This international standard was developed in accordance with internationally recognized principles on standardization established in the Decision on Principles

for the
Development of International Standards, Guides and Recommendations issued by the World Trade Organization Technical Barriers to Trade (TBT) Committee.

Designation: C1871 − 22

Standard Test Method for

Determination of Uranium Isotopic Composition by the
Double Spike Method Using a Thermal Ionization Mass
Spectrometer1
This standard is issued under the fixed designation C1871; the number immediately following the designation indicates the year of
original adoption or, in the case of revision, the year of last revision. A number in parentheses indicates the year of last reapproval. A
superscript epsilon (´) indicates an editorial change since the last revision or reapproval.

1. Scope ments of low enriched or natural uranium isotopic reference

1.1 This test method describes the determination of the
isotope amount ratios of uranium material as nitrate solutions
by the double spike (DS) method using a thermal ionization
mass spectrometer (TIMS) instrument.
1.2 The analytical performance in the determination of the
235
U/238U major isotope amount ratio by the DS method is five
to ten times better in terms of the internal and external
reproducibility compared to the (“classical”) total evaporation
(TE) method as described in Test Method C1672 and the
“modified total evaporation” (MTE) as described in Test
Method C1832. This is due to the use of an internal rather than
external mass fractionation correction by using a double spike
material with a known or certified 233U/236U isotope ratio,
which is mixed with the sample prior to the measurement,
either during the sample preparation or directly on the TIMS
filament.
1.3 The DS method cannot be applied for the determination
of the 236U/238U minor isotope amount ratio, and is also not
recommended for the determination of the 234U/238U minor
isotope amount ratio.
1.4 In case the uranium amount concentration of the double
spike is known or certified, the uranium amount concentration
of the sample can be determined using the isotope dilution
mass spectrometry (IDMS) method as described in Test
Method C1672, by blending the sample gravimetrically with
the double spike and performing a DS measurement.
1.5 An external mass fractionation correction by measure-
ments of a certified reference material loaded on different
filaments and measured in the same measurement sequence, as
recommended for TE and required for MTE measurements, is
not necessary for the DS method. However, for quality control
(QC) purposes it is recommended to perform DS measure-
1
This test method is under the jurisdiction of ASTM Committee C26 on Nuclear
Fuel Cycle and is the direct responsibility of Subcommittee C26.05 on Methods of
Test.
Current edition approved Feb. 1, 2022. Published March 2022. Originally
approved in 2018. Last previous edition approved in 2018 as C1871 – 18a. DOI:
10.1520/C1871-22.
materials on a regular basis.
1.6 The DS method can only be applied to uranium samples
with relative isotope abundances 233U/U below 10–5 and
236
U/U below 5 × 10–4, the DS method is therefore mainly used
for low enriched or close to natural uranium samples.
1.7 Units—The values stated in SI units are to be regarded
as the standard. When no SI units are provided, the values are
for information only.
1.8 This standard does not purport to address all of the
safety concerns, if any, associated with its use. It is the
responsibility of the user of this standard to establish appro-
priate safety, health, and environmental practices and deter-
mine the applicability of regulatory limitations prior to use.
1.9 This international standard was developed in accor-
dance with internationally recognized principles on standard-
ization established in the Decision on Principles for the
Development of International Standards, Guides and Recom-
mendations issued by the World Trade Organization Technical
Barriers to Trade (TBT) Committee.
2. Referenced Documents
2.1 ASTM Standards:2
C753 Specification for Nuclear-Grade, Sinterable Uranium
Dioxide Powder
C776 Specification for Sintered Uranium Dioxide Pellets for
Light Water Reactors
C787 Specification for Uranium Hexafluoride for Enrich-
ment
C833 Specification for Sintered (Uranium-Plutonium) Diox-
ide Pellets for Light Water Reactors
C859 Terminology Relating to Nuclear Materials
C967 Specification for Uranium Ore Concentrate
C996 Specification for Uranium Hexafluoride Enriched to
Less Than 5 % 235U
2
For referenced ASTM standards, visit the ASTM website, www.astm.org, or
contact ASTM Customer Service at service@astm.org. For Annual Book of ASTM
Standards volume information, refer to the standard’s Document Summary page on
the ASTM website.

Copyright © ASTM International, 100 Barr Harbor Drive, PO Box C700, West Conshohocken, PA 19428-2959. United States

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

1
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22
C1008 Specification for Sintered (Uranium-Plutonium)
DioxidePellets—Fast Reactor Fuel (Withdrawn 2014)3
C1068 Guide for Qualification of Measurement Methods by
a Laboratory Within the Nuclear Industry
C1128 Guide for Preparation of Working Reference Materi-
als for Use in Analysis of Nuclear Fuel Cycle Materials
C1156 Guide for Establishing Calibration for a Measure-
ment Method Used to Analyze Nuclear Fuel Cycle Mate-
rials
C1347 Practice for Preparation and Dissolution of Uranium
Materials for Analysis
C1411 Practice for The Ion Exchange Separation of Ura-
nium and Plutonium Prior to Isotopic Analysis
C1672 Test Method for Determination of Uranium or Pluto-
nium Isotopic Composition or Concentration by the Total
Evaporation Method Using a Thermal Ionization Mass
Spectrometer
C1832 Test Method for Determination of Uranium Isotopic
Composition by Modified Total Evaporation (MTE)
Method Using Thermal Ionization Mass Spectrometer
D1193 Specification for Reagent Water
E2586 Practice for Calculating and Using Basic Statistics
E2655 Guide for Reporting Uncertainty of Test Results and
Use of the Term Measurement Uncertainty in ASTM Test
Methods
3. Terminology
3.1 Terminology C859 contains terms, definitions, descrip-
tions of terms, nomenclature, and explanations of acronyms
and symbols specifically associated with standards under the
jurisdiction of Committee C26 on Nuclear Fuel Cycle.
3.2 Definitions:
3.2.1 abundance sensitivity, n—in isotope amount ratio
measurements, the ratio of the measured intensity of an ion
beam at a mass, m, to the measured intensity from the same
isotope measured at one mass unit difference (for example, m
6 1).
3.2.1.1 Discussion—Abundance sensitivity is a measure of
the magnitude of the peak tailing correction. For measuring
uranium on thermal ionization mass spectrometer (TIMS) and
inductively coupled plasma mass spectrometry (ICP-MS)
instruments, the abundance sensitivity is typically calculated as
the ratio of the measured signal intensities at masses 237 and
238 using a suitable uranium sample.
3.2.2 modified total evaporation, MTE, n—analytical
method for determination of isotope amount ratios of uranium,
as described in Test Method C1832.
3.2.3 total evaporation, TE, n—analytical method for deter-
mination of isotope amount ratios of uranium or plutonium, as
described in Test Method C1672, also called “classical” total
evaporation in this test method.
3.2.4 turret, n—holder for sample filaments.
3.2.4.1 Discussion—Alternate names for turret are carousel,
magazine, and wheel.
3
The last approved version of this historical standard is referenced on
www.astm.org.
&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07
2
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
3.3 Acronyms:
3.3.1 CRM—certified reference material
3.3.2 DS—double spike
3.3.3 DU—depleted uranium
3.3.4 EU—European Union
3.3.5 FAR—Faraday Cup
3.3.6 HEU—high enriched uranium
3.3.7 IAEA—International Atomic Energy Agency
3.3.8 ICPMS—inductively coupled mass spectrometry
3.3.9 IRMM—Institute for Reference Materials and Mea-
surements (since 1 July 2016 called JRC-Geel, the only unit
working with nuclear materials at JRC-Geel is JRC-G.2)
3.3.10 ITU—Institute for Transuranium Elements (since 1
July 2016 called JRC-Karlsruhe, the only unit involved with
thermal ionization mass spectrometry measurements of nuclear
materials at JRC-Karlsruhe is JRC-G.II.6)
3.3.11 JRC—Joint Research Centre
3.3.12 LEU—low enriched uranium
3.3.13 MTE—modified total evaporation
3.3.14 NBL—New Brunswick Laboratory (since 15 May
2016 called NBL-Program Office)
3.3.15 NML—Nuclear Material Laboratory (part of the
IAEA)
3.3.16 QC—quality control
3.3.17 RSD—relative standard deviation—SD (see below)
divided by the mean value of the observations in repeated
sampling.
3.3.18 RSE—relative standard error—SE (see below) di-
vided by the mean value of the observations in repeated
sampling.
3.3.19 SD—standard deviation—according to Practice
E2586, 3.1.30: The square root of the sum of the squared
deviations of the observed values in the sample divided by the
sample size minus 1.
3.3.20 SE—standard error—according to Practice E2586,
3.1.29: Standard deviation of the population of values of a
sample statistic (that is, the mean value) in repeated
measurements, or an estimate of it.
3.3.20.1 Discussion—According to Practice E2586, 3.1.30:
If the standard error (SE, see above) of a statistic is estimated,
it will itself be a statistic with some variance that depends on
the sample size, that is, the number of observed values in the
sample (Practice E2586, 3.1.26).
3.3.20.2 Discussion—According to Practice E2655, 5.8.4.1:
From statistical theory, a 95 % confidence interval for the mean
of a normal distribution, given n independent observations x1,
x2, ..., xn drawn from the distribution, is x̄ 6 t × SD / √n, where
x̄ is the sample mean, SD is the standard deviation of the
observations (see above), and t is the 0.975 percentile of the
Student’s t distribution with n-1 degrees of freedom. Because
Student’s t distribution approaches the normal as n increases,
the value of t approaches 1.96 as n increases. This is the basis
for using the (coverage) factor 2 for expanded uncertainty. The
 C1871 − 22
standard error (SE) of the mean value of a series of n
independent repeated measurements can be derived from that
by using t = 1, so the standard error (SE) is given by SD / √n.
3.3.21 TIMS—thermal ionization mass spectrometry
3.3.22 WRM—working reference material
4. Summary of Test Method
4.1 The double spike method has been developed with the
intention to improve the precision and decrease the uncertain-
ties for 235U/238U major isotope ratio measurements compared
to the known methods such as the “classical” total evaporation
technique (1-4),4 also described in Test Method C1672, and the
modified total evaporation technique (5 and 6), also described
in Test Method C1832. For the double spike method the mass
fractionation correction for the 235U/238U ratio is performed
internally throughout the measurement rather than externally,
by using the mass fractionation observed for a double spike
material with a known or certified 233U/236U isotope ratio (also
spanning three mass units), which is mixed with the sample
prior to the measurement, either during the sample preparation
or directly on the TIMS filament. If necessary, uranium is
separated from plutonium and other elements (to eliminate
isobaric interferences) by selective extraction, anion exchange
(see Practice C1411), or extraction chromatography. The puri-
fied uranium fraction as nitrate solution is loaded onto an
evaporation filament (made of metals such as rhenium, zone-
refined rhenium, or tungsten with high evaporation
temperature), and blended with an appropriate amount of
double spike solution, and converted to an oxide by controlled
heating of the filament under atmospheric conditions. In case
only the 235U/238U ratio of the sample has to be determined, it
is recommended to mix the sample with the double spike
during the loading process on the filament. In case the uranium
amount concentration of the sample has to be determined, the
sample solution has to be blended gravimetrically with the
double spike solution prior to filament loading, for which
weighable amounts have to be used.
4.2 The sample amount to be loaded for DS analyses is
within a range of about 4 to 6 µg to achieve ion beam signals
of about 20 to 30 V for the major isotope 238U for DU, NU, and
LEU samples.
4.3 The 235U/238U isotope amount ratios are corrected for
mass fractionation for each integration step individually. This
is accomplished in an internal manner, the magnitude of the
mass fractionation is calculated from the measured mass
fractionation of the 233U/236U ratio. The peak tailing contribu-
tions are determined at two mass positions, 0.5 mass units
below and 0.5 mass units above the isotope masses of interest.
4.4 For the correction of isobaric interferences, a separate
measurement of the isotopic composition of the (unspiked)
sample is required, unless this information is already available.
4
The boldface numbers in parentheses refer to a list of references at the end of
this standard.
&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07
3
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
This measurement can be performed using the TE or MTE
methods (Test Methods C1672 and C1832, respectively).
5. Significance and Use
5.1 Uranium material is used as a fuel in certain types of
nuclear reactors. To be suitable for use as nuclear fuel, the
starting material shall meet certain specifications such as those
described in Specifications C753, C776, C787, C833, C967,
C996, and C1008, or as specified by the purchaser. The
235
U/238U isotope amount ratios and the amount content of
uranium material can be measured by mass spectrometry
following this test method to ensure that they meet the
specification.
5.2 The double spike method has been used for studies of
uranium fractionation effects in isotope geochemistry and
cosmochemistry, for uranium source attribution in nuclear
forensics and for investigation of conversion or sampling
processes in nuclear industry and nuclear safeguards (7-11).
Most recently, the double spike method has been used for the
validation of the Cristallini sampling method of UF6 (12 and
13). The double spike method can be used for a wide range of
sample sizes even in samples containing as low as 50 µg of
uranium. The concentration of the loading solution for the DS
method has to be in the range of 1 to 6 mg/g to allow a sample
loading of 4 to 6 µg of uranium. A minimum loading of 4 µg
uranium per filament is recommended.
5.3 The measurement of 236U/238U ratios using this method
is not possible due to the large isobaric interference from the
236
U ion beam of the double spike onto the 236U ion beam from
the sample (>50.000 times for close to natural material, for
example, like IRMM-184).
5.4 The application of the double spike method for mea-
surements of 235U/238U ratio is limited by the isobaric inter-
ference between the 236U from the double spike material and
the 236U contained in the sample. As a consequence, the
method is not suitable for samples which contain significant
amounts of 236U due to prior neutron capture from 235U in the
predecessor materials. For samples with 236U/238U ratios
higher than about 10–6, the double spike method should be
applied with care for the isobaric correction. For an appropriate
isobaric correction, the 236U/238U ratios of the samples should
be determined separately using a suitable measurement
method, for example, the modified total evaporation MTE
method (Test Method C1832, Ref (5) and (6)).
5.5 The measurement of 234U/238U ratios using this method
is very limited in the analytical performance due to the isobaric
interference of the 234U from the double spike with the 234U
from the sample (range from 5 to 15 %). The correction
algorithms are presented in 14.3, but statements for precision
and bias are not given. Other methods like MTE (Test Method
C1832, Ref (5) and (6)) are better suited and more reliable for
measurements of 234U/238U ratios.
5.6 The DS method described here can also be extended to
measurement of elements other than uranium, if a suitable
double spike material is available.
 C1871 − 22
6. Interferences
238
6.1 Isobaric nuclides such as Pu interfere in the uranium
measurements. The removal of interferences is generally ac-
complished by chemical separation leading to ionization of
uranium only and improved precision of measured isotope
amount ratios.
6.2 For the isotopes 234U, 235U, 236U, and 238U isobaric
interferences between the sample and the double spike occur.
The accurate correction of isobaric interferences is a prerequi-
site for obtaining results for the DS method with satisfactory
precision and accuracy. The corrections depend strongly on the
mixing proportions between the sample and the double spike.
Usually the sample/spike amount ratio is adjusted in such a
manner that the ion beam intensity at mass m/z=236 is lower
compared to that at mass m/z=235, in order to reduce the
influences from low-mass tailings, that is, abundance
sensitivities, at one mass unit below and beyond the U peaks.
Therefore a sample-to-spike amount ratio of >20 is recom-
mended. The correction of isobaric interferences is explained
in detail in Section 14 (“calculations”) of this test method.
6.3 It has to be ensured that samples are not contaminated
by environmental uranium. The level of effort required to
minimize contamination shall be based upon the sample size
and the levels of contamination present in the analytical
facility. For extremely small samples or extremely low 236U
abundances, residual uranium from chemicals used for sample
dissolution and sample preparation is possible source for bias
in the isotopic data.
6.4 Samples shall be chemically purified to assure reliable
analyses by TIMS. Impurities, especially alkali elements,
produce unstable ion emission leading to poor precision in the
isotope amount ratios. Organic contaminants or oxide layers on
the filaments also adversely influence TIMS analyses. Isobaric
interferences, if not removed, will bias the isotope amount
ratios. Contaminants in reagents, lab ware, or filament material
are also sources for bias in the isotope amount ratios.
6.5 The performance of the instrument can be adversely
affected by changes in the environmental conditions of the
laboratory, that is, temperature and humidity. For this reason,
controlled laboratory environmental conditions should be
maintained (within the manufacturer’s specifications) during
instrument operation.
7. Apparatus
7.1 The suitability of the mass spectrometer for carrying out
measurements by the DS method shall be evaluated by means
of performance tests. The relevant instrument characteristics
are as follows:
7.1.1 A thermal ionization source for using single, double,
or triple filament assemblies with rhenium or tungsten
filaments, or both;
7.1.2 A mass analyzer sufficient to resolve adjacent masses
in the mass-to-charge range being studied, m/z = 233 to 238 for
U+. Resolution shall be greater than 350 (full width at 1 % of
peak height) and the abundance sensitivity at mass 237 for ions
of 238U less than 8 × 10–6;
&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07
4
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
7.1.3 A multiple Faraday collector system to allow simulta-
neous detection of isotope beams from m/z = 233 to 238 for U+
ions;
7.1.4 For the Faraday cups used to measure the major ion
beams of 235U and 238U, there shall be current amplifiers
equipped with 1011 Ω resistors and, for the ion beams of 233U
and 236U, there shall be current amplifiers equipped with at
least 1011 Ω, and preferably 1012 Ω resistors to improve the
signal-to-noise ratio. In case the ion beam of 235U is below the
ion beams of 233U and 236U, the use of an amplifier equipped
with a 1012 Ω resistor is recommended, if available.
7.1.5 A sample turret to allow automatic measurement
sequences of several replicate filament loadings per sample and
per quality control standard (preferentially a CRM);
7.1.6 A pumping system that is able to attain a vacuum of
<4.0 × 10–5 Pa (3 × 10–7 torr) in the ion source, the analyzer,
and the detector is required. Tailing corrections are dependent
on the vacuum levels inside the mass spectrometer. Analyzer
pressures below 7.0 × 10–7 Pa (5 × 10–9 torr) are preferred;
7.1.7 A mechanism to scan masses by varying the magnetic
field or the accelerating voltage or both;
7.1.8 A computer for control of the data acquisition accord-
ing to a predefined sequence.
7.2 Special MTE Capabilities—It is recommended to have a
mass spectrometer software to be flexible enough to implement
a user-defined filament-heating program as for MTE.5
7.3 A separate filament degassing device for cleaning of the
filaments before sample loading can be used.
7.4 A pipette or microsyringe to transfer microliter volumes
of solution.
7.5 A separate filament heating device for drying and
oxidizing the sample on the filament ribbon after loading.
8. Reagents and Materials
8.1 Purity of Reagents—Ultra-high purity reagents shall be
used for processing small sample amounts or samples with
extremely small isotope amount ratios. The level of uranium
contamination from chemicals, water, and the sample handling
environments shall be determined to ensure that the materials
and the environment are sufficiently pure for the samples being
analyzed.
8.2 Nitric Acid (HNO3, 15.8 M)—Concentrated nitric acid.
8.3 Nitric Acid (HNO3, 1 M)—One volume of concentrated
nitric acid (HNO3, 15.8 M) brought to 15.8 volumes with
water.
8.4 Purity of Water—Unless otherwise indicated, references
to water shall be understood to mean laboratory accepted
demineralized or deionized water as described by Type I of
Specification D1193.
5
The sole source of supply of the apparatus known to the committee at this time
is Thermo Fisher Scientific Inc., 81 Wyman St., Waltham, MA 02451. If you are
aware of alternative suppliers, please provide this information to ASTM Interna-
tional Headquarters. Your comments will receive careful consideration at a meeting
of the responsible technical committee,1 which you may attend.
 C1871 − 22
8.5 Filaments—Filaments with sufficient purity, for
example, zone refined or high purity Re or W, should be used.
The size and configuration of the filament is instrument
dependent.
8.6 Liquid Nitrogen—Liquid nitrogen can be filled into the
cold trap of a mass spectrometer to improve the vacuum
pressure.
9. Hazards
9.1 TIMS instruments operate at 8 to 10 kV electrical
potential. Ensure that the high-voltage is switched off before
insertion or removal of the sample turret into/from the
instrument, and working with the ion source, or accessing other
electronic components.
9.2 The filaments reach temperatures in excess of 2000 °C.
The filament holders, sample wheel, and ion sources parts are
expected to be hot. Ensure that a sufficient time has lapsed
since the last filament heating before accessing the filaments,
sample turrets, and ion source.
9.3 Wear eye protection and suitable gloves when filling
cold traps with liquid nitrogen. Protect hands, torso, and feet in
the event of splashing or spilling of the liquid nitrogen.
9.4 Handle radioactive materials with appropriate attention
to radiological safety.
9.5 Handle chemical hazards and toxins like uranium with
appropriate care.
10. Sampling, Test Specimens, and Test Units
10.1 Isotope Reference Materials—Uranium reference ma-
terials used in the analysis should be prepared from certified
reference materials (CRMs) traceable to SI units. Examples
include the Double Spikes IRMM-3636 (1 mg U/g), IRMM-
3636a (0.1 mg U/g), and IRMM-3636b (0.01 mg U/g), which
all have the same isotopic composition (uncertainties with
coverage factor k = 2, 95 % confidence level):
233
U/236U = 1.01906(16),
234
U/236U = 0.00036606(48),
235
238
U/236U = 0.000045480(74), and
U/236U = 0.00023481(38).
In addition, various in-house double spike materials are
being used at numerous facilities, which have been calibrated
using isotope reference materials, like NBL CRM U500
(235U/238U > 1) or IRMM-184 (close to natural U). For the
preparation of in-house double spike reference materials, see
Guide C1128 for additional guidance on preparation of trace-
able working reference materials.
10.2 Uranium samples to be measured and isotope reference
materials used for quality control purposes shall be in the same
medium, same concentration and in the same oxidation state.
The solutions for loading onto the filaments are usually 1 to 5
M nitric acid solutions. The loading and drying sequence of the
filaments shall also be similar.
10.3 In the case of characterization studies of test materials,
possible inhomogeneity between test units shall be evaluated
statistically and included in the uncertainty calculations of the
isotope amount ratios assigned.
&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07
5
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
11. Preparation of Apparatus
11.1 Filament Degassing—Filaments can be degassed be-
fore using them for DS measurements. This is recommended in
case the heating of the filaments during the mass spectrometric
measurement is causing the vacuum pressure in the ion source
to increase beyond 1.3 × 10–4 Pa (1 × 10–6 torr) is reached.
Recommended filament currents for degassing are in the range
4.0 to 5.0 A, corresponding to temperatures in the range of
1700 to 2000 °C. Perform the degassing for a duration of at
least 30 min.
11.2 “Initialization” of the Sample Turret—Adjust, if
needed, the position of the sample turret in the ion source and
verify proper electrical connections for both the evaporation
and ionization filament for each sample loading position. It
shall be ensured that the electrical contact is not interrupted in
case the turret is slightly moved for the purpose of ion beam
focusing.
11.3 Electronics Test—Modern mass spectrometric instru-
ments offer an automated routine for testing the stability and
performance of the electronic systems (for example, Faraday
cup amplifier baselines and gains, high-voltage unit, and
magnet current supply units). A report is produced flagging
systems or components that are out of specification. Users of
the instruments should perform routine checks of the perfor-
mance of the electronic systems and ensure that the perfor-
mance is within manufacturer’s specifications. The frequency
for this test shall be established by the user based on manu-
facturer recommendations or as specified in the user’s quality
assurance program.
11.4 Amplifier Signal Decay Adjustment—Adjust the signal
decay characteristics of the current amplifiers of the Faraday
cups. This is important for measuring isotope amount ratios
with a large dynamic range, high precision and accuracy, or
both. Depending on the combination of the capacitance and
resistance of the current amplifier, the response time for a
sudden change in the ion beam signal to the Faraday cup can
reach up to 5 s. For amplifier resistances higher than the 1011
Ω, longer response times of about 15 s can be expected. The
DS method has to be designed by taking into consideration the
required response times. The amplifier response can be
checked either using a custom-made software module within
the operating software (when available), or “manually” by
means of a large ion beam that is abruptly directed into a
Faraday cup to check the signal ingrowth time, or away from
a Faraday cup (for example, by closing a valve between ion
source and analyzer) to check the signal decay time.
11.5 Ion Source and Analyzer Pressure—It is important to
achieve a certain level of vacuum before the isotope amount
ratio measurements can be started; see 7.1.6 for the recom-
mended pressure. The peak tailing depends strongly on the
vacuum pressure in the detector system since the number of ion
collisions with gas molecules inside the mass spectrometer is a
direct function of the ambient pressure. An increase of the
pressure within the ion source caused by the heating of the
ionization and evaporation filaments can be subdued, to a
certain extent, by using a cold trap filled with liquid nitrogen.
 C1871 − 22
12. Calibration and Standardization
NOTE 1—The measurement method may be qualified following Guide
C1068 and calibrated following Guide C1156.
12.1 Mass Calibration—The relationship between the
known atomic masses and the magnetic field necessary to
direct the isotope beams into the detectors shall be updated on
a regular basis. Mass calibration shall be performed at intervals
specified by the manufacturer or the user’s quality assurance
program.
12.2 Peak Centering—The peak centering routine is used as
a fine adjustment to ensure that the ion beam is centered within
the detector. Peak centering usually occurs via fine adjustments
of the accelerating voltage, and any difference between the
value optimized during peak centering from the default accel-
erating voltage requires a readjustment of the mass calibration
curve. Peak centering shall be performed for at least at three
uranium masses as part of the mass calibration before the start
of each DS measurement sequence. During the DS
measurement, peak centering is performed on a regular basis.
12.3 Amplifier Baseline Calibration—The baselines of the
Faraday cup amplifiers, that is, the amplifier responses without
incoming ion beam to the cup, shall be measured on a regular
basis and checked for stability. During the DS measurements,
baseline measurements are performed on a regular basis. Note
that the integration time for the baseline measurement has a
significant influence on the uncertainty of Faraday cup
measurements, particularly at lower ion beam intensities.
Therefore, the integration time of the baseline (within a
measurement) shall be comparable to the integration time of
the actual ion beam signal integration. The long-term historical
baseline data shall be regularly reviewed by the user to assure
that the system performance is within manufacturer specifica-
tions and quality system requirements.
12.4 Amplifier Gain Calibration—The stability and re-
sponse of individual Faraday detector amplifiers shall be
measured and differences between amplifiers corrected for via
the amplifier gain calibration. Gain calibration is normally
performed by sequentially applying a stable calibration current
to the input of each Faraday cup amplifier and the output is
then normalized to a reference value to generate a gain
calibration factor for each amplifier. A gain calibration shall be
performed prior to each automatic DS sequence. Historical
gain calibration data can be used to evaluate the stability of the
amplifiers.
12.5 Faraday Cup Effıciency Test—The response of indi-
vidual Faraday cups depends on several factors, for example,
extent of usage, manufacturing variability, and can also be
affected by an insufficient electron suppression voltage. The
relative response of the Faraday cups, therefore, shall be
determined periodically. Usually, the Faraday cups of a multi-
collector system are only intercalibrated for the current ampli-
fiers connected to them (see 12.4) but not for the differences in
the efficiencies of the Faraday cups themselves. The efficien-
cies of the Faraday cups are expected to be similar to each
other, which means that the relative efficiencies (relative to one
reference cup) are normally close to unity. Note that an
(electronic) amplifier gain calibration (see 12.4) shall be
&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07
6
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
performed prior to the Faraday cup efficiency test. The Faraday
cup efficiency test can be performed in several ways, as
described in 12.5.1 – 12.5.4.
12.5.1 The calibration may be performed by switching a
stable ion beam of 187Re (from a blank filament) between each
Faraday cup and a reference Faraday cup. In case a relative
efficiency between the detectors is significantly different from
unity, this result can be used to correct for differences in the
detector response. This procedure can be performed with a
relative uncertainty at the level of <0.1 %.
12.5.2 A series of peak-jumping measurements between all
Faraday cups and a reference cup to be checked can also be
performed using a sufficiently large uranium sample and one
large stable ion beam, for example, a 10 to 20 V ion beam of
238
U from a LEU or natural uranium sample. The drift of the
signal intensity shall be corrected for using the operating
software. This procedure can be performed with a relative
uncertainty at the level of <0.01 %.
12.5.3 A series of comparative neodymium (Nd) isotope
amount of ratio measurements can be performed in two
different modes such as the multi-dynamic mode and the static
mode with “amplifier rotation” (only for TRITONTM TIMS,
also called “virtual amplifier”: each Faraday cup is connected
to each amplifier for regular time intervals during the measure-
ment). This procedure can be performed with a relative
uncertainty at the level of few ppm (5). It shall be repeated
until all Faraday cups of interest for DS measurements have
been included.
12.5.4 A series of static measurements can be performed
using special “multi-isotope” reference materials, such as
IRMM-3100a (233U/235U/236U/238U=1/1/1/1), IRMM-072/1,
IRMM-074/1, or IRMM-199 (233U/235U/238U=1/1/1), to in-
clude all Faraday cups. This procedure can be performed with
relative uncertainties of about 0.03 %.
12.6 Linearity Test—There are various procedures to check
the linearity of an isotope mass spectrometer detection system.
The procedures described in 12.6.1 and 12.6.2 are mainly
applicable for Faraday multi-collector systems.
12.6.1 The linearity of the mass spectrometer is determined
over the working range of the Faraday cups by measuring the
235
U/238U ratios of various reference materials under identical
conditions. The mass spectrometer system is linear if the K
factor, that is, the ratio of the certified 235U/238U ratio to the
measured 235U/238U ratio, is independent of the isotopic
composition of the material. For this procedure, the NBL
U-series of reference materials (U005a to U970, 0.5 to 97 % of
235
U) is ideal and can be combined with the IRMM-183-187
series (0.3 to 5 % of 235U) and the IRMM 019-029 series (0.17
to 5 % of 235U, to be converted from UF6). This procedure shall
be performed sequentially for all Faraday cups of the multi-
collector system needed for the DS analyses.
12.6.2 The IRMM-072 and IRMM-074 series of reference
materials are characterized by 238U/235U ratios of ≈1 and
233
U/235U ratios ranging from ≈1 down to ≈10–6 for the 15 or
10 units, respectively, of the used series. For each unit, the bias
of the measured 238U/235U ratios from the certified ones can be
used for internal mass fractionation correction of the measured
233
U/235U ratios. The comparison of the corrected 233U/235U

ratios with the certified ones allows the linearity of the
detection system to be checked over a dynamic range of six
orders of magnitude for the ion beam intensity. A detailed
description of the procedure is given in (14). This procedure
shall be performed sequentially for all Faraday cups needed for
the DS analyses.
12.7 Peak Overlap—When a Faraday multi-collector sys-
tem for the simultaneous detection of several masses is used, it
needs to be ensured that the peak overlap is acceptable. A mass
scan, usually by scanning the magnetic field, shall be per-
formed by which all ion beams are simultaneously moved
through the respective cups. The measured intensities for all
detectors shall be plotted versus the mass of a reference
detector to make the peak overlap visible. All peaks shall have
a symmetric shape with a common flat region in the center,
with the peak centers reasonably close together, as specified by
the manufacturer or the user quality system. After a satisfactory
peak overlap is realized (by moving cups relative to one
another if necessary), the positions of all detectors shall be
saved, for example, as a Faraday cup configuration file. The
positions shall be checked and possibly readjusted, manually or
using stepping motors, as needed before a new automatic
measurement sequence.
12.8 Mass Fractionation Correction:
12.8.1 For the double spike method the mass fractionation
correction for the 235U/238U ratio is performed for each
integration step (called “mass cycle,” see below) internally
throughout the measurement rather than externally, by using
the mass fractionation observed for a double spike material
with a known or certified 233U/236U isotope ratio (also span-
ning three mass units).
12.8.2 The mass fractionation correction factor, K, is calcu-
lated as follows:
K 5 ~ R c ⁄ R m!
where:
K = mass fractionation correction factor,
Rm = measured 233U/236U isotope amount ratio for the
double spike, and
Rc = known or certified 233U/236U isotope amount ratio
value for the double spike.
Details about the mass fractionation and further correction
algorithms are presented in 14.2.
13. Procedure
13.1 Sample Preparation:
13.1.1 Sample Dissolution—Dissolve an appropriate sample
amount to obtain the desired filament loading solution for the
mass spectrometric analysis. See Practice C1347 for the
dissolution of uranium.
13.1.2 Prepare the sample and any reference material solu-
tions as purified nitrates, using identical chemical preparation
and handling steps. For uranium samples hydrolyzed from
uranium hexafluoride, it is recommended that the samples are
converted to U3O8 before dissolution in nitric acid and analy-
sis. The solution concentrations shall be chosen to allow for a
convenient filament loading (for example, a 2-mg U/mL
solution yields 2 µg of uranium per µL, see also 13.2).
&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
C1871 − 22
13.1.3 Sample Purification—Use Practice C1411 or similar
procedure to separate uranium from plutonium and other
impurities, if necessary.
13.2 Sample Loading and Conditioning—Samples for the
DS method are usually directly loaded on the filament by drop
deposition. Samples and QC materials shall be prepared for
analysis by the same method at similar mass loadings. Drop
deposition onto the filament can be accomplished with the use
of a microsyringe or pipette fitted with a plastic tip. Change the
tip between sample loadings to prevent cross contamination. In
particular for loading and mixing a sample solution and the
double spike solution on the same filament, cross contamina-
tion between these solutions has to be prevented by changing
pipette tips. It is recommended to load the double spike
solution first and the sample afterwards in order to minimize
the risk of contaminating the double spike solution with any
sample material. For filaments loaded by drop deposition, the
solution shall be evaporated by passing sufficient electrical
current through the filament to cause gentle drying without
boiling. Samples for DS are usually prepared in a 1 to 5 M
nitric acid with a uranium concentration between 1 to 6 mg/g,
which is equivalent to 1 to 6 µg/µL. Depending on the uranium
amount to be loaded, more than 1 µL of the sample solution
may be needed. The recommended uranium amount for load-
ing is 4 to 6 µg. Deposit drops very carefully and slowly. It is
recommended to keep the filament heated by passing 0.5 to
0.7 A current and depositing 1-µL-drops at a time. After all
drops are loaded, the solution on the filament is heated until
dryness, for at least one more minute, and then heated for
several seconds at a higher current of 1.5 to 2.0 A for
conditioning. Alternatively, a stepped-heating program can be
used to condition samples, that is, to convert samples to
suitable chemical forms. Avoid quick evaporation of the
sample or melting the filament. At different facilities, different
(1)
loading and conditioning procedures have been established and
validated. Each procedure shall be applied in a consistent
manner for all samples, and quality control samples.
13.3 Mount all sample filaments and ionization filaments on
a sample turret and insert the sample turret into the ion source
of the mass spectrometer.
13.4 Close the source and start evacuating.
13.5 Perform adjustment (also called initialization) of the
sample turret if needed. In case of problems with electrical
connections, the source might have to be vented again to
resolve the problem.
13.6 Evacuate ion source to the manufacturer’s recom-
mended minimum pressure or according to the user’s proce-
dure.
13.7 Add liquid nitrogen to the cold trap if desired.
13.8 Isotope Amount Ratio Measurement—The following
steps 13.8.1 – 13.10 are typically performed automatically
under computer control depending upon the instrument.
13.8.1 Perform an amplifier gain calibration for each new
automatic sequence.
13.8.2 Measure the baseline during the course of each
measurement of a sample and QC standard.
7
 C1871 − 22
13.8.3 Usually under computer control, the ionization fila-
ment is heated up to a temperature of about 1800 to 1950 °C.
For automatic sequences, usually the magnitude of the 187Re
ion beam is used as the regulated quantity instead of the
filament temperature by a pyrometer because only the narrow
sides of the filaments are oriented towards the pyrometer.
Typical 187Re ion beams of about 300 to 600 mV (on a 1011 Ω
resistor) are used for non-zone refined filaments and lower
values of 150 to 400 mV are used for zone-refined filaments,
depending on the thickness and brand.
13.8.4 The 187Re ion beam is peak centered and focused. If
necessary, the 187Re ion beam size is readjusted towards the
target value, which shall be similar (within about 20 %) for
each measurement within an automatic sequence, by changing
the filament current.
13.8.5 The sample filament is heated to a temperature
sufficient to yield and ion beam sum intensity from 235U and
238
U of about 1 to 4 V (on an amplifier with a 1011 Ω resistor).
The beam is focused and peak centered using the largest U ion
beam, which is usually the 238U beam.
13.8.6 Data acquisition is started. The data acquisition is
performed on a per block basis in which each block consists of
a minimum of two and a maximum of five mass cycles and
each mass cycle of (usually) four integration steps. The data
acquisition is usually continued until the whole sample is
evaporated; see 13.10.
13.8.7 DS Mass Cycle—The DS mass cycle consists of four
steps as shown in Table 1. Depending on the ion beam
intensities observed the use of amplifiers with 1012 Ω resistors
is recommended. For the recommended sample-to-spike
amount ratios >20, the 233U and 236U intensities coming from
the double spike shall be detected using amplifiers with 1012 Ω
resistors, if available, in case of depleted samples with low
235
U ion beams this applies as well.
13.8.7.1 The first step is the main integration for all iso-
topes; the integration time is usually about 16 s.
13.8.7.2 In Steps 2 and 3 of the DS mass cycle, the
background intensities at the low and high mass side of all
uranium isotopes of interest are measured. The mutual back-
grounds for 235U and 236U are the most critical ones and
depend a lot on the sample to spike ratio. Due to the differences
in the tailing effect between the low and high mass sides, an
interpolation for the isotope ratios shall be performed, using a
linear approximation.
13.8.7.3 Step 4 is an optional “dummy” step, which might
be needed to move the mass setting back to the main cup
configuration (as in step 1) for checking the ion beam signals
13.9 Interblock Actions and Filament Heating for DS:
13.9.1 Peak Centering and Baseline—Each measurement
block usually consists of a maximum of five mass cycles, with
each cycle having a duration of about 60 to 90 s. Before each
block, a peak centering is performed using the 238U isotope.
Additionally, an ion source focusing is performed before each
block. Typically, every five blocks, the electronic baselines of
all the Faraday cup amplifiers are re-measured. In case 1012 Ω
resistors are used in some of the amplifiers, the idle times for
the baseline measurements have to be sufficiently long, for
example, at least 15 s.
13.9.2 DS Interblock Heating—The DS interblock heating
is recommended to be performed similar to the MTE interblock
heating as described in Test Method C1832. The filament
heating is controlled by a special program script executed after
each measurement block. This program script first measures
the actual sum intensity (mainly from 235U and 238U) and
compares it with the predefined (initial) target sum intensity.
This predefined target sum intensity is typically in the range of
20 to 30 V, selected by the operator depending on the sample
amount loaded, the experience with the ion source and the
instrument transmission. Based on the comparison of the
actually measured sum intensity with the target sum intensity,
the following filament heating step is calculated. A detailed
description of the interblock heating script is given in Test
Method C1832.
13.10 Termination of DS Measurement—The DS measure-
ment is terminated when the sum intensity is below a user-
defined limit of 1 to 2 V.
14. Calculations
14.1 Within this section, the DS data evaluation and calcu-
lation of the various correction factors is discussed. The mass
fractionation correction for the major ratios 235U/238U is
performed internally for each mass cycle throughout the
measurement based on the results of the 233U/236U ratio using
the exponential fractionation law. The differences between
different fractionation laws, for example, power law, exponen-
tial law, linear law, or Rayleigh law are at the level of few parts
per million for heavy elements like uranium, which is insig-
nificant for the DS measurements.
14.2 Evaluation for Major Ratio 235U/238U:
14.2.1 The K factor is derived from the 233U/236U ratio for
each mass cycle:
K5
S D
233

236
U
U DS
(2)
at the very end of each block. This is needed to determine the
ion beam intensity before the next heating step (see 13.9).
S D
233

236
U
U
ME

TABLE 1 Mass Cycle for DS

A A
Cup L2 L1 C (FAR)A H1A H2A Idle Time/
Measurement Time
234 235 236 238
Step 1 U U U 237 u U 12 s/16 s
234 235 236 238
Step 2 U – 0.5 u U – 0.5 u U – 0.5 U – 0.5 u 5 s/8 s
234 235 236 238
Step 3 U + 0.5 u U + 0.5 u U + 0.5 u U + 0.5 u 5 s/8 s
234 235 236 238
Step 4 U U U 237 u U 3 s/1 s
A
The acronyms L2, L1, C (FAR), H1, and H2 indicate the names of the five Faraday cup detectors of the Faraday multi-collector system, which are typically used for DS
measurements.

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

8
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22
where:
ME = measured ratio (not corrected for background and
S D S D S D S SS
238
Ui
238
U ME
5
238
U
233
U DS
233

238
U
U ME
1 2
232.55
233
U D ME

isobaric interferences, for details about the corrections

see below), and S D DD 1
233.55
233
U ME
⁄2 (6)
DS = known ratio of the double spike, preferentially a
certified reference material. Where (238U/233U)DS is the 238U/233U ratio of the double
spike, which can be calculated from the known or certified
14.2.2 The K factor is applied in the following way: (238U/236U)DS and (233U/236U)DS ratios given on the certificate
S D
235

238
U
5 K R235 S D 235
U
238 (3)
using
U CO
U ME
S D 238
U
where:
S D 238
U
5
236
U DS
(7)
CO = corrected ratio, and
ln~ 235 ⁄ 238!
S D
233
U DS
233

236
U
U
DS
the exponent R235 is given by R2355 ln 233 ⁄ 236
~ ! 14.3.4 The relative isobaric contribution (235Ui/235U)ME
>0.991543, according the exponential fractionation law. from the double spike is given by
14.2.3 The exponent R235 is given by R235 = 1 in case the
linear fractionation law is preferred as an approximation. S DS D 235
U 233
U

S D
235
Ui
5
233
U DS
238
U ME
(8)
14.3 Background and Isobaric Corrections—All back-
ground and isobaric corrections of the isotope ratios are
235
U
S D ME
235

238
U
U
ME
performed internally on a per mass cycle basis for each 235 233 235 233
measurement. Where ( U/ U)DS is the U/ U ratio of the double
14.3.1 The measured 233U/236U ratio is corrected for back- spike, which can be calculated from the certified (235U/236U)DS
ground and the relative isobaric contribution (236Ui/236U) from and (233U/236U)DS ratios given on the certificate using:
the sample:
S D 235
U

S D S D
233
U 233
U S D 235
U
5
236
U DS
(9)
236
U CO
5 236
U ME
·
S D
233
U DS
233

236
U
U

S SS D S D D D 1 2
232.55
233
U ME
1
233.55
233
U ME
⁄2
14.3.5 The relative isobaric contribution (234Ui/234U)ME
DS

S SS D S D D S D D
1 2
235.55
236 1
236.55
236 ⁄2 2
236

236
Ui from the double spike is given by
U ME
U ME
U ME
S DS D 234
U 233
U
(4)
S D
234
Ui
5
233
U DS
238
U ME
(10)
where:
ME = measured ratio, and
234
U
S D ME
234

238
U
U
ME

CO = corrected ratio. 234 233 234 233

Where ( U/ U)DS is the U/ U ratio of the double
14.3.2 The relative isobaric contribution (236Ui/236U)ME spike, which can be calculated from the certified (234U/236U)DS
from the sample is given by and (233U/236U)DS ratios given on the certificate using

S D S D 236
U 233
U
S D 234
U

S D
236
Ui 238
U Sample
236
U ME
S D 234
U
5
236
U DS
(11)
236
U
S DME
5 233

238
U
U
ME
S D
233
U DS
233

236
U
U
DS

S SS D S D D S D D
1 2
237.55
238
U ME
1
238.55
238
U ME
⁄2 2
238

238
Ui
U ME
14.3.6 The K factor for a double spike measurement is
derived from the certified (233U/236U)DS ratio for each mass
S SS D S D D D 1 2
235.55
236
U ME
1
236.55
236
U ME
⁄2
cycle according to Eq 2 by using the (233U/236U)CO ratio from
Eq 4 which is corrected for background and isobaric interfer-
(5) ences:
Where (236U/238U)Sample is the 236U/238U ratio of the sample,
which should be approximately known from separate mea-
surements (for example, using the MTE method, Test K5
S D 233

236
U
U DS
(12)
Method C1832); and (238Ui/238U)ME is the relative isobaric
contribution from the double spike.
S D 233

236
U
U
CO

238 238
14.3.3 The relative isobaric contribution ( Ui/ U)ME 14.3.7 The K factor is applied in the following way to obtain
from the double spike is given by the corrected 235U/238U ratio of the sample:

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

9
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22

S D 235
U
238
U CO
S D
5 K R235
235

238
U
U ME
Expression of Uncertainty in Measurements (GUM) (15). For
DS measurements, the uncertainty evaluation steps are ex-

S SS D
1 2
234.55
235
U ME
1 S 235.55
235
U D D S D D
ME
⁄2 2
Ui
U
235

235
ME
plained in the following.
235
14.4.2 For the uncertainty of the corrected major ratio
U/238U calculated according to Eq 12 and Eq 13, the relative
S SS D
1 2
237.55
238
U ME
1 S 238.55
238
U D D S D D
ME
238
⁄2 2 238
Ui
U ME
uncertainties of the measured 233U/236U ratios of the double
(13) spike material used for mass fractionation correction and the
measured 235U/238U ratios of the sample, as well as the relative
234 238
14.3.8 The corrected U/ U ratio of the sample can be uncertainty of the known or certified 233U/236U ratio of the
obtained in the following way: double spike, are added in quadrature to obtain the relative
uncertainty of the correct 235U/238U ratio of the sample.
S D 234
U
238
U CO
S D
5 K R234
234

238
U
U ME
Because of the good repeatability of DS measurements (about
0.003 to 0.006 % RSD, only slightly dependent of the value of
S SS D
1 2
233.55
235
U ME
1 S 234.55
235
U D D S D D
ME
⁄2 2
Ui
U
234

234
ME
the ratio), this uncertainty is largely dominated by the uncer-
tainty of the known or certified ratio of the double spike
S SS D
1 2
237.55
238
U ME
1 S 238.55
238
U D D S D D
ME
238
⁄2 2 238
Ui
U ME
(typically in the range of 0.015 to 0.03 %). Typically values for
the expanded uncertainty (coverage factor k = 2) are about
(14)
ln~ 234 ⁄ 238! 0.016 to 0.020 % (see 16.1 for additional details).
The exponent R234 is given by R2345 ln 233 ⁄ 236 >1.32487, 14.4.3 The uncertainty contributions of the corrected ratio
~ ! 235
which is close to 4⁄3 . U/238U ratio arising from the background and isobaric
corrections are negligible, if recommended sample/spike
14.3.9 Quality Control for the Corrected Ratio (233U/
236 amount ratios of >20 are applied.
U)CO—In case the entire sample is evaporated and used for
14.4.4 For the uncertainty of the corrected ratio 234U/238U
the data acquisition using an MTE heating script (see 4.1 and
calculated according to Eq 14, the uncertainty from the isobaric
13.9.2), it is recommended to calculate a weighted mean of the
correction due to 234U stemming from the double spike
corrected (233U/236U)CO ratios derived using Eq 4, as usually
material may become the dominant source of uncertainty.
done according to the total evaporation principle (see Test
Methods C1672 and C1832): 14.5 Calculation of Isotope Amount Fractions (“Atom
Percent”), Isotope Mass Fractions (“Weight Percent”), and
( FS D233
U
· I ~ 236U ! G Molar Mass (“Atomic Weight”):
S D
233

236
U
U
CO2TE
5
ALL_INTEGRATIONS

(
236
U CO

I~ 236
U!
(15) 14.5.1 The isotope amount fractions (also called “atom
percent”), isotope mass fractions (also called “weight
ALL_INTEGRATIONS
percent”), and the molar mass can only be calculated if all
where: isotope ratios 234U/238U, 235U/238U, and 236U/238U of the
I(236U) = signal intensity (in V) for 236U measured sample are known. The 234U/238U and 236U/238U ratios of the
on a Faraday cup, corrected for the sample have to be measured using a method other than the DS
Faraday cup amplifier gain and baseline, method, for example, by TE (Test Method C1672) or MTE
and (Test Method C1832).
(233U/236U)CO-TE = mean for the (233U/236U)CO ratios ac- 14.5.2 Isotope Amount Fraction for Isotope i (i = 234, 235,
quired for all mass cycles during a DS 236, 238):
measurement, weighted by I(236U).
n ~ iU ! n ~ iU ! Ri
The results for (233U/236U)CO-TE are expected to be in mutual A ~ iU ! 5 5 5 (16)
agreement for all measurements on individual filaments as well
n~U! (
j5234, 235, 236, 238
n ~ jU ! (
j5234, 235, 236, 238
Rj

as for all different samples within the same sequence, because

14.5.3 Isotope Mass Fraction for Isotope i (i = 234, 235,
they should be independent on the sample/spike ratio on
236, or 238):
individual filaments and also on the isotopic composition of the
different samples. If this is not the case, there could be a m ~ iU ! R iM i
W ~ iU ! 5 5 (17)
mistake in the application of some of the isobaric corrections m~U! (
j5234, 235, 236, 238
R jM j
according to Eq 4-13. Therefore the results for (233U/
236 14.5.4 Molar Mass:
U)CO-TE serves as quality control for the isobaric correc-
tions. But it is possible that all the results for (233U/236U)CO-TE
consistently deviate (usually less than 0.05 %) from the known (
j5234, 235, 236, 238
R jM j
M~U! 5 (18)
or certified 233U/236U ratio of the double spike, due a possible ( Rj
j5234, 235, 236, 238
overall mass bias effect (13). This does not have an influence
on the (average) internally corrected (235U/238U)CO ratios where:
calculated according to Eq 13. n(iU) = number of moles for isotope i;
234
14.4 Uncertainty Estimation: n(U) = number of moles for all isotopes, usually U,
235
14.4.1 The uncertainties for DS measurements are estimated U, 236U, and 238U;
according to the principles described in the Guide to the m(iU) = mass for isotope i;

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

10
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22
m(U) = mass for all isotopes, usually 234U, 235U, 236U, and
238
U;
Ri = isotope amount ratio (i = 234, 235, 236, and 238)
relative to one (no matter which) of the isotopes;
and
Mi = molar mass for isotope i.
15. Evaluation and Statements for Precision and Bias
15.1 A total of two thermal ionization mass spectrometers at
JRC-G.2 (formerly IRMM), and the NML (IAEA) were used to
determine the precision and bias for uranium isotope amount
ratio measurements via the DS method. Only TIMS instru-
ments of the type TRITONTM were used for the analyses. The
following uranium certified reference materials were used to
evaluate the precision and bias of DS measurements:
15.1.1 From NBL (U.S. DOE), the CRM 112A was used as
a QC material. It is also known with the name NBS SRM 960.
15.1.2 From JRC-G.2, the 235U/238U base material from the
IRMM-074 series (labelled unofficially IRMM-3050, not for
sale), IRMM-184 and the converted UF6 materials IRMM-012,
IRMM-22, and IRMM-023 were applied, which were used as
well for the validation of the Cristallini sampling method for
UF6 (see (12) and (13)). Only measurements of IRMM-021,
IRMM-22, and IRMM-023 samples prepared by direct hydro-
lysis are considered for the evaluation of precision and bias
within this test method.
15.1.3 The used materials cover the range of 235U enrich-
ments from 0.2 to 50 %. The reference materials used for
quality control of the DS method are not identical between
JRC-G.2 and NML. Therefore, common general observations
and some examples for precision and bias are presented within
this test method.
15.1.4 For the double spike material, only the IRMM-3636a
reference material was used by both JRC-G.2 and NML.
15.2 Precision for DS Measurements of the Major Ratio
235
U/238U:
15.2.1 For the corrected major ratio, 235U/238U, the internal
measurement precision varies within a range of 0.0015 % and
0.0035 % relative standard error (RSE) for all mass cycles
during the measurement. The precision slightly depends on the
235
U enrichment. For depleted samples the 235U ion beams are
smaller causing slightly inferior precision due to the inferior
signal-to-amplifier noise ratio. Therefore the use of amplifiers
with 1012 Ω resistors for detecting 235U in depleted samples is
recommended. An example for internal measurement preci-
sions obtained in DS measurements is shown in A1.1.1. The
precision is at the same level as reported for measurements
within the scientific community, see references (8-11, 16-19).
15.2.2 For the corrected major ratio, 235U/238U, the within-
turret precision varies within a range of 0.0015 % and
0.0050 % relative standard deviation (RSD) for replicate (>5)
filament loadings of reference materials analyzed as reported in
(13). The precision slightly depends on the 235U enrichment.
An example for within-turret precisions obtained in DS mea-
surements is shown in A1.1.2.
15.2.3 For the corrected major ratio, 235U/238U, the
between-turret precision varies between 0.0015 % and 0.006 %
RSD as reported in (13). Examples for between-turret preci-
&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07
11
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
sions obtained in DS measurements is shown in A1.1.3 as well
as by the QC charts in A1.1.4 – A1.1.7. In contrast to the
internal measurement precision and the within-turret precision,
for the between-turret precision the decrease with increasing
enrichment of 235U towards the sample with 50 % enrichment
is not observed. The reason for the absence of a trend is not
known. Among the used QC materials, apparently the between-
turret precision is best for NBL CRM 112A. This might be due
to the fact that the loading solution for this material is the only
one prepared from directly dissolving a uranium metal instead
of an oxide. A similar observation has been made for the
precision for MTE measurements of samples such as the metal
reference materials NBL CRM 115 and NBL CRM 116A (see
Test Method C1832).
15.3 Bias for DS Measurements of the Major Ratio, 235U/
238
U:
15.3.1 No significant biases (that is, deviations of measured
and corrected ratios from the known or certified ratios) for the
major ratios, 235U/238U, were observed for the CRM 112A
from NBL. The deviations shown in Fig. A1.1 (in A1.1.4) for
the measurements of NBL CRM 112A were calculated based
on the new average value of 0.00725495(80) which was
measured in a collaborative effort by several geochemistry
laboratories and JRC-G.2 (11). This new average value has
been acquired using the double spike IRMM-3636a, but also
other double spike materials, combined with variety of instru-
mentation types (for example, TIMS and MC-ICPMS) and new
measurement methods. This “inter-laboratory comparison”
(11) also showed that the result for NBL CRM 112A using the
method described in this test method is in good agreement (at
a level of better than 0.002 %) with all results from other
laboratories (other than JRC-G.2 and NML), who were also
using other DS materials and other techniques like MC-
ICPMS. Further confirmatory results for NBL CRM 112A can
be found in (8). This new consensus value is about 0.031 %
higher than the old consensus value (1/137.88=0.0072527), but
in agreement with the new certified value 0.0072543(40) from
NBL. Moreover, it is traceable to the SI and an uncertainty
statement is provided according to the Guide to the Expression
of Uncertainty in Measurements (15). As an alternative to NBL
CRM 112A, the (close to) natural reference material IRMM-
184 has been re-measured as well by several laboratories using
the double spike IRMM-184 has been re-measured as well by
several laboratories using the double spike IRMM-3636, re-
sulting in a 235U/238U value of 0.0072631(11), which is in
agreement with the certified value of 0.0072623(22). But NBL
CRM 112A still remains the primary choice for quality control,
as a reference material for external normalization for high
precision 235U/238U measurements and even for calibration of
non-certified in-house double spike WRMs (see also Guide
C1128). This popularity is due to its widespread 236U relative
abundance, which is below the detection limit of 6 × 10–10 of
the MTE method (5, 6), compared to IRMM-184 (1.2 × 10–7)
and IRMM-3050 (3.8 × 10–5). The metallic form of the original
CRM 112A reference material was also found to be an
advantage for high precision measurements using the DS and
MTE techniques.
 C1871 − 22
15.3.2 For the IRMM reference materials, IRMM-3050, the
gravimetrically prepared 235U/238U-base material from the
IRMM-074 series (not for sale, (14)) was used at JRC-G.2 only
(see A1.1.5, Fig. A1.2), and the IRMM-184 was used at
JRC-G.2 (see A1.1.6, Fig. A1.3) and NML (see A1.1.7, Fig.
A1.4). No significant biases for the major ratios, 235U/238U
were observed for measurements of these materials, as shown
in A1.1.8.
15.3.3 Additionally, Table A1.5 and Fig. A1.5 show that the
result for the major ratio of NBL CRM 112A, expressed as
238
U/235U here, obtained at JRC-G.2 using the method de-
scribed in this test method, is in good agreement with numer-
ous results from other laboratories within the nuclear safe-
guards and scientific community, where not only IRMM-3636
but also other DS materials and other mass spectrometric
techniques like MC-ICPMS were used. Further detailed dis-
cussions about this matter can be found in (17).
15.3.4 Among the used QC materials, only IRMM-3050 is
certified based on gravimetric preparation, like the double
spike reference materials IRMM-3636, IRMM-3636a, and
IRMM-3636b are as well. The agreement of the measured ratio
with the certified one also confirms the accuracy of the DS
method, however with a combined expanded uncertainty of
0.022 % which is dominated by the uncertainties of the DS and
IRMM-3050 themselves. For NBL CRM 112A, the bias is
insignificant over the 9 year period. For IRMM-184 the very
early results from 2009 at JRC-G.2 seem to be lower (about
–0.005 %) than the reference value (11) but the recent results in
2016 agree better. At the NML the DS method was imple-
mented in 2016, and the results for IRMM-184 are slightly
(0.0025 %) higher than the reference value (11). This could in
principle be due to slight differences in Faraday cup efficien-
cies between the two TIMS instruments used at JRC-G.2 and
NML. As a confirmation for this assumption, measurements
performed using both TIMS instruments on the same samples
for the validation of the Cristallini samples (IRMM-020,
IRMM-022, and IRMM-023, see (13) showed the same trend).
Therefore, it is recommended to normalize all DS results to the
same common standard reference material, for which the
NBL-CRM 112A is recommended. However, if all uncertainty
contributions are considered, there was no significant bias
observed for any of the used QC materials.
16. Measurement Uncertainty
16.1 Major Isotope Amount Ratios 235U/238U—The propor-
tions of the uncertainty contributions (see 14.4.2) depend on
the precision and number of replicates of the DS
measurements, as well as on the uncertainty of the 233U/236U
isotope amount ratio of the double spike material. The com-
bined uncertainty is usually largely dominated by the uncer-
tainty of the known or certified 233U/236U ratio of the double
spike. Typical values for the expanded uncertainty (coverage
factor k = 2) are about 0.016 to 0.020 % independent of the
ratios.
17. Keywords
17.1 certified reference materials; double spike; isotope
amount ratios; mass fractionation correction; modified total
evaporation; thermal ionization mass spectrometry; total
evaporation; uranium

ANNEX

(Mandatory Information)

A1. PRECISION AND BIAS FOR DS MEASUREMENTS

A1.1 A discussion and statements regarding precision and TABLE A1.2 Within-Turret Precision (% RSD) for DS
bias for DS measurements are given in Section 15. Associated Measurements of the Major Ratio 235U/238U
235
tables and figures are presented in A1.1.1 – A1.1.9. CRM U/238U 235
U/U, % Average RSD, %
Data from (13, 20)
A1.1.1 See Table A1.1. IRMM-020 0.00210 0.2 0.0047 %
IRMM-021 0.00441 0.4 0.0041 %
A1.1.2 See Table A1.2. IRMM-022, IRMM-184 0.00726 0.7 0.0025 %
IRMM-023 0.03388 3.3 0.0027 %
A1.1.3 See Table A1.3. IRMM-3050 (-074) 1.00026 50.0 0.0018 %
A1.1.4 QC chart to show bias and between turret precision
for 235U/238U measurements of NBL CRM 112A performed at
JRC-G.2, taken from (13). See Fig. A1.1. A1.1.5 QC chart to show bias and between turret precision
for 235U/238U measurements of IRMM-3050 (IRMM-074 se-
TABLE A1.1 Internal Measurement Precision (% RSE) for DS
Measurements of the Major Ratio 235U/238U ries) performed at JRC-G.2, taken from (13). See Fig. A1.2.
CRM 235
U/238U 235
U/U, % Average RSE, % A1.1.6 QC chart to show bias and between turret precision
Data from (13, 20) for 235U/238U measurements of IRMM-184 performed at JRC-
IRMM-020 0.00210 0.2 0.0036 %
IRMM-021 0.00441 0.4 0.0027 %
G.2, taken from (13). See Fig. A1.3.
IRMM-022, IRMM-184 0.00726 0.7 0.0022 % A1.1.7 QC chart to show bias and between turret precision
IRMM-023 0.03388 3.3 0.0015 %
IRMM-3050 (-074) 1.00026 50.0 0.0016 % for 235U/238U measurements of IRMM-184 performed at NML,
taken from (13). See Fig. A1.4.

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

12
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22
TABLE A1.3 Between-Turret Precision (% RSD) for DS A1.1.8 See Table A1.4.
Measurements of Major Ratio 235U/238U
CRM 235
U/238U 235
U/U, % Average RSD, % A1.1.9 See Table A1.5 and Fig. A1.5.
Data from (13, 20)
IRMM-020 0.00210 0.2 0.0057 %
IRMM-184 (natural) 0.00726 0.7 0.0029 %
IRMM-112A (natural) 0.00726 0.7 0.0015 %
IRMM-3050 (-074) 1.00026 50.0 0.0045 %

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

13
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22

FIG. A1.1 QC Chart NBL CRM 112A, Measurements Performed at JRC-G.2

FIG. A1.2 QC Chart IRMM-3050, Measurements Performed at JRC-G.2

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

14
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22

FIG. A1.3 QC Chart IRMM-184, Measurements Performed at JRC-G.2

FIG. A1.4 QC Chart IRMM-184, Measurements Performed at NML

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

15
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22
235
TABLE A1.4 Bias (% RD) for DS Measurements of the Major Ratio U/238U
235 238 235
CRM U/ U U/U, % RD (%) Uncertainty (w/o DS) Uncertainty (all contr.)
Data from (13)
IRMM-184 (natural), IAEA, only 2016 0.00726 0.7 0.0025 % 0.0016 % 0.015 %
IRMM-184 (natural), JRC-G.2 0.00726 0.7 –0.0024 % 0.0023 % 0.015 %
IRMM-184 (natural), JRC-G.2, only 2009 0.00726 0.7 –0.0052 % 0.0023 % 0.015 %
IRMM-184 (natural), JRC-G.2, only 2016 0.00726 0.7 0.0000 % 0.0030 % 0.015 %
IRMM-112A (natural), JRC-G.2 0.00726 0.7 –0.0013 % 0.0015 % 0.011 %
IRMM-3050 (-074), JRC-G.2 1.00026 50.0 –0.0012 % 0.0027 % 0.022 %

238
TABLE A1.5 Results for DS Measurements of the Major Ratio U/235U for NBL CRM 112A
Laboratory, Reference Instrumentation Reference Materials used for Instrument Calibration NBL 112A 238U/235U
Uncertainty, k=2
NBL New Certified Value (21) Triton TIMS NBL-U030A, by MTE/TIMS (see Test Method C1832) 137.849(76)
“New Average Value” as introduced in (11) Triton TIMS, Neptune MC-ICPMS Double Spike IRMM-3636, and other Double Spikes 137.837(15)
calibrated using CRMs such as IRMM-074, IRMM-184
233
JRC-G.2/Geel (11) Triton TIMS U/236U Double Spike IRMM-3636, 137.836(23)
233
U/236U=1.01906(16)
233
NIGL Isotope Geoscience Laboratory (2010) Triton TIMS U/236U Double Spike IRMM-3636, 137.844(25)
233
(11) U/236U=1.01906(16)
233
NERC Isotope Geoscience Laboratory Triton TIMS U/236U Double Spike IRMM-3636, 137.832(22)
233
(2012) (16) U/236U=1.01906(16)
233
University of Frankfurt (11) Neptune MC-ICPMS U/236U Double Spike IRMM-3636, 137.833(28)
233
U/236U=1.01906(16)
233
Thermo Fisher Scientific (11) Neptune MC-ICPMS U/236U Double Spike IRMM-3636, 137.836(23)
233
U/236U=1.01906(16)
233
NERC Isotope Geoscience Laboratory Neptune MC-ICPMS U/236U Double Spike IRMM-3636, 137.829(22)
233
(2012) (16) U/236U=1.01906(16)
233
National Taiwan University, NTU, (11) Neptune MC-ICPMS U/236U Double Spike made by UMN, calibrated using 137.834(21)
IRMM-074 ⁄10, 238U/235U=0.99974(15)
233
University of Minnesota, UMN, (11) Neptune MC-ICPMS U/236U Double Spike made by UMN, calibrated using 137.830(25)
IRMM-074 ⁄10, 238U/235U=0.99974(15)
233
Lawrence Livermore National Laboratory Triton TIMS U/236U Double Spike made by LLNL, calibrated using 137.823(42)
LLNL, (11) IRMM-184, 238U/235U=137.697(41)
233
Arizona State University (18) Neptune MC-ICPMS U/236U Double Spike IRMM-3636, 137.843(23)
233
U/236U=1.01906(16)
233
Enrico Fermi Institute (19) Neptune MC-ICPMS U/236U Double Spike IRMM-3636, 137.842(23)
233
U/236U=1.01906(16)

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

16
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
 C1871 − 22
FIG. A1.5 Results for DS Measurements for the Major Ratio
REFERENCES
(1) Callis, E. L. and Abernathy, R. M., “High-Precision Isotopic Analyses
of Uranium and Plutonium by Total Sample Volatilization and Signal
Integration,” Int. J. Mass Spectrom. Ion Proc., Vol 103, 1991, pp.
93–105.
(2) Fiedler, R. et al., “Report on Preliminary Experience with Total
Evaporation Measurements in Thermal Ionization Mass
Spectrometry,” Int. J. Mass Spectrom. Ion Proc., Vol 132, 1994, pp.
207–215.
(3) Fiedler, R., “Total Evaporation Measurements—Experience with
Multi-Collector Instruments and a Thermal Ionization Quadrupole
Mass-Spectrometer,” International Journal of Mass Spectrometry, Vol
146, 1995, pp. 91–97.
(4) Mathew, K. J., O’Connor, G., Hasozbek, A., and Kraiem, M., “Total
Evaporation Method for Uranium Isotope-amount Ratio
Measurements,” Journal of Anal. At. Spectrom., Vol 28, 2013, pp.
866–876.
(5) Richter, S. and Goldberg, S. A., “Improved Techniques for High
Accuracy Isotope Ratio Measurements of Nuclear Materials using
Thermal Ionization Mass Spectrometry,” International Journal of
Mass Spectrometry, Vol 229, 2003, pp. 181–197.
(6) Richter, S., Kühn, H., Aregbe, Y., Hedberg, M., Horta-Domenech, J.,
et al, “Improvements in Routine Uranium Isotope Ratio Measure-
ments using the Modified Total Evaporation Method for Multi-
Collector Thermal Ionization,” Mass Spectrometry Journal of Anal.
At. Spectrom., Vol 26, 2011, pp. 550–564.
(7) Richter, S., Alonso, A., Eykens, R., Jacobsson, U., Kühn, H.,
Verbruggen, A., Aregbe, Y., Wellum, R., and Keegan, E., “The
Isotopic Composition of Natural Uranium Samples—Measurements
using the New n(233U)/n(236U) Double Spike IRMM-3636,” Interna-
tional Journal of Mass Spectrometry, Vol 269, 2008, pp. 145–148.
(8) Brennecka, G. A., Wasylenki, E., Bargar, J. R., Weyer, S., and Anbar,
A. D., “Uranium Isotope Fractionation during Adsorption to Mn-
Oxyhydroxides,” Environ. Sci. Technol., Vol 45, 2011, pp. 1370–1375.
&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07
17
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG
238
U/235U for NBL CRM 112A
(9) Keegan, E., Richter, S., Kelly, I., Wong, H., Gadd, P., Kuehn, H., and
Alonso, A., “The Provenance of Australian Uranium Ore Concentrates
by Elemental and Isotopic Analysis,” Applied Geochemistry, Vol 23,
2008, pp. 765–777.
(10) Cheng, H., Edwardsa, R. L., Shenc, C.-C., Polyak, V. J., Asmerom,
Y., Woodhead, J., Hellstrom, J., Wang, Y., Kong, X., Spötl, C., Wang,
X., and Alexander Jr., E. C., “Improvements in 230Th Dating, 230Th
and 234U Half-life Values, and U-Th Isotopic Measurements by
Multi-collector Inductively Coupled Plasma Mass Spectrometry,”
Earth and Planetary Science Letters, Vol 371–372, 2013, pp. 82–91.
(11) Richter, S., Eykens, R., Kühn, H., Aregbe, Y., Verbruggen, A., and
Weyer, S., “New Average Values for the n(238U)/n(235U) Isotope
Ratios of Natural Uranium Standards,” International Journal of
Mass Spectrometry, Vol 295, 2010, pp. 94–97.
(12) Galdoz, E., Esteban, A., Cristallini, O., and Perrotta, J., “UF6
Sampling Method Using Alumina,” 49th INMM Annual Meeting,
USA, 2008.
(13) Richter, S., Hiess, J., and Jacobsson, U., “Validation of Cristallini
Sampling, Method for UF6 by High Precision, Double-Spike
Measurements,” 2016, JRC-103668, https://ec.europa.eu/jrc/en/
news/validation-cristallini-method-sampling-uranium-hexafluoride-
uf6).
(14) Richter, S., Alonso, A., Aregbe, Y., Eykens, R., Kehoe, F., et al, “A
New Series of Uranium Isotope Reference Materials for Investigat-
ing the Linearity of Secondary Electron Multipliers in Isotope Mass
Spectrometry,” International Journal of Mass Spectrometry, Vol 281,
2009, pp. 115–125.
(15) BIPM, “Joint Committee for Guides in Metrology, Evaluation of
Measurement Data—Guide to the Expression of Uncertainty in
Measurement,” JCGM, Vol 100, 2008.
(16) Hiess, J., Condon, D. J., McLean, N., and Noble, S. R., “Systematics
in Terrestrial Uranium-Bearing Minerals,” Science, Vol 315, 2012,
pp. 1610–1614.
 C1871 − 22
(17) Andersen, M. B., Stirling, C. H., and Weyer, S., “Uranium Isotope
Fractionation,” Reviews in Mineralogy & Geochemistry, Vol 82,
2017, pp. 799–850.
(18) Goldmann, A., Brennecka, J., Noordmann, J., Weyer, S., and
Wadhwa, M., “The Uranium Isotopic Composition of the Earth and
the Solar System,” Geochim Cosmochim Acta, Vol 148, 2015, pp.
145–158.
(19) Tissot, F. L. H. and Dauphas, N., “Uranium Isotopic Compositions of
the Crust and Ocean: Age Corrections, U Budget and Global Extent
of Modern Anoxia,” Geochim Cosmochim Acta, Vol 167, 2015, pp.
113–143.
(20) Mialle, S., Richter, S., Hennessy, C., Truyens, J., Jacobsson, U., et al,
“Certifications of Uranium Hexafluoride Reference Materials for
Isotopic Composition,” 8th International Conference on Isotopes,
Chicago, Aug. 24–29, 2014, J Radioanal Nucl Chem, Vol 305, 2015,
pp. 255–266.
(21) Mathew, K., Mason, P., Voeks., and Narayanan, U., “Uranium
Isotope Abundance Ratios in Natural Uranium Metal Certified
Reference Material 112-A, International Journal of Mass
Spectrometry, Vol 315, 2012, pp. 8–14.

ASTM International takes no position respecting the validity of any patent rights asserted in connection with any item mentioned
in this standard. Users of this standard are expressly advised that determination of the validity of any such patent rights, and the risk
of infringement of such rights, are entirely their own responsibility.

This standard is subject to revision at any time by the responsible technical committee and must be reviewed every five years and
if not revised, either reapproved or withdrawn. Your comments are invited either for revision of this standard or for additional standards
and should be addressed to ASTM International Headquarters. Your comments will receive careful consideration at a meeting of the
responsible technical committee, which you may attend. If you feel that your comments have not received a fair hearing you should
make your views known to the ASTM Committee on Standards, at the address shown below.

This standard is copyrighted by ASTM International, 100 Barr Harbor Drive, PO Box C700, West Conshohocken, PA 19428-2959,
United States. Individual reprints (single or multiple copies) of this standard may be obtained by contacting ASTM at the above
address or at 610-832-9585 (phone), 610-832-9555 (fax), or service@astm.org (e-mail); or through the ASTM website
(www.astm.org). Permission rights to photocopy the standard may also be secured from the Copyright Clearance Center, 222
Rosewood Drive, Danvers, MA 01923, Tel: (978) 646-2600; http://www.copyright.com/

&RS\ULJKWE\$670,QW O DOOULJKWVUHVHUYHG )UL-DQ*07

18
'RZQORDGHGSULQWHGE\
8&5 8QLYHUVLGDGGH&RVWD5LFDSXUVXDQWWR/LFHQVH$JUHHPHQW1RIXUWKHUUHSURGXFWLRQVDXWKRUL]HG