The PIGE technique at ATOMKI
and its applications in archaeometry
Árpád Zoltán Kiss
Institute of Nuclear Research of the Hungarian Academy of Sciences
ATOMKI, Debrecen
IAEA 1st Research Coordination Meeting on
Reference Database of Cross Sections for PIGE Spectroscopy
IAEA Headquarters, Vienna, Austria, 16-20 May 2011
OUTLINE
 Introduction:
The Section of Ion Beam Physics, ATOMKI
From nuclear gamma-spectroscopy to PIGE in ATOMKI
 Thick target gamma yields for PIGE
 PIGE cross section measurements
 Depth distribution measurements
 Planned work in the frame of PIGE CRP
 Examples of the application of PIGE in archaeometry
SECTION OF ION BEAM PHYSICS
Nuclear Astrophysics Group
Laboratory of Ion Beam Applications
RESEARCH PERSONNEL
participating in the IAEA PIGE CRP
László Csedreki
György Gyürky
Gusztáv Áron Sziki
Zita Szikszai
Imre Uzonyi
SECTION OF ION BEAM PHYSICS
Instrumentation
The 5MV VdG accelerator
 Beam: H+, D+, 4He+
 Energy range: 0.6-3.8 MeV
Home made particle accelerators
from the 1970’s
The 1 MV VdG accelerator
 Beam: H+, 4He+ 12C+, 14N+
 Energy range: 0.2-1.5 MeV
MGC-20 Cyclotron
ATOMKI Laboratory of Ion Beam Applications, Debrecen
Nuclear
microprobe
macro-PIXE
PIGE/DIGE
DIGE or d-PIGE= deuteron induced gamma-ray emission
Scanning Nuclear Microprobe (VdG-5 0o beamline)
 Oxford Microbeams Ltd.
 1.5 um x 1.5 um beam size
 HPT XZY-stage two-axis goniometer
 PIXE, PIGE, RBS, STIM techniques
 Simultaneous u-PIXE and PIGE
measurements of heavy and light
elements
(STIM = scanning transmission ion microscopy)
Applications:




Geology
Archaeology
Materials science
Characterisation of single aerosol
particles
 Micro-machining
Beamline for gamma spectroscopy (VDG-5 J30o)
Turntable for 2 Ge detectors
5 cm thick lead shielding
Applications:
 Nuclear astrophysics
 p-PIGE, d-PIGE
Gamma and X-ray detectors
HPGe 40% (ORTEC),
HPGe 20%(CANBERRA),
Clover 120%,
NaI(Tl)
X-ray detectors
Si(Li) and SUTW Si(Li)
Laboratory for sample preparation
Leybold UINIVEX 350
vacuum coating system
Zeiss Axio Imager Optical Microscope
with CCD digital camera
FROM GAMMA-SPECTROSCOPY to PIGE in ATOMKI
Examples I.
Study of radiative gamma capture reactions
(in collaboration with the University of Helsinki)
DSA measurement of short lifetimes in27Al.
A., Bister M., Luukkainen A., Kiss Á. Z., Somorjai E.: Anttila
Nucl.Phys. A 385 (1982)194.
The reaction 36S(,)40Ar: yield curve, excitation
energies and decay of 40Ar resonance levels,
Józsa M., Kiss Á.Z., Koltay E., Nyakó B. M. , Somorjai E., Keinonen J.,
Nucl. Phys. A 456 (1986)365.
FROM GAMMA-SPECTROSCOPY to PIGE in ATOMKI
Examples II.
Cross section measurements in nuclear astrophysics
(Collaboration with Bochum, LUNA, etc)
Absolute measurement of the 5/2+
resonance of 36Ar(p,)37K at Ep=918 keV.
Mohr P., Oberhummer H., Gyürky Gy. , Somorjai E., Kiss Á.
Z., Borbély-Kiss I., Phys. Rev. C 59 (1999)3:1790.
Proton capture cross section of Sr isotopes
and their importance for nucleosynthesis
of proton-rich nuclides
Gy. Gyürky, E. Somorjai, Zs. Fülöp, S. Harissopulos and P.
Demetriou, T. Rauscher, Phys.Rev. C64 (2001) 065803
Not for direct use in PIGE
but experience gained useful also for PIGE
THE PIGE TECHNIQUE AT ATOMKI
earlier results
Thick target gamma-yields for p-PIGE
Extension of the work done in
Helsinki
Ep: 1.7, 2.4, 3.1, 3.8, 4.2 MeV
Elements: Li – Sc (except Ne, Ar)
Results published
in the form of spectra…
… and in tabulated form.
Thick target gamma-yields for d-PIGE
(in collaboration with LRMF, Paris)
Deuteron energy interval:
0.7-3.4 MeV
Elements:
Li – Sc (except Ne, Ar)
Gamma ray production cross-sections for d-PIGE
120
100
80
60
40
20
T a rg e t: L iF
0
500
1000
11B(d,p)12B,
16O(d,p)17O
19F(d,p)20F
10
9
B e (d ,n ) 1 0 B
0
0
500
1000
1500
2000
D euteron energy[keV ]
35
12
E  = 1 6 7 4 ke V
10
8
6
T a rg e t: L iB O 2
4
E  = 9 5 3 ke V
2
11
500
1000
25
20
E  = 8 7 1 ke V
10
2000
5
16
O (d ,p ) 1 7 O
0
0
500
1000
1500
2000
D euteron energy[keV ]
D e u te ro n e n e rg y[ke V ]
6
T a rg e t: tita n iu m -o xid e
15
B (d ,p ) 1 2 B
1500
D ata from R ef.[14]
This w ork (m easured)
C ontrol m easurem ents
This w ork (extrapolated)
30
C o n tro l m e a su rem e n ts
5
4
3
2
E  = 6 5 6 ke V
T a rg e t: L iF
1
1 9 F (d ,p ) 2 0 F
0
G. A. Sziki, A. Simon, Z. Szikszai, Zs. Kertész, E.
Dobos, Nucl. Instr.Meth. B 251 (2006) 343
T a rg e t: B e
5
2000
C o n tro l m e a su rem en ts
0
C ro s s s e c tio n [m b a rn /s r]
9Be(d,n)10B,
478 keV (Li)
718 keV (Be)
953 keV (B)
1674 keV (B)
871 keV (O)
656 keV (F)
E  = 7 1 8 ke V
D e u te ro n e n e rg y [k e V ]
0
6Li(d,p)7Li,
1500
C o n tro l m e a su rem en ts
15
6 L i(d ,p ) 7 L i
0
C ro ss se ctio n [m b a rn /sr]
Reactions and most dominant -lines
E  = 4 7 8 ke V
C ross section [m barn/sr]
140
14
Deuteron energy: 0.6-2 MeV
Energy steps: 20-50 keV
20
C o n tro l m e a su rem en ts
C ross section [m barn/sr]
Standards:LiBO2, LiF, LiNO3, BN,
NH4BF4, BeO, CaF2
160
C ro s s s e c tio n [m b a rn /s r]
Thin samples: ~ 10-70 ug/cm2
Vacuum evaporation or
DC reactive magnetron sputtering
Thin film RBS analysis
0
500
1000
1500
D e u te ro n e n e rg y [k e V ]
2000
Estimated
accuracy: 5-10%
depending on Ed
Depth distribution of fluorine in implanted standard
samples
Samples: fluorine implanted into silicon wafer
energy and dose:
2 keV, 11015 at.cm-2
100 keV, 11015 at.cm-2
Experimental conditions:
Eres
= 872 keV
Ibeam
= 9 nA
Dbeamspot = 1 mm
Detector: 10 cm  10 cm
NaI(Tl)
Ddet-sample:  1cm
=0
Excitation curve and used resonance
Results:
Ion ranges of 3keV I in Si
(SRIM calculation)
PLANNED EXPERIMENTAL WORK
in the frame of the
IAEA CRP Reference Database of Cross Sections for PIGE Spectroscopy
To obtain accurate experimental cross section data
accurate determination needed:
- bombarding particle energy
- collected charge
- number of bombarded target nuclei
- efficiency of gamma detection
Planned new target chamber
on gamma spectroscopy beamline
 Positions for sample and calibration target
 Accurate measurement of beam current
 Gamma detector – target distance
and detection angle to the beam direction
easily variable
 Possibility to measure RBS simultaneously
Target validation is possible in the nuclear microprobe: micro-PIXE/RBS
Cross section measurements
Questions to be answered
 What detector angle to the beam axis to be used?
In literature one can find: 0, 30, 45, 55, 60, 90 and 135 degrees
 What is the detector solid angle?
 What about d-PIGE cross section measurements?
Further possibility to investigate:
Effect of various factors (experimental, matrix, etc.)
influencing analytical accuracy of PIGE data.
Application of PIGE in archaeometry
(examples)
Study of obsidian glasses
PIGE: 3.5 MeV proton energy,
PIXE: 2.0 MeV
Improvenments in detection technique:
Clover-BGO detector system
The aim of the work: to find
sub-groups among the classified
obsidian sources of the volcanic
Tokaj Mountains (NE Hungary-E
Slovakia).
Investigation of classical ring-stones and their imitations
In 17-18th c. Europe, a great interest towards the Greak and Roman art and
culture.  Great number of classicizing style objects or precise imitations .
Nowodays in museums they are often mixed with the originals.
 Hard to make difference between them.
Primarily made from minerals or glass
pastes.
In the later centuries different sorts of
artificial masses also appeared as
base materials.
The determination of elemental
compositions can make
differences betwen original
artefacts and later produced
copies.
PIXE/PIGE analysis similar to obsidians
Concentration
correspondences
for Na – Al (both
normalized to Si)
Similarity dendogram for
specimens using PIXE
data for elements occuring
in each sample
One of the results:
„Sacrificing Amor” is made of
glassy material.
Boron content
indicates that the glass-paste
can not be a Roman origin.
Investigation of incrusted pottery
• clay surface is incised to form a
pattern,
• coloured (white) substance is pressed
into the resulting lines,
• after burning: stable incrustation on
the pottery
 a very decorative
type of ornamentation
Questions to be answered:
 Can we identify the material used for this type of decoration?
 Can we observe regional/temporal differences in the composition of
the material used for the decoration?
micro-PIXE
C to Fe detected simultaneously by UTW and Be-W Si(Li)
micro-d-PIGE for N determination
Recent results
obtained in the frame of FP7 project CHARISMA
Archaeological glass seals
produced from ca. 1750-1850.
(Finnish Glass Museum)
All elements above C measured by PIXE
Monitoring the presence of boron
PIXE/PIGE simultaneously
Incrusted pottery (Bükk culture)
Determination of fluorine content
In the incrustation
Micro-PIXE/PIGE simultaneously
Thank you for your attention!