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Acta Materialia 56 (2008) 1890–1896

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Analytical treatment of diffusion during precipitate growth

in multicomponent systems
Qing Chen a,*, Johan Jeppsson b, John Ågren b
a
Thermo-Calc Software AB, Björnnäsvägen 21, 113 47 Stockhlom, Sweden
b
Department of Materials Science and Engineering, KTH, 100 44 Stockholm, Sweden

Received 17 October 2007; received in revised form 19 December 2007; accepted 19 December 2007
Available online 4 March 2008

Abstract

We propose an approximate growth rate equation that takes into account both cross-diffusion and high supersaturations for modeling
precipitation in multicomponent systems. We then apply it to an Fe-alloy in which interstitial C atoms diffuse much faster than substi-
tutional solutes, and predict a spontaneous transition from slow growth under ortho-equilibrium to fast growth under the non-partition-
ing local equilibrium condition. The transition is caused by the decrease in the Gibbs–Thomson effect as the growing particle becomes
larger. The results agree with DICTRA simulations where full diffusion fields are calculated.
Ó 2008 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.

Keywords: Precipitation; Diffusion; Kinetics; Thermodynamics; NPLE

1. Introduction In general, for multicomponent alloys the operating tie-

Precipitation processes may be modeled in detail by dif-
fuse interface methods such as phase-field [1] or sharp
interface methods like DICTRA [2]. These simulations
are based on numerical calculations of full diffusion fields
and may be quite time consuming. Consequently, only a
small number of particles may reasonably be handled. In
many applications one is less interested in fine details but
more interested in handling complex alloys with more than
10 elements and in the size distributions of several precipi-
tate phases. It is then necessary to take a simpler approach.
Usually one avoids solving the full diffusion problem and
rather applies analytical expressions for the diffusive fluxes
of the solute elements. Such expressions may be obtained
from the steady-state field approximation or similar
approaches [3–6]. These solutions only use the precipitate,
the interface and the matrix average compositions to repre-
sent the diffusion field [3–5]. In some approaches not even
the interface compositions are used [6].
*
Corresponding author. Tel.: +46 8 54595939; fax: +46 8 6733718.
E-mail address: qing@thermocalc.se (Q. Chen).
line at the phase interface has to be found numerically by
seeking a common growth rate for all independent compo-
nents. In previous studies the growth rate was formulated
by either neglecting the cross-terms in the diffusivity matrix
in order to consider high supersaturations [4], or by includ-
ing cross-diffusion terms but restricting the calculations to
small supersaturations [3]. Sometimes, even for small super-
saturations, the cross-diffusion was ignored [5]. In Ref. [4], it
was felt impossible to use the analytic binary growth rate
equation for multicomponent systems, and the consequence
of neglecting the cross-diffusion terms was severe deviation
of the modeled results from experimental observations so
that an ad hoc growth rate had to be found. The approach
in Ref. [3] was not aimed specifically at high supersatura-
tions. However, for a system with significantly different
atomic mobilities, large supersaturations can occur for
slow-moving elements even though the overall supersatura-
tion of the system is very small. In the extreme case of a non-
partitioning local equilibrium (NPLE) growth, the super-
saturations of substitutional elements approach unity. The
approach is then not applicable. Therefore, it seems neces-
sary to find a multicomponent growth rate equation that

1359-6454/$34.00 Ó 2008 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.actamat.2007.12.037
 Q. Chen et al. / Acta Materialia 56 (2008) 1890–1896
can take both cross-diffusion terms and high supersatura-
tions into account at the same time. In this work, we present
such an equation and apply it to a steel to predict a sponta-
neous transition from slow growth to fast growth due to the
Gibbs–Thomson effect.
2. Model
For the sake of simplicity, we treat a spherical particle of
stoichiometric composition or with negligible atomic diffu-
sivity growing under the diffusion-controlled condition. We
start from the exact solution to binary systems and refor-
mulate it by introducing an effective diffusion distance fac-
tor, and then derive a general multicomponent growth rate
equation on the basis of the local equilibrium assumption
and the flux balance equations that depends on individual
effective diffusion distances, which in turn varies with
changing supersaturations of individual components.
Finally, we break up diffusivities into mobilities and ther-
modynamic factors, and present an equation to treat
cross-diffusion directly by working with mobilities and
chemical potential gradients.
2.1. Binary systems
Given an alloy of concentration cM, the concentration in
the matrix at the phase interface cI and that in the precip-
itate cP can be uniquely determined by the phase equilib-
rium tie-line under the isothermal local equilibrium
assumption. With these well-defined interface conditions,
the diffusion-controlled growth of an isolated precipitate
in an infinite matrix can be solved exactly [7,8] and the
growth rate t can be written as
2Dk2
t¼ ; ð1Þ
R
where D is the diffusivity in the matrix, R is the radius and
k is given by
pffiffiffi
2k2  2k3 p expðk2 ÞerfcðkÞ ¼ X; ð2Þ
where X ¼ ðcM  cI Þ=ðcP  cI Þ is the so-called dimension-
less supersaturation. Eqs. (1) and (2) are actually obtained
from the flux balance equation:
tðcP  cI Þ ¼ Drc;
where rc is the concentration gradient close to the phase
interface. Let us introduce an effective diffusion distance
d and rewrite the above equation as
tðcP  cI Þ ¼ DðcM  cI Þ=d:
Comparing this result with Eq. (1), we get:
X
d¼ R ¼ nR;
2k2
where n ¼ X=2k2 is a factor for adjusting the effective diffu-
sion distance from the radius as the supersaturation varies.
Inserting the above expression into Eq. (4), we get:
1891
tðcP  cI Þ ¼ DðcM  cI Þ=nR: ð6Þ
If thepsupersaturation
ffiffiffiffiffiffiffiffiffi is very small, i.e. X ! 0, one obtains
k ¼ X=2 and thus n ¼ 1, which recovers the well-known
steady-state equation used, for example, in coarsening the-
ory [9]:
DðcM  cI Þ
t¼ : ð7Þ
RðcP  cI Þ
If the supersaturation is very large, i.e. X ! 1, one obtains
pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
k ¼ 3=2ð1  XÞ and thus n ¼ Xð1  XÞ=3 ! 0, i.e. the
effective diffusion distance becomes very small and the
growth rate very large.
2.2. Multicomponent systems
In an n-component alloy of concentration cM i , generally
speaking, the interface concentrations cIi and cPi in the
matrix and precipitate phases are determined simulta-
neously [10] with the interface velocity from the flux bal-
ance equation for each element:
  Xn1
t cPi  cIi ¼ Dij rcj ð8Þ
j¼1
where Dij is the chemical diffusivity in the matrix phase and
rcj is the concentration gradient of element j at the inter-
face. Both i and j go from 1 to n  1 because there are n  1
independent concentration variables in an n-component
system. So far we have only n  1 equations for 2n  1
unknowns. Invoking the local equilibrium assumption,
we obtain n more necessary equations:
lPi ¼ lIi ; ð9Þ
where lPi and lIi are chemical potentials of element i in the
precipitate and matrix at the interface, respectively, and are
functions of cPi and cIi . Now we have to define rcj in order
to solve 2n  1 (Eqs. (8) and (9)). Supposing that the effec-
tive diffusion distance dj or the factor nj for each element j
depends only on its own supersaturation Xj , we can obtain
a general multicomponent growth rate equation directly
from Eq. (6):
  Xn1  .
t cPi  cIi ¼ Dij cM I
j  cj nj R: ð10Þ
ð3Þ j¼1
During the coarsening stage of a precipitate, Xj ! 0 and
thus nj ! 1, and we obtain the same multicomponent
coarsening rate equation as that of Morral and Purdy [11].
ð4Þ
2.3. Direct treatment of cross-diffusion with mobilites and
chemical potentials
ð5Þ The off-diagonal terms in the diffusivity matrix are
mostly related to thermodynamic effects but also depend
on the choice of frame of reference. The first effect comes
from expressing fluxes as functions of concentration gradi-
ents. The driving force for diffusion is essentially a gradient
1892 Q. Chen et al. / Acta Materialia 56 (2008) 1890–1896

in chemical potential and it can therefore be more suitable

to work directly with mobilities rather than with chemical
diffusivities. The diffusivity matrix can be divided into a
mobility M and a thermodynamic factor ol/oc, and the
large off-diagonal elements in the matrix come from the
thermodynamic factor:
X
n1
olj
Dik ¼ cj M ij : ð11Þ
j¼1
ock

The diffusional flux of element i can then be expressed as

X
n1 X
n1 X
n1
olj
Ji ¼  Dik rck ¼  cj M ij rck
k¼1 j¼1 k¼1
ock
X
n1
¼ cj M ij rlj :
j¼1
The off-diagonal terms in the last part of Eq. (12) are only
related to the frame of reference; they are zero in the lattice
fixed frame of reference and non-zero in any other frame of
reference due to the Kirkendall effect. The effect is, how-
ever, small compared to the approximations introduced
earlier with the modified steady-state equation. Neglecting
these cross-terms, Eq. (10) can be expressed with mobilities
and chemical potential gradients as
 
t cPi  cIi ¼ cIi M i ðlM I
i  li Þ=ni R: ð13Þ
In the above equation, the cross-diffusion is accounted for
directly by the dependence of chemical potentials on
concentrations.
3. Results and discussion
We now apply our model to calculate the growth rate of
a M23C6 particle metastably formed from a supersaturated
ferrite alloy A (Fe–2 wt.% Cr–0.2 wt.% C) at 1053 K. All
necessary thermodynamic and kinetic data, i.e. the temper-
ature- and composition-dependent Gibbs free energy and
atomic mobility, were taken from the well-assessed dat-
abases TCFE4 [12] and MOB2 [13]. When mobility varies
with composition, an average value was used. The
Gibbs–Thomson effect was taken into account during the
calculation of chemical potentials by adding a pressure dif-
ference term, 2rV m =R, to the Gibbs energy of the M23C6
phase. The interfacial energy r and the molar volume
V m , based on substitutional elements, were assumed con-
stant and equal to 0.4 J m2 and 6  106 m3 mol1,
respectively. For each given particle radius R, the growth
rate t was obtained together with the interface concentra-
tions cPi and cIi (i = C, Cr) by numerically solving five non-
linear equations that consist of Eqs. (9) and (13).
The calculated results are shown as curve A in Fig. 1. It
is interesting to see that the growth rate increases dramat-
ically from zero as the particle size increases from the crit-
ical radius, 0.78 nm, and then reaches almost a plateau,
and then shoots up again and reaches a maximum, and
finally decreases gradually. This is obviously different from
ð12Þ
Fig. 1. The calculated growth rates of metastable M23C6 particles of
different sizes in supersaturated ferrite alloys A (Fe–2 wt.% Cr–0.2 wt.%
C) and B (Fe–2 wt.% Cr–0.05 wt.% C).
a normal t vs. R curve, such as curve B, where the growth
rate of a M23C6 particle from another supersaturated fer-
rite alloy B (Fe–2 wt.% Cr–0.05 wt.% C) at the same tem-
perature is shown to increase sharply to its maximum at
around twice the critical nucleus size and then decreases
slowly.
We now examine the other results obtained at the same
time during the simulation, i.e. the dependence of interface
concentrations on the particle size for alloys A and B. The
results are depicted in Figs. 2 and 3, where u-fractions or
atomic fractions per mole of substitutional elements are
used. The C and Cr contents in the body-centered cubic
(bcc) matrix phase far away from the interface are shown
as dotted lines, which coincide with the left end points of
those curves for the bcc phase, i.e. concentrations at the
interface in the bcc phase for a particle of the critical
nucleus size. As can clearly be seen, for alloy A at a particle
size of about 2.1 nm, abrupt changes occur for the Cr con-
tent in both bcc and M23C6 phases and for the C content in
bcc. For particles larger than 2.1 nm in radius, their Cr
content at the interface is almost the same as that in the
matrix. In contrast, no sudden changes exist for the varia-
tions of interface concentrations in alloy B, and the redis-
tributions of solutes in the matrix and precipitate phases
are continuous and very smooth.
Returning to Fig. 1, we see from curve A that the
growth rates for small particles around 1–2 nm are several
orders of magnitude slower than those for particles larger
than 2.1 nm. So the curve can be easily divided into two
parts, one corresponding to a slow growth mode and the
other to a fast growth mode. In fact, from Figs. 2 and 3,
we know immediately that the slow growth mode involves
redistribution of Cr in the matrix and precipitation under
local ortho-equilibrium, and the fast growth mode involves
no such redistribution as the Cr content in the particles is
the same as that in the matrix, which corresponds to a
 Q. Chen et al. / Acta Materialia 56 (2008) 1890–1896
Fig. 2. The calculated interface compositions for the metastable growth of
M23C6 particles in supersaturated ferrite alloy A (Fe–2 wt.% Cr–0.2 wt.%
C). The dotted line represents the matrix composition.
phase transformation under the so-called NPLE condition.
For alloy B, the growth of the particle is governed by the
slow mode and is not influenced by particle size.
To find out why the behavior for alloys A and B are so
different and why the growth mode can change spontane-
ously as the particle grows larger, we need to examine the
metastable phase equilibrium between the bcc and M23C6
phases and the influence of the Gibbs–Thomson effect on
it. The isothermal section of the Fe–Cr–C system at
1053 K is calculated by using Thermo-Calc software [14]
and the thermodynamic database TCFE4 [12]. The result-
ing Fe-rich corner is shown in Fig. 4. To calculate the meta-
stable bcc and M23C6 phase equilibrium, all other phases in
the database are suspended during the calculation. The
black solid line is the solvus of the bcc phase, and the green
solid lines are the tie-lines of the two phases being consid-
ered here. For particles with a finite radius, the phase equi-
librium can be calculated by adding a curvature-induced
pressure difference term, 2rV m =R, to the Gibbs energy of
1893
Fig. 3. The calculated interface compositions for the metastable growth of
M23C6 particles in supersaturated ferrite alloy B (Fe–2 wt.% Cr–0.05 wt.%
C). The dotted line represents the matrix composition.
the M23C6 phase, i.e. the contribution due to the so-called
Gibbs–Thomson effect. Therefore, for a series of given par-
ticle radius, we may draw a series of corresponding bcc sol-
vus lines and the related tie-lines. For clarity, only the lines
for the particle size of 2.1 nm, where the growth mode
changes in alloy A, are plotted and they have the same col-
ors, but are dashed. The two circle symbols mark the con-
centrations of alloys A and B. If we calculate the bcc solvus
lines for the M23C6 particles of critical sizes in alloys A and
B, they should certainly pass through points A and B,
respectively.
By ignoring the M23C6 phase, the iso-carbon-activity
lines for the two alloys can also be calculated, and these
are shown by the red lines passing through points A and
B. The former intersects at C with the solvus line of only
the 2.1 nm particles, and the latter crosses both solvus lines,
especially at E for that corresponding to an infinitely large
particle. It should be mentioned that two special tie-lines
for M23C6 containing the same amount of Cr as in the
1894 Q. Chen et al. / Acta Materialia 56 (2008) 1890–1896

value, which was calculated to be 2.8 nm, because there

exists no cross-point for the bcc solvus and iso-carbon-
activity lines above this critical value. For particles that
are smaller than 2.8 nm but larger than 2.1 nm, the bcc sol-
vus and iso-carbon-activity line do intersect with each
other, but this does not mean that the slow growth mode
is possible. In fact, the intersection points for particles in
this range of size would yield tie-lines suggesting that the
Cr content in M23C6 at the interface is lower than that in
the matrix. This is simply not viable for the growth of
M23C6 particles from the bcc matrix where the distribution
coefficient of Cr is greater than 1.

3.1. Comparison with DICTRA simulation results

The derived model is intended for multiparticle, multi-

Fig. 4. The calculated isothermal Fe–Cr–C phase diagram at 1053 K. The
phase simulations in complex alloys and is therefore a sim-
solid black line is the solvus of the bcc phase, and the solid green lines are plified approach to the diffusion problem. The model has
the conjugate tie-lines of the bcc and M23C6 phases. The dashed black and been compared to solutions of the full diffusion problem
green lines are similar ones corresponding to a particle size of 2.1 nm. The to show that the introduced approximations are not severe.
red lines are iso-carbon-activity lines for ferrite alloys A and B, The software DICTRA [2] was used to simulate the growth
respectively. The heavy blue lines are the loci of the compositions of the
bcc phase at the interface with M23C6 particles of different sizes.
of one spherical M23C6 particle in alloys A and B. All ther-
modynamic and kinetic data were taken from the databases
TCFE4 [12] and MOB2 [13], and the Gibbs–Thomson
matrix have also been calculated for infinitely large and effect was accounted for in the usual way.
2.1 nm particles. They are those lines starting from the It should be mentioned that the simulations in DICTRA
bcc side at D and C, respectively. The loci of the composi- were numerically tricky to perform due to large differences in
tions of the bcc phase at the interface shown in Figs. 2 the magnitude of both particle size and growth rate. For
and 3 are also superimposed in the diagram as heavy blue example, in the case of alloy A, concentration gradients in
lines. As we can see, for alloy B, the locus starts from B the range of fractions of nanometers have to be resolved
and follow the iso-carbon-activity line and end at E; for in the matrix close to the particle, and the matrix has to be
alloy A, the locus starts from A and follow the iso-car- of the order of micrometers to avoid impingement. The growth
bon-activity line to C, and then change its course abruptly rate also changes abruptly by five orders of magnitude.
and move almost horizontally to D. As expected, the locus
corresponding to the slow mode coincides with the iso-car-
bon-activity lines and this means that the chemical potential
gradient of carbon near the interface in the bcc phase is
almost negligible. However, despite the negligible gradient,
a small finite interface velocity, which matches that of the
very slow-moving Cr atoms, can be obtained for carbon
due to its extremely large atomic mobility. Hence, the
growth of the particles is controlled by the diffusion of Cr
in this mode.
In the case of alloy A, when the particle size is larger
than 2.1 nm, the fast growth mode is adopted because it
is now possible for the precipitates to inherit the Cr content
in the matrix, which means undergoing a NPLE during
growth that is fully controlled by the diffusion of carbon.
In this mode, the supersaturation of Cr is almost 1, so its
effective diffusion distance factor is approaching 0, and
the gradient of chemical potential of Cr becomes tremen-
dously large, which makes it possible for the slow-moving Fig. 5. The calculated growth rates of metastable M23C6 particles of
Cr to acquire a very high interface velocity, the same as different sizes in supersaturated ferrite alloys A (Fe–2 wt.% Cr–0.2 wt.%
C) and B (Fe–2 wt.% Cr–0.05 wt.% C). The solid black lines indicate
that for C, whose chemical potential gradient is now finite
results from direct treatment of cross-diffusion. The dashed lines indicate
and whose mobility is always very large. results from indirect treatment of cross-diffusion. The dotted lines indicate
It is understandable that the NPLE growth mechanism results from indirect treatment without use of cross-diffusivities. The
is the only feasible one for particles larger than a critical square and diamond symbols indicate results from DICTRA simulations.
 Q. Chen et al. / Acta Materialia 56 (2008) 1890–1896
Fig. 6. Same as Fig. 4 except that the dashed blue lines are the results
from indirect treatment of cross-diffusion, and the dotted blue lines are the
results from indirect treatment without use of cross-diffusivities, and the
square and diamond symbols are the results from DICTRA simulations.
The results from the DICTRA simulations are indicated
by square and diamond symbols in Figs. 5 and 6, together
with the results from our simplified approach indicated by
solid lines. For both the growth rate and composition as a
function of particle size, the agreement is very good. The
simplified model can even in the extreme case of alloy A
fully describe the switch of the growth mode from ortho-
equilibrium to NPLE.
3.2. Method with diffusion coefficients
In Section 2.2, we derived a method of treating multi-
component particle growth including cross-diffusion with
diffusion coefficients. The method is indirect in the sense
that the cross-diffusion can be accounted for directly by
using mobilities and chemical potentials as shown in Sec-
tion 2.3.
The results from the simulations for alloys A and B
using this indirect method, i.e. solving Eqs. (9) and (10),
are also shown in Figs. 5 and 6. For comparison, the results
from the calculations using diffusivities without cross-terms
have also been added.
Starting with alloy B, it is easy to see that the cross-
terms are important. Neglecting cross-diffusivities results
in large deviations from the direct method and the DIC-
TRA simulation results. The growth rates are overesti-
mated because the obtained operating compositions at
the interface are wrong. Ignoring the cross-terms in Eq.
(10), we see that in order to achieve a slow growth mode,
the matrix carbon composition at the interface has to be
about the same as that far away from the interface. Note
that it is composition and not chemical potential or activity
that is used. This is why, without cross-terms, the operating
interface compositions follow almost the iso-carbon-com-
position line in Fig. 6. The correct interface compositions
should follow the iso-carbon-activity line as indicated by
1895
the direct method or DICTRA. The indirect method of
treating cross-terms gives a similar result as the direct
method and agrees more or less with the DICTRA simula-
tion, which indicates that the chemical potential gradients
are described well with cross-diffusivities and composition
gradients for alloy B in our individual effective diffusion
distance approach.
In the case of alloy A, the results are different. By
neglecting the cross-diffusivities, the transition from
ortho-equilibrium to NPLE is captured but the growth
rates are overestimated and the transition is not at the cor-
rect particle size. This is due to the same reason as
discussed in the preceding paragraph, i.e. the wrong inter-
face compositions that follow the iso-carbon-composition
line and deviate from the iso-carbon-activity line. An even
worse, and maybe surprising, result is that the indirect
method of treating cross-terms cannot capture the transi-
tion to NPLE, and the growth rate is orders of magnitude
too low when the particle size is over 2.1 nm. In Fig. 6, we
can see that the interface compositions never reach NPLE
and the growth therefore never gets fully controlled by car-
bon diffusion. The indirect method of treating cross-diffu-
sion estimates incorrectly the cross-term effect in this
extreme case where the diffusion distance of one compo-
nent is very short and therefore the cross-terms become
very important. The direct method of treating cross-diffu-
sion estimates correctly the cross-term effect because it is
accounted for directly by the dependence of chemical
potential on concentrations.
4. Summary and conclusions
We have proposed an approximate growth rate equation
that takes into account both cross-diffusion and high super-
saturations for modeling precipitation in multicomponent
systems. Although the derivation is confined to spherical
particles, it can be readily extended to other simple geom-
etries. With this equation, different possible growth modes
can be captured automatically without any ad hoc treat-
ment. We have applied the equation to a Fe-alloy where
interstitial C atoms diffuse much faster than substitutional
solutes and found a spontaneous transition from slow
growth under ortho-equilibrium to fast growth under the
NPLE condition. From analysis of phase equilibrium and
thermodynamics subjected to pressures induced by the cur-
vature of particles of finite sizes, we understand that the
transition is caused by the decrease in the Gibbs–Thomson
effect as the growing particle becomes larger. DICTRA
simulations have also been carried out and the obtained
results corroborate that of our simplified approach. It has
also been found that the method using mobilities instead
of diffusivities within our individual effective diffusion dis-
tance approach is probably always superior due to the fact
that chemical potential gradients instead of composition
gradients are then used and the cross-term effect can there-
fore be accounted for directly by the composition depen-
dence of chemical potentials.
1896 Q. Chen et al. / Acta Materialia 56 (2008) 1890–1896
Acknowledgments
One of the authors (J.J.) gratefully acknowledges sup-
port from the Swedish foundation for strategic research
(SSF) through the MATOP program.
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