PIGE and resonant PIGE: Past efforts
and current needs
M. Kokkoris,
National Technical University of Athens, Greece
Structure of the Presentation:
1.
2.
3.
4.
5.
6.
7.
Historical Aspects
Status in Literature
Present Status
Interesting Contributions (since 1990)
Relevant Works from our Team
Experimental Capabilities – Tandem Accelerator
Future Measurements and Perspectives
1.
Historical Aspects
First (?) well-known publication introducing NRA in 1962 (the
original acronym refers to: Nuclear Reaction microAnalysis): ‘The
Mechanism of Anodic Oxidation’, G. Amsel, D. Samuel, Journal of
Physics and Chemistry of Solids [involves 18O(p,α) and 27Al(p,γ)]
First ‘Fight’: 1968 between B. Cox and G. Amsel over the use of
the 16O(d,p) reaction for the study of oxygen diffusion in solids
[raises questions about the shape of the cross section needed
for profiling]
First Ion Beam Analysis Conference: 1975
First Review Article on the Field: 1984 (‘Nuclear Reaction
Techniques in Materials Analysis’, G. Amsel, W.A. Lanford, Annual
Review of Nuclear and Particle Science 34: 435-460
2.
Status in Literature
It can be divided into 3 time periods: ‘Early years’ (>1960-1980),
‘Development’ (1980-1990), ‘Data and Applications’ (1990-today)
There is a great problem in terminology: The terms NRA,
resonant NRA, PIGE, AIGE, DIGE, HIGE or nothing (!) have been
used to describe the same technique, namely ‘material analysis
implementing nuclear data from low-energy γ-ray emission
reactions’. I could not find when the modern term (Particle
Induced Gamma-ray Emission) was first introduced – still the
community is divided. Here follows a short list (# papers, many
have been omitted):
TERM
>1960 – 1990
1990 – today
Main Journal
PIGE
~45
~285
Nucl. Instr. and Meth. (191), J. Rad. And
Nucl. Chem. (24)
NRA
~100 (mixed)
~770 (mixed)
Nucl. Instr. and Meth. (340), J. Nucl.
Materials (~60)
~20
Nucl. Instr. and Meth. (9), Proc. AMS (7)
DIGE
AIGE
~5
-
HIGE
~2-3
-
2.
Status in Literature
Remarks: The term ‘NRA’ remains almost time – invariant in
paper production, the term ‘PIGE’ is related to the IBA conference
proceedings (increase by a factor of ~2), denoting ‘applications’
not methodology or new data (especially after 2000)!
‘PIGE’
‘NRA’
(more than 50%
involve γ-rays)
No more than 20-30 papers concern nuclear data, methodology,
software and analysis data over the last ~20 years! What is the
meaning of this?
3.
Present Status
According to an IAEA survey there are ~200 small VdG type
accelerators over 40 countries. One can assume that PIGE
capabilities are available practically everywhere.
 PIGE is usually combined with PIXE (competition): PIXE is
generally preferred for Z>20 elements due to the much higher cross
sections involved, and the existence of reliable, widely used
analysis software (GUPIX etc.)
R-PIGE is usually combined with / compared to
RBS/EBS/ERDA/NRA (with charged particles): The former has
superior depth resolution but it is time-consuming, and cannot
depth profile efficiently all light isotopes/elements, while the latter
are based on reliable, widely used analysis software (SIMNRA,
WINDF etc.), evaluated and new data + library (IBANDL). How are
PIGE measurements performed in the vast majority of cases? NOT
absolutely, but through comparisons with standards.
3.
Present Status
 Present situation in software: IAEA has organized CRPs for
software evaluation for all the other profiling techniques, but not
for r-PIGE! Namely, ‘IAEA intercomparison of IBA software’ N.P.
Barradas et al., Nucl. Instr. and Meth. B262 (2007) 281,
‘Intercomparison of PIXE Spectrometry Software Packages’, IAEATEXDOC-1342. There have been two CRPs for γ-rays’ software, but
they did not touch the ‘core’ of PIGE, that is, how to perform
material analysis + element profiling: ‘Intercomparison of γ-Ray
Analysis Software Packages’, IAEA-TEXDOC-1011, and ‘Specialized
Software Utilities for γ-Ray Spectrometry’, IAEA-TEXDOC-1275. As a
result, all labs use home made codes (Greece: PGAMMA, Portugal:
ERYA, etc.) , thus how reliable are the obtained results?
 Present situation in data: PIGE involves (p,γ), (α,γ), (p,αγ), (p,p’),
(d,nγ), (d,pγ) etc. reactions in light and medium-Z elements with
and without strong resonances. Data exist in EXFOR (mainly) in the
form of ‘absolute reaction yield’, ‘total cross section’, ‘differential
cross section’. What is really needed? What is lacking?
3.
Present Status
 Present situation in scientific politics: Most traditional Nuclear
Physics labs in low energy reaction physics have shifted their efforts
to Nuclear Astrophysics, involving γ-ray measurements for medium,
medium-heavy ions. Possible reasons: a) ‘Modern’, exciting field,
good for young researchers, more closely related to NP than to CM
Physics, b) Theoretical treatment is easier (HF calculations, several
software codes available etc.) c) Publications in several high impact
factor journals (PRC, NP, EPJ) d) Existence of several academic
position openings while IBA is more closely related to accelerator
labs.
 Present situation in IBA: All competitive techniques, as shown
before, are in a better starting point. PIGE tends to become a
‘supplementary’ technique and to assume a semi-quantitative
nature (indirect comparison with standards).
4.
Interesting Contributions (since 1990)
 Portugal: Contributions both in cross section measurements for
the most important light elements with thin targets (23Na, 7Li, 19F,
10B, 27Al) and in methodology (software, sensitivity etc.).
 Italy: Contributions mainly in cross section measurements (19F,
7Li, 23Na) using thin targets.
 Hungary and Greece: Contributions in d-PIGE and PIGE for
several light and medium-Z elements using thick targets and usually
calculating absolute thick target yields.
 Russia and Finland: Thick target γ-ray yields and methodology.
 Spain and Germany: Thick target γ-ray measurements for 14N.
Romania: Interesting applications in coincidence with neutrons.
5.
Relevant Works from our Team
PIGE Data and Applications (1/2):
1.
2.
3.
4.
5.
6.
7.
‘On the Determination of Beryllium in Light Element Matrices using PIGE
and NRA’, G. Perdikakis, A. Spyrou, M. Kokkoris et al., Nucl. Instr. and Meth.
B 226 (2004) 622-630.
‘Fluorine Determination in Human Healthy and Carious Teeth using the
PIGE Technique’, M.L. Carvalho, C. Casaca, A.G. Karydas, M. Kokkoris et al.,
Nucl. Instr. and Meth. B 179 (2001) 561-567.
‘Analysis of Ancient Glass using Ion Beams and Related Techniques’, S.
Kossionides, M. Kokkoris et al., Nucl. Instr. and Meth. B 195 (2002) 408-413.
‘Investigation of Deep Implanted Fluorine Channeling Profiles in Silicon
using Resonant NRA’, M. Kokkoris, R. Groetzschel et al., Nucl. Instr. and
Meth. B 201 (2003) 623-629.
‘Determination of Sulphur and Copper Depth Distribution in Patina Layers
Using NRA’, P. Misaelides et al., Nucl. Instr. and Meth. B 170 (2000) 467-473.
‘Proton Induced Thick Target γ-Ray Yields of Light Nuclei at the Energy
Region Ep=1.0-4.1 MeV’, T. Paradellis et al., Nucl. Instr. and Meth. B 152
(1999) 12-18.
‘Analysis of Copper Alloys by Proton Beams’, A.A. Katsanos, B. Katselis, A.
Aravantinos, Nucl. Instr. and Meth. B 15 (1986) 647-650.
5.
Relevant Works from our Team
PIGE Data and Applications (2/2):
8. ‘Cross-sections of the 32S(p,p’γ)32S nuclear reaction used for the determination of
sulfur on materials surfaces’, Ch. Tsartsarakos, P. Misaelides, A. Katsanos, Nucl. Instr.
Meth. B45 (1990) 33.
9. ‘Application of the 27Al(p,γ)28Si nuclear reaction to the characterization of the nearsurface layers of acid-treated HEU-type zeolite crystals’, P. Misaelides, A. Godelitsas,
F. Link, H. Baumann, Microporous Materials 6 (1996) 37.
10. ‘Aluminium diffusion in Al-implanted AISI 321 stainless steel using accelerator-based
characterization techniques’ Noli, P. Misaelides, K. Bethge: Nucl. Instr. and Meth. B139
(1998) 322.
11. ‘Investigation of fluorine distribution on the surface of acid-treated apatite single
crystals using nuclear resonant reaction analysis’, W. Theodossiu, P. Misaelides and A.
Godelitsas, Cryst. Res. Technol. 36 (2001) 1147-1151.
12. Determination of copper and sulphur distribution on chemically modified HEU-type
zeolite crystals by means of nuclear resonant reaction analysis techniques, scanning
electron microscopy and X-ray fluorescence’ A. Godelitsas, P. Misaelides, D. Charistos
and E. Pavlidou, Application of Particle and Laser Beams in Materials Technology, P.
Misaelides (Ed.), Kluwer Academic Publishers, Dordrecht, 1995, pp. 493-500.
13. ‘Investigation of natural prehnite using spectroscopic and accelerator-based
analytical techniques’ Α. Godelitsas, P. Misaelides, N.K. Moroz, R.S.W. Braithwaite, S.P.
Gabuda, A. Filippidis, K. Bethge, 6th V.M. Goldschmidt Conference, Heidelberg, 1996,
Journal of Conference Abstracts 1 (1), 205 (1996).
5.
Relevant Works from our Team
Other γ-Ray Measurements for Nuclear Astrophysics (1/2):
1. Cross section measurements of (p,γ) reactions on Pd isotopes relevant to the p
process Spyrou, A., Lagoyannis, A., Demetriou, P., Harissopulos, S., Becker, H.-W.
2008 Physical Review C - Nuclear Physics 77 (6), art. no. 065801
2. Cross-section measurements of capture reactions relevant to the p process using
a 4π γ-summing method Spyrou, A., Becker, H.-W., Lagoyannis, A., Harissopulos, S.,
Rolfs, C. 2007 Physical Review C - Nuclear Physics 76 (1), art. no. 015802
3. Alpha-capture reactions relevant to the p-process nucleosynthesis Spyrou, A.,
Lagoyannis, A., Zarkadas, Ch., Demetriou, P., Harissopulos, S., Becker, H.-W.,
Strieder, F., (...), Julin, R. 2006 AIP Conference Proceedings 831, pp. 314-318
4. Proton and alpha-particle capture reactions at sub-Coulomb energies relevant to
the p process Harissopulos, S., Lagoyannis, A., Spyrou, A., Zarkadas, Ch.,
Galanopoulos, S., Perdikakis, G., Becker, H.-W., (...), Demetriou, P. 2005 Journal of
Physics G: Nuclear and Particle Physics 31 (10), pp. S1417-S1420
5. Systematic measurements of proton- and alpha-capture cross sections relevant
to the modelling of the p process, Harissopulos, S., Spyrou, A., Lagoyannis, A.,
Zarkadas, Ch., Becker, H.-W., Rolfs, C., Strieder, F., (...), Goriely, S. 2005
Nuclear
Physics A 758 (1-4 SPEC. ISS.), pp. 505c-508c
6. Cross section measurements of the 89Y(p, γ)90Zr reaction at energies relevant to
p-process nucleosynthesis Tsagari, P., Kokkoris, M., Skreti, E., Karydas, A.G.,
Harissopulos, S., Paradellis, T., Demetriou, P. 2004 Physical Review C - Nuclear
Physics 70 (1), pp. 015802-1-015802-10
5.
Relevant Works from our Team
Other γ-Ray Measurements for Nuclear Astrophysics (2/2):
7. Proton induced reaction cross section measurements on Se isotopes for the astrophysical p
process Gyurky, Gy., Fulop, Zs., Somorjai, E., Kokkoris, M., Galanopoulos, S., Demetriou, P.,
Harissopulos, S., (...), Goriely, S. 2003 Physical Review C - Nuclear Physics 68 (5), pp. 5580315580319
8. Se(p-γ) cross section measurements for p-process studies Gyürky, G., Fülöp, Zs., Somorjai,
E., Elekes, Z., Kokkoris, M., Galanopulos, S., Demetriou, P., (...), Rauscher, T. 2003 Nuclear
Physics A 723 (1-2), pp.599c-601c
9. A systematic study of proton capture reactions in the Se-Sb region at energies relevant to
the p process Harissopulos, S., Galanopoulos, S., Demetriou, P., Spyrou, A., Kriembardis, G.,
Kokkoris, M., Karydas, A.G., (...), Goriely, S. 2003 Nuclear Physics A 719 (1-4), pp. 115c-118c
10. The 88Sr(p,γ)89Y reaction at astrophysically relevant energies Galanopoulos, S., Demetriou,
P., Kokkoris, M., Harissopulos, S., Kunz, R., Fey, M., Hammer, J.W., (...), Goriely, S. 2003
Physical Review C - Nuclear Physics 67 (1), pp. 158011-1580110
11. Proton capture cross section of Sr isotopes and their importance for nucleosynthesis of
proton-rich nuclides Gyürky, Gy., Somorjai, E., Fülöp, Zs., Harissopulos, S., Demetriou, P.,
Rauscher, T. 2001 Physical Review C -Nuclear Physics 64 (6), pp. 658031-658038
12. Cross section measurements of the 93Nb(p,γ)94Mo reaction at Ep=1.4-4.9 MeV relevant to
the nucleosynthetic p process Harissopulos, S., Skreti, E., Tsagari, P., Souliotis, G., Demetriou,
P., Paradellis, T., Hammer, J.W., (...), Rauscher, T. 2001 Physical Review C - Nuclear Physics 64
(5), pp. 558041-558049
5.
Relevant Works from our Team
Other γ-Ray Measurements for Nuclear Astrophysics
(but PIGE related):
1. The 27Al(p, γ)28Si reaction: Direct capture cross-section and resonance strengths at Ep =
0.2-1.12 MeV, Harissopulos, S., Chronidou, C., Spyrou, K., Paradellis, T., Rolfs, C., Schulte,
W.H., Becker, H.W. 2000 European Physical Journal A 9 (4), pp. 479-489.
2. Cross section and resonance strength measurements of 19F(p,αγ)16O at Ep = 200-800
keV Spyrou, K., Chronidou, C., Harissopulos, S., Kossionides, S., Paradellis, T., Rolfs, C.,
Schulte, W.H., Borucki, L. 2000 European Physical Journal A 7 (1), pp. 79-85.
3. Resonance strength measurements of the 27Al(p,γ)28Si reaction in the energy range Ep =
0.8 - 2.0 MeV Chronidou, C., Spyrou, K., Harissopulos, S., Kossionides, S., Paradellis, T.
1999 European Physical Journal A 6 (3), pp. 303-308.
4. A compilation of charged-particle induced thermonuclear reaction rates Angulo, C.,
Arnould, M., Rayet, M., Descouvemont, P., Baye, D., Leclercq-Willain, C., Coc, A., (...),
Lamehi Rachti, M. 1999 Nuclear Physics A 656 (1), pp. 3-183.
(2006 – today)
6.
Experimental Capabilities – Tandem Accelerator
 4 HPGe Detectors, ~100% relative efficiency for 6 months/year
in the framework of the LIBRA project (from Stuttgart’s
Dynamitron): 3 could be set at 55o, 125o and 90o for PIGE
measurements, but there also exist 4 portable HPGe detectors (rel.
eff. 80%, 50%, 45%, 18%)
7.
Future Measurements and Perspectives
Data and Software:
1. The situation seems to be quite complicated. In my opinion, no new data library is
needed, EXFOR or IBANDL (even better) are adequate. A new CRP is absolutely
necessary to stimulate and organize the field and it should be mainly concentrated on
data needs / new measurements.
2. The CRP should accept realities and concentrate on r-PIGE or PIGE in general, but
setting an upper limit in Z (e.g. 20-25 at the most).
3. The new measurements should follow certain guidelines in order to be useful for the
scientific community (cross sections, differential or total, thin targets, analogous
situation as in the recent CRP for IBA)
4. The final outcome of the CRP should be a complete ‘guide’ for PIGE users, for the
profiling of all the light elements and a big review article should be produced, in parallel
of the other IAEA requirements.
5. In this aspect, we would like to contribute e.g. in the cases of 9Be(p,γ), 13C(p,γ) and
32S(p,p’) [resonant – non-resonant parts] or according to the recommendations of the
other members of the present meeting.
6. All new datasets will be of limited use, unless the software situation concerning light
element profiling utilizing PIGE cross sections is also addressed in this forthcoming CRP.
A recommended code should be made available to the scientific community and
supported by benchmarking experiments (round-robin?).
7. The theoretical /evaluation part should also be addressed.