LA-UR-19-27580

Approved for public release; distribution is unlimited.

Title: A Test of ASTM Methods E1245-03 and E562-11 in Calculating the Volume
Fraction of Carbides in a U-10Mo Foil

Author(s): Lopez, Jessica Jazmin

Miller, Cody
Tegtmeier, Eric Lee

Intended for: Report

Issued: 2019-07-31
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A Test of ASTM Methods E1245-03 and E562-11 in Calculating the Volume
Fraction of Carbides in a U-10Mo Foil

Jessica J. Lopez, Cody A. Miller, Eric L. Tegtmeier

Sigma Manufacturing Science Division
Los Alamos National Laboratory

28 January 2019

Memo Sigma-DO-19-0002

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 The CONVERT M3 Reactor Conversion Program

The United States government is committed to further strengthening nuclear security and
nonproliferation in order to reduce the threat of terrorists acquiring nuclear material. To meet this
important mission, the U.S. Department of Energy/National Nuclear Security Agency’s
Administration’s Office of Material Management and Minimization (M3) Reactor Conversion
Program (CONVERT) minimizes the use of highly enriched uranium (HEU) in civilian
applications by working with governments and facilities around the world to convert research
reactors to the use of non-weapons-usable low-enriched uranium (LEU) fuels. Each reactor
converted not only eliminates the need for HEU at civilian sites, but also reduces the amount of
HEU being manufactured, stored, and transported, where it is at its most vulnerable. In instances
where suitable LEU fuels do not exist for particular reactors to convert, the M3 Reactor
Conversion Program contributes to the development of new LEU fuels.
Currently, the CONVERT M3 Reactor Conversion Program is developing a high-density,
monolithic U-Mo fuel for the research reactor conversion, while at the same time establishing
efficient and economic fabrication and manufacturing capabilities. These U-Mo fuel foils will be
clad in 6061 aluminum. In order to prevent interaction between the fuel meat and the cladding, a
zirconium metal diffusion barrier will be applied to the fuel prior to cladding.

Prerequisites and Precautions

Staff members who perform this work are qualified Radiological Workers. Assigned staff and
members comply with all control procedures as indicated by the Integrated Work Document
(IWD). Handling of all radioactive material can result in exposure of workers to doses of
radiation, and therefore proper control procedures are upheld. Samples must be kept clean and
stored safely both during and after testing.

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 Acronyms and Abbreviations

ASTM American Society for Testing and Materials

BSE Backscattered electron
DU Depleted Uranium
HEU High-Enriched Uranium
IWD Integrated Work Document
LANL Los Alamos National Laboratory
LEU Low-Enriched Uranium
SEM Secondary electron microscope
U-10Mo Uranium + 10 wt.% Molybdenum

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 Contents

A Test of ASTM Methods E1245-03 and E562-11 in Calculating the Volume Fraction of
Carbides in a U-10Mo Foil ..............................................................................................................1 
The CONVERT M3 Reactor Conversion Program .........................................................................2 
Prerequisites and Precautions ..........................................................................................................2 
Acronyms and Abbreviations ..........................................................................................................3 
Contents ...........................................................................................................................................4 
List of Figures ..................................................................................................................................5 
List of Tables ...................................................................................................................................6 
Abstract ............................................................................................................................................7 
1.0  Introduction ..........................................................................................................................7 
2.0  Sample Preparation ..............................................................................................................8 
3.0  Constituent area measurement methods...............................................................................8 
3.1  AUTOMATIC IMAGE ANALYSIS ................................................................................................................................. 8 
3.2  MANUAL POINT COUNT ...................................................................................................................................... 10 
4.0  Discussion ..........................................................................................................................12 
5.0  Conclusion .........................................................................................................................14 
6.0  Acknowledgements ............................................................................................................15 
7.0  References ..........................................................................................................................15 

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 List of Figures

Figure 1: (a) Original BSE micrograph and (b) thresholded BSE micrograph. .............................9
Figure 2: 725 points placed over micrograph 001. Grid taken from ASTM E562-11. ................11

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 List of Tables

Table 1:  Metallographic preparation steps for U-10Mo. Polishing was done using a Struers
Mol cloth. .......................................................................................................................8
Table 2:  Relevant spatial quantities calculated for each micrograph using automatic image
analysis...........................................................................................................................9
Table 3:  Average area fraction and relevant statistics. ................................................................9
Table 4:  Point interception counts using 725-point grid for each micrograph. .........................10
Table 5:  Average point count fraction and final volume fraction calculation using a 725-point
grid ...............................................................................................................................10

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 Abstract

Volume fraction measurements of carbides in DU-10Mo castings and foils were performed as
part of a round robin study aimed at ensuring characterization efforts by multiple laboratories
were yielding consistent results. Three of the four labs employed an automatic image analysis
method to determine volume fraction of carbides in the metal and reported results around 2%.
The other laboratory used a grid intercept count method and reported a fraction percentage of
above 5%, about 3% higher than the other labs. At LANL, the method ASTM E1245-03,
Determining the Inclusion or Second-Phase Constituent Content of Metals by Automatic Image
Analysis was employed with a result of 2.02 ± .26%. There was a need to resolve the large
discrepancy in volume fraction measurements reported from the round robin participant that used
the grid intercept method. To do this, the grid intercept method outlined in ASTM E562-11,
Determining Volume Fraction by Systematic Manual Point Count was also performed on the
exact set of micrographs already analyzed by image analysis software at LANL. Calculations
carried out following the manual point count method reported a percentage of 2.2 ± .6% similar
to the result yielded by the automated image analysis method. Explanations for discrepancies in
the results of the two methods are proposed.

1.0 INTRODUCTION

Volume fraction calculations were performed as a working group effort to ensure

characterization of key aspects of U-10Mo castings and foils were consistent between the
participating laboratories. Samples of U-10Mo castings and foils were prepared for
metallographic characterization at LANL. BSE micrographs of one U-10Mo casting sample were
taken at 1000x using an Inspect F SEM. Five of the micrographs were used to calculate a volume
fraction of the inclusions. ASTM E1245-03, Determining the Inclusion or Second-Phase
Constituent Content of Metals by Automatic Image Analysis was followed using Fiji, a
distribution of an image processing program called ImageJ. In each micrograph, the areas of the
inclusions were measured, summed, and divided by the whole micrograph area. The final volume
fraction percentage was the average of all five micrographs, a result of 2.02 ± .26%.

When the results were compared between the laboratories, one laboratory reported an inclusion
volume fraction percentage of over 5%, while the others had results around 2%. A variety of
factors were considered as a cause for the discrepancy including differences in material, sample
preparation, and measurement method. The lab that reported a higher percentage used a point
grid intercept method to determine the volume fraction, as opposed to the automatic
measurement method used by the other participants. In this memo, the two methods are
performed on the same micrographs, and the results are compared.

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2.0 SAMPLE PREPARATION

The U-10Mo samples were mounted in epoxy resin, ground by hand with grinding paper,
polished with diamond suspensions on an automatic polisher.

Table 1: Metallographic preparation steps for U-10Mo. Polishing was done using a
Struers Mol cloth.
Step Media Size
Grinding 120, 320, 600, 800 grit
Mechanical
3µm diamond, 1µm diamond
Polishing

3.0 CONSTITUENT AREA MEASUREMENT METHODS

SEM micrographs of the U-10Mo casting sample were taken with a Thermo Fisher Inspect FEG-
SEM at 1000x with accelerating voltage of 20kV, spot size of 4, and a 40 micron aperture. Five
of the micrographs were used to make inclusion volume fraction measurements with two
different ASTM measurement methods. The first uses an image processing and analysis program
to isolate the constituents of interest by their grayscale intensity and measure their areas. In the
second method, a grid of points is arranged over the micrographs and the points that intersect
with the features of interest are counted manually by eye.

3.1 Automatic Image Analysis

The standard practice ASTM E1245-03, Determining the Inclusion or Second-Phase Constituent
Content of Metals by Automatic Image Analysis [2016ast] was followed using Fiji, a distribution
of an image processing program called ImageJ. First, threshold settings were imposed on a
micrograph so that the inclusions were converted to black but not enlarged, and the rest of the
micrograph converted to white. The thresholded micrograph was constantly compared to the
original to improve accuracy in identifying constituents of interest and removal of artifacts
(Figure 1). If obvious dust particles appeared in the micrograph, they were manually removed
using the paintbrush tool. The software then counts the isolated particles and counts the number
of pixels comprising each. Finally, the areas of all the inclusions in the micrograph were summed
and divided by the total area of the micrograph. This process was repeated for all five
micrographs and the estimate of the volume fraction of carbides in the metal was taken to be the
average of all five micrographs (Table 3).

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Table 2: Relevant spatial quantities calculated for each micrograph using automatic
image analysis.
Average Feature Total
Total Feature Area Fraction
Micrograph Size Micrograph Area
Area (𝝁𝒎𝟐 ) (%)
(𝝁𝒎𝟐 ) (𝝁𝒎𝟐 )
001 11.047 1391.9 56623.7 2.4582
002 9.2697 973.31 56623.7 1.7189
003 10.039 1044.1 56623.7 1.8439
004 10.808 1232.1 56623.7 2.1760
005 8.3959 1091.5 56623.7 1.9276
Note: A pixel/micron conversion factor was entered into the program using the scale on the BSE
micrographs. This conversion is not necessary for calculation of area fraction but can be done
easily if it is preferred.

Table 3: Average area fraction and relevant statistics.

Mean Fraction
Standard 95% Confidence Relative Volume Fraction
over all Fields
Deviation (%) Interval (%) Accuracy (%) (%)
(%)
2.0249 0.22 0.26895 13.282 2.02 ± 0.27
Note: Because of the low volume fraction and low sampling number, the standard deviation,
confidence interval, and relative accuracy do not accurately represent the data as it does not
follow a Gaussian distribution.

Figure 1 is an example of a micrograph set to a threshold with aim to turn the inclusions black
without shrinking or enlarging them.

(a) (b)
Figure 1: (a) Original BSE micrograph and (b) thresholded BSE micrograph.

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3.2 Manual Point Count

The LANL group performed a grid point intercept method using the standard test method ASTM
E562-11, Determining Volume Fraction by Systematic Manual Point Count, [2011ast].

The square grid provided in the standard method was made transparent and regularly arranged
over an image for a total of 725 grid points. A point was counted when it fell within an inclusion.
When a point landed on the boundary of an inclusion, only one half a count was added to the
total. Note, the very centers of the crosshairs are what is used to determine counts; the crosshair
is only there for visual assistance. Care was taken to ignore any dust. The counts were summed
and divided by 725 (the number of grid points). This process was repeated for each micrograph
and the average over all five of the micrographs was the estimate for the final volume fraction
percentage (Table 5).

Table 4: Point interception counts using 725-point grid for each micrograph.
Counted Points
Micrograph Counted Points Total Points on Grid
Fraction (%)
001 23 725 3.17
002 15.5 725 2.14
003 14.5 725 2
004 15.5 725 2.14
005 13 725 1.79

Table 5: Average point count fraction and final volume fraction calculation using a 725-
point grid
Mean Fraction
Standard 95% Confidence Relative Volume Fraction
Over All Fields
Deviation (%) Interval (%) Accuracy (%) (%)
(%)
2.25 0.54 0.66 29.5 2.25 ± 0.66
Note: Because of the low volume fraction and low sampling number, the standard deviation,
confidence interval, and relative accuracy do not accurately represent the data as it does not
follow a Gaussian distribution.

Figure 2 is an example of the grid systematically arranged over one of the micrographs for a total
of 725 points.

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Figure 2: 725 points placed over micrograph 001. Grid taken from ASTM E562-11 [2011ast].

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4.0 DISCUSSION

The mean volume fraction of the five micrographs reported by the manual point count method
(2.25 ± 0.66 %) was higher than that reported by the automatic image analysis method (2.02 ±
0.27 %). The 95% confidence interval was calculated using 95% 𝐶𝐼 𝑡 , where 𝑠 is the
√
standard deviation, 𝑛 5 is the number of fields (micrographs), and 𝑡 2.776 is the 95%
confidence interval multiplier. The number of fields 𝑛 is smaller than what is typically
recommended for any sampling as it corresponds to a larger 95% confidence interval. It must be
noted that the distribution of the inclusion volume fraction measurements among the fields does
not necessarily follow a normal distribution, so the arithmetic standard deviations, confidence
intervals, and relative accuracies do not accurately describe the data [1970moo, 1980voo,
2004gok]. These calculations are still included for comparative purposes. In determining the
inclusion content of a steel, G. A. Moore used a four-moment calculation method in which the
distribution of the averages approaches normality [1976moo]. This method is not covered here
but is explained in 1980voo.

The ASTM method for manual point counting instructs avoiding adjacent grid points falling on
the same inclusion. This step was compromised minimally in the execution above as a higher
grid point density was desired because of the low volume fraction and low number of fields.
Allowing multiple points to land on the same feature results in a more complex sampling
variance between fields because of the redundancy in point counts but may be the necessary
thing to do if the inclusions vary in size or are non-spherical [1961hil]. The automatic analysis
method uses a dense grid comprised of pixels with multiple pixels falling on one constituent but
gives a higher level of validity and the time taken for the computer to count the pixels is
unnoticed. The manual method resulting in a wider confidence interval (assuming a normal
distribution) could be because the counting is done in ½ integer increments and the resulting
fraction will always be a larger overestimation or underestimation than the fraction of thousands
of pixels.

The variability in measurements like the ones done here comes from the composition and
structure of the material, statistical variances inherent to the measurement method, and human
bias in the measurements [1970moo]. The following is a list of errors and biases possible in these
measurement methods:

i. Bias in choosing which sections and fields are to be representative of a material.

ii. Misinterpretation of steps associated with the manual point count method resulting in a
higher volume fraction estimate:
a. Counting a whole point as opposed to one half when a point lands on the
boundary of an inclusion.
b. Making a count when any part of the crosshair intersects an inclusion instead
of just using the center.
iii. Visual judgment and bias in the determination of where a grid point has landed and in the
automatic method, the threshold that will represent the presence of inclusions. When
thresholding, some features may be either lost or exaggerated in size because of
variations in shading in the original image. Different persons may also threshold
differently according to how they see fit.

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As the results from most of the labs agreed, it was not necessary to redo the measurements with
more fields.

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5.0 CONCLUSION

The manual point count method, ASTM E562-11, resulted in an inclusion volume fraction
estimate of 2.25 ± 0.66 % while the automatic analysis method, ASTM E1245-03, resulted in
2.02 ± 0.27 %. The estimates fell within the 95% confidence intervals of the other.

The automatic method, ASTM E1245-03, resulted in a tighter 95% confidence interval, took less
time, and was less tedious and strenuous on the eyes than the manual method.

The following recommendations are made:

1. The use of ASTM E1245-03, Determining the Inclusion or Second-Phase Constituent

Content of Metals by Automatic Image Analysis [2016ast] is recommended for
estimating the inclusion content in a material instead of ASTM E562-11, Determining
Volume Fraction by Systematic Manual Point Count, [2011ast]. To follow the automatic
method, a software than can threshold an image and give a ratio of pixels is necessary.
Fiji is an example of a free, open source image processing program that can do these
processes and more.
2. A magnification should be chosen such that the field size is maximized and all of the
inclusions are clearly resolved. The automatic method works best when there is little
doubt on whether an inclusion is present or not. However, the higher the magnification
chosen the higher the field to field variability will be and the amount of fields necessary
to cover the same area is increased.

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6.0 ACKNOWLEDGEMENTS

This work is supported by the U.S. Department of Energy/National Nuclear Security

Administration’s M3 Reactor Conversion Program. Los Alamos National Laboratory, and
affirmative action equal opportunity employer, is operated by Los Alamos National Security,
LLC for DOE/NNSA under contract DE-AC52-06NA25396.

7.0 REFERENCES

1947how Howard, R. T., and Cohen, M., Quantitative Metallography by Point-Counting and
Lineal Analysis, Transactions AIME, Vol 172, 1947, pp. 413–426.
1961hil Hilliard, J. E., and Cahn, J.W., An Evaluation of Procedures in Quantitative
Metallography for Volume-Fraction Analysis, Transactions AIME, Vol 221, 1961,
pp. 344-352
1970moo Moore, G.A. Is Quantitative Metallography Quantitative? Applications of Modern
Metallographic Techniques, ASTM STP 480, American Society for Testing and
Materials, 1970, pp.3-48.
1976moo Moore, G.A. Automated Measurements for Determination of the Statistical Nature of
the Distribution of Inclusions in Steel, Fourth International Congress for Stereology:
proceedings of the fourth International Congress for Stereology held at the National
Bureau of Standards. Washington, D.C.: U.S. Dept. of Commerce, National Bureau
of Standards. 1976.
1998van Vander Voort, G., Inclusion measurement by ASTM E 1245. 1998. CIM Bulletin. 91.
104-106.
2004gok Gokhale, A.M., Quantitative Characterization and Representation of Global
Microstructural Geometry. Georgia Institute of Technology, Metallography and
Microstructures, Vol. 9, ASM Handbook, ASM International, 2004, pp. 428-447
2011ast ASTM Standard E562-11, Standard Test Method for Determining Volume Fraction
by Systematic Manual Point Count, ASTM International, West Conshohocken, PA,
2011, DOI: 10.1520/E0562-11.
2012sch Schindelin, J.; Arganda-Carreras, I. & Frise, E. et al. (2012), "Fiji: an open-source
platform for biological-image analysis", Nature methods 9(7): 676-682, PMID
22743772, doi:10.1038/nmeth.2019 (on Google Scholar).
2015pab W. Pabst, E. Gregorová and T. Uhlířová, Microstructure characterization via
stereological relations — A shortcut for beginners. Materials Characterization 105,
2015, 1-12.
2016ast ASTM E1245-03(2016), Standard Practice for Determining the Inclusion or Second-
Phase Constituent Content of Metals by Automatic Image Analysis, ASTM
International, West Conshohocken, PA, 2016, DOI: 10.1520/E1245-03R16.

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