1.

07 Radiation Damage Using Ion Beams

G. S. Was
University of Michigan, Ann Arbor, MI, USA
R. S. Averback
University of Illinois at Urbana-Champagne, Urbana, IL, USA

ß 2012 Elsevier Ltd. All rights reserved.

1.07.1 Introduction 195

1.07.2 Motivation for Using Ion Beams to Study Radiation Damage 196
1.07.3 Review of Aspects of Radiation Damage Relevant to Ion Irradiation 197
1.07.3.1 Defect Production 197
1.07.3.2 Primary and Weighted Recoil Spectra 199
1.07.3.3 Damage Morphology 200
1.07.3.4 Damage Rate Effects 202
1.07.4 Contributions of Ion Irradiation to an Understanding of Radiation Effects 204
1.07.4.1 Electron Irradiations 204
1.07.4.1.1 Displacement threshold surfaces 204
1.07.4.1.2 Point defect properties 205
1.07.4.2 Ion Irradiations 206
1.07.4.2.1 The damage function 206
1.07.4.2.2 Freely migrating defects 207
1.07.4.2.3 Alloy stability under ion irradiation 207
1.07.4.2.4 Mechanical properties 209
1.07.4.2.5 Multiple ion beams 209
1.07.4.2.6 Swift ions 209
1.07.4.3 Comparison with Neutrons 211
1.07.5 Advantages and Disadvantages of Irradiations using Various Particle Types 215
1.07.5.1 Electrons 216
1.07.5.2 Heavy Ions 217
1.07.5.3 Light Ions 219
1.07.6 Practical Considerations for Radiation Damage Using Ion Beams 219
References 221

NWC Normal water chemistry

Abbreviations
PKA Primary knock-on atom
AES Auger electron spectroscopy
RCS Recoil collision sequence
APT Atom probe tomography
RIS Radiation induced segregation
bcc Body-centered cubic
SCC Stress corrosion cracking
BWR Boiling water reactor
STEM/EDS Scanning transmission electron
dpa Displacements per atom
microscopy/energy dispersive
fcc Face-centered cubic
spectrometry
FMD Freely migrating defect
TEM Transmission electron microscopy
FP Frenkel pair
IASCC Irradiation assisted stress corrosion
cracking
IGSCC Intergranular stress corrosion 1.07.1 Introduction
cracking
LWR Light water reactor Radiation effects research has been conducted using
MD Molecular dynamics a variety of energetic particles: neutrons, electrons,
NRT Norgett–Robinson–Torrens protons, He ions, and heavy ions. Energetic ions

195
196 Radiation Damage Using Ion Beams
can be used to understand the effects of neutron
irradiation on reactor components, and interest in
this application of ion irradiation has grown in recent
years for several reasons including the avoidance of
high residual radioactivity and the decline of neutron
sources for materials irradiation. The damage state and
microstructure resulting from ion irradiation, and thus
the degree to which ion irradiation emulates neutron
irradiation, depend upon the particle type and the
damage rate. This chapter will begin with a summary
of the motivation for using ion irradiation for radiation
damage studies, followed by a brief review of radia-
tion damage relevant to charged particles. The contri-
bution of ion irradiation to our understanding of
radiation damage will be presented next, followed by
an account of the advantages and disadvantages of
the various ion types for conducting radiation damage
studies, and wrapping up with a consideration of prac-
tical issues in ion irradiation experiments.
1.07.2 Motivation for Using Ion
Beams to Study Radiation Damage
In the 1960s and 1970s, heavy ion irradiation was
developed for the study of radiation damage pro-
cesses in materials. As ion irradiation can be
conducted at a well-defined energy, dose rate, and
temperature, it results in very well-controlled experi-
ments that are difficult to match in reactors. As such,
interest grew in the use of ion irradiation for the
purpose of simulating neutron damage in support of
the breeder reactor program.1–3 Ion irradiation and
simultaneous He injection were also used to simulate
the effects of 14 MeV neutron damage in conjunction
with the fusion reactor engineering program. The
application of ion irradiation (defined here as irradi-
ation by any charged particle, including electrons)
to the study of neutron irradiation damage caught
the interest of the light water reactor community to
address issues such as swelling, creep, and irradiation
assisted stress corrosion cracking of core structural
materials.4–6 Ion irradiation was also being used to
understand the irradiated microstructure of reactor
pressure vessel steels, Zircaloy fuel cladding, and
materials for advanced reactor concepts.
There is significant incentive to use ion irradiation
to study neutron damage as this technique has the
potential for yielding answers on basic processes
in addition to the potential for enormous savings in
time and money. Neutron irradiation experiments
are not amenable to studies involving a wide range
of conditions, which is precisely what is required for
investigations of the basic damage processes. Simula-
tion by ions allows easy variation of the irradiation
parameters such as dose, dose rate, and temperature
over a wide range of values.
One of the prime attractions of ion irradiation is
the rapid accumulation of end of life doses in short
periods of time. Typical neutron irradiation experi-
ments in thermal test reactors may accumulate dam-
age at a rate of 3–5 dpa year
1. In fast reactors, the
rates can be higher, on the order of 20 dpa year
1. For
low dose components such as structural components
in boiling water reactor (BWR) cores that typically
have an end-of-life damage of 10 dpa, these rates are
acceptable. However, even the higher dose rate of a
fast reactor would require 4–5 years to reach the peak
dose of 80 dpa in the core baffle in a pressurized
water reactor (PWR). For advanced, fast reactor con-
cepts in which core components are expected to
receive 200 dpa, the time for irradiation in a test
reactor becomes impractical.
In addition to the time spent ‘in-core,’ there is an
investment in capsule design and preparation as well
as disassembly and allowing for radioactive decay, add-
ing additional years to an irradiation program. Analysis
of microchemical and microstructural changes by
atom probe tomography (APT), Auger electron spec-
troscopy (AES) or microstructural changes by energy
dispersive spectroscopy via scanning transmission
electron microscopy (STEM-EDS) and mechanical
property or stress corrosion cracking (SCC) evalua-
tion can take several additional years because of the
precautions, special facilities, and instrumentation
required for handling radioactive samples. The result
is that a single cycle from irradiation through micro-
analysis and mechanical property/SCC testing may
require over a decade. Such a long cycle length does
not permit for iteration of irradiation or material
conditions that is critical in any experimental research
program. The long cycle time required for design and
irradiation also reduces flexibility in altering irradia-
tion programs as new data become available. The
requirement of special facilities, special sample
handling, and long irradiation time make the cost
for neutron irradiation experiments very high.
In contrast to neutron irradiation, ion (heavy,
light, or electrons) irradiation enjoys considerable
advantages in both cycle length and cost. Ion irradia-
tions of any type rarely require more than several
tens of hours to reach damage levels in the 1–100 dpa
range. Ion irradiation produces little or no residual
radioactivity, allowing handling of samples without

the need for special precautions. These features
translate into significantly reduced cycle length and
cost. The challenge then is to verify the equivalency
between neutron and ion irradiation in terms of
the changes to the microstructure and properties
of the material. The key question that needs to be
answered is how do results from neutron and charged
particle irradiation experiments compare? How, for
example, is one to compare the results of a component
irradiated in-core at 288  C to a fluence of 1  1021 n
cm
2 (E > 1 MeV) over a period of one year, with an ion
irradiation experiment using 3 MeV protons at 400  C
to 1 dpa (displacements per atom) at a dose rate of
10
5 dpa s
1 (1 day), or 5 MeV Ni2þ at 500  C to
10 dpa at a dose rate of 5  10
3 dpa s
1 (1 h)?
The first question to resolve is the measure of radia-
tion effect. In the Irradiation assisted stress corrosion
cracking (IASCC) problem in LWRs, concern has cen-
tered on two effects of irradiation: radiation-induced
segregation of major alloying elements or impurities to
grain boundaries, which may cause embrittlement or
enhance the intergranular stress corrosion cracking
(IGSCC) process, and hardening of the matrix that
results in localized deformation and embrittlement.
The appropriate measure of the radiation effect in the
former case would then be the alloy concentration at
the grain boundary or the amount of impurity
segregated to the grain boundary. This quantity is
measurable by analytical techniques such as AES, APT,
or STEM-EDS. For the latter case, the measure of the
radiation effect would be the nature, size, density, and
distribution of dislocation loops, black dots, and the
total dislocation network, and how they impact
the deformation of the alloy. Hence, specific and mea-
surable effects of irradiation can be determined for
both neutron and ion irradiation experiments.
The next concern is determining how ion irradia-
tion translates into the environment describing neu-
tron irradiation. That is, what are the irradiation
conditions required for ion irradiation to yield the
same measure of radiation effect as that for neutron
irradiation? This is the key question, for in a postirra-
diation test program, it is only the final state of
the material that determines equivalence, not the
path taken. Therefore, if ion irradiation experiments
could be devised that yielded the same measures
of irradiation effects as observed in neutron irradiation
experiments, the data obtained in postirradiation
experiments will be equivalent. In such a case, ion
irradiation experiments can provide a direct substitute
for neutron irradiation. While neutron irradiation will
always be required to qualify materials for reactor
Radiation Damage Using Ion Beams 197
application, ion irradiation provides a low-cost and
rapid means of elucidating mechanisms and screening
materials for the most important variables.
A final challenge is the volume of material that can
be irradiated with each type of radiation. Neutrons
have mean free paths on the order of centimeters
in structural materials. One MeV electrons penetrate
about 500 mm, 1 MeV protons penetrate about 10 mm,
and 1 MeV Ni ions have a range of less than 1 mm.
Thus, the volume of material that can be irradiated
with ions from standard laboratory-sized sources
(TEMs, accelerators), is limited.
1.07.3 Review of Aspects of Radiation
Damage Relevant to Ion Irradiation
1.07.3.1 Defect Production
The parameter commonly used to correlate the dam-
age produced by different irradiation environments is
the total number of displacements per atom (dpa).
Kinchin and Pease7 were the first to attempt to deter-
mine the number of displacements occurring during
irradiation and a modified version of their model
known as the Norgett–Robinson–Torrens (NRT)
model8 is generally accepted as the international
standard for quantifying the number of atomic dis-
placements in irradiated materials.9 According to the
NRT model, the number of Frenkel pairs (FPs),
nNRT(T ), generated by a primary knock-on atom
(PKA) of energy T is given by
kED ðT Þ
nNRT ðT Þ ¼ ½1
2Ed
where ED(T ) is the damage energy (energy of the
PKA less the energy lost to electron excitation), Ed is
the displacement energy, that is, the energy needed to
displace the struck atom from its lattice position, and k
is a factor less than 1 (usually taken as 0.8). Integration
of the NRT damage function over recoil spectrum and
time gives the atom concentration of displacements
known as the NRT displacements per atom (dpa):
ðð
dpa ¼ fðEÞvNRT ðT ÞsðE; T ÞdT dE ½2
where f(E) is the neutron flux and s(E,T ) is the proba-
bility that a particle of energy E will impart a recoil
energy T to a struck atom. The displacement damage is
accepted as a measure of the amount of change to the
solid due to irradiation and is a much better measure
of an irradiation effect than is the particle fluence.
As shown in Figure 1, seemingly different effects of
198 Radiation Damage Using Ion Beams

300 300

250 LASREF, 40 ⬚C 250 LASREF, 40 ⬚C

Yield stress change (MPa)

Yield stress change (MPa)

RTNS-II, 90 ⬚C RTNS-II, 90 ⬚C
OWR, 90 ⬚C OWR, 90 ⬚C
200 200

150 150

100 100

50 50

0 0
1017 1018 1019 1020 10−3 10−2
Neutron fluence, E > 0.1 MeV DPA

Figure 1 Comparison of yield stress change in 316 stainless steel irradiated in three facilities with very different neutron
energy flux spectra. While there is little correlation in terms of neutron fluence, the yield stress changes correlate well
against displacements per atom (dpa). Reprinted, with permission, from ASTM, copyright ASTM International, 100 Barr
Harbor Drive, West Conshohocken, PA 19428.

10−14
1014
Neutron flux/lethergy (n cm−2 s−1)

7.5 MeV tantalum

proton flux (ions cm−2 s−1)

1012 10−15
5 MeV nickel
Calculated dpa/(incident particle) (cm2)

1010
10−16 20 MeV carbon
Protons
108 ITER be first wall
HFIR target
FFTF mid-core 10−17
106 PWR 1/4-T RPV

1.3 MeV hydrogen

104 −9
10 10−7 10−5 10−3 10−1 10 10−18
Particle energy (MeV)

Figure 2 Energy spectrum for neutrons from a variety

10−19
of reactor types and a monoenergetic proton beam.
Reproduced from Stoller, R. E.; Greenwood, L. R. 14 MeV neutrons
J. Nucl. Mater. 1999, 271–272, 57–62.
−20 1 MeV neutrons
10
irradiation on low temperature yield strength for the
same fluence level (Figure 1(a)) and disappear when
10−21
dpa is used as the measure of damage (Figure 1(b)). 0 2 4 6 8 10 12
A fundamental difference between ion and neu- Distance into solid (m)
tron irradiation effects is the particle energy spectrum Figure 3 Displacement–damage effectiveness for various
that arises because of the difference in the way the energetic particles in nickel. Reproduced from Kulcinski,
particles are produced. Ions are produced in accel- G. L.; Brimhall, J. L.; Kissinger, H. E. In Proceedings of
erators and emerge in monoenergetic beams with Radiation-Induced Voids in Metals; Corbett, J. W.,
Ianiello, L. C., Eds.; USAEC Technical Information Center:
very narrow energy widths. However, the neutron Oak Ridge, TN, 1972; p 453, CONF-710601.
energy spectrum in a reactor extends over several
orders of magnitude in energy, thus presenting a
much more complicated source term for radiation Another major difference in the characteristics of
damage. Figure 2 shows the considerable difference ions and neutrons is their depth of penetration. As
in neutron and ion energy spectra and also between shown in Figure 3, ions lose energy quickly because
neutron spectra in different reactors and at different of high electronic energy loss, giving rise to a spa-
locations within the reactor vessel. tially nonuniform energy deposition profile caused
 Radiation Damage Using Ion Beams 199

by the varying importance of electronic and nuclear recoil atom to other target atoms. The fraction of
energy loss during the slowing down process. Their recoils between the displacement energy Ed, and T is
penetration distances range between 0.1 and 100 mm ð
1 T
for ion energies that can practically be achieved by PðE; T Þ ¼ sðE; T 0 ÞdT 0 ½6
laboratory-scale accelerators or implanters. By virtue N Ed
of their electrical neutrality, neutrons can penetrate where N is the total number of primary recoils and
very large distances and produce spatially flat dam- s(E,T ) is the differential cross-section for a particle
age profiles over many millimeters of material. of energy E to create a recoil of energy T. The recoil
Further, the cross-section for ion–atom reaction is fraction is shown in Figure 4, which reveals only a
much greater than for neutron–nuclear reaction giving small difference between ions of very different masses.
rise to a higher damage rate per unit of particle fluence. Figure 5 shows the difference in the types
The damage rate in dpa per unit of fluence is propor- of damage that are produced by different types of
tional to the integral of the energy transfer cross-section
and the number of displacements per PKA, nNRT(T):
1.0
ð gE He
Rd
¼ sðE; T ÞnNRT ðT ÞdT ½3
Nf Ed 0.8 H
Kr
Fraction of recoils
where Rd is the number if displacements per unit vol-
Ar
ume per unit time, N is the atom number density, and f 0.6
is the particle flux (neutron or ion). In the case of Ne
neutron–nuclear interaction described by the hard-
0.4 Fraction of recoils
sphere model, eqn [3] becomes with energy above
  Ed and below T
Rd gE
¼ ss ½4 0.2
Nf 4Ed 1 MeV ions ® Cu

where g ¼ 4mM/(m þ M)2, M is the target atom mass, m 0

101 102 103 104
is the neutron mass, E is the neutron energy, and ss is T (eV)
the elastic scattering cross-section. For the case of ion–
Figure 4 Integral primary recoil spectra for 1 MeV
atom interaction described by Rutherford scattering,
particles in copper. Curves plotted are the integral fractions
eqn [3] becomes of primary recoils between the threshold energy and recoil
  energy, T from eqn [6]. Reproduced from Averback, R. S.
Rd pZ2 Z2 e4 M1 gE J. Nucl. Mater. 1994, 216, 49.
¼ 1 2 ln ; ½5
NI 4EEd M2 Ed
1 MeV electrons E 106
where e is the unit charge, M1 is the mass of the ion, and T = 60 eV
M2 is the mass of the target atom. As shown in Figure 3, e = 50−100% 105
for comparable energies, 1.3 MeV protons cause over Tn
100 times more damage per unit of fluence at the 104
1 MeV protons Ti
sample surface than 1 MeV neutrons, and the factor T = 200 eV
e = 25% 103
for 20 MeV C ions is over 1000. Of course, the damage Tp
depth is orders of magnitude smaller than that for 102
Te
neutron irradiation. 1 MeV heavy ions
T = 5 keV Ed 101
e = 4% E
1.07.3.2 Primary and Weighted
Recoil Spectra 1 MeV neutrons
T = 35 keV
A description of irradiation damage must also con- e = 2%
sider the distribution of recoils in energy and space.
Figure 5 Difference in damage morphology, displacement
The primary recoil spectrum describes the relative efficiency, and average recoil energy for 1 MeV particles of
number of collisions in which the amount of energy different types incident on nickel. Reproduced from
between T and T þ dT is transferred from the primary Was, G. S.; Allen, T. R. Mater. Char. 1994, 32, 239.
200 Radiation Damage Using Ion Beams
particles. Light ions such as electrons and protons
will produce damage as isolated FPs or in small
clusters while heavy ions and neutrons produce dam-
age in large clusters. For 1 MeV particle irradiation of
copper, half the recoils for protons are produced with
energies less than 60 eV while the same number
for Kr occurs at about 150 eV. Recoils are weighted
toward lower energies because of the screened
Coulomb potential that controls the interactions of
charged particles. For an unscreened Coulomb inter-
action, the probability of creating a recoil of energy
T varies as 1/T2. However, neutrons interact as
hard spheres and the probability of creating a recoil
of energy T is independent of recoil energy.
In fact, a more important parameter describing the
distribution of damage over the energy range is a
combination of the fraction of defects of a particular
energy and the damage energy. This is the weighted
average recoil spectrum, W(E,T ), which weights the
primary recoil spectrum by the number of defects or
the damage energy produced in each recoil:
ðT
1
W ðE; T Þ ¼ sðE; T 0 ÞED ðT 0 ÞdT 0 ½7
ED ðEÞ Ed
ð T^
ED ðEÞ ¼ sðE; T 0 ÞED ðT 0 ÞdT 0
Ed
^ is the maximum recoil energy given by
where T
^ will need to be considered when designing an irradi-
T ¼ gEi ¼ 4EiM1M2/(M1 þ M2)2. Ignoring electron
excitations and allowing ED(T ) ¼ T, then the
weighted average recoil spectra for Coulomb and
hard sphere collisions are
lnT
lnEd
WCoul ðE; T Þ ¼
^
lnEd
lnT
T 2
Ed2
WHS ðE; T Þ ¼ ½10
Ed2
Equations [9] and [10] are graphed in Figure 6 for
1 MeV particle irradiations of copper. The character-
istic energy, T1/2 is that recoil energy below which
half of the recoils are produced. The Coulomb
forces extend to infinity and slowly increase as the
particle approaches the target; hence the slow
increase with energy. In a hard sphere interaction,
the particles and target do not interact until their
separation reaches the hard sphere radius at which
point the repulsive force goes to infinity. A screened
Coulomb is most appropriate for heavy ion irradia-
tion. Note the large difference in W(E,T ) between
the various types of irradiations at E ¼ 1 MeV.
1.0
Copper
0.8 Protons
0.6 Ne
Kr
W (T)
0.4
Neutrons
0.2
0
101 102 103 104 105 106 107
T (eV)
Figure 6 Weighted recoil spectra for 1 MeV particles in
copper. Curves representing protons and neutrons are
calculated using eqns [9] and [10], respectively. W(T ) for other
particles were calculated using Lindhard cross-sections
and include electronic excitation. Reproduced from
Averback, R. S. J. Nucl. Mater. 1994, 216, 49.
While heavy ions come closer to reproducing the
energy distribution of recoils of neutrons than do
light ions, neither is accurate in the tails of the distri-
½8 bution. This does not mean that ions are poor simu-
lations of radiation damage, but it does mean that
damage is produced differently and this difference
ation program that is intended to produce microche-
mical and microstructural changes that match those
from neutron irradiation.
There is, of course, more to the description of
radiation damage than just the number of dpa.
½9
There is the issue of the spatial distribution of damage
production, which can influence the microchemistry
and microstructure, particularly at temperatures
where diffusion processes are important for micro-
structural development. In fact, the ‘ballistically’
determined value of dpa calculated using such a
displacement model is not the appropriate unit to
be used for dose comparisons between particle
types. The reason is the difference in the primary
damage state among different particle types.
1.07.3.3 Damage Morphology
The actual number of defects that survive the dis-
placement cascade and their spatial distribution
in solids will determine the effect on the irradiated
microstructure. Figure 7 summarizes the effect of
 Radiation Damage Using Ion Beams 201

Total dpa

Particle type
and energy

Loss to Freely migrating

displacement defects
cascades

Mutual Loss to sinks Loss at grain

recombination in matrix boundaries
outside of cascade
Void swelling
Defect diffusion loop structure Boundary
matrix chemistry structure
and micro
chemistry

Radiation-induced
segregation
Figure 7 History of point defects after creation in the displacement cascade.

damage morphology from the viewpoint of the grain Displacement cascade efficiency
boundary and how the defect flow affects radiation- (x)
induced grain boundary segregation. Of the total
defects produced by the energetic particle, a fraction Intracascade thermal
recombination (z )
appears as isolated, or freely migrating defects, and the
balance is part of the cascade. The fraction of the Surviving defect
‘ballistically’ produced FPs that survive the cascade fraction (QDF) (x – z )
quench and are available for long-range migration is
an extremely important quantity and is called the Clustered point defect Isolated point defect
fraction (CDF) (d i,v) fraction (IDF) (g i,v)
migration efficiency, e. These ‘freely migrating’ or ‘avail-
able migrating’ defects10 are the only defects that will
affect the amount of grain boundary segregation, Mobile Immobile
which is one measure of radiation effects. The migra- clusters clusters
tion efficiency can be very small, approaching a few
percent at high temperatures. The migration effi- Evaporating
defects
ciency, e, comprises three components:
Available
gi,v: the isolated point defect fraction, defects (li,v)
di,v: clustered fraction including mobile defect
clusters such as di-interstitials, and Figure 8 Interdependence of isolated point defects,
z: fraction initially in isolated or clustered form mobile defect clusters, and thermally evaporating defect
clusters that contribute to the fraction of surviving defects
after the cascade quench that is annihilated during
that are ‘available’ for radiation effects. Reproduced from
subsequent short-term (>10
11 s) intracascade Zinkle, S. J.; Singh, B. N. J. Nucl. Mater. 1993, 199, 173.
thermal diffusion.
They are related as follows:
Due to significant recombination in the cascade,
e ¼ di þ g i þ z i ¼ d v þ g v þ z v ½11
only a fraction (30%) is free to migrate from the
Figure 8 shows the history of defects born as vacan- displacement zone. These defects can recombine out-
cies and interstitials as described by the NRT model. side of the cascade region, be absorbed at sinks in the
202 Radiation Damage Using Ion Beams
matrix (voids, loops), or be absorbed at the grain
boundaries, providing for the possibility of radiation-
induced segregation.
The fraction of defects that will be annihilated
after the cascade quench by recombination events
among defect clusters and point defects within the
same cascade (intracascade recombination), z, is
about 0.07, for a migration efficiency of 0.3 (see
below for additional detail).10 The clustered fraction,
d includes large, sessile clusters and small defect
clusters that may be mobile at a given irradiation
temperature and will be different for vacancies and
interstitials. For a 5 keV cascade, di is about 0.06 and
dv is closer to 0.18.10 Some of these defects may be
able to ‘evaporate’ or escape the cluster and become
‘available’ defects (Figure 8).
This leaves g, the isolated point defect fraction
that are available to migrate to sinks, to form clus-
ters, to interact with existing clusters, and to partic-
ipate in the defect flow to grain boundaries that
gives rise to radiation-induced segregation. Owing
to their potential to so strongly influence the irra-
diated microstructure, defects in this category, along
with defects freed from clusters, make up the freely
migrating defect (FMD) fraction. Recall that electrons
and light ions produce a large fraction of their
defects as isolated FPs, thus increasing the likeli-
hood of their remaining as isolated rather than clus-
tered defects. Despite the equivalence in energy
among the four particle types described in Figure 5,
the average energy transferred and the defect pro-
duction efficiencies vary by more than an order of
magnitude. This is explained by the differences in
the cascade morphology among the different parti-
cle types. Neutrons and heavy ions produce dense
cascades that result in substantial recombination
during the cooling or quenching phase. However,
electrons are just capable of producing a few widely
spaced FPs that have a low probability of recombi-
nation. Protons produce small widely spaced cas-
cades and many isolated FPs due to the Coulomb
interaction and therefore, fall between the extremes
in displacement efficiency defined by electrons and
neutrons.
The value of g has been estimated to range from
0.01 to 0.10 depending on PKA energy and irradia-
tion temperature, with higher temperatures resulting
in the lower values. Naundorf12 estimated the freely
migrating defect fraction using an analytical treat-
ment based on two factors: (1) energy transfer to
atoms is only sufficient to create a single FP, and
(2) the FP lies outside a recombination (interaction)
Table 1 Efficiency for producing freely migrating
defects, g, in nickel by different kinds of irradiations (Ed ¼ 40
eV, riv ¼ 0.7 nm) using Lindhard’s analytical differential
collision cross-section
Irradiation  (%)
1 MeV Hþ 24.0
2 MeV Hþ 19.2
2 MeV Liþ 16.9
1.8 MeV Neþ 8.7
300 keV Niþ 2.3
3 MeV Niþ 3.8
3.5 MeV Krþ 3.0
2 keV Oþ 9.8
Source: Naundorf, V. J. Nucl. Mater. 1991, 182, 254.
radius so that the nearby FPs neither recombine nor
cluster. The model follows each generation of the
collision and calculates the fraction of all defects
produced that remain free. Results of calculation
using the Naundorf model are shown in Table 1 for
several ions of varying mass and energy. Values of Z
range between 24% for proton irradiation to 3% for
heavy ion (krypton) irradiation. Recent results,13
however, have shown that the low values of FMD
efficiency for heavy ion or neutron irradiation cannot
be explained by defect annihilation within the parent
cascade (intracascade annihilation). In fact, cascade
damage generates vacancy and interstitial clusters
that act as annihilation sites for FMD, reducing the
efficiency of FMD production. Thus, the cascade
remnants result in an increase in the sink strength
for point defects and along with recombination in the
original cascade, account for the low FMD efficiency
measured by experiment.
1.07.3.4 Damage Rate Effects
As differences in dose rates can confound direct
comparison between neutron and ion irradiations, it
is important to assess their impact. A simple method
for examining the tradeoff between dose and temper-
ature in comparing irradiation effects from different
particle types is found in the invariance requirements.
For a given change in dose rate, we would like to know
what change in dose (at the same temperature) is
required to cause the same number of defects to be
absorbed at sinks. Alternatively, for a given change
in dose rate, we would like to know what change in
temperature (at the same dose) is required to cause
the same number of defects to be absorbed at
sinks. The number of defects per unit volume, NR,
that have recombined up to time t, is given by Mansur14
 Radiation Damage Using Ion Beams 203

ðt invariant at a fixed dose, the following relationship

NR ¼ Riv Ci Cv dt ½12 between ‘dose rate and temperature’ must hold:
   
0 kT12 K2
Evm þ2Evf ln K1
where Riv is the vacancy–interstitial recombination T2
T1 ¼     ½16
coefficient and Ci and Cv are interstitial and vacancy 1
EvmkT 1
þ2Evf ln K2
K1
concentrations, respectively. Similarly, the number of
where Evf is the vacancy formation energy. In the steady-
defects per unit volume that are lost to sinks of type j,
state recombination dominant regime, for NS to be invariant
NSj, up to time t, is
at a fixed temperature, the following relationship
ðt between ‘dose (F) and dose rate’ must hold:
NSj ¼ kSj Cj dt ½13  1=2
F2 K2
0 ¼ ½17
F1 K1
where kSj is the strength of sink j and Cj is the sink
concentration. The ratio of vacancy loss to interstitial Finally, in the steady-state recombination dominant regime,
loss is for NS to be invariant at a fixed dose rate, the following
relationship between ‘dose and temperature’ must hold:
RS ¼
NSv
½14    

2kT12
NSi Evm ln F 2
F1
T2
T1 ¼     ½18
where j ¼ v or i. The quantity NS is important in 1
kT 1
ln F2
Evm F1
describing the microstructural development involving
total point defect flux to sinks (e.g., RIS), while RS is the Figure 9 shows plots of the relationship between the
relevant quantity for the growth of defect aggregates ratio of dose rates and the temperature difference
such as voids that require partitioning of point defects required to maintain the same point defect absorption
to allow growth. In the steady-state recombination dominant at sinks (a), and the swelling invariance (b).
regime, for NS to be invariant at a fixed dose, the follow- The invariance requirements can be used to
ing relationship between ‘dose rate (Ki) and temperature prescribe an ion irradiation temperature–dose rate
(Ti)’ must hold: combination that simulates neutron radiation. We
 2   take the example of irradiation of stainless steel
kT1 K2
Evm ln K1 under typical BWR core irradiation conditions of
T2
T1 ¼     ½15
1
kT 1
ln K2 4.5  10
8 dpa s
1 at 288  C. If we were to conduct
Evm K1
a proton irradiation with a characteristic dose rate of
where Evm is the vacancy migration energy. In the 7.0  10
6 dpa s
1, then using eqn [15] with a vacancy
steady-state recombination dominant regime, for RS to be formation energy of 1.9 eV and a vacancy migration

700 50

600
40
Eνm = 0.5
DTemperature (⬚C)
DTemperature (⬚C)

500 Em
ν = 0.5
30
400 1.0
1.5
300 20

200 1.0
10
1.5
100

0 0
1 10 100 1000 1 10 100 1000
(a) Ratio of dose rates (b) Ratio of dose rates

Figure 9 Temperature shift from the reference 200  C required at constant dose in order to maintain (a) the same point
defect absorption at sinks, and (b) swelling invariance, as a function of dose rate, normalized to initial dose rate. Results are
shown for three different vacancy migration energies and a vacancy formation energy of 1.5 eV. Adapted from Mansur, L. K.
J. Nucl. Mater. 1993, 206, 306–323; Was, G. S. Radiation Materials Science: Metals and Alloys; Springer: Berlin, 2007.
204 Radiation Damage Using Ion Beams
energy of 1.3 eV, the experiment will be invariant in
NS with the BWR core irradiation (e.g., RIS) at a
proton irradiation temperature of 400  C. Similarly,
using eqn [16], a proton irradiation temperature of
300  C will result in an invariant RS (e.g., swelling
or loop growth). For a Ni2þ ion irradiation at a dose
rate of 10
3 dpa s
1, the respective temperatures are
675  C (NS invariant) and 340  C (RS invariant). In
other words, the temperature ‘shift’ due to the higher
dose rate is dependent on the microstructure feature
of interest. Also, with increasing difference in dose
rate, the DT between neutron and ion irradiation
increases substantially. The nominal irradiation tem-
peratures selected for proton irradiation, 360  C and
for Ni2þ irradiation, 500  C represent compromises
between the extremes for invariant NS and RS.
1.07.4 Contributions of Ion
Irradiation to an Understanding of
Radiation Effects
Ion irradiations have been critical to the development
of both our fundamental and applied understanding
of radiation effects. As discussed in Sections 1.07.2
and 1.07.3, it is the flexibility of such irradiations and
our firm understanding of atomic collisions in solids
that afford them their utility. Principally, ion irradia-
tions have enabled focused studies on the isolated
effects of primary recoil spectrum, defect displace-
ment rate, and temperature. In addition, they have
provided access to the fundamental properties of
point defects, defect creation, and defect reactions.
In this section, we highlight a few key experiments
that illustrate the broad range of problems that can
be addressed using ion irradiations. We concentrate
our discussion on past ion irradiations studies that
have provided key information required by modelers
in their attempts to predict materials behavior in
existing and future nuclear reactor environments,
and particularly information that is not readily
available from neutron irradiations. In addition, we
include a few comparative studies between ion
and neutron irradiations to illustrate, on one hand,
Table 2 Minimum displacement energies in pure metals, semiconductors, and stainless steel (SS)
Materials Al Cgraph Cu Fe
Tm (eV) 16 25 19 17
Source: Lucasson, P. In Fundamental Aspects of Radiation Damage in Metals; Robibnson, M. T., Young, F. W., Jr., Eds.; ERDA Report
CONF-751006; 1975; p 42; Andersen, H. H. Appl. Phys. 1979, 18, 131.
the good agreement that is possible, while on the other,
the extreme caution that is necessary in extrapolating
results of ion irradiations to long-term predictions
of materials evolution in a nuclear environment.
1.07.4.1 Electron Irradiations
The unique feature of electron irradiations in compari-
son to ions and neutrons is that they create defects in
very low-energy recoil events. As a consequence, nearly
all FPs are produced in isolation. This has been of
foremost importance in developing our understanding
of radiation damage, as it made studies of defect crea-
tion mechanisms as well as the fundamental properties
of FPs possible. Recall that the properties of vacancies
andvacancy clusters, for example, formation and migra-
tion energies, stacking fault energies, etc., could be
determined from quenching studies. It is not possible,
however, to quench in interstitials in metals. Very little
was therefore known about this intrinsic defect prior
to about 1955 when irradiation experiments became
widely employed. In this section, we highlight some of
the key findings derived from these past studies.
1.07.4.1.1 Displacement threshold surfaces
The creation of a stable FP requires that a lattice
atom receives an energy greater than Tm, which is
the minimum displacement energy. This value has
been determined experimentally in many materials
by measuring the change in some physical property,
such as electrical resistivity or length change, as a
function of maximum recoil energy of a target atom.
Such experiments are practical only for electron
irradiations for which recoil energies can be kept
low, but with the irradiation particles still penetrating
deeply into, or through, the specimen. Typical values
are shown in Table 2.
As a crystal is not homogeneous, the threshold
energy depends on the crystallographic direction in
which the knock-on atom recoils. The anisotropy of
the threshold energy surface has been mapped out in
various crystals by measuring the production rate of
defects as a function of both the electron energy, near
threshold, and the orientation of single crystalline
Ge Mo Ni W Si SS
15 33 23 41 13 18
 Radiation Damage Using Ion Beams 205

specimens with respect to the electron beam direc- The primary knock-on atom in an RCS recoils in
tion.15,16 The total cross-section for FP production the direction of its nearest neighbor, h110i in fcc
rate is given by the expression crystals, and replaces it, with the neighbor recoiling
2ðp p=2
also in the h110i and replacing its neighbor. A vacancy
ð
dsðy2 ; E1 Þ df2 is left at the primary recoil site, and an interstitial is
sd ðY1 ; F1 ; E1 Þ ¼ created at the end of the sequence. Replacement
dy2 2p ½19
0 0 sequences are the most efficient way to separate
nðY2 ; F2 ; T Þdy2 the interstitial far enough from its vacancy, 2–3
interatomic spacings, for the FP to be stable. While
where the subscripts 1 and 2 refer to incoming elec- the lengths of these sequences are still debated, it is
tron and recoiling ion, respectively, and Y1, F1, Y2, clear that the mechanism results in both defect pro-
F2 are the polar and azimuthal angles of the electron duction and atomic mixing. For neutron irradiations,
beam relative to the crystal axis; y2, f2, are these higher energy recoils are numerous, and the average
same angles relative to the beam direction; n is the displacement energy, Ed, becomes more relevant for
anisotropic damage function. Near threshold, n ¼ 1 calculations of defect production (see eqn [1]). This
for T > Tm, and 0 for T < Tm. By measuring the value, which can be obtained by averaging over the
production rate for many sample orientations and threshold displacement energy surface, is usually dif-
energies, the damage function can be obtained using ficult to determine experimentally. A rough estimate,
eqn [19], although various approximations are required however, can be obtained from, Td  1.4Tm in fcc
in the deconvolution. The results are illustrated metals and 1.6Tm in bcc metals.19
in Figure 10 for Cu.17 It is noteworthy that the
minimum threshold energy is located in the vicinity 1.07.4.1.2 Point defect properties
of close-packed directions. This is also true for bcc As FPs are produced in isolation during electron
metals. The anisotropy reflects the basic mechanism irradiation, the properties of single point defects
of defect production, viz., replacement collision and their interactions with impurities and sinks
sequences (RCSs), which had been identified by can be systematically investigated. An example is
molecular dynamics simulations as early as 1960.18 shown in Figure 11(a), where the results of low-
temperature isochronal annealing of Cu are shown
[111] following 1.4 MeV electron irradiation at 6 K.20
Recovery is observed to occur in ‘stages.’ These stud-
55 56 ies have revealed that interstitial atoms become
406 150 mobile at very low temperatures, always below
43 60 61 100 K, in so-called Stage I, while vacancies become
47
a 683 81 215 253 mobile at higher temperatures, Stage III. The various
18
43 43 31 24 26
substages IA–IE seen in Figure 11(a) arise from the
2 interaction between interstitial–vacancy pairs, which
b 208 103 11 4 0
22 are produced in close proximity. Stage IE refers to
28 45 25 20 22
6 9 69 3
the free migration of interstitials in the lattice, away
3 4
from its own vacancy, and annihilation at distant
30 26 24 23 20 20
27 vacancies; these interstitials are freely migrating as
11 10 3 4 6 3 4
discussed earlier. For comparison, Stage I annealing
23 25 25 29 23 21 20
23 of Cu following neutron irradiation is shown in
4 4 5 12 9 4 4 3
Figure 11(b).21 Notice that the close pair substages
23 23 25 29 23 21 20 22 are suppressed during neutron irradiation, illustrat-
18
2 2 2 4 10 3 3 2 3
ing the dramatic difference in the defect production
[100] [110] process for these types of irradiation. Similarly,
(a)
annealing studies on electron-irradiated Al doped
Figure 10 Displacement energy threshold surface for Cu. with Mg or Ga impurities are shown in Figure 12.22
The general anisotropy is typical of all fcc metals, although For these, it is observed that Stage I recovery is
specific values vary. bcc metals show similar behavior of
minima along close-packed directions. Reproduced from
suppressed as interstitials trap at impurities and do
King, W. E.; Merkle, K. L.; Meshii, M. Phys. Rev. B 1981, not recombine. The recovery at higher temperature,
23, 6319. in Stage II, reveals distinct subannealing stages.
206 Radiation Damage Using Ion Beams

IB ID 40

ID
7 IC Cu
30

dDr (% K–1)
(% K–1)

5
dDr

dT
dT

20
4 IE

°
°

IA IC

1
− Dr
1
− Dr

3
10 IB
2
IA
1

0 0
10 20 30 40 50 60 70 80 10 20 30 40 50 60 70
(a) T (K) (b) T (K)

Figure 11 Low-temperature isochronal annealing of Cu following (a) electron (reproduced from Corbett, J. W.; Smith, R. B.;
Walker, R. M. Phys. Rev. 1959, 114, 1452) or (b) fast neutron irradiation (reproduced from Burger, G.; Isebeck, K.;
Volkl, J.; Schilling, W.; Wenzl, H. Z. Angew. Phys. 1967, 22, 452).

threshold energies using low energy protons, to tens

100
Dr [nW.cm]
of keV using MeV self-ions. In addition, defect pro-
90 Al-0.06° at.%Mg °
Al-0.085 at.%Ga
2.5 duction rates can be varied over many orders of
magnitude, reaching values over 0.1 dpa s
1. More-
80 2.7
Al-(99.995%pure) 3.3
70
over, by using more than one ion beam, the primary
Dr/Dr0 (%)

60
recoil spectrum can be tailored to closely match that
50
produced by an arbitrary fission neutron spectrum.
40
30
1.07.4.2.1 The damage function
20
Calculations of defect production, eqn [2], require
10
knowledge of the damage function, n(T ). While it is
0
10 30 100 300 not possible to measure this function directly, as no
T (K)
irradiation creates monoenergetic recoils except near
Figure 12 Recovery of electrical resistivity in Al, the surface, it can be obtained by measuring defect
Al–0.06 at.% Ga, and Al–0.085 at.% Ga following 1 MeV production for a wide range of ion irradiations and
electron irradiation. Reproduced from Garr, K. R.; Sosin,
subsequently deconvoluting eqn [3]. Low-energy
A. Phys. Rev. 1969, 162, 669.
light ions, for example, weight the recoil spectrum
near the threshold energy, 25–100 eV, while more
These annealing stages are generally attributed to
energetic heavy ions weight it at high energies.
either the interstitial dissociating from the impurity,
Results are shown for Cu in Figure 13. Here, electri-
or the interstitial–impurity complex migrating to a
cal resistivity measurements are employed to monitor
vacancy or a defect sink. Migrating interstitial–solute
the absolute number of FPs produced per unit dose
complexes lead to segregation. A compilation of the
of irradiation. Included in this figure are the damage
properties of point defects for many metals, and their
efficiency function, x(T1/2), deduced from the experi-
interactions with impurities can be found in Ehrhart.23
ments and x(T ) calculated using molecular dynamics
This information has played a crucial role in develop-
computer simulation. The damage efficiency function
ing an understanding of radiation damage in more
is defined as
complex engineering alloys and under more complex
irradiation conditions. nðT Þ ¼ xðT ÞnNRT ðT Þ; ½20
where nNRT(T ) is the NRT damage function defined
1.07.4.2 Ion Irradiations
by eqn [1]. The good agreement between experiment
Ion irradiations are the most flexible method for and simulations illustrates that the damage function
irradiating materials. As discussed in Section 1.07.2, in Cu is now well understood. This is now true for
the primary recoil spectrum can be shifted from near many other pure metals as well.24 In alloys and ceramic

Cu
1 H
Experiment
Calculation
0.8 He
Li
0.6
x
CN
O Cu
Ne Kr
0.4 Ar Fe
Ag Bi
FF
0.2
FN
MD simulation
0 3.25 MeV Kr
10 2
10 3
10 4 5
10
T, T1/2 (eV)
Figure 13 Damage function efficiency factor of Cu
(see eqn [20]) showing the decrease in efficiency versus
cascade energy. The experimental data (solid squares)
represent efficiencies for different ion irradiations plotted
versus the characteristic cascade energy for the irradiation,
T1/2 (see text). The open triangles represent the efficiency
versus cascade energy, T, obtained by molecular dynamics
(MD) simulation. The open circles represent the calculated
efficiencies for the different irradiations using the MD
efficiency function and eqn [2]. Reproduced from Averback,
R. S.; de la Rubia, T. D. In Solid State Physics; Ehrenreich,
H., Spaepen, F., Eds.; Academic Press: New York, 1998; pp
281–402.
materials, however, the damage function remains
poorly known.
1.07.4.2.2 Freely migrating defects
The damage function refers to the number of FPs
created within the first several picoseconds of the
primary recoil event. At longer times, defects migrate
from their nascent sites and interact with other
defects and microstructural features. As noted earlier,
many radiation effects, such as radiation-enhanced
diffusion, segregation, and void swelling, depend more
strongly on the number of defects that escape their
nascent cascades and migrate freely in the lattice before
annihilating, trapping, or forming defect clusters. The
same general approach used to determine the damage
function has been employed to determine the relative
fraction of freely migrating defects, that is, e/nNRT, as
illustrated by Figure 14. Here, the relative number of
Si atoms segregating to the surface during irradiation,
per dpa, is plotted versus a characteristic energy of
the recoil spectrum, T1/2. It is seen that the fraction
decreases rapidly with increasing recoil energy. Simi-
lar experiments were performed using radiation-
enhanced diffusion, as described in Section 1.07.2.
While ion irradiation has proved extremely useful
in illustrating the spectral effects on freely migrating
Radiation Damage Using Ion Beams 207
1.0 1 MeV H
Relative efficiency
0.8
0.6
2 MeV He
0.4 2 MeV Li
0.2
3 MeV Ni
0
102 103 104 105 106 107
T1/2 (eV)
Figure 14 Relative efficiencies for producing freely
migrating defects plotted as a function of the characteristic
recoil energy, T1/2. Reproduced from Rehn, L. E.;
Okamoto, P. R.; Averback, R. S. Phys. Rev. 1984,
B30, 3073.
defects, extracting quantitative information about
freely migrating defects from such experiments is
difficult. These measurements, unlike the damage
function, require very high doses, and several dpa;
the buildup of the sink structure must be adequately
taken into account. It is also difficult to estimate,
for example, how many interstitials are required to
transport one Si atom to the surface. We mention in
passing that experiments performed using ordering
kinetics in order–disorder alloys have provided a
more direct measure of the number of freely migrat-
ing defects (vacancies in this case), as these experi-
ments require doses less than 10
7 dpa so that no
damage build-up can occur.25 These experiments
show similar effects of primary recoil spectrum on
the fraction of freely migrating defects, although the
fractions of such defects were found to be somewhat
higher in these experiments, 5–10%. These frac-
tions are in good agreement with radiation-enhanced
diffusion experiments using self-ions on Ni, when the
effect of sink strength is taken into account.26
1.07.4.2.3 Alloy stability under ion irradiation
Irradiation of materials with energetic particles drives
them from equilibrium, and in alloys, this becomes
manifest in a number of ways. One of them concerns
nonequilibrium segregation. The creation of large
supersaturations of point defects leads to persistent
defect fluxes to sinks. In many cases, these point defect
fluxes couple with solutes, resulting in either the
enrichment or depletion of solutes at these sinks.
This effect was first discovered by using in situ electron
208 Radiation Damage Using Ion Beams

irradiations in a high voltage electron microscope,27
and it has been systematically investigated subse-
quently using ion irradiations,28 as the surface sink
provides a convenient location to measure composi-
tion changes. Unlike neutron irradiation, moreover,
the damage created by ions is generally inhomoge-
neous, reaching a peak level at some depth in the
sample. As a consequence, point defect fluxes ema-
nate from these regions. An example of this effect is
shown in Figure 15 where a Ni–12.7 at.% Si alloy
was irradiated with protons. As the alloy is supersat-
urated with Si prior to irradiation, Ni3Si precipitates
Ni3Si surface film
Ni plating
Bombarded surface
Figure 15 Behavior of silicon in a Ni–12.7 Si alloy
following irradiation with protons. Note the region depleted
of Ni3Si precipitates at the peak damage location and just
below the surface. Courtesy of P. R. Okamoto.
form in the sample. At the location of peak damage,
the concentration of interstitials is the highest, and
hence these defects flow outward from this region.
These interstitials form interstitial–solute complexes
with Si, resulting in a Si flux out of this area as well,
depleting the region of Si. As a consequence, a region
depleted of Ni3Si precipitates is observed at the
peak damage depth. Note too that the surface sink
for interstitials leads to enrichment of Si, resulting in
a surface layer of Ni3Si. The region just below the
surface accordingly becomes depleted of Si, leaving a
zone depleted of Ni3Si precipitates.
While irradiation induced segregation can lead to
nonequilibrium segregation and precipitation in sin-
gle phase alloys, irradiation can also lead to dissolu-
tion of precipitates in nominally two-phase alloys.
An interesting example of this behavior concerns
Ni–12 at.% Al alloys irradiated with 300 keV Ni
ions.29 These alloys were first annealed at high tem-
peratures to develop a two-phase structure of Ni3Al
(g0 ) and Ni–10.5 at.% Al (g). The initial precipitate
size, depending on the annealing time was 2.5 or
Peak 4.6 nm. As shown in Figure 16, the precipitates dis-
damage
region order during irradiation at room temperature, owing
to atomic mixing in cascades. The rate of disordering
depends on the size of the precipitates, being slowest
for homogeneous Ni3Al sample and fastest in the
alloy with the smallest precipitates. The authors

1.0
1.0 Ni3AI Ni3AI
Degree of LRO S/S0

Degree of LRO S/S0

NiAI (r = 4.6 nm) NiAI (r = 4.6 nm)

0.8 NiAI (r = 2.5 nm)
0.6
0.5
0.4
550 ⬚C
0.2
450 ⬚C
0.0 0.0
0.00 0.05 0.10 0.15 0.20 0.25 0.30 0.0 2.0 4.0 6.0
(a) Irradiation dose F (dpa) (b) Irradiation dose F (dpa)

0.8
0 dpa 2 dpa 5 dpa
f(r )

0.4

0.0
0.0 4.0 8.0 0.0 4.0 8.0 0.0 4.0 8.0
(c) Radius (nm)
Figure 16 (a) Disordering rate Ni3Al precipitates in two-phase Ni–12 at.% Al alloys and homogeneous Ni3Al during 300 keV
Ni bombardment at room temperature; (b) same as (a) but irradiation at 550  C; (c) size distribution of Ni3Al precipitates
after irradiation to two doses. After 5 dpa, a steady state size is obtained. Reproduced from Schmitz, G.; Ewert, J. C.;
Harbsmeier, F.; Uhrmacher, M.; Haider, F. Phys. Rev. B 2001, 63, 224113.

suggest that the reason for this dependence on pre-
cipitate size is that atomic mixing reduces the
concentration of Al in the precipitates, which
thereby accelerates the disordering. When the same
irradiation is performed at higher temperatures, and
radiation-enhanced diffusion takes place, the system
does not completely disorder, but rather remains
partially ordered, owing to a competition between
disordering in the displacement cascades and reor-
dering by radiation-enhanced diffusion. Noteworthy,
however, is the size of the precipitate, as shown in
Figure 16(c), where it is observed that the precipi-
tates initially shrink in size, but then reach a steady
state radius. Therefore, unlike in thermal aging, pre-
cipitates in irradiated alloys can reach a stable steady
state size that is a function of irradiation intensity and
temperature. Similar behavior has been observed in
two-phase immiscible alloys in which case a steady
state size of precipitates is formed.30 This so-called
‘patterning’ phenomenon has been explained on the
basis of a competition between disordering by atomic
mixing in energetic collision events and reordering
during thermally activated diffusion. For patterning,
however, it is required that the atomic relocation
distances during collisional mixing are significantly
larger than the nearest neighbor distance. An inter-
esting consequence of this requirement in regard to
the present discussion of using ion irradiation to
simulate neutron damage is that electron and proton
irradiations, which do not produce energetic cascades
or long relocation distances, should not induce com-
positional patterning, but heavy ions and fast neutron
irradiation, which do produce cascades, will cause
patterning. Further details can be found in Enrique31
and Enrique et al.32
1.07.4.2.4 Mechanical properties
Measurements of mechanical properties on irra-
diated materials usually require bulk samples and
therefore neutron irradiation. Ion beams, however,
can be employed for some measurements, such as
plastic deformation. Typically, these experiments
employ high energy protons, E >  2 MeV, or He
ions, E > 7 MeV, as these particles can penetrate
through thin foils, such as Fe or steel, that are greater
than 15 mm in thickness. Moreover, displacement
rates 10
5 dpa s
1 are obtainable without excessive
beam heating.33 Deformation experiments have also
been performed using GeV heavy ions, as these pen-
etrate targets several microns in thickness. The dis-
placement rates, however, are low as most of the beam
energy is lost through electronic excitations. Heavy
Radiation Damage Using Ion Beams 209
ions with lower energies, E  1–4 MeV, have also
been used in deformation studies; for these, however,
specimen must be very thin, 200 nm, and effects of
the surface must be taken into account.34,35
1.07.4.2.5 Multiple ion beams
One of the difficulties in using ion beams to simulate
neutron irradiation damage is the potential for miss-
ing certain synergistic behaviors in the damage evo-
lution. For example, neutron irradiation leads to
transmutation products and the generation of He
and fission gases in addition to displacement damage.
Generation of gas is particularly relevant to 14 MeV
neutron irradiation for which large amounts of
He and H are produced. Ion beams, however, offer
the opportunity of using two or even three beams
simultaneously and thus to tailor test irradiations to
meet expected reactor conditions; see, for example,
Serruys et al.36 This is often not possible in existing
test reactor facilities, and the building of new test
facilities for fusion machines has been formidably
expensive. The application of multiple ion beams is
illustrated in Figure 17 in a study of void swelling in
vanadium. Here, the synergistic effects of simulta-
neously implanting 350 keV H and 1 MeV He, while
irradiating with 12 MeV Ni ions are shown. Without
the He beam, swelling is negligible, even with the
implantation of H, but with it, the H greatly enhances
the swelling. H implantation, on the other hand, is
seen to reduce the density of cavities.
1.07.4.2.6 Swift ions
An important contribution to the damage in nuclear
fuels derives from fission fragments. There are two
groups of fission products: one group with atomic
number near 42 (Mo) and energy 100 MeV and
the other with atomic number near 56 (Ba) and
energy 70 MeV. The maximum electronic stopping
powers of these energetic particles, 18 keV nm
1
for the heavier and 22 keV nm
1 for the lighter, are
far greater than their respective nuclear stopping
powers. Similar to ion irradiation studies described
above, where the primary recoil spectrum can be
systematically varied, the masses and energies of
ions can be varied to examine effects of electronic
stopping power. An example is shown in Figure 18
where the electronic stopping power is plotted as a
function of energy (per nucleon) for different ion
irradiations of UO2. The two boxes in the figure
indicate stopping powers associated with the fission
fragments and the heavy particle recoils of a emit-
ters. One of the questions addressed by such studies
210 Radiation Damage Using Ion Beams

20

Cavity density (1020 m−3)

20

Swelling (%)
15
10
20 10
20
5
15
0
0
20 10 10
20
He

He
10
(ap

10 5

(ap
pm

pm
0
)d

0 0 0

)d
20
pa

20 10

pa
10 0
–1

0 pa–1

–1
p p m ) d p a–1 (b) H (a p p m ) d
(a) H(a
Figure 17 Cavity volume fraction (a) and cavity density (b) in pure vanadium irradiated with 12 MeV Ni3þ ions to 30 dpa
at 873 K with and without simultaneous irradiation of He and H. Reproduced from Sekimura, N.; Iwai, T.; Arai, Y.; et al.
J. Nucl. Mater. 2000, 283–287, 224–228.

70
dE/dx (keV nm–1)

Energy (MeVamu–1)

238U
20 1.4
1.2
60 Light FP Heavy FP 1.0 208Pb
0.8
10
0.6
50 0.4
197Au
235
U Fission 0.2
0 0.0
−8 −6 −4 −2 0 2 4 6 8
dE/dx (keV nm–1)

40 FPs range (μm)

129Xe

116Sn
30
GANIL GSI 106Cd
HMI TASCC 100Mo
127I
20 dE/dxFP

70Zn
Recoils
10
Zn70Zn
Efission
0
10−5 10−4 10−3 10−2 10−1 1 10 102
Energy (MeVamu–1)
Figure 18 Plot of dE/dx as a function of the energy for a series of ions. The circle indicates the conditions for 72 MeV
ions of 127I. The two large squares show dE/dx representative of fission products and for the heavy recoil atoms of
a-decaying actinides. The inset shows the energy loss and the remaining energy of typical light and heavy fission
products along their range of 7 mm length. Reproduced from Matzke, Hj.; Lucuta, P. G.; Wiss, T. Nucl. Instrum. Meth. B
2000, 166–167, 920.

has been the formation of fission fragment tracks.
Tracks have not yet been observed in the bulk of
UO2 due to fission; however, by using ion irradiation,
the stopping powers could be increased. The dashed
line at 29 keV nm
1 in Figure 18 represents the
threshold stopping power for track formation.37
This value is 30% greater than the maximum for
fission fragments, thus helping to explain why fission
fragment tracks are not seen in the bulk. Such tracks
are observed, however, close to the surface. They are
explained by fission products passing near or parallel
to the surface and creating shock waves which inter-
act with the surface.38 These studies have also been
useful in gaining important data for understanding
fission gas evolution in nuclear fuels. For example,
72 MeV iodine ions (see Figure 18), approximate
very closely the stopping power of fission fragments.
Such studies have shown that 72 MeV I irradiations
cause Kr atoms preimplanted into UO2 to nucleate
into bubbles, and preformed bubbles to undergo res-
olution. A radiation-enhanced diffusion coefficient
for the Kr was estimated from these studies to be
D  1.2  10
30 cm5  F_ , where F_ is the fission rate
per cubic centimeter, and found independent of tem-
perature below 500  C (see Matzke et al.37 for details).
The importance of such studies as these is that
the basic processes in complex nuclear fuels can be
elucidated by studies that carefully control singly
the irradiation conditions and materials parameters
in the fuel, such as fission gas concentration, damage, etc.
1.07.4.3 Comparison with Neutrons
Proton irradiation has undergone considerable
refinement as a radiation damage tool. Numerous
experiments have been conducted and compared
to equivalent neutron irradiation experiments in
order to determine whether proton irradiations cap-
ture the effects of neutron irradiation on microstruc-
ture, microchemistry, and hardening. In some cases,
benchmarking exercises were conducted on the same
native alloy heat as neutron irradiation in order to
eliminate heat-to-heat variations that may obscure
comparison of the effects of the two types of irradiat-
ing particles. The following examples cover a number
of irradiation effects on several alloys in an effort to
demonstrate the capability of proton irradiation
to capture the critical effects of neutron irradiation.
Figures 19–23 show direct comparisons of the
same irradiation feature on the same alloy heats
(commercial purity (CP) 304 and 316 stainless steels)
following either neutron irradiation at 275  C or
Radiation Damage Using Ion Beams 211
24 8
CP-316 SS
Protons at 360 ⬚C to 1.0 dpa
Neutrons at 275 ⬚C to
7
1.1⫻1021 n cm–2 (~1.5 dpa)
20
6
Measured Cr or Ni (wt%)
Measured Si (wt%)
5
16 Cr
4
Ni
3
12
2
Si
8 1
0
−12 −8 −4 0 4 8 12
Distance from grain boundary (nm)
Figure 19 Comparison of grain boundary segregation of
Cr, Ni, and Si in commercial purity 16 stainless steel
following irradiation with either protons or neutrons to
similar doses. From Was, G. S.; Busby, J. T.; Allen, T.; et al.
J. Nucl. Mater. 2002, 300, 198–216.
3 MeV proton irradiation at 360  C to similar doses.
Figure 19 compares the RIS behavior of Cr, Ni, and
Si in a 316 stainless steel alloy following irradiation to
approximately 1 dpa. Neutron irradiation results are
in open symbols and proton irradiation results are in
solid symbols. This dose range was chosen as an
extreme test of proton irradiation to capture the
‘W’-shaped chromium depletion profile caused by
irradiation of a microstructure, which contained
grain boundaries that were enriched with chromium
prior to irradiation. Note that the two profiles track
each other extremely well, both in magnitude and
spatial extent. Good agreement is obtained for all
three elements.
Figure 20 shows a comparison of the dislocation
microstructure as measured by the dislocation loop
size distribution (Figure 20(a)) and the size and
number density of dislocation loops (Figure 20(b))
for 304 SS and 316 SS. The main features of the loop
size distributions are similar for the two irradiations,
viz. a sharply peaked distribution in the case of 304
SS and a flatter distribution with a tail in the case of
316 SS. The agreement in loop size is good for the
304 SS alloy, while loops are smaller for the proton-
irradiated 316 alloy. The loop density is about a
factor of 3 less for the proton-irradiated case than
the neutron-irradiated case, which is expected as the
proton irradiation temperature was optimized to
track RIS (higher temperature) rather than the
212 Radiation Damage Using Ion Beams

Fraction of loop population (%)

50
Fraction of loop population (%)
30 Protons at 360 ⬚C (1.0 dpa)
Protons at 360 ⬚C 40
(1.0 dpa) Neutrons at 275 ⬚C (1.1 dpa)
Neutrons at 275 ⬚C 30
20 (0.7 dpa)
20
10
CP 304 SS 10 CP 316 SS

0 0
0 5 10 15 20 25 30 0 5 10 15 20 25 30
(a) Loop diameter (nm) Loop diameter (nm)

12 1024

10
Loop diameter (nm)

Loop density (m−3)

8 1023

4 1022
304 316 304 316
2 Protons at 360 ⬚C Protons at 360 ⬚C
Neutrons at 275 ⬚C Neutrons at 275 ⬚C
0 1021
0 1 2 3 4 5 6 0 1 2 3 4 5 6
(b) Dose (dpa) Dose (dpa)

Figure 20 Comparison of (a) loop size distributions and (b) loop diameter and loop number density for commercial
purity 304 and 316 stainless steels irradiated with neutrons or protons to similar doses. From Was, G. S.; Busby, J. T.;
Allen, T.; et al. J. Nucl. Mater. 2002, 300, 198–216.

1500 1500
CP 304 SS CP 316 SS
Yield strength (MPa)

Yield strength (MPa)

1000 1000

500 500

0 0
0 1 2 3 4 5 6 0 1 2 3 4 5 6
(a) Dose (dpa) (b) Dose (dpa)

Protons at 360 ⬚C (hardness)

Neutrons at 275 ⬚C (hardness)
Neutrons at 275 ⬚C (shear punch)

Figure 21 Comparison of hardening in commercial purity 304 (a) and 316 (b) stainless steel irradiated with neutrons or
protons to similar doses. From Was, G. S.; Busby, J. T.; Allen, T.; et al. J. Nucl. Mater. 2002, 300, 198–216.

dislocation loop microstructure. That the loop sizes much smaller than those from neutron irradiation.
and densities are even close is somewhat remarkable The surviving fraction of interstitial loops, however,
considering that loop density is driven by in-cascade is greater for proton irradiation, partially compensat-
clustering, and cascades from proton irradiation are ing the greater loop formation rate under neutron
 Radiation Damage Using Ion Beams 213

Fast neutron fluence (E > 1 MeV) ⫻1025 n m−2 1.4

0 0.5 1 1.5 2 2.5 3 3.5 4
Neutrons
1.2
100 With He
CP 304 SS
Protons at 360 ⬚C Without He
Neutrons at 275 ⬚C 1
NWC
80
Measured IG percentage

0.8

s/s0
60 0.6

0.4
40

0.2
20
0
0 0.5 1 1.5 2 2.5
Dose (dpa)
0
0 1 2 3 4 5 6 Figure 24 Comparison of relaxation in residual stresses
Dose (dpa) between neutron- and proton-irradiated stainless steel after
removing the effect of thermally-induced relaxation. From
Figure 22 Comparison of the extent of intergranular Sencer, B. H.; Was, G. S.; Yuya, H.; Isobe, Y.; Sagasaka, M.;
stress corrosion cracking in commercial purity 304 stainless Garner, F. A. J. Nucl. Mater. 2005, 336, 314–322.
steel following similar stress corrosion cracking tests of
either neutron- or proton-irradiated samples from the same
heat. From Was, G. S.; Busby, J. T.; Allen, T.; et al. J. Nucl.
Mater. 2002, 300, 198–216. are again similar, with proton irradiation resulting in
slightly lower hardness. Figure 22 shows the IASCC
susceptibility of CP 304 SS as measured by the %IG on
the fracture surface following constant load testing
80 0.14
(neutron-irradiated samples) and constant extension
Ni+ irradiation
70 675 ⬚C 0.13 rate testing (proton-irradiated samples) in BWR nor-
Swelling (%) neutron and Ni ion

60
140 dpa
0.12
mal water chemistry (NWC). Despite the significantly
Swelling (%) protons

different testing mode, the results are in excellent

50 Proton irradiation 0.11 agreement in that both proton and neutron irradiation
400 ⬚C
40 3.0 dpa 0.10 result in the onset of IGSCC, at about 1 dpa.40
Figure 23 shows the swelling behavior in austen-
30 Neutron irradiation 0.09 itic stainless steels as a function of nickel content
510 ⬚C
20 2.6 ⫻ 1026 n m−2 0.08 for proton, Ni ion, and neutron irradiation. While
E > 0.1 MeV these experiments were conducted on different sets
10 0.07
of alloys, and under highly disparate irradiation con-
0 0.06 ditions, they all show the same dependence of nickel
0 20 40 60 80 100
Bulk nickel concentration (at.%)
on swelling. In the two commercial purity alloys,
no voids were formed in either neutron or proton-
Figure 23 Effect of bulk nickel concentration on swelling
irradiated samples.
resulting from irradiation with different particles: neutrons,
nickel ions, and protons. Reproduced from Allen, T. R.; As a last example of stainless steel alloys,
Cole, J. I.; Gan, J.; Was, G. S.; Dropek, R.; Al Kenik, E. Figure 24 shows the relaxation of residual stress by
J. Nucl. Mater. 2005, 341, 90–100. neutron and proton irradiation. Here again, results
are from different alloys and different types of
tests, but both show the same dependence of stress
irradiation and resulting in loop densities that are relaxation on dose.
within a factor of 3.39 The next examples are from reactor pressure vessel
Figure 21 shows a comparison of irradiation hard- steel and Zircaloy. Figure 25 shows an experiment on
ening between the two types of irradiation. The results model reactor pressure vessel alloys in which the
214 Radiation Damage Using Ion Beams

500 300
VA, Fe, neutron Tin = 300 ⬚C (all)
VA, Fe, proton −7
Proton: 3–7 ⫻ 10 dpa s–1
−10
400
VA, Fe, electron Neutron: 3 ⫻ 10 dpa s–1 280
VD, Fe–0.9Cu–1.0 Mn, neutron −9
Electron: 7 ⫻ 10 dpa s–1
VD, Fe–0.9Cu–1.0 Mn, proton
Change in yield strength (MPa)

VD, Fe–0.9Cu–1.0 Mn, electron

260

Vickers hardness (Hv)

VH, Fe–0.9Cu, neutron
300
VH, Fe–0.9Cu, proton

240
200
220

100
200
p - Zircaloy 4, 350 ⬚C
n - Zircaloy 2, 350–400 ⬚C
0
180 p - Zircaloy 4, 310 ⬚C

−100 160
10−5 10−4 10−3 10−2 10−1 0 1 2 3 4 5 6 7 8
Dose (dpa) Dose (dpa)
Figure 25 Irradiation hardening in model reactor pressure Figure 26 Hardening of Zircaloy-4 irradiated with 3 MeV
vessel steels following neutron, proton, and electron protons at 310 and 350  C and comparison to neutron-
irradiation at about 300  C. From Was, G. S.; Hash, M.; irradiated Zircaloy-2. From Zu, X. T.; Sun, K.; Atzmon, M.;
Odette, G. R. Philos. Mag. 2005, 85(4–7), 703–722. et al. Philos. Mag. 2005, 85(4–7), 649–659.

same model alloy heats were irradiated with neu- 2.5 MeV electrons, 3.0 MeV protons, and fission neu-
trons, electrons, or protons at 300  C to doses span- trons.41 An attempt was made to keep all irradiation
ning two orders of magnitude. The alloys include a variables constant during the experiments, sample
high-purity Fe heat (VA) that hardens very little purity, defect production rate, and temperature; only
under irradiation, an Fe–0.9Cu (VH) heat that hard- the primary recoil spectrum was varied. The results
ens rapidly initially, followed by a slower hardening for nucleation rates of voids and void swelling are
rate above 0.1 mpda, and a Fe–0.9Ce–1.0Mn alloy shown in Figure 27(a) and 27(b), respectively.
(VD) in which the hardening rate is greatest over Clearly observed is that void swelling and void
the dose range studied. Despite the very different nucleation are significantly enhanced for neutron
compositions and hardening rates, the results of the irradiation in comparison to proton or electron
three types of irradiation agree well. irradiation. This result is notably in strong contrast
Figure 26 shows hardening for Zircaloy-2 and to the efficiencies obtained for defect production and
Zircaloy-4 irradiated with either neutrons or protons. radiation-induced segregation (or FMDs) for these
Although the irradiations were not conducted three types of irradiation. The reduced efficiency of
on the same heats of material, or using similar the production of FMDs was attributed to defect anni-
irradiation parameters, there is good agreement in hilation within the cascade core; these results for void
the magnitude and dose dependence of hardening. swelling, however, indicate that the defect clustering
Proton irradiation also induced amorphization of a process is also critical to microstructural evolution in
Zr(Fe,Cr)2 precipitate after irradiation to 5 dpa irradiated alloys. Singh and coworkers41,42 argue that
at 310  C, similar to that observed in reactor. These the clustering of interstitials in cascades, and their
examples represent a comprehensive collection of collapse into dislocation loops, result in interstitial
comparison data between proton and neutron irradia- migration by one-dimensional glide of loops, the
tion and taken together serve as a good example for the so-called production bias model.43 As a consequence,
capability of charged particles to emulate the effect of interstitials and vacancies become efficiently sepa-
neutron irradiation on the alloy microstructure. rated. Swelling therefore is more severe for irradia-
As a final example, to emphasize the care that tions that produce energetic cascade, for example,
must be exercised in extrapolating the results of one neutrons, than for those that do not, electrons. Proton
type of irradiation to make predictions for another, irradiation is intermediate; that is, small cascades are
we discuss a comparison of void swelling in Cu due to produced.
 Radiation Damage Using Ion Beams 215

100
Copper
523 K
10−1
1022
Copper
10−2 523 K
Swelling (%)

1021

Void density (m−3)

Fission neutrons
10−3
20 3 MeV protons
10

10−4
Fission neutrons 1019
3 MeV protons 2.5 MeV electrons
2.5 MeV electrons
10−5 −4 1018 −4
10 10−3 10−2 10−1 100 10 10−3 10−2 10−1 100
Dose (NRT dpa) Dose (NRT dpa)

Figure 27 Void swelling as a function of dose in oxygen-free high conductivity (OFHC)-copper during irradiations with
electrons, protons, and fission neutron. Reproduced from Singh, B. H.; Eldrup, M.; Horsewell, A.; Ehrhart, P.; Dworschak,
F. Philos. Mag. A 2000, 80, 2629.

1.07.5 Advantages and 60

Disadvantages of Irradiations using
ton = 50 ms
Various Particle Types
50 toff = 2000 ms

Each particle type has its advantages and disadvan-

tages for use in the study of radiation effects or for 40
emulating neutron irradiation damage. Common dis-
K0/K0,avg

advantages of charged particle beams are the lack of

30
transmutation reactions and the need to use a raster-
scanned beam. With the exception of some minor
transmutation reactions that can occur with light 20
ion irradiation, charged particles do not reproduce
the types of transmutation reactions that occur in
10
reactor core materials due to the interaction with
K0,avg
neutrons. The most important of these is the produc-
tion of He by transmutation, particularly in alloys 0
0 1 2 3 4 5 6 7
that contain elements such as Ni or B. But a second
Time (ms)
consideration is that of a raster-scanned beam in
which any volume element of the target is exposed Figure 28 The effect of a raster-scanned beam on the
instantaneous production rate of point defects with the
to the beam for only a fraction of the raster-scan
same time averaged rate as a continuous source. From
cycle. For a typical beam scanner and beam para- Was, G. S.; Allen, T. R. In Radiation Effects in Solids, NATO
meters, the fraction of time that any particular vol- Science Series II: Mathematics, Physics and Chemistry;
ume element in the solid is being bombarded is Sickafus, K. E., Kotomin, E. A., Uberuaga, B. P., Eds.;
0.025. Thus, the instantaneous dose rate during Springer: Berlin, 2007; Vol. 235, pp 65–98.
the beam-on portion of the cycle is 40 times that of
the average, Figure 28. The result is that the defect rate in raster-scanned systems will be less, and must
production rate is very high and defects can anneal be accounted for.
out in the remaining 0.975 portion of the cycle One objective of ion irradiation is to emulate
before the beam again passes through the volume the effect of neutrons, and a second is to understand
element. As such, the effective defect production basic physical radiation damage processes, for which
216 Radiation Damage Using Ion Beams
neutron irradiation is often less well suited. While
ion irradiation can be conducted with great control
over temperature, dose rate, and total dose, such
control is a challenge to reactor irradiations. For
example, instrumented tubes with active temperature
control are expensive to design, build, and operate.
Even so, frequent power changes can be difficult
to handle as the flux–temperature relationship will
change and this can result in artifacts in the irradiated
microstructure.44 On the other hand, temperatures in
cheaper irradiation vehicles that use passive gas gaps
and gamma heating (such as ‘rabbit’ tubes) are known
with even less certainty. While neutron dosimetry
is used in some experiments, doses and dose rates
are often determined by neutronic models of the
core locations and are not verifiable. As such, ion
irradiations enjoy the advantage of better control
and verification of irradiation conditions as compared
to neutron irradiation. Table 3 provides a list for
each of three particle types: electrons, heavy ions,
and light ions (protons), and they are discussed in
detail in the following sections.
1.07.5.1 Electrons
Electron irradiation is easily conducted in a high-
voltage transmission electron microscope using either
Table 3 Advantages and disadvantages of irradiations with various particle types
Advantages
Electrons
Relatively ‘simple’ source – TEM
Uses standard TEM sample
High dose rate – short irradiation times
Heavy ions
High dose rate – short irradiation times
High Tavg
Cascade production
Light ions
Accelerated dose rate – moderate irradiation times
Modest DT required
Good depth of penetration
Flat damage profile over tens of microns
Source: Was, G. S.; Allen, T. R. In Radiation Effects in Solids, NATO Science Series II: Mathematics, Physics and Chemistry;
Sickafus, K. E., Kotomin, E. A., Uberuaga, B. P., Eds.; Springer: Berlin, 2007; Vol. 235, pp 65–98.
a hot filament or a field emission gun as an electron
source. An advantage is that the same instrument
used for irradiation damage can be used to image
the damage. Another advantage is that the high dose
rate requires very short irradiation time, but will
also require a large temperature shift as explained
in the Section 1.07.3.
There are several disadvantages to electron irra-
diation using a TEM. First, energies are generally
limited to 1 MeV. This energy is sufficient to produce
an isolated FP in transition metals, but not cascades.
The high dose rate requires high temperatures that
must be closely monitored and controlled, which is
difficult to do precisely in a typical TEM sample
stage. Another drawback is that as irradiations are
often conducted on thin foils, defects are created in
close proximity to the surface and their behavior may
be affected by the presence of the surface. Perhaps
the most serious drawback is the Gaussian shape to
the electron beam that can give rise to strong dose
rate gradients across the irradiated region. Figure 29
shows the composition profile of copper around a
grain boundary in Ni–39%Cu following electron
irradiation. Note that while there is local depletion
at the grain boundary (as expected), the region adja-
cent to the minimum is strongly enriched in copper
because of the strong defect flux out of the irradiated
Disadvantages
Energy limited to 1 MeV
No cascades
Very high beam current (high dpa rate) leading to large temperature
shifts relative to neutrons
Poor control of sample temperature
Strong ‘Gaussian’ shape (nonuniform intensity profile) to beam
No transmutation
Very limited depth of penetration
Strongly peaked damage profile
Very high beam current (high dpa rate) leading to large temperature
shifts relative to neutrons
Potential for composition changes at high dose via implanted ion
No transmutation
Minor sample activation
Smaller, widely separated cascade
No transmutation
 Radiation Damage Using Ion Beams 217

8
9
7
8
6 494 ⬚C
D+

Si concentration (at.%)
7
5
Cu concentration (at.%)

e-beam 6
4 diameter
8
6 400 ⬚C
e−
7
5
6
4
5
6
−4 −3 −2 −1 0 1 2 3 4
400 ⬚C
Distance from grain boundary (μm)
5
Figure 31 Comparison of (a) deuteron and (b) electron
4 irradiation showing the greater amount of segregation and
−6 −4 −2 0 2 4 6 the narrower profile for the deuteron irradiation. From
Distance from grain boundary (μm) Wakai, E. Trans. J. Nucl. Mater. 1992, 33(10), 884.

Figure 29 Enrichment of copper surrounding a local

depletion at the grain boundary. The enrichment is caused zone defined by the horizontal line below the spec-
by the high defect flux away from the irradiated region trum. This outward-directed defect flux causes a
defined by the horizontal line. From Ezawa, T.; Wakai,
E. Ultramicroscopy 1991, 39, 187.
reversal in the direction of segregation from that
caused by a defect flux to the sink. Another often
observed artifact in electron irradiation is very
broad grain boundary enrichment and depletion
60
profiles. Figure 30 shows that the enrichment profile
for Ni and the depletion profiles for Fe and Cr in
stainless steel have widths on the order of 75–100 nm,
50 which is much greater than the 5–10 nm widths
Solute concentration (wt%)

Iron observed following neutron irradiation under similar

Chromium conditions and model simulations of radiation-
Nickel induced segregation. A similar effect was observed
40
by Wakai45 using electron and Dþ irradiation of the
same alloy in which the segregation profile was much
30 higher and narrower around the grain boundary in
the deuteron-irradiated sample as compared to the
electron irradiation (Figure 31).
20

1.07.5.2 Heavy Ions

10 Heavy ions enjoy the benefit of high dose rates
0 100 200 300 400 500 600
Distance (nm)
resulting in the accumulation of high doses in short
times. Also, because they are typically produced in
Figure 30 Broad grain boundary enrichment and the energy range of a few MeV, they are very efficient
depletion profiles in Fe–20Cr–25Ni–0.75Nb–0.5Si following
irradiation with electrons at 420  C to 7.2 dpa. From
at producing dense cascades, similar to those pro-
Ashworth, J. A.; Norris, D. I. R.; Jones, I. P. J. Nucl. Mater. duced by neutrons. The disadvantage is that as with
1992, 189, 289. electrons, the high dose rates require large
218 Radiation Damage Using Ion Beams

15
dpa versus depth for

14 MeV nickel ions (dpa per 1016 ions cm−2)

various ions
incident on nickel C

5 MeV carbon ions (dpa per 1016 ions cm−2)

12 1.2

(dpa per 1016 ions cm−2)

8.1 MeV aluminum ions
Ni
5 1.0
9
Al
4 0.8

6 3 0.6

2 0.4
3
1 0.2

Ni
Al
C
0 0 0
0 0.5 1 1.5 2 2.5 3
Depth (μm)

Figure 32 Damage profiles for C, Al, and Ni irradiation of a nickel target at energies selected to result in the same
penetration depth. From Whitley, J. B. Ph.D. Thesis, University of Wisconsin-Madison, Madison, WI, 1978.

250 1.5 1.5

3.2
5 MeV Ni2+ on Ni
Displacement rate (10−3 dpa s–1)

2.8
200
2.4
Observed 1
1
Swelling (%)

2 150

1.6
dpa 100
1.2
0.5 0.5
0.8
50
0.4

0 0 0 0
0 0.2 0.4 0.6 0.8 1 1.2 1.4 1.6 0 0.2 0.4 0.6 0.8 1 1.2 1.4 1.6
(a) Depth (μm) (b) Depth (μm)
þ
Figure 33 (a) Subsurface swelling resulting from 5 MeV Ni ion irradiation of Fe–15Cr–35Ni at 625  C and (b) displacement
rate and ion deposition rate calculated for 5 MeV Ni2þ on nickel. Adapted from Garner, F. A. J. Nucl. Mater. 1983, 117,
177–197; Lee, E. H.; Mansur, L. K.; Yoo, M. H. J. Nucl. Mater. 1979, 85&86, 577–581.

temperature shifts so that irradiations must be con- peaks sharply at only 2 mm below the surface. As a
ducted at temperatures of 500  C in order to create result, regions at a very well-defined depth from the
similar effects as neutron irradiation at 300  C. surface must be isolated and sampled in order to
Clearly, there is not much margin for studying neu- avoid dose or dose rate variation effects from sample
tron irradiations at higher reactor temperature to sample. Small errors (500 nm) made in locating the
as higher ion irradiation temperatures will cause volume to be characterized can result in a dose that
annealing. Another drawback is the short penetration varies by a factor of 2 from the target value.
depth and the continuously varying dose rate over A problem that is rather unique to nickel ion irra-
the penetration depth. Figure 32 shows the damage diation of stainless steel or nickel-base alloys is that in
profile for several heavy ions incident on nickel. addition to the damage they create, each bombarding
Note that the damage rate varies continuously and Ni ion constitutes an interstitial. Figure 33(a) shows

that 5 MeV Ni2þ irradiation of a Fe–15Cr–35Ni alloy
resulted in high swelling in the immediate subsurface
region compared to that near the damage peak. As
shown in Figure 33(b), the Ni2þ ions come to rest at a
position just beyond the peak damage range. So even
though the peak damage rate is about 3 that at the
surface, swelling at that location is suppressed by
about a factor of 5 compared to that at the surface.46
The reason is that the bombarding Ni2þ ions consti-
tute interstitials and the surplus of interstitials near
the damage peak results in a reduction of the void
growth rate.47,48 In the dose rate–temperature regime
where recombination is the dominant point defect
loss mechanism, interstitials injected by Ni2þ ion
bombardment may never recombine as there is no
corresponding vacancy production.
1.07.5.3 Light Ions
In many ways, proton irradiation overcomes the
drawbacks of electron and neutron irradiation.
The penetration depth of protons at a few MeV can
exceed 40 mm and the damage profile is relatively flat
such that the dose rate varies by less than a factor
of 2 over several tens of micrometers. Further, the
depth of penetration is sufficient to assess such prop-
erties as irradiation hardening through microhardness
measurements, and stress corrosion cracking through
crack initiation tests such as the slow strain rate test.
10−15
2+
5 MeV Ni
10−16
10−17
dpa/(ion cm−2)
3.2 MeV protons
10−18
10−19
10−20
1 MeV neutrons
10−21
10−22
0 10 20 30
Depth (μm)
Figure 34 Damage profiles for 1 MeV neutrons, 3.2 MeV
protons, and 5 MeV Ni2þ ions in stainless steel. From Was,
G. S.; Allen, T. R. In Radiation Effects in Solids, NATO
Science Series II: Mathematics, Physics and Chemistry;
Sickafus, K. E., Kotomin, E. A., Uberuaga, B. P., Eds.;
Springer: Berlin, 2007; Vol. 235, pp 65–98.
Radiation Damage Using Ion Beams 219
Figure 34 shows schematics of 3.2 MeV proton and
5 MeV Ni2þ damage profiles in stainless steel. Super-
imposed on the depth scale is a grain structure with a
grain size of 10 mm. Note that with this grain size,
there are numerous grain boundaries and a significant
irradiated volume over which the proton damage rate
is flat. The dose rate for proton irradiations is 2–3
orders of magnitude lower than that for electrons or
ions, thus requiring only a modest temperature shift,
but as it is still 102–103 times higher than neutron
irradiation, modest doses can be achieved in reason-
ably short irradiation time.
The disadvantages are that because of the
small mass of the proton compared to heavy ions,
the recoil energy is smaller and the resulting damage
morphology is characterized by smaller, more widely
spaced cascades than with ions or neutrons. Also,
as only a few MeV are required to surmount the Cou-
lomb barrier for light ions, there is also a minor amount
of sample activation that increases with proton energy.
1.07.6 Practical Considerations for
Radiation Damage Using Ion Beams
In the process of setting up an ion irradiation experi-
ment, a number of parameters that involve beam
105
Ion
H
1000 He
Ni
Calculated range (μm)
10
0.1
Calculated by SRIM 2000
Stainless steel (Fe–20Cr–10Ni)
0.001
40 0.01 0.1 1 10 100
Energy (MeV)
Figure 35 Range of hydrogen, helium, and nickel ions in
stainless steel as a function of ion energy. From Was, G. S.;
Allen, T. R. In Radiation Effects in Solids, NATO Science
Series II: Mathematics, Physics and Chemistry; Sickafus,
K. E., Kotomin, E. A., Uberuaga, B. P., Eds.; Springer: Berlin,
2007; Vol. 235, pp 65–98.
220 Radiation Damage Using Ion Beams

characteristics (energy, current/dose) and beam-
target interaction must be considered. ASTM E 521
provides standard practice for neutron radiation
damage simulation by charged-particle irradiation49
and ASTM E 693 provides standard practice for
characterizing neutron exposures in iron and low
alloy steels in units of dpa.9 One of the most important
considerations is the depth of penetration. Figure 35
shows the range versus particle energy for protons,
helium ions, and nickel ions in stainless steel as
calculated by SRIM.50 The difference in penetration
depth between light and heavy ions is over an order
of magnitude in this energy range. Figure 36 shows
how several other parameters describing the target
10−4
Dose rate (dpa s−1)
behavior during proton irradiation vary with energy,
dose rate, the time to reach 1 dpa, deposited energy,
and the maximum permissible beam current (which
will determine the dose rate and total dose), given a
temperature limitation of 360  C. With increasing
energy, the dose rate at the surface decreases because
of the drop in the elastic scattering cross-section
(Figure 36(a)). Consequently, the time to reach a
target dose level, and hence the length of an irradia-
tion, increases rapidly (Figure 36(b)). Energy depo-
sition scales linearly with the beam energy, raising
the burden of removing the added heat in order
to control the temperature of the irradiated region
(Figure 36(c)). The need to remove the heat due
to higher energies will limit the beam current at
a specific target temperature (Figure 36(d)), and a
limit on the beam current (or dose rate) will result in
a longer irradiation to achieve the specified dose.

Figure 37 summarizes how competing features of

10−5 an irradiation vary with beam energy, creating trade-
offs in the beam parameters. For example, while
10−6 greater depth is generally favored in order to increase
(a)
the volume of irradiated material, the higher energy
10−7
600 required leads to lower dose rates near the surface
Time to reach 1 dpa (h)

500 At 360 ⬚C
and higher residual radioactivity. For proton irradia-
At 400 ⬚C tion, the optimum energy range, achieved by balanc-
400
300 ing these factors, lies between 2 and 5 MeV as shown
200 by the shaded region.
100
0
(b) 400
Energy deposited (W)

500 400
300
Residual
activity Energy 350
200
maximum
Residual activity (arbitrary units)

400 Energy
minimum due to
100 residual 300
due to
depth activity Time to reach 1 dpa (h)
0 penetration 250
(c) 300
Range (μm)

100 Range
Beam current (μA)

80 Maximum current at 360 ⬚C 200

Maximum current at 400 ⬚C
60 200
150
40
Time to 1 dpa
100
20 100
0 50
5 10 15 20
(d) Energy (MeV)
0 0
1 2 5 10 20
Figure 36 Behavior of beam-target parameters as a
Energy (MeV)
function of beam energy proton irradiation at 360  C;
(a) dose rate, (b) time to reach 1 dpa, (c) energy deposition, Figure 37 Variation of ion range, residual activity, and
and (d) beam current limit to maintain a sample temperature time to reach 1 dpa as a function of proton energy.
of 360  C. From Was, G. S.; Allen, T. R. In Radiation Reproduced from Was, G. S.; Allen, T. R. In Radiation
Effects in Solids, NATO Science Series II: Mathematics, Effects in Solids, NATO Science Series II: Mathematics,
Physics and Chemistry; Sickafus, K. E., Kotomin, E. A., Physics and Chemistry; Sickafus, K. E., Kotomin, E. A.,
Uberuaga, B. P., Eds.; Springer: Berlin, 2007; Vol. 235, Uberuaga, B. P., Eds.; Springer: Berlin, 2007; Vol. 235,
pp 65–98. pp 65–98.
 Radiation Damage Using Ion Beams 221

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