Theory and Experimental Background On Dimensional Changes in Irradiated Alloys
Theory and Experimental Background On Dimensional Changes in Irradiated Alloys
Theory and Experimental Background On Dimensional Changes in Irradiated Alloys
Abstract
When a material is irradiated with energetic neutrons or charged particles, a complex sequence of reactions takes
place. Structure, composition, and properties are altered over an extremely wide scale, spanning atomic defects,
meso-scale microstructures and macroscopic properties. Particularly interesting are radiation-induced dimensional
changes, Such changes, which can occur in engineered components of fission and fusion reactors on a scale of
meters, are driven by lattice defects at the subnanometer level. Because of their technological importance and their
high scientific challenge, the dimensional changes termed radiation-induced swelling and creep have elicited
sustained intensive research by basic and applied materials scientists for many years. The present paper is intended
as a brief tutorial on salient features of this work. The presentation is divided into three parts. Background is first
sketched emphasizing experimentally observed features and applications. Next, the theoretical framework and
specific models that have been developed to understand radiation-induced swelling and creep in isotropic materials
are described. Lastly, selected experiments designed and/or interpreted in terms of theory are highlighted to
illustrate the current state of understanding of the physical bases of these phenomena.
particles can displace atoms in a material by elastic developed to understand the dimensional changes, are
collisions, by other types of nuclear reactions, or, in the described. This section includes necessary background
case of y-rays, by the production of reaction electrons. on microstructures and mechanisms. The following
The primary knock-on atoms (pkas), ions and electrons part, Section 4, describes direct comparisons of the
also can cause extensive ionization and electronic exci- theory with special experiments designed to probe
tation. Generally, neutrons and heavy ions in the MeV mechanisms. Such comparisons have been key to devel-
range impart so much energy to the pka that a dis- oping the present high level of understanding of di-
placement cascade is produced consisting of highly mensional changes under irradiation.
localized production of interstitials and vacancies asso- The present paper is intended to be tutorial in
ciated with a single initiating event. The processes and nature, for readers interested in the above topics. By
reaction pathways by which the displacement and elec- reference, it incorporates an extended book chapter by
tronic energy are dissipated determine the structure the author [l], that more fully develops the theory and
and property changes exhibited by the material. the experimental background, and contains a more
In the present paper we concentrate on swelling complete set of references.
and creep in metals and alloys. Related phenomena in
a range of these and other materials must be excluded
because of length limitations. The presentation is given 2. Experimental background
in three major subdivisions. First, in Section 2, basic
experimental background and facilities are described. 2.1. Dimensional changes
This includes a sketch of the historical origins of re-
search on swelling and creep. Next, in Section 3, major Swelling was discovered in 1967 during electron
elements of the kinetic theory of radiation effects, microscopy investigations of a stainless steel irradiated
Fig. 1. Photograph of 316 stainless steel rods before and after irradiation at 533°C to a fluence of 1.5 X 10z3 n/m* in the EBR-11
reactor.
L.K. Mansur/Jounuzl of Nuclear Materials 216 (1994) 97-123 99
Fig. 3. Artist’s rendition of the Experimental Breeder Reactor-II (EBR-II). Shown are the reactor vessel, internals, and reactor
core. EBR-II is located at Idaho Falls, Idaho.
100 L.K. Mansur/Journal of Nuclear Materials 216 (1994) 97-123
Fig. 5. Artist’s rendition of the multiple ion laboratory at Oak Ridge, TN. The three beam lines are configured so that the ion
beams can be impinged on a target simultaneously.
L.K Manmr/Joumal of Nuclear Materials 216 (1994) 97-123 101
Irradiation creep can help accommodate stresses these property changes are shown. The striped ellipti-
induced by differential swelling. If it is too large, cal images are interstitial dislocation loops formed by
however, irradiation creep can lead to buckling of the planar aggregation of interstitials. The light images
components. Another significant consequence of irra- are cavities, a new ‘phase’ consisting of empty space,
diation creep is that it can rapidly undo engineered introduced by irradiation. Cavity volume in aggregate
stress distributions. Thus, for example, clamps or other represents the macroscopic swelling of the crystal; the
devices designed to maintain a stress under normal empty atomic lattice sites in the cavities account for an
conditions would be quickly rendered ineffective under equivalent enlargement of the crystal by the addition of
irradiation. Fig. 7 illustrates this point. A tightened new atomic lattice sites. The darker images are second
bolt irradiated under the typical conditions of a fast phase precipitates, in general of different structure and
reactor would loosen its hold after a small dose [12]. composition than the matrix. Tangled linear images in
the micrograph are dislocation lines.
2.3. Structure and composition The dislocations are major participants in the pro-
cesses of swelling and creep. An extra lattice site
Wholesale development of structure and composi- created by the attachment of an interstitial to a dislo-
tion on near-atomic and larger scales, often referred to cation, corresponding to an empty site in a cavity,
as ‘microstructure’ and ‘microcomposition’, is responsi- causes climb of the dislocation by one lattice site.
ble for swelling, creep and other property changes. Fig. Irradiation creep can occur by the stress-directed glide
8 is a transmission electron micrograph of a 300 series of dislocations released from obstacles by climb result-
stainless steel irradiated at about 500°C to a dose of 10 ing from the absorption of point defects. This is termed
dpa [13]. Many of the extended defects that underlie climb-enabled glide creep. Another type of creep, climb
Fig. 8. Transmission electron micrograph of a 300 series stainless steel irradiated at 500°C to a dose of 10 dpa. After Ref. [13].
L.R Mansur/Joumal of Nuclear Materials 216 (1994) 97-123 103
Precipitates, examples of which can be seen in Fig. UNSTABLE htATRIx 10” 6 DISPLAcaD PRIMAaY lo%V
1 *
8, may affect swelling and creep in several ways. These INIzRsTlTlAL DIFFUSION 10' I DISPLKED SECONDARIES 10’ eV
1 I
ways include what can be termed direct, indirect and
VACANCY DIIWJSION 1 I UNSI-ABE h5Allux 1 CV
mediated effects [15]. An example of a direct effect 1 &
would be the attachment of a cavity to a precipitate. MIcROSt’R”cIuRAL EVOLUTION 1~7’
I THERMAL DIFFUSION kT
1261. The equations for j = 1 have special importance Here L? is atomic volume, rc is cavity radius, the D’s
and will be described subsequently. If we imagine j to are diffusion coefficients, the Zc’s are cavity capture
be a continuous variable and use a Taylor series expan- efficiencies, the C’s are physical point defect concen-
sion in Eq. (2) to relate all functions to their values at trations and C”(r,) is the thermal concentration of
size j, we simplify the description to a continuum point defects at a cavity of radius rc. The subscripts i
diffusional approximation in size space, known as a and v denote interstitials and vacancies, respectively.
Fokker-Planck equation, The concentrations are obtained by solving the con-
tinuity equations
acj(r)
-=-$Cj(t)[w(j: j+l)-w(i;i-I)]} Wv
at kTVU, + G, - RC,Ci - K,C, = ~
+~~{Cj(t)[W(j;i-l)+W(j;i+l)l}. (6)
and
(3)
DiCi ac,
The first term in Eq. (3) describes a ‘drift’ in size V DiVCi + - kT VUi + Gi- RC,Ci - KiCi= at
space driven by the excess condensation of one point
defect type over the other, in analogy with the physical (7)
drift of diffusing species in real space due to elastic or
Here G denotes vacancy or interstitial generation by
coulombic forces, for example. The second term de-
displacement and thermal emission from sinks. R is
scribes a ‘diffusion’ in size space, analogous to diffu-
the recombination coefficient given by rlrr,(Di + D,),
sion of matter or energy in real space. The first term
where rr, is the radius of the recombination volume.
ensures that a large cluster will grow inexorably in a
The remaining terms on the left sides describe losses to
radiation field; the second term accounts for the fact
sinks. These are modeled in two ways. The terms
that two different clusters introduced at the same time
involving spatial derivatives describe leakage and drift
at the same size may differ in size at a later time due to
to a sink modeled as discrete. The symbol U is interac-
random encounters with point defects.
tion energy with the discrete sink, and the K, is the
Cavity nucleation theory and cavity growth theory
reaction rate constant that describes the loss rates per
start with Eqs. (2) or (3), as described in Ref. 111.Both
unit point defect concentration of type (Y to sinks
theories are developed in some detail there. Later
modeled as distributed throughout the continuum. Of
discussion in the present paper is based on cavity
these sinks there may be II types such as dislocations,
growth theory and, therefore, its origin is sketched
cavities, dislocation loops, and so on, and K,,i = C,
below. The simplest form of the theory assumes that
Kc,i where K:,i is the vacancy or interstitial loss rate to
there are only point defects and point defect sinks,
the particular sink of type n. Here K:,i is defined as
such as dislocations, cavities, grain boundaries and
the product of a sink strength S~,i, and the appropriate
precipitates, for example. The clusters such as cavities
diffusion coefficient Dv,i. It should also be pointed out
and dislocation loops are characterized by the dimen-
that here and in the remainder of this paper, diffusion
sion j, indicating the number of contained point de-
is considered to be isotropic. The form of the sink
fects or the dimension r, indicating the cluster radius.
strength is discussed in the next section.
In Eq. (3) only the first term in curly braces is
The right sides of Eqs. (6) and (7) express changes
retained in growth theory. Rewriting in terms of the
in defect concentration with time. However, except at
variable r gives
low temperatures, the relaxation times for changes in
the concentrations are generally much shorter than
at ar ’ (4) characteristic times for changes in K, and K, by
microstructural evolution. When the right sides of Eqs.
where now r replaces j and N(r) dr replaces Cj as the (6) and (7) are set to zero (steady-state conditions), and
number density of clusters at sizes between r and when we treat all sinks according to continuum de-
r + dr. The important term in describing the cluster scriptions, Eqs. (6) and (7) become algebraic equations
growth rate is i,, the time derivative of the cavity that are easily solved for C, so that
radius. Cluster growth theory centers on physical
mechanisms affecting i,. The growth rate of a cavity of c = [KiKv+R(Gi-Gv)I
radius rc is determined by the net flux of vacancy ” 2R.K
volume per unit cavity area per unit time
[(
4RG,KiK,
dr,_fi
- ; [ Z,CD,C, - - r,)] . x If (8)
dt
ZtDiCi Z;D$Z( (5) [KiK,+R(Gi-G,)]’
106 L.K. Mansur/Journal of Nuclear Materials216 (1994) 97-123
and I I I I I I I
T=275% Cdm)
c,= [KiKv+R(Gv-Gi)I ,n-6~__,_ C,(6) /
I
2RKi
4RGiKiK,
(9)
[K,K,+R(G,-GJ]~
More will be said about non-steady state conditions
later.
Table 1
Concentrations and losses of point defects - limiting cases
Regime CV =i NS NR
Steady state
Sinks dominant
G G RGqA
(7 > 7,) 118
E Ki KiK,
L.K. h4ansur/Joumal of Nuclear Materials 216 (1994) 97-123 107
temperature shift derived in the same way and for the tion capture radius for the point defect. The subscripts,
recombination dominated steady-state case to keep v or i are used to denote the different radii for vacan-
swelling rate invariant is, cies and interstitials. Generally, Zd > Z,” because rdi >
rdv. When cavities or other sinks are included, Eq. (18)
(kTf/( JY + 2.@))ln(G2/Gl)
PI takes on a more complex form that includes not only
T2 - T1 = 1 - (kT,/( EF + 2E,f)) In(G,/G,) ’ dislocation parameters but parameters of all other
where Et denotes the vacancy formation energy. The sinks in the system. Results for both random and
derivation of temperature shifts for swelling is de- periodic arrays are given elsewhere [31].
scribed more fully in Ref. [30]. The treatment in Ref. The sink strength of a grain boundary is obtained in
[30] for swelling is general in the sense that equations a similar way
are derived for temperature shift where point defect 60
sink strengths are different under conditions 1 and 2 @= _ S1’2d -C 1,
d2 ’
and where point defect loss can be dominated by
recombination or by sinks. Eq. (16) is highly simplified. and
Similar generalizations for Eqs. (13)-(15) are straight- 6S”2
forward. S@’= -, S”2d > 1, (21)
d
3.4. Sink strengths and sink efficiencies where d is the grain diameter. Note that when other
The sink strengths in Eqs. (8) and (9) determine the sinks are important, Eq. (21), the strengths of these
point defect concentrations. In these equations, K = other sinks are an inherent part of the grain boundary
DS, where S is the sink strength, i.e., the sink strength sink strength.
is that quantity which, when taken in a product with
3.5. Swelling
the volume-averaged point defect concentration and
the point defect diffusion coefficient, gives the loss rate When the expressions (8) and (9) for the point
to all sinks of that specific type. The sink strength is defect concentrations are substituted into Eq. (51, we
obtained by solving the spatial diffusion problem for obtain
the type of sink in question, such as a cavity, disloca-
tion, or grain boundary. This solution shows that the dr,_R
- ,(zfz: -Z,dZF)F,
point defect loss rate is given by a simple integral dt
property of the sinks times the bulk point defect con- where F is a function of total dislocation and cavity
centration. The theory of sink strengths has been dis- sink strengths and of their ratio, of dose rate, and of
cussed extensively in Ref. [31]. point defect recombination [l]. The quantity ZdZt -
A derivation of the sink strength of a cavity is given Z,dZF is the bias. It determines the capacity for swelling;
in Ref. [l], where results for other sinks are also it must be positive in order for any swelling to occur. It
quoted. The sink strength of a cavity is obtained as expresses the partitioning of vacancies to cavities and
wr,/D interstitials to dislocations. Values of this quantity nec-
SC= 4ar,( 1 + S112rC) (17)
1 + S’12rC + wr,/D ’ essary to explain observed swelling range from about
0.01 to 1 depending on the material and on values
where S is the total sink strength of all types of sinks.
assigned to other parameters, particularly defect gener-
The first part (4prC) is a simple geometric term, the
ation rate and vacancy migration energy. About an
second part (1 + S112rJ is often designated as a multi-
order of magnitude of this two orders of magnitude
ple sink correction or interactive term, and the third
range is trivial. Some researchers assume that the
part is the sink capture efficiency, designated as Zc.
defect production rate is the same as the damage
The latter measures how good an absorber the sink is.
production rate (i.e., K = G, for example). Thus, a
Alternatively, the second (interactive) and third terms
small bias will produce the correct void growth, since
can be lumped together as a generalized capture effi-
G and bias, ZdZyC- Z,dZF, occur only as a product.
ciency. Here w is the point defect transfer velocity at
Other researchers use a more realistic value of G -C K.
the cavity surface.
In this case the bias must be larger, but the product of
The result for the straight dislocation is
G and bias is unaffected. These considerations are
Sd = ZdL) (18) discussed fully in Ref. [l].
where Eq. (22) can be written in two limiting forms:
2?r
Zd= 1’2 Qf/“Q:/‘( ZfZ,c - Z,“??)
(19)
ln(rL/rd)
(1 + Qi)l’*( 1 + QV)1’2
Here L is the dislocation density, r,=(TL)-l/* is a
measure of dislocation spacing and r, is the disloca- (recombination dominated) (23)
L.L Mansur/Journal of Nuclear Materials 216 (1994) 97-123 109
DOSE DEPENDENCE
RELATlVE RATES
OF SWELLlNG
OF EVOLUTlON
IS DETERMINED
OF THE VARIOUS
BY THE
MODES OF
(23) and (24) are multiplied by 4ar,fN, so that the left
POINT DEFECT LOSS AND GENERATION side becomes I’; the void volume fraction, V= $rr2Nc.
DOSE DEPENDENCE OF SWELLING CAN BE PREDICTED BY THE
THEORY. FOR EXAMPLE, FOR RECOMBINATION MINOR AND
Large classes of experimental observations can be ex-
DISLOCATION DENSITY SENSlBLY CONSTANT pressed as simple phenomenological relations [l]. At
the early stages every vacancy in a cavity may be
matched by an interstitial in a dislocation loop. In this
case L a V’/*. At higher doses dislocation loops give
way to a dislocation network whose density is main-
tained constant by competing loop formation and seg-
ment annihilation processes. In this case, L = constant.
DOSE
These results are inserted into Eqs. (23) and (24).
The results show that swelling may be expressed as
proportional to (dose)“, where n may take on values
EXPERlMENTALLY OBSERVED BEHAVIOR OF SEVERAL TYPES IS
CONSISTENT WlTH THIS PICTURE. KEY PARAMETER IS 0. from 3/5 to 3 [l]. In general, during an extended
irradiation, several regimes of characteristic exponents
will be traversed. Fig. 13 is a schematic depiction of the
predicted dose dependence of swelling. These theoreti-
cal predictions for dose dependence of swelling are
generally in agreement with results observed experi-
OBSERVED FOR FAST REACTOR OBSERVED FOR MATERIALS.
IRRADIATION OF STAINLESS WlTH HlGH CAVITY DENSITY, mentally, as discussed in section 4.3.
STEEL, LOW HELIUM, TYPICAL HIGH HELIUM, LOW
SINK STRENGTHS DISLOCATION DENSITY
The temperature dependence of swelling implied by
Eq. (5) can be obtained by computation. Ref. [33], for
Fig. 13. Schematic behavior of predicted dose dependence of
example, shows calculated temperature dependences
swelling. When the ratio of dislocation to cavity sink strength
compared with experimental data. Swelling peaks at
is much greater than unity, the swelling rate is low and the
dose exponent is high; when the ratio is reversed, the swelling intermediate temperatures and is negligible at much
rate is low and the dose exponent is low. After Ref. [l]. lower and higher temperatures. The swelling is low at
low temperatures because the vacancy is practically
immobile. Its concentration in the matrix therefore
and builds up, and more vacancies and interstitials are lost
OGQ,Q,( ZfZ; - Z,dZf ) by mutual recombination. At high temperatures an-
dr,
-= other process diminishes swelling. Cavities emit ther-
dt r,ZdZ,dL(l + Q,)(l + Q,)
mal vacancies rapidly at high temperatures, and this
(sink dominated). (24) counterbalances the net vacancy influx driven by irradi-
ation. At intermediate temperatures swelling is maxi-
In these equations Qi,” denotes the ratio of dislocation
mized - both thermal emission and mutual recombina-
to cavity sink strength, Eq. (23) applies where most
tion are less important, and the excess flow of vacan-
point defects are lost by bulk recombination, and Eq.
cies to cavities is maximized. ‘High’ and ‘low’ tempera-
(24) applies where most are absorbed at sinks ‘. These
tures are dependent on the properties of the material
are the two extremes in modes of point defect loss. As
and in particular on how the overall sink strength
can be seen, in the former case the cavity growth rate
changes with temperature. In some materials, over a
depends parabolically on the dose rate; in the latter
certain temperature range, lowering the temperature
case the cavity growth rate depends linearly on the
increases the sink strength so that recombination is
dose rate. Here, Q is defined as
reduced at the lower temperature.
Z&L The location of the peak swelling temperature de-
Qi,v = pends on dose rate, sink strength, and the predominant
4ar,N,ZF,, ’
mode of defect loss. When dose rate is increased, more
where L is the dislocation density and N, is the cavity point defects are created, but their diffusion velocities
density. remain fixed. To remove defects at the higher rate in
To obtain a swelling-versus-dose prediction, the dose the steady state requires the point defect concentra-
dependence of dislocation density must be known. Eqs. tions to be higher. This results in more recombination.
However, by increasing temperature, the same relative
ratio of recombination rate to absorption rate at sinks
r Of course, most point defects absorbed at sinks recom- may be restored. By requiring this ratio to be invariant,
bine there because of their absorption in nearly equal num- we can obtain a temperature shift for swelling as a
bers. Only a small excess accumulates at each sink dictated by function of dose rate, following along the lines of
the bias. Section 3.3 above.
110 L.K. Mansur/Journal of Nuclear Materials 216 (1994) 97-123
Fig. 14. Cavity growth rate versus cavity radius for the critical
number of gas atoms, n:, and both lower and higher numbers (27)
of contained gas atoms.
Here y is the surface energy and P is the gas pressure
A general equation for the temperature shift of the in the cavity. When Eq. (27) is substituted into Eq. (51,
swelling rate has been derived [30], the resulting cavity growth rate versus radius is as
T2 - Tl shown in Fig. 14. For a given number of contained gas
= [ kTf/(Et’ + nEJ)] [W%/Gd + In ~1 atoms, there are two roots, one at a stable radius, r,S,
1 - [ kT,/(EF + no,‘)] [ln(G,/G,) + ln M] ’ and one at a critical radius r,“. The cavity must achieve
a size beyond r,” to grow by bias-driven growth. The
(26) point on the figure denoted rf is the critical radius
for which Eq. (16) is a special case. The number n is 1 with no gas. Gas makes achieving critical radius easier.
or 2 depending on whether loss is dominated by sinks With more contained gas r,” is reduced. At the same
or by recombination, respectively. The quantity M con- time more gas brings rf closer to r,‘. As more gas is
tains microstructural information about the material in added, r,’ is decreased and r,” is increased up to a
conditions 1 and 2. The appropriate expressions for M critical number of gas atoms, nz, where r,” and r,” meet
are contained in Ref. [30]. at r,*. These quantities are also shown in Fig. 14. If any
more gas is added, a critical radius no longer exists,
3.6. Critical cavity radius
and bias-driven cavity growth is inevitable. There are
The effects of gaseous impurities on swelling are of thus two qualitatively different paths to achieve bias-
particular interest in the theory because they affect the driven growth. The cavity may depart from its stable
0 10 20 30 40 50 60 70 60 90 loo
5.2 X 1O-3 2.9 x lo-2
TIME (sl tw
Fig. 15. Point defect concentrations calculated using the cascade diffusion theory at an arbitrary reference point for a typical
neutron irradiation of nickel at 500°C and 10V6 dpa/s: left, vacancy concentration; right, interstitial concentration. After Ref. [25].
L.K. Mansur/Joumal of Nuclear Materials 216 (1994) 97-123 111
interval). However, for any time interval, even one Herring-Nabarro creep is a mechanism that oper-
much shorter than the average one, there is a finite ates by the transport of thermal vacancies between
probability that n cascades will occur. When the vol- oriented grain boundaries in the absence of irradiation
ume is of radius of the order of the mean point defect [34]. A similar process operates between oriented dislo-
absorption length, S-i/‘, and the time interval is of cations. We may term this process stress-induced pre-
the order of the mean point defect diffusion time, the ferred emission (SIPE). In addition, however, stress
probability of multiple cascade occurrence may be of also changes the capture efficiencies of oriented dislo-
physical interest. Ref. 1251calculates and illustrates the cations for the point defects that are generated during
magnitude of n-fold intervals. Although the fraction of irradiation. The largest effect is on the absorption of
n-fold intervals for times of very short duration is self-interstitials. The greater capture efficiency of dis-
small, it nevertheless may be significant when it is locations whose Burgers vectors are more nearly aligned
realized that typically 102i-10” cascades/s m3 occur with the stress axis can then lead to creep. The varia-
during irradiation. Thus, highly unlikely events may be tion in capture efficiency of a dislocation with orienta-
responsible for part of the microstructural develop- tion can arise because of the inhomogeneity interac-
ment observed in experiments. tion, caused by a change in elastic polarizability of the
As pointed out in Ref. 1251,very often (high proba- point defects [35-371. Recently, it has been suggested
bility) within intervals on the order of the vacancy that the capture efficiency can be changed even more
lifetime, and occasionally (low probability) within inter- strongly by a stress-induced anisotropy in point defect
vals on the order of the interstitial lifetime at elevated diffusion, termed elastodiffusion [38]. It arises because
temperatures, multiple cascades may occur in a volume the material is actually built on a discrete atomic
whose linear dimension is on the order of the point lattice (as opposed to a continuum), which results in a
defect absorption length. The coincidence of multiple change in symmetry of the diffusion field in the pres-
cascades within these physically meaningful volumes ence of an applied stress. Originally, the specific effect
and time intervals ensures intense interaction of de- of the inhomogeneity interaction on creep was termed
fects from different cascades, possibly resulting in dif- stress-induced preferred absorption (SIPA). However,
ferent microstructures than in cases of no coincidence. we now include all the stress-induced interactions that
Although such events are relatively rare, enough of result in a change of dislocation capture efficiencies
them can occur over large volumes and long times to under this acronym.
be important in the macroscopic manifestations of ra- The climb-enabled glide mechanisms of irradiation
diation effects. creep can operate whenever climb occurs. This in-
cludes the processes described above, but also includes
3.8. Irradiation creep by dislocation climb and glide swelling; as cavities grow, dislocations absorb excess
interstitials and climb. Climb-enabled glide caused by
Much of the theoretical work on irradiation creep swelling, and by SIPA, termed preferred absorption
has been in terms of steady-state point defect concen- glide (PAG), have been described in a unified formula-
trations. More recently we have understood that large tion in Ref. [39]. These climb and the climb-enabled
contributions to creep can occur as a result of several glide processes have been most highly developed on a
types of transients in point defect populations. In the theoretical level and in application to experimental
present section the basic elements of irradiation creep data. A number of other mechanisms also have been
mechanisms are described, with emphasis on behavior proposed. For a review of the wide variety of mecha-
in the steady state. In the following section the more nisms that have received attention, see Ref. [14].
recent theoretical work on transient mechanisms is The relationships of irradiation creep to swelling
outlined. were exposed in Ref. [40]. For the specific mechanism
Creep can take place by two distinct processes, of swelling-driven creep, the relationship is direct and
atomic absorption (climb of dislocations) and relative simply expressed. However, even for processes where
motion of crystal planes (glide of dislocations). In the there is no direct cause and effect relationship between
former, atoms are transferred from planes more nearly swelling and creep, there is a lock-step relation, ex-
parallel to those more nearly perpendicular to the pressible in simple mathematical form, for each creep
stress direction. In the latter, planes inclined to the process. Thus, even where one does not cause the
stress direction slip, atom row by atom row, with re- other, definite relationships can be extracted because
spect to one another through the glide of dislocations. both swelling and creep are driven by the same point
The latter process generally also is coupled with atomic defect concentrations.
transport (climb-enabled glide), since gliding disloca- Referring to Fig. 11 we see that the time interval
tions become pinned at obstacles and planar slip stops before 7, can be described as a transient regime, and
unless they are released by atomic absorption or emis- the time after T, can be referred to as the (quasi-l
sion. steady-state regime (A, = Kflr, is shown on the figure.)
LX Mansur/Joumal of Nuclear Materials 216 (1994) 97-123 113
The interval rV can range from milliseconds to unlimit- tions of density Lj, whose Burgers vectors are aligned
edly large times, depending on the material, the sink in the j direction,
strength and especially the temperature. After T, the Ii = a( Z”jD,C, - Z,d’D,C, + Z,“‘D,C, ) L’.
point defect concentrations change only gradually in
response to the relatively slow evolution of microstruc- Here 0 is the atomic volume, Zdpi is the ca:t
ture. Hence, the term quasi-steady-state rather than efficikncy of dislocations in orientation j, the D are
steady-state. As mentioned above, much of the theoret- diffusion coefficients and the C are concentrations,
ical work on irradiation creep has been for this quasi- with the identity of the defect denoted by the corre-
steady-state. This averaged picture is an appropriate sponding subscript. The symbol CT is the thermal
foundation for the point defect concentrations neces- equilibrium concentration of vacancies at a dislocation
sary for the calculation of fluctuation-insensitive defor- of orientation j. For a tensile stress D aligned with the
mation processes. These include processes that depend l-axis,
only on cumulative point defect currents: swelling; Ctl = Ct exp(cTR/kT), (34)
creep by SIPA, and creep by climb-enabled glide driven
cd2 = cd3 = ce
by swelling and/or SIPA. ” ” “7 (35)
By considering the local point defect concentration where Ct is the thermal equilibrium vacancy concen-
fluctuations as revealed by cascade diffusion theory, tration in the bulk. Conservation of atoms requires that
Fig. 15, we discovered a new mechanism of irradiation this current be related to the climb velocity of disloca-
creep that we termed cascade-induced creep 1411.Simi- tions by
larly considering transients in the average picture prior
vi = I’/bL’. (36)
to time T,, Fig. 11, two additional transient irradiation
creep mechanisms are apparent, startup-induced tran- From [39], the magnitude of the average climb velocity
sient interstitial creep [42], and glide-induced transient is
vacancy creep [43]. These will be outlined in Section
3.9. First, however, we sketch the formulation for creep u= ; (( Z;‘D,C, - Z,d’D,C, + Z,“‘D,C,“’ 1
by dislocation climb and climb-enabled glide.
Creep rate by climb-enabled glide may be expressed + 21Zf2DiCi - Z,d2DvC, + Z,“‘D$,“’ I), (37)
as assuming Lj = L/3 for j = 1, 2, 3, where L is the total
dislocation density. Eq. (37) contains contributions from
icr = uf3 (30)
swelling, SIPA and SIPE.
where v is the average dislocation climb velocity and f If there were no SIPA, i.e., Zdl = Zd2 = Zd3 = Zd,
is a function that translates climb to glide. In the then Eq. (37) reduces to
dislocation bowing model [44],
u = ; [ ZfD,C, - Z:Dv( C, - cf)] , (38)
f = (PzyE, (31)
where c: is the sink-weighted average of the C given
where E = u/E is the elastic deflection caused by a in Eqs. (34) and (35). When inserted in Eq. (30), Eq.
stress u in a material with Young’s modulus E. The (38) produces the swelling-driven creep discussed in
process modeled is the climb of a dislocation over an Ref. [40], with SIPE superimposed when ci is non-
obstacle, the subsequent glide, and pinning at another negligible.
obstacle. The released segments again bow out under For no swelling, but SIPA and SIPE processes oper-
the applied stress after repinning, leading to strain. ating, a second specialized form of v in Eq. (37) may
When climb again releases the segments, the strain E be derived. In the steady state,
represented by a bowed dislocation is converted to an
increment of permanent deformation. ( ZflDiCi - Z,d’D,C, + Z,d’D,C,d’)
Another model for f is an obstacle model, where = - 2( Zd2DiCi - Z,d2D,C, + Z,d2D,C,d2). (39)
precipitates, dislocation loops or dislocation segments,
for example, may act as barriers to glide [45]. In this This reduces Eq. (37) to
case
u= ; ; 1Z:‘DiCi - Z,d’Dv( C, - Cv”‘) I.
f =adbL/h, (32)
Similarly, in the absence of irradiation (no swelling and
where a is a numerical constant of order unity, d is the no SIPA), SIPE may occur, and a third specialized
obstacle spacing and h is the obstacle height. The form of Eq. (37) is obtained
symbol b denotes the magnitude of the Burgers vector.
The velocity v is obtained directly from the current
(41)
of excess interstitial volume per unit volume to disloca-
114 LX Mansur/Journal of Nuclear Materials216 (1994) 97-123
nearby dislocations have been examined. The results Fig. 17. Vacancy concentration profiles after a dislocation has
are input into the more global description outlined arrived at an obstacle. The labels (a)-(d) correspond to nor-
above in the form of the Zd” and the AZ. The analysis malized times between 0 and 3000 nm-* respectively, curve
has usually been restricted to the steady state. In terms (e) corresponds to the profile at infinite time. After Ref. [43].
of Fig. 11, the concentrations far to the right are
assumed to apply, i.e., the condition
sion profiles at the new location 2. The time to achieve
Z”D,(C, - cv’) = z,D,C, (43) steady state, T, = K;’ = (D,S,)-’ is essentially the
time it takes a vacancy created at a mean position in
is imposed. Here the .?! and c,” are, respectively, the
the material to reach a sink. Using reasonable sink
sink-weighted average capture efficiency and thermal
strength parameters, T, can range from 3 x lo-’ to
vacancy concentration at sinks.
2 X 10” s for temperatures from 873 to 273 K, respec-
tively. Yet, when a stress, (T, is applied to an unpinned
3.9. Irradiation creep caused by transients dislocation, the glide velocity is given by
butions to climb-enabled glide that result from point stability has been to develop and compare theory with
defect absorption. The additional point defect absorp- experimental results. In general, two types of compar-
tion is calculated under a continuum reaction rate isons can be distinguished. The first is based on the
theory where point defect production is modeled as fact that a great deal of experimental data has been
taking place at its average rate at every point in space obtained to characterize swelling and to a lesser extent
and continuously in time. In an average sense this is irradiation creep, in terms of dependences on parame-
correct. However, as the discussion of Section 3.7 ex- ters such as dose, temperature and material, for exam-
plains, point defect production in cascades leads to ple. Such data is often collected on a purely empirical
local fluctuations in point defect concentrations and level, without any deliberate comparisons with theory
fluxes. The existence of these fluctuations can lead to in mind. After the fact, such data can sometimes be
an additional mechanism of irradiation creep, termed collated and compared with theoretical predictions.
cascade-induced creep [41]. Such comparisons are of some use for ascertaining the
In response to the cascade-induced fluctuations in correctness of predicted broad trends and overall be-
point defect fluxes, a dislocation segment makes climb havior. However, because these experiments were gen-
excursions. During an excursion there is a probability erally not designed with forethought as critical tests of
that the segment will reach an unpinning position on the theory, the comparisons are of a low level of
the obstacle and be freed to glide. The calculation of applicability that is not commensurate with the enor-
this unpinning frequency and the subsequent creep mous amounts of effort represented by the collection
deformation has been carried out [41]. It has been of experimental data. This is natural, since much of the
found that the unpinning frequency can be substantial experimental work was directed to the practical devel-
when compared to that caused by swelling and by opment of nuclear power and not at physical research.
stress-induced preferred absorption. For obstacles of Another type of comparison involves experiments
height 40b (where b is a lattice dimension), for exam- that have been designed with the objective of providing
ple, it was found that cascade-induced creep gave the critical tests of mechanistic understanding. Below, we
largest contribution for the parameter values em- review comparisons of each type. The intent is to give
ployed. However, for increasing obstacle size the rela- the flavor of how theory and experiment have played
tive contribution of cascade induced creep diminishes, mutually supporting roles. The examples shown are
and for obstacles twice this height, swelling driven only a few of the many that are available and no claim
creep becomes the dominant mechanism. is made that this section is exhaustive or representative
in its coverage.
4. Comparisons of theory with experiments 4.1. Temperature shift of swelling with dose rate
One of the continuing long-term themes of the In Sections 3.3 and 3.5, expressions were derived for
more fundamentally oriented research on dimensional temperature shift of total point defect absorption and
net point defect absorption with dose rate. In Ref. [49],
Packan, Farrell and Stiegler compared experimentally
Ki’ observed temperature shifts with the theoretically pre-
I I I I I I I
1 dicted values. Both their own data and data gathered
Ni from the literature were included in the comparison.
Fig. 20, from Ref. [49], shows the observed swelling
and its dose rate-temperature shift in nickel. The line
represents both the Packan et al. experimental results
and the theoretically calculated temperature shift for
those conditions. It can be seen that the theoretical
predictions track the experimental data reasonably well.
group existed below the TEM resolution limit for cavi- of cavities collecting helium, the gas buildup rate in
ties, about 1 nm diameter. each cavity was reduced and the onset of swelling was
Another study, corresponding to approach (2) above, delayed. Calculations accompanying the analysis of Fig.
shows how the achievement of the critical radius/ 23 showed that several thousand appm He can be
critical number of gas atoms can be delayed by tailor-
ing the microstructures [55,56]. The approach was to
slow the accumulation rate of gas atoms in each indi-
vidual cavity in order to delay the onset of swelling.
The alloys were irradiated with dual beams of Ni and
He ions. One alloy was the pure ternary Fe-lSNi-13Cr. 0
z .7
Another had a similar base composition, but was al- IL
p .6
loyed with 0.8 Si, 0.2 Ti, 0.04 C and 0.05 P. z
Swelling was observed early in the pure ternary, at I?
= .5
0.0
accommodated when the cavity density is > lo** rnm3. I 1
AUSTENITIC ALLOYS
I I I I
Such swelling suppression results have been observed l .kMmmlelal. oSpmQueelal.(a) 0LeasndMmsur
r&Q!abynal. 0 wmmw9landal~. c COllacmce _
in a number of experiments where extreme gas disper- 0.5 -
~P&lMMdF~l ASmMelal.
v Mazlru 0 hnlka et al.
sion has been achieved.
p 0.4 - HIGH SWELLING
LOWL - _ HIGHL
4.3. Cavity growth rate
0.10 . Gellee
(a) 0 Halon at-d Mansur
rC”O
4 5
the bubbles at the particles and elsewhere were simi- types - after the fact juxtapositions of theory with
lar. Further irradiation was then carried out with 4 relevant experimental data, and comparisons of theory
MeV Ni ions to a peak dose of 20 dpa. During this with specially designed controlled-variable critical ex-
irradiation, growth of both the dislocation-nucleated periments performed as direct tests of the theory.
and the particle-nucleated cavities occurred. The pre- The kinetic theory of radiation effects spans a vast
cipitate-attached cavities grew at a substantially faster range of phenomena that ultimately translate the ini-
rate than the matrix cavities. The dislocation-nucleated tial interactions of irradiating particles with matrix
cavities increased their radii by factors of 2-3. During atoms to macroscopically measurable property changes.
the same time interval, the precipitate-attached cavi- In its most general form, all transport and reaction
ties grew by factors of 4-8. The initial precipitate to processes of point and extended defects are included
cavity size ratio was in the range 15-30. The experi- in principle. Particular aspects reviewed here include
mental data are represented by the cross-hatched area the framework of clustering and the concept of irradia-
in Fig. 26, superimposed on the calculated curves. tion variable shifts based on point defect absorption
These results confirmed the predictions of the precipi- invariance. Cascade diffusion theory is outlined and
tate point defect collector model. contrasted with standard homogeneous rate theory.
More specific models for swelling including bias, sink
4.5. Startup-induced transient interstitial creep strengths, critical radius and the effects of sink strength
ratios are described. Aspects of creep by climb-enabled
Above, in Section 3.9, we described three mecha- glide of dislocations are covered. Transient point de-
nisms of irradiation creep driven by transients in the fect processes are emphasized, since it has been real-
point defect concentrations. The mechanism of ized more recently that such transients may contribute
startup-induced transient interstitial creep, which oper- more dimensional change than steady-state processes
ates at relatively low temperatures, consistently ex- under some circumstances.
plains observations of high creep rates in recent neu- The theory based on defect reactions has estab-
tron irradiation experiments [42,48]. lished a basic understanding of swelling. Alloys and
Using the time-dependent solutions of Eqs. (6) and special experiments based on theoretical concepts have
(7) together with derived expressions that translate the been successful at demonstrating swelling resistance
associated climb into glide [39], Stoller et al. [48] calcu- and other predictions. Swelling resistant alloys can now
lated the creep by this process. Fig. 19 shows the be designed with confidence for technological applica-
results. Below about 200°C most of the creep is calcu- tions. Irradiation creep is understood to a reasonable
lated to be from transient interstitial absorption with a level, and calculations for creep are in rough agree-
minor part contributed by steady-state processes. At ment with experiments.
temperatures much above 2OO”C,most of the creep is Challenging prospects for future work can perhaps
from steady-state processes. The points on Fig. 19 best be framed as questions. For example, in other
represent the experimental measurements of irradia- papers in this volume, discrete atomic descriptions are
tion creep in the ORR at about 8 dpa and at the used to calculate point defect production. Continuum
temperatures indicated. The theoretical calculations reaction rate theory, as described herein, makes use of
show reasonable agreement with the experiment and the results of such calculations as relatively simple
are consistent with the idea that startup-induced tran- source terms for point defects, for in-cascade recombi-
sient interstitial creep is the main contributor to irradi- nation, and for in-cascade clustering. The level of the
ation creep in neutron-irradiated stainless steels below two descriptions is completely different. What is the
about 200°C. optimum mixture or fusion of the continuum and dis-
crete approaches to achieve the best description of
structure, composition and property changes? Another
5. Summary and conclusions worthy question is how best to take advantage of the
extensive theoretical work on radiation-induced
A tutorial is presented that covers dimensional swelling and creep to advance the mechanistic under-
changes in structural alloys caused by irradiation. standing of other related phenomena that have not
Background, including experimentally observed phe- been treated so thoroughly, such as hardening and
nomena as well as facilities and applications, is first embrittlement. As outlined in this paper, the two most
sketched. Dimensional changes are emphasized since powerful tools for understanding how irradiation leads
historically they have received most attention. This is to property changes are theoretical modeling and the
followed by a more or less self-contained description of thorough-experimental characterization of microstruc-
the kinetic theory of radiation-induced swelling and ture. How can we further improve the combined appli-
creep. Lastly, several comparisons of the theory with cation of these tools to attack new problems in radia-
experiments are described. The comparisons are of two tion effects?
122 L.K Man.w/Joumal of Nuclear Materials 216 (1994) 97-123
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