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 onReference 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 GroupLaboratory of Ion Beam Applications

RESEARCH PERSONNELparticipating in the IAEA PIGE CRP

László CsedrekiGyörgy GyürkyGusztáv Áron SzikiZita SzikszaiImre Uzonyi

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

SECTION OF ION BEAM PHYSICSInstrumentation

ATOMKI Laboratory of Ion Beam Applications, Debrecen

macro-PIXE

Nuclear microprobe

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

Applications:: Geology Archaeology Materials science Characterisation of single aerosol

particles Micro-machining

(STIM = scanning transmission ion microscopy)

Beamline for gamma spectroscopy (VDG-5 J30o)

Applications: Nuclear astrophysics p-PIGE, d-PIGE

Turntable for 2 Ge detectors 5 cm thick lead shielding

Gamma and X-ray detectorsHPGe 40% (ORTEC), HPGe 20%(CANBERRA), Clover 120%, NaI(Tl)

X-ray detectorsSi(Li) and SUTW Si(Li)

Leybold UINIVEX 350 vacuum coating system

Laboratory for sample preparation

Zeiss Axio Imager Optical Microscopewith CCD digital camera

FROM GAMMA-SPECTROSCOPY to PIGE in ATOMKIExamples 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.

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.

FROM GAMMA-SPECTROSCOPY to PIGE in ATOMKI Examples II.

Not for direct use in PIGEbut experience gained useful also for PIGE

Proton capture cross section of Sr isotopes and their importance for nucleosynthesisof proton-rich nuclidesGy. Gyürky, E. Somorjai, Zs. Fülöp, S. Harissopulos and P. Demetriou, T. Rauscher, Phys.Rev. C64 (2001) 065803

Extension of the work done in Helsinki

Ep: 1.7, 2.4, 3.1, 3.8, 4.2 MeVElements: Li – Sc (except Ne, Ar)

Thick target gamma-yields for p-PIGE

THE PIGE TECHNIQUE AT ATOMKIearlier results

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)

G. A. Sziki, A. Simon, Z. Szikszai, Zs. Kertész, E. Dobos, Nucl. Instr.Meth. B 251 (2006) 343

Gamma ray production cross-sections for d-PIGE

Reactions and most dominant -lines

6Li(d,p)7Li, 478 keV (Li)9Be(d,n)10B, 718 keV (Be) 11B(d,p)12B, 953 keV (B)

1674 keV (B) 16O(d,p)17O 871 keV (O) 19F(d,p)20F 656 keV (F)

D e u te ro n e n e rg y [k e V ]

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C o n t ro l m e a s u re m e n ts

C o n t ro l m e a s u re m e n ts

T a r g e t : L iF

T a r g e t : B e

T a r g e t : L iB O 2

T a r g e t : t i t a n iu m - o x id e

T a r g e t : L iF

E = 6 5 6 k e V

E = 8 7 1 k e VE = 9 5 3 k e V

E = 1 6 7 4 k e V

E = 4 7 8 k e V

E = 7 1 8 k e V

9 B e ( d ,n ) 1 0 B

1 6 O ( d ,p ) 1 7 O

6 L i( d ,p ) 7 L i

1 1 B ( d ,p ) 1 2 B

1 9 F ( d ,p ) 2 0 F

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T a r g e t : L iF

T a r g e t : B e

T a r g e t : L iB O 2

T a r g e t : t i t a n iu m - o x id e

T a r g e t : L iF

E = 6 5 6 k e V

E = 8 7 1 k e VE = 9 5 3 k e V

E = 1 6 7 4 k e V

E = 4 7 8 k e V

E = 7 1 8 k e V

9 B e ( d ,n ) 1 0 B

1 6 O ( d ,p ) 1 7 O

6 L i( d ,p ) 7 L i

1 1 B ( d ,p ) 1 2 B

1 9 F ( d ,p ) 2 0 F

Thin samples: ~ 10-70 ug/cm2

Vacuum evaporation orDC reactive magnetron sputteringThin film RBS analysis

Standards:LiBO2, LiF, LiNO3, BN, NH4BF4, BeO, CaF2

Deuteron energy: 0.6-2 MeVEnergy steps: 20-50 keV

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, 11015 at.cm-2 100 keV, 11015 at.cm-2

Eres = 872 keV

Ibeam = 9 nA

Dbeamspot = 1 mm

Detector: 10 cm 10 cm NaI(Tl)Ddet-sample: 1cm=0

Experimental conditions:

Overall view of the 19F(p,)16O excitation curve at =90°, normalized to a 3.8 g/cm2 F target, 60 C per point; 3”3” NaI(Tl) detector at 7 cm; detected E>4.7 MeV. [D. Dieumegard, B. Maurel, G Amsel, NIM 168 (1980) 93.

Overall view of the 19F(p,)16O excitation curve at =90°, normalized to a 3.8 g/cm2 F target, 60 C per point; 3”3” NaI(Tl) detector at 7 cm; detected E>4.7 MeV. [D. Dieumegard, B. Maurel, G Amsel, NIM 168 (1980) 93.

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

Effect of various factors (experimental, matrix, etc.) influencing analytical accuracy of PIGE data.

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:

Study of obsidian glasses

The aim of the work: to find sub-groups among the classified obsidian sources of the volcanic Tokaj Mountains (NE Hungary-E

Slovakia).

PIGE: 3.5 MeV proton energy, PIXE: 2.0 MeV

Improvenments in detection technique:Clover-BGO detector system

Application of PIGE in archaeometry(examples)

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-pastecan 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 decorativetype 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-PIXEC to Fe detected simultaneously by UTW and Be-W Si(Li)

micro-d-PIGE for N determination

obtained in the frame of FP7 project CHARISMA

Incrusted pottery (Bükk culture)

Determination of fluorine contentIn the incrustationMicro-PIXE/PIGE simultaneously

Archaeological glass sealsproduced from ca. 1750-1850.(Finnish Glass Museum)All elements above C measured by PIXE

Monitoring the presence of boronPIXE/PIGE simultaneously

Recent results

Thank you for your attention!