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High Resolution Neutron Resonance Absorption Imaging at a Pulsed Neutron Beamline

High Resolution Neutron Resonance Absorption Imaging at a Pulsed Neutron Beamline

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Published by Jimmy Fallony
The existence of resonance peaks in neutron absorption spectra in the epithermal range of energies enables unique non-destructive testing techniques. The deep penetration of epithermal neutrons provides an opportunity to perform a compositional analysis of a sample which is opaque to X-rays and thermal
neutrons. The neutron resonances in the transmission spectra constitute a characteristic pattern for many isotopes, which can be used to identify the isotope and to map the distribution of the isotope in a sample. The neutron transmission spectra can be measured with the time of flight (TOF) technique using a pulsed neutron source. Combining this method with a high resolution neutron counting detector enables substantial improvements of spatial
resolution of neutron resonance transmission imaging. Such a detector has been developed to register neutrons with 55um spatial
and 10–1000 ns temporal resolution Our proof-of-principle experiments at the ISIS pulsed neutron spallation source demonstrate
that compositional analysis of multi-element samples can now be performed with ~150um spatial resolution. Images of a test mask consisting of collected in the 1–100 eV energy range. The experimental results
demonstrate the potential for compositional analysis via resonance absorption transmission with high spatial resolution. In-bulk temperature measurement through Doppler broadening analysis will also benefit from this technique.
The existence of resonance peaks in neutron absorption spectra in the epithermal range of energies enables unique non-destructive testing techniques. The deep penetration of epithermal neutrons provides an opportunity to perform a compositional analysis of a sample which is opaque to X-rays and thermal
neutrons. The neutron resonances in the transmission spectra constitute a characteristic pattern for many isotopes, which can be used to identify the isotope and to map the distribution of the isotope in a sample. The neutron transmission spectra can be measured with the time of flight (TOF) technique using a pulsed neutron source. Combining this method with a high resolution neutron counting detector enables substantial improvements of spatial
resolution of neutron resonance transmission imaging. Such a detector has been developed to register neutrons with 55um spatial
and 10–1000 ns temporal resolution Our proof-of-principle experiments at the ISIS pulsed neutron spallation source demonstrate
that compositional analysis of multi-element samples can now be performed with ~150um spatial resolution. Images of a test mask consisting of collected in the 1–100 eV energy range. The experimental results
demonstrate the potential for compositional analysis via resonance absorption transmission with high spatial resolution. In-bulk temperature measurement through Doppler broadening analysis will also benefit from this technique.

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Published by: Jimmy Fallony on Feb 03, 2013
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3272 IEEE TRANSACTIONS ON NUCLEAR SCIENCE, VOL. 59, NO. 6, DECEMBER 2012
High Resolution Neutron Resonance AbsorptionImaging at a Pulsed Neutron Beamline
Anton S. Tremsin
 , Member, IEEE 
, Jason B. McPhate, John V. Vallerga, Oswald H. W. Siegmund,Winfried Kockelmann, Erik M. Schooneveld, Nigel J. Rhodes, and W. Bruce Feller 
 Abstract— 
The existence of resonance peaks in neutron absorp-tion spectra in the epithermal range of energies enables uniquenon-destructive testing techniques. The deep penetration of ep-ithermal neutrons provides an opportunity to perform a composi-tional analysis of a sample which is opaque to X-rays and thermalneutrons. The neutron resonances in the transmission spectra con-stitute a characteristic pattern for many isotopes, which can beused to identify the isotope and to map the distribution of the iso-tope in a sample. The neutron transmission spectra can be mea-sured with the time of 
ight (TOF) technique using a pulsed neu-tron source. Combining this method with a high resolution neu-tron counting detector enables substantialimprovements ofspatialresolution of neutron resonance transmission imaging. Such a de-tector has been developed to register neutrons with 55 spatialand 10–1000 ns temporal resolution Our proof-of-principle exper-iments at the ISIS pulsed neutron spallation source demonstratethat compositional analysis of multi-element samples can now beperformed with spatial resolution. Images of a testmaskconsistingof thickfoilsofAu,Ag,InandGdwerecollected in the 1–100 eV energy range. The experimental resultsdemonstrate the potential for compositional analysis via resonanceabsorption transmissionwith high spatial resolution. In-bulk tem-perature measurement through Doppler broadening analysis willalso bene
t from this technique.
 Index Terms— 
High-resolution imaging, materials testing, neu-tron radiography, nondestructive testing.
I. I
 NTRODUCTION
N
EUTRON resonance absorption spectroscopy is basedon the presence of narrow neutron absorption featuresat unique energies characteristic of individual isotopes of eachelement. For many elements the energies of neutron resonantabsorption are in the epithermal range of 1 eV. The ab-sorption of a neutron results in a nucleus in an excited state
Manuscript received January 20, 2012; revised June 20, 2012 and August09, 2012; accepted August 22, 2012. Date of publication October 03, 2012;date of current version December 11, 2012. This work was supported in part bythe U.S. Department of Energy under STTR Grants DE-FG02-07ER86322 andDE-FG02-07ER86353.A. S. Tremsin, J. B. McPhate, J. V. Vallerga and O. H. W. Sieg-mund are with the Space Sciences Laboratory, 7 Gauss Way, Universityof California, Berkeley, CA 94720 USA (e-mail: ast@ssl.berkeley.edu;mcphate@ssl.berkeley.edu; jvv@ssl.berkeley.edu; ossy@ssl.berkeley.edu).W.Kockelmann,E.M.SchooneveldandN.J.RhodesarewithSTFC,Ruther-ford Appleton Laboratory, ISIS Facility, Harwell Oxford, Didcot, OX11 0QX,U.K. (e-mail: winfried.kockelmann@stfc.ac.uk; erik.schooneveld@stfc.ac.uk;nigel.rhodes@stfc.ac.uk).W. B. Feller is with Nova Scienti
c, Inc., Sturbridge, MA 01566 USA(e-mail: bfeller@novascienti
c.com).Color versions of one or more of the
gures in this paper are available onlineat http://ieeexplore.ieee.org.Digital Object Identi
er 10.1109/TNS.2012.2215627
that promptly returns to the ground state via the emission of several gamma-ray photons. These photons can be detected byconventional gamma-ray detectors and the energy of absorbedneutron can be obtained with a neutron time of 
ight technique, providing the sample is interrogated by a shar  p neutron pulse[1]. In this method, often referred to as neutron resonancecapture analysis (NRCA), there is no need to measure theenergy of the gamma photons. This substantially simpli
es thedetection equipment used in the experiment, however that iscompensated by the requirement to use a pulsed neutron beam. NRCA is somewhat similar to prompt gamma ray activationanalysis (PGAA) [2], [3], where the sample is irradiated bythermal or cold neutrons and the spectrum of prompt gammarays is measured. In the latter case a continuous beam of neu-trons can be used, but the energyof gamma ray photons needsto be registered. However, some materials can be activated bythis method and can be radioactive for a long period of time.In contrast, the interrogation by epithermal neutrons leads to alower activation of the samples as the absorption primarily oc-curs only at the nuclear r esonances and only a small fraction of incoming
ux contributes to sample activation and the excitednucleus, in many cases, returns to the ground state promptly.The thermal and cold neutrons in these experiments often can be
ltered out by a relatively thin thermal neutron absorber.Another advantageof interrogation with epithermal neutronsis their ability to penetrate thick samples which are opaque tothermal and cold neutrons as well as to X-rays.Both NRCA and PGAA techniques have limited spatial res-olution de
ned by the area of the interrogation beam. A vari-ation of the NRCA technique, where the spectrum of neutron beam transmitted through the sample is measured enables neu-tron resonance absorption imaging [4]–[9]. In this method theneutrons transmitted through the sample are measured by thedetection system and theenergyof eachregistered neutron isre-constructed from its time of 
ight (TOF), providing the detector has suf 
cient spatial and temporal resolution for each detectedneutron.This non-destructive imaging technique is unique in itsability to provide a spatial distribution of isotopes within thesample.Moreover, the 2-dimensional distribution of isotopescan be obtained from a single measurement performed with a proper neutron counting detection system.The potential of neutron resonance absorption imaging(NRAI) was demonstrated by previous measurements, wherea number of museum artifacts were studied in terms of their constituent materials [4], [6], [9]. The depths of neutron ab-sorption resonances can be translated into quantitative amountsof speci
c elements in the sample, with the spatial resolution
0018-9499/$31.00 © 2012 IEEE
 
TREMSIN
et al.
: HIGH RESOLUTION NEUTRON RESONANCE ABSORPTION IMAGING AT A PULSED NEUTRON BEAMLINE 3273
de
ned by the detector pixellation used in the experiments. For a typical
ight path of 15 m the time of 
ight of a 10 eV neutronis . For such a beamline the timing resolution of thedetector needs to be in the sub- range to well characterizethe narrow resonance features. A detector with a small number of GS20 glass scintillator pixels coupled to multichannel photomultipliers has demonstrated the power of the neutronresonance absorption imaging to spatially map given elementswithin samples [9].To advance these experiments to a higher spatial resolution aneutroncountingdetectorwithmicrochannelplates(MCPs)anda Timepix readout was tested in initial proof-of-principle exper-iments conducted at the ISIS pulsed neutron source at Ruther-ford Appleton Laboratory, UK. The MCP detector used in our experiments is capable of neutron counting with simultaneousspatial and temporal resolution, enablingan order of magnitude improvement compared to previous mea-surements performed with a 10 10 pixel detector with pixels [6], [9].II. E
XPERIMENTAL
S
ETUP
Microchannelplatebasedeventcountingdetectorsarewidelyused in time of 
ight applications (e.g. detecting electrons inangle-resolved photoemission spectroscopy, ARPES, on syn-chrotronsources[10]aswellasphotonsin
uorescencelifetimeimaging [11] requiring sub-ns temporal resolution). With theadvent of neutron sensitive MCPs all the advancements in thistechnology can now be applied to NRAI. The spatial resolutionofMCPdetectionsystemsistypicallyonthescaleof20–50 .Their intrinsic temporal resolution is sub-nanosecond, however for neutron detection it is energy dependent and is de
ned bythe depth of the neutron interaction within 1 mm thick MCPs.For thermal neutrons the resolution is , while in theepithermal range it is much better since these neutrons travelwith higher velocities. The ef 
ciency of our MCP detector wasshown to reach 70% for cold neutrons [12], [13], while in theepithermalrangeitissigni
cantlylowerduetothesmallercrosssection of absorption, which provides the primary signal intheMCP neutron detectors.However,the combinationof arela-tively low ef 
ciency and a high
ux of epithermal neutrons still provide suf 
cient statistics for NRAI, as is demonstrated by theresults of our experiments described in the next section.The active area of the detector used in the experiments waslimited to by the size of the Timepix readout [14].The detector was mounted 16 m from the source moderator in the direct neutron beam at the ROTAX beamline [15]. Thesamples were placed 12 mm from the detector active area.For each detected neutron the position (55 precision) andtime of 
ight ( 40 ns precision) were provided by the detector.During data acquisition the energy of each detected neutron wascalculatedfromitstimeof 
ightandthenthecountwasaddedtoa corresponding energy slice at the position of the event XY. Aset of images,each corresponding to a 500 ns time of 
ight in-terval, was recorded in our experiments. From this X, Y, T “datacube” a transmission spectrum can be reconstructed for each pixel of the detector. From transmission spectrain the epithermal range the elemental distribution of certain ma-terials was reconstructed through the resonance absorption fea-tures which provide a high contrast in a narrow energy range.III.
ESULTS
 A. NRAI Imaging of an In, Gd, Ag, Au Foil Mask 
To test the sensitivity of our experimental system in the reso-nance absorption range, a mask consisting of foils made fromseveral materials known to have resonances in the few eVrange was imaged (Fig. 1). The foils had straight edges whichwere offset so that edges of individual materials could be im-aged at the resonance energies. In order to reconstruct the trans-mission spectrum of a particular material the measured trans-mission of the material shouldbenormalized bythespectrumof the unattenuated neutron beam. An area not containing any foilswas used to obtain a spectrum of the unobscured (“open”) neu-tron beam. It was discovered by post-experiment analysis thatthe spectrum of the neutron beam had some variation across the
eld of view. Therefore, for an accurate normalization of mate-rialtransmissioninagivenarea,theopenbeamspectrumshould be measured for exactly the same area. The largest spectral gra-dient across the
eld of view was observed at the highest ener-gies (shortest time of 
ight) and was most likely caused by theresidual shadow of the beam chopper, which was used to elim-inate the gamma
ash emitted at the time of the spallation. Thetime of 
ight spectrum measured for the entire active area of thedetector and the spectrum of the “open beam” area are shownin Fig. 2. Resonance absorption dips are seen at certain ener-gies in the spectrum shown in Fig. 2(a). In the present work alltransmission spectra were normalized by the open beam mea-sured over the entire area, Fig. 2(b). For accurate quanti
cationexperiments the open beam spectrum should be taken for thesameareaastheoneto benormalized.Variationofthespectrumacross the
eld of view can be properly corrected in the latter case. The high
ux at the TOF 0–100 range indicates thatthere are a large number of fast neutrons as well as secondarygammas in the neutron beam. The neutron counting capabilityof our detection system with accurate timing for each neutroncan be used to eliminate these neutrons from transmission ra-diography measurements as the contrast in this energy range inmost objects is low.Transmission spectra of areas corresponding to different foilsare shown in Fig. 3 as a function of neutron energy calculatedfrom the time of 
ight. Two resonance lines are fully saturated,absorbingallneutronsfromtheincidentbeam;thenon-zerobot-tomsoftheselinesareduetobackgroundneutronspresentintheexperimental bunker that are not correlated with the interroga-tion neutron pulse or arrive at the detector from a different di-rection. Absorption spectra, produced by normalizing the trans-mission spectra by the spectrum of interrogating neutron beam,are shown in Fig. 4 together with the database spectra [16]. Thetransmission spectra of Fig. 4 were obtained by normalizationof spectracorresponding to Au,Ag,and In (Fig.3(b),3(c),3(d)) by the open beam spectra Fig. 3(a). The gradual increase of thetransmission at low energies seen in Fig. 4(c) and 4(e) is dueto the variation of open beam intensity across the
eld of view,which was not properly normalized in the present work as no
 
3274 IEEE TRANSACTIONS ON NUCLEAR SCIENCE, VOL. 59, NO. 6, DECEMBER 2012
Fig. 1. Schematic diagram of a test mask containing thin foils of Au (20 ),Ag (50 ), In (400 ) and Gd (250 ). The mask was placed on the inputwindow of the detector at a distance of 12 mm from the active area.Fig. 2. Transmission spectra measured with the foil mask as a function of neu-tron time of 
ight. Vertical axis represents the average number of counts in a 55 pixel per 0,521 time bin. Integration time 3 hours. (a) Transmissionspectrum integrated over the entire image. (b) Unobscured (“open beam”) areaat the left bottom corner. This spectrum is used to normalize the transmissionof the foils.
 properopenbeam spectrumwasacquired.Theabsorptionpeaksare also somewhat smoothed by the 0.5 binning used duringmeasurements.The amplitude of a resonance absorption peak is determined by the strength of the resonance as well as the thickness of thefoil and some of the peaks reached the saturation value. The ab-solute value of some measured peaks does not correspond ex-actly to the values predicted by theory due to two factors: the
Fig. 3. Neutron transmission spectra measured with the foil mask. Pixels incertain areas, corresponding to particular materials as well as open beam area,were grouped together and the average number of registered neutrons per pixel per energy bin is shown as a function of neutron energy.Fig. 4. Neutron absorption spectra measured (and calculated from tabulatednuclear data on cross sections) at the regions of the image containing foil of thematerial speci
ed in the legend. The theoretical curves are calculated for theabsorption of 50, 400 and 20 thick foils of Ag, In and Au, respectively. Thenormalization of experimental data was performed by the same open beam areain the left bottom corner of Fig. 1 as there was no full open beam transmissionspectra acquired in the measurements.
 presence of background and scattered neutrons in the experi-mental bunker and the
nite time binning of our data acquisi-tion system. A proper beam characterization can be performedto account for the background neutrons and used for all consec-utive measurements at the same beamline. A set of thick foilsor sheets of different materials with saturated peaks at differentenergies can be measured, and the difference between the satu-rated unity value and the measured peaks can be obtained at dif-ferent energies. An interpolated curve of background level can becalculatedfromthismeasurementandusedforproperspectra

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