Download Radioactive decay data: powerful aids in medical

Radiochim. Acta 100, 615–634 (2012) / DOI 10.1524/ract.2012.1959
© by Oldenbourg Wissenschaftsverlag, München
Radioactive decay data: powerful aids in medical diagnosis and
therapy, analytical science and other applications
By A. L. Nichols1 , 2 , ∗
1
2
Department of Physics, University of Surrey, Guildford, GU2 7XH, UK
Manipal University, Madhav Nagar, Manipal 576104, Karnataka, India
(Received January 31, 2012; accepted in revised form April 10, 2012)
(Published online July 30, 2012)
Radioactive decay / Decay data measurements /
Decay data evaluations / Decay data files /
Reactor operations / Fuel cycle applications /
Non-energy applications / Nuclear medicine
Summary. Decay data are commonly used to characterise
and quantify radioactive material, and provide an important
means of understanding the properties and structure of the
nucleus. Experimental measurement techniques are reviewed,
with the emphasis placed on recent developments that represent a potential quantum leap in advancing our knowledge,
particularly by means of γ -ray spectroscopy. A select number
of internationally-accepted decay-data evaluations and compilations are also discussed in terms of their contents. Both
energy and non-energy related applications require the input
of well-defined decay data, and such activities have been
reviewed. Various important decay-data issues are assessed,
and note taken of any significant requirements for better
quantified data.
1. Introduction
In-depth assessments, evaluations and measurements of radioactive decay data have been requested and undertaken
over many years. Recommended decay data are normally
derived from all relevant publications that include quantification of decay-scheme data primarily by means of direct
measurement but also by calculation. The measurement and
derivation of such recommended data sets are welcomed by
nuclear physicists and engineers (a) to define the status and
our current knowledge of particular decay parameters, and
determine whether there is a need for further investigation
and study, and (b) hopefully to provide highly reliable input
data for modelling codes in order to quantify the operational
characteristics and behaviour of irradiated fuel and other
materials with reasonable confidence.
Atomic and nuclear decay-data parameters encompass
the following [1–3]: half-life; total decay energies (Qvalues); branching fractions (if more than one known decay mode); α-particle energies and emission probabilities; β − -particle energies, emission probabilities and tran*E-mail: [email protected].
sition types; electron-capture and β + -particle energies,
transition/emission probabilities and transition type (also
EC/β + ratios when appropriate); γ -ray energies, emission probabilities and internal conversion coefficients (also
internal-pair formation coefficients for β + β − when appropriate); Auger- and conversion-electron energies and emission
probabilities; X-ray energies and emission probabilities;
spontaneous fission properties (branching fraction and recoil
energies); delayed-neutron energies and emission probabilities; delayed-proton energies and emission probabilities; and
comprehensive quantification of the uncertainties associated
with all of the above atomic and nuclear parameters.
Additional ancillary data requirements can be met from
the above, including various total mean energies which need
to be quantified and adopted for particular applications:
mean heavy-particle energy (includes mean α, neutron, proton, fission fragment, and associated recoil energies); mean
light-particle energy (includes mean β − , β + , Auger-electron
and conversion-electron energies); and mean electromagnetic energy (includes mean γ , X-ray, β + β − annihilation
radiation and internal bremsstrahlung). While more exotic
modes of decay have been detected (e.g. double-beta (ββ)
and cluster/heavy-ion decay), these low-probability phenomena are not considered further in this review.
The need for well-defined radioactive decay data was
recognised over 80 years ago with the publication of a paper
by the International Radium-Standards Commission which
included such world-renowned scientists as Marie Curie,
Otto Hahn, Hans Geiger and Lord Rutherford [4]. Recommended radioactive constants were proposed with no uncertainties, based predominantly on known measurements
by members of the Commission and their co-workers. This
work led on to more extensive nuclear reaction data listings
by Fea [5] and Livingston and Bethe [6], and the first recognizable Table of Isotopes format by Livingood and Seaborg
in 1940 [7] that appeared every four or five years in Reviews of Modern Physics until 1958. Subsequent editions of
the Table of Isotopes have been published at regular intervals up to an including the 8th edition in 1996 [8], which also
contains a CD-ROM of the full contents. Recommended nuclear structure and decay data for this particular edition of
the Table of Isotopes have primarily been extracted from the
Evaluated Nuclear Structure Data File (ENSDF, see below).
Unauthenticated
Download Date | 6/12/17 1:06 PM
616
A. L. Nichols
Katharine Way began collecting and compiling nuclear
data in the early/mid 1940s, and a compilation of her work
first appeared in 1950 [9] – no specific values were recommended, nor uncertainties given. Nevertheless, this work
evolved into Nuclear Data Sheets (as published by Academic Press, and subsequently by Elsevier Inc.) and the
Evaluated Nuclear Structure Data File (ENSDF) [10]. Evaluations of nuclear structure and decay-data measurements
were carried out at regular intervals of time, and formatting
codes were developed to display the recommended nuclear
data in a clear, concise and well-defined manner. These studies continue as a multinational work programme, with biennial meetings held to discuss both managerial and technical
issues under the auspices of the Nuclear Data Section of the
International Atomic Energy Agency [11].
2. Experimental techniques
Radioactive nuclides of interest are normally prepared by
means of either reactor irradiation or charged-particle acceleration and controlled bombardment of carefully prepared targetry. Isotopic enrichment of the target material
and purification of the resulting product represent important requirements when striving to measure accurate decay data. Various radiochemical procedures have been successfully adopted to achieve elemental separation of the
irradiated target, including anion-exchange chromatography, application of many forms of liquid-liquid extraction,
and dry distillation [12–14]. For example, the adoption
of various radiochemical techniques to achieve high levels of radionuclidic purity was very important in forming the basis for accurate measurements of the positron
emission probabilities of 64 Cu, 76 Br and 124 I for medical
applications [14].
Long-established experimental techniques can be used
to quantify in detail specific features of a decay scheme,
ranging from α, γ and electron spectroscopy operated in singles and various coincidence modes, time-dependent studies of these emissions to determine important parameters
such as half-lives, and angular correlation measurements for
greater structural detail. The more substantive techniques are
briefly discussed below, along with some thoughts on future
developments.
2.1 α-spectroscopy
Obviously, measurements of α spectra play an important
role in quantifying and defining the decay schemes of αparticle emitting nuclides, and impact most significantly on
studies of the many heavy elements and actinides. One loss
over recent years has been the decline in maintenance of
dedicated magnetic spectrometers that offer extremely good
energy resolution. Precise, well-defined studies of α spectra were feasible with homogeneous-field magnetic spectrographs [15, 16]. Silicon-based ionization detectors such as
the silicon barrier detector (SBD) and passivated implanted
planar silicon (PIPS) detector are now much more commonly used to measure the energies and emission probabilities of α particles [17]. Good resolution α spectra obtained
by means of a 450-mm2 PIPS detector are shown in Fig. 1
for mass-separated sources of 237 Np and 243 Am [18].
Fig. 1. Alpha-particle spectra of thin mass-separated sources of (a)
237
Np, and (b) 243 Am measured by means of a 450-mm2 passivated implanted planar silicon (PIPS) detector – main α peaks are labelled in
keV energy units [18].
Significant developments have recently occurred with respect to improvements in energy resolution by means of
cryogenic microcalorimetry:
1. Detector system consisting of a superconducting transition-edge sensor (TES) with Mo:Cu bilayer and an absorber of superconducting tin has been shown to give
an energy resolution of (1.06 ± 0.04) keV FWHM for
5.3 MeV α particles [19, 20].
2. Sensor of gold doped with a small concentration of erbium (Au:Er) for which the magnetization changes as
a function of modification in temperature by α-particle
absorption – energy resolution of (2.83 ± 0.05) keV
FWHM was determined for 5.5 MeV α particles [21].
Such ultra-high resolutions are a significant improvement
beyond the theoretical limit of conventional silicon detectors. Alpha-particle measurements with this type of detector
system would greatly reduce uncertainties in decay schemes
and specific aspects of their decay data, with an inevitably
beneficial knock-on effect involving the accuracy and efficacy of their application.
2.2 X- and γ -ray spectroscopy
The extremely successful development and adoption of silicon and germanium crystals as detectors in X- and γ -ray
spectroscopy has contributed immensely to our understanding of the atomic nucleus across the known Chart of the
Nuclides. Since the late 1960s, Si- and Ge-based detectors
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
have offered the best compromise between energy resolution
and efficiency to ensure sound, accurate and reliable X- and
γ -ray spectral studies. More specifically, major advances
into the 1980s were associated with increased volume and
improved purity of Ge crystals, while the more recent introduction of segmented Ge systems has further improved their
detection capabilities and performance characteristics.
A significant amount of nuclear structure data measured and evaluated for inclusion in recommended decay
databases originates from γ -ray spectroscopy undertaken
with single-crystal Ge(Li) and HPGe detectors which operate satisfactorily below 110 K (and therefore are normally
maintained by means of liquid nitrogen at 77 K). Directly
measured data include X- and γ -ray energies and emission
probabilities, with the added potential to derive the spins,
parities and lifetimes of excited states, determine γ transition types and mixing ratios, and calculate directly other features of the decay scheme under investigation. Low-energy
photon spectrometers (LEPS) based on a planar small-area
HPGe crystal have also been specifically developed to measure γ -ray spectra over the low to intermediate energy range
from 3 to approximately 300 keV – these detector systems
operate at high resolution, and an example γ spectrum of
a chemically-purified 233 Pa source is shown in Fig. 2 [18].
The division of a Ge crystal into sections offers additional information identified with the γ interactions, referred
to as γ -ray tracking expressed in terms of energy, time and
location – the net result has been the twin achievements
of unprecedented efficiency and energy resolution. The development and operational characteristics of single-crystal
Ge detectors and more advanced Ge detector arrays can be
found in the substantial review articles of Lee et al. [22], and
Eberth and Simpson [23]. Only a brief semi-historic summary is given below.
Rapid progress in the discovery and understanding of
nuclear structure and decay data in the 1970s was almost en-
Fig. 2. Gamma-ray spectrum of a chemically-purified 233 Pa source
measured by means of a 2-cm2 × 1-cm planar low-energy photon spectrometer (LEPS), at a source-to-detector distance of 5 cm – main γ
peaks are labelled in keV energy units [18].
617
Fig. 3. Half of the modular layout of HPGe detectors for (a) Gammasphere, and (b) Euroball.
tirely related to the advent of Ge(Li) detectors in γ -ray spectroscopy. Such beginnings led on to technological advances
in the growth of large high-purity Ge crystals to increase
the peak-to-Compton ratio, reduce background effects, and
improve the coincidence rate and spectral statistics. Escapesuppression shields were introduced in order to reject partly
absorbed events from the γ spectra, and the number of
escape-suppressed Ge detectors was increased into arrays
during the course of the 1980s to compensate for the commensurate loss in coincidence efficiency [23]. Such HPGe
arrays with double gating and ancillary detectors opened up
the possibility of measuring γ -γ -γ coincidences to quantify
weak and complex γ cascades. Second-generation systems
consisting of 4π solid-angle arrays of germanium detectors and BGO (bismuth germanate (Bi4 Ge3 O12 )) shields have
proved to be very costly, and therefore resulted in the evolution of only two recognised primary projects (Fig. 3): Gammasphere – multi-laboratory programme based in the USA;
and the Euroball collaboration in Europe. Gammasphere and
Euroball are seen as achieving the highest feasible goals for
4π solid-angle arrays with escape-suppressed Ge detectors.
Their impressive achievements in the continued evolution
and resolution of nuclear structure and decay scheme data
can be found on the Web [24, 25].
Scientific interest has tended to focus in recent years on
extraordinary N/Z ratios close to the proton and neutron
drip lines as a consequence of the growing need to support
Unauthenticated
Download Date | 6/12/17 1:06 PM
618
the study of nuclear reactions generated by emerging radioactive ion beam facilities (RIB). Theoretical analyses and
experimental studies on Ge-based detector design has led to
the concept of γ -ray tracking in terms of the position, energy
and time of all γ -ray interaction points within Ge detector
systems:
– GRETA (Gamma Ray Energy Tracking Array, USA [22];
geodesic configuration of 120 to 130 segmented HPGe
detectors);
– AGATA (Advanced GAmma Tracking Array, Europe
[23, 26]; geodesic configuration of 180 hexagonal and 12
pentagonal segmented HPGe detectors).
Identification of the interaction points and quantification
of the energy deposited at these locations can be achieved
with highly-segmented Ge detectors and pulse-shape analyses. However, the sequence of a γ -ray scattering process
is too fast for measurement compared with the time resolution of a Ge detector, and therefore tracking algorithms
based on the underlying interaction processes have to be
used. While GRETA and AGATA will permit access to the
farthest reaches of the Chart of the Nuclides, other areas of
nuclear application will also benefit from the operational advances in Ge detector technology. Thus, the development
of position-sensitive γ -ray detectors for nuclear structure
studies will have important repercussions in astrophysics,
medical imaging and nuclear safeguards.
GRETINA represents a significant stepping-stone towards GRETA, and consists of coaxial Ge crystals of tapered
hexagonal shape that make up seven modules, each containing four 36-fold segmented crystals (Fig. 4). This set of 28
Ge crystals covers a quarter of the 4π solid angle envisaged for GRETA, and will be extensively tested in a series
of nuclear structure, reaction and symmetry studies [27].
Similarly, an AGATA sub-array consisting of five triple clusters of highly-segmented Ge detectors has been assembled
at Laboratori Nazionali di Legnaro, Padova (total of 15 Ge
Fig. 4. Quarter-based layout of the GRETINA detectors (foreground)
compared with the full 4π solid-angle system proposed for GRETA
(background).
A. L. Nichols
crystals compares with the full AGATA 4π geometry of 60
triple clusters (180 Ge detectors)). Complementary analysis systems are available to operate in conjunction with the
AGATA sub-array, and so extend the measurement capabilities to a broader range of nuclear physics topics [28].
Assembled stacks of planar double-sided Ge strip detectors (DSSD) possess sufficient pixelation to achieve γ -ray
positional resolution [22]. Possible drawbacks are envisaged, such as the existence of dead layers at the edge of
each planar crystal and the need for mechanical structure to
ensure the provision of sufficient cooling to the HPGe detectors. Nevertheless, such systems are being studied for their
γ -ray tracking potential and possible application in highresolution photon imaging.
The ability to discriminate between γ rays of slightly different energies by means of a scintillator is of importance
in medical imaging, γ -ray spectroscopy and X-ray astronomy. Both NaI(Tl) and CsI(Tl) have been the scintillators
of choice for over 50 years because of their reasonable energy resolution, while other scintillators such as Bi4 Ge3 O12
in positron emission tomography (PET) and PbWO4 in highenergy nuclear physics have found appropriate application.
However, lanthanum halides doped with Ce3+ have also
been shown to exhibit significant promise based on good
energy resolution in combination with fast luminescence decay [29–31]. The superior energy resolution of LaBr3 (Ce)
scintillator has successfully been used with Gammasphere to
quantify with good precision the lifetimes of nuclear levels
between 50 ps and 1 ns, as populated in the IT and β − decay
of 177m Lu [32]. Potentially new and improved scintillators
are constantly being assessed for adoption in high-resolution
γ -ray spectroscopy, and studies of their performance provide essential guidance as to their suitability and application [33].
Another noteworthy technique for accurate X- and
low-energy γ -ray detection is the X-ray microcalorimeter [34, 35]. Effectively, the detector system consists of 36
microcalorimeters in 6 × 6 array, although only 32 are electronically active: 28 pixels use 8-µm thick HgTe absorbers,
and the remaining four pixels use 30-µm thick Bi absorbers.
Maximum sensitivity is achieved when this device operates
at 60 mK to give an energy resolution of 6 eV (FWHM) from
0 to 10 keV, while an operating temperature of 90 mK gives
FWHM of ∼ 26 eV up to about 60 keV. This device senses
and quantifies the heat deposited by incident photons on the
HgTe absorbers, and has been used with impressive accuracy
to determine an energy split of only (7.6 ± 0.5) eV between
the ground and first excited states of 229 Th, based on precisely measured differences in the more substantial γ rays
populating both members of the doublet [36].
Total Absorption Gamma-ray Spectroscopy (TAGS) has
been successfully used to determine the β − strength functions of a significant number of complex decay schemes
[37–41] on the basis of calculations involving the data derived from 4π γ -ray spectroscopy. Normally, the main spectrometer consists of a substantial well-type NaI(Tl) detector
in which the γ -ray emitting source is contained, along with
an auxiliary NaI(Tl) detector that fits into and closes the well
to achieve an approximately 97% 4π solid-angle geometry.
Various other ancillary γ -ray detectors may also be used
to study coincidence gating. More recent assemblies have
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
involved the assessment, design and construction of other
suitable detector materials and arrays. Good overall detection efficiency and energy resolution are required, along
with a sound spectral understanding in order to disentangle
the decay components from each other and any background
activity. TAGS has proved to be of importance in the development of a more correct and comprehensive understanding
of the nucleus, reaching beyond some of the specific limitations of γ singles and coincidence measurements [39, 40].
Furthermore, TAGS studies have been used to determine the
average β − and γ energies of particular fission produces,
aiding considerably in calculations of the decay heat emitted
by irradiated reactor fuel [38, 41] – see also Sect. 4.2.
2.3 Electron spectroscopy
Appropriate studies of β, Auger-electron and internal
conversion-electron emissions have yielded important data
in the resolution of difficulties associated with the population and depopulation of daughter nuclear levels and the
derivation of a normalisation factor to convert relative γ -ray
emission probabilities to absolute values. Various types of
detector system have been used, e.g. permanent-magnet 180◦
spectrograph, permanent-magnet pre-accelerating
√ spectrograph, six-gap spectrometer and iron-free π 2 doublefocusing spectrometer [42–44]. While sound quantification
of electron emissions has proved important input to the evolution of fully consistent decay schemes and well-defined
decay data, this type of complex spectrometric study has
been seriously neglected in recent years. A major problem
is the bulky nature of the magnet systems, coupled with the
delicate nature of the multi-element detector assemblies –
their maintenance and operation have historically proved to
be costly.
β − intensity distributions are normally determined from
any calculated imbalances in the γ population and depopulation of nuclear levels of the decay schemes assembled
and quantified by means of γ -ray spectroscopy. However,
such experimental studies can be fraught with difficulties
resulting from the failure to detect all of the weak γ transitions. Faced with this basic problem of omission in the study
of complex decay schemes, Total Absorption Gamma-ray
Spectroscopy (TAGS) has been used to determine unambiguous β − feeding data, as outlined above in Sect. 2.2.
2.4 Specific activity and mass spectrometry
Accelerator mass spectrometry (AMS) and thermal ionization mass spectrometry (TIMS) have been successfully used
to determine the half-lives of long-lived radionuclides by
counting the number of ions of interest after acceleration,
and relating these data to the specific activity of the radionuclide in the ion source. Normal procedures involve
irradiation processes to generate the radionuclide of interest, followed by purification through the removal of undesirable elements/species by chemical separation. Small
fractions of the resulting purified solutions are used to prepare targets for mass spectrometric studies in order to determine radionuclide/element ratios, and measurements are
also made on carefully weighed bulk samples to determine their specific γ -ray activities by means of standard
619
γ -counting techniques. The half-life of the radionuclide of
interest is determined by substituting the results of the two
forms of measurement into the basic equation of radioactive
decay.
Half-lives of approximately 20 to 50 years and above
can prove awkward to measure by standard spectroscopic
techniques, and have been shown to benefit from quantification via ultrasensitive mass-spectrometric measurements of isotopic concentrations. Examples of the successful adoption of this approach include 32 Si (half-life
of 133 ± 9 a [45]), 44 Ti (half-life of 54.2 ± 2.1 a [46]),
60
Fe (half-life of (1.5 ± 0.3) ×106 a [47]), 126 Sn (half-life
of (2.07 ± 0.21) ×10+5 a [48, 49] and (2.35 ± 0.07) ×10+5 a
[50]). Similar studies have also been carried out by a combination of inductively-coupled plasma mass spectrometry (ICP-MS) and specific activity measurements to determine the half-lives of 79 Se (half-life of (3.77 ± 0.19) ×
10+5 a [51]) and 126 Sn (half-life of (2.33 ± 0.10) × 10+5 a
[52] and (1.98 ± 0.06) × 10+5 a [53]). Further mass-spectrometric studies should be encouraged to address existing
anomalies and uncertainties that remain in half-life values
for long-lived radionuclides of recognised importance (i.e.
32
Si, 60 Fe, 59 Ni, 79 Se and others).
3. Recommended decay data
Compilations and evaluations of nuclear data have been produced since the early 1930s to inform and assist nuclear
physicists, α and γ spectroscopists, and basic nuclear science researchers. More specifically, extended libraries of
reaction cross sections, fission yields, nuclear structure and
decay data have evolved in well-defined formats for application by nuclear engineers and plant operators in power
generation, fuel reprocessing and waste management. As
outlined below, such libraries have historically been updated
over agreed time intervals either by means of international
consensus, or more localised efforts based on immediate national needs. Regular improvements to and subsequent controlled studies of the contents of a decay-data library also
provide a rapid means of assessing their applicability and
suitability – such activities assist greatly in defining further
requirements to improve the existing decay data.
3.1 Decay-data files
Consideration has been given to the most comprehensive
databases that are judged to be most relevant to defining the
status of and existing requirements for improved decay data:
1) ENSDF (Evaluated Nuclear Structure Data File) –
consists of nuclear structure and decay data for all known
radionuclides (www.nndc.bnl.gov/ensdf/). Complete mass
chains are evaluated at regular intervals (nominally every
seven to ten years) by members of the International Network of Nuclear Structure and Decay Data Evaluators,
and published in Nuclear Data Sheets [10]. The strength
of ENSDF is to be found within the completeness of this
comprehensive database (e.g. see Fig. 5 for the IT decay
data of 99m Tc in ENSDF). NuDat represents an electronic
chart of the nuclides based primarily on the contents of
ENSDF and constitutes a user-friendly means of accessing decay data (www.nndc.bnl.gov/nudat2/), while MIRD
Unauthenticated
Download Date | 6/12/17 1:06 PM
620
A. L. Nichols
Fig. 5. Nuclear data sheet for the IT decay of 99m Tc (ENSDF); comparison with equivalent data in Ref. [54] reveals some subjective differences –
e.g. 140.511-keV γ emission, with recommended Pγ of 89(4)% in ENSDF and 88.5(2)% in DDEP.
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
621
Table 1. Sub-libraries of decay-data files in ENDF-6 format for nuclear applications.
Sub-library
Year
No. of
nuclides a
Comments
JENDL-FP b [68]
2001
1229
From ENSDF + gross β theory
JEFF3.1.1 [69]
2007
3852
From NUBASE [72], DDEP, UKPADD6.7 [73] c,
UKHEDD2.5 [74] d and ENSDF + TAGS data e
ENDF/B-VII.1 [71]
2011
3817
From ENSDF + extension of atomic radiation +
delayed-neutron emissions + TAGS data e
a: Specified number of nuclides also includes files of stable nuclides.
b: New version in preparation: ENSDF + TAGS data + delayed neutrons (Fukahori, T., JAEA, private
communication, May 2011).
c: More recent version available as UKPADD6.11 [75].
d: More recent version available as UKHEDD2.6 [76].
e: Average β and γ energy data obtained from various dedicated gross βγ and TAGS studies (Total
Absorption Gamma-ray Spectroscopy).
(Medical Internal Radiation Dose) generates the result of
processing ENSDF decay data through the RADLST code
to give the energies and intensities of all emitted radiation, along with their dose rates (www-nds.iaea.org/mird/).
NSR (Nuclear Science References) is an ancillary bibliographic database through which mass-chain evaluators
and other users can accesses all publications of interest
(www-nds.iaea.org/nsr/index.jsp).
2) DDEP (Decay Data Evaluation Project) – contains
comprehensive atomic and nuclear decay data evaluations
of selected radionuclides, with emphasis placed on the completeness of each decay scheme and the derivation of X-ray
and electron decay data [54–60]. Multinational evaluations
are submitted via a coordinator to the custodian of both the
database and associated comments files at the Laboratoire
National Henri Becquerel, CEA Saclay, France. Comprehensive decay data for 194 radionuclides are contained
within the DDEP files (www.nucleide.org/DDEP_WG/
DDEPdata.htm), as observed on 4 June 2012.
3) Relevant IAEA databases – a number of nuclear
data initiatives organised as Coordinated Research Projects
(CRPs) under the auspices of the International Atomic Energy Agency (IAEA) have resulted in the generation of highquality decay data.
a) Update of X ray and gamma ray decay data standards for detector calibration and other applications, 1998–
2005 [61–63], www-nds.iaea.org/xgamma_standards/,
www-nds.iaea.org/publications/tecdocs/sti-pub-1287_Vol1.
pdf, www-nds.iaea.org/publications/tecdocs/sti-pub-1287_
Vol2.pdf. Nuclides within this particular database of high
relevance to nuclear medicine include 60 Co, 64 Cu, 66 Ga,
67
Ga, 99m Tc, 111 In, 123 I, 125 I, 131 I, 137 Cs, 153 Sm, 166 Ho, 169 Yb,
192
Ir and 201 Tl [62, 63].
b) Updated actinide decay data library, 2005–2011
[64–66] – data also forwarded for inclusion in the DDEP
database, and listed on the web site www.nucleide.org/
DDEP_WG/DDEPdata.htm. Nuclides within this particular
decay database address requirements in (i) nuclear power
generation with the inclusion of all important Th, Pa, U, Np,
Pu, Am and Cm radionuclides and their natural decay products, and (ii) nuclear medicine applications identified with
212
Bi (228 Th decay chain), 213 Bi (229 Th/225 Ac decay chain),
211
At/211 Po, 223 Ra (within 227 Ac decay chain), 241 Am and
Cf [66].
Other nuclear data libraries have been assembled and
subsequently updated in various ways, based on the guidance and requirements of the nuclear power industry and
related fuel-cycle activities. These decay-data sub-libraries
have been prepared via a combination of evaluation and
direct adoption of recommendations from respected data
sources (e.g. data extraction from ENSDF, DDEP and other
evaluated atomic and nuclear data files). These recognised nuclear applications databases are maintained in
the internationally-accepted ENDF-6 format [67], and are
briefly described in Table 1. JENDL-FP files have been
assembled by staff working at the Japan Atomic Energy Research Institute [68], and now part of the Japan Atomic Energy Agency; JEFF3.1.1 constitutes a combination of multinational assessments and evaluations carried out under the
auspices of the Nuclear Energy Agency of the OECD [69];
ENDF/B-VII.1 is a predominantly USA initiative with
a number of significant international inputs (latter are mainly
files dedicated to nuclear reaction excitation functions) and
retention of various data from the earlier ENDF/B-VII.0
library [70, 71]. The decay data include half-lives, decay
modes and Q-values, branching ratios, average decay energies, α, β, EC/β + , Auger-electron, conversion-electron, γ ,
X-ray, etc. energies and emission probabilities, and various
other nuclear parameters (e.g. internal conversion coefficients), along with comprehensive uncertainty data.
Communication links with many electronic decay-data
files are rapid and comparatively easy to implement in
the age of the PC, Internet, CD and DVD. As mentioned
above, NuDat provides a user-friendly means of extracting decay data from ENSDF (www.nndc.bnl.gov/nudat2/);
LiveChart also accesses ENSDF, and offers the user a wide
range of procedures to interrogate this database and display the nuclear parameters of interest in various ways
(www-nds.iaea.org/relnsd/vchart/index.html). JANIS constitutes an equivalent software platform for the rapid inspection and display of numerical data within the JEFF nuclear
data library (www.oecd-nea.org/janis/).
Dedicated catalogues of γ -ray spectra have been assembled to assist greatly in the characterisation and quan252
Unauthenticated
Download Date | 6/12/17 1:06 PM
622
tification of the radioactive content of materials [77, 78].
Systematic studies of the γ -ray emissions of individual radionuclides have been carried out by means of NaI(Tl)
scintillation, Si(Li), Ge(Li) and HPGe detectors, and these
“fingerprint” spectra are of immense value in spectroscopic
analyses. With the advent of the Internet, these γ -ray spectrum catalogues and enhancements have conveniently been
made available in electronic form through the Web site
http://www.inl.gov/gammaray/catalogs/catalogs.shtml, for
NaI – http://www.inl.gov/gammaray/catalogs/pdf/naicat.pdf,
and for Ge and Si(Li) detectors – http://www.inl.gov/
gammaray/catalogs/pdf/gecat.pdf.
3.2 Status of decay data
Important work continues or is being planned to explore
further structural facets of the nucleus, particularly through
the use of radioactive ion beams to study specific areas of
the chart of the nuclides in a highly focussed manner. Furthermore, significant efforts are constantly being made to
respond fully to the demands of decay-data users in support
of their energy and non-energy applications. Accurate measurements and sound evaluations of decay data have been
proposed and are underway to provide information to assist
in basic nuclear physics research and ensure the efficacy and
validity of nuclear data as applied to fission and fusion reactor physics, nuclear medicine and analytical science.
Some of the sub-libraries of recommended decay data
are primarily dedicated to reactor operations and fissionbased fuel cycles (JENDL-FP, JEFF3.1.1 and ENDF/BVII.1), although they can be used further afield for fusion
research studies and various non-energy applications, if desired. Updating of these ENDF-6 decay-data files is predominantly reliant on the regular evaluation efforts within the
ENSDF initiative, although some sub-libraries do contain
a limited number of recommended decay-data files that have
been individually evaluated and assembled in a more dedicated manner (e.g. within JEFF3.1.1). DDEP evaluations
are based on the implementation of a series of agreed evaluation procedures, with the aim of assembling high-quality
files of recommended decay data of immediate value as standards in radionuclide metrology; these particular data sets
have also been assessed and are now supported by the Bureau International des Poids et Mesures (BIPM) as a means
of encouraging worldwide adoption.
Specific inadequacies and uncertainties remain to be
addressed with respect to the decay-scheme data for a number of radionuclides, whether considering either a particular radionuclidic application (e.g. nuclear medicine), or
encompassing a relatively large number of radionuclides
(e.g. shielding and decay heat calculations). These envisaged needs are discussed in Sects. 4 and 5, below, covering
such disparate issues as power reactor control and safety,
shielding/storage of irradiated fuel, radiation dosimetry, nuclear medicine, radioactive dating, and astrophysics. Further
work is required to build on previous initiatives such as
IAEA CRPs through consideration of possible decay-data
needs over the next 5 to 15 years. Improvements to some
of the existing data are required, along with new additions
to ensure that some pre-emptive measures are in place to
address our future needs.
A. L. Nichols
4. Applications in reactor technology
Along with various neutron-induced cross sections as
a function of neutron energy, the decay data of actinide
fuels, their (n, γ ) reaction products and heavy-element decay chains, fission products and activation products are
important inputs to the calculation of the radionuclide inventories generated by irradiated fuel bundles within the
reactor core of a power reactor. Such inventory data are
essential in the plant design (particularly the provision of
adequate shielding), operational safety measures that include annual shutdown procedures, decommissioning, fuel
handling, storage and reprocessing, and waste disposal. Furthermore, studies of efficient transmutation by means of the
recycling of high burn-up fuel need to be assessed from
the points of view of power production and reducing the
quantities of long-term actinide and fission-product waste
inventories.
Stable and radioactive nuclides introduced into inventory
calculations are of the order of 120 actinides and heavyelement nuclides within their decay chains, 1050 fission
products, and 700 possible activation products. While the
decay data of the important actinides (identified as specific
Th to Cf radionuclides), their heavy-element decay-chain
products and the commonly-occurring activation products
are judged to be sufficiently well quantified for purpose,
a number of notable fission products merit improvement and
further experimental study (see below).
4.1 Normal operational characteristics of reactor
systems
Many technical features of reactor operations such as criticality and power distributions are basically dependent on
neutron physics (neutron-induced cross sections, angular
distributions, secondary energy distributions, and ν̄ (average
prompt neutron emissions)). The importance of well-defined
decay data arises when consideration is given to the following: (a) shielding requirements, (b) proposed utilisation of
recycled and high burn-up fuel, and (c) irradiated fuel storage and reprocessing, along with the subsequent needs of
waste management.
Power, rod worth and structural damage are regularly assessed during plant operation, and in this regard the decay of
short-lived fission and activation products need to be known.
Furthermore, changes occur in the fuel, structure and absorber materials under neutron irradiation, and the half-lives
and emissions of all major fission products (of the order of
90 radionuclides) and the actinide decay chains are required
as inputs in such analyses. Modelling codes have been developed to determine neutron and gamma transport within
and in close association with the reactor core. The gamma
decay data are normally grouped into bins for ease of calculation, covering the energy range from zero to 10 MeV.
Half-lives and branching fractions are also required as input and, together with inventory calculations, provide the
means of performing time-dependent studies of the necessary shielding requirements. Equivalent shielding studies are
also undertaken for irradiated fuel storage, transport, reprocessing and disposal. All of the required decay data originate
from ENDF-6 files [68, 69, 71], and are judged to be accurately known.
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
4.2 Decay heat
A sound knowledge of the time-dependent energy release
from radioactive nuclides is extremely important in formulating safe operational procedures for nuclear power reactors, identified primarily with the need to maintain cooling to
previously irradiated fuel. Accurate estimates of the resulting decay heat are needed in safety assessments of all types
of reactor and fuel-handling plant, the storage of spent fuel,
the transport of fuel-storage flasks, and the intermediateterm management of any resulting radioactive waste.
Actinide and fission-product inventories are calculated
for the specified conditions during reactor operation and
the subsequent cooling period. These data are used in conjunction with the radionuclidic half-lives, and all heavyparticle, light-particle and electromagnetic radiation characteristics to determine the total energy release rates for
heavy-particles, light-particles and electromagnetic radiations [79–81]:
M
i
λTi Ni (t)E HP
HHP (t) =
623
of γ -ray singles data to calculate β − transitions by means
of gamma population-depopulation balances of the proposed
nuclear levels [82]. TAGS (Total Absorption Gamma-ray
Spectroscopy) measurements can overcome these difficulties, and provide the necessary mean beta and gamma decay
energies for sound decay heat calculations [37, 38, 41, 83].
i=1
HLP (t) =
M
i
λTi Ni (t)E LP
i=1
HEM (t) =
M
i
λTi Ni (t)E EM
i=1
where HHP (t), HLP(t) and HEM (t) are the total decay heat of
the heavy-particle, light-particle and electromagnetic radiations, respectively, at time t after reactor shutdown; λTi is the
total decay constant of radionuclide i; Ni (t) is the number of
i
i
i
, E LP
and E EM
are
atoms of radionuclide i at time t; and E HP
the energy release rates for heavy-particle, light-particle and
electromagnetic radiations, respectively, per disintegration
of radionuclide i. The heavy-particle component includes
α, neutrons, protons, recoil nuclei and fission fragments;
light particles are defined as β − , β + , Auger electrons and
internal-conversion electrons; and electromagnetic radiation
is identified with γ , X-rays, annihilation radiation and internal bremsstrahlung. Neutron-induced cross sections, fission yields and radioactive decay data constitute the input
to the summation calculations used to determine the release
of decay heat as a function of time after the termination
of neutron-induced fission [79–81]. These calculations require the inclusion of mean α, β and γ energies derived
normally from the discrete α, β and γ energies and emission
probabilities for a significant number of fission products,
and the results are compared with experimental decay-heat
benchmarks. However, the determination of β − emission
probabilities has long been problematic in decay-scheme
studies. Although γ -ray emission probabilities and internal
conversion coefficients can be used to derive β − feeding to
daughter nuclear levels, all forms of singles-based Ge detector possess low intrinsic efficiency for the detection of
high-energy γ rays above ∼ 1.5 MeV that undermines such
an exercise. Furthermore, the determination of direct β − decay to the ground state of the daughter nucleus can pose even
more serious problems for various other reasons. Hardy et
al. have demonstrated that ∼ 20% of the true γ -ray intensity
above 1.7 MeV for a fictional radionuclide (Pandemonium)
may remain undetected, impacting significantly on the use
Fig. 6. Decay-heat calculations for irradiated 239 Pu as a function of
cooling time in terms of (a) total energy release rate per fission second,
(b) light-particle/electron energy release rate per fission second, constituting the β − , β + , Auger and conversion electron components, and
(c) electromagnetic energy release rate per fission second, constituting
the γ , X-rays, annihilation radiation and internal bremsstrahlung components. Tobias (1989) denotes benchmark data for 239 Pu as determined
by a least squares fit to all available measured data [84]; JEFF311
defines the calculated decay heat when the JEFF3.1.1 decay-data sublibrary was adopted [69] in which TAGS data from Greenwood et al.
had been included [38]; JEFF311 + TAGS are equivalent decay-heat
calculations in which TAGS data from Algora et al. had also been
added [41].
Unauthenticated
Download Date | 6/12/17 1:06 PM
624
A. L. Nichols
Table 2. Requested TAGS measurements for decay-heat studies of Th-U and U-Pu fuels.
Radionuclides
Common to Th-U and U-Pu fuel
Br, 87 Br(β − n), 88 Br(β − n), 89 Kr,
Kr, 92 Rb, 96 Y, 99 Zr, 100 Zr, 98 Nb,
99
Nb, 100 Nb, 101 Nb, 102 Nb, 103 Mo,
102
Tc, 103 Tc, 104 Tc, 132 Sb, 135 Te, 136 I,
136m
I, 137 I(β − n), 137 Xe, 139 Xe, 140 Xe
Additional for U-Pu fuel
86
90m
90
105
Rb a , 89 Sr, 97 Sr, 105 Mo,
Tc, 106 Tc, 107 Tc,
142
Cs(β − n), 145 Ba a , 143 La a ,
145
La a
Additional for Th-U fuel
85
Se, 86 Se, 84 Br, 89 Br, 87 Kr, 91 Kr, 88 Rb,
Rb, 92 Sr, 96m Y, 97 Y, 98 Zr(?), 99m Nb,
100m
Nb, 102m Nb, 101 Mo, 128m Sb, 129m Sb,
130m
Sb, 133 Sb, 138 Xe, 139 Ba, 141 La, 146m La
94
a: TAGS measurement recommended in repeat of equivalent studies by Greenwood et al. [38].
As determined from the TAGS measurements of Greenwood et al. [38], total mean β − and γ energies ( Ē β− and
Ē γ ) for twenty-nine fission products of importance in decayheat calculations have been incorporated into the JEFF3.1.1
decay-data sub-library [69] to replace inadequate values that
arose from the evaluation of gamma-ray spectroscopic studies. However, even with these more reliable data in place,
significant disagreements are still observed when the reformulated decay-heat calculations are compared with available benchmark data [84]. As shown in Fig. 6, calculations
of the total and component energy release rate per fission
second for thermal-neutron irradiated 239 Pu, in which the adjusted JEFF3.1.1 decay data were used, differ significantly
from the decay-heat benchmark at cooling times between
5 and 8000 seconds (i.e. up to 2.2 h). Under these circumstances, WPEC Sub-group 25 (SG-25) of the NEA-OECD
addressed the requirements for additional experimentallyderived fission-product decay data of relevance to 235 U and
239
Pu reactor systems, and emphasised the need for further
TAGS measurements [85]. A similar assessment exercise
has been undertaken for Th-U fuel in which 233 U(n,f) occurs – while U-Pu and Th-U fuels exhibit much in common,
there are also a number of notable differences [86]. The two
sets of proposals for new TAGS studies are brought together
in Table 2. Some of the listed radionuclides represent repeat
measurements of Greenwood et al. as a sensible means of
cross checking different sets of TAGS data [38]. A consequence of these particular assessments is that recent dedicated TAGS studies have focussed on the β − decay of 101 Nb,
105
Mo and 102,104,105,106,107 Tc [41]. As depicted in Fig. 6, these
additional measurements have clearly addressed much of the
long-standing discrepancy in the γ component of the decay
heat for 239 Pu between cooling times of 5 and 8000 s [87].
However, the same cannot be said for the equivalent 235 U
decay-heat calculations – very little change arises from the
introduction of the new decay-energy data, and significant
disagreements with the decay-heat benchmark remain for
cooling times up to 4000 secs. This significantly differing
impact of thermal-neutron fission on the release of decay
heat from 235 U and 239 Pu can be attributed to the marked
differences between the light-peak fission yields of the two
systems. While further TAGS measurements are underway
to study the β − decay of 87,88 Br, 94 Rb and 137 I [88], much
remains to be done as specified above.
4.3 Other reactor-related issues
Delayed-neutron decay is an important process in the control
of nuclear fission, as well as providing insights into uncertain features of nuclear structure and the population of un-
bound levels of nuclei. Extensive studies of delayed-neutron
and related gamma-ray emissions have been undertaken by
means of singles and coincidence counting techniques in
order to provide level-density information and well-defined
evidence of complex β − n decay for many important fissionproduct nuclides [89–93]. However, various short-lived fission products that undergo β − n decay still remain to be
characterised in a similar manner, along with other delayedneutron emitting nuclides of both lower and higher mass to
assist in astrophysical and basic nuclear structure investigations [94].
Antineutrinos are emitted as part of the β − -decay process
of fission products generated in the reactor core:
A
Z
X → Z+1A Y + e− + ν̄,
and undergo virtually no attenuation in their flux over long
distances. Therefore, their unchanged spectral signature
could be used to monitor the efficacy of reactor operations based on the nature of the irradiation, particularly with
respect to the detection of clandestine procedures and unannounced fuel movements. Various collaborations have aided
in the development of antineutrino detection techniques to
probe reactor operations non-invasively [95, 96]. Reliable
fission-product databases are also required that contain radionuclides from which the uncertainties identified with
Pandemonium have been removed by measurement (see
Sect. 4.2), allowing β − -decay data to be used with confidence in the derivation of predicted antineutrino spectra for
comparison with and interpretation of the measured antineutrinos [88].
5. Non-energy based applications
The nature and properties of radioactivity can be successfully used in a significant number of non-energy based applications. Some applications are highly significant because
there are no satisfactory alternatives, while others represent
important supportive procedures in various forms of integrated multi-method approach (e.g. combinations of medical
treatment: surgery-chemotherapy-radiotherapy).
5.1 Radiation dosimetry
Quantification of the absorption of atomic and nuclear radiation is important in defining the dose received and damage inflicted on structural materials and human tissues, and
hence the consequences of exposure to all forms of radioactive emission. Radiation dose refers to the amount of energy
deposited in matter and the resulting biological effects that
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
625
Table 3. Radionuclides used commonly in nuclear medicine for gamma imaging of body functions: relevant
decay properties [10, 54–59].
Radionuclide
Half-life
Noteworthy gamma emissions: E γ (keV), Pγ (%)
67
Ga
3.2613(5) d
81
Rb/81m Kr generator
81m
93.307(12), 38.1(7)%; 184.577(17), 20.96(44)%;
300.232(21), 16.60(37)%; 393.528(20), 4.59(10)%
190.46(16), 67.66(32)%
Kr: 13.10 s
Rb: 4.572(4) h
82
Rb: 1.2575(2) min
82
Sr: 25.34(2) d
99m
Tc: 6.0067(5) h
99
Mo: 2.7479(6) d
2.8049(4) d
13.2234(37) h
8.0233(19) d
81
82
Sr/82 Rb generator
99
Mo/99m Tc generator
111
In
I
131
I
123
133
201
Xe
Tl
5.2474(5) d
3.0421(17) d
511 annihilation, 190.9(4)%; 776.52(1), 15.08(16)%
140.511(1), 88.5(2)%
171.28(3), 90.61(20)%; 245.35(4), 94.12(6)%
158.97(5), 83.25(21)%
80.1850(19), 2.607(27)%; 284.305(5), 6.06(6)%;
364.489(5), 81.2(8)%; 636.989(4), 7.26(8)%
80.9979(11), 37.0(3)%
135.312(34), 2.604(22)%; 167.45(3), 10.0(1)%
are dependent on such parameters as radionuclidic activity,
energy of the radiation, time of exposure, and distance from
the source. Data requirements for dosimetry studies are as
follows:
1. Isotopic abundances for all target elements,
2. Cross-section data for perceived nuclear reactions,
3. Radiation damage cross sections, and
4. Decay data of all reaction product nuclides.
Overall nuclear data requirements need to cover the operation of accelerators, reactor cores and their fuel cycles,
and all relevant features of nuclear medicine involving diagnosis, therapy, magnetic resonance imaging and associated
research studies.
Safe operations of reactor power plant, related fuel-cycle
processes and non-energy-based nuclear procedures are determined from the perspective of the envisaged radiation
dose rates and the need to undertake reputable calculations
in the design and introduction of mitigating features such
as appropriate shielding. Dedicated libraries of nuclear data
have been assembled to assist in such analyses, and would
normally include sub-sets of reaction-product decay data.
The International Reactor Dosimetry File IRDF-2002 was
released in 2005/2006 [97], and has become internationallyrecognised as a validated source of data assembled in the
desired format for safety studies of fission-reactor systems.
This file contains decay data for 85 radionuclides (58 ground
states, 25 first isomeric states, and two second isomeric
states), including half-lives, decay modes and intensities
as taken from ENSDF (see Sect. 3.1, and Ref. [10]) and
reformatted for nuclear applications. Proposals have been
formulated to extend IRDF-2002 further as IRDFF-1.0 (International Reactor Dosimetry and Fusion File) in order
to encompass fusion systems [98, 99] – good progress has
been made in this respect with the introduction of newlyevaluated excitation functions and related decay data [100].
5.2 Nuclear medicine
Both diagnostic and therapeutic nuclear procedures extend
across a wide range of medical activities to address and benefit human health in a safe and efficacious manner [101].
Specific radionuclides have been identified as potentially
suitable for various life-saving applications. While their production routes and decay properties need to be defined with
confidence, some deficiencies remain, especially with regard
to the optimum generation of specific radionuclides, either
the minimization or elimination of impurities, and the accurate quantification of various decay parameters [102–104].
The latter requirements include a sound knowledge of the
half-life and α, β − , Auger-electron, conversion-electron, β + ,
γ and X-ray energies and emission probabilities as appropriate for patient dose-rate calculations.
Various radionuclides of the desired purity and decay
characteristics have been adopted for the diagnostic imaging of physiological and biochemical processes within the
human body. Nuclear techniques such as Single-Photon
Emission Computer Tomography (SPECT) and Positron
Emission Tomography (PET) complement other imaging
methods (e.g. magnetic resonance and ultrasound) to furnish an extremely powerful means of detecting functional
abnormalities and disease. A number of γ -emitting radionuclides possess decay characteristics that are highly suitable
for diagnostic studies by means of gamma cameras (Table 3)
– their chemical form is particularly important in ensuring efficient and precise delivery to the body function(s) of
interest.
Charged-particle cyclotrons and linear accelerators are
increasingly being used to generate radionuclides for both
diagnostic and therapeutic purposes [105, 106], along with
nuclear reactors employed to produce various activation and
fission products for similar applications. Sealed sources of
60
Co and 137 Cs provide external γ beams that penetrate
the body and constitute the means of controlled therapeutic treatment to internal tumours. Studies of heavy-ion beam
therapy have provided striking evidence for the accurate
delivery of a well-defined, localised dose to a particular
site, and carbon-ion beams exhibit particular promise in this
respect. Brachytherapy involves the use of sealed sources
placed in or close to the tumour, while attempting to ensure minimal damage to healthy tissue – 103 Pd, 125 I (as Xray emitters), 137 Cs and 192 Ir (as γ emitters) with effective
ranges of a few centimetres are commonly used, while β −
Unauthenticated
Download Date | 6/12/17 1:06 PM
626
emitters include 32 P, 90 Y and 188 Re with effective ranges of
a few millimetres. Radio-immunotherapy involves the covalent bonding and labelling of monoclonal antibodies and
peptides with radionuclides such as 90 Y, 131 I, 153 Sm and 213 Bi
for injection into the bloodstream, followed by transport and
attachment to tumours. PET has become an extremely noteworthy and successful technique for the diagnosis of cancer
– the most popular radionuclide for such studies has been 18 F
(half-life of 1.83 h), which requires the radionuclide production and patient treatment facilities to be close to each other
geographically.
The proposed use of radionuclides in nuclear medicine
necessitates a sound knowledge of their production cross
sections, half-lives and decay schemes, and much effort has
been expended to derive such data through measurement and
evaluation. IAEA initiatives have included a Coordinated
Research Project (CRP) on “Charged particle cross-section
database for medical radioisotope production: diagnostic radioisotopes and monitor reactions” to consider the nuclear
data requirements for diagnostic radionuclides [107], followed by an equivalent study for therapeutic radionuclides
defined as “Nuclear data for the production of therapeutic radionuclides” [108]. While both projects were primarily dedicated to measurements and evaluations of relevant
cross sections for product nuclides and impurities, limited
amounts of recommended decay data were tabulated from
ENSDF [10].
An IAEA consultants’ meeting was held from 3 to 5
September 2008 in Vienna, Austria, dedicated to “Highprecision beta-intensity measurements and evaluations for
specific PET radioisotopes”. Participants assessed the decay
data for approximately 50 positron-emitting radionuclides,
and recommended a series of measurements and evaluations to improve the known decay characteristics of existing and potential PET nuclides [109]. Furthermore, an
IAEA consultants’ meeting was held at the same venue from
21 to 24 June 2011 to discuss “Improvements in chargedparticle monitor reactions and nuclear data for medical isotope production”, and formulate a work programme for
a Coordinated Research Project aimed at improving the excitation functions of charged-particle monitor reactions and
the nuclear decay data for a number of medical radionuclides [110].
Continued developments in medical imaging and therapy will involve the utilization of improved diagnostic and
therapeutic techniques, along with the production of potentially more effective and suitable radionuclides. Such an
envisaged set of circumstances merits the consideration of
future needs to expand and improve the content of nuclear
databases for medical applications. Thus, a further technical meeting was organised by the IAEA from 22 to 26
August 2011 in which invited specialists were asked to assess “Intermediate-term nuclear data needs for medical applications: cross sections and decay data” [111]. A summary of their recommendations for decay data is given
below, based on the envisaged requirements for (a) diagnostic γ -ray emitters, (b) positron emitters, (c) therapeutic β − , X-ray and γ -ray emitters, (d) therapeutic Augerelectron emitters, and (e) therapeutic α emitters, and covering an estimated timescale of approximately fifteen years.
The reader is also referred to the original IAEA report for
A. L. Nichols
the recommended measurements and evaluations of excitation functions in order to optimize the production of these
radionuclides [111].
5.2.1 Diagnostic γ -ray emitters
Reactor-produced 99m Tc is the most commonly used γ -ray
emitting radionuclide for diagnostic purposes, and both the
cross-section and decay data are well known. Decay data for
67
Ga, 97 Ru, 111 In, 123 I, 147 Gd, 201 Tl and 203 Pb are also reasonably well defined. Both 67 Ga and 111 In possess relatively
long half-lives and are rarely used anymore for diagnostic
purposes, although they have been adopted as therapeutic
radionuclides (see Sect. 5.2.4); 99m Tc: Auger-electron and
other low-energy electron decay data are required to assess
possible application in microdosimetry; 123 I: Auger emissions may become an issue, if therapeutic applications arise
in the future.
5.2.2 Positron emitters
Excitation functions for the four most commonly used shortlived positron emitters in PET studies have been recently
evaluated and well quantified (11 C, 13 N, 15 O and 18 F [107]).
Noteworthy decay data needs are as follows: 57 Ni, 66 Ga,
72
As, 73 Se, 75 Br, 76 Br, 77 Kr, 81 Rb, 82m Rb, 83 Sr, 86 Y, 89 Zr,
94m
Tc, 120 I and 121 I: decay-data measurements and evaluations are required; 44 Ti/44 Sc, 52 Fe/52m Mn, 62 Zn/62 Cu,
72
Se/72 As and 140 Nd/140 Pr generators: decay-data measurements and evaluations are required.
5.2.3 Therapeutic β −, X-ray and γ -ray emitters
Comprehensive production cross sections and relevant decay
data for β − -emitting radionuclides used to perform internal
radiotherapy have undergone study in a recent IAEA CRP
(see IAEA Technical Reports Series No. 473 for the production of 32 P, 89 Sr, 90 Y, 131 I, 186 Re, 188 Re and others [108]).
The decay data of sources used commonly in external radiation therapy (e.g. 60 Co and 137 Cs) and brachytherapy (e.g.
192
Ir) are also well defined. Focus is best placed on β −
emitters with known discrepant data, and radionuclides believed to possess future therapeutic potential (specifically
low-energy β − and X-ray emitters): 67 Cu, 103 Pd, 161 Tb, 169 Er
and 175 Yb: decay-data measurements and evaluations are required; 191 Pt/191m Ir generator: require decay-data measurements and evaluation of 191 Pt parent.
5.2.4 Therapeutic Auger-electron emitters
125
I is the most commonly used Auger-electron emitter for
internal radiotherapy – both reactor-production and decay
data are well characterized. The following radionuclides are
also identified as potentially suitable for application with respect to microdosimetry at the molecular and cellular levels,
and therefore would require much improved Auger-electron
decay data: 67 Ga, 71 Ge, 77 Br, 99m Tc, 103 Pd, 111 In, 123 I, 140 Nd,
178
Ta, 193m Pt, 195m Pt and 197 Hg.
5.2.5 Therapeutic α emitters
230
U/226 Th: decay-data measurements and evaluations are
required.
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
5.3 Neutron activation analysis
When nuclear research reactors became more accessible in
an increasing number of countries during the 1960s, neutron
activation analysis (NAA) evolved as a common method of
determining low-level concentrations of the elements. Thus,
a flux of 2 × 1013 n cm−2 s−1 provided the means of achieving detection limits of 10 ng or less for about 50 elements,
given that any radiation from many interfering radionuclides
can be removed by radiochemical separation.
The introduction of solid-state Ge crystals as gammaray detectors refined simultaneous detection considerably,
and instrumental neutron activation analysis (INAA) and
prompt gamma-ray neutron activation analysis (PGAA)
became extremely powerful, non-destructive techniques.
These neutron-activation procedures are capable of simultaneous, in-situ multi-element assay in a rapid, quantitative
manner across almost all of the Periodic Table from hydrogen to uranium. Elemental coverage of PGAA complements
that of conventional, delayed INAA, and the list of measurable elements includes the low Z and high abundance
elements in organic and geological materials, along with
high cross-section elements such as B, Cd, Sm and Gd.
Analyses of hydrogen and boron are especially important
because of the paucity of other reliable analytical techniques
for trace levels of these two elements. Together, PGAA and
INAA can measure all elements except oxygen in most common materials.
Nearly every neutron capture involves the (n, γ ) reaction, and therefore the yield of prompt γ rays per neutron
is greater than that of delayed γ rays. Unfortunately, PGAA
usually has a poorer sensitivity compared with that of INAA
because the neutron flux is some five orders of magnitude
lower in an external reactor beam than for irradiation adjacent to the core. Over the previous 20 years, the adoption of PGAA has increased because of the growing availability of high-flux thermal and cold beams from neutron
guides [112]. Such guided beams can be made free of fast
neutrons and superfluous γ rays to give improved signalto-background ratios and spectral quality. Comprehensive
review articles and books dedicated to PGAA have also been
regularly published [113–115].
A major advance in PGAA was the assembly of a comprehensive compilation of more than 10,000 neutron-capture
γ rays of the elements [116], quantified in terms of their
energies, abundances and cross sections. Furthermore, a substantial computer readable sub-set of these data was made
available on diskette (International Nuclear Geophysics
Database-90 (INGD-90)), along with an IAEA Technical
Report [117]. This work continued through an IAEA initiative from 1999 to 2005, designed to improve the quality and
quantity of the nuclear data in order to apply PGAA reliably
and with much greater confidence in such fields as materials
science, chemistry, geology, mining, archaeology, environmental monitoring, food analysis and medicine [118].
Despite what has been written above, there are recognised to be two drawbacks to the use of all forms of neutron
activation analysis: (a) even though the technique is essentially non-destructive, the neutron-irradiated sample may
remain radioactive for years after analysis, requiring the
need to implement strict handling and disposal protocols; (b)
627
the number of suitable nuclear reactors is declining – with
a lack of irradiation facilities, the technique has declined
in popularity, become more expensive, and has been replaced to a significant degree by ICP-MS/AES (inductivelycoupled plasma mass spectrometry and atomic emission
spectroscopy) and PIXE (proton-induced X-ray emission
spectroscopy).
5.4 Radioactive dating
Natural radioactive decay can be used to determine the age
of samples that contain a rather select number of specific
radionuclides and/or their related in-growth radioactive or
stable daughter nuclides. Atomic bomb tests in the atmosphere over the course of the 1950s and early 1960s, along
with other nuclear activities and accidents, have also generated discrete radioactive markers which provide the means
of dating certain environmental materials and samples accurately. Such changes in nuclidic content are described by
the standard radioactive decay laws, and provide very accurate dating mechanisms based entirely on the half-lives of
the radionuclides involved [119–122].
5.4.1 Time markers
Atmospheric testing of large nuclear devices at specific
times has deposited discrete amounts of radioactivity in the
environment. Under certain circumstances, some of these radionuclides will remain firmly at their original location, and
can be subsequently used as time markers. Thus, 3 H, 14 C,
137
Cs and 239 Pu are known to mark the years 1962–63 accurately, and are firmly absorbed onto soils, sediments and
other materials, with the possibility of being buried by sedimentation and soil-forming processes, as well as by snow
precipitation.
Cosmogenic radionuclides are produced in the earth’s
atmosphere by the interactions of high-energy cosmic radiation with various available atoms such as nitrogen and oxygen. An important nuclide in this respect is 14 C within the
natural CO2 bio-cycle, for which the sensitivity of detection
has increased dramatically with the advent of accelerator
mass spectrometry (AMS) and the potential to analyse very
small specimens. The most popular radioactive time markers based on direct measurements are listed in Table 4, along
with their recommended half-lives.
5.4.2 Radioactive parent and stable decay product
Specific radionuclides possess half-lives sufficiently long for
a significant fraction of their atoms to be present today, many
years after their formation and incorporation into the solar
system. Identified as geochronometers, their existence provides an accurate means of quantifying the absolute ages
of events that go back to the formation of the solar system,
with even the potential to date events prior to this particularly important process. Several such long-lived radionuclides are listed in Table 5, and their suitability is determined
by a number of critical factors:
– Maintenance of a closed system during the course of radioactive decay to ensure no escape of parent and daughter products from the geological feature/sample.
Unauthenticated
Download Date | 6/12/17 1:06 PM
628
A. L. Nichols
Table 4. Radioactive time markers and their recommended half-lives [10, 54–59].
Parent radionuclide
Half-life
3
12.312(25) y
1.387(12) × 106 a
5.70(3) × 103 a
7.17(24) × 105 a
153(19) y
H
Be
14
C
26
Al
32
Si
Time marker in glaciology and hydrology
Lunar, meteor and marine geosciences, and glaciology
Archaeology, geology, glaciology, hydrology, etc.
Lunar, meteor and marine geosciences
Half-life covers time span inaccessible by 14 C
and 210 Pb studies
3.01(3) × 105 a
Cosmology, geoscience and hydrology
1.61(7) × 107 a
Hydrology, and other possible applications
30.05(8) a
Recent sedimentation rates in aquatic systems, and
accumulation rates of glaciers
210
Pb 22.23(12) a
Dating over the previous 100 to 150 years (e.g. lake
(226 Ra 1.600 (7) × 103 a) sediments and glacier ice)
2.4100 (11) × 104 a
Recent sedimentation rates in aquatic systems, and
accumulation rates of glaciers
10
36
Cl
I
137
Cs
129
226
Ra-222 Rn-210 Pb
239
Pu
Comments
Table 5. Long-lived radionuclidic chronometers applicable to geological and cosmological dating [10, 54–59].
Parentdaughter
40
40
Parent half-life
1.2504(30) ×109 a
K(EC)-40 Ar
K(β − )-40 Ca
4.81(9) ×1010 a
1.02(1) ×1011 a
Rb(β − )-87 Sr
La(EC)-138 Ba
138
La(β − )-138 Ce
147
Sm(α)-143 Nd
176
Lu(β − )-176 Hf
187
Re(β − )-187 Os
190
Pt(α)-186 Os
87
138
1.060(11) ×1011 a
3.76(7) ×1010 a
4.33(7) ×1010 a
6.5(3) ×1011 a
Th and U
decay chains
232
Th-208 Pb
Noteworthy half-lives
232
Th
Ra
228
Th
235
U
231
Pa
227
Ac
238
U
234
U
230
Th
226
Ra
210
Pb
228
235
238
U-207 Pb
U-206 Pb
1.402(6) ×1010 a
5.75(4) a
1.9126(9) a
7.04(1) ×108 a
3.267(26) ×104 a
21.772(3) a
4.468(5) ×109 a
2.455(6) ×105 a
7.54(3) ×104 a
1.600(7) ×103 a
22.23(12) a
Measured
isotope ratio
40
40
Ar/38 Ar
Ca/42 Ca
Sr/86 Sr
Ba/137 Ba
138
Ce/142 Ce
143
Nd/144 Nd
176
Hf /177 Hf
187
Os/188 Os
186
Os/188 Os
Comments
EC branch of 10.75(15)%, and β − branch of
89.25(15)%; tendency towards preference for
40
Ar/39 Ar ratio method (see Sect. 5.4.2)
87
138
EC branch of 65.6(5)%, and β − branch of
34.4(5)%; not commonly used
T1/2 (186 Os(α)) of 2.0(11) ×1015 a;
not commonly used
Measured
isotope ratio
Comments
208
Dating based on secular equilibrium
Pb/232 Th
207
235
206
234
226
Pb/235 U
U/231 Pa
Dating based on secular equilibrium;
disequilibrium studies
Pb/238 U
U/230 Th
Dating based on secular equilibrium;
various disequilibrium studies
Ra/230 Th
– No daughter material incorporated into the geological
feature/sample during or after formation.
– Able to quantify the parent and daughter products to the
desired accuracy.
– Well-defined parent half-lives.
These requirements present significant technical challenges
to geologists, analysts and measurers of decay data (latter in their determination of the half-lives of such longlived radionuclides). However, developments in analytical techniques such as high-precision mass spectrometry
and inductively-coupled plasma optical emission spectroscopy have assisted greatly in improving the accuracy of
geochronology. Furthermore, given the difficulty in measuring the absolute abundance of a specific nuclide, researchers
have benefitted from determining particular isotopic ratios
of the daughter element (Table 5), and using these data
to calculate the date of sample formation based on the
assumption that the system has been closed to both parent and daughter mobility from the time of interest to the
present.
Major natural phenomena prevent the retention of inert
argon (and 40 Ar) within the crystalline structure of many
forms of geological feature, and also result in argon absorption from the atmosphere. Faced with such serious uncertainties in the long-term stability of argon content for sample
analysis and the need to undertake two separate analytical
procedures in order to measure parent potassium and daughter argon, research scientists have increasingly preferred to
date their samples of interest by the more sophisticated
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
quantification of 40 Ar/39 Ar ratios that arise within samples
irradiated in a well-defined fast-neutron flux. Within the
carefully controlled conditions of a suitable nuclear reactor,
39
Ar can only be produced via the 39 K(n f , p)39 Ar reaction,
which is dependent upon the amount of 39 K within the irradiated sample, length of irradiation, neutron-flux density
and neutron-capture cross section of 39 K, whereas the 40 Ar
content arises from the natural EC decay of 40 K. Massspectrometric measurements can be made more precisely on
isotopes of the same element (argon), although corrections
may still be required to allow for the presence of atmospheric argon and interference from other reactor-produced
isotopes. Under these better considered circumstances, studies of 40 Ar/39 Ar ratios are more commonly undertaken in
preference to 40 Ar/38 Ar ratio measurements. Other debatable assumptions and various analytical difficulties also exist
within the other systems listed in Table 5 [120–122], although they will not be considered further in this particular
review.
When deemed to be in secular equilibrium, the three
naturally-occurring decay chains of 232 Th, 235 U and 238 U
to particular stable Pb nuclides constitute independent
geochronometers, based on the parent radionuclides possessing much longer half-lives than their respective daughters (Table 5). Measurements of sample 208 Pb/232 Th, 207 Pb/
235
U and 206 Pb/238 U ratios in conjunction with their
208
Pb/204 Pb, 207 Pb/204 Pb and 206 Pb/204 Pb ratios, respectively,
provide a means of standardising and dating closed geological systems accurately for ages greater than 30 million
years [120, 122]. Non-radiogenic 204 Pb is used as the reference isotope within such samples, possessing a very weak
radioactive half-life for α decay of ≥ 1.4 × 1017 a, which
effectively permits the nuclide to be defined as stable.
Externally-driven geological events can significantly disturb secular equilibrium. If measurements can be made of (a)
subsequent decay of a radionuclide that has been separated
from precursors, or (b) ingrowth of a radioactive daughter, the resulting data can be used to establish the date of
the original geological disturbance (e.g. time at which parent separated from daughter nuclei during a sedimentation
process, and initiated radioactive disequilibrium). Important
information on the geological and geochemical history of
geographical features and deposits can be determined in this
manner [123].
The decay data of importance in radioactive dating are
the half-lives and relevant branching fractions (e.g. for the
EC and β − decay modes of 40 K and 138 La). Geologists, geochemists and other specialists in the field of geochronometry
believe that these parameters need to be known with greater
accuracy in many cases. Uncertainties in the parent half-life
range from 1.0% for 138 La and 147 Sm, 1.6% for 187 Re, 1.9%
for 87 Rb and 176 Lu, to as much as 4.6% for 190 Pt – half-lives
for these long-lived radionuclides need to be determined
with improved accuracy in order to derive more precise ages.
The equivalent data for both 40 K and 87 Rb, and the Th-UPb decay chains are known to higher precision, and therefore
can be adopted in age calculations with greater confidence –
however, there are other more substantial issues to consider
in such studies that relate to analytical difficulties and the
extremely important prerequisite for sample stability over
many years.
629
5.5 Other industrial and research applications
Extremely unfortunate incidents and terrorist activities over
recent years have underlined the essential need to detect,
identify, localise and minimise/eliminate nuclear and radiological threats at both the national and international levels.
Thus, there exists the need to develop increasingly userfriendly nuclear detection and identification systems in order
to improve support towards ensuring the safety and security
of the populace. Recommended nuclear data are a very important aid in addressing criticality safety and sound stockpile stewardship, and preventing the illicit trafficking of nuclear materials. Such onerous requirements include the need
to adopt agreed sub-sets of recommended decay data from
a respected database such as ENSDF [10]. Thus, a particularly specific set of well-defined data have been adopted with
a reasonable degree of confidence in their correctness and
permanency [124], hopefully to ensure a consistently correct
approach through these parameters towards the maintenance
of the desired level of national and international security.
Decay data adopted in such circumstances include the radionuclide half-life, major radiations, and energies of the
main γ -ray emissions to be effectively used as fingerprints
for any radioactivity detected.
Radioactive tracers are often used to measure the rates
of reaction of chemical processes for (a) basic research purposes, (b) optimisation of industrial production routes, and
(c) determination of the movement of molecules through
biological systems and tissue to obtain important physiological data and understanding for application in human
health, livestock control and plant husbandry. A number of
radionuclides have been commonly applied to studies of
complex biochemical, biological and metabolic behaviour
to resolve existing uncertainties, particularly the more suitable radionuclides of H, C, P, S and I. Research studies into
reaction kinetics and mechanisms have also benefited immensely from these labelling techniques. Obvious care has
to be taken to adopt radiotracers that permit the phenomena of interest to be successfully monitored (e.g. by means
of γ -ray spectroscopy), with decay-data parameters defined
sufficiently well that they do not hinder accurate studies of
the chemical reactions and transport mechanisms of interest [125–127].
Accurate information describing the spatial distribution
of a wide range of minerals in the Earth is an essential requirement for the development of economic routes in the
exploration, extraction and processing of oil, coal, metalliferous and non-metalliferous materials, including such properties as total clay content, grain density and porosity. Rapid
on-line elemental analysis of natural products such as oil and
coal (H, C, N, O, Al, Si, S, Ca, Fe), raw minerals for construction (O, F, Na, Mg, Al, Si, P, S, K, Ca, Ti, Mn, Fe),
and mixed ores for manufacture (Al, Mn, Fe, Ni, Cu, Ag, Au
and others) can be achieved by means of nuclear borehole
logging [117, 127]. The popular neutron activation sources
are 252 Cf, 241 Am-Be and 14-MeV neutron tubes based on
d(t, n)4 He. Decay-data needs that arise from such remote irradiations can be readily adopted from ENSDF [10]: natural
abundances, half-lives, decay modes and branching fractions, and the energies, intensities and uncertainties of the
γ rays emitted following neutron capture were collected toUnauthenticated
Download Date | 6/12/17 1:06 PM
630
gether in the early 1990s to create the International Nuclear
Geophysics Database (INGD-90) [117].
Nuclear astrophysics constitutes productive collaboration
between astrophysicists and nuclear physicists to study the
nuclear reactions of relevance to stellar modelling, γ -ray,
optical and X-ray astronomy, and the formation and evolutionary existence of the cosmos. A primary aim is to improve
our understanding of the origins of the universe through
the concept of nucleosynthesis, which can be defined in
terms of the formation mechanisms of the elements and the
commensurate generation of energy in the stars. Various
proposed cosmological phenomena need to be satisfactorily addressed through nuclear physics (helium fusion; s,
r and rp processes; X-ray processes; etc.) in order to improve our understanding of the driver mechanisms for active galaxies, core collapse, supernova neutrinos, neutron
stars and black holes. Spectral studies of complex nuclear
structure play an important role in addressing the fundamental nature of the universe, and will continue to do so
for many years to come. Recent and future advances in our
ability (a) to generate unstable radionuclides close to the
proton and neutron drip lines, and (b) to detect and quantify their decay characteristics will aid considerably in the
advance of basic research within both nuclear physics and
astrophysics.
6. Concluding remarks and future perspectives
An extremely important requirement in the adoption and application of radioactive decay data is that such numerical
data and their uncertainties should be sound and sufficiently
accurate. These needs have been satisfactorily addressed
with respect to the main fission products and actinides produced in power reactors, although highly-specific decaydata measurements and evaluations remain outstanding to
address particular needs in decay-heat calculations and the
potential future implementation of various high burn-up fuel
strategies. Other significant issues that have arisen in recent
years include the provision of improved delayed-neutron
data, and the beneficial requirement for well-defined β −
spectra to assist in non-invasive studies of the antineutrino
emission from operational reactors.
A wide range of activation products are identified with
various proposed designs of fusion reactor. Their decay
properties also need to be sufficiently well known to address standard operational requirements, and study radiation
dosimetry, longer-term radiotoxicity, and the bulk handling
of activated structural materials as radioactive waste. While
much of the decay data would appear to be readily available from various well-established databases, the quantity of
such data would suggest a need for careful assessment to
ensure all envisaged requirements are met.
Significant diagnostic and therapeutic developments continue to occur in both organ imaging and radiotherapy. Thus,
efforts are underway to couple positron-emission tomography (PET) with X-ray computed tomography (CT) and magnetic resonance imaging (MRI), with the aim of achieving
comprehensive and detailed organ assessment. New possibilities for improved internal radiotherapy are also being
explored on the basis of the following procedures:
A. L. Nichols
1. combination of PET and radiotherapy derived from radioimmuno reactions, and
2. Auger-electron and α-particle therapy at the cellular and
molecular levels.
Long-term decay-data needs in nuclear medicine will depend upon the relative success of such proposed developments and the commensurate identification of the most suitable radionuclides in these studies and medical treatments.
Overall, demands are expected to gravitate towards positron
emitters and appropriate therapeutic radionuclides, as outlined in Sect. 5.2. An increased adoption of metallic-based
positron emitters can be envisaged to occur as a consequence
of improved coordination chemistry (especially for Ti, Ga
and Cu radionuclides) arising from advances in the preparation of organometallic compounds. The consequences of
adopting highly-focused therapeutic treatment through microdosimetry techniques will also require improved characterisation and quantification of the atomic and nuclear
decay data of the most suitable low-energy Auger-electron
emitters.
Another noteworthy decay-data issue is the requirement
for more accurately known half-lives of specific long-lived
radionuclides that are used as geochronometers in the dating
of localised geological events (see Sect. 5.4) and nucleosynthesis within the solar system. The half-lives and associated
uncertainties of 87 Rb, 176 Lu, 187 Re and 190 Pt may be significant in this respect, although other features of such work are
of considerable importance, particularly the requirement for
sample stability over many hundred-million years and potentially serious inadequacies in the adoption of a particular
analytical technique to quantify multi-element and multiisotope content.
Requests for new nuclear data measurements are driven
primarily by the results of methodical evaluations to identify inconsistencies and unforeseen gaps in the desired data.
Thus, a healthy synergy exists in which αβγ spectroscopy
laboratories undertake decay-data studies driven by data inadequacies highlighted by decay-scheme evaluations of direct relevance to basic nuclear physics research and application in the industrial, medical and environmental sectors.
Under these circumstances, the communication and transfer of such data and information has improved considerably,
and large quantities of nuclear data can be rapidly accessed
within seconds, thanks to the work undertaken over many
years by staff at the various national and international nuclear data centres.
7. Data uncertainties
Data and their uncertainties are presented throughout the
text and tables in the form 1234(x), where x is the uncertainty in the last digit or digits quoted in the measured or
evaluated number. This uncertainty is generally expressed at
the 1σ confidence level. Examples: 1739(8) means 1739 ±
8; 0.0171(22) means 0.0171 ± 0.0022; 1.13(17) × 10+6
means (1.13 ± 0.17) × 10+6 .
Acknowledgment. Advice and information has been gratefully received
from Roberto Capote Noy (IAEA, Vienna, Austria), Christopher J.
Dean (Serco, Winfrith Newburgh, Dorset, UK), Filip G. Kondev (Argonne National Laboratory, USA), Robert W. Mills (National Nuclear
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
Laboratory, Seascale, Cumbria, UK), Alexander R.L. Nichols (JAMSTEC, Yokosuka, Japan), Syed M. Qaim (Forschungszentrum Jülich,
Germany) and Balraj Singh (McMaster University, Hamilton, Canada).
References
1. Magill, J., Galy, J.: Radioactivity Radionuclides Radiation. Springer, Berlin, Heidelberg and New York (2005).
2. Nichols, A. L., Decay data: review of measurements, evaluations
and compilations. Appl. Radiat. Isot. 55, 23–70 (2001).
3. Nichols, A. L., Nuclear decay data: on-going studies to address
and improve radionuclide decay characteristics. In: AIP Conf.
Proc. – Int. Conf. on Nuclear Data for Science and Technology.
(Haight, R. C., Chadwick, M. B., Kawano, T., Talou, P., eds.) Vol.
769, Part 1, AIP, Melville, New York, USA, ISBN 0-7354-0254X, ISSN 0094-243X (2005), pp. 242–251.
4. Curie, M., Debierne, A., Eve, A. S., Geiger, H., Hahn, O., Lind,
S. C., Meyer, St., Rutherford, E., Schweidler, E.: The radioactive constants as of 1930 – report of the International RadiumStandards Commission. Rev. Mod. Phys. 3, 427–445 (1931).
5. Fea, G.: Tabelle riassuntive e bibliografia delle transmutazioni artificiali. Nuovo Cim. 12, 368–406 (1935).
6. Livingston, M. S., Bethe, H. A.: Nuclear physics – C. Nuclear dynamics, experimental. Rev. Mod. Phys. 9, 245–390 (1937).
7. Livingood, J. J., Seaborg, G. T.: A table of induced radioactivities.
Rev. Mod. Phys. 12, 30–46 (1940).
8. Firestone, R. B., Shirley, V. S. (Eds.), Baglin, C. M., Chu, S. Y. F.,
Zipkin, J. (Ass. Eds.): Table of Isotopes. 8th Edn., Vols. I and II
(1996), Wiley, New York, ISBN 0-471-14918-7.
9. Way, K.: Nuclear data: a collection of experimental values of
half-lives, radiation energies, relative isotopic abundances, nuclear
moments and cross sections compiled by the National Bureau
of Standards nuclear data group. NBS circular no. 499 (1950),
National Bureau of Standards, US Department of Commerce,
Washington DC, USA.
10. Evaluated Nuclear Structure Data File, National Nuclear Data
Center, Brookhaven National Laboratory, Upton, New York,
USA, also Nuclear Data Sheets, Elsevier Inc., Amsterdam, The
Netherlands, and http://www.nndc.bnl.gov/ensdf/.
11. Nichols, A. L., Tuli, J. K.: The aims and activities of the International Network of Nuclear Structure and Decay Data Evaluators.
In: Proc. Int. Conf. on Nuclear Data for Science and Technology.
(Bersillon, O., Gunsing, F., Bauge, E., Jacqmin, R., Leray, S., eds.)
Vol. 1, EDP Sciences, Les Ulis, France, ISBN 978-2-7598-0090-2
(2008), pp. 37–42.
12. Szelecsényi, F., Steyn, G. F., Kovács, Z., Vermeulen, C., van der
Meulen, N. P., Dolley, S. G., van der Walt, T. N., Suzuki, K.,
Mukai, K.: Investigation of the 66 Zn( p, 2 pn)64 Cu and 68 Zn( p, x)
64
Cu nuclear processes up to 100 MeV: production of 64 Cu, Nucl.
Instrum. Methods Phys. Res. B 240, 625–637 (2005).
13. Nye, J. A., Avila-Rodriguez, M. A., Nickles, R. J.: A new binary
compound for the production of 124 I via the 124 Te( p, n)124 I reaction. Appl. Radiat. Isot. 65, 407–412 (2007).
14. Qaim, S. M., Bisinger, T., Hilgers, K., Nayak, D., Coenen, H. H.:
Positron emission intensities in the decay of 64 Cu, 76 Br and 124 I.
Radiochim. Acta 95, 67–73 (2007).
15. Walen, R. J., Nedovessov, V., Bastin-Scoffier, G.: Spectrographie
α de 223 Ra (AcX) et de ses dérivés. Nucl. Phys. 35, 232–252
(1962).
16. Grennberg, B., Rytz, A.: Absolute measurements of α-ray energies. Metrologia 7, 65–77 (1971).
17. Garcia-Toraño, E.: Current status of alpha-particle spectrometry.
Appl. Radiat. Isot. 64, 1273–1280 (2006).
18. Kondev, F. G., Ahmad, I., Greene, J. P., Nichols, A. L., Kellett, M. A.: Measurements of absolute gamma-ray emission probabilities in the decay of 233 Pa. Nucl. Instrum. Methods Phys. Res.
A 652, 654–656 (2011).
19. Horansky, R. D., Ullom, J. N., Beall, J. A., Hilton, G. C., Irwin, K. D., Dry, D. E., Hastings, E. P., Lamont, S. P., Rudy, C. R.,
Rabin, M. W.: Superconducting calorimetric alpha particle sensors
for nuclear non-proliferation applications. Appl. Phys. Lett. 93,
123504, 1–3 (2008).
631
20. Croce, M. P., Bacrania, M. K., Hoover, A. S., Rabin, M. W., Hoteling, N. J., Lamont, S. P., Plionis, A. A., Dry, D. E., Ullom, J. N.,
Bennett, D. A., Horansky, R. D., Kotsubo, V., Cantor, R.: Cryogenic microcalorimeter system for ultra-high resolution alphaparticle spectrometry, in AIP Conf. Proc. – 13th Int. Workshop on
Low Temperature Detectors. (Cabrera, B., Miller, A., Young, B.,
eds.) Vol. 1185, AIP, Melville, New York, USA, ISBN 0-73540751-0/09 (2009), pp. 741–744.
21. Ranitzsch, P. C., Kempf, S., Pabinger, A., Pies, C., Porst, J.-P.,
Schäfer, S., Fleischmann, A., Gastaldo, L., Enss, C., Jang, Y. S.,
Kim, I. H., Kim, M. S., Kim, Y. H., Lee, J. S., Lee, K. B., Lee,
M. K., Lee, S. J., Yoon, W. S., Yuryev, Y. N.: Development of
cryogenic alpha spectrometers using metallic magnetic calorimeters. Nucl. Instrum. Methods Phys. Res. A 652, 299–301 (2011).
22. Lee, I. Y., Deleplanque, M. A., Vetter, K.: Developments in large
gamma-ray detector arrays. Rep. Prog. Phys. 66, 1095–1144
(2003).
23. Eberth, J., Simpson, J.: From Ge(Li) detectors to gamma-ray
tracking arrays – 50 years of gamma spectroscopy with germanium detectors. Prog. Part. Nucl. Phys. 60, 283–337 (2008).
24. Korten, K., Lunardi, S. (Eds.): Achievements with the Euroball
spectrometer, 1997–2003 – http://www.lnl.infn.it/∼annrep/other_
reports/euroball/eb_index.htm.
25. Gammasphere –
http://www.physics.fsu.edu/GS10Yr/introduction.htm.
26. Akkoyun, S., Algora, A., Alikhani, B., et al.: AGATA – Advanced
GAmma Tracking Array. Nucl. Instrum. Methods Phys. Res. A
668, 26–58 (2012).
27. Lee, I. Y.: Gamma-ray tracking detectors: physics opportunities
and status of GRETINA. Nucl. Phys. A 834, 743c–746c (2010).
28. Gadea, A., Farnea, E., Valiente-Dobón, J. J., Million, B., Mengoni, D., Bazzacco, D., Recchia, F., Dewald, A., Pissulla, Th.,
Rother, W., et al.: Conceptual design and infrastructure for the installation of the first AGATA sub-array at LNL. Nucl. Instrum.
Methods Phys. Res. A 654, 88–96 (2011).
29. van Loef, E. V. D., Dorenbos, P., van Eijk, C. W. E., Krämer, K.,
Güdel, H. U.: High-energy-resolution scintillator: Ce3+ activated
LaCl3 . Appl. Phys. Lett. 77, 1467–1468 (2000).
30. van Loef, E. V. D., Dorenbos, P., van Eijk, C. W. E., Krämer, K.,
Güdel, H. U.: High-energy-resolution scintillator: Ce3+ activated
LaBr3 . Appl. Phys. Lett. 79, 1573–1575 (2001).
31. Glodo, J., Moses, W. W., Higgins, W. M., van Loef, E. V. D.,
Wong, P., Derenzo, S. E., Weber, M. J., Shah, K. S.: Effects of Ce
concentration on scintillation properties of LaBr3 :Ce. IEEE Trans.
Nucl. Sci. 52, 1805–1808 (2005).
32. Zhu, S., Kondev, F. G., Carpenter, M. P., Ahmad, I., Chiara, C. J.,
Greene, J. P., Gurdal, G., Janssens, R. V. F., Lalkovski, S., Lauritsen, T., Seweryniak, D.: γ -ray coincidence and fast-timing measurements using LaBr3 (Ce) detectors and Gammasphere. Nucl.
Instrum. Methods Phys. Res. A 652, 231–233 (2011).
33. Cherepy, N. J., Payne, S. A., Asztalos, S. J., Hull, G., Kuntz, J. D.,
Niedermayr, T., Pimputkar, S., Roberts, J. J., Sanner, R. D., Tillotson, T. M., et al.: Scintillators with potential to supersede lanthanum bromide. IEEE Trans. Nucl. Sci. 56, 873–880 (2009).
34. Stahle, C. K., Allen, C. A., Boyce, K. R., Brekosky, R. P., Brown,
G. V., Cottam, J., Figueroa-Feliciano, E., Galeazzi, M., Gygax,
J. D., Jacobson, M. B., et al.: The next-generation microcalorimeter array of XRS on Astro-E2. Nucl. Instrum. Methods Phys. Res.
A 520, 466–468 (2004).
35. Porter, F. S., Brown, G. V., Boyce, K. R., Kelley, R. L., Kilbourne,
C. A., Beiersdorfer, P., Hui Chen, Terracol, S., Kahn, S. M.,
Szymkowiak, A. E.: The Astro-E2 x-ray spectrometer/EBIT microcalorimeter X-ray spectrometer. Rev. Sci. Instrum. 75, 3772–
3774 (2004).
36. Beck, B. R., Becker, J. A., Beiersdorfer, P., Brown, G. V., Moody,
K. J., Wilhelmy, J. B., Porter, F. S., Kilbourne, C. A., Kelley, R. L.:
Energy splitting of the ground-state doublet in the nucleus 229 Th.
Phys. Rev. Lett. 98, 142501, 1–4 (2007).
37. Greenwood, R. C., Helmer, R. G., Lee, M. A., Putnam, M. H.,
Oates, M. A., Struttmann, D. A., Watts, K. D.: Total absorption
gamma-ray spectrometer for measurement of beta-decay intensity distributions for fission product radionuclides. Nucl. Instrum.
Methods Phys. Res. A 314, 514–540 (1992).
Unauthenticated
Download Date | 6/12/17 1:06 PM
632
38. Greenwood, R. C., Helmer, R. G., Putnam, M. H., Watts, K. D.:
Measurement of β − -decay intensity distribution of several fissionproduct isotopes using a total absorption γ -ray spectrometer.
Nucl. Instrum. Methods Phys. Res. A 390, 95–154 (1997).
39. Gierlik, M., Płochocki, A., Karny, M., Urban, W., Janas, Z.,
Batist, L., Moroz, F., Collatz, R., Górska, M., Grawe, H., et al.:
Gamow-Teller strength distribution near 100 Sn – the beta decay of
102
In. Nucl. Phys. A 724, 313–332 (2003).
40. Poirier, E., Maréchal, F., Dessagne, Ph., Algora, A., Borge,
M. J. G., Cano-Ott, D., Caspar, J. C., Courtin, S., Devin, J., Fraile,
L. M., et al.: B(GT) strength from β-decay measurements and inferred shape mixing in 74 Kr. Phys. Rev. C69, 034307, 1–8 (2004).
41. Algora, A., Jordan, D., Tain, J. L., Rubio, B., Agramunt, J., PerezCerdan, A. B., Molina, F., Caballero, L., Nácher, E., Krasznahorkay, A., et al.: Reactor decay heat in 239 Pu: solving the γ
discrepancy in the 4–3000 s cooling period. Phys. Rev. Lett. 105,
202501, 1–4 (2010).
42. Bisgard, K. M., Dahl, P., Olesen, K.: Multipolarities of U233 transitions. Nucl. Phys. 12, 612–618 (1959).
43. Albridge, R. G., Hollander, J. M., Gallagher, C. J., Hamilton, J. H.:
The energy levels of U233 . Nucl. Phys. 27, 529–553 (1961).
44. Woods, S. A., Christmas, P., Cross, P., Judge,
√ S. M., Gelletly, W.:
Decay studies of 237 Np with an iron-free π 2 double-focusing βray spectrometer of improved efficiency. Nucl. Instrum. Methods
Phys. Res. A 264, 333–356 (1988).
45. Hofmann, H. J., Bonani, G., Suter, M., Wölfli, W., Zimmermann, D., von Gunten, H. R.: A new determination of the half-life
of 32 Si. Nucl. Instrum. Methods Phys. Res. B 52, 544–551 (1990).
46. Frekers, D., Henning, W., Kutschera, W., Rehm, K. E., Smither,
R. K., Yntema, J. L., Santo, R., Stievano, B., Trautmann, N.: Halflife of 44 Ti. Phys. Rev. 28, 1756–1762 (1983).
47. Kutschera, W., Billquist, P. J., Frekers, D., Henning, W., Jensen,
K. J., Ma, X., Pardo, R., Paul, M., Rehm, K. E., Smither, R. K.,
Yntema, J. L., Mausner, L. F.: Half-life of 60 Fe. Nucl. Instrum.
Methods Phys. Res. B 5, 430–435 (1984).
48. Gartenmann, P., Golser, R., Haas, P., Kutschera, W., Suter, M.,
Synal, H.-A., Wagner, M. J. M., Wild, E.: Absolute measurement
of 126 Sn radionuclide concentration with AMS. Nucl. Instrum.
Methods Phys. Res. B 114, 125–130 (1996).
49. Haas, P., Gartenmann, P., Golser, R., Kutschera, W., Suter, M.,
Synal, H.-A., Wagner, M. J. M., Wild, E., Winkler, G.: A new halflife measurement of the long-lived fission product 126 Sn. Nucl.
Instrum. Methods Phys. Res. B 114, 131–137 (1996).
50. Oberli, F., Gartenmann, P., Meier, M., Kutschera, W., Suter, M.,
Winkler, G.: The half-life of 126 Sn refined by thermal ionization
mass spectrometry measurements. Int. J. Mass Spectrom. 184,
145–152 (1999).
51. Bienvenu, Ph., Cassette, Ph., Andreoletti, G., Bé, M.-M., Comte, J., Lépy, M.-C.: A new determination of 79 Se half-life. Appl.
Radiat. Isot. 65, 355–364 (2007).
52. Catlow, S. A., Troyer, G. L., Hansen, D. R., Jones, R. A.: Half-life
measurement of 126 Sn isolated from Hanford nuclear defense
waste. J. Radioanal. Nucl. Chem. 263, 599–603 (2005).
53. Bienvenu, Ph., Ferreux, L., Andreoletti, G., Arnal, N., Lépy,
M.-C., Comte, J., Bé, M.-M.: Determination of 126 Sn half-life
from ICP-MS and gamma spectrometry measurements. Radiochim. Acta 97, 687–694 (2009).
54. Bé, M.-M., Chisté, V., Dulieu, C., Browne, E., Chechev, V., Kuzmenko, N., Helmer, R., Nichols, A., Schönfeld, E., Dersch, R.:
Table of radionuclides (Vol. 1 – A = 1 to 150). Monographie BIPM-5, Bureau International des Poids et Mesures,
Sévres, France (2004), ISBN 92-822-2206-3, also available from
http://www.bipm.org/utils/common/pdf/monographieRI/Monogra
phie_BIPM-5_Tables_Vol1.pdf.
55. Bé, M.-M., Chisté, V., Dulieu, C., Browne, E., Chechev, V., Kuzmenko, N., Helmer, R., Nichols, A., Schönfeld, E., Dersch, R.:
Table of radionuclides (Vol. 2 – A = 151 to 242). Monographie BIPM-5, Bureau International des Poids et Mesures,
Sévres, France (2004), ISBN 92-822-2207-1, also available from
http://www.bipm.org/utils/common/pdf/monographieRI/Monogra
phie_BIPM-5_Tables_Vol2.pdf.
56. Bé, M.-M., Chisté, V., Dulieu, C., Browne, E., Baglin, C.,
Chechev, V., Kuzmenko, N., Helmer, R., Kondev, F., MacMahon, D., Lee, K. B.: Table of radionuclides (Vol. 3 – A = 3 to 244).
A. L. Nichols
57.
58.
59.
60.
61.
62.
63.
64.
65.
66.
67.
Monographie BIPM-5, Bureau International des Poids et Mesures,
Sévres, France (2006), ISBN 92-822-2218-7, also available from
http://www.bipm.org/utils/common/pdf/monographieRI/Monogra
phie_BIPM-5_Tables_Vol3.pdf.
Bé, M.-M., Chisté, V., Dulieu, C., Browne, E., Chechev, V.,
Kuzmenko, N., Kondev, F., Luca, A., Galán, M., Pearce, A.,
Huang, X.: Table of radionuclides (Vol. 4 – A = 133 to 252).
Monographie BIPM-5, Bureau International des Poids et Mesures,
Sévres, France (2008), ISBN 92-822-2230-6, also available from
http://www.bipm.org/utils/common/pdf/monographieRI/Monogra
phie_BIPM-5_Tables_Vol4.pdf.
Bé, M.-M., Chisté, V., Dulieu, C., Mougeot, X., Browne, E.,
Chechev, V., Kuzmenko, N., Kondev, F., Luca, A., Galán, M.,
Nichols, A. L., Arinc, A., Huang, X.: Table of radionuclides (Vol.
5 – A = 22 to 244). Monographie BIPM-5, Bureau International
des Poids et Mesures, Sévres, France (2010), ISBN-13 97892-822-2234-8, also available from http://www.bipm.org/utils/
common/pdf/monographieRI/Monographie_BIPM-5_Tables_Vol5
.pdf.
Bé, M.-M., Chisté, V., Dulieu, C., Mougeot, X., Chechev, V. P.,
Kuzmenko, N. K., Kondev, F. G., Luca, A., Galán, M., Nichols,
A. L., Arinc, A., Pearce, A., Huang, X., Wang, B.: Table of radionuclides (Vol. 6 – A = 22 to 242). Monographie BIPM-5,
Bureau International des Poids et Mesures, Sévres, France (2011),
ISBN-13 978-92-822-2242-3, also available from http://www.
http://www.bipm.org/utils/common/pdf/monographieRI/Monogra
phie_BIPM-5_Tables_Vol6.pdf.
Bé, M.-M., Chisté, V., Dulieu, C., Mougeot, X., Browne, E.,
Baglin, C., Chechev, V. P., Egorov, A., Kuzmenko, N. K., Sergeev,
V. O., et al.: Table of radionuclides, comments on evaluations (Vols. 1–6). Monographie BIPM-5 (2011) Bureau International des Poids et Mesures, France, also available from
http://www.bipm.org/utils/common/pdf/monographieRI/Monogra
phie_BIPM-5_Comments_Vol1-6.pdf.
Nichols, A. L.: IAEA Co-ordinated Research Project: update of
X-ray and gamma-ray decay data standards for detector calibration and other applications. Appl. Radiat. Isot. 60, 247–256
(2004).
Bé, M.-M., Chechev, V. P., Dersch, R., Helene, O. A. M., Helmer,
R. G., Herman, M., Hlaváč, S., Marcinkowski, A., Molnár, G. L.,
Nichols, A. L., Schönfeld, E., Vanin, V. R., Woods, M. J.: Update
of X ray and gamma ray decay data standards for detector calibration and other applications, Volume 1: Recommended decay
data, high energy gamma ray standards and angular correlation
coefficients. IAEA Scientific and Technical report STI/PUB/1287,
May 2007, International Atomic Energy Agency, Vienna, Austria,
ISBN 92-0-113606-4, http://www-nds.iaea.org/publications/tec
docs/sti-pub-1287_Vol1.pdf
Bé, M.-M., Chechev, V. P., Dersch, R., Helene, O. A. M., Helmer,
R. G., Herman, M., Hlaváč, S., Marcinkowski, A., Molnár, G. L.,
Nichols, A. L., Schönfeld, E., Vanin, V. R., Woods, M. J.: Update
of X ray and gamma ray decay data standards for detector calibration and other applications, Volume 2: Data selection, assessment
and evaluation procedures. IAEA Scientific and Technical report
STI/PUB/1287, May 2007, International Atomic Energy Agency,
Vienna, Austria, ISBN 92-0-113606-4, also available from
http://www-nds.iaea.org/publications/tecdocs/sti-pub-1287_Vol2.
pdf.
Kellett, M. A., Kondev, F. G., Nichols, A. L.: IAEA Coordinated
Research Project: updated decay data library for actinides. Appl.
Radiat. Isot. 66, 694–700 (2008).
Kellett, M. A., Bé, M.-M., Chechev, V., Huang, X., Kondev, F. G.,
Luca, A., Mukherjee, G., Nichols, A. L., Pearce, A.: New IAEA
actinide decay data library. J. Korean Phys. Soc. – Proc. Int. Conf.
on Nuclear Data for Science and Technology 59, No. 2, 1455–
1460 (2011), Korean Physical Society, South Korea.
Bé, M.-M., Chechev, V. P., Huang, X., Kellett, M. A., Kondev, F. G., Luca, A., Mukherjee, G., Nichols, A. L., Pearce, A. K.:
Updated decay data library for actinides. IAEA technical report,
in preparation.
Trkov, A., Herman, M., Brown, D. A., and members of the Cross
Sections Evaluation Working Group: ENDF-6 formats manual – data formats and procedures for the evaluated nuclear
data files ENDF/B-VI and ENDF/B-VII. BNL technical re-
Unauthenticated
Download Date | 6/12/17 1:06 PM
Radioactive decay data: powerful aids in medical diagnosis and therapy, analytical science and other applications
68.
69.
70.
71.
72.
73.
74.
75.
76.
77.
78.
79.
80.
81.
82.
83.
84.
85.
port BNL-90365-2009, Rev. 2, CSEWG document ENDF-102,
Brookhaven National Laboratory, December 2011, also available
from http://www.nndc.bnl.gov/csewg/docs/endf-manual.pdf.
Katakura, J., Yoshida, T., Oyamatsu, K., Tachibana, T.: JENDL FP
decay data file 2000. Japan Atomic Energy Research Institute report JAERI 1343, Tokai-mura, Ibaraki, Japan (2001).
Kellett, M. A., Bersillon, O., Mills, R. W.: The JEFF-3.1/3.1.1 radioactive decay data and fission yields sub-libraries. JEFF report
20, NEA No. 6287, Nuclear Energy Agency, OECD, Paris, 2009,
ISBN 978-92-99087-6, also available from http://www.oecd-nea.
org/dbdata/nds_jefreports/jefreport-20/nea6287-jeff-20.pdf
Chadwick, M. B., Obložinský, P., Herman, M., Greene, N. M.,
McKnight, R. D., Smith, D. L., Young, P. G., MacFarlane, R. E.,
Hale, G. M., Frankle, S. C., et al.: ENDF/B-VII.0: next generation
evaluated nuclear data library for nuclear science and technology.
Nucl. Data Sheets 107, 2931–3060 (2006).
Chadwick, M. B., Herman, M., Obložinský, P., Dunn, M. E., Danon, Y., Kahler, A. C., Smith, D. L., Pritychenko, B., Arbanas, G.,
Arcilla, R., et al.: ENDF/B-VII.1 nuclear data for science and technology: cross sections, covariances, fission product yields and decay data. Nucl. Data Sheets 112, 2887–2996 (2011).
Audi, G., Bersillon, O., Blachot, J., Wapstra, A. H.: The NUBASE
evaluation of nuclear and decay properties. Nucl. Phys. A729, 3–
128 (2003).
Nichols, A. L., Perry, R. J.: Activation product decay data: UKPADD6.7. Serco Assurance report SA/NST/18923/W001, Issue 1,
UKNSF(2007)P212, JEF/DOC-1165, February 2007.
Nichols, A. L., Perry, R. J.: Heavy element and actinide decay
data: UKHEDD2.5. Serco Assurance report SA/NST/18923/
W002, Issue 1, UKNSF(2007)P213, JEF/DOC-1166, February
2007.
Nichols, A. L., Perry, R. J.: Activation product decay data: UKPADD6.11. Serco Assurance report SERCO/TCS/005398.25/002,
Issue 1, UKNSF(2012)P248, JEF/DOC-1424, April 2012.
Nichols, A. L., Perry, R. J.: Heavy element and actinide decay data: UKHEDD2.6. Serco Assurance report SERCO/TAS/
000343/W002, Issue 1, UKNSF(2008)P225, JEF/DOC-1224,
February 2008.
Heath, R. L.: Gamma-ray spectrum catalogue. AEC report ANC1000-2 (1974).
Helmer, R. G., Gehrke, R. J., Davidson, J. R., Mandler, J. W.: Scientists, spectrometry and gamma-ray spectrum catalogues, 1957–
2007. J. Radioanal. Nucl. Chem. 243, 109–117 (2000).
Tobias, A.: Decay heat. Prog. Nucl. Energy 5, 1–93 (1980).
Nichols, A. L.: Nuclear Data Requirements for Decay Heat Calculations. In: Proc. Modern Reactor Physics and the Modelling
of Complex Systems, 21–30 August 2000, The 2000 Frederic Joliot/Otto Hahn Summer School in Reactor Physics, CEA
Cadarache, France (2000), pp. 212–278.
Nichols, A. L.: Nuclear Data Requirements for Decay Heat Calculations. In: ICTP Lectures Notes, Vol. 20, Workshop on Nuclear
Reaction Data and Nuclear Reactors: Physics, Design and Safety,
25 February–28 March 2002, The Abdus Salam International
Centre for Theoretical Physics (ICTP)- (Herman, M., Paver, N.,
eds.) ICTP Publ., Trieste, Italy (2005), pp. 65–195, also available
from http://users.ictp.it/∼pub_off/lectures/lns020/Nichols/Nichols
.pdf.
Hardy, J. C., Carrez, L. C., Jonson, B., Hansen, P. G.: The essential decay of Pandemonium: a demonstration of errors in complex
beta-decay schemes. Phys. Lett. B 71, 307–310 (1977).
Greenwood, R. C., Putnam, M. H., Watts, K. D.: Ground-state β − branching intensities of several fission-product isotopes using
a total absorption γ -ray spectrometer. Nucl. Instrum. Methods
Phys. Res. A 378, 312–320 (1996).
Tobias, A.: Derivation of decay heat benchmarks for U-235 and
Pu-239 by a least squares fit to measured data. Central Electricity
Generating Board report RD/B/6210/R89, May 1989.
Kellett, M. A., Nichols, A. L., Bersillon, O., Henriksson, H., Jacqmin, R., Roque, B., Katakura, J., Oyamatsu, K., Tachibana, T.,
Yoshida, T., et al.: Assessment of fission product decay data for
decay heat calculations, a report by the Working Party on International Evaluation Co-operation of the NEA Nuclear Science
Committee, Vol. 25, NEA/WPEC-25, OECD/NEA, Paris (2007),
ISBN 978-92-64-99034-0.
633
86. Gupta, M., Kellett, M. A., Nichols, A. L., Bersillon, O.: Decay heat calculations: assessment of fission product decay
data requirements for Th/U fuel. IAEA report INDC(NDS)0577, May 2010, IAEA, Vienna, Austria, also available from
http://www-nds.iaea.org/publications/indc/indc-nds-0577.pdf.
87. Yoshida, T., Hagura, N., Umezu, R., Algora, A., Tain, J. L., Jordan, D., Tachibana, T.: Impact of TAGS measurement on FP decay
data and decay heat calculations. J. Korean Phys. Soc. 59, 1543–
1546 (2011).
88. Nichols, A. L., Nordborg, C.: Consultants’ meeting on Total Absorption Gamma-ray Spectroscopy (TAGS) – current status of
measurement programmes for decay heat calculations and other
applications, 27–28 January 2009, IAEA report INDC(NDS)0551, February 2009, IAEA, Vienna, Austria, also available from
http://www-nds.iaea.org/publications/indc/indc-nds-0551.pdf.
89. Kratz, K.-L., Rudolph, W., Ohm, H., Franz, H., Zendel, M., Herrmann, G., Prussin, S. G., Nuh, F. M., Shihab-Eldin, A. A., Slaughter, D. R., Halverson, W., Klapdor, H. V.: Investigation of beta
strength functions by neutron and gamma-ray spectroscopy, I: the
decay of 87 Br, 137 I, 85 As and 135 Sb. Nucl. Phys. A 317, 335–362
(1979).
90. Kratz, K.-L., Schröder, A., Ohm, H., Zendel, M., Gabelmann, H.,
Ziegert, W., Peuser, P., Jung, G., Pfeiffer, B., Wünsch, K. D., Wollnik, H., Ristori, C., Crancon, J., Beta-delayed neutron emission
from 93−100 Rb to excited states in the residual Sr isotopes, Z. Phys.
A – Atoms and Nuclei 306, 239–257 (1982).
91. Raman, S., Fogelberg, B., Harvey, J. A., Macklin, R. L., Stelson, P. H., Schröder, A., Kratz, K.-L.: Overlapping β decay and
resonance neutron spectroscopy of levels in 87 Kr. Phys. Rev. C 28,
602–622 (1983), Erratum, Phys. Rev. C 29, 344 (1984).
92. Greenwood, R. C., Caffrey, A. J.: Delayed-neutron energy spectra
of 93−97 Rb and 143−145 Cs. Nucl. Sci. Eng. 91, 305–323 (1985).
93. Greenwood, R. C., Watts, K. D.: Delayed neutron energy spectra
of 87 Br, 88 Br, 89 Br, 90 Br, 137 I, 138 I, 139 I and 136 Te. Nucl. Sci. Eng.
126, 324–332 (1997).
94. Abriola, D., Singh, B., Dillmann, I.: Consultants’ meeting on betadelayed neutron emission evaluation. 10–12 October 2011, IAEA
report INDC(NDS)-0599, December 2011, IAEA, Vienna, Austria, also available from http://www-nds.iaea.org/publications/
indc/indc-nds-0599.pdf.
95. Bemporad, C., Gratta, G., Vogel, P.: Reactor-based neutrino oscillation experiments. Rev. Mod. Phys. 74, 297–328 (2002).
96. Bowden, N. S., Bernstein, A., Allen, M., Brennan, J. S., Cunningham, M., Estrada, J. K., Greaves, C. M. R., Hagmann, C., Lund, J.,
Mengesha, W., Weinbeck, T. D., Winant, C. D.: Experimental results from an antineutrino detector for cooperative monitoring of
nuclear reactors. Nucl. Instrum. Methods Phys. Res. A 572, 985–
998 (2007).
97. Bersillon, O., Greenwood, L. R., Griffin, P. J., Mannhart, W.,
Nolthenius, H. J., Paviotti-Corcuera, R., Zolotarev, K. I., Zsolnay, É.M., McLaughlin, P. K., Trkov, A.: International Reactor Dosimetry File 2002 (IRDF-2002). IAEA Technical Reports Series No. 452, International Atomic Energy Agency,
Vienna, Austria, 2006, ISBN 92-0-105106-9, also available from
http://www-pub.iaea.org/MTCD/Publications/PDF/TRS452_web.
pdf.
98. Greenwood, L. R., Nichols, A. L.: Consultants’ meeting to review the requirements to improve and extend the IRDF library
(International Reactor Dosimetry File (IRDF-2002)). 25–26 January 2007, IAEA report INDC(NDS)-0507, January 2007, IAEA,
Vienna, Austria, also available from http://www-nds.iaea.org/
publications/indc/indc-nds-0507.pdf.
99. Zsolnay, É.M., Nolthenius, H. J., Nichols, A. L.: Investigation of
new reaction cross-section evaluations in order to update and extend the IRDF-2002 reactor dosimetry library. In: Proc. 13th Int.
Symp. Reactor Dosimetry State of the Art 2008. (Voorbraak, W.,
Debarberis, L., D’Hondt, P., Wagemans, J., eds.) World Scientific,
Singapore (2009), pp. 625–634, ISBN 981-4271-10-1.
100. Kellett, M. A., Greenwood, L. R.: Consultants’ meeting on improvements and extensions to IRDF (International Reactor
Dosimetry File (IRDF-2002)). 5–7 May 2010, IAEA report
INDC(NDS)-0575, December 2010, IAEA, Vienna, Austria, also
available from http://www-nds.iaea.org/publications/indc/indcnds-0575.pdf.
Unauthenticated
Download Date | 6/12/17 1:06 PM
634
101. Stöcklin, G., Qaim, S. M., Rösch, F.: The impact of radioactivity
on medicine. Radiochim. Acta 70/71, 249–272 (1995).
102. Qaim, S. M.: Nuclear data for medical applications: an overview.
Radiochim. Acta 89, 189–196 (2001).
103. Qaim, S. M.: Nuclear data relevant to the production and application of diagnostic radionuclides. Radiochim. Acta 89, 223–232
(2001).
104. Qaim, S. M.: Therapeutic radionuclides and nuclear data. Radiochim. Acta 89, 297–302 (2001).
105. Qaim, S. M.:, Use of cyclotrons in medicine. Radiat. Phys. Chem.
71, 917–926 (2004).
106. Qaim, S. M.: Development of novel positron emitters for medical
applications: nuclear and radiochemical aspects. Radiochim. Acta
99, 611–625 (2011).
107. Gul, K., Hermanne, A., Mustafa, M. G., Nortier, F. M., Obložinský, P., Qaim, S. M., Scholten, B., Shubin, Y., Takács, S., Tárkányi,
F. T., Zhuang, Y.: Charged particle cross-section database for medical radioisotope production: diagnostic radioisotopes and monitor
reactions. IAEA technical report IAEA-TECDOC-1211, International Atomic Energy Agency, Vienna, Austria (2001), also
available from http://www-nds.iaea.org/publications/tecdocs/iaeatecdoc-1211.pdf.
108. Běták, E., Caldeira, A. D., Capote, R., Carlson, B. V., Choi, H. D.,
Guimarães, F. B., Ignatyuk, A. G., Kim, S. K., Kiraly, B., Kovalev, S. F., Menapace, E., Nichols, A. L., Nortier, M., Pompeia, P., Qaim, S. M., Scholten, B., Shubin, Yu. N., Sublet, J.-Ch.,
Tárkányi, F. T.: Nuclear data for the production of therapeutic radionuclides. IAEA Technical Reports Series No. 473
(Qaim, S. M., Tárkányi, F. T., Capote, R., eds.) International
Atomic Energy Agency, Vienna, Austria (2011), ISBN 978-920-115010-3, also available from http://www-pub.iaea.org/MTCD/
Publications/PDF/trs473_web.pdf.
109. Capote, R., Nichols, A. L.: Consultants’ meeting on high-precision beta-intensity measurements and evaluations for specific PET
radioisotopes, 3–5 September 2008, IAEA report INDC(NDS)0535, December 2008, IAEA, Vienna, Austria, also available
from http://www-nds.iaea.org/publications/indc/indc-nds-0535.
pdf.
110. Capote, R., Nortier, F. M.: Consultants’ meeting on improvements
in charged-particle monitor reactions and nuclear data for medical
isotope production, 21–24 June 2011, IAEA report INDC(NDS)0591, August 2011, IAEA, Vienna, Austria, also available from
http://www-nds.iaea.org/publications/indc/indc-nds-0591.pdf.
111. Nichols, A. L., Qaim, S. M., Capote, R.: Technical meeting on
intermediate-term nuclear data needs for medical applications:
cross sections and decay data, 22–26 August 2011, IAEA report INDC(NDS)-0596, September 2011, IAEA, Vienna, Austria,
also available from http://www-nds.iaea.org/publications/indc/
indc-nds-0596.pdf.
112. Lindstrom, R. M., Yonezawa, C.: Prompt-gamma activation analysis with guided neutron beams. In: Prompt Gamma Neutron
Activation Analysis. (Alfassi, Z. B., Chung, C., eds.) CRC Press,
Boca Raton, USA (1995), pp. 93–100.
113. Alfassi, Z. B., Chung, C. (eds.): Prompt Gamma Neutron Activation Analysis. CRC Press, Boca Raton, USA (1995).
A. L. Nichols
114. Paul, R. L., Lindstrom, R. M.: Prompt gamma-ray activation analysis: fundamentals and applications. J. Radioanal. Nucl. Chem.
243, 181–189 (2000).
115. Molnár, G. L. (ed.): Handbook of Prompt Gamma Activation Analysis with Neutron Beams. Kluwer, Dordrecht, The Netherlands
(2004).
116. Lone, M. A., Leavitt, R. A., Harrison, D. A.: Prompt gamma rays
from thermal-neutron capture. At. Data Nucl. Data Tables 26,
511–559 (1981).
117. Clayton, C. G., Ekström, P., Harrison, D. A., Kocherov, N. P.,
Leavitt, R. A., Lone, M. A., Schweitzer, J., Spanier, L., Tuli, J. K.:
Handbook on nuclear data for borehole logging and mineral
analysis. IAEA Technical Reports Series No. 357, International Atomic Energy Agency, Vienna, Austria (1993), ISBN
92-0-102393-6, also available from http://www-nds.iaea.org/
publications/tecdocs/technical-reports-series-357.pdf.
118. Choi, H. D., Firestone, R. H., Lindstrom, R. M., Molnár, G. L.,
Mughabghab, S. F., Paviotti-Corcuera, R., Révay, Z., Trkov, A.,
Zerkin, V., Zhou, C.: Database of prompt gamma rays from slow
neutron capture for elemental analysis. IAEA Scientific and Technical Publication STI/PUB/1263, International Atomic Energy
Agency, Vienna, Austria (2007), ISBN 92-0-101306-X, also available from http://www-nds.iaea.org/publications/tecdocs/sti-pub1263.pdf.
119. Allègre, C. J.: Isotope Geology. Cambridge University Press,
Cambridge, UK (2008), ISBN 978-52186-228-8.
120. McSween Jr., H. Y., Richardson, S. M., Uhle, M. E.: Geochemistry: Pathways and Processes. 2nd Edn., Columbia University
Press, New York, USA (2003), ISBN 0-231-12440-6.
121. McSween Jr., H. Y., Huss, G. R.: Cosmochemistry. Cambridge
University Press, Cambridge, UK (2010), ISBN 978-0-52187862-3.
122. von Gunten, H. R.: Radioactivity: a tool to explore the past. Radiochim. Acta 70/71, 305–316 (1995).
123. Ivanovich, M., Latham, A. G., Ku, T.-L.: Uranium series disequilibrium – applications in geochronology. In: Uranium-Series
Disequilibrium: Applications to Earth, Marine and Environmental
Sciences. (Ivanovich, M., Harmon, R. S., eds.) Oxford University
Press, Oxford, UK (1992), ISBN 0-19-854278-X, pp. 62–94.
124. Tuli, J. K.: Nuclear Wallet Cards for Radioactive Nuclides,
March 2004. Brookhaven National Laboratory, Upton, New York,
USA.
125. Blet, V., Berne, Ph., Tola, F., Vitart, X., Chaussy, C.: Recent developments in radioactive tracers methodology. Appl. Radiat. Isot.
51, 615–624 (1999).
126. Blet, V., Berne, Ph., Legoupil, S., Vitart, X.: Radioactive tracing
as aid for diagnosing chemical reactors. Oil Gas Sci. Technol. 55,
171–183 (2000).
127. Axelsson, G., Barry, B. J., Berne, P., Bjørnstad, T., Cameron, R.,
Charlton, S., Maggio, G. E., Pang, Z., Thereska, J., Vitart, X.: Radiotracer applications in industry – a guidebook, IAEA Technical
Reports Series No. 423, International Atomic Energy Agency, Vienna, Austria (2004), ISBN 92-0-114503-9, also available from
http://www-pub.iaea.org/MTCD/Publications/PDF/TRS423_web.
pdf.
Unauthenticated
Download Date | 6/12/17 1:06 PM