ANSTO Accelerator Capabilities for Materials Characterisation - - PowerPoint PPT Presentation

ANSTO Accelerator Capabilities for Materials Characterisation

Mihail Ionescu, Rainer Siegele, David Cohen

Mihail.Ionescu@ansto.gov.au

IAEA Vienna 15-19 Sept 2008

Outline:

• ANSTO’s Ion Beam Accelerators
• Examples from ANSTO’s research

projects on the use of accelerators for characterization of materials

ANSTO’s Ion Beam Accelerators

ANTARES (Australian National Tandem for Applied Research).

• Opened in September 1991.
• 10 MV heavy ion machine (HVEE) with 3 ion sources and 5 high energy

beamlines (2 IBA and 3 AMS).

• Can accelerate most ions in the periodic table (H- U)

STAR (Small Tandem for Applied Research).

• Opened in January 2005.
• 2 MV heavy ion machine (HVEE) with 3 ion sources and 3 high energy

beamlines (2 IBA and 1 AMS 14C).

• Can accelerate (H, He, C)

Ion Beam Accelerators Usage

• To provide accelerator based expertise for:
• internally and externally driven research with

Australian Universities, CSIRO, Local and State Governments, industry and international organisations including the International Atomic Energy Agency (IAEA)

• training for local and international researchers,

workshops, fellowships etc for developing countries in our region

• Main techniques include:
• Ion Beam Analysis (IBA): PIXE, PIGE, RBS, ERDA,

RToF, NRA and Heavy ion µ-probe (X-ray mapping; lithography; IBIC)

• Accelerator Mass Spectrometry (AMS) – 14C, 10Be, 26Al,

129I, Actinides

ANTARES

ANTARES 10 MV Tandem

HVEE 846 multi sample 860 single NEC alphatross Microprobe IBA-ToF AMS: C, Be, Al AMS: Actinides 10m

• Microprobe: µ-PIXE; µ-RBS
• ToF: Heavy ion ERDA; RBS; ion implantation
• AMS: 14C, 10Be, 26Al, 129I, Actinides

5m

STAR

• SIBA1: Automated PIXE; PIGE; RBS; PESA
• SIBA2: He-ERDA; Variable angle RBS; NRA
• AMS (14C) dating

358 Ion Source 846B Ion Source

2MV HVEE Tandetron Accelerator

AMS 14C IBA Beam line 1 IBA Beam line 2 Ionisation chamber Recombinator

IBA Materials Projects at ANSTO

• Elemental analysis (PIXE, PIGE)
• Characterization of thin films near-surface layers and interfaces:
• thickness (RBS, NRA, variable angle RBS)
• depth profile of elements (RBS, NRA, ERDA)
• defects (variable angle RBS-channelling)
• 2D mapping (µ-PIXE; µ-RBS)
• Modification of thin films, near-surface layers and interfaces:
• ion implantation (conductive polymers; ZnO/STO; other)
• Device testing (IBIC, single event upset)

Can do:

• Materials testing for radiation damage
• Micro-machining
• Ion beam induced chemical reactions

PIXE, PIGE: Aerosols in Asia PIXE, PIGE: Aerosols in Asia

Cheju Is. Sado Is.

D us t S

Hong Kong Hanoi Manila

• Large throughput of samples
• PMF→Source identification
• Events correlation (back trajectories)
• Large database

Lead vs Bromine Mascot 1992-2000

200 400 600 800 1000 1200 100 200 300 400 500 Br (ng/m3) Pb (ng/m3) Pb=(2.12±0.30)*Br +(27±29) R2=0.98

Mascot 1992-2000

100 200 300 400 500 600 700 800 900 1000 D e c

• 9

D e c

• 9

1 D e c

• 9

2 D e c

• 9

3 D e c

• 9

4 D e c

• 9

5 D e c

• 9

6 D e c

• 9

7 D e c

• 9

8 D e c

• 9

9 D e c

• Lead (ng/m

3)

PIXE, PIGE: Study of Archaeological Artefacts [1]

• Non destructive
• Large throughput
• PMF→Source identification
• Ancient trade routs identified

[1] T. Doelman, R. Torrence, V. Popov, M. Ionescu, N. Kluyev, I. Sleptsov, I. Pantyukhina, P. White and M. Clements, Geoarchaeology 23, 234, (2008)

PIXE Bremsstrahlung [1]

[1] D. D. Cohen, E. Stelcer, R. Siegele, M. Ionescu, M. Prior, NIM B 266, 1149-1153, (2008) [2] K. Murozono, K. Ishii, H. Yamazaki, S. Matsuyama, S. Iwasaki, NIM B 150, 76, (1999)

• Important for quantitative analysis
• Theoretical background calculated for 3MeV protons on C[2]

Be 1843 µg/cm2 C 1767 µg/cm2

• Data corrected for self absorption; detector efficiency;

γ-ray background component and normalised to unit charge (µC), unit solid angle (Sr) and unit target thickness (µg/cm2)

• Normalised yield (Yld) was fitted to a 9-th order polynomial

ln(Yld)=a0+a1ln Ex+a2 (ln Ex)2+…+a9(lnEx)9

Heavy Ion Microprobe Heavy Ion Microprobe

• Spot sizes of 1-10µm
• 1-10 nA target current
• Focussing of ions with Me/q2 = 100 (H to U)
• 2D mapping
• Applications:

2D mapping (µ-PIXE, µ-RBS) Nuclear reactions Resonances Heavy Ion Elastic Recoil Detection IBIC Ion Beam Lithography

Au 50 x 50 µm Cr

1-2 µm spot size at 100 pA; 3MeV H

Elemental Mapping using the Ion Microprobe Elemental Mapping using the Ion Microprobe

PIXE Spectrum of Aerosol Filter

Exposed Filter Unexposed Filter

soil cars sea spray FeS ores

50µm

K Ca Ni

Characterization of Characterization of Microdosimeters Microdosimeters by IBIC by IBIC [1]

[1]

Charge collection maps of 20 MeV C4+ beams on Silicon on Insulator (SOI) micro-dosimeters

K

[1] I. M. Cornelius, R. Siegele, I. Orlic, A. B. Rosenfeld, D. D. Cohen, NIM B 210, 191, (2003)

Single Ion irradiation [1]

• Damage in tracks depend on LET
• Diameter of a damage track is

~10nm

• Used in single ion implant and high

resolution IB lithography

Low Medium High

PMMA Si

Ion E

(MeV)

LET elect

(eV/nm)

LET nucl

(eV/nm)

H 2 15 <0.1 MARC He 2 150 0.1 MARC C 30 44 0.3 ANSTO C 9 760 0.8 ANSTO F 8 1380 2.8 ANSTO Cu 6 1460 77 ANSTO

AFM

100nm

F damage tracks

[1] A. Alves, P. Reichart, R. Siegele, P. N. Johnston, D. N. Jamieson, NIM B 249, 730, (2006)

Ni Uptake in Plants [1]

Ca

100 µm Leaf cross-section scan :

• current 0.8 nA
• spot size 3 µm
• count rate 2 kHz
• Study of Hybantus Floribundus- a Ni hyperaccumulator
• Thin sections (~10 µm) freeze substitution
• Localization of Ni in various parts of the plant

Ni

100 µm

50 µm

K

[1] R. Siegele, A. G. Kachenko, N. P. Bhatia, Y. D. Wang, M. Ionescu, B. Singh,

• A. J. M. Baker, D. D. Cohen, X-ray Spectrometry 37, 133, (2008)

RBS: multi-layer MgB2/Mg2Si/Al2O3 [1]

50 100 150 200 250 300 0.0 5.0x10

1.0x10

1.5x10

2.0x10

75

• 8x 15 nm Mg2Si

9x 80 nm MgB2

Yield [cts/2µC] Channel No

experimental simulated B O Mg Al Si

2MeV He

1+

15

• C-Al2O3
• Role of Mg2Si layers in increasing the pinning
• comparison with single MgB2 film
• Increase in activation energy U0
• Increase in anisotropy of U0

[1] Y. Zhao, M. Ionescu, P. Munroe, S. X. Dou, APL 88, 012502, (2006)

RBS: channelling in Si

200 400 600 800 1000 1200 1400 1000 2000 3000 4000 5000

RBS yield [cts/200µC] Energy [keV]

(101) (111)

C

Surface Surface (101) 1MeV He

+

Detector 1MeV He

+

Detector (111)

• Study of Al-Ti-C MAX phase [1]
• Part of C diffused in Si (001) substrate
• A buried layer of C by channelling of 2MeV He+ in Si
• Substrate replaced by MgO

[1] J. Rosen, P. O. A. Persson, M. Ionescu, A. Kondyurin, D. R. McKenzie, M. M. M. Bilek, APL 92, 064102, (2008)

50 100 150 200 250 300 350 100 200 300 400 500 600 700 C Mg Nd Exp Simul C O Mg Al Ti Nd

Yield [cts/1.2µC Channel No

Ti Al O in MgO

HeERDA-SBD: Hydrogen in SiNx thin film [1]

recoiled (H) ) (

2 2

E E E E

foil d

∆ − = dx dE x E E

x x 1 1 2

cosβ − =       − = dx dE x E k E

cosα

) (

1 1

E E E E

foil d

∆ − =

E0x

At depth x:

2 2 1 2 2 1 1

) ( cos 4 M M M M E E + = θ θ σ cos 4 )] ( [

M E M M e Z Z d d + = Ω Ω Ω = d d N cts Y cm at N

σ α cos ] [ ] / [

Ed E2 E0 E1x M1 (He) M2 (H)

α β θ

E1 x

scattered (He) recoiled (He)

At the surface:

Filter Energy Detector

N- number of ions incident on sample surface

Ω - detector solid angle σ - scattering cross section

200 400 600 800 1000 10 20 30 40 50 60

H Yield [counts] Energy [keV]

Si Wafer thin SiN thick SiN

He H Si SiNx:H Surface H

• Passivating role of Hydrogen in thin

SiNx films

• Depth of analysis: up to few 100nm
• Depth resolution: few nm
• Sensitivity: ~0.1 at%

200 400 600 800 1000 5 10 15 20 25

Depth [x10

15 at/cm 2]

Si

5 10 15 20 25

Hydrogen [x10

15 H/cm 2]

SiN20

5 10 15 20 25

SiN70

[1] M. Ionescu, B. Richards, K. McIntosh, R. Siegele, E. Stelcer, O Hawas, D. D. Cohen, T. Chandra, Materials Science Forum Vols. 539-543, pp. 3551-3556, (2007)

ANSTO Heavy Ion ERDA-ToF [1]

T2

Secondary Electron

MCP W electrodes C foils

Recoils

0.5m

Electrostatic Mirrors

SBD 45

• 4-way slits

Ion Beam

67.5

• Secondary

electron

Anode plate

Energy Time

T1 25 50 75 100 125 150 175 200 225 250 275 300 325 17 18 19 20 21 22 23 24

Depth resolution [nm] C foil thickness [µg/cm

2]

82.5 MeV Iodine

• Ion beams: C; O; F; Na; Si; Cl; Ca; Ti;

Co; Ni; Cu; Br; Nb; Ag, I; W; Pt; Au

• Beam shape: rectangular
• Incident angle: 67.5o
• Exit angle: 45o
• Scattering angle: 45o
• C foils: 25µg/cm2
• Sample manipulation: XYZ, rotation
• Sample heating up to 1,000oC
• Gas ports (O, N)
• Further development:
• H absorption/desorption
• In-line sample preparation: ion implanter + EB

evaporator

TRIG

(86) QD (821) CH3 CH1 CH0 (94)

STOP START (T)

(93)

(E)

Sample CFD Delay CFD PA FPA FPA e

• e
• T2

TOF-ERDA Diagram

Ion Beam Recoils T1 SBD

PC (571) AMP (474) TFA (463) CFD (89) NIM-TTL (567) TAC (419) MCA

[1] J. W. Martin, D. D. Cohen, N. Dytlewski, D. B. Garton, H. J. Whitlow,

• G. J. Russell, NIM B 94, 277, (1994)

ERDA-ToF: analysis of MgB2 thin film with 82MeV I [1]

400 800 1200 1600 2000 2400 2800 3200 3600 4000 400 800 1200 1600 2000 2400 2800 3200 3600 4000

Time [channel no] Energy [channel no]

O Mg Al

82MeV I

Al2O3 MgB2

112.5

• 50

100 150 200 250 500 1000 1500 2000 2500 3000 3500 4000 4500 5000

Substrate

10B 11B

O Mg Al

Yield [counts] Depth [nm]

Film

16 18 20 22 24 26 28 30 32 34 36 38

• 0.2

0.0 0.2 0.4 0.6 0.8 1.0 1.2 3 7 8 6 5 4 2

On axis-Si On axis-Al2O3 Off axis; Mg cap layer Off axis; ion beam sputtered

Normalized Oxygen in MgB2 film Tc [K]

1

• Isotope effect in MgB2 can be measured as

a function of 10B/11B

• Magnesium is diffusing into the substrate
• Oxygen amount critical for the quality of the film
• Tc correlated with the amount of Oxygen, type of

substrate, and deposition geometry

[1] M. Ionescu, Y. Zhao, R. Siegele, D. D. Cohen, E. Stelcer, M. Prior, NIM B 266, 1701–1704, (2008)

NRA: Oxygen in Ta2(16O1-x+18Ox)5 thin film [1]

25 50 75 100 125 150 175 200 100 200 300 400 500 600 700 800 900 1000

α yield [counts]

Channel Number 0.2 0.6 1 1.6 1.8 2.1 2.5 4

18O concentrations [at%]

0.0 0.5 1.0 1.5 2.0 2.5 3.0 3.5 4.0 4.5 5.0 0.0 2.0x10

4.0x10

6.0x10

8.0x10

1.0x10

1.2x10

1.4x10

1.6x10

1.8x10

2.0x10

2.2x10

Standard samples Liniar Fit

α yield [counts]

18O concentration [at%]

y=4577 x+148 R=0.99964

α

Ta2(

16O1-x 18Ox)5

p 845keV

18O(p,α) 15N

200nm Ta

500 600 700 800 900 1000 10 20 30 40 50 60 70

dσ/dΩ [mb/sr] Energy [keV]

18O(p,α) 15N

845 keV 641 keV

[1] M. Ionescu, D. Bradshaw, R. Siegele, D. D. Cohen, O. Hawas, E. Stelcer, D. Button,

• D. Garton, NTA 14 Conference, 20-22 November 2005, Wellington, New Zealand

NRA: Hydrogen in thick DLC film

Γ = σ π

i

N dx dE cts Y cm at N ] [ 2 ] / [

2

σ Ω =

i

N cts Y cm at N ] [ ] / [

2

E4 E3 E2x

γ dx dE x E E x cosα − =

1H( 15N,αγ) 12C

dx dE x E E

x x 1 1 2

cos β − =

E0x

At depth x:

E2 E0≥ 6.385 MeV E1x

15N

α β θ

E1 x

At the surface:

Energy Detectors

Ni - number of ions incident on sample

Ω − detector solid angle σ −

15N reaction cross section

Γ − FWHM of resonance (1.8keV)

4He 1H 12C

γ

E1= 4.43 MeV

• Depth of analysis: few nm up to few

microns

• Depth resolution: 5-20nm
• Sensitivity: 1-100ppm

5.5 6.0 6.5 7.0 7.5 8.0 8.5 9.0 9.5 1 10 100 1000 10000

Si

γ Yield [counts/2.5µC]

Energy

15N + ions [MeV] 15N +

γ Detector

Si

DLC film ~700nm

• Thick DLC film grown by CVD for implants
• Hydrogen content plays a role in the biologic

response [1]

• Hydrogen content is higher at the surface and

decreases toward the interface

• Questions remains on Hydrogen yield due to

the production of 15N- (15NH3

• ), the flux

measurement, energy spread, etc

[1] W. J. Ma, A. J. Ruys, R. S. Mason, P. J. Martin, A. Bendavid,

• Z. Liu, M. Ionescu, H. Zreiqat, Biomaterials 28, 1620–1628, (2007)

Ion beam implantation and mixing

nanostructures depth

Ion implantation

burried layer supersaturation nucleation growth ripening coalescence

time

annealing

surface nanostructures interface

Ion irradiation

time

annealing

surface interface mixing phase separation

• Near surface layers and interfaces

can be engineered for specific properties

10K

Zn0.99Co0.01O Zn0.99Co0.005Eu0.005O Zn0.99Eu0.01O

10

3

2x10

3

• 10

3

• 2x10

3

B [Oe] Magnetization [amu]

2x10

• 4

10

• 4
• 10
• 4
• 2x10
• 4
• ZnO thin film implanted with Eu and Co
• Annealed
• Magnetization measured at 300K and

10K

Conclusions

• IBA nuclear techniques at ANSTO suitable for characterisation of thin

films, near surface layers and interfaces

• film thickness
• depth profile of light and heavy elements
• defects in single crystals
• 2D X-ray mapping of surfaces
• radiation damage in materials
• ion beam-induced chemical reactions
• micro-machining
• Modification of properties by ion implant
• Micro device testing (IBIC, single event upset)

Acknowledgment:

• D. Garton, G. Cooke; O. Evans; M. Mann; D. Lynch; E. Stelcer; P. Bond; P. Druer