Using neutron resonances for non-destructive material analysis: the ANCIENT CHARM project

Using neutron resonances for non-destructive material analysis: the ANCIENT CHARM project Enrico Perelli Cippo and the ANCIENT CHARM Collaboration Departement of physics Giuseppe Occhialini, University of Milan-BICOCCA

ANCIEN CHARM is an EU funded adventure project under the New and Emerging Science and Technology (NEST) program of FP6. http://ancient-charm.neutron-eu.net/ach Partner Country Università degli Studi di Milano-Bicocca Italy Università degli Studi di Roma Tor Vergata Italy Leiden University the Netherlands Hungarian National Museum Hungary Universität Bonn Germany Technical University Delft the Netherlands Institute of Isotopes Chemical Research Centre Hungary Universität Köln Germany Central Laboratory of the Research Councils United Kingdom EC - JRC - IRMM Belgium And the expertise in neutron physics and instrumentation: H. Postma, M. Moxon

Aim of the project is to conjugate...neutron resonant Capture Imaging and other Emerging Neutron Techniques... for nondestructive analysis of material. Neutron Resonance Capture Imaging combined with Neutron Resonance Transmission Imaging non-invasive techniques for element-sensitive imaging

Aim of the project is to conjugate...neutron resonant Capture Imaging and other Emerging Neutron Techniques... for nondestructive analysis of material. Neutron Resonance Capture Imaging combined with Neutron Resonance Transmission Imaging In addition, related imaging methods: Prompt Gamma Activation Imaging (FRM II, IKI) Fe Cu Images thanks to T. Belgya, IKI

Aim of the project is to conjugate...neutron resonant Capture Imaging and other Emerging Neutron Techniques... for nondestructive analysis of material. Neutron Resonance Capture Imaging combined with Neutron Resonance Transmission Imaging In addition, related imaging methods: Prompt Gamma Activation Imaging Neutron Tomography (FRM II, IKI) (FRM II, IKI) Images thanks to FRM II ANTARES NT station

NRCA and NRT make use of epithermal neutrons E n up to 1 kev No sample preparation needed Non - destructive Negligible residual activation Neutron absorption resonances can be used for: Nuclide identification and quantification Elemental (& isotopic) composition

NRCA and NRT make use of epithermal neutrons E n up to 1 kev Pulsed white neutron beam (GELINA, ISIS) INES beamline at the ISIS spallation source Average current Neutron pulse width Flight path length Beam dimensions Flux at sample pos. 150 180 µa (p) 300 ns 23.0 m 50 x 50 mm 10 3 n/ev s cm2 at 10 ev

NRCA and NRT make use of epithermal neutrons E n up to 1 kev Pulsed white neutron beam (GELINA, ISIS) INES beamline at the ISIS spallation source 10 10 10 8 10 6 Average current Neutron pulse width Flight path length Beam dimensions Flux at sample pos. 150 180 µa (p) 300 ns 23.0 m 50 x 50 mm 10 3 n/ev s cm2 at 10 ev 10 4 10 2 Undermoderated beam at INES 10 0 1 100 10 4 10 6 10 8 Energy (mev)

NRCA and NRT make use of epithermal neutrons E n up to 1 kev Pulsed white neutron beam (GELINA, ISIS) Absorption resonances are identified with the TOF technique E n = 72.2985L t + t 0 2 FAST detectors and electronics are crucial

NRCA and NRT make use of epithermal neutrons E n up to 1 kev H <10 ev 1000-10000 ev He 10-100 ev 10000-100000 ev Li Be 100-1000 ev B C N O F Ne Na Mg Al Si P S Cl Ar K Ca Sc Ti V Cr Mn Fe Co Ni Cu Zn Ga Ge As Se Br Kr Rb Sr Y Zr Nb Mo (Tc) Ru Rh Pd Ag Cd In Sn Sb Te I Xe Cs Ba La-Lu Hf Ta W Re Os Ir Pt Au Hg Tl Pb Bi (Po ) (At) (Rn) (Fr) (Ra ) (Ac- Lr) noble gasses Lanthanides (Rare Earth elements) La Ce Pr Nd (Pm) Sm Eu Gd Tb Dy Ho Er Tm Yb Lu Actinides (Ac) Th (Pa) U (Np) (Pu)

The neutron resonance transmission set-up

The neutron resonance transmission set-up GS20 Pixel Frame neutron beam Glass disperser 2 mm Fibers PSND 10 x 10 GS20 Li-enriched scintillator pixels 25% efficiency at 10 ev 4 % efficiency at 1 kev 8 mm

Neutron spectrum from a GS20 pixel Counts 10 7 10 6 10 5 10 4 10 3 10 2 10 1 10 0 010 0 1 10 6 2 10 6 3 10 6 4 10 6 5 10 6 Energy (ev)

The transmission TOF spectrum 1000 100 Intensity (counts/µah) 10 1 0.1 0.01 10 5 10 6 10 7 TOF (ns)

The physical quantity measured is the transmission factor: T ( E) = C C in out = e X n x σ ( E) tot R( E)

The physical quantity measured is the transmission factor: T ( E) = T exp( t) = where S in, out are the signal obtained from the sample-in and sample-out for the flux, and B in, out are the background levels in the two cases. N is a normalisation constant. C C N in out S S = in out e ( t) ( t) X n x σ ( E) B B in tot out ( t) ( t) R( E) This is valid for all the values of t (in and off-resonances).

S in is the TOF transmission spectrum of the sample that has undergone - Dead time correction: DTCF = Co (1 - β ) 0 ; β = 0 ((2t-1)/2) + t i= (2t-1)/2 N( t) t 275 ns DT correction function is an integral function in t M. S. Moore, Rate dependence of counting losses in neutron time-of-flight measurements, Nucl. Instr. Meth. 169 245 (1980)

S in is the TOF transmission spectrum of the sample that has undergone - Dead time correction - Normalisation to neutron flux

S in is the TOF transmission spectrum of the sample that has undergone - Dead time correction - Normalisation to neutron flux - Normalisation to bin width

Definition of B in n n S n sample detector Only direct neutron passed through the sample give Signal.

Definition of B in 1000 Signal (exp. data) Baseline 3861 (SI,nofilters) 100 10 1 Background (estimated) 5 10 4 1 10 5 1.5 10 5 2 10 5 2.5 10 5 3 10 5 TOF (ns)

How to determine B in Black resonances background from SI with filters 100 10 1 0.1 8 10 4 1.6 10 5 2.4 10 5 3.2 10 5 4 10 5 4.8 10 5 TOF (ns)

How to determine B in Resonances used: Bi 800 ev 59 µs Co 132 ev 150 µs W 19 ev 390 µs Ag 5 ev 750 µs Cd 0.5 ev 3000 µs (also for reducing activitation by thermal neutrons)

How to determine B in Spectrum from a sample-in + black resonances run 1000 100 Intensity 10 1 Cadmium cut 0.1 Black resonances 0.01 10 5 10 6 10 7 TOF (ns)

How to determine B in Estimated background level 1000 100 Intensity 10 1 0.1 Background level 0.01 10 5 10 6 10 7 TOF (ns)

How to determine B in Estimated background interpolation 1000 100 Intensity 10 1 0.1 Background level 0.01 10 5 10 6 10 7 TOF (ns)

How to determine B in Estimated background level B in compared with Sample-in (no filters) S in 1000 100 Intensity 10 1 0.1 0.01 10 5 10 6 10 7 TOF (ns)

Bismuth problem: Resolution problems make the bismuth black resonance to be not a strightforward background point. Moreover, bismuth is itself a source of background 03851 DT-reduced intensity 100 Red: 03849 ( 7 mm Bi) Black: 03951 (14 mm Bi) Blue: 03952 (26 mm Bi) 10 5 10 4 5.5 10 4 6 10 4 6.5 10 4 7 10 4 TOF (ns)

How to determine B in The background is given by the interpolation of the background points whith the function: a + b exp(-ct) + d exp(-et) + f t g

How to determine B in T ( t) = N S S in out ( t) ( t) B B in out ( t) ( t) experimental data evaluated analytical function

AGS: a code for manipulation of TOF spectra Step 1: DT correction and normalisation to all spectra, calculation of background points Input: all the TOF spectra from INES DAE (in special format) N. B. Step 1 macro needs information about time channels and time offset: it has to be adapted to every different ISIS cycle

AGS: a code for manipulation of TOF spectra Step 1: DT correction and normalisation to all spectra, calculation of background points Step 2: calculation of the transmission factor and production of a REFITcompatible file Input: S in, out, B in, out spectra from Step 1, and 7 x 2 guess parameters (calculated outside AGS) Output: transmission factor in REFIT format and in text format

Transmission factor for Cu samples (INES, may june 2009) 2 mm Cu 8 mm Cu 1 0.8 0.6 T 0.4 0.2 0 2 10 4 3 10 4 4 10 4 5 10 4 6 10 4 7 10 4 8 109 4 10 4 10 5 TOF (ns)

Optimum NRT analysis approach: REFIT REFIT is a toolkit for analysis of transmission (and capture) neutron resonances spectra. Advantage: fully quantitative T ( E) = C C in out = e X n x σ ( E) tot R( E) Resonaces are Doppler broadened Data do not have infinitely good resolution

Optimum NRT analysis approach: REFIT REFIT is a toolkit for analysis of transmission (and capture) neutron resonances spectra. energy dependence of the nuclear crosssection from the resonance parameters Calculation of Doppler broadening (various models) Calculation of resolution Fitting of the simulated spectra with experimental data to find n(x)

Measured intensity Fitted intensity Measured intensity Fitted intensity 1 1 0.8 0.95 Measured intensity 0.6 0.4 0.2 Cu 65 As 75 Cu 63 0.9 0.85 Ag 109 Sb 121 0 200 300 400 500 600 0.8 3 4 5 6 7 8 9 10 Energy (ev) Energy (ev) Element As Sn Zn Sb Mn Ag Certified %wt 0.194 7.2 6.02 0.5 0.2 - Estimated %wt 0.20 7.65 6.97 0.45 0.21 12e -3

Simplified NRT analysis approach: area calibration REFIT is ideal but quite long Imaging requres the analysis of > 1000 spectra

Simplified NRT analysis approach: area calibration

Some previous NRT applications Investigations on nuclear fuel Priesmeyer and Harz, Isotopic content determination in irradiated fuel by neutron transmission analysis Atomkernenergie 25 109 (1975) Schrack et al., Resonance neutron radiography using an electron linac IEEE Trans. Nucl. Scie. 28 1640 (1981)

Some previous NRT applications Investigations on nuclear fuel Detecion of explosives C. Chen and R.C. Lanza, IEEE Trans. Nucl. Scie. 49 1919 (2002)

Some previous NRT applications Investigations on nuclear fuel Detecion of explosives Detection of diamonds in rocks Watterson and Ambrosi, Nucl. Instr. Meth. A 513 367 (2003)

ANCIENT CHARM gives IMAGES Imaging Non-destructive Cultural Heritage No sample preparation needed Negligible residual activation

Spatial resolution in NRT Intensity (AU) Indium wire scan 10 9 8 7 6 5 4 3 2 1 0 17 18 19 20 21 22 Position (mm) Space resolution of about 2.5 mm FWHM

Spatial resolution in NRT A mistery stack of many layers folded in a closed metal sheet..

Spatial resolution in NRT 40 mm.. Is revealed as thin (1 mm ) wires of different materials) ELEMENT-SENSITIVE IMAGING

ELEMENT-SENSITIVE IMAGING Ancient gegenbeschlag belt mount from the National Hungarian Museum, with glass and metal inlaying 3 x 3 pictures element-sensitive radiography Ag (16 ev) Cu ( 230 ev ) Zn ( 514 ev ) Images thanks to T. Materna and the AC collaboration

ELEMENT-SENSITIVE IMAGING 2D radiographies can be developed in 3D images with standard tomographic methods work in progress 0º 72º Cu (230 ev) Au foil on Al rod Au (58.5 ev) X Bronze rod Zn (514 ev) Cu Brass rod 20 mm Sn (111 ev)

NEUTRON RESONANT CAPTURE IMAGING SET-UP Array of 28 γ-detectors YAP scintillator: 51mm ø, 25mm thick ~20% solid angle coverage

NEUTRON RESONANT CAPTURE IMAGING SET-UP YAP scintillators 10 6 Counts 10 5 10 4 1000 Fast τ = 27 ns Neutron-insensitive 100 Efficiency about 35 % at 5 MeV 10 0 5 10 5 1 10 6 1.5 10 6 2 10 6 2.5 10 6 3 10 6 3.5 10 6 4 10 6 Energy (kev) Energy treshold to optimise S/B Simulated background spectrum

NEUTRON RESONANT CAPTURE IMAGING SET-UP Lithium carbonate collimators for pencil neutron beam INES shutter AC blockhouse collimation Pre-existing INES collimation AC shutter collimation Sample position 450 mm 400 mm

NEUTRON RESONANT CAPTURE IMAGING SET-UP Lithium carbonate collimators for pencil neutron beam INES shutter collimation (already present) 150 mm 50 mm Variable diameter AC shutter collimation 150 mm Variable diameter AC block-house collimation 100 mm 100 mm

Pencil beam : full collimation In sample: 2x2x0.5 mm scan step: 2.5 mm, 20 µamps

Conclusions and future perspectives Aim of ANCIENT CHARM is to conjugate...neutron resonant Capture Imaging and other Emerging Neutron Techniques... for non-destructive analysis of material. NRT offers element-sensitive imaging possibility Fast, non destructive Flexible Possibility of developing a 3D tomographic technique Future integration in the phase 2 ISIS TS2 plan