PIGE experience in IPPE
A.F. Gurbich
Institute of Physics and Power Engineering,
Obninsk, Russia
Overview
•
For the analysis of carbon, sodium, aluminum, and chromium resonance PIGE was
employed. The excitation functions for the corresponding reactions were measured in the
vicinity of resonances favorable for analytical applications.
•
The oxygen analysis using gammas from direct non-resonant radiative capture was
undertaken.
•
PIGE was used for the analysis of various samples including semiconductor structures and
nuclear reactor materials.
•
Hydrogen analysis using resonance 1H(19F,ag)16O reaction was used to study hydrogen
penetration into coating layers on the surface of zirconium pipes.
•
Propagation of the spectrometer efficiency calibration on the high energy region was made
using cascade gamma quanta from the resonance 27Al(p,g)28Si reaction with known
gamma ray branching.
•
Tickonov’s regularization method was applied to resolve the ill-posed problem of the
determination of concentration on depth distribution.
•
Pulsed incident beam was used to substantially enhance the sensitivity of the PIGE
analysis due to suppression of the background gamma-radiation.
Experimental facilities
Thick target yield for resonance
The resonance yield per unity solid angle and unity incident particles charge for prompt gamma-rays
emission from homogenous target with energy thickness of ET is defined as
Y  c
E
N
0
A

( p , g )
E  E T
dE / dx
dE ,
where N0 - is Avogadro constant, A - is a molecular mass, c - is element concentration in the target.
Assuming the Breit-Wigner resonance

( p , g )   R
2
/ 4
( E  ER )
2


2
4
where R - is a cross section at resonance energy ER and  - is a resonance width,
the yield for an infinitely thick target (ET>>) is
Y 
cN
0
R
2 A dE / dx
(

2
 t an
1
E  ER
 / 2
)
The R, , and ER may be regarded as free parameters and these have to be found by fit of theoretical yield
to measured data.
Thick target yield for the 23Na(p,p’g)23Na reaction (Eg=439 keV) in the vicinity
of the resonance and its theoretical description
− Bodart F., Deconninck G., Demortier G. Quantitative analysis of sodium by (p,g)-reactions. J. Radioanal.
Chem. 35 (1977) 95
− This measurement (target – NaCl, detector – Ge(Li), proton beam from the EG-2.5 Van de Graaff
accelerator of IPPE)
Deduced resonance parameters ER=1456 1.8 keV and =8.30.8 keV
Thick-target yield of gamma rays from the 27Al(p,g)28Si reaction
Ex, keV
12549
Gamma-Ray Yield, Rel. Units
400
27
12742
12935
13128
13321
1400
1600
1800
28
Al(p,g) Si
Eg= 9-11 MeV
300
200
100
0
1000
1200
Ep, keV
Resonance energies are indicated by bars
Thick target yield of g-rays at the 991.9 keV resonance in the
27Al(p,g)28Si reaction
Proton energy, keV
− Deconninck G., Demortier G. Quantitative analysis of aluminium by prompt
nuclear reactions. J. Radioanal. Chem. 12 (1972)189.
− This measurement
PIGE analysis of carbon
Ng
12
800
E g =2366 keV
кэВ
13
Intense resonances in the reaction
12С(p,g)13N (Q=1944.010.22 keV) are
observed at 0.457 and 1.699 MeV.
(а)
C (p, g ) N
E p =550 keV
кэВ
For the Еp= 457 keV resonance (total
width Г=35 keV, resonance crosssection =127 mb) the gray energy is
2.366 MeV.
600
E g =2452 keV
кэВ
max
400
For the Еp = 1.699 MeV resonance
(total width Г=70 keV, resonance crosssection =35 mb) the g-ray energy is
3.51 MeV.
200
0
6
(б)
(b)
4
2
0
2000
2100
2200
2300
2400
2500
2600
ray
energy
ЭGamma
нергия гам
м а-квантов
(a) – graphite
(b) – steel (~0.1% of carbon concentration)
Excitation function of the 52Cr(p,g)53Mn reaction
From R.L.Schulte et al. Nucl. Phys. A243 (1975) 202
Thick target yield of g-rays at the 1005 keV resonance in
the 52Cr(p,g)53Mn reaction
Proton energy, keV
The IAR at Еp = 1005 keV decays mainly through the levels at 2.87 MeV
(26%) and 3.18 MeV (20%) whereas the contribution of all other
resonances in population of these levels is small. Thus measured
spectra contain gamma quanta which are specific only for this resonance.
Gamma-ray spectrum (high energy part) for the decay of
the IAR at Ep=1005 keV in the 52Cr(p,g)53Mn reaction
100
52
53
C r(p , g ) M n
26%
R
80
2 8 7 5 ke V
E p= 1 0 2 0 k e V
2497 keV
60
20%
R
3 1 8 2 ke V
2804 keV
C o u n ts /C h a n n e l
E p= 1 0 0 0 k e V
40
20
0
1200
1400
1600
C hannel N um ber
1800
2000
Gamma-ray spectrum (low energy part) for the decay of the
IAR at Ep=1005 keV in the 52Cr(p,g)53Mn reaction
3000
378 keV
E p= 1 0 2 0 k e V
C o u n ts /C h a n n e l
E p= 1 0 0 0 k e V
2000
52
53
C r(p , g ) M n
511 keV
1000
0
100
200
300
Channel Num ber
400
Counts/Channel
Oxygen analysis using gammas from direct non-resonant radiative capture
Channel Number
E g (E p ) 
M
M m
E p (x )  Q  E 1  E g
N ( E g ,  )E 
N
A
M
 ( E p )  ( E g ( E p ))  const
q  c( x )  ( E g ( E p ( x )))  ( E p ( x ),  )
x
co s 
The resonance parameters for the 1H(19F,ag)16O reaction
ER, MeV
6.418
9.121
, keV
44.1
17.1
Peak value
1675
669
11.198
12.583
15.686
575
80.1
105.5
2954
3867
3039
16.441
17.634
85.4
152.9
69847
38201
The gamma ray yield for the 1H(19F,ag)16O reaction. The EXFOR data for
the 19F(p,ag)16O reaction were converted for the case when 19F is a
projectile
G a m m a R a y Y ie ld , a rb itra ry u n its
600
1
500
19
16
H ( F ,a g ) O
400
300
 0 .1
200
100
0
6000
8000
10000
12000
14000
E n e rg y , k e V
16000
18000
20000
A typical spectrum of gamma quanta from the
1H(19F,ag)16O reaction measured with a NaI(Tl) detector at
the 19F2+ beam energy of 9.2 MeV
1500
NaI(Tl) 160150 mm
1
1200
Counts/Channel
19
16
H( F,ag) O
Eg = 6.13 MeV
900
600
300
0
0
50
100
150
200
250
Channel Number
300
350
400
The spectrum of gamma rays for the 27Al(p,g)28Si reaction
from which the spectrometer efficiency for high energy
gamma quanta was determined
2
1

I1 S 2
I 2 S1
,
Branching for a resonance in the 27Al(p,g)28Si reaction at Ep=767 keV
Angular distribution
100
W (  )  1  A 2 P2 (cos  )  A 4 P4 (cos  )
28
Al(p,g) Si
90
120
Ep=767 кэВ
12.323  4.617 MeV
10
60
30
150
4.617  1.779 MeV
Probability for emission, %
27
180
0
330
210
240
300
270
Solid line – Eg=7.706 MeV
1
0
1
2
3
4
5
6
g-ray energy, MeV
7
8
9
10
Dashed line – Eg=2.873 MeV
Resolving inverse problem using the regularization method
In order to derive the concentration on depth distribution c(x) the Fredholm
 c ( x ) F  E , x  dx
should be resolved. This ill-posed problem was resolved using Tickonov’s
equation of the first kind
Y E 0   
x max
0
0
regularization method.
The gamma ray yield
The derived hydrogen profile
units ед.)
arbitrary (отн.
Yield,
Гамма-выход
Gamma-ray yield for the aluminized steel sample
35000
30000
27Al(p,g28Si
25000
20000
15000
10000
5000
0
1000 1100 1200 1300 1400 1500 1600 1700
Ep, keV
кэВ
Dots – experiment
Line – theoretical fit
Block diagram of the electronics
P rea m p lifie r
L o g ic
Shaper
D e la y
P ic k -u p
s to p
s ta rt
T im e to
Am p litu d e
C o n v e rte r
D iffe r e n tia l
D is c r im .
T a rg e t
t
D e tec to r
Fas t
Am p lifie r
C o n s ta n t
F r ac tio n
D is c r .
s tro b e
P rea m p lifie r
E
S p e c tr o s c o p ic
Am p lifie r
An a lo g to
D igita l
C o n v e rte r
Channel Number (Energy)
Slits
Counts/Channel
Counts/Channel
0.75 ns/channel
Target
Energy and timing spectra
Channel Number (Time)
Characteristics of the reactions used for PIGE analysis of
the BN-600 atomic power plant steam generator wall
Reaction
g-ray energy, MeV
12C(p,g )13N
o
2.366
16O(p,g
17
1) F
Resonance
energy, MeV
0.457
16/17Ep(x)+0.105
Proton beam
energy
Depth resolution, Maximal
mm
depth, mm
0.5
0.2
4
0.8
0.04
3
23Na(p,ag)20Ne
1.634
1.011
1.011-1.070
0.016
0.6
23Na(p,p’g)23Na
0.440
1.283
1300
0.07

52Cr(p,g)53Mn
0.378
1.005
1.005-1.080
0.05
0.8
mass %
Sodium distribution near the surface of an oxidized silicon wafer
mm
The insert shows a part of gamma-spectrum around the sodium line at Eg=439 keV for
oxidized () and virgin () samples for irradiation with a proton beam of Ep=1470 keV
PIGE analysis of a semiconductor laser structure
~1~ mm
1м км
p -э митте р
p-emitter
p - G a 1-x A lx A s
N g (E p )
650
~ 0.2mm
м км
~0.2
~0.2
mm
А Active
ктивны йlayer
с ло й
p - G aA s
nn-emitter
- э митте р
4 - 5 mm
м км
4-5
n - G a 1-x A lx A s
~0 .8 mm
м км
600
550
П оSurface
в е р хн о сть
500
~0 .2 м
км
mm
450
400
П од слой
Sub-layer
4-5
4 - 5 mm
м км
350
n - G aA s
300
П од ло ж ка
Substrate
980
1000
1020
1040
1060
E p , кэ
В
keV
1080
1100
1120
1140
Aluminum depth profile near surface of the samples tested in the flow of melted lead.
Solid line – results obtained using 27Al(d,p0+1)28Al reaction. Dashed line – PIGE results.
0.45
Virgin
0.40
0.35
0.30
0.25
2000 hours
Atomic Concentration
0.4
0.3
0.2
0.1
0.0
3000 hours
0.4
0.3
0.2
0.1
0.0
4000 hours
0.3
0.2
0.1
0.0
0
1
2
Depth, mm
3
Mistakes in PIGE data presentation in IBANDL
PIGE data presentation in IBANDL
PIGE data problems
18
Na(p,p'g1-0)23Na
23
16
Mateus et al.
Caciolli et al.
Cross-section, mb
14
12
10
8
6
4
2
2200
2250
2300
2350
Proton energy, keV
2400
2450
Atomic Energy Review
Supplement No.2 (1981)
J.R. Bird, M.D. Scott, L.H. Russel, M.J.
Kenny, Analysis using Ion Induced g Rays.
Aust. J. Phys., 31 (1978) 209.