on a relatively small
volume of NE213 liquid scintillator with neutron-gamma discrimination can be used to
measure the spectral yield of leakage neutrons in the 1.2-15 MeV range (Oláh et al.
1998), in addition to the multiple foil activation method. The latter has advantages in
the determination of the spectral yield especially in the Eth  En  3 MeV interval. Slabs
and spheres of the most important shielding, construction, biological and geological
materials are used in these studies. The use of quasi-monoenergetic 2H(d,n), 3H(d,n)
neutrons and broad spectra of 9Be(d,n), 252Cf, Pu-Be source neutrons can assure the
integral tests of the differential data. Recently, the backscattering spectrometry as a tool
for elemental analysis of bulky samples based on the broad spectrum of Pu-Be neutrons
has been investigated (Csikai and ElAgib 1999). The broad spectrum of Pu-Be neutrons
can cover a large energy interval (1.5-8 MeV) of the elastic scattering cross sections
(EL) of C, N and O. Therefore, the spectral yields of backscattered neutrons are
affected by the structures present in the EL(En) functions and so the reaction rate versus
incident neutron energy is given by R(En) = Y0(En) EL(En), where Y0(En) is the relative
yield of the source neutrons while the EL(En) data are taken from different libraries.
The geometrical arrangements used for a neutron leakage and backscattering spectro-
metries are shown in FIGURE 7. Some typical spectra compared with the calculated
values are shown in FIGURE 8.
382 Chapter 10

Among the neutron sources the low voltage (100-200 kV) D-T 14 MeV generators
play a special role in many applications (standard cross sections, activation and prompt
radiation analysis, irradiation effects, radiography, well logging, shielding). Therefore,
the flux density distributions of thermal and primary 14 MeV neutrons have been
measured in different source-sample-detector geometries and calculated for different
configurations of bulk samples (Ali et al. 1995). On the basis of these results the
differential and integrated reaction rates as a function of sample thickness could be
determined.

FIGURE 9. Neutron flux fraction and reaction rate vs. neutron energy for a 2H(d,n) source.

The removal cross section is a useful parameter for the characterization of the
attenuation property of shielding materials. The flux of neutrons of energy E from a
point source is given by
e Σ (E)x
Φ ( x, d , E )  Y (12)
4d 2 π

where d, Y, x, and  are the distance from the source (cm), the source strength (s–1), the
shield thickness (cm), and the macroscopic removal cross section (cm−1), respectively.
Using either the activation or the PHRS methods the value of ln( d 2) plotted against x
results in a straight line from the slope of which Σ can be determined for different
geometries and energies. The samples, in general, are slabs with dimensions of
30×30 cm2 and disks of 30 cm diameter. The thickness is changed in the range
0  x  25 cm. The values of macroscopic removal cross sections of fission, 14 MeV
and 3 MeV neutrons for elements and some compounds are given in the literature
Applications of Neutron Generators 383

(Nargolwalla and Przybylowicz 1973, Csikai 1987, 1995). A comparison of the 

values measured by TOF technique indicates the effect of sample-detector geometry on
the removal cross section.
In general the three-dimensional Monte Carlo transport codes MCNP-4A, -4B, -4C
are used to predict the measured spectra. Point-wise cross sections from FENDL/E-1 are
used mainly in the calculations. These data were derived by MacFarlane from
ENDF/B-VI, JENDL-3.1 and BROND-2 evaluations using the NJOY code system for
different elements. The ENDF/B-IV and ENDF/B-V libraries are also used in
continuous energy calculations (Jordanova et al. 1999).
As shown in FIGURE 9 the spectrum-averaged integrated reaction rates and through
them the possible use of the prompt gamma method for the detection of C, O and Si
depends strongly on the type of the neutron source. The integrated reaction rates, R, can
be determined as a function of sample thickness x using the leakage spectra of different
source neutrons. The R(x) function is given by


R( x)   Φ( E
Ethr
n , x )  ( E n ) dE . (13)

Recent investigations have shown that the rate function R(d ) depends exponentially
on the sample thickness, i.e.

d
R (d )   R( x) dx  R0 e  b d (14)
0

where the attenuation parameter b is related to the spectrum of the source neutrons and
the shielding materials.

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