Materialia 6 (2019) 100294

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Materialia
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Full Length Article

Microstructural characterization of plutonium oxalate and oxide particles

by three-dimensional focused ion beam tomography
Brandon W. Chung∗, Richard A. Torres
Lawrence Livermore National Laboratory, P.O. Box 808, Livermore, CA 94551, USA

a r t i c l e i n f o a b s t r a c t

Keywords: Focused ion beam (FIB) tomography was used to characterize three-dimensional (3D) internal microstructures of
Plutonium Oxalate plutonium oxalate and oxide particles. Sequential two-dimensional (2D) sectioning and imaging using FIB and
Plutonium Oxide 3D image reconstruction were used to elucidate and distinguish internal pore microstructure and distribution
3D microscopy
in plutonium oxide particles calcined from plutonium oxalate precipitates. The results show that the plutonium
Focused ion beam tomography
oxide particles have a significant increase in pore volume fraction while retaining the exterior morphological
Nuclear forensics
shape of the corresponding oxalate precipitates. This technique enables the examination of the internal structure
of radioactive microparticles for nuclear forensics that is not available with conventional microscopy.

1. Introduction
Nuclear forensics is a scientific methodology to understand the his-
tory of nuclear materials as fully as possible to identify their process
history and provenance [1–7]. Among the various forms of nuclear ma-
terials, the most common chemical form of plutonium (Pu) found in
nuclear facilities is Pu oxide, mainly PuO2 . Thus, its particle analy-
sis is one of the most important tasks in the field of nuclear forensics
[8–10]. Various processing parameters in the synthesis are known to
affect the morphology of Pu oxide products [2,11–14]. Therefore, tem-
poral changes in the microstructure and morphology of Pu oxide ma-
terials could provide insight into processing parameters and storage
conditions. Using these salient material characteristics, one can nar-
row down the possible process history and provenances of Pu oxide
products.
While there has been significant radiochemistry work to evaluate
characteristics such as isotopic compositions and trace elements rele-
vant to nuclear forensics [2,3,5,8,15–22], there is a dearth of inves-
tigative effort into the microstructural characteristics of Pu oxide prod-
ucts [9,23–28]. Past studies suggested that the microstructures of Pu
oxalate precipitates are retained after calcining in air to Pu oxide prod-
ucts [25,27,28]. However, these studies were based on microstructural
features in two dimensions (2D) from the particle’s surface, and do not
include the exact nature of material features within the bulk. There
are many internal microstructural features that can only be measured
in three dimensions (3D), such as the true shape and size of internal
microstructural features and their distribution and population inside
particles.
∗
Corresponding author.
E-mail address: chung7@llnl.gov (B.W. Chung).
Focused ion beam (FIB) and scanning electron microscopy (SEM) to-
mography (FIB-SEM or FIB tomography) has proven very useful in ob-
taining high-resolution 3D microstructural information from the sam-
pled volume [29–40]. With this technique, we can alternate the use of
FIB and SEM to remove material and image areas of interest. Although
FIB tomography has proven useful in diverse material characterizations,
it is not as common in nuclear forensics studies involving highly radioac-
tive materials, such as Pu materials. We have been evaluating the appli-
cability of the FIB-SEM instrument (FEI DualBeam Quanta 3D FEG) to
improve quantification of key microstructural features entrained in nu-
clear materials. In this study, FIB tomography was used to characterize
the 3D internal morphology of Pu oxalate and oxide products to show
how the processing parameters affect the internal morphology. Further-
more, we discuss current limitations and suggest areas for the future
development of nuclear forensics.
2. Experimental methods
The materials investigated are Pu oxalate, Pu2 (Ox)3 ·10H2 O, and ox-
ide, PuO2 , products. The preparation of Pu oxalate/oxide products is
described in detail elsewhere [40,41]. Briefly, we dissolved high-purity
Pu metal with 1.0 M hydrochloric acid (HCl) to produce PuCl3 solu-
tions at ambient temperature in a nitrogen glovebox. We used a Mettler
T50 autotitrator with a three-bladed stirrer and the burette tip near the
bottom edge of the cup to add reagents at controlled rates into a near-
cylindrical 100-mL titration cup. We used 6.7 mmol Pu in 65 mL of
solution for the direct strike syntheses (adding oxalate acid solution to
the metal solution). We added ∼15 mL of 1 M oxalic acid (a 50 mol%
excess) to precipitate the Pu (III) oxalates. One sample of oxalate was
produced under reverse strike conditions (adding the metal solution
to the oxalic acid solution). In this case, the Pu was added in 1-mL

https://doi.org/10.1016/j.mtla.2019.100294
Received 27 December 2018; Accepted 3 March 2019
Available online 15 March 2019
2589-1529/© 2019 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
B.W. Chung and R.A. Torres
increments with a plastic-tipped pipettor until 20 mL of 0.33 M Pu in
2 M HCl had been added to the oxalate solution.
After vacuum-filtering the precipitates and drying them overnight
with continued suction, portions of the oxalates were calcined in air
in ceramic crucibles to produce the oxides. Pu oxalates were calcined at
500 °C for 6 h, cooled overnight, agitated, and reignited for an additional
6 h at 500 °C. This temperature ensured conversion to pure PuO2 [40].
The furnace was in a nitrogen glove box with an air supply to the interior
of the furnace. We found 9.4 ± 0.4 waters of 4 hydration per Pu2 (Ox)3
molecule. The PuO2 phase purity was confirmed by X-ray diffraction
analysis.
The FIB tomography method used in this work is a modified version
of the method described for the bulk uranium (U) and Pu metals [7].
A FIB-SEM microscope—FEI DualBeam Quanta 3D—was used for mor-
phological investigation. This instrument consists of an electron column
with field emission gun (FEG) and a focused ion column containing a
gallium (Ga) ion source. For FIB-SEM analysis, Pu oxalate and oxide par-
ticles were dispersed onto carbon tape attached to a SEM sample holder
inside the nitrogen glovebox. The prepared specimens were coated ei-
ther with a titanium layer for SEM analysis or a thick (∼2 𝜇m) gold
layer to prevent the spread of radiological contamination during han-
dling and transfer to the FIB-SEM microscope. Although details such as
how the radiological sample is handled in the microscope are specific
to this work, it is likely that the general FIB-SEM DualBeam operational
techniques are applicable.
3. Results and discussion
Images of Pu oxalate precipitates and calcined oxide particles were
collected and assessed to benchmark as-produced materials through the
analysis of SEM images and FIB tomography. Fig. 1 shows some exam-
Fig. 1. Example SEM images of Pu oxalate and oxide particles (coated with titanium) [40]: (a) oxalate from reverse strike synthesis and (b) resulting oxide from
calcining at 500 °C in air; and (c) oxalate from direct strike synthesis and (d) resulting oxide from calcining at 500 °C in air.
Materialia 6 (2019) 100294
ples of the 2D microstructures of collected Pu oxalate and oxide sam-
ples. Qualitatively, the macro-particles of the oxalate precipitates and
calcined oxides all consist of similar clumps or massive agglomerates.
Table 1 shows 2D equivalent circuit diameters (ECD) and circularities
of single particles that were easily discerned with image processing (Im-
agePro 3D v.9.3.3). It is clear the collected Pu particles are made of two
types of agglomerated particles: the reverse strike process producing
irregularly shaped oxalate particles and the direct strike process pro-
ducing spherically shaped particles. Our results are consistent with pre-
vious studies that showed the Pu oxalate morphology is retained when
calcined to PuO2 [24,25,28]. For 3D tomography, we selected single
particles that were of average size and well separated from clumps or
massive agglomerates.
The main advantage of using FIB-SEM tomography to image Pu par-
ticles is the ability to reveal their internal microstructures and to gener-
ate their 3D structures. Figs. 2 and 3 show some representative internal
microstructures of oxalate and oxide particles. The FIB cuts a 2D cross-
sectional surface through the sample (Fig. 2(a), (d) and Fig. 3(a), (d)).
Here we used milling current of 0.5 nA as a compromise between a sharp
section profile and reasonable milling time. The 2D sectioning and imag-
ing sequence is repeated with removing a predetermined thickness of
material from the sample. These images show complex pore and micro-
crack structures in the interior of the sample. We describe details of large
microcracks in the next section and small internal pores/microcracks in
the later section for 3D microstructural study.
Both oxalate (Fig. 2(a)) and oxide (Fig. 2(d)) particles from the re-
verse strike process clearly show large microcracks (dark areas) that
propagate through the entire volume, indicating these particles formed
from aggregations of smaller particles. In contrast, the cross-sectional
investigation of both oxalate and oxide particles from the direct strike
process do not show identical internal microcracks (Fig. 3). While the
B.W. Chung and R.A. Torres Materialia 6 (2019) 100294

Table 1
Two-dimensional morphological shape parameters from Pu oxalate and oxide particles. Measurement is from single
particles that were easily discerned from clumps or massive agglomerates. ECD is the equivalent circular diameter,
and N is the number of single particles that were well separated from clumps or massive agglomerates.

Process Sample ECD (μm) Minimum diameter (μm) Maximum diameter (μm) Circularity N

Reverse strike Oxalate 5.7 3.1 10.5 0.61 32

Calcined oxide 5.5 2.4 10.2 0.62 50
Direct strike Oxalate 14.3 4.8 38.4 0.75 46
Calcined oxide 10.9 3.7 25.5 0.77 97

Fig. 2. Example FIB tomography and 3D rep-

resentations from reverse strike oxalate (a–c)
and corresponding calcined oxide (d–f) parti-
cles. (a) and (d) show 2D cross-sections; (b) and
(e) show 3D internal pore morphology; and (c)
and (f) show 3D particle and internal pore mor-
phology. Gold coating on the surface is shown
as bright white in (a) and (d).

oxalate particle shows large, continuous microcracks that appear to
break the particle to smaller pieces (Fig. 3(a)), the corresponding ox-
ide particle shows short, discontinuous microcracks (Fig. 3(b)). We be-
lieve this observed morphological difference is likely caused by chemical
changes in the oxalate particles from longer exposure to trace amount
of air in a nitrogen glove box. While the more stable oxide particles
were prepared by calcination in air approximately one month after fab-
ricating oxalate particles, the gold coating to seal the oxalate particles
occurred approximately two months later. Further work is required to
understand the morphological changes observed with oxalates from the
direct strike process under inert and air atmospheres.
Sequential slicing and imaging with FIB-SEM allows us to create 3D
representation of a particle’s shape and interior structure from a stack
of 2D images. The higher-quality microstructural characterization can
be extracted by 3D microscopy using a precision sectioning and imag-
ing process known as the “slice and view” technique [7,30,42,43]. The
image stack acquired during sequential slicing is then input to a 3D ren-
dering software (ImagePro 3D v.9.3.3) to create a spatial model of the
particle. Figs. 2 and 3 show the 3D rendering of the particle’s shape and
internal microstructures. Unlike the conventional 2D micrographs, 3D
representation provides us with 3D information of the probed volume,
such as the real shape, size, and distribution of internal microstructural
B.W. Chung and R.A. Torres
features. To the best of our knowledge, this is the first report of manip-
ulating Pu oxalate and oxide particles in this way for cross-sectioning to
generate 3D internal microstructural features.
With 3D tomography, we can measure the surface areas and vol-
umes of internal pores and microcracks. Thus, the sphericity can be
measured instead of the circularity, which is used in 2D morphologi-
cal images. Using the image analysis software (ImagePro 3D v.9.3.3),
we performed preliminary quantification of pores and microcracks. The
morphological map is presented in Fig. 4(a) and (b) for samples from
reverse and direct strikes, respectively. These maps show that internal
pores and microcracks have smooth ellipsoidal geometry [44]. How-
ever, these maps also show that the morphological analysis using all
the pores and microcracks together produce results of nearly identical
morphological maps between the samples. Rather than directly quanti-
fying all the morphological features, we need to explore statistical anal-
ysis to allow the combination of a number of morphological features
or identifying primary morphological features (PMF) tied to the process
history.
Materialia 6 (2019) 100294
Fig. 3. Example FIB tomography and 3D repre-
sentations from direct strike oxalate (a–c) and
corresponding calcined oxide (d–f) particles.
(a) and (d) show 2D cross-sections; (b) and (e)
show 3D internal pore morphology; and (c) and
(f) show 3D particle and internal pore morphol-
ogy. Gold coating on the surface is shown as
bright white in (a) and (d).
The 3D model elucidates the actual sizes and shapes of internal pores
and microcracks identified from 2D images. Both oxalate and oxide par-
ticles contain complex networks of pores and microcracks. From the 3D
representation, we observed that both oxalate and oxide have a rough
outer surface. Occasionally, irregularity of their surfaces is so great that
their sections present roughly jagged or toothed boundaries. As observed
in the 2D cross-sectional images, their internal pores are typically iso-
lated acicular pores and have smooth outer geometry. Based on past
studies [11,25,28], it is likely that each oxalate is formed from aggrega-
tions of smaller particles.
The internal morphology of Pu oxide shows a significantly higher
density of internal pores and microcracks than Pu oxalate. By 3D quan-
tification, we found that a typical combined pore and microcrack vol-
ume of oxalates from both reverse and direct strike processes was ap-
proximately 1.9% while the oxides were 5.2%. In the oxide sample, there
appears to be a significant population of nanoscale pores that cannot
be visualized clearly due to the resolution limit of the SEM imaging.
Thus, the combined pore and microcrack volume fraction in oxide is
B.W. Chung and R.A. Torres Materialia 6 (2019) 100294

sometimes milling of a fiducial mark. While it is not possible to avoid

all damage to the specimen surface when ions are used in the milling
operation, the damage can be minimized through the careful selection
of FIB operational parameters.
Even with high resolution and quality of microstructural images from
FIB tomography, the rate-limiting step in characterizing microstructural
features in 3D is in performing segmentation of FIB tomography data for
visualization and analysis. As shown in Figs. 2 and 3, images from inter-
nal structures are likely composed of complex grayscale gradients that
are difficult to segment through standard automated segmentation. Im-
age artifacts such as bright areas are caused by charging around pores
or microcracks and from lack of a conductive path that removes excess
electrons. Higher-resolution SEM imaging with improved stability of FIB
milling could help with quantification of nanoscale pores in the bulk.
Furthermore, the morphological analysis using 3D tomography is a com-
plex effort. We need to develop better morphological descriptions, sta-
tistical analysis, and identifying primary morphological features (PMF)
to improve interpreting wide-ranging geometrical features of internal
pores and microcracks. Analysis of crystallographic or chemical maps
rather than the analysis of image data can also alleviate some of these
difficulties.
For application in nuclear forensics, it is imperative that we preserve
discriminating microstructural features that betray materials’ processes
and provenances. From the examples in this paper, we demonstrated
application of the FIB technique as a potent tool in microstructural char-
acterization of highly radioactive Pu particles. Internal microstructural
characteristics, such as the volume fraction of pores, present evidentiary
examples for nuclear forensics. The impact of using the FIB-SEM tech-
nique in nuclear forensics to extract and evaluate entrapped material
signatures is evident from this work, where we see for the first time
the exact nature of microstructural morphology, including inner mi-
crostructural features, in Pu oxalate and oxide particles that have been
elusive. Rather than identifying discriminating microstructural features
by highly idealized and a priori known conventional 2D microstructural
images, the FIB technique has potential for high-fidelity quantification
of microstructural features for nuclear forensics.

Fig. 4. Morphological map (Shape factor versus Sphericity) of each internal 4. Conclusions
pore/microcrack of samples from reverse strike (a) and direct strike (b) pro-
cesses. Shape factor is the ratio of the minimum and the maximum Feret diam- This work demonstrates the capabilities of FIB tomography for inves-
eters [44]. Sphericity is the ratio of the volume of the pore/microcrack to the tigating the internal microstructure of radioactive microparticles. The
volume of a sphere with the same surface area of the pore/microcrack. key microscopic structural features of the internal cavities of Pu oxalate
and oxide particles and their distribution were investigated. From in-
anticipated to be larger than determined from this work. Consistent with
ternal microstructural images and 3D reconstructions, our preliminary
2D images, these internal pores and microcracks generally give the ap-
results show that the oxide particle has a significantly higher concen-
pearance of radiating outward toward the surface, and the preservation
tration of internal pores from the thermal decomposition of volatile
of the outer particle shape is related to exit pathways created by the
chemical species in the oxalate. Unlike the conventional 2D SEM im-
original pores and microcracks in the oxalate. During thermal decompo-
age, which only shows that the exterior morphological shape is retained
sition in air of the Pu oxalate precipitates, the escaping gases attributed
through heat treatment, the 3D representations clearly show differences
to the increase in the formation of additional pores and microcracks.
in the population and distribution of internal pores between Pu oxalate
Past work on Pu (IV) oxalate and surrogate particles show that most of
and oxide particles. Further research is needed from a larger dataset of
their surface area is due to internal porosity and interconnected internal
internal structures from various processing conditions such as calcina-
pores formed by carbon product removal during thermal decomposition
tion temperatures. A new dataset built through advanced morphological
[11–14]. This work confirms past studies that calcining oxalate does not
quantification processes could provide well characterized forensic sig-
change the outer morphological shape of the oxide product [25,27,28].
natures. FIB tomography opens the door to an improved quantitative
The particle shape is retained despite the loss of gases during the calcin-
study of microstructures in 3D at the microscale for nuclear forensics.
ing process. The preservation of the particle shape can be related to the
large number of internal pores and microcracks providing exit pathways
for gases. Acknowledgments
As the results presented here show, FIB tomography for bulk Pu ox-
alate and oxide particles offers advantages over earlier conventional 2D This work was performed under the auspices of the U.S. Department
SEM images that evaluate surface morphology. It allows for precision of Energy by Lawrence Livermore National Laboratory under Contract
micro-surgery by ion milling to expose inner microstructures and more DE-AC52-07NA27344. This work was supported by the Department of
accurate 3D microscopy of microstructural features that have been elu- Homeland Security, under competitively awarded contract HSHQDN-
sive using conventional 2D-imaging techniques. However, FIB tomog- 16-X-00044. This support does not constitute an expressed or implied
raphy is a destructive technique that requires sample preparation and endorsement on the part of the Government. We thank William Talbot,
B.W. Chung and R.A. Torres
Denise Ashley, Cheng Saw, and David Roberts for their assistance in
X-ray diffraction and handling radioactive materials.
Declaration of interest
None.
References
[1] S.S. Hecker, Plutonium and its alloys: From atoms to microstructure, Los Alamos Sci.
26 (2000) 290–335.
[2] K. Mayer, M. Wallenius, Z. Varga, Nuclear Forensic Science: Correlating Measurable
Material Parameters to the History of Nuclear Material, Chem. Rev. 113 (2) (2013)
884–900.
[3] K. Mayer, M. Wallenius, T. Fanghaenel, Nuclear forensic science - From cradle to
maturity, J. Alloys Compd. 444 (2007) 50–56.
[4] K. Mayer, M. Wallenius, I. Ray, Nuclear forensics - a methodology providing clues on
the origin of illicitly trafficked nuclear materials, Analyst 130 (4) (2005) 433–441.
[5] K.J. Moody, P.M. Grant, I.D. Hutcheon, Nuclear Forensic Analysis, CRC Press, Boca
Raton, FL, 2015.
[6] M.J. Kristo, A.M. Gaffney, N. Marks, K. Knight, W.S. Cassata, I.D. Hutcheon, Nu-
clear Forensic Science: Analysis of Nuclear Material Out of Regulatory Control, in:
R. Jeanloz, K.H. Freeman (Eds.), Annual Review of Earth and Planetary Sciences,
44, Annual Reviews, Palo Alto, 2016, pp. 555–579.
[7] B.W. Chung, R.G. Erler, N.E. Teslich, Three-dimensional microstructural characteri-
zation of bulk plutonium and uranium metals using focused ion beam technique, J.
Nucl. Mater. 473 (2016) 264–271.
[8] M. Wallenius, K. Luetzenkirchen, K. Mayer, I. Ray, L.A.I.d.l. Heras, M. Betti, O. Crom-
boom, M. Hild, B. Lynch, A. Nicholl, H. Ottmar, G. Rasmussen, A. Schubert, G. Tam-
borini, H. Thiele, W. Wagner, C. Walker, E. Zuleger, Nuclear forensic investigations
with a focus on plutonium, J. Alloys Compd. 444 (2007) 57–62.
[9] T. Shinonaga, D. Donohue, A. Ciurapinski, D. Klose, Age determination of single
plutonium particles after chemical separation, Spectrochim. Acta Part B-Atom. Spec-
trosc. 64 (1) (2009) 95–98.
[10] D. Donohue, A. Ciurapinski, J. Cliff III, F. Ruedenauer, T. Kuno, J. Poths, Microscopic
studies of spherical particles for nuclear safeguards, Appl. Surf. Sci. 255 (5) (2008)
2561–2568.
[11] P.K. Smith, G.A. Burney, D.T. Rankin, D.T. Bickford, R.D. Sisson Jr., Effect of ox-
alate precipitation on PuO2 microstructures, in: Proceedings of 6th Int. Materials
Symposium Berkeley, 1977, pp. 223–232.
[12] L. Claparede, N. Clavier, N. Dacheux, A. Mesbah, J. Martinez, S. Szenknect, P. Moisy,
Multiparametric Dissolution of Thorium-Cerium Dioxide Solid Solutions, Inorg.
Chem. 50 (22) (2011) 11702–11714.
[13] L. Claparede, N. Clavier, N. Dacheux, P. Moisy, R. Podor, J. Ravaux, Influence of
Crystallization State and Microstructure on the Chemical Durability of Cerium–
Neodymium Mixed Oxides, Inorg. Chem. 50 (18) (2011) 9059–9072.
[14] L. Claparede, F. Tocino, S. Szenknect, A. Mesbah, N. Clavier, P. Moisy, N. Dacheux,
Dissolution of Th1-xUxO2: Effects of chemical composition and microstructure, J.
Nucl. Mater. 457 (2015) 304–316.
[15] K. Mayer, M. Wallenius, M. Hedberg, K. Luetzenkirchen, Unveiling the history of
seized plutonium through nuclear forensic investigations, Radiochim. Acta 97 (4–5)
(2009) 261–264.
[16] Y. Miyamoto, D. Suzuki, F. Esaka, M. Magara, Accurate purification age determi-
nation of individual uranium-plutonium mixed particles, Anal. Bioanal. Chem. 407
(23) (2015) 7165–7173.
[17] U. Nygren, H. Rameback, C. Nilsson, Age determination of plutonium using induc-
tively coupled plasma mass spectrometry, J. Radioanal. Nucl. Chem. 272 (1) (2007)
45–51.
[18] Z. Varga, G. Suranyi, Detection of previous neutron irradiation and reprocessing of
uranium materials for nuclear forensic purposes, Appl. Radiat. Isot. 67 (4) (2009)
516–522.
[19] S.P. LaMont, G. Hall, Uranium age determination by measuring the Th-230/U-234
ratio, J. Radioanal. Nucl. Chem. 264 (2) (2005) 423–427.
Materialia 6 (2019) 100294
[20] R.P. Keegan, R.J. Gehrke, A method to determine the time since last purification of
weapons grade plutonium, Appl. Radiat. Isot. 59 (2–3) (2003) 137–143.
[21] Y. Chen, Z.-y. Chang, Y.-g. Zhao, J.-l. Zhang, J.-h. Li, F.-j. Shu, Studies on the age de-
termination of trace plutonium, J. Radioanal. Nucl. Chem. 281 (3) (2009) 675–678.
[22] K. Mayer, M. Wallenius, K. Lutzenkirchen, J. Galy, Z. Varga, N. Erdmann, R. Buda,
J.V. Kratz, N. Trautmann, K. Fifield, Iop, Nuclear Forensics: A Methodology Ap-
plicable to Nuclear Security and to Non-Proliferation, in: Proceedings of the 2010
International Nuclear Physics Conference, IOP Publishing Ltd, Bristol, 2010.
[23] T. Shinonaga, D. Donohue, H. Aigner, S. Buerger, D. Klose, T. Karkela, R. Zilliacus,
A. Auvinen, O. Marie, F. Pointurier, Production and Characterization of Plutonium
Dioxide Particles as a Quality Control Material for Safeguards Purposes, Anal. Chem.
84 (6) (2012) 2638–2646.
[24] X. Machuron-Mandard, C. Madic, Plutonium dioxide particle properties as a function
of calcination temperature, J. Alloys Compd. 235 (2) (1996) 216–224.
[25] R.M. Orr, H.E. Sims, R.J. Taylor, A review of plutonium oxalate decomposition reac-
tions and effects of decomposition temperature on the surface area of the plutonium
dioxide product, J. Nucl. Mater. 465 (2015) 756–773.
[26] G.A. Burney, P.K. Smith, Controlled Pu02 Particle Size from Pu(III) Oxalate Precipi-
tation, in: DP-1689, Aiken, 1984, pp. 1–35.
[27] P.C. Doto, P.K. Peabody, Production of Ceramic Grade Plutonium Dioxide, in:
ARH-SA-213, Richland, 1975, pp. 1–16.
[28] D.T. Rankin, G.A. Burney, Particle Size of 238PuO2 Obtained by Oxalate Precipita-
tion, 1974, pp. 1–25. DP-MS-74-37, Aiken.
[29] A. Aitkaliyeva, J.W. Madden, B.D. Miller, J.I. Cole, Implementation of focused ion
beam (FIB) system in characterization of nuclear fuels and materials, Micron 67
(2014) 65–73.
[30] M.D. Uchic, L. Holzer, B.J. Inkson, E.L. Principe, P. Munroe, Three-dimensional mi-
crostructural characterization using focused ion beam tomography, MRS Bull. 32 (5)
(2007) 408–416.
[31] C.A. Volkert, A.M. Minor, Focused ion beam microscopy and micromachining„ MRS
Bull. 32 (5) (2007) 389–395.
[32] Y.Z. Wang, R.W. Revie, M.W. Phaneuf, J. Li, Application of focused ion beam (FIB)
microscopy to the study of crack profiles„ Fatigue Fract. Eng. Mater. Struct. 22 (3)
(1999) 251–256.
[33] P.G. Kotula, G.S. Rohrer, M.P. Marsh, Focused ion beam and scanning electron mi-
croscopy for 3D materials characterization, MRS Bull. 39 (4) (2014) 361–365.
[34] U. Admon, Single Particles Handling and Analyses, Radioactive Particles in the En-
vironment, Springer, 2009, pp. 15–55.
[35] H. Chen, V.H. Grassian, L.V. Saraf, A. Laskin, Chemical imaging analysis of envi-
ronmental particles using the focused ion beam/scanning electron microscopy tech-
nique: microanalysis insights into atmospheric chemistry of fly ash, Analyst 138 (2)
(2013) 451–460.
[36] M.W. Phaneuf, Applications of focused ion beam microscopy to materials science
specimens, Micron 30 (3) (1999) 277–288.
[37] D.C. Joy, J.R. Michael, Modeling ion-solid interactions for imaging applications,
MRS Bull. 39 (4) (2014) 342–346.
[38] J.M. Conny, Internal Composition of Atmospheric Dust Particles from Focused
Ion-Beam Scanning Electron Microscopy, Environ. Sci. Technol. 47 (15) (2013)
8575–8581.
[39] B.D. Miller, J. Gan, J. Madden, J.F. Jue, A. Robinson, D.D. Keiser, Advantages and
disadvantages of using a focused ion beam to prepare TEM samples from irradiated
U-10Mo monolithic nuclear fuel, J. Nucl. Mater. 424 (1–3) (2012) 38–42.
[40] R.A. Torres, B.W. Chung, P.C. Lan, D.J. Roberts, Exploratory Pu(III) Oxalate/Pu(IV)
Oxide Morphology Studies, Lawrence Livermore National Laboratory, Livermore,
2018.
[41] O.J. Wick, Plutonium Handbook, A Guide to the Technology - Volume I & II, in:
O.J. Wick. (Ed.), The American Nuclear Society, 1980.
[42] S. Cao, W. Tirry, W. Van Den Broek, D. Schryvers, Optimization of a FIB/SEM
slice-and-view study of the 3D distribution of Ni4Ti3 precipitates in Ni-Ti, J. Mi-
crosc. 233 (1) (2009) 61–68.
[43] J.E. Spowart, Automated serial sectioning for 3-D analysis of microstructures, Scr.
Mater. 55 (1) (2006) 5–10.
[44] T.M. Puscas, M. Signorini, A. Molinari, G. Straffelini, Image analysis investigation
of the effect of the process variables on the porosity of sintered chromium steels,
Mater. Charact. 50 (1) (2003) 1–10.