![Page 1: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/1.jpg)
In Cooperation with our University Partners
Radiochemistry Webinars
Nuclear Materials Analysis: Physical
Methods of Characterization
![Page 2: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/2.jpg)
Meet the Presenter… Dr. Jeff Terry
Contact Information: [email protected]
Dr. Jeff Terry is a professor of physics at the Illinois Institute of Technology, where his main research focus is on energy systems. His group works to develop new ways of dealing with radioactive waste, understand radiation damage mechanisms in materials, and synthesize novel materials for energy storage and conversion. He also simulates the economic costs of building new energy systems, including small modular nuclear reactors. Prior to joining the faculty at Illinois Tech, he was a staff scientist at Los Alamos National Laboratory (LANL). There, he worked on the Stockpile Stewardship
2
and Management Program and the Waste Isolation Pilot Plant (WIPP) and was a member of the LANL team that sent the first waste shipment to WIPP. He is a former scientific director of the Advanced Test Reactor National Scientific User Facility. Dr. Terry is very active in science communication. He writes a regular column for the Bulletin of the Atomic Scientists and is an editor for the journal Applied Surface Science. Dr. Terry earned his doctorate in chemical physics from Stanford University in 1997 and his bachelor’s degree in chemistry from the University of Chicago in 1990.
![Page 3: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/3.jpg)
Physical Methods of
Characterization of Advanced
Nuclear Materials
Dr. Jeff Terry Illinois Institute of Technology
National Analytical Management Program (NAMP)
U.S. Department of Energy Carlsbad Field Office
TRAINING AND EDUCATION SUBCOMMITTEE
![Page 4: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/4.jpg)
Nuclear Materials Science • PWR Sustainability
–Average age of 439 operating nuclear reactors is 24 years
–Average age of 119 shutdown reactors 22 years
–The Bulletin of the Atomic Scientists 2008 Status Report
• Push Lifetime To 40, 60, 90 Years
–Aging
–Stress
–Corrosion
–Fatigue
–Irradiation effects
4
![Page 5: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/5.jpg)
Nuclear Materials Science • Beyond design basis
–High temperature
–Fuel cladding reactions
–Hydrogen generation
5
![Page 6: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/6.jpg)
Nuclear Materials Science • Gen IV
–Reactor design
–Materials issues
–Corrosion
–Neutronics
–High temperature
• Fuel
–Corrosion
–Pellet cladding interaction
–Fission gas release and swelling
–Hydrogen induced embrittlement of cladding alloys
6
![Page 7: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/7.jpg)
Nuclear Materials Science • Nuclear Waste
–Fate
–Transport
–Geochemistry
–Biochemistry
–Repository Science
• Fundamental Science
–5f Electron Behavior
–Highly correlated electrons
–5f Chemistry
7
![Page 8: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/8.jpg)
Techniques • Electronic Structure
–Photoelectron Spectroscopy –X-ray Absorption Near Edge Spectroscopy –Tunneling Spectroscopy –X-ray Emission Spectroscopy
• Geometric Structure –Extended X-ray Absorption Fine Structure –X-ray Scattering –Electron Microscopy –Scanning Probe Microscopy –Atom Probe
• Physical Structure –Tomography
8
![Page 9: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/9.jpg)
Probes • Scattering Probes
9
![Page 10: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/10.jpg)
Electronic Structure • Chemical Environment - Energy Position
• Physical Environment - Broadening
10
![Page 11: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/11.jpg)
Photoelectron Spectroscopy
11
![Page 12: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/12.jpg)
Resonant Photoemission of Pu • 5f Electron systems are different
Terry, J, et al., Surface Science 499, L141 (2002) Tobin, J. G, et al., Physical Review B 68, 155109 (2003)
12
![Page 13: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/13.jpg)
Terry, J, et al., Surface Science 499, L141 (2002) Tobin, J. G, et al., Physical Review B 68, 155109 (2003)
13
Resonant Photoemission of Pu
q ~ <5d105f5|r|5d95f6> / <5d105f5|r|5d105f4 + e->
• Fano profile • FCC Pu suggests more
atomic-like character
![Page 14: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/14.jpg)
Photoemission Of Disordered Alloys • High resolution core level spectroscopy allows one to
measure disorder broadening • Can now calculate by calculating the core level shift for
every atom
Cu 2p
14
![Page 15: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/15.jpg)
X-ray Absorption
• Photon In
• Electron Excite
• Electron Scatters
• Electron Interference
15
![Page 16: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/16.jpg)
X-ray Absorption
16
J. Stohr Nexafs Spectroscopy
![Page 17: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/17.jpg)
XAS Analysis
Convert to k-space and extract oscillations as a function of wavenumber
Fourier transform into R-space
17
![Page 18: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/18.jpg)
Irradiated Zircaloy-2
• Zr2Fe0.6Ni0.4
• Dissolution and disorder of secondary phase
Kuri, et al., Appl Phys A (2010) 98: 625–633
1A - 5.9 x 1021 n/cm2
1B - 14.2 x 1021 n/cm2
18
![Page 19: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/19.jpg)
ZrC as Cladding
19
![Page 20: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/20.jpg)
ZrC • Sphere 1.8 nm in diameter • Model undefected regions as spherical
20
![Page 21: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/21.jpg)
X-ray Scattering
• Geometric structure
• Phase identification
• Size/Shape/Stress
Calculate lattice strains (elastic) from change in atomic spacing.
Liu, et al., Materials Science & Engineering A 651, 55 (2016)
21
![Page 22: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/22.jpg)
Alloy 617: Intermediate Heat
Exchanger (IHX) of VHTR
Liu, et al., Materials Science & Engineering A 651, 55 (2016)
22
• M23C6 and M6C
• Carbide phase analysis complicated by containment
![Page 23: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/23.jpg)
Alloy 617: Intermediate Heat
Exchanger (IHX) of VHTR • Initial Linear Increase in M23C6 Lattice Strain
23
Liu, et al., Materials Science & Engineering A 651, 55 (2016)
![Page 24: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/24.jpg)
Alloy 617: Intermediate Heat Exchanger
(IHX) of VHTR • Becomes constant as nucleation of microcracks or
microvoids occur • Leading to the fracture or decohesion of the particles
24
Liu, et al., Materials Science & Engineering A 651, 55 (2016)
![Page 25: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/25.jpg)
U10Mo Fuel
25
Okuniewski, et al., J. Nuc. Mater., submitted
1.5 mm total thickness. 0.25mm thick U10Mo foil. Foil was cold rolled with Zr diffusion layer, then HIP bonded.
![Page 26: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/26.jpg)
U10Mo
• Map Full Strain Tensor
Okuniewski, et al., J. Nuc. Mater., submitted
26
![Page 27: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/27.jpg)
U10Mo • Rapid approach to zero stress at boundary suggest the material
is not bonded on lateral interface
~5000 data points, 72 diffraction patterns per point = ~350K diffraction patterns
Okuniewski, et al., J. Nuc. Mater., submitted
27
![Page 28: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/28.jpg)
Small Angle X-ray Scattering • Sensitive To Shape and Distribution of Electrons
28
Irving unpublished
![Page 29: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/29.jpg)
SAXS of ODS Steel • Y2Ti2O7 and Y2TiO5 nanoparticles at 960 C Diameter
2.6 nm
Kim, et al., Materials Transactions, Vol. 50, No. 4 (2009) pp. 917 to 921
29
![Page 30: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/30.jpg)
Tomography • Microtomography
Schematic diagram of the Zernike phase contrast X-ray microscope
X-ray transmission image of the Siemens calibration
standard with 30 nm minimum features. FOV:
30x30 microns2
Pianetta unpublished
Zabler, et al., OPTICS LETTERS 32, 2987 (2007)
30
• Nanotomography
![Page 31: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/31.jpg)
Friction Weld Crack TiAl/Ti6Al4V
• 150 keV at 50 μm Resolution
Sun, et al., AIP Conf. Proc. 1430, 1251-1258 (2012)
31
![Page 32: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/32.jpg)
Tomography of Fuel Pin • High Energy Tomography Of UO2 Fuel In a Steel Clad
Fuel Pin –White Beam Filtered To 251 KeV –Cadmium-Tungstate Scintillator - 5 μm Resolution
32
![Page 33: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/33.jpg)
Mapping
• All the aforementioned techniques can be combined with mapping by using the spacial profile of the X-ray beam
33
![Page 34: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/34.jpg)
Pu(VI) Sorption on WIPP 1A Bacteria
• C K-edge Map
• 100 nm Resolution
Strietelmeier, et al., LANL
34
![Page 35: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/35.jpg)
Kropf, Fortner, DOE-OSTI Report www.ipd.anl.gov/anlpubs/2006/11/57766.pdf
35
Corrosion of Commercial Spent Fuel • Fluorescence map
• Only spent fuel sample at synchrotron???
• [Np] drops with 20 microns from 1:1500 to 1:7000 proportional U 4+/6+ fraction
![Page 36: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/36.jpg)
Electron Microscopy
JEOL Manual
36
![Page 37: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/37.jpg)
Scanning Electron Microscopy (SEM) • Secondary Electrons
– Lost energy due to inelastic scattering
– Sensitive to physical structure (topography)
• Backscattered Electrons – Elastically scattered – Sensitive to atomic
number (elemental) • X-ray Fluorescence
– Collisionally excited states relax emitting X-rays
FEWER
secondary e– escape
MORE
secondary e– escape
37
JEOL Manual
![Page 38: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/38.jpg)
SEM Boron Nitride
• Large BN flakes grown on thin film silver
38
Velazquez, et al., JOURNAL OF APPLIED PHYSICS 119, 095306 (2016)
![Page 39: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/39.jpg)
Transmission Electron Microscopy
(TEM)
• Topography
• Morphology
• Composition
• Crystallography
SiC
39
Seibert, et al., in preparation
![Page 40: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/40.jpg)
TEM • Thin (<100nm)
specimen
• Electrons illuminate the specimen
• Objective lenses form an image or a diffraction pattern
• Electrons either pass through the sample unimpeded, or are scattered
• Image is viewed on a fluorescent screen
40
![Page 41: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/41.jpg)
TEM
Petrova, PhD Dissertation (2006)
41
• Bright field
Dark field Bright field
![Page 42: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/42.jpg)
High Angle, Annular Dark field
(HAADF)
• High scattering angle
• Inelastic, incoherent electrons
• No diffraction
Senapati, MS Dissertation (2005)
42
![Page 43: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/43.jpg)
TEM ZrC
• Dislocation loops • TEM - proton
irradiated 1.5 DPA @ 800 °C
• White arrows edge-on dislocation loops on (111) planes
• Angle between the edge-on dislocations on different (111) planes is ~70.5°
Olive, et al., Journal of Nuclear Materials 475, 123 (2016)
43
![Page 44: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/44.jpg)
Scanning Probe Microscopy
• Scanning Tunneling Microscopy
–Tunneling current to tip
• Atomic Force Microscopy
–Force on tip
44
![Page 45: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/45.jpg)
SPM • Tip dragged across a sample
45
![Page 46: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/46.jpg)
Ag on Si(111)
• Single atomic step islands of epitaxial Ag on Si(111)
46
Velazquez, et al., Applied Surface Science 360, 762 (2016)
![Page 47: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/47.jpg)
Putting Them All Together to Tell a
Story
• Accident tolerant fuels
• High temperature reactors
–TRISO Fuel
47
Seibert, et al., in preparation
![Page 48: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/48.jpg)
Barrier Layer
• SiC is the barrier layer in TRISO fuels
• To get TRISO fuels qualified for use
–Must understand mechanisms of damage
48
![Page 49: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/49.jpg)
Irradiated TRISO
• Irradiated in the Advanced Test Reactor
• After deconsolidation, select particles annealed to high temperatures for accident simulation
• Isolation of SiC shell through chemical processing
X-ray Tomography of SiC fragments – C. Silva (ORNL)
49
![Page 50: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/50.jpg)
Irradiated TRISO
50
![Page 51: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/51.jpg)
Fluorescence
• Elemental analysis
51
Seibert, et al., in preparation
![Page 52: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/52.jpg)
XAS • Ag is metallic
–May be an alloy
52
Seibert, et al., in preparation
![Page 53: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/53.jpg)
Microscopy • Focused Ion Beam Milling
53
Seibert, et al., in preparation
![Page 54: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/54.jpg)
As-Irradiated Sample: IPyC/SiC
Interface • High angle, annular dark field shows high Z
Bright Field HAADF
54
Seibert, et al., in preparation
![Page 55: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/55.jpg)
As-Irradiated Sample: IPyC/SiC
Interface • Lot of overlap among fission products
• Some co-location with actinides
Fission Actinides
55
Seibert, et al., in preparation
![Page 56: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/56.jpg)
What Did We Learn By Combining
Techniques? • Fission products and actinides found along grain
boundaries and triple points in the SiC.
• Fission products (specifically Pd) found all the way to the OPyC interface
• U has been found in large quantities as deep as 13μm from the IPyC interface, and in trace quantities near the OPyC interface
• Ag is metallic
56
![Page 57: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/57.jpg)
Safety Concerns
• Working with radioactive materials does require extra precaution
• Minimize worker exposure
–Use long tools
–Redesign holders to minimize handling time
57
![Page 58: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/58.jpg)
Safety
58
Terry, unpublished
![Page 59: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/59.jpg)
Nuclear Science User Facility
• Almost all of these techniques are available to all through the Nuclear Science User Facility
–Write a proposal
–If awarded, assigned Subject Matter Expert to work with you
–Great way to get access to these techniques
59
![Page 60: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/60.jpg)
References
60
• Rotenberg: www-b17.lbl.gov/BL7/who/eli/SRSchoolER.pd • Terry, J, et al., Surface Science 499, L141 (2002) • Tobin, J. G, et al., Physical Review B 68, 155109 (2003) • Cole, et al., J. Phs.:Condens. Matter 10 (1998) 5679-5695 • Martin, et al, Physical Review B 72, 054210 (2005) • W. Olovsson et al, Journal of Electron Spectroscopy and Related
Phenomena 178-179 (2010) 88-99 • J. Stohr Nexafs Spectroscopy • Kuri, et al., Appl Phys A (2010) 98: 625–633 • Olive, et al., Journal of Nuclear Materials 475, 123 (2016) • Liu, et al., Materials Science & Engineering A 651, 55 (2016) • Okuniewski, et al., J. Nuc. Mater., submitted • Kim, et al., Materials Transactions, Vol. 50, No. 4 (2009) pp. 917 to
921 • Zabler, et al., OPTICS LETTERS 32, 2987 (2007) • Sun, et al., AIP Conf. Proc. 1430, 1251-1258 (2012) • Strietelmeier, et al, LBNL/ALS—29523 (1999) • Kropf, Fortner, DOE-OSTI Report
www.ipd.anl.gov/anlpubs/2006/11/57766.pdf • JEOL Manual • Velazquez, et al., JOURNAL OF APPLIED PHYSICS 119, 095306
(2016) • Petrova, PhD Dissertation (2006) • Senapati, MS Dissertation (2005) • Velazquez, et al., Applied Surface Science 360, 762 (2016) • Seibert, et al., in preparation • C. Silva, ORNL
![Page 61: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/61.jpg)
Students and Postdocs
61
• Dan Olive • Hasitha Ganegoda • Daniel Velazquez • Joshua Wright • Hamdi Man • Rachel Seibert • ZhengRong Lee
![Page 62: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/62.jpg)
Questions???
62
![Page 63: Radiochemistry Webinars Nuclear Materials Analysis ... · Radiochemistry Webinars Nuclear Materials Analysis: Physical ... –Atom Probe •Physical Structure –Tomography 8 . Probes](https://reader031.vdocuments.net/reader031/viewer/2022040317/5e323c0cf9096d3be4097667/html5/thumbnails/63.jpg)
Upcoming Webinars
• Nuclear Materials Analysis — Chemical Methods • Nuclear Materials Analysis — Non-Destructive Analysis • Nuclear Materials Analysis — Mass Spectoscopy
NAMP website: www.wipp.energy.gov/namp