Portable Neutron Generator for NAA Applications

Research Group Dr. Ing. Antonio Cannuli

Prof. Salvatore Magazù acannuli@unime.it

National Institute of Nuclear Physics, INFN – Catania Section

Department of Mathematical and Informatics Sciences, Physical Sciences and Earth Sciences (MIFT)
of Messina University
 Introduction on
neutrons

Neutron Activation
Analysis (NAA)

Portable Neutron Generator Portable neutron

for NAA Applications generators

Results of simulations for a shield for

indoor applications

Conclusions

National Institute of Nuclear Physics, INFN Catania Section

Department of Mathematical and Informatics Sciences, Physical Sciences and Earth Sciences (MIFT)
of Messina University
The 1994 Nobel Prize in Physics – Shull & Brockhouse

C.G. Shull

source
B.N. Brokhouse
 Neutrons’ development
A neutron source
Expanding horizons
allows to probe the
structure and the
dynamics of materials
in a wide range of
lenghts and time
scales

Physics

1960 Physics
 Neutrons’ development
Expanding horizons

Chemistry

1970

1960 Physics
 Neutrons’ development
Expanding horizons

Geology
Biology
Engineering

1980
Chemistry

1970

1960 Physics
 Neutrons’ development
Expanding horizons
Soft multidisciplinary
condensed matter science

1990

1980

1970

1960 Hard
 Neutrons’ development
expanding horizons

2000

1990

1980

1970

1960
 Available Experimental Techniques:
spectroscopic techniques (structure and dynamics) and purely structural methods
Neutron properties

energy-moment plan
corresponding to Interatomic
spatial-temporal grains spacing
Intermolec
ular
energies
Comparison of neutron
scattering and the most Semplificati
current spectroscopic on neutron-
technique core
interaction

Highly
penetrating
(neutral
particle)

in the case of neutrons, the continued Techniques are Isotopic

expansion of the domain complementary rather substitutio
than competitive when n
their temporal and (high
spatial scales overlap, contrast
because spatial and possible
temporal needs are not e.g. H/D)
the sole determinants
 Neutron imaging: scientific and industrial applications

Neutron imaging is used to

locate and visualize
inhomogeneity on various
length scales providing
information about the structure
and microstructure
 
magnetic domains porosity distribution crystalline phase distribution 3D Curie temperature
in casted Al specimen in martensitic steel sample map in NiPd crystal

Alternative energy, environment,

aerospace and automotive
research in conjunction with
commercial product
development have developed
into a central field of application
for neutron imaging

water in operating fuel cell strain map in a rilled

particulate filter
whole in steel
 Principle of function of NAA for
elemental analysis
Hevesy and Levi, who first noticed how samples exposed to a It is an extremely sensitive technique used for
source of neutrons became highly radioactive, discovered NAA
in 1936 and so they apply neutron irradiation for the qualitative the quantitative analysis of trace elements in
and quantitative identification of the elements present within a the analyzed material. It is based on the ability
sample
that elements have, to a different extent, to
interact with a neutron field, transforming into
radioactive elements different from the starting
ones. The analysis of the energy and the
intensity of the emitted radiation allows to trace
the elements initially present in the sample and
their quantity
A target, via a non-elastic collision in the atomic nucleus, absorbs a neutron
and a compound nucleus in an excited state is formed. Then the compound
nucleus will de-excite into a more stable configuration through emission of one
or more characteristic prompt γ-rays. The process ends, when the ground
state formed during the de-excitation, is stable. This occurs, when an isotope
of the same element, with a mass number increased by one, is produced
 to perform NAA you need…

1) a source of neutrons (particle accelerators, radioisotopes, nuclear reactors)

2) the instrumentation to detect gamma spectrum emitted by the activated sample
3) knowledge of the complex nuclear reactions that occur when neutrons interact with
the target nucleus (activation) and during the subsequent decay
Advantages
• simultaneous measure of different elements
• selectivity: it allows the measurement of independent parameters such as gamma energy
and the average life of the radionuclide
• high applicability: not only practicable if the halving time is very short or very long, or in the
case of pure beta emitters with very low energy
• high sensitivity

Disadvantages
• the need of a neutron source (costs, risk, .....)
• no possibility of chemical discrimination (valence, bonds, ...)
• it is not applicable for the analysis of pure beta emitters: 3H, 14C, 32P, 10Be
 Research activity @ neutron facilities
Reactor technology, developed in 1940s reached a plateau in performance in 1970s with the construction of ILL (F) and HFIR (USA).
The spallation process, developed in the 1970s, opened the opportunity to produce brighter beams.
Some important nuclear reactors and the relative
construction dates, starting from 1930…

Currently operating
high-flux spallation
sources include ISIS
The long pulse and low (UK), SNS (USA) and
repetition rate time structure of the MLF at J-PARC
the proton pulses will make ESS
the ideal source for long-
(J).
wavelength neutrons, with
energies in the range of about The European
0.1 meV to 50 meV
Spallation Source
(ESS) will surpass
current neutron
sources
 Portable neutron generators
Thermo Fisher Scientific, Inc.
Maximum
Typical Tube Operating
Model Applications Neutron Yield
Lifetime Mode
[n/s]
Explosive detection, Buried land mines,
1,200 hours @
API 120 NG Chemical weapons, UXO analysis, Drugs 2.00E+07
107 n/s
Continuous only
detenction, In-Vivo body composition
Large object imaging in cargo, Radiation effects
1,000 hours @
D 711 NG research, Fast neutron radiography, Neutron 2.00E+10
1010 n/s
Continuous only
activation analysis
Explosive detection, Buried land mines,
Chemical weapons, UXO analysis, Drug
1,200 hours @ Continuous and
MP 320 NG detection, In-Vivo body composition, Minerals 1.00E+08
108 n/s pulsed
mining and exploration, Bulk materials (coal,
cement)
Up to 500 hours Continuous and
P 211 NG Transuranic waste assay, Fissionable Materials 1.00E+08
or greater pulsed
Explosives detection, Bulk materials analysis,
4,500 hours @ Continuous and
P 385 NG WMD detection, UXO analysis, Contraband 5.00E+08
108 n/s pulsed
detection, Vehicle inspection

Nowadays a valid alternative to existing large-scale neutron scattering facilities, is offered by the new generation of portable neutron devices
Portable neutron generators
applications

Security detection of explosive material, illegal drugs, chemical and nuclear weapons, luggage or cargo inspections
Arts and
art objects and archaeological artefacts typically not permitted to investigate with destructive techniques
Archaeology
on-line analysers of raw materials transported on conveyor belts, especially in cement factories; analysis of minerals or materials with
Industries similar compositions
(glass, cement, coal)
Research reaction cross-sections and interfering reactions

training of young scientists in various aspects of neutron generation and diagnostics and a wide spectrum of modern technologies,
Educational such as those related to ion sources, particle acceleration techniques, beam handling and diagnostics, magnet technology, vacuum
techniques, detector technology, nuclear electronics, data acquisition as well as processing techniques

environmental studies focused on elements of interest such as Hg, Cd, As, Cu; recycled material (metals, plastics or mixtures
Environmental and Geological thereof), waste rock piles, mine tailings, etc…; in agriculture it is useful for detecting pesticide residues on crops

Electronics measure of impurities in silicon semiconductors and neutrons testing on electronic devices

living material is composed mainly of carbon, hydrogen, oxygen, and nitrogen, the presence or absence of other elements can have a
 Biology and Medicine profound effect on the well being of an organism. Thus, it is being used in several laboratories to measure the concentrations of
magnesium, copper, zinc and other metals in human blood
 How function a portable neutron generator

Among the various light-ion accelerators, compact devices

designed as hermetic, sealed tubes use Deuterium–
Deuterium (D–D) and Deuterium–Tritium (D–T) reactions:

These accelerators generate neutrons of ~2.5 and ~14.1 MeV, respectively. They consist of a source
able to generate positively charged ions; one or more devices to accelerate the ions; a metal hydride
target loaded with either deuterium, tritium, or a mixture of the two and a gas-control reservoir, also made
of a metal hydride material. The most common ion source used in neutron generators is a cold-cathode,
or Penning ion source, which is a derivative of the Penning trap used in Penning ion gauges. As far as
the elemental analysis is concerned, a low neutron flux of 107 ÷ 108 n/s is required, that furnishes the
advantage to measure easily prompt gamma from (n,γ) and (n,n’,γ) reaction and allows to work safer,
both in steady and in pulse mode, compared to radioactive neutron sources. In order to produce this
neutron flux an ion source is used, such as Deuterium ions, of a few tens of microamperes and more
than 80 KeV energy, which produce neutrons of 106 ÷ 108 n/s from D-D or D-T reactions
 Experimental set-up for NAA

A portable neutron source, a shield-moderator, a gamma-ray

spectrometer, and a computer form the experimental set-up, aligned
by a fixed support
• A neutron source is located at the front edge of a polyethylene moderator that slows down
the neutrons. The source emits fast neutrons toward the sample. Fast neutrons excite nuclei
by inelastic scattering, while some neutrons suffer capture reactions. A neutron generator
produces one million neutrons per second omni-directionally
• A tungsten shadow shield is interposed between moderator and spectrometer, to protect
germanium crystal from neutron damage. A collimator of annular bismuth surrounds the
crystal, for excluding the background of gamma rays and for maximizing the signal/noise
ratio of the gamma-ray spectrum.
• The γ-ray detector is a Portable Isotopic Neutron Spectroscopy (PINS), a non-
destructive assessment system that analyses and provides on-site identification information.
The PINS spectrometer probes the investigated sample with neutrons; these excite the
atomic nuclei within, producing γ-rays. The spectrum of the γ-rays energy intensity is
characteristic of the chemical element. The PINS software permits to identify each element
inside the sample and determines its composition. PINS uses neutrons produced by a
portable deuterium-deuterium neutron generator, with a kinetic energy of approximately 2.5
MeV, to excite nuclei inside the testing sample. The spectrometer includes a High-Purity
Germanium (HPGe) detector, used to detect γ-rays emitted from the sample; a digital signal
processing multichannel analyzer, an internal battery, and an electrical-powered refrigerator.
The detector is connected to a computer, which acts as control panel, through an Ethernet.
• The PC allows the analysis of the instrument, start and stop data acquisition, such as
display of the spectrum resulting and interlock for the neutron generator. The support aligns
the experimental set-up in an optimal geometry for measurements. The system allows to
identify chemicals inside a container without the need for disassembly, contact, physical
 MP320 Thermo Scientific neutron generator
The MP320 Thermo Scientific is a very lightweight portable neutron generator. It is possible to use the generator in laboratories for
different kind of research applications also because is relatively compact and has very low power requirements. It is possible to
operate with either a Deuterium-Tritium (DT) or a Deuterium-Deuterium (DD) neutron tube. In “DT mode” the source generates a
neutron yield of 1.0x108 n/s with energy of ~14.1 MeV. In “DD mode” will be generated a neutron yield of 2.0x10 6 n/s with energy of
~2.5 MeV. The neutron generator will be used also in conjunction with ORTEC PINS-GMX solid-state photon detector, made of n-type
high-purity germanium which permits the entire outer contact to be ion-implanted, for INNA investigations 1. For indoor application,
such as research activities, the neutron generator needs the realization of a specific bunker necessary to avoid damage from
radiation exposition for users and instrumentation

N. Marchese, A. Cannuli, M.T. Caccamo, C. Pace 2016 New generation non-stationary portable neutron generators for biophysical applications of neutron activation analysis Biochimica et
1

Biophysica Acta (BBA) BBAGEN-28495 1861 Issue 1 Part B 3661-3670

 Shielding design
Shielding calculation for neutron sources or neutron generators depends fundamentally on the way in which neutrons
interact with different atomic nuclei
For the calculation of shielding is possible to proceed substantially with following methods: 
• Solution of Neutron Transport Equation: Transport theory is relatively simple in principle, and an exact equation governing transport
phenomena can easily be derived. This is called the Boltzmann equation, or the transport equation, and the study of transport theory is essentially
the study of this equation. Under certain conditions the equation simplifies considerably and can be treated in a rather straightforward way. This
simplified version of transport theory is called diffusion theory and the neutron diffusion equation is: This equation is valid for uniform materials and
for neutrons with the same energy. Many of the diffusion problems met in practice cannot be solved by the analytical techniques. These problems
must be handled by numerical methods.
• Monte Carlo method: Monte Carlo obtains answers by simulating individual particles and recording some aspects (tallies) of their average
behaviour. The average behaviour of particles in the physical system is then inferred from the average behaviour of the simulated particles. Monte
Carlo can be used to duplicate theoretically a statistical process (such as the interaction of nuclear particles with materials) and is particularly useful
for complex problems that cannot be modelled by computer codes that use deterministic methods. It consists of actually following each of many
particles from a source throughout its life to its death in some terminal category (absorption, escape, etc.). Probability distributions are randomly
sampled using transport data to determine the outcome at each step of its life.
• Removal Cross Section method: The method of removal cross section takes into account the ability of materials to "remove" the neutrons of
different energies from the primary beam. The interactions that slow down neutrons and cause their eventual removal from a beam are probabilistic:
they either occur or they do not. Consequently, a flux of neutrons of intensity I will be diminished in a thickness x of absorber proportionally to the
intensity of the neutron source and the neutron removal coefficient , of the absorbing material: which has the solution , where is the
initial intensity and refers to those neutrons that penetrate a distance in the absorber without a collision; therefore, represents the probability that a
given neutron travels a distance without an interaction. Conceptually, can be thought of as the probability per unit path length that a neutron will
undergo an interaction as it moves through an absorber and be removed from the beam either by absorption or scattering. Then, in this context, it
very much resembles the attenuation coefficient for photons in “good (or narrow-beam) geometry,” and can be similarly developed and used for
neutron shielding and dosimetry.
 Shielding calculation for MP320 Thermo
Scientific neutron generator
For the design of the MP320 Neutron Generator shielding, the following features were taken as a reference

Shielding materials and thickness

Material Σ [cm-1] t [cm]

30% Borated PE 0.1191 15

Barite Concrete 0.0945 15 PE = PolyEthilene

In order to perform a preliminarily evaluation of the shielding thicknesses was used the method of Removal Cross section. In a
second moment, data preliminarily obtained were verified with simulations with MCNP Monte Carlo code.
Preliminary Shielding evaluation
In order to optimize the shielding size, both from the point of view of the “weight” and cost, it is necessary to select a materials that
offer a good shielding power (high ). It is also important to utilize the interactions of neutrons with the different materials in order to
optimize the processes of "slowing down" and "capture". Therefore the shielding is made of successive layers of different materials
(lead, iron, hydrogenated materials). The exponential attenuation law is valid only for collimated neutron beam, while in the case in
which the source can be considered as a "point source", the spatial dependence of the neutron flux has to be considered. Therefore
the attenuation law becomes the following:

where is the initial neutron yield (n s-1), is the distance at which neutron flux is calculated respect to the source position, is the
neutron flux at distance from the source and is the thickness of shielding material
The evaluation of the different materials thickness was made considering their characteristics (, weight) in order to limit the weight of
the whole structure. Therefore the following materials and thickness were chosen. Neutron flux was calculated on the external
surfaces at the end of the shielding. Because the source is not symmetric, respect to the shielding structure, it is necessary to
evaluate the neutron flux on every external surface. The following parameters was taken in consideration: distance between the
source, considered a point source; internal surface of the shielding; entire shielding thickness. The values of neutron flux obtained for
the different surfaces are shown below Neutron flux on external shielding surfaces

 Surfaces Up Lateral Back Front

t t t t
Material
[cm] [n cm-2 s-1] [cm] [n cm-2 s-1] [cm] [n cm-2 s-1] [cm] [n cm-2 s-1]
Air 33 146.15 15 397.89 23 300.86 57 48.99

30% Borated PE 15 11.57 15 21.77 15 18.47 30 0.59

Barite Concrete 15 1.63 15 2.59 15 2.30 0 0.59

Different thicknesses of the shielding: green represents the 30% borated PE; grey the barite concrete. In section view it is possible to identify the
“window” for the samples irradiation, positioned between the floor and the neutron generator. Neutrons irradiate target in correspondence of the window

Shielding
structure

Shielding
Shielding section view
thicknesses
Shielding representation inside
the laboratory
 Monte Carlo code simulation
Several simulations were performed with a software based on Monte Carlo method, in order to verify the values obtained with the application of
removal cross section. The code used was MCNP5. The code include information relatively to the geometry, the materials and the source
characteristics.
The cells in which evaluate the neutron flux were also specified. These were placed on the external surfaces of the shielding in correspondence to the
specification addressed in the design phase. For neutron flux evaluation was chosen the Track Length Estimate of Cell Flux (F4), that allow to obtain
the average neutron flux in a volume , as described in following formulation.

where is the density of particles, regardless of their trajectories, at a point.

Two sections of the shielding are reported in figure: blue represents 30% borated PE; yellow represents barite concrete; the green point represents
the cells in which neutron flux was calculated. The cross in the two figures represents the point at which the “neutron source” is located.

Shielding sections from MCNP simulations

Up Lateral

Back Front Back Front

Down Lateral
 Dose rate evaluation
In order to evaluate the effect of shielding, we have to calculate the neutron dose rate. The following parameters were taken into
account as references for the dose rate limits evaluation
• Project Equivalent Dose [mSv/y] 0.5
• Annual duty hours [h/y]1,200
The project neutron dose rate was chosen as half of the annual limit for the population in order to consider also the photons contribute
to the total dose rate. The annual duty hours were chosen as the typical lifetime of the target. Taking into account of the set
parameters, the reference value for the dose rate is equal to

Considering the neutron spectrum obtained with Monte Carlo simulations and applying the conversion factors, were obtained the
following values of neutron dose rate.

Neutron Dose rate values on external shielding surfaces

  Shielding

  Up Lateral Back Front

Equivalent Dose Rate [mSv/h] 1.51x10-3 2.81 x10-2 4.0E x10-2 1.62 x10-2

TheDetail
values of neutronEquivalent
of spectrum dose rate obtained
Dose Rate @ 0.1 m are over
from the the limit
shielding , however, 1.20
[mSv/h] taking
x10-8 into account
2.23 x10-7 the 3.18
geometric
x10-7 attenuation
1.29 x10-7 is possible to
evaluate thatpoint
evaluation the neutron dose rate goes down rapidly below the limit. Therefore is possible to define a restricted zone outside of
which the neutron dose rate is surely below the considered limit.
In order to complete the shielding, it is necessary to evaluate the contribute of gamma-rays to the dose rate and take this contribute
into account in the design of the gamma shielding
 Next employment in Electronics for SEE testing

According with the standard JESD89A, this system could be used for accelerated Single Event Effects (SEE)
testing of electronic devices. SEE consists of a failure into electronic devices, caused by the ionizing radiation
coming from the atmosphere. Without the shield and with the future development of the mini-bunker, the facility
allows the SEE cross section estimation at 14 MeV (with the T target) and 2.45 MeV (with the D target). This allows
the estimation of the threshold energy at which the SEE cross section rapidly rises. In fact, for recent technologies,
this energy threshold is in the range of 1÷10 MeV. Moreover thermal neutron test could be also performed, using
the shield described previously , placing the samples not in‑view of the main neutron beam. To this purpose, a
careful simulated and measured characterization of the facility will be required

The Earth’s atmosphere acts as a shield against ionizing radiation coming from the deep space. However, the interaction of
galactic cosmic rays with the terrestrial atmosphere produces a “shower” of secondary particles, mainly neutrons, which come
down to sea level. Thus, all electronic devices are exposed to this “natural” radiation environment. Despite the neutron flux is quite
low (especially at sea level) even a single neutron, under certain conditions, can cause a failure into electronic devices: in this
case, we have a so-called Single Event Effect (SEE). From a physical point of view, SEEs are related to the charge generated in
the semiconductor, through ionization realized by the incident particle. For example, two very common reactions involving the
silicon nucleus are:
n + 28Si → 28Al + p

n + 28Si → 25Mg + α
 Conclusions

 the MP 320 Thermo Scientific neutron generator represent a valid research

tool
 the areas where it can be used are numerous
 the reduced operating costs, the compactness and the possibility of varying
the duty factor make the neutron generator very competitive within the
panorama of the European neutron sources
 the data obtained with the method of removal cross section and through
simulations with MCNP represent a basic support in the design of the shield,
necessary for the indoor use of the neutron source
 this work is therefore a starting point for the construction of the shield and the
obtained data will be verified experimentally
 Collaborations

 National Institute of Nuclear Physics, INFN – Catania and Messina

Sections

 Department of Computer Engineering, Modelling, Electronics and

Systems Science (DIMES), University of Calabria, Cosenza

 Department of Energy, Engineering of the Information and Mathematical

Models (DEIM), University of Palermo
 Thanks
for your attention!