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Material classification by Fast Neutron Scattering Analysis

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Nuclear Instruments and Methods in Physics Research B 173 (2001) 483±502<br />

www.elsevier.nl/locate/nimb<br />

<strong>Material</strong> classi®cation <strong>by</strong> fast neutron scattering<br />

A. Bu‚er a , F.D. Brooks a, *<br />

, M.S. Allie a , K. Bharuth-Ram b , M.R. Nchodu c<br />

a Physics Department, University of Cape Town, Rondebosch 7700, South Africa<br />

b Physics Department, University of Durban-Westville, Durban 4000, South Africa<br />

c Physics Department, University of the Western Cape, Bellville 7535, South Africa<br />

Received 10 May 2000; received in revised form 22 August 2000<br />

Abstract<br />

The scattering of a beam of fast monoenergetic neutrons is used to determine elemental compositions of bulk<br />

samples (0.2±0.8 kg) of materials composed from one or more of the elements H, C, N, O, Al, S, Fe and Pb. Scattered<br />

neutrons are detected <strong>by</strong> liquid scintillators placed at forward and at backward angles. Di€erent elements are identi®ed<br />

<strong>by</strong> their characteristic scattering signatures derived either from a combination of time-of-¯ight and pulse height<br />

measurements, or from pulse height measurements alone. <strong>Scattering</strong> signatures measured for multi-element samples are<br />

analysed to determine atom fractions for H, C, N, O and other elements in the sample. Atom fractions determined from<br />

scattering signatures are insensitive to neutron interactions in material surrounding the scattering sample, provided the<br />

amount of material is not excessive. The atom fraction data are used to classify scattering material into categories<br />

including ``explosives'', ``illicit drugs'' and ``other materials'' for the purpose of contraband detection. Ó 2001 Elsevier<br />

Science B.V. All rights reserved.<br />

PACS: 87.53Pb; 29.30Hs<br />

Keywords: HCNO analysis; <strong>Fast</strong> neutron scattering; Non-intrusive contraband detection<br />

1. Introduction<br />

<strong>Neutron</strong> methods for examining materials in<br />

bulk are currently under investigation and a variety<br />

of di€erent approaches [1±19] are being explored.<br />

There is particular interest in the<br />

possibility of using neutrons for the non-intrusive<br />

* Corresponding author. Tel.: +27-21-6503325; fax: +27-21-<br />

6503342.<br />

E-mail addresses: abu‚er@physci.uct.ac.za (A. Bu‚er),<br />

brooks@physci.uct.ac.za (F.D. Brooks).<br />

detection of hidden contraband, especially explosives<br />

or illicit drugs, in packages ranging in size<br />

from carry-on airline baggage to cargo containers.<br />

Among the neutron-based techniques that have<br />

been proposed for baggage or cargo inspection are<br />

pulsed fast neutron transmission spectroscopy<br />

(PFNTS) [8±11], thermal neutron analysis (TNA)<br />

[12], pulsed fast neutron analysis (PFNA) [13,14]<br />

and pulsed fast-thermal neutron analysis<br />

(PFTNA) [15,16]. PFNTS is based on measurements<br />

of the attenuation of a pulsed fast neutron<br />

beam as it passes through the object or material<br />

0168-583X/01/$ - see front matter Ó 2001 Elsevier Science B.V. All rights reserved.<br />

PII: S 0 168-583X(00)00425-0


484 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

being interrogated. TNA, PFNA and PFTNA<br />

identify di€erent chemical elements via characteristic<br />

gamma rays which are excited either <strong>by</strong><br />

thermal neutron capture (TNA, PFTNA) or <strong>by</strong><br />

inelastic neutron scattering (PFNA, PFTNA) in<br />

the interrogated material. The technique of fast<br />

neutron scattering analysis (FNSA) is an alternative<br />

approach [4,17±19] in which neutrons scattered<br />

out of the interrogated material are detected.<br />

The nuclides responsible for the scattering are<br />

determined from measurements of the dependence<br />

of scattered neutron intensity and energy on scattering<br />

angle and the incident neutron energy.<br />

The FNSA technique described in [18] consists<br />

of bombarding the sample of material being examined<br />

with a beam of monoenergetic neutrons,<br />

alternating the incident neutron energy between<br />

two carefully chosen values, and using two detectors<br />

to observe scattered neutrons, one detector at<br />

a forward angle (45°) and the other at a backward<br />

angle (150°). The pulse height resolution of the<br />

neutron detectors should ideally, but not necessarily,<br />

be sucient to resolve the small energy<br />

di€erences (4%) between neutrons backscattered<br />

<strong>by</strong> the elements C, N and O. Time-of-¯ight can<br />

also be used to resolve larger energy di€erences,<br />

for example to separate elastically and inelastically<br />

scattered neutrons. Measurements from the two<br />

detectors at two di€erent incident neutron energies<br />

are combined to form a ``scattering signature'' [18].<br />

Recent tests of FNSA [18] were concentrated on<br />

materials composed exclusively from the elements<br />

H, C, N and O, which are the most important<br />

atomic constituents of contraband materials such<br />

as explosives and illicit drugs. Measurements on<br />

pure elemental samples such as carbon (graphite),<br />

liquid nitrogen or liquid oxygen and on a water<br />

sample provide scattering signatures for these four<br />

elements. The signatures are strongly characteristic<br />

of the scattering element and provide a reference<br />

matrix which can be used to analyze the scattering<br />

signature measured for a multi-element sample.<br />

The signature measured for a scattering sample of<br />

unknown material is unfolded into components<br />

corresponding to elemental scattering signatures<br />

(H, C, N and O) to determine the atom fraction of<br />

each element in the sample. Atom fractions are<br />

then used to identify the scattering material. It has<br />

been shown [18] that atom fractions of the elements<br />

in a small sample (0.2±0.8 kg) of a HCNO<br />

material can be measured to an accuracy of a few<br />

percent <strong>by</strong> means of FNSA and that explosive or<br />

illicit drug material can be reliably identi®ed from<br />

these measurements.<br />

In this paper we describe further experimental<br />

studies of FNSA and present a new method for<br />

using the atom fractions determined from FNSA<br />

measurements to classify materials into categories<br />

appropriate for contraband detection, such as<br />

``explosive'', ``illicit drug'' and ``other''. The new<br />

experimental studies aimed (a) to extend the<br />

FNSA method to materials containing a wider<br />

range of elements, namely H, C, N, O, Al, S, Fe<br />

and Pb, (b) to investigate alternative FNSA scattering<br />

signatures, and (c) to investigate the e€ects<br />

of neutron interactions in material close to the<br />

scattering sample, especially material in the incident<br />

neutron beam, or between the sample and the<br />

detectors. Information obtained from these studies<br />

provides a further proof-of-principle test of FNSA<br />

and can be used to assess the feasibility of possible<br />

practical applications of this technique.<br />

2. Experiments<br />

The experimental arrangement used for the<br />

FNSA studies is shown schematically in Fig. 1.<br />

Monoenergetic neutrons were obtained from the<br />

2 H…d; n† 3 He reaction <strong>by</strong> bombarding a deuterium<br />

gas target (30 mm long, 1.0 atm) with a pulsed<br />

beam (repetition frequency 2 MHz, FWHM 2 ns)<br />

of 4.7 MeV deuterons, and selecting neutrons<br />

emitted at 0° <strong>by</strong> means of the aperture in the shield<br />

SH. The pulsed deuteron beam was provided <strong>by</strong><br />

the 5.5 MV pulsed Van de Graa€ accelerator of the<br />

South African National Accelerator Centre, Faure,<br />

Western Cape. The energy E n of the neutron<br />

beam was alternated between 6.8 and 7.5 MeV<br />

[18,19] at intervals of about 2 min <strong>by</strong> moving an<br />

energy-degrading Havar foil HF (11 lm) in and<br />

out of the deuteron beam. <strong>Neutron</strong>s scattered <strong>by</strong><br />

the sample S were detected <strong>by</strong> the liquid scintillators<br />

F and B at forward and backward scattering<br />

angles h F ˆ 45° and h B ˆ 150°, respectively. Detectors<br />

F and B were NE213 liquid scintillators of


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 485<br />

Fig. 1. Schematic diagram of the geometry used for FNSA test measurements, showing: NE213 neutron detectors, F, B and M; degrader<br />

foil HF; neutron shielding SH; copper scatterer CS; scattering sample S; and additional scatterer positions S 1 ±S 4 . Distances are<br />

indicated in mm.<br />

dimensions 130 130 70 mm and 40 mm<br />

diam: 30 mm, respectively, subtending solid<br />

angles of 89 and 13 msr at S. The neutron beam<br />

was monitored <strong>by</strong> an NE213 liquid scintillator<br />

detector M (50 mm diam: 50 mm) embedded in<br />

the shield (Fig. 1) and positioned to detect neutrons<br />

scattered <strong>by</strong> a copper plate CS (1 mm thick)<br />

mounted inside the collimator. Detectors B, F<br />

and M were connected to scintillation pulse shape<br />

discriminators to select neutrons and reject gamma<br />

rays.<br />

The scattering samples studied included<br />

graphite (carbon), liquid nitrogen, liquid oxygen,<br />

aluminium, sulphur, iron and lead, and compounds<br />

of these elements with one-another and<br />

with the elements hydrogen, lithium and boron.<br />

For scattering measurements on liquid nitrogen or<br />

liquid oxygen, the liquid was contained in a<br />

spherical Dewar ¯ask of inner diameter 100 mm.<br />

The other scattering samples were cylinders<br />

(60 mm diam: 120 mm), which were suspended<br />

so that their axes were aligned along the neutron<br />

beam. Solid cylinders were used for the metal and<br />

graphite samples. Samples of the other materials<br />

were contained in light (0.03 kg) aluminium canisters.<br />

Backgrounds were measured using either no<br />

sample or an empty sample container. All measurements<br />

were normalized to the same incident<br />

neutron ¯uence based on the counts recorded <strong>by</strong><br />

the monitor M (Fig. 1). The regions labelled S 1 ±S 4<br />

in Fig. 1 indicate positions at which one or more<br />

additional scatterers were placed for the experiments<br />

described in Section 4.3. These experiments<br />

were carried out to study the e€ects of neutron<br />

scattering outside the sample (in the incident beam<br />

or between the sample and the detectors) on<br />

FNSA signatures.<br />

Pulse height L and time-of-¯ight T were measured<br />

for neutrons detected <strong>by</strong> F and B in the<br />

scattering experiments. Data were acquired on<br />

disk in multiparameter event mode, at 12-bit (4096<br />

channels) resolution for each parameter. In the o€line<br />

analysis adjacent channels were binned in<br />

groups of between 2 and 32 channels, in order to<br />

achieve appropriate dispersions in L and T, as<br />

shown in Figs. 2±6. A pattern register was used to<br />

record whether the Havar foil HF (Fig. 1) was in<br />

or out of the beam, and which detector (F, B or M)<br />

was active in the event.<br />

Figs. 2 and 3 show numbers of events as a<br />

function of L and T, recorded using graphite and<br />

water scattering samples, respectively: (a) and (b)<br />

<strong>by</strong> detector F; (c) and (d) <strong>by</strong> detector B; (a) and (c)<br />

for 6.8 MeV incident neutrons; and (b) and (d) for<br />

7.5 MeV incident neutrons. Pulse height scales L<br />

are calibrated in terms of the recoil proton energy<br />

E p recorded <strong>by</strong> the liquid scintillator detector.<br />

Time-of-¯ight scales T are calibrated in terms of


486 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

Fig. 2. Counts (vertical) as a function of pulse height L and time-of-¯ight T, recorded using a graphite scattering sample: (a) and (b) <strong>by</strong> detector F (45°); (c) and (d) <strong>by</strong><br />

detector B (150°); (a) and (c) for incident neutrons of energy 6.8 MeV; and (b) and (d) for incident neutrons of energy 7.5 MeV. Ridges attributed to elastic and inelastic<br />

neutron scattering are indicated <strong>by</strong> EC and I4, respectively. Ridge B is attributed to neutron background. LC1±LC4 and TC1±TC4 indicate pulse height and time-of-¯ight<br />

cuts, respectively. LTF and LBF indicate pulse height thresholds for the F and B detectors. Count scales are normalized to a standard number of neutron beam monitor<br />

counts and to a sample mass corresponding to 100 NA carbon nuclei, where NA ˆ Avogadro's number.


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 487<br />

Fig. 3. Counts (vertical) as a function of pulse height L and time-of-¯ight T, recorded using a water scattering sample. Ridges attributed to elastic neutron scattering on<br />

hydrogen and oxygen are indicated <strong>by</strong> EH and EO, respectively. Count scales are normalized to a standard number of neutron beam monitor counts and to a sample mass<br />

corresponding to 100 NA oxygen nuclei. Other details are the same as for Fig. 2.


488 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

Fig. 4. S D0 scattering signatures for the elements hydrogen (H),<br />

carbon (C), nitrogen (N), oxygen (O), aluminium (Al), sulphur<br />

(S), iron (Fe) and lead (Pb). Each signature shows counts S…n†<br />

as a function of channel number n, and is a combination of<br />

projected-L and projected-T spectra, as detailed in Table 1(a).<br />

The signatures are normalized to the same number of incident<br />

neutrons and the same number (100 N A ) of target nuclei in the<br />

scatterer. The numbers 1±10 at the top of the ®gure indicate the<br />

components of the S D0 signature as listed in Table 1(a).<br />

the energy E n of the scattered neutron detected.<br />

Prominent features in the plots are the ridges E C ,<br />

E O and E H which are attributed to recoil protons<br />

associated with neutrons detected after elastic<br />

scattering on carbon, oxygen and hydrogen, respectively.<br />

The ridge I 4 in Fig. 2 is attributed to the<br />

lower energy neutrons originating from inelastic<br />

neutron scattering in which the 4.43 MeV level of<br />

12 C is populated. The ridge labelled B in panels (c)<br />

and (d) of Figs. 2 and 3 is a background component<br />

attributed to source neutrons which either<br />

penetrate the shield SH (Fig. 1) or are scattered in<br />

SH near the collimator exit and thus arrive at<br />

detector B ahead of the neutrons backscattered <strong>by</strong><br />

the sample.<br />

The features (other than B) observed in L±T<br />

spectra such as Figs. 2 and 3 clearly depend<br />

strongly on the elements contained in the scattering<br />

sample. For carbon (Fig. 2(c) and (d)), for<br />

example, the intensity of backscattered components,<br />

both elastic (E C ) and inelastic (I 4 ), increases<br />

markedly with the increase of incident neutron<br />

energy from 6.8 to 7.5 MeV, whereas for oxygen<br />

(Fig. 3(c) and (d)) an opposite and smaller energydependence<br />

is observed for the elastic scattering<br />

components (E O ). The incident neutron energies of<br />

6.8 and 7.5 MeV were in fact selected [18] to take<br />

advantage of these features. The presence of the<br />

inelastic group I 4 (Fig. 2) is also a unique and<br />

prominent feature in the carbon signature. Two<br />

features in Fig. 3 indicate the presence of hydrogen<br />

in the measurement made using the water sample:<br />

®rstly the strong group E H (Fig. 3(a) and (b)) at<br />

the forward scattering angle of 45°, which extends<br />

to a proton recoil energy of half the incident<br />

neutron energy; and secondly the absence of any<br />

associated contribution from hydrogen to the yield<br />

at backward angles (Fig. 3(c) and (d)), as expected<br />

from the kinematics of n±p elastic scattering. The<br />

L±T spectra for all of the elements investigated in<br />

this study each displayed unique features of the<br />

type seen in Figs. 2 and 3, con®rming that FNSA<br />

can provide information which is highly elementspeci®c<br />

and can therefore be used to identify different<br />

elements and measure their concentrations.<br />

3. <strong>Scattering</strong> signatures<br />

The L±T spectra measured for single-element<br />

samples, such as those measured using a carbon<br />

scatterer (Fig. 2), incorporate information which<br />

characterizes the scattering element and therefore<br />

constitute a signature for that element. The raw<br />

signatures shown in Figs. 2 and 3 each consist of<br />

16k channels of numerical data. In order to simplify<br />

the analysis of FNSA measurements made<br />

using multi-element samples it is convenient to<br />

introduce a compact ``scattering signature'' which<br />

summarizes the important features of the raw<br />

signature [18]. The scattering signature for an


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 489<br />

Fig. 5. (a) S L0 scattering signatures for the elements H, C, N, O, Al, S, Fe and Pb; (b) S DZ scattering signatures for the elements H, C, N<br />

and O; and (c) S LZ scattering signatures for the elements H, C, N and O. All signatures are normalized as described in Fig. 4. The<br />

numbers 1±4 at the top of panel (a) indicate the components of the S L0 signature, as listed in Table 1(b). The numbers 1±8 on the bar<br />

above panel (a) indicate the regions which are summed to form the S LZ signature (c).<br />

element (or other) sample is obtained <strong>by</strong> projecting<br />

certain selected regions of the raw 2-parameter<br />

data (e.g. Fig. 2 for carbon) onto either the L-axis<br />

or the T-axis and then assembling the resulting<br />

projected spectra (L and T) serially, into a single,<br />

spectrum-like, distribution (see Fig. 4). Each region<br />

that is selected for projection is de®ned <strong>by</strong> a<br />

T-cut (time-of-¯ight window) and an L-cut (pulse<br />

height window) or a pulse height threshold. The<br />

cuts and thresholds used to de®ne the selected regions<br />

are indicated in Figs. 2 and 3, in which TC1±<br />

TC4 are T-cuts, LC1±LC4 are L-cuts and LTB<br />

and LTF are L-thresholds. Reference signatures<br />

measured for elemental samples are corrected for<br />

background <strong>by</strong> subtracting a background signature<br />

that is constructed <strong>by</strong> applying the same selection<br />

procedure to the appropriate background<br />

measurement.<br />

Several alternative types of scattering signature<br />

were investigated in these studies. Some of these<br />

signatures included both projected T-components<br />

and projected L-components. Other types of signature<br />

included only projected L-components and<br />

used the time-of-¯ight information T only for<br />

background suppression. Signatures based on L-<br />

components only are of special interest because


490 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

Fig. 6. <strong>Scattering</strong> signatures for an acetamide scattering sample of mass 0.212 kg: (a) measured (histogram) and refolded (full curve) S D0<br />

signature, and background component (dashed curve); and (b) measured (histogram) and refolded (full curve) S L0 signature (background<br />

subtracted). The peaks labelled B in panel (a) correspond to projections of the background ridges B in Fig. 2(c) and (d).<br />

they can be used in conjunction with a neutron<br />

source which does not incorporate nanosecond<br />

beam pulsing, provided other means for suppressing<br />

background are available.<br />

Two basic types of signature were used in the<br />

studies presented here: ®rstly, a dual parameter<br />

signature, S D0 , which incorporates projections of<br />

both L- and T-components; and secondly a single<br />

parameter signature, S L0 , which is based exclusively<br />

on projections of the pulse height parameter<br />

L. The structures of the two basic signatures are<br />

summarized in Table 1 and discussed below. Some<br />

analyses made using variations of the two basic<br />

signatures are also presented.<br />

3.1. The S D0 signature<br />

The S D0 signature is de®ned <strong>by</strong> a procedure<br />

similar to that described in [18], but modi®ed so as<br />

to obtain additional useful information from the<br />

two neutron detectors F and B. This signature<br />

consists of ten components, as shown in Table<br />

1(a). Components 1 and 2 (see Table 1(a)) are<br />

projected L-spectra from detector B and provide<br />

channels 1±150 and 151±300, respectively, of the<br />

signature (see Fig. 4). Both components are selected<br />

<strong>by</strong> the L-cut LC1 and the T-cut TC1 (see<br />

Figs. 2 and 3). Component 1 is derived from data<br />

taken at 6.8 MeV, and component 2 from data<br />

taken at 7.5 MeV. In the S D0 signature for carbon<br />

(panel C of Fig. 4), for example, the distribution<br />

from n ˆ 1±150 is therefore the projection of the<br />

rectangle bounded <strong>by</strong> cuts LC1 and TC1 of Fig.<br />

2(c) onto the L-axis. Channels 1±150 of Fig. 4<br />

(panel C), in other words, show the L-spectrum<br />

(within the window LC1) that is obtained <strong>by</strong> integrating<br />

the data in Fig. 2(c) over T, between the<br />

T-limits de®ned <strong>by</strong> cut TC1. Channels 151±300 of<br />

the same panel show the L-spectrum obtained <strong>by</strong><br />

applying the same procedure to the data of Fig.<br />

2(d).<br />

Components 3±10 of the S D0 signature (Table<br />

1(a)) are projected T-spectra (projections onto the<br />

T-axis) and provide the remaining channels, 301±


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 491<br />

Table 1<br />

Components of the S D0 and S L0 scattering signatures<br />

Signature No. Channels Detector E n (MeV) Parameter L-cut T-cut Weight<br />

(a) S D0 1 1±150 B 6.8 L LC1 TC1 1<br />

2 151±300 B 7.5 L LC1 TC1 1<br />

3 301±375 B 6.8 T LC1 TC3 0.25<br />

4 376±450 B 7.5 T LC1 TC3 0.25<br />

5 451±525 F 6.8 T LC2 TC4 0.01<br />

6 526±600 F 7.5 T LC2 TC4 0.01<br />

7 601±675 F 6.8 T LC3 TC4 0.01<br />

8 676±750 F 7.5 T LC3 TC4 0.01<br />

9 751±825 F 6.8 T LC4 TC4 0.01<br />

10 826±900 F 7.5 T LC4 TC4 0.01<br />

(b) S L0 1 1±150 B 6.8 L LTB TC2 1<br />

2 151±300 B 7.5 L LTB TC2 1<br />

3 301±450 F 6.8 L LTF TC4 0.1<br />

4 451±600 F 7.5 L LTF TC4 0.1<br />

900, of the signature. Components 3 and 4 are<br />

derived from the B detector, and components 5±10<br />

from the F detector. The cuts and incident neutron<br />

energies used to extract these components are<br />

listed in Table 1(a). The L-cuts LC2-LC4 select<br />

events according to pulse height from detector F as<br />

follows: LC2, a low pulse height window, selects<br />

inelastically scattered neutrons as well as elastically<br />

scattered neutrons from both hydrogen and<br />

heavier nuclides; LC3, an intermediate pulse<br />

height window, excludes most inelastically scattered<br />

neutrons, due to their low pulse height; and<br />

LC4, a higher pulse height window, excludes both<br />

inelastically scattered neutrons and neutrons elastically<br />

scattered <strong>by</strong> hydrogen, retaining only higher<br />

energy neutrons from elastic scattering on A P 2<br />

nuclei.<br />

The S D0 scattering signatures are thus combinations<br />

of projected L-spectra and projected T-<br />

spectra. Each signature embodies, in a more<br />

compact form (S…n† for n ˆ 1±900), salient characteristics<br />

of the raw two-parameter data (e.g.<br />

Figs. 2 or 3) measured for the corresponding<br />

scatterer. In order to ensure that the di€erent L-<br />

and T-components in the signatures are accorded<br />

approximately equal weight in subsequent ®tting<br />

procedures [18,19] each component has been<br />

multiplied <strong>by</strong> the weighting factor shown in the<br />

right-hand column of Table 1(a).<br />

The S D0 signatures derived as described above<br />

for the eight elements used in this study and corrected<br />

for background are shown in the eight<br />

panels of Fig. 4. The hydrogen signature (panel H)<br />

was derived from measurements made using the<br />

water scatterer (Fig. 3), after applying a correction<br />

for the oxygen contribution, based on the data<br />

measured using the liquid oxygen scatterer. In<br />

addition to being adjusted as described above and<br />

normalized to the same incident neutron ¯uence,<br />

as noted earlier, each signature shown in Fig. 4 has<br />

also been normalized so as to correspond to the<br />

same number of target element nuclides, 100 N A ,<br />

in the scatterer, where N A ˆ Avogadro's number.<br />

The eight elemental signatures shown in Fig. 4<br />

exhibit distinct individual characteristics and are<br />

therefore well suited for unfolding signatures<br />

measured for multi-element compounds or materials<br />

into elemental components [18]. For example,<br />

the hydrogen signature is unique in having negligible<br />

intensity in channels 1±450 and 751±900, a<br />

consequence of the kinematics of np elastic scattering.<br />

Components 1 and 2 (channels 1±300) for<br />

the A P 12 elements display upper limits which<br />

increase systematically with incident beam energy<br />

and with target mass number A, as expected from<br />

the kinematics of neutron backscattering. Components<br />

1±4 of the carbon signature show a strong<br />

dependence on the incident neutron energy, in-


492 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

creasing in intensity with the energy change from<br />

6.8 to 7.5 MeV. The intensities of the corresponding<br />

components in the oxygen signature exhibit<br />

a weaker energy dependence in the opposite<br />

direction. The low energy forward-scattered components<br />

(channels 451±600) of all the elements<br />

shown, except hydrogen and oxygen, display<br />

characteristic inelastic scattering contributions at<br />

low pulse height. The four heavier elements studied<br />

(Al, S, Fe, Pb) also show characteristic contributions<br />

from inelastic scattering in the<br />

backscattered components (channels 1±450) of<br />

their signatures. All of these features are consistent<br />

with expectations based on nuclear data such as<br />

di€erential cross-sections [20] and excited state<br />

energies [21], which were important guiding considerations<br />

in the choice [18] of the incident neutron<br />

energies used, 6.8 and 7.5 MeV.<br />

3.2. The S L0 signature<br />

The S L0 signature, shown in Fig. 5(a), consists<br />

of four components (Table 1(b)), each of which is<br />

a projected L-spectrum. Components 1 and 2<br />

(channels 1±150 and 151±300) of this signature are<br />

derived from the B detector, at E n ˆ 6:8 and 7.5<br />

MeV, respectively, and selected <strong>by</strong> T-cut TC2 and<br />

pulse height threshold LTB (see Figs. 2 and 3).<br />

Components 3 and 4 (channels 301±450 and 451±<br />

600) are derived from the F detector at the same<br />

two energies, and selected <strong>by</strong> T-cut TC4 and pulse<br />

height threshold LTF. The weights assigned to the<br />

B and F components are shown in Table 1(b). The<br />

S L0 signatures include contributions from both<br />

elastically and inelastically scattered neutrons. The<br />

signatures for the eight elements, shown in Fig.<br />

5(a), have been corrected for background and<br />

normalized in the same way as described in Section<br />

3.1 for the S D0 signatures.<br />

Results obtained using the S L0 signature provide<br />

a guide to the quality of FNSA that should be<br />

attainable using a monoenergetic neutron source<br />

without nanosecond beam pulsing. The T-cuts TC2<br />

and TC4 employed to derive the signatures shown<br />

in Fig. 5(a) were used only for the purpose of<br />

suppressing background components such as ridge<br />

B in Figs. 2 and 3. If backgrounds were eciently<br />

suppressed <strong>by</strong> other means, for example <strong>by</strong><br />

improving the shielding and collimator used in the<br />

experiments (Fig. 1), then these T-cuts (and hence<br />

T-measurements) would be unnecessary.<br />

3.3. The S D1 and S D2 signatures<br />

The S D1 and S D2 signatures are subsets of the<br />

dual-parameter signature S D0 . The S D1 signature<br />

consists of the S D0 signature reduced from 10<br />

components (900 channels) to 5 components (450<br />

channels) <strong>by</strong> including only the components associated<br />

with the 6.8 MeV incident neutron energy,<br />

that is the odd-numbered components in Table<br />

1(a). The S D2 signature is derived similarly <strong>by</strong> using<br />

only the 7.5 MeV components, in other words the<br />

even-numbered components in Table 1(a). Results<br />

obtained using the S D0 , S D1 and S D2 signatures were<br />

compared in order to determine the extent to<br />

which the use of two incident neutron energies,<br />

rather than one, improved the quality of the<br />

FNSA result obtained.<br />

3.4. The S DZ and S LZ signatures<br />

The two signatures denoted S DZ and S LZ are<br />

compact signatures consisting of integrals derived<br />

from the S D0 and S L0 signatures. Each signature<br />

consists of an 8-channel distribution (S…n† for<br />

n ˆ 1±8) obtained <strong>by</strong> summing selected sections of<br />

the parent signature, S D0 or S L0 . The eight channels<br />

of the S DZ signature are integrals of components 3±<br />

10, respectively, of the S D0 signature (Table 1(a)).<br />

Channels 1 and 2 of the S LZ signature are integrals<br />

of components 1 and 2 of the S L0 signature (Table<br />

1(b)). Channels 3±8 of this signature are obtained<br />

<strong>by</strong> summing the following subsections (channels)<br />

of the S L0 signature (Fig. 5(a)): (3) 301±325; (4)<br />

326±350; (5) 351±450; (6) 451±475; (7) 476±500 and<br />

(8) 501±600. Thus, channels 1 and 2 of the S LZ<br />

signature are a measure of the backscattered neutron<br />

yields for 6.8 and 7.5 MeV incident neutrons,<br />

respectively, and channels 3±5 and 6±8 measure<br />

forward-scattered neutrons for the same two energies.<br />

The summation limits speci®ed for channels<br />

3±8 are chosen so as to emphasize the contributions<br />

of inelastic neutron scattering (3 and 6), n±p<br />

elastic scattering (4 and 7) and elastic scattering on<br />

A P 2 nuclides (6 and 8), as discussed in Section


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 493<br />

3.1. Studies of the S DZ and S LZ signatures have been<br />

con®ned to scattering samples composed exclusively<br />

from the elements H, C, N and O. The S DZ<br />

and S LZ signatures for these elements are shown in<br />

Figs. 5(b) and (c), respectively.<br />

3.5. The Q-signatures<br />

The signatures described above can be modi®ed<br />

as outlined below to deal with problems that arise<br />

if neutron scattering materials are present in signi®cant<br />

amounts between the scattering sample<br />

and one or both of detectors B and F. For example,<br />

neutrons on paths (Fig. 1) leading directly<br />

from the scatterer to detector B (F) may interact<br />

with material present in region S 3 …S 4 †, thus reducing<br />

the intensity of the B (F) components of the<br />

scattering signature. If this attenuation is signi®cant<br />

then the ratio of B and F intensities will be<br />

a€ected and the signature will be distorted. This<br />

problem may be expected to occur in the envisaged<br />

practical applications of FNSA, for example when<br />

screening packages in which contraband items are<br />

hidden amongst other scattering material. It can<br />

be overcome <strong>by</strong> introducing Q-signatures, which<br />

are identical to the S-signatures listed in Table 1,<br />

except for the fact that the Q-signatures include an<br />

additional parameter k FB , which represents the<br />

ratio of the attenuation factors for neutrons scattered<br />

towards detectors B and F, respectively.<br />

Each Q-signature is derived from the corresponding<br />

S-signature, for example Q D0 is obtained from<br />

S D0 , <strong>by</strong> multiplying the F components of the S<br />

signature <strong>by</strong> the factor k FB . Thus Q-signatures are<br />

the same as corresponding S-signatures (Table 1)<br />

apart from the additional parameter k FB . When a<br />

Q-signature is used k FB is a free parameter which is<br />

determined in the unfolding procedure (Section 4)<br />

used to ®t the raw scattering signature measured<br />

for the sample under analysis. Experiments carried<br />

out to test the use of Q-signatures are described in<br />

Section 4.3.1.<br />

4. Analyses of scattering measurements<br />

The analysis of the FNSA signatures obtained<br />

in these test measurements (Section 2) followed a<br />

procedure similar to that described in [18]. Signatures<br />

were unfolded into elemental scattering signatures<br />

and background components, in order to<br />

determine atom fractions for the eight (or four, in<br />

certain cases) candidate elements in the scattering<br />

sample. The procedures used are summarized below,<br />

followed <strong>by</strong> a description of the least squares<br />

procedure used to assign materials to categories<br />

such as explosive, illicit drug or other.<br />

4.1. Unfolding of scattering signatures<br />

The scattering signature measured for each<br />

sample was unfolded into N ‡ 4 components,<br />

where N is the number of candidate elements<br />

considered in the analysis. The additional four<br />

components represent two measured backgrounds<br />

and two neutron multiple scattering components,<br />

respectively, one for E n ˆ 6:8 MeV and the other<br />

for E n ˆ 7:5 MeV in each case [18]. For analyses<br />

based on the S D0 (S L0 ) signature (N ˆ 8) the elemental<br />

signatures were those shown in Fig. 4 (Fig.<br />

5(a)). For analyses based on the S DZ or S LZ signatures<br />

(N ˆ 4) the elemental signatures were those<br />

shown in Figs. 5(b) and (c), respectively. For analyses<br />

based on the other signatures the elemental<br />

signatures were appropriate subsets of those<br />

shown in Figs. 4 or 5. Background and multiple<br />

scattering components were determined or speci-<br />

®ed as described in [18].<br />

Unfolding was carried out using the MIEKE<br />

program [22,23] which forms part of the HEPRO<br />

spectrum unfolding package [24,25]. The MIEKE<br />

code makes use of a Monte Carlo importance<br />

sampling algorithm which draws spectra at random<br />

from a probability density distribution [25] in<br />

order to calculate expectation values and uncertainties<br />

for the N ‡ 4 components which are ®tted<br />

to the unknown scattering signature. The unfolding<br />

procedure using the S D0 signature is described<br />

below. The same description is valid for all S-signatures<br />

and Q-signatures described in Section 3.<br />

When a Q-signature is used, the factor k FB (Section<br />

3.5) is an additional parameter which is also determined<br />

in the unfolding procedure.<br />

Using notation similar to that introduced previously<br />

[18], the scattering signature S…n† measured<br />

for a sample composed from N elements in un-


494 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

known proportions can be represented <strong>by</strong> the<br />

equation<br />

S…n† ˆXN‡4<br />

iˆ1<br />

f i S i …n†<br />

…1†<br />

in which the functions S i …n† represent the following:<br />

i ˆ 1toN represent the elemental scattering<br />

signatures (as in Fig. 4) for the N elements;<br />

i ˆ N ‡ 1 and N ‡ 2 represent smoothed distributions<br />

based on the background measurements<br />

made at 6.8 and 7.5 MeV, respectively; and<br />

i ˆ N ‡ 3andN ‡ 4 denote linear functions which<br />

are used [18,19] to represent small multiple scattering<br />

contributions at 6.8 and 7.5 MeV, respectively.<br />

The unfolding analysis determines the<br />

values and standard deviations for the N ‡ 4, coecients<br />

f i which give the best ®t to the scattering<br />

signature S…n†. The atom fraction a i of element i in<br />

the sample is given [18] <strong>by</strong><br />

,<br />

X N<br />

a i ˆ f i f i<br />

…2†<br />

iˆ1<br />

and the mass M of the scattering sample, in kg, is<br />

given [18] <strong>by</strong><br />

M ˆ 0:1 XN<br />

iˆ1<br />

f i A i ;<br />

…3†<br />

where A i is the mass number of nuclide i. Masses<br />

determined from Eq. (3) will be underestimated if<br />

there is signi®cant attenuation of neutrons between<br />

the scattering sample and either of the<br />

neutron detectors, B or F, in other words if a Q-<br />

signature has to be used in the unfolding analysis.<br />

However, the atom fractions obtained from Eq. (2)<br />

should be insensitive to such scattering e€ects.<br />

Fig. 6(a) shows, for example, the raw S D0 signature<br />

(histogram) measured for a sample of<br />

acetamide (H 5 C 2 NO, mass 0.212 kg), together<br />

with the refolded distribution (curve) obtained<br />

from the MIEKE unfolding of this signature. The<br />

atom fractions derived (Eq. (2)) from the unfolding<br />

are plotted in panel (iii) of Fig. 7(a). Points<br />

show the experimentally determined values for the<br />

elements H, C, N, O, Al, S, Fe and Pb, corresponding<br />

to i ˆ 1±8, respectively, and the histogram<br />

shows the atom fractions calculated from the<br />

chemical formula of acetamide. The results of<br />

similar measurements and analyses made on ®ve<br />

other compounds, using the S D0 signature, are<br />

shown in the other panels of Fig. 7(a). Masses of<br />

the six samples determined from the same measurements<br />

(Eq. (3)) are in good agreement with<br />

values obtained <strong>by</strong> weighing (see Table 2).<br />

The S L0 signature measured for acetamide is<br />

shown in Fig. 6(b), together with the refolded<br />

distribution obtained from MIEKE unfolding<br />

analysis. Atom fractions and masses obtained<br />

from the unfolding of the S L0 signatures obtained<br />

for the same six compounds as in Fig. 7(a) are<br />

shown in Fig. 7(b) and Table 2, respectively. The<br />

atom fractions obtained using the S L0 signature are<br />

less accurate than those obtained using the S D0<br />

signature, but both signatures lead to results (Fig.<br />

7) which are consistent with the known values for<br />

the samples used. Masses determined (Eq. (3))<br />

using the S L0 signatures are less reliable than those<br />

obtained using the S D0 signatures (Table 2). Previous<br />

work [18] demonstrated that FNSA was<br />

successful in determining atom fractions for H, C,<br />

N and O in samples composed from these elements<br />

alone. The present results (Fig. 7) show that the<br />

atom fractions of these important light elements<br />

can still be determined accurately when a larger set<br />

of candidate elements (8 instead of 4, and including<br />

heavy elements) is used in the samples and the<br />

analysis.<br />

4.2. Identi®cation of scattering materials<br />

The identi®cation of speci®c compounds or<br />

materials from atom fractions determined in the<br />

unfolding analysis can be facilitated <strong>by</strong> introducing<br />

a weighted chi-square coecient<br />

v 2 …x; k† ˆXN<br />

iˆ1<br />

,<br />

2<br />

a i b ik<br />

N XN<br />

Da i<br />

iˆ1<br />

…Da i † 2 ; …4†<br />

where a i (Da i ) are the atom fractions measured<br />

for the N elements in an unknown sample x and<br />

b ik are the corresponding atom fractions for a<br />

candidate material k of known chemical composition.<br />

Eq. (4) is used to calculate v 2 …x; k† for each<br />

member k of a set of M candidate materials. If a


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 495<br />

Fig. 7. Atom fractions a i , measured (points) and calculated (histograms), for six di€erent compounds, (i)±(vi). The measured values<br />

were determined using: (a) the S D0 ; and (b) the S L0 signatures. Points indicate di€erent elements, plotted in order of increasing atomic<br />

number, as follows: crosses, H; solid circles, C; open triangles, N; open circles, O; solid triangles, Al; diamonds, S; open squares, Fe;<br />

solid squares, Pb. The six compounds were: (i) methanol; (ii) ammonium nitrate: (iii) acetamide; (iv) ammonium acetate; (v) aluminium<br />

oxide; and (vi) crystalline iron sulphate.<br />

Table 2<br />

Masses (in kg) determined for the test samples<br />

Sample<br />

Method Methanol Ammonium<br />

nitrate<br />

Acetamide<br />

Ammonium<br />

acetate<br />

Aluminium<br />

oxide<br />

Iron sulphate<br />

S D0 signature 0.286 (15) 0.305 (17) 0.208 (8) 0.272 (17) 0.601 (39) 0.318 (15)<br />

S L0 signature 0.348 (25) 0.350 (19) 0.223 (11) 0.265 (15) 0.584 (45) 0.615 (60)<br />

Weighing 0.288 (1) 0.298 (1) 0.212 (1) 0.272 (1) 0.618 (1) 0.284 (1)<br />

deep minimum value of v 2 …x; k† is found for one<br />

member k of the set, showing that x has atom<br />

fractions similar to those of k, it can be argued<br />

that x is most likely to be identi®ed with material<br />

k. For a convenient presentation of the screening<br />

tests, the reciprocal R…x; k† ˆ1=v 2 …x; k† is used<br />

and a screening function P…x; k† is introduced <strong>by</strong><br />

normalizing R…x; k† to a percentage value as follows:<br />

,<br />

X M<br />

P…x; k† ˆ100 R…x; k† R…x; k† : …5†<br />

kˆ1


496 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

Thus P…x; k† is a v 2 -based, percentage measure of<br />

the degree to which sample x matches member k of<br />

the set of M candidate materials. The distribution<br />

P…x; k† versus k displays a pro®le of the screening<br />

of x against the M candidate materials and the<br />

values of k corresponding to maxima in this pro®le<br />

indicate the candidate materials whose elemental<br />

compositions most closely resemble that of the<br />

unknown material x.<br />

Fig. 8 shows pro®les P…x; k† derived from<br />

screening of the scattering measurements made<br />

using the methanol sample. The pro®les presented<br />

in panels (a)±(f) of this ®gure were determined<br />

from atom fractions obtained using the scattering<br />

signatures S D0 , S L0 , S D1 , S D2 , S DZ and S LZ , respectively,<br />

with N ˆ 8 (4) for the ®rst four (last two)<br />

signatures. For example, the pro®les shown in<br />

panels (a) and (b) of Fig. 8 were calculated from<br />

the atom fractions shown in panels (i) of Figs. 7(a)<br />

and (b), respectively. Forty-®ve materials<br />

(M ˆ 45) were selected for using as candidates in<br />

the screening process. These materials are listed in<br />

Table 3, together with their assigned k-numbers<br />

and atomic compositions. The candidates are<br />

classi®ed in four groups, numbered g ˆ 1±4 as<br />

follows: g ˆ 1, element samples (k ˆ 1±8), comprising<br />

the eight elements used in this study; g ˆ 2,<br />

explosives (k ˆ 9±18), ten well-known explosives;<br />

g ˆ 3, illicit drugs (k ˆ 19±23), ®ve well-known<br />

drug materials; and g ˆ 4(k ˆ 24±45), 22 other<br />

materials, including chemical compounds used in<br />

the test measurements and some other commonly<br />

occurring materials.<br />

All pro®les obtained from the screening of the<br />

methanol data (Fig. 8) show a clear peak at the<br />

expected candidate number, k ˆ 27. The<br />

``strength'' P…x; k† of this peak varies between 43%<br />

and 80% depending on the signature used in the<br />

analysis. These results demonstrate the capability<br />

of FNSA to identify this material clearly from the<br />

other 44 candidates considered in the screening<br />

process. As expected, the S D0 signature provides<br />

the most positive identi®cation (P ˆ 0:80).<br />

In the screening of packages for contraband it<br />

will be more important to determine whether a<br />

suspect item or sample belongs to either of the<br />

contraband groups, g ˆ 2 or 3, than to identify the<br />

speci®c material k of the item. The group identi-<br />

®cation is facilitated <strong>by</strong> introducing a group pro®le<br />

function G…x; g† for unknown sample x, which is<br />

obtained <strong>by</strong> summing P…x; k† over the members k<br />

of each group g,<br />

G…x; g† ˆXq<br />

kˆp<br />

P…x; k†;<br />

…6†<br />

Fig. 8. Pro®le functions P…x; k† determined for the methanol<br />

sample (k ˆ 27) using six di€erent scattering signatures: (a) S D0 ,<br />

(b) S L0 , (c) S D1 , (d) S D2 , (e) S DZ and (f) S LZ . Also shown are the<br />

boundaries (in k) which de®ne the four groups g of candidate<br />

materials (see Table 3).<br />

where p and q represent the ®rst and last members<br />

of group g.<br />

The four histograms plotted in Fig. 9(a)±(d)<br />

show group pro®les G…x; g† obtained from the<br />

methanol data shown in panels (a), (b), (e) and (f),<br />

respectively, of Fig. 8. The point plotted below<br />

each histogram indicates the value of P…x; k† for<br />

methanol (k ˆ 27) for the corresponding signatures<br />

and is plotted at the value g ˆ 4, corresponding<br />

to the group in which methanol is<br />

classi®ed in Table 3. This presentation is used to<br />

illustrate the proportion of G…x; 4† strength that is<br />

allocated in the screening process to the correctly<br />

identi®ed material, in this example methanol. The


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 497<br />

Table 3<br />

Candidate materials and group classi®cations g<br />

g a k <strong>Material</strong> Atomic proportions<br />

H C N O X a<br />

1 1 Hydrogen 1 0 0 0 0<br />

2 Carbon 0 1 0 0 0<br />

3 Nitrogen 0 0 1 0 0<br />

4 Oxygen 0 0 0 1 0<br />

5 Aluminium 0 0 0 0 1<br />

6 Sulphur 0 0 0 0 1<br />

7 Iron 0 0 0 0 1<br />

8 Lead 0 0 0 0 1<br />

2 9 Ammonium nitrate 4 0 2 3 0<br />

10 C-4 16 8 11 11 0<br />

11 RDX/HMX 2 1 2 2 0<br />

12 EGDN 4 2 2 6 0<br />

13 PETN 8 5 4 12 0<br />

14 Nitrocellulose 7 6 3 10 0<br />

15 Nitroglycerine 5 3 3 9 0<br />

16 TNT 5 7 3 6 0<br />

17 Tetryl 5 7 5 8 0<br />

18 Picric acid 3 6 3 7 0<br />

3 19 Heroin 20 17 1 1 0<br />

20 LSD 25 20 3 1 0<br />

21 Cocaine 21 17 1 4 0<br />

22 Morphine 19 17 1 3 0<br />

23 Mandrax 14 16 2 1 0<br />

4 24 Paran wax 37 18 0 0 0<br />

25 Polyethylene 2 1 0 0 0<br />

26 Ethanol 6 2 0 1 0<br />

27 Methanol 4 1 0 1 0<br />

28 Water 2 0 0 1 0<br />

29 Ammonium acetate 7 2 1 2 0<br />

30 Nylon 11 6 1 1 0<br />

31 Lucite 4 2 0 1 0<br />

32 Polyurethane 10 5 2 1 0<br />

33 Acetamide 5 2 1 1 0<br />

34 Benzene 6 6 0 0 0<br />

35 Sugar 24 13 0 12 0<br />

36 Fe 2 …SO 4 † 3<br />

15H 2 O 30 0 0 27 5<br />

37 Wood 31 22 0 12 0<br />

38 Paper 10 6 0 5 0<br />

39 Cotton 27 18 0 13 0<br />

40 Silk 13 8 5 4 0<br />

41 Orlon 6 6 2 0 0<br />

42 Wool 9 6 3 3 0<br />

43 Melamine 2 1 2 0 0<br />

44 Polyester 2 3 0 1 0<br />

45 Aluminium oxide 0 0 0 3 2<br />

a Groups g are: 1, elements; 2, explosives; 3, illicit drugs; and 4, other materials.<br />

a Element X ˆ Al, S, Fe or Pb.


498 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

Fig. 9. Group pro®le functions G…x; g† (histograms) determined for the following scattering samples: (a)±(d) methanol; (e)±(h) and (n)±<br />

(p) ammonium nitrate; (i)±(l) acetamide; and (m) an illict drug simulant. The scattering signatures used in the analyses were: S D0 for (a),<br />

(e), (i) and (m); S L0 for (b), (f) and (j); S DZ for (c), (g) and (k); S LZ for (d), (h) and (l); Q D0 for (n); Q L0 for (o) and S D1 for (p). The points<br />

plotted beneath the histograms indicate the pro®le strength P…x; k† allocated to the correct sample material k in each case (see text).<br />

points in Fig. 9(a)±(d) therefore show the same<br />

data as the associated peaks at k ˆ 27 in Fig. 8.<br />

While the point values vary between 43% and 80%,<br />

as already noted with reference to Fig. 8, the associated<br />

g ˆ 4 strengths, G…x; 4†, exceed 90% for<br />

all four signatures, as can be seen from the histograms<br />

in Fig. 9(a)±(d). The group identi®cation for<br />

methanol is therefore emphatic even when the<br />

pro®le strength P…x; 27† measured for the compound<br />

itself is as low as 43%.<br />

Fig. 9(e)±(h) and Fig. 9(i)±(l) show results obtained<br />

from similar analyses of the data measured<br />

using samples of ammonium nitrate and acetamide,<br />

respectively. These results assign ammonium<br />

nitrate and acetamide unambiguously to the correct<br />

groups, explosives (g ˆ 2) and ``other materials''<br />

(g ˆ 4), respectively, for all signatures. For<br />

ammonium nitrate (Fig. 9(e)±(h)) the pro®le<br />

strength assigned to the compound is a large<br />

fraction of that assigned to the group, for all signatures.<br />

For acetamide (Fig. 9(i)±(l)) this fraction<br />

is smaller and more variable, probably because<br />

group 4 contains a wider selection of candidate<br />

materials with atomic compositions similar to<br />

acetamide. Similar results have been obtained<br />

from the measurements and analyses made for<br />

many other samples. Without exception the correct<br />

group is indicated <strong>by</strong> the maximum in the<br />

G…x; g† distribution.<br />

The total number of neutrons incident on the<br />

sample during each of the measurements represented<br />

in Fig. 9(a)±(l) was about 10 9 . A series of<br />

analyses were also carried out using various different<br />

subsets (di€erent numbers of events) of the<br />

data measured for acetamide. These analyses<br />

showed that a measurement for a minimum number<br />

of 10 8 neutrons incident on the sample would<br />

provide sucient data (using the arrangement of<br />

Fig. 1) to identify the group g of this typical<br />

scatterer (mass 0.2 kg) unambiguously. The minimum<br />

number of incident neutrons required for a<br />

successful analysis can be reduced simply <strong>by</strong> extending<br />

the F and B detectors so as to increase<br />

their solid angles. If the detectors shown in Fig. 1


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 499<br />

were extended into rings coaxial with the beam<br />

axis, for example, the minimum number of neutrons<br />

required would be reduced <strong>by</strong> a factor of 25.<br />

Fig. 9(m) shows the group pro®le G…x; g† obtained<br />

from a measurement made using a 0.11 kg<br />

sample of a material X, not listed in Table 3, which<br />

has H:C:N:O atom ratios of 15:11:1:1, similar to<br />

those of the g ˆ 3 group (illicit drugs) of Table 3.<br />

This screening of X, which was based on the S D0<br />

signature, points clearly to the illicit drugs group<br />

(g ˆ 3) and identi®es heroin (k ˆ 19) as the candidate<br />

of composition closest to that of X. The<br />

point plotted in Fig. 9(m) corresponds to the value<br />

of P…x; k† determined from the measurements on<br />

X, for k ˆ 19. This result con®rms that FNSA<br />

should be e€ective for detecting illicit drugs.<br />

4.3. E€ects of neutron interactions in material other<br />

than the scattering sample<br />

The S-signatures described in Sections 3.1±3.4<br />

are designed for analyzing measurements made in<br />

the open laboratory geometry depicted in Fig. 1, in<br />

which no additional neutron scattering material is<br />

present either in the neutron beam, e.g. in the regions<br />

S 1 or S 2 , or between the scattering sample S<br />

and neutron detectors F or B, e.g. in regions S 3 or<br />

S 4 . In any practical implementation of FNSA it is<br />

very likely that additional scattering material will<br />

be present in the package to be interrogated,<br />

possibly in the regions represented <strong>by</strong> S 1 ±S 4 in the<br />

laboratory geometry (Fig. 1). To investigate possible<br />

consequences of this situation, scattering experiments<br />

were carried out with additional<br />

scattering material placed in one or more of these<br />

regions. The e€ects of additional material in the<br />

neutron beam (regions S 1 and S 2 ) or between the<br />

scattering sample S and the neutron detectors<br />

(regions S 3 and S 4 ) were investigated independently.<br />

4.3.1. <strong>Material</strong> between sample and detectors (regions<br />

S 3 and S 4 )<br />

The Q-signatures described in Section 3.5 are<br />

designed to deal with problems caused <strong>by</strong> neutron<br />

interactions in material between the scattering<br />

sample and either or both of the neutron detectors<br />

F and B (Fig. 1). The e€ectiveness of these signatures<br />

was experimentally tested, for example in a<br />

measurement made using an ammonium nitrate<br />

scattering sample at S in Fig. 1, with slabs of lucite,<br />

60 mm thick, placed at positions S 3 and S 4 , between<br />

the scattering sample and detectors B and F.<br />

Independent experimental checks con®rmed that<br />

the lucite blocks reduced the intensities of scattered<br />

neutrons (3±8 MeV) reaching the detectors<br />

<strong>by</strong> about 30±50%. Pro®les G…x; g† obtained from<br />

the screening of the results obtained in the test<br />

measurement, using signatures Q D0 and Q L0 , are<br />

shown in Figs. 9(n) and (o), respectively. The<br />

corresponding k FB factors determined in the analysis<br />

(see Section 3.5) were 1.26 and 1.38, respectively.<br />

The analyses based on Q-signatures give<br />

G…x; 2† P 0:7 and thus assign this sample unambiguously<br />

to the correct group, g ˆ 2. These results,<br />

together with those of several other tests<br />

made using slabs of various materials and thickness<br />

in positions S 3 and/or S 4 (Fig. 1), con®rm that<br />

the procedures used to assign the sample group g<br />

can be rendered insensitive to moderate amounts<br />

of neutron scattering material between scatterer S<br />

and the detectors if Q-signatures are used in the<br />

analysis.<br />

4.3.2. <strong>Material</strong> in the neutron beam (regions S 1 and<br />

S 2 )<br />

The introduction of additional scattering material<br />

in the neutron beam, for example at positions<br />

S 1 or S 2 (Fig. 1) will obviously increase the<br />

numbers of neutrons detected <strong>by</strong> the scintillators F<br />

and B and therefore distorts the signature recorded<br />

for the scatterer S. Two possible solutions are<br />

suggested for this problem. Firstly, if the distribution<br />

of scattering material around S is known,<br />

or can be monitored, then it may be possible to<br />

orient the package being interrogated so as to<br />

position S in the neutron beam while also reducing<br />

other scattering material in the beam to a tolerable<br />

minimum. Alternatively, and assuming that a<br />

pulsed neutron beam is used, neutron time-of-<br />

¯ight information can be used to distinguish the<br />

scattering signatures from di€erent regions (volume<br />

elements) along the neutron beam. Experiments<br />

were undertaken as follows to test this<br />

approach. Two additional scattering samples were<br />

placed in the neutron beam (Fig. 1) at positions S 1


500 A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502<br />

and S 2 adjacent to S, thus forming an extended<br />

scattering sample consisting of three components<br />

or volume elements. One such test was carried out<br />

using an ammonium nitrate sample at S, an<br />

acetamide sample at S 1 and a methanol sample at<br />

S 2 . Before measuring the scattering signature of<br />

this triple sample arrangement two additional sets<br />

of scattering signatures were determined for the<br />

elements H, C, N and O, one set for samples at<br />

position S 1 and the other for samples at position<br />

S 2 . Together with the elemental signatures (Figs. 4<br />

and 5) measured for samples at the standard position<br />

S, this provided three signatures per element,<br />

one signature per element for each of the three<br />

positions or volume elements. The scattering signature<br />

measured for the triple scattering sample<br />

was then unfolded (Section 4.1) in the standard<br />

way, as expressed in Eq. (1), but summing to<br />

3N ‡ 4 terms instead of N ‡ 4 terms, to accommodate<br />

the additional two positions per element.<br />

The factors f i obtained from this analysis were<br />

then grouped into three sets, one for each position,<br />

and processed separately through Eqs. (2)±(6) to<br />

obtain atom fractions, pro®les and group pro®les<br />

for the three volume elements.<br />

Results obtained for sample S (ammonium nitrate)<br />

in the triple sample measurement are shown<br />

in Fig. 9(p). The ammonium nitrate sample is still<br />

clearly assigned (G…x; 2† > 0:6) to the g ˆ 2 group<br />

(explosive), regardless of the presence of two other<br />

samples in the incident neutron beam, one upstream<br />

and the other downstream of it. The group<br />

assignments for the two additional samples used at<br />

S 1 and S 2 in this test were also correct. These results<br />

demonstrate that reliable group assignments<br />

are obtained, even when signi®cant amounts of<br />

additional material are present in the neutron<br />

beam, if the appropriately modi®ed (multi-position)<br />

FNSA analysis procedure is used.<br />

5. Discussion and conclusions<br />

The nuclear characteristics on which the elemental<br />

scattering signatures used in FNSA are<br />

based are: (a) the elastic and inelastic di€erential<br />

scattering cross sections of the nuclides of di€erent<br />

elements, which determine the relative intensities<br />

of the elemental signature components (Figs. 4 and<br />

5) at di€erent incident neutron energies and scattering<br />

angles; and (b) the dependence of backscattered<br />

neutron energy on target mass number<br />

A, analogous to that underlying the well-known<br />

charged particle technique of Rutherford backscattering<br />

analysis. The FNSA test measurements<br />

presented here explored six di€erent scattering<br />

signatures of varying complexity, based on these<br />

properties. In the analyses of the FNSA test<br />

measurements each test sample was classi®ed in<br />

one of the four groups, element, explosive, illicit<br />

drug or other. All the signatures considered<br />

proved reliable for determining group aliations g<br />

(Table 3) of the test samples. In every test carried<br />

out, without exception, the correct group g was<br />

assigned.<br />

The signature which should be best-suited for<br />

detecting contraband in a given situation will depend<br />

on factors such as the size, nature and shape<br />

of the package to be screened, the energy and type<br />

of neutron beam available and the time available<br />

for carrying out the screening. Other signatures<br />

superior to, or more convenient than, those considered<br />

here might be devised. For example, signatures<br />

incorporating 2, 3 or 4 multiplexed<br />

neutron energies in the range 1±6 MeV appear<br />

promising because this region is rich in resonance<br />

structure for the nuclides 12 C, 14 N and 16 O and<br />

might therefore o€er distinctive signatures for<br />

these nuclides at conveniently lower neutron energies.<br />

The success achieved using pulse height only<br />

signatures, such as S L0 and S LZ (Sections 3.2 and<br />

3.4) should be particularly noted, in view of the<br />

associated implication that nanosecond pulsed<br />

neutron beams are not essential for FNSA. This<br />

success implies that it should be possible to construct<br />

FNSA systems, capable of identifying contraband<br />

such as illicit drugs or explosives with high<br />

reliability, from less expensive accelerator-based<br />

neutron sources.<br />

We have presented data and analyses from<br />

measurements in which an NE213 scintillator was<br />

used as the backward-angle detector B (Fig. 1).<br />

Parallel measurements were made using a deuterated<br />

scintillator (NE230) as detector B and gave<br />

results which achieved slightly better discrimina-


A. Bu‚er et al. / Nucl. Instr. and Meth. in Phys. Res. B 173 (2001) 483±502 501<br />

tion between di€erent elements than the results<br />

shown here for the NE213 detector. However, the<br />

improved performance obtained <strong>by</strong> using NE230<br />

is not considered sucient to justify the substantial<br />

extra cost of this detector for FNSA applications.<br />

Results obtained using an NE230 detector<br />

were presented in an earlier report [18].<br />

An important feature of the FNSA technique is<br />

the fact that it measures the elements which are<br />

essential for contraband detection (H, C, N and O)<br />

with similar sensitivity. This ensures that the<br />

atomic proportions of these di€erent elements in<br />

the sample are determined with similar accuracy,<br />

which leads to a more reliable identi®cation of<br />

contraband materials (groups 2 or 3 in Table 2).<br />

The potential of FNSA for identifying the lighter<br />

elements, lithium to boron, remains to be properly<br />

explored but looks promising, since the energy<br />

transfer in neutron backscattering increases as the<br />

mass number of the scattering nuclide is reduced.<br />

The tests described in Section 4.3 show that<br />

FNSA is insensitive to interference caused <strong>by</strong><br />

neutron interactions in materials other than the<br />

sample, provided the amounts of such materials<br />

present between sample and detectors or in the<br />

neutron beam are not excessive. Interference<br />

caused <strong>by</strong> limited amounts of material between<br />

sample and detectors is counteracted <strong>by</strong> using Q-<br />

signatures (Sections 3.5 and 4.3.1). Extended dual<br />

parameter signatures (Section 4.3.2) are successful<br />

in counteracting the e€ects of additional scattering<br />

material in the neutron beam.<br />

In conclusion, these laboratory studies provide<br />

further proof-of-principle con®rmation that<br />

FNSA o€ers a reliable, non-intrusive method for<br />

determining whether a sample material of mass 0.2<br />

kg, or more, is an illicit drug or an explosive. In all<br />

tests carried out, without exception, the test sample<br />

was assigned to the correct group (Table 3).<br />

Test measurements also demonstrated that FNSA<br />

is e€ective even when additional scattering material<br />

is present in the neutron beam or between the<br />

scattering sample and the neutron detectors. The<br />

tests also provided count rate information (see<br />

Section 4.2) from which inspection times for<br />

FNSA screening can be estimated. Further work<br />

should be directed towards the development of a<br />

pilot system that can be tested and evaluated in an<br />

environment similar to that in which screening for<br />

contraband would take place.<br />

Acknowledgements<br />

We thank the following for their interest in this<br />

work and their support: Dr. H Klein and Dr. M<br />

Matzke of PTB, Braunschweig, Germany, for<br />

valuable discussions and for making the HEPRO<br />

spectrum unfolding package available to us; M<br />

Herbert for assistance in the experimental work;<br />

D. Momsen, D. Boulton, G. Fowle and L. van<br />

Heerden for their technical assistance; the NAC<br />

Van de Graa€ group for their support, interest and<br />

assistance in the accelerator experiments; and the<br />

International Atomic Energy Agency, Vienna, and<br />

the South African Foundation for Research Development,<br />

for ®nancial support.<br />

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