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NSUF Annual Review

Increasing instrumentation capability for irradiated nuclear material characterization at Idaho National Laboratory

Fidelma Giulia Di Lemma, Ph.D.Instrument & Metallurgy scientist

PIE & Advanced Characterization DepartmentP.O. Box 1625, MS 6157 Idaho Falls, ID 83415

(208)-533-8005 FidelmaGiulia.DiLemma@inl.gov

from 11/2016,Instrument scientist and metallurgy

2012-2015Ph.D. in applied Sciences

4/2015-10/2016Postdoc on FP and structural material behavior during SA

2006-2011B.Sc.+M.Sc.Nuclear Engineering

1987 Born

2011-2015Intern and grant-holder on aerosol behavior from RDD and SA

Understanding materials

behavior in extreme

conditions

Thermodinamicscalculations

(ThermoCalc, Factsage)

ICP-MS

TG-DTA

Knudsen Cell

X-Ray and Rietveld analyses

+Raman

Spectroscopy

SEM/EDX

+

WDX/EBSD

NSUF ProjectIncreasing instrumentation

capability for irradiated nuclear material characterization

EPMA (Electron Probe MicroAnalysis) Capabilities

EBSD (Electron BackScatterDiffraction) analyses on reactive

irradiated metals

Metallurgy and instrument scientist

1) EBSD characterization

EBSD (Electron BackScatter Diffraction) is an analytic technique to evaluate the microstructure of a specimen.

Grain size,

Grain shape,

Grain distribution,

Grain boundary,

Grain orientation,

Deformation and stresses,

Phases determination and inclusions (carbides and precipitates).

The quality of the information dependent upon absolute removal of all surface defects on the sample due to mechanical preparation steps.*

*Unfortunately there is no single technique that works with all materials, and an experimental approach is often required to achieve a suitable result.

NSUF Task

Goal:

to develop a reliable sample preparation technique for EBSD analyses for reactive metals and especially highly radioactive samples (irradiated/fuel).

Challenges:

Samples are prone to rapid oxidation*, which can influence the EBSD results.

Samples are radioactive and thus must handle following specific safety procedure.

Part 1Analysis of current

techniques and results obtained

Part 2 Proposal of

alternative solution

Part 3Testing of proposed

techniques on various sample

Part 4Develop of a method and

report/publication

*EBSD patterns are generated within a depth of less than 50-100 nm. Because of this, the data quality is extremely sensitive to the integrity of the crystallographic lattice order at the surface of the sample and to oxidation.

Available techniques in MFCTechnique Pros Contras

1. Mechanical polish (down to 0.05 µm)

Large areas, Available expertise,Multiple samples, Fast (half day ).

Performed in air,Needs a final finishing

2. Vibratory polish Large areas, Available expertise, Multiple samples, alkaline effect

Performed in air, Long (overnight/multiple days).

3. Jet polishLarge areas, Available expertise, Fast

(minutes).Performed in air.

4. EtchLarge areas, Available expertise,

Fast (seconds/minutes)Performed in air, Multiplephases different finishing.

5. FIB/P-FIB(Focused Ion Beam / Plasma Focused Ion Beam)

Good finishing, connected with EBSD, in high vacuum.

Long (hours), small areas.

6. PIPS(Precision Ion Polishing System)

Small areas, Available expertise,Fast (minutes).

Works with small samples.

7. PECS(Precision broad argon Ion Polishing System)

Good results obtained in the past, Available expertise,

Fast (minutes).

Risk of spreading contaminations.

Possible improvements

Current method Improvements I Improvements 2

1. Mechanical polish 1. Mechanical polish 1. Mechanical polish

2. Vibratory/Jet polish 2. PIPS/PECS 2. Vibratory Polishing

3. FIB/PFIB 3. Transfer tight chamber or specific sample holder or protective layer (coating/spray)

3. Transfer tight chamber or specific sample holder or protective layer (coating/spray)

Current limitations:Long time, Limited FIBs, Oxidation

4. FIB/PFIB on small area of interest

4. FIB/PFIB on small area of interest

Why PECS?

• Residual oxidation or hydrocarbon contamination is minimal.Lattice damage is on the nanoscale.

• To avoid alteration/contamination* following ion milling, the sample should be transferred to the SEM (Scanning Electron Microscope) immediately.

- Current available machine can be attached directly to SEM chamber.- Current available machine can coat/apply a protective layer directly the sample in PECS.- A transfer chamber could be developed to interface different available instruments.

* Such as dust or dirt on the surface, scratching, formation of oxide layers, moisture.

Possible plan of action

1. Sample prep with improved

methods

2. EBSD analyses

3. Compare with previous method

Successful?

New sample

YES

Steel

Al/Zr

U*

Irr. steel

Irr. fuel

Sample to test

Method

Implement new techniques

*Collaboration with Dr. D. Murray

NO

Example benchmarkStainless steel

2) EPMA• In the EPMA (Electron Probe MicroAnalysis) we bombard a micro-volume

of a sample with a focused electron beam and collect the X-rays emitted.

• WDS (Wavelength Dispersive Spectroscopy) is use to identify the X-rays,and quantify the element present in the sample.

• EPMA is a fully qualitative and quantitative method of non-destructiveelemental analysis of micron-sized volumes at the surface of materials,with sensitivity at the level of ppm.

• EPMA allow simultaneous collection X-ray, SEM, BSE (Back ScatterElectrons) and optical images.

Advantages

• WDS cannot determineelements below 5 (boron).

• X-rays peaks can overlap andmust be then separated.

• Time consuming.

• Need of accurate standards.

• Need of a complex correctionmatrix.

• Analyses of light elements.

• Quantitative analyses down toppm (High Sensitivity).

• WDS as a better spectralresolution (vs EDS - EnergyDispersive x-ray Spectroscopy).

• WDS better dead time thanEDS.

• Reliable and repeatablemeasurements.

Limitations

NSUF Task

Goal:

to develop human workforce in operating the EPMA in the INL MFC (Material Fuel Complex) for nuclear and irradiated materials, to support the current instrument scientist.

Part 1Literature

review on the instrument and

analyses

Part 2Training on instrument

Part 3Training on data

analyses

Part 4Perform analyses

independently

Beam Set up

Instrument conditions and

navigation

Imaging

Peak calibration

Map acquisition

Map Processing

Project Part IIChoice of KV

Filament saturation

Aperture

Beam stability

Instrument Menu operation

Stage movement

Sample and Standard position

Focusing/Astigmatism

Acquisition

Storage

Diffuse vs focused beamCondition for standards

Background selection (from PFE Probe for EPMA)

Acquisition and peak setting

Overlap correction

AutomatizationPeak setting

Beam and optical setting

Mosaic setting

Save method

AutomatizationMosaic Assemblage

Overlap correction

Quantification

Saving

ExampleIrradiated metallic fuel

SampleFUTURIX-FTA-DOE1

CompositionU-29Pu-4Am-

2Np-30Zr

Irradiation 2.08 x 1021 f/cm3

(9.5% burnup)

Probe softwareSet up

Standards

Set up

New sample

Set up

ProcessingData

Project Part II TBP

Conclusion

Increasing instrumentation capability for irradiated nuclear

material characterization

EPMA CapabilitiesEBSD analyses on reactive

irradiated metals

Metallurgy and instrument scientist

Acknowledgment

This work was supported by the U.S. Department of Energy, Office of Nuclear Energy.

Thanks go to

• Dr. Rory Kennedy for his support and participation in the development of this project

• Dr. Mitch Meyer for his support on these projects.

• Karen Wright, Brandon Herrandez, Tammy Townbridge, Jason Harp for their technical advice, support in data collection and elaboration.

Reference• E.A. Fischione Instruments, Application Note “Metallic sample preparation for EBSD by

mechanical method and argon ion beam milling” AN012 Revision 01 04/2014

• Streurs, Application Notes “Preparation of ferrous metals for Electron Backscatter Diffraction (EBSD) analysis” 02.2010 / 62140410

• M.M. Nowell, R.A. Witt, and B.W. True “EBSD Sample Preparation: Techniques, Tips, and Tricks”, Microscopy today, p. 44-48 July 2005

• Oxford Instrument Application note “EBSD Sample preparation”

• S. Suwas, and R.K. Ray “Crystallography Texture of Materials” 2014, XIII, p. 260.

• Thermoscientific “Wavelength dispersive (X-ray) Spectroscopy” Essential Knowledge Brifieng, 2016.

• CAMECA_SXFiveFE_2_page_flyer.pdf

• https://www.bruker.com/fileadmin/user_upload/8-PDF-Docs/X-rayDiffraction_ElementalAnalysis/XRF/Webinars/Bruker_AXS_EDX_vs_WDX_Webinar_Slides.pdf

• https://www.ems.psu.edu/~ryba/harbin/EPMA.ppt.pdf

• http://etd.library.vanderbilt.edu/available/etd-07192013-160603/unrestricted/Hammonds.pdf

• http://tech.snmjournals.org/content/32/3/139/F4.expansion.html

• https://www.jeolusa.com/RESOURCES/Electron-Optics/Documents-Downloads?EntryId=5

• http://www.ebsd.com/

WDX

Detector RangeK line

RangeL line

RangeM line

TAP F(9)-P(15) Mn(25)-Y(39) La(57)-Ir(77)

PET Si(14)-Cr(24) Sr(38)-Eu(63) W(74)-Pu(94)

LiF Sc(21)-Br(35) Te(52) to Bi(83) N.A.