Revision of the ISO 8529 Standards Calculations of the (AmBe) neutron spectrum

J.-L. Chartier

Production of the (AmBe) neutron spectrum

- Homogeneous compressed mixture - 2 types of (a , n) reactions a) 9Be + a 12C + n + 5.701 MeV - Break up reaction b) 9Be + a 8Be + a + n 1.665 MeV - Fission of Am

Computational tools for calculations (1)

Code SPAR (RSICC CCC-0228_001)

Calculations of stopping powers and ranges

Code Sources-4C (RSICC CCC-661)

Code system for calculating (a,n), spontaneous fission and delayed neutron sources and spectra

Code Norio
Code system for calculating (a,n) and (a,an) neutron spectra. Distributed by N.Tsujimura (JAEA)

Computational tools for calculations (cont.)

Code MCNPX 2.6.0

Transport of neutrons and alphas

Code SRIM 2008

Stopping and Ranges of Ions in Matter

Microsoft Studio Developer

Used for home-made Fortran softwares and modifications in SPAR code

Model of (AmO2 /Be) mixture

Spherical clusters of AmO2

Radius range from Rc= 0 up to 3 mm

Calculation of the a spectra at the cluster surface (modified SPAR code) for several values of Rc Graphs : a) with MCNPX b) with SPAR* code

0,10

Normalised alpha spectra versus cluster radius MCNPX

0,08

Na in E ( = 50 keV)

0,06

cluster cluster cluster cluster cluster cluster

radius = 2.5 microns radius = 2.0 microns radius = 1.5 micron radius = 1.0 micron radius = 0.5 micron radius = 0.1micron

0,04

0,02

0,00 3,5 4,0 4,5 5,0 5,5

Energy/MeV

0,10

Normalised alpha spectra versus cluster radius (f02_five)

0,08

cluster cluster cluster cluster cluster

radius radius radius radius radius

= = = = =

0.1 micron 0.5 micron 1.5 microns 2.5 microns 0.01 micron

Na in E ( = 50 keV)

0,06

0,04

0,02

0,00 3,5 4,0 4,5 5,0 5,5

Energy/MeV

Characteristics of (AmBe) source type X3

Capsule type X3, material stainless steel Capsule diameter x height (mm) : 22.4 x 31 Capsule lateral wall thickness (mm) : 2.4 Source materials : Be 4.6g ; AmO2 0.37g Nominal activity (appr.) : 37GBq (1 Ci) Emission rate (appr.) : 2.2 (10**6) n/s ISO spectrum : E average = 4.16 MeV

Calculations with Sources_4C code (1)

Option 1 : "homogeneous mixture" (tape 1) Modification of the "tape 5 input data" by inserting the a spectrum calculated at the Rc cluster surface (tape 5) instead of 241Am a spectrum Graphs: - theoretical neutron spectrum versus Rc - emission rate versus Rc (n/cm3) - average neutron energy versus Rc

Spectres-4C

(AmBe) theoretical spectra

0,8

AmBe_Sources_4C (normalised homogeneous) Model AmO2Be

0,6

neutrons per lethargy unit

0,4

ISO - LOG SOURCES-4C-LOG

0,2

0,1

10

Energy/MeV

0,8

AmBe_Sources_4C (normalised homogeneous) Model AmO2Be MC aspectrum cluster R=0.1mm f02_five

0,6

neutrons/s per lethargy unit

ISO - LOG SOURCES-4C-LOG

0,4

0,2

0,1

10

Energy / MeV

0,8

AmBe_Sources_4C (normalised homogeneous) Model AmO2Be MC aspectrum cluster R=0.5mm f02_five

0,6

neutrons/s per lethargy unit

ISO - LOG SOURCES-4C-LOG

0,4

0,2

0,1

10

Energy/MeV

0,8

AmBe_Sources_4C (normalised homogeneous) Model AmO2Be MC a spectrum cluster R=1.5mm f02_five

0,6

neutrons/s per lethargy unit

ISO - LOG SOURCES-4C-LOG-1.5m

0,4

0,2

0,1

10

Energy/MeV

0,8

AmBe_Sources_4C (normalised homogeneous) Model AmO2Be MC a spectrum cluster R=2.0mm f02_five

0,6

neutrons/s per lethargy unit

ISO - LOG SOURCES-4C-LOG-2.0mm

0,4

0,2

0,1

10

Energy/MeV

0,8

AmBe_Sources_4C (normalised homogeneous) Model AmO2Be MC a spectrum cluster R=2.5mm f02_five

0,6

neutrons/s per lethargy unit

ISO - LOG SOURCES-4C-LOG-2.5mm

0,4

0,2

0,1

10

Energy/MeV

"Sources-4C" X3 (AmBe) emission rate "Sources-4C" average energy

3,40x106

5,0 3,20x106

Emission rate for 37 GBq (X3 type source)

3,00x106 4,8

2,60x106

4,6

2,40x106

4,4 2,20x106 Emission rate "4C" vs Rc Eaverage "4C" vs Rc 2,00x106 4,2

1,80x106 0,0 0,5 1,0 1,5 2,0 2,5 3,0

Rc / mm

Average Energy / MeV

2,80x106

Calculations with Sources_4C code (2)

Taking into account the geometry of the neutron source type X3 with MCNPX 2.6.0 Graphs: - emergent neutron spectrum versus Rc (average spectrum on a spherical surface surrounding the source Tally F2) - emission rate versus Rc (n/cm3) - average neutron energy versus Rc

Sources-4C + MCNPX

(AmBe) theoretical spectra

0,8

AmBe only ISO - (4c+ MCNPX) - log

0,6

neutrons/s per lethargy unit

0,4

ISO 8529 - log (4c+MCNPX) AmBe only

0,2

0,0 0,1

10

Energy/MeV

0,8

AmO2Be ISO - (4c+ MCNPX) - log cluster radius = 0.1 micron

0,6

neutrons/s per lethargy unit

0,4

ISO 8529 - log (4c+MCNPX) cluster : 0.1mm

0,2

0,0 0,1

10

Energy/MeV

0,8

AmO2Be ISO - (4c+ MCNPX) - log cluster radius = 0.5 micron

0,6

neutrons/s per lethargy unit

0,4

ISO 8529 - log (4c+MCNPX) cluster : 0.5mm

0,2

0,0 0,1

10

Energy/MeV

0,8 0,8

AmO AmO Be Be 2 2 ISO ISO--(4c+ (4c+MCNPX) MCNPX) -- log log cluster clusterradius radius= = 2.0 1.5 micron micron
0,6 0,6

neutrons/s neutrons/s per per lethargy lethargy unit unit

0,4 0,4

ISO ISO8529 8529- -log log (4c+MCNPX) (4c+MCNPX)cluster cluster::2.0 1.5mm

0,2 0,2

0,0 0,0 0,1 0,1

1 1

10

Energy/MeV Energy/MeV

0,8

AmO2Be ISO - (4c+ MCNPX) - log cluster radius = 2.5 micron

0,6

neutrons/s per lethargy unit

0,4

ISO 8529 - log (4c+MCNPX) cluster : 2.5 mm

0,2

0,0 0,1

10

Energy/MeV

"Sources-4C_MCNPX" X3 (AmBe) emission rate "Sources-4C_MCNPX" average energy

3,40x106 4,8

3,20x106

Emission rate for 37 GBq (X3 type source)

3,00x106

4,6

2,60x106

4,4

2,40x106

2,20x106 Emission rate "4C" vs Rc Eaverage "4C" vs Rc 2,00x106

4,2

1,80x106 0,0 0,5 1,0 1,5 2,0 2,5 3,0

4,0

Rc / mm

Average Energy / MeV

2,80x106

Calculations with Sources_4C code (3)

Conclusions:
the general shape of the ISO reference spectrum is obtained, but: Strong differences (peaks, resolution, ) Much higher average energies No spectral contribution of the break-up reaction in the low energy range Sources_5A version

Calculations with Sources_5A code (1)

Version Sources_5A code E.F. Shores,G.E. Mueller and G.A. Schlapper Appl. Rad. and Isot. 59 (2003) pp. 151-158 A new 9Be(a,n) cross-section evaluation for use in the Sources computer code Should take into account the breakup reaction 9Be(a,a'n) by modification of tape4 branching fraction file

Calculations with Sources_5A code (2)

Practically the same results as those with Sources_4C code !!!

Calculations with "Norio" code (1)

Norio Tsujimura, T. Yoshida and T. Momose (Nuclear Fuel Cycle Engineering Laboratories) JAEA Rad. Prot. Dos. (2007), pp. 1-6
Calculations of anisotropy factors for radionuclide neutron sources due to scattering from source encapsulation and support structures

Calculations with "Norio" code (2)

Same model : spherical AmO2 clusters embedded in thick Be target Calculation of the a-particles spectrum at the sphere surface ( modified SPAR code) Calculation of the theoretical neutron spectrum taking into account both reactions: - 9Be (a,n) and 9Be (a,a'n) - cross-sections and their angular distributions (JENDL file 2005)

Calculations with "Norio" code + MCNPX 2.6

The "Norio" theoretical neutron spectrum is used as an input neutron spectrum in the input MCNPX file The characteristics of the X3 type source (geometry, materials, ) are also included in the MCNPX input file Calculation of the average emitted neutron spectrum on a spherical surface surrounding the source (Tally F2)

Calculated neutron spectrum of X3 source derived from ("Norio" + MCNPX) codes

Graphs: - neutron spectra (Tally F2) - emission rate versus Rc - average neutron energy

Norio + MCNPX

(AmBe) theoretical spectra

Influence of the initial alpha spectrum (1)

0,8

AmO2// Be (Norio23 + MCNPX) MCNPX Monte Carlo a spectrum cluster R=1.5mm JLC Monte Carlo aspectrum cluster R=1.5mm - neww -

3,0

2,5

0,6

neutrons/s per lethargy unit

Norio23+MCNPX R=1.5mm Norio23+MCNPX R=1.5mm Ratio JLC / MCNPX

2,0

0,4

1,5

1,0

0,2

0,5

0,0 0,1

0,0 1 10

Energy/MeV

Ratio

Influence of the initial alpha spectrum (2)

0,8 3,0

AmO2// Be (Norio23 + MCNPX) MCNPX Monte Carlo a spectrum cluster R=2.0mm JLC Monte Carlo aspectrum cluster R=2.0mm - neww 2,5

0,6

neutrons/s per lethargy unit

Norio23+MCNPX R=2.0mm Norio23+MCNPX R=2.0mm Ratio JLC / MCNPX

2,0

0,4

1,5

1,0

0,2

0,5

0,0 0,1

0,0 1 10

Energy/MeV

Ratio

0,8

AmO2/ Be ISO - (Norio23 + MCNPX) 241 Am alpha spectrum new version

0,6

neutrons/s per lethargy unit

ISO 8529 - log Norio23+MCNPX (AmO2Be)

0,4

0,2

0,0 0,1

10

Energy/MeV

0,8

AmO2// Be ISO - (Norio23 + MCNPX) Monte Carlo a spectrum cluster R=0.1mm new version
0,6

neutrons/s per lethargy unit

ISO 8529 - log Norio23+MCNPX R=0.1mm

0,4

0,2

0,0 0,1

10

Energy/MeV

0,8

AmO2// Be ISO - (Norio23 + MCNPX) Monte Carlo a spectrum cluster R=0.5mm new version
0,6

neutrons/s per lethargy unit

ISO 8529 - log Norio23+MCNPX R=0.5mm

0,4

0,2

0,0 0,1

10

Energy/MeV

0,8

AmO2// Be ISO - (Norio23 + MCNPX) Monte Carlo a spectrum cluster R=1.5mm new version
0,6

neutrons/s per lethargy unit

ISO 8529 - log Norio23+MCNPX R=1.5mm

0,4

0,2

0,0 0,1

10

Energy/MeV

0,8

AmO2// Be ISO - (Norio23 + MCNPX) Monte Carlo a spectrum cluster R=2.0mm new version
0,6

neutrons/s per lethargy unit

ISO 8529 - log Norio23+MCNPX R=2.0mm

0,4

0,2

0,0 0,1

10

Energy/MeV

0,8

AmO2// Be ISO - (Norio23 + MCNPX) Monte Carlo a spectrum cluster R=2.5mm new version
0,6

neutrons/s per lethargy unit

ISO 8529 - log Norio23+MCNPX R=2.5mm

0,4

0,2

0,0 0,1

10

Energy/MeV

"Norio_MCNPX" X3 (AmBe) emission rate "Norio_MCNPX" average energy

3,20x106 4,8

3,00x106

Emission rate for 37 GBq (X3 type source)

2,80x106

4,6

2,40x106

4,4

2,20x106

2,00x106 Emission rate "Norio" vs Rc Eaverage "Norio" vs Rc 1,80x106

4,2

1,60x106 0,0 0,5 1,0 1,5 2,0 2,5 3,0

4,0

Rc / mm

Average Energy / MeV

2,60x106

Characteristics of the (AmBe) source type X4

Capsule type X4,material stainless steel Capsule diameter x height (mm): 22.4 x 48.5 Capsule lateral wall thickness (mm); 2.4 Source material: same density as X3 source Nominal activity (appr.): 111Gbq (3 Ci)

0,8

AmO2// Be - source type X4 Y and Z Axis (Norio23 + MCNPX) Monte Carlo a spectrum cluster R=2.0mm
0,6

neutrons/s per lethargy unit

(Norio23+MCNPX) Y axis R=2.0mm (Norio 23+MCNPX) Z Axis R=2.0mm

0,4

0,2

0,0 0,1

10

Energy/MeV

(AmBe) source type X4

Fluence Z (tally F5) : 3.0129 E-3 n/cm per p.

Fluence Y (tally F5) : 3.4083 E-3 n/cm per p. Eaver = 4.340 MeV Fluence (tally F2) : 3.2914 E-3 n/cm per p. Eaver = 4.375 MeV

A few comments (1)

2 series of results were presented Neutron spectra obtained withNorio code are consistent with measured ones Higher average energy Continuation of calculations Which ones ? Estimation of uncertainties ?

A few comments (2)

Estimation of uncertainties is not easy - the manufacturer doesnt want to communicate the radioactive materials characteristics - the manufaturer doesnt know the r.m.s characteristics (density, ) with an accuracy lower than 20 to 30% - reproducibility of production ? - granulometry ?

A few comments (3)

For calculations modelling is necessary How to validate a model when input data are not accurately known? Calculations enable to visualize some modifications of the neutron spectrum with respect to selected input data Normalisation of calculated results ?

Many thanks for your patience