Acta Materialia 51 (2003) 2971–2987

www.actamat-journals.com

A model of solidification microstructures in nickel-based

superalloys: predicting primary dendrite spacing selection
W. Wang, P.D. Lee ∗, M. McLean
Department of Materials, Imperial College, Prince Consort Road, London SW7 2BP, UK

Received 3 December 2002; accepted 11 February 2003

Abstract

A combined cellular automaton-finite difference (CA-FD) model has been developed to simulate solute diffusion
controlled solidification of binary alloys. Constitutional and curvature undercooling were both solved to determine the
growth velocity of the solid/liquid interface. A modified decentered square/octahedron (in two or three dimensions)
growth technique was implemented in the cellular automaton to account for the effect of crystallographic anisotropy.
The resulting model is capable of simulating the growth of equiaxed and columnar dendritic grains in 2D and 3D,
with the ⬍100⬎ directions either aligned or inclined with the grid. The algorithm used can also be used on coarser
grids, with a concomitant loss in resolution, allowing simulation of sufficiently large numbers of dendrites in 3D to
investigate the distribution of spacings, as well as average behavior.
Simulations were performed for directional solidification with a range of withdrawal velocities and nucleation con-
ditions, but a constant thermal gradient. The simulations capture the full microstructural development and primary
spacing selection by both branching and overgrowth mechanisms. The model illustrates that there is a range of possible
stable spacings, and that the final spacing is history dependent. It was also found that a minimum deviation from the
steady state dendrite spacing is required before the spacing adjustment mechanisms are activated. The influence of
perturbing the withdrawal velocity upon the stability of the spacing was also investigated. It was found that perturbations
significantly reduce the range of stable primary dendrite spacing.
 2003 Acta Materialia Inc. Published by Elsevier Science Ltd. All rights reserved.

Keywords: Cellular automaton; Solute diffusion; Directional solidification; Primary dendrite spacing

1. Introduction umnar dendrites where microsegregation of

Many multi-component industrial alloys are sol-
idified in conditions (i.e. low velocity or high ther-
mal gradient) that produce a complex array of col-
∗
Corresponding author. Tel.: +44-20-7594-6801; fax: +44-
20-7594-6758.
E-mail address: p.d.lee@imperial.ac.uk (P.D. Lee).
alloying elements occurs. This segregation pattern
is characterized by primary dendrites parallel to,
and secondary dendrites perpendicular to, the
⬍100⬎ directions closest to the macroscopic sol-
idification direction; these features can have sig-
nificant effects on the mechanical properties of sol-
idified products [1,2]. In case of the nickel-based
superalloys used for gas turbine blades and discs,
these features are of particular importance as their

1359-6454/03/$30.00  2003 Acta Materialia Inc. Published by Elsevier Science Ltd. All rights reserved.
doi:10.1016/S1359-6454(03)00110-1
2972 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
influence can persist through the subsequent
thermo-mechanical and/or heat treatment processes
[3]. In order to improve the properties of the cast
alloys, as well as controlling the formation of sol-
idification defects, a fundamental knowledge of the
growth of the initial dendritic microstructure dur-
ing solidification is required. Over the past thirty
years or so, considerable progress has been made
in understanding dendritic growth from both
experimental and theoretical studies.
Several experimental studies have used trans-
parent organic analogues to directly observe the
development of dendrites under well-defined ther-
mal conditions and have identified the mechanism
for adjusting the dendrite spacing to a change in
solidification condition [4–6]. These experimental
results show no unique primary cellular/dendritic
spacing, but rather a range of spacing, for a given
processing condition. The development of the pri-
mary spacing is apparently dependent not only on
the current processing parameters, but also on the
sequence of previous solidification conditions to
which the system has been subjected. Recently, the
effect of changing the solidification velocity during
directional solidification has been investigated; the
dendritic structure that develops depends on the
effectiveness of different selection mechanisms
including dendrite branching and competitive
growth [7,8].
Many theoretical approaches have been used to
calculate the morphology and size of dendrites.
Initially, analytical models of the primary dendrite
tip were proposed that assumed the dendrite to be
ideally spaced, i.e. only an averaged interaction
was assumed between the neighboring dendrites
[9,10]. For the primary dendrite spacing, l1, most
of the theoretical treatments give the following
functional form:
l1 ⫽ A·G⫺0.5V⫺0.25⌬T0.25
0 (1)
where G is the temperature gradient, V the growth
velocity, ⌬T0 the freezing range of the alloy and
A is a function of the alloy. It should be noted that
during the growth of a dendritic array, solute is
rejected by each dendrite so that the solute-fields
of neighboring dendrites interact. This feature
determines the small range of dendrite spacings
that are stable with respect to branching and over-
growth mechanisms. Based on this concept,
numerical models have been proposed for the ste-
ady and transient growth of a cellular/dendritic
array in binary alloys that predict dendrite spacing
and tip undercooling [11,12].
Recently, a numerical technique, the phase field
method, was proposed. Phase field simulations
accurately reproduce the morphology of
developing dendrites in simple thermal conditions,
capturing most of the phenomena associated with
dendrite formation (e.g. dendrite tip kinetics, pre-
ferred growth direction, coarsening, coalescence,
etc.) [13–15]. Initially developed for thermal dif-
fusion controlled growth of dendrites in two
dimensions, it has been extended to solute-dif-
fusion controlled dendrite growth [13] and to three
dimensions [16].
Another numerical technique used to simulate
solidification is the cellular automaton (CA) stoch-
astic based method where rules are applied that in
the limit are solutions of the governing differential
equations [17,18]. Although these techniques do
not capture the same level of detail, nor have they
previously incorporated all of the growth phenom-
ena, they are able to simulate grain structures on
much larger simulation domains than is possible
using the phase field method. CA models trace the
position of a sharp solid/liquid interface, while the
phase field method expresses it as a transition layer
with a finite thickness that separates the liquid and
solid phases. However, molecular dynamic studies
show that this thickness should only extend over a
few atomic dimensions [19]. To capture the inter-
face, the phase field method requires a very fine
grid, leading to very high computational cost.
Compared to the phase field method, the CA mod-
els can run on a much coarser grid and, therefore,
are more computationally efficient when solved
over the same domain.
In CA models, kinetic undercooling is often neg-
lected, and the velocity of the interface is determ-
ined by other methods. The most commonly
applied method of determining the interface velo-
city is the application of the Kurz–Giovanola–Tre-
vedi (KGT) model [20], which is based on the
assumption that the dendrite tip has an ideal para-
bolic shape and is advancing with a steady state
velocity. The resulting relationship between the
 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
growth velocity and the total undercooling of the
tip has been widely used by other researchers in
simulations of grain growth. Since kinetic
undercooling is neglected, the only contributions
to the total undercooling at the tip arise from the
effect of solute pileup in front of the interface and
from surface tension. This model is a reasonable
approximation for the average behavior of a pri-
mary tip, but cannot be used to simulate the inter-
action of dendrite tips that are not ideally spaced.
Neither is it valid for simulating the development
of the secondary and tertiary arms where the solute
fields interact in a complex manner.
Crystallographic anisotropy is another important
factor that affects the solidification process. For
cubic metals, ⬍100⬎ are the preferential growth
directions, and the growth velocity along these
directions is faster than other directions. Therefore,
in the directional solidification process, grains with
one of the ⬍100⬎ directions closely aligned with
the temperature gradient will overgrow those with
larger deviations from ⬍100⬎. In order to account
for the effect of crystallographic anisotropy in CA,
a neighborhood selection procedure within a
square grid was developed [21,22]. However, this
technique only allows limited deviations in the
growth direction that depend on the complexity of
the network; different types of neighborhood inter-
actions will result in the prediction of different
occupancy of cells.
Another approach to accounting for crystallo-
graphic anisotropy is the decentered square growth
technique developed by Gandin and Rappaz [23].
They assumed, in 2D simulations, that grains of
cubic metals always grow in a square shape with
the diagonal aligned with the preferential ⬍10⬎
direction. The rate of growth of the tip (corner of
the square) was then calculated using the KGT
approximation. These growing squares were super-
imposed upon a regular CA grid, but with the pre-
ferred growth direction of the grain represented by
the misorientation of the square’s diagonal from
the grid direction. A growing square captures the
neighboring cells when it touches their centers. At
this stage, a new square, decentered from the old
one, is then associated with the newly captured
cell. The decentered square method was then
extended for three-dimensional simulations using
2973
an approach described as the decentered octa-
hedron technique [23].
These CA models are capable of simulating
many solidification processes on a macroscopic
scale. However, if the solute diffusion equations
are not solved, the dendritic structure remains
unknown. In order to simulate the dendrite mor-
phology and the extent of micro-segregation, the
CA method can be coupled to a finite element or
the finite difference model to solve for solute dif-
fusion, termed a modified cellular automaton
(MCA) model [24]. One of the greatest challenges
of these MCA models is the method of determining
the growth velocity of solid/liquid interface at all
points on the dendrite, not just at the tip.
In this paper, a CA model is introduced in which
constitutional undercooling and curvature
undercooling are related to the growth velocity of
the solid/liquid interface. The solute distribution in
the liquid causing constitutional undercooling is
calculated using a finite difference (FD) solution
of solute diffusion. The crystallographic aspect of
growth is considered by adapted implementation of
the decentered square/octahedron growth algorithm
developed by Gandin and Rappaz [23]. The
resulting model has several novel aspects: the treat-
ment of the tip velocity using an iterative scheme;
grid independence; and scaling using a blurring of
the solid–liquid interface. These novel aspects
allow the model to be applied to predict the den-
drite spacing selection mechanisms and the effect
of perturbation of solidification velocity on the
dendritic microstructure including growth history
dependence, using as an example a binary approxi-
mation of a nickel-based superalloy.
2. Model theory
The present model combines a continuous func-
tion cellular automaton description of grain growth
with a finite difference computation of solute dif-
fusion. Both the CA and FD components of the
model run on the same regular spatial square grid
and with the same time step. Each spatial cell can
have three states: liquid, solid and growing (i.e. a
mixture of solid and liquid). The model builds
upon prior work by some of the authors [25–27],
2974 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987

and novel extensions to track the tip location due 1 0

to solute and curvature terms in a grid-independent C∗L ⫽ C0 ⫹ [T ⫺⌫k⫺T], (8)
ml liq
manner within a CA framework are described
below. where C0 is the initial concentration, T0liq the liqui-
dus temperature at C0, ␬ the average curvature of
2.1. Solute diffusion analysis the solid/liquid interface, and T the local tempera-
ture. ␬ is calculated by an approximate method
Assuming the equilibrium partition coefficient, described by Nastac [28]:
k, is a constant, the partitioning of solute in the
growing cell is determined by: ␬⫽
1
⌬x 再
1⫺
2
f ⫹
N⫹1 S 冋 冘 册冎
N

j⫽1
fSj , (9)
CS ⫽ kCL, (2)
where N is the number of neighboring cells.
where CS and CL are the average solute concen- The solute concentration gradient, GC, which is
trations of the solid and liquid, respectively, in a calculated using values from a previous time step,
specific cell. An equivalent concentration, CE, is is then substituted into Eq. (7) to calculate the con-
defined as: centration in the growing cells at the current time
CE ⫽ CL(1⫺fS) ⫹ CSfS ⫽ CL[1⫺(1⫺k)fS], (3) step. Eq. (6) is solved using an explicit FD scheme,
allowing the change in the solid fraction in the
where fS is the solid fraction. The diffusion equa- growing cells and the concentration in other cells
tions in the liquid and solid can now be expressed to be calculated. Although nucleation models are
in a general form: included in the code, this paper only presents
∂CE results for growth of seeded grains. Each seed has
⫽ ⵜ·(DEⵜCL), (4) a crystallographic orientation, q, associated with it.
∂t
where DE is an equivalent diffusion coefficient, 2.2. Grain growth in 2D
expressed as:
DE ⫽ (1⫺fS)DL ⫹ fSkDS. (5) The 2D decentered square algorithm developed
by Gandin and Rappaz [23] is not directly appli-
DL and DS are diffusion coefficients in liquid and cable for simulating grain growth from the liquid
solid, respectively. The equivalent diffusion Eq. (4) when solute diffusion is considered. In order to
can be rewritten as: solve the diffusion equation, the solid fraction
∂fs within cells must be allowed to change continu-
CL(1⫺k) ⫽ ⫺ⵜ·(DEⵜCL) ⫹ [1⫺(1 (6) ously and smoothly from 0 to 1 if numerical insta-
∂t
bilities are to be avoided. The KGT model is no
∂CL longer appropriate since the model has already
⫺k)fS] .
∂t taken into account the effect of solute diffusion. A
novel modified 2D decentered square growth
The solute concentration, CL, in the liquid within algorithm, that has been developed to overcome
a growing cell, is given by: these problems, is presented below. A schematic
1⫺fS illustration of the modified 2D decentered square
CL ⫽ C∗L ⫺ ⌬xGC, (7) growth algorithm is shown in Fig. 1. Only nine
2
cells of a whole CA network are displayed for clar-
where C∗L is the concentration in the liquid at the ity. A grain with misorientation angle, q, has
solid/liquid interface, ⌬x the cell size, and GC the nucleated at the central cell and is growing into a
concentration gradient in front of the solid/liquid square shape. The increment of the half width of
interface. C∗L can be determined from a linearised the square is related to the increment of fraction
equilibrium phase relation: solid by:
 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
Fig. 1. Schematic diagram of modified 2D decentered square CA growth algorithm: (a) a grain nucleated in the central cell is
growing within a square envelope; (b) the grain has captured the four neighboring cells and four new squares are associated with
them (only parts of these squares are shown for clarity); (c) the grain captures more cells.
⌬L ⫽ ⌬x·⌬fS.
When the misorientated square envelope asso-
ciated with the solid in the central cell touches its
four neighboring cells, their state indices change
to that of the original. In each of these ‘touched’
neighboring cells, a new square is created with the
same orientation as the solid cell that grew into it.
One corner of each of the new squares overlaps
the original square, hence the term “decentered
square” method. The growth velocities of these
new squares can be different from the original
square depending on the solute diffusion or local
temperature. Parts of the growing new squares are
shown in Fig. 1(b). The misoriented solid squares
progressively encroach on more reference cells, as
illustrated in Fig. 1(c).
2.3. Grain growth in 3D
The 2D modified decentered square growth tech-
nique was also extended into three dimensions,
termed the 3D modified decentered octahedron
growth technique. The underlying approach is the
same. A misoriented grain is considered to
nucleate and grow within a regular array of cubic
cells having an octahedral shape. When the solid
grows along one of the crystallographic cube direc-
tions to touch any of the six neighboring cubic
cells, growth continues from that point along
⬍100⬎ directions into the captured cells by gener-
ating a new octahedron. Shifting the original octa-
2975
(10) hedron along the diagonal towards the corner point
that touches the neighboring cell generates the new
octahedron that can keep growing along the same
⬍100⬎ directions as the nuclei.
Thus, constitutional and curvature undercooling,
together with crystallographic orientation, are all
incorporated in the model through the application
of this modified decentered square/octahedron
technique within a CA-FD framework.
2.4. Solution techniques
Simulations were performed on a regular square
grid in 2D and a regular cubic grid in 3D with a
cell edge length of 5 µm. A range of solidification
rates with a constant thermal gradient (varying in
the vertical direction) were used in the simulations.
In the 2D simulations, periodic boundary con-
ditions were applied to the left and right sides of
the domain, while a zero flux boundary condition
was applied to the top and bottom of the domain.
In the 3D simulations, a periodic boundary con-
dition was applied to the left and right, front and
back surfaces of the domain, respectively, while a
zero flux boundary condition was applied at the top
and bottom.
A moving frame of reference technique was
applied in the simulations of directional solidifi-
cation. When the temperature at the bottom
decreased to a predetermined value, the bottom
layer of cells was removed, all the other layers are
2976 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
shifted down by one cell and a new layer with the
initial concentration added to the top of the simul-
ation domain. This technique allows the dendrites
to grow to a sufficient length to ensure a stable
state is reached, without increasing the domain size
and hence reducing the computational resources
required.
3. Two dimensional simulations
Numerical simulations of directional solidifi-
cation of a binary approximation of a nickel-based
alloy were performed to investigate the influence
of a number of material parameters and process
variables on the development of the dendritic struc-
ture. The material properties and model parameters
used in the simulations are given in Table 1. The
simulations were carried out in both two and three
dimensions, with the results presented and dis-
cussed in this and the next section, respectively.
In this section, 2D simulations, the effects on the
dendritic structure of the initial nucleation density,
rate of solidification and of perturbation of the sol-
idification rate are considered in turn.
3.1. The effect of nucleation density
In the following simulations the same imposed
solidification conditions were used: i) a thermal
gradient of 12 K/mm, and ii) a growth velocity of
150 µm/s (giving a cooling rate of ⫺1.8 K/s). It
Table 1
Material properties and model parameters used in the simulations
Property
Liquidus temperature
Liquidus slope
Partition coefficient
Diffusion coefficient in liquid
Diffusion coefficient in solid
Gibbs Thomson Coefficient
Initial concentration
Cell size
Time step
was assumed that no nucleation occurs in the bulk
liquid; only the growth of the seeds placed at the
base of the directionally solidified ingot is con-
sidered. Therefore, the final microstructure
develops only by branching and overgrowth mech-
anisms from these initial seeds. The undercooling
for the nucleation of the seeds was taken to be 4
K throughout this work. Several simulations were
run for directional solidification from different
numbers of seeds (from 2–60) and the preferred
growth direction of all the seeds, ⬍10⬎, were per-
fectly aligned with the grid. Different growth
phenomena are observed in the simulations with
different numbers of seeds, which can be roughly
divided into three categories: i) steady growth; ii)
dendrite branching; and iii) competitive growth.
Fig. 2 shows the dendritic structure after 40 s of
growth in these simulations with: (a) 8 seeds (375
µm initial spacing); (b) 12 seeds (250 µm initial
spacing); and (c) 20 seeds (150 µm initial spacing).
In these simulations, the secondary dendrites are
shown to develop perpendicular to the macroscopic
solidification direction and to coarsen with distance
from the primary dendrite tips, as shown in Fig.
2(b1) and (b2). Unlike the primary dendrites from
which they emanate, the secondary dendrites are
not identically arranged nor are they of uniform
size, indicating a degree of randomness in their
nucleation and competition in their growth. In case
(a), where the primary dendrite spacing is 375 µm,
some tertiary dendrites are observed emanating
from secondary dendrites and growing in the same
Variable Value
TLIQ 1609 K
m ⫺10.9 K/wt%
k 0.48
DL 3.0×10⫺9 m2/s
DS 3.0×10⫺12 m2/s
⌫ 1.0×10⫺7 K·m
C0 4.85 wt%
x 5 µm
t
1
ⱕ min
5 冉
⌬x ⌬x2
,
Vmax DL冊S
 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987 2977

Fig. 2. Simulation results of columnar dendrites developing form (a) 6, (b) 12 and (c) 20 seeds after 40 s of growth, under conditions
of a temperature gradient of 12 K/mm and a solidification rate of 150 µm/s. (a1) is an amplified (×2) section from (a) showing a
tertiary dendrite emanating from a secondary dendrite and blocked by another secondary dendrite. (b1) and (b2) show amplified (×2)
dendritic structure at the tip and about 2 mm below the tip position from (b). (c1) shows amplified (×2) dendritic structure about
2mm below the tip position from (c).

direction of the primary dendrites, but they are all
blocked by other secondary dendrites, with one
example shown in Fig. 2(a1). In case (b), no appar-
ent tertiary dendrites are observed due to smaller
primary dendrite spacing (250 µm). In case (c),
where the initial primary spacing is even smaller
(150 µm), the secondary dendrites are less
developed and have a smaller spacing than in case
(b). In these simulations, there is no indication of
dendrite branching or overgrowth and, conse-
2978 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
quently, no noticeable deviation from the initial
spacings during 40 s of solidification. The primary
spacings remain unchanged when the three simula-
tions were continued to 200 s.
From Fig. 2, a conclusion can be drawn that the
model predicts that columnar dendrites can pro-
ceed in a stable state 40 s after nucleation with a
quite wide range of primary spacings, from 150–
375 µm for the same thermal conditions. This
raises the question of how wide a range is possible,
and what will happen if the initial seed spacing is
outside this range. Fig. 3(a) and (b) show the den-
drite development during the initial growth stage
in two simulations from 2 and 60 seeds, respect-
ively. In Fig. 3(a) the dendrites develop from a
sparse distribution of seeds with an initial spacing
of 1500 µm. As solidification proceeds, many
small tertiary dendrites emanate from the second-
ary dendrites where the undercooling is progress-
ively increased. Some of the tertiary dendrites
grow very quickly and catch up with the two orig-
inal primaries. As a result, l1 is significantly
reduced, reaching 214 µm after 40 s. Fig. 3(b)
shows the dendrite development from a much more
closely spaced set of seeds that have an initial
spacing of 50 µm. Within 12 s, a few dendrites
have grown ahead, the others blocking their growth
by the formation of secondary dendrites. After 40
s of growth the dendrite spacing l1 increases also
to 214 µm. When the two simulations continue to
200 s, l1 in case (a) increases slightly to 231 µm
while in case (b) it remains unchanged. Although
the initial spacings in the two simulations are very
different, one is 1500 µm and the other only 50
µm, the final dendritic structures show little differ-
ence, and with a similar primary dendrite spacing.
More simulations with different initial seed spa-
cings (l01) were run to explore the relationship
between the final primary dendrite spacing and
initial seed spacing, with the results given in Fig.
4. The initial seed spacing ranged from 50–1500
µm, resulting in predicted final stable primary den-
drite spacing (lS1) of 130–430 µm, or an upper limit
of approximately 3 times the lower limit. The
stable spacing can be divided into three categories:
lS1 ⬎ l01: when l01 is less than 130 µm, the diffusion
field interaction of neighboring dendrites is so
strong that competitive growth occurs, with the
spacing increasing by an overgrowth mechanism.
lS1 = l01: when lS falls between 130–430 µm, the
simulation results show no change in primary spac-
ing, with a final l1 equal to l01; therefore, the initial
spacing is stable for the given thermal conditions.
lS1 ⬍ l01: when lS is larger than 430 µm, the gaps
between the original dendrites are so large that ter-
tiary dendrites can form reducing the spacing by a
branching mechanism.
3.2. Effect of solidification rate
The stable primary dendrite spacing reached in
the simulations starting from a wide range of initial
seed spacings with a constant solidification rate of
150 µm/s is shown in Fig. 4. A series of simula-
tions with the same initial nucleation conditions
were then carried out with a range of solidification
rates from 10–300 µm/s, all at the same constant
temperature gradient of 12 K/mm. The distribution
of calculated values of the average dimensionless
primary dendrite spacing, defined as l⬘ = lmC0 /
⌫, against dimensionless solidification rate, defined
as V⬘ = V⌫ / (DLmC0), for various initial nucleation
conditions at different solidification rates is shown
in Fig. 5. The graph is plotted on a logarithmic
scale, with two sets of axis, one for dimensionless
values and the other for dimensional values. The
points at each solidification rate represent the final
stable primary dendrite spacing in the simulation
with different numbers of seeds. It is noticed in
the figure that fewer points are obtained at some
solidification rates that others, because simulations
starting with different numbers of seeds could
result in the same final primary dendrite spacing.
A noticeable characteristic of the results is that all
these points are all located within a narrow band
demarcated by two parallel lines:
l⬘1max ⫽ 1.49 ⫻ 104(V⬘)⫺0.288
. (11)
l⬘1min ⫽ 4.51 ⫻ 103(V⬘)⫺0.288
These two lines give the upper and lower limits
of the allowable primary dendrite spacing, both of
which are power functions of solidification rate.
The value of the exponent is marginally higher
than the value of 0.25 predicted by early analytical
 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987 2979

Fig. 3. Predicted evolution of dendritic structure in directional solidification processes with (a) 2 and (b) 60 seeds nucleated at the
bottom under conditions of a temperature gradient of 12 K/mm and a solidification rate of 150 µm/s.

solutions of dendrite growth (Eq. (1)), but well
within the range of values predicted by Hunt and
Lu [12] using a quasi-3D simulation (i.e. 2D
axisymmetric). The upper limit of the l⬘1 distri-
bution is about three times that of the lower limit,
whereas Hunt and Lu [12] suggested a factor of
approximately two. In practical solidification there
are inevitable fluctuations in the processing con-
ditions, which may affect the dendrite growth and
thereby change the final l⬘1.
2980 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
Fig. 4. Final stable primary dendrite spacing (lS1) versus the
initial seed spacing (l01).
Fig. 5. Distribution of primary dendrite spacing against solidi-
fication rate.
3.3. The effect of perturbations of solidification
rate
Since perturbations of the control parameters in
practical solidification are usually unavoidable,
artificial perturbation of the solidification rate has
been incorporated in the simulations to investigate
its effect. Fig. 6 shows the change of the dendritic
structure in the simulation with 6 seeds, undergo-
ing the following cycle of perturbation: (i) 0–40 s,
V = 150 µm / s; (ii) 40–50 s, V = 300 µm / s; (iii)
50–60 s, V = 75 µm / s; and (iv) 60–75 s, V =
150 µm / s. The primary dendrite spacing remains
unchanged in the first 40 s of growth, maintaining
the initial seed spacing of 500 µm (see Fig. 6(a)).
Doubling the solidification rate causes almost
immediate dendrite branching and a rapid increase
in the density of primary dendrites reducing l1
from 500 to 188 µm (see Fig. 6(b)). Subsequent
reduction in the growth rate to half of the original
value, leads to a very slow increase in dendrite
spacing, which continues on returning to original
growth velocity to approach a stable state spacing
of 231 µm (see Fig. 6(c) and (d)). Fig. 6(e) shows
the global structure, from which the generation and
annihilation of dendrites can be clearly observed.
Similar perturbations of the solidification rate
were then applied to all the simulations with differ-
ent numbers of seeds at each solidification rate.
The predicted dimensionless average primary den-
drite spacing l⬘1 against dimensionless solidifi-
cation rate V⬘ from different nucleation conditions
after perturbations of the withdrawal velocity are
plotted in Fig. 7. The upper and lower limits of
the l⬘1 distribution after perturbation of the solidi-
fication rate are expressed as:
l⬘1max ⫽ 1.22 ⫻ 104(V⬘)⫺0.291
. (12)
l⬘1min ⫽ 5.24 ⫻ 103(V⬘)⫺0.291
Comparing the results to those without pertur-
bation (Eq. (11)), the values of the exponents are
similar, but the upper limit is now about twice that
of the lower limit, which is in better agreement
with the suggested values of Hunt and Lu [12]. The
change in the ratio between the upper limit and the
lower limit shows that perturbation of the growth
rate reduces the dendrite spacing to a narrower
range than the steady state growth condition.
The Kurz–Fisher prediction [10] and previous
experimental results [7,29,30] are also shown for
comparison. However, the simulated primary den-
drite spacings are higher than experimental results.
This discrepancy may be due to the experiments
being carried out in 3D, and the simulations in 2D.
In order to carry out direct comparison between
simulations and experiments, some 3D simulations
were carried out, with results displayed and dis-
cussed in the next section.
 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987 2981

Fig. 6. Simulated dendrite structures undergoing a cycle of perturbation of the withdrawal velocity around a mean value. (a) t =
40 s, V = 150 µm / s, (b) t = 50 s, V = 300 µm / s, (c) t = 60 s, V = 75 µm/ s, (d) t = 75 s, V = 150 µm/ s, (e) the global structure.

4. Three dimensional simulations
A 3D simulation was first performed for a single
grain nucleated at a undercooling of 5 K and grow-
ing under conditions of a temperature gradient of
12 K/mm and a constant cooling rate of ⫺1.8 K/s.
The simulation was run on a regular cubic grid
composed of 100 × 100 × 100 cells with a cell size
of 5 µm. The grain is nucleated at the center of
the box, with an initial misorientation characterized
by three Euler angles (0°, 20°, 0°). The dendritic
morphology of the grain after 1 s of growth is
shown in Fig. 8(c). The envelope of the dendritic
grain shows excellent accordance with both the
2982 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987

analytical and numerical predictions of a dendritic

Fig. 7. Distribution of primary dendrite spacing against solidi-
fication rate after a cycle of perturbation of the withdrawal velo-
city.
grain envelope by Gandin and Rappaz [23], as
shown in Fig. 8(a) and (b). A major improvement
of the current model is its capability of reproducing
the micro-scale dendritic structure, such as primary
and secondary dendrites, and hence allows the
interaction of the solute fields of both dendrite tips
and between grains to be studied.
Using this model, simulations of directional sol-
idification were then performed on a domain of
150 × 50 × 250 cells with the same cell size, under
conditions of a temperature gradient of 12 K/mm
and a constant solidification rate of 150 µm/s. The
effects of the initial nucleation density at the base
and perturbations of the solidification rate on the
dendritic structure are considered in turn.

Fig. 8. 3D views of (a) analytical and (b) numerical predictions of a dendritic grain envelope without considering solute diffusion
(after [23]), and (c) simulated dendritic structure coupled with solute diffusion. Simulation (c) was run on a regular cubic grid with
a cell size of 5 µm under conditions of a temperature gradient of 12 K/mm and a cooling rate of ⫺1.8 K/s. The original misorientation
of the grain is characterized by three Euler angles (0°, 20°, 0°).
 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
4.1. Effect of initial nucleation density
Similar to the preliminary 2D simulations, the
initial seed spacing has an important effect on the
development of columnar dendrites. Fig. 9 shows
the development of three dendrites at different time
steps: (a) 2 s, (b) 4 s, (c) 6 s and (d) 40 s. Three
seeds are nucleated at the bottom, equally spaced
along the x direction, with the ⬍100⬎ directions
perfectly aligned with the coordinate axis.
Although some tertiary dendrites are observed
Fig. 9. 3D simulation for 3 seeds at a solidification time of
(a1) 2 s, (b1) 4 s, (c1) 6 s, and (d1) 40 s. (a2) transverse slice
at z = 150µm, t = 2 s, (b2) transverse slice at z = 450 µm, t
= 4 s, (c2) transverse slice at z = 750 µm, t = 6 s, and (d2)
transverse slice at z = 750 µm, t = 40 s.
2983
emanating from the secondary arms at the initial
growth stage, they are blocked by the secondary
dendrites growing from the primary dendrites, as
shown in Fig. 9(a1). The three primary dendrites
proceed at the same velocity along the z direction,
and the primary dendrite spacing remains
unchanged (see Fig. 9(b), and (c)). At 6 s the mov-
ing frame of reference technique is activated and
the whole domain is cooled down at a constant rate
of ⫺1.8 K/s. The dendrites keep growing, but their
tip position remains roughly unchanged relatively
to the moving reference frame. This simulation was
continued until 40 s from the start of growth, and
no apparent change was observed in the primary
dendrite spacing. Because of the periodic boundary
conditions along x and y directions, these primary
dendrites are of quadratic arrangement in the trans-
verse section perpendicular to the macroscopic sol-
idification direction. This can be viewed by rep-
licating the transverse slide shown in Fig. 9(d2)
along both the x and y directions infinitely. The
primary dendrite spacing along the y direction is
equal to the box size along y direction, 250 µm,
and the primary dendrite spacing along x direction
is the box size along x direction divided by 3,
which is also 250 µm.
A 3D example of steady growth for a simulation
with 3 seeds has been shown in Fig. 9, and two
examples of transient growth are shown in Fig. 10
(1 seed) and Fig. 11 (15 seeds). When only one
seed is placed at the bottom (see Fig. 10(a)), it
grows freely along all the directions at the initial
solidification stage. The secondary dendrites along
the x direction grow faster than in the z direction,
because of greater tip undercooling. Many small
tertiary dendrites were observed emanating from
the fast growing secondary dendrites, growing in
the same direction as the original primary dendrite.
The newly formed tertiary dendrites have a random
initial spacing, and some of them grow very
quickly at the expense of others (see Fig. 10(b)).
After 6 s of solidification, only 6 primary dendrites
survive the competitive growth; among which 5
have developed from the tertiary dendrites and 1
directly from the seed (see Fig. 10(b)). The 6 den-
drites all continue to grow for 40 s, without any
obvious change in the structure (see Fig. 10(b)),
2984 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
Fig. 10. 3D simulation for 1 seed at a solidification time of
(a1) 2 s, (b1) 4 s, (c1) 6 s, and (d1) 40 s. (a2) transverse slice
at z = 150 µm, t = 2 s, (b2) transverse slice at z = 450 µm, t
= 4 s, (c2) transverse slice at z = 750 µm, t = 6 s, and (d2)
transverse slice at z = 750 µm, t = 40 s.
resulting in an average primary dendrite spacing
along x direction of about 250 µm.
Fig. 10 gives an example of solidification with
sparse nucleation, during which both branching
and competitive growth phenomena are observed.
A contrary example with dense nucleation is
shown in Fig. 11, where 15 seeds were set at the
bottom (50 µm initial spacing). Because of the
dense packing along x direction, the growth of sec-
ondary dendrites along this direction is suppressed,
and the secondary dendrites show severe asym-
Fig. 11. 3D simulation for 15 seeds at a solidification time of
(a1) 2 s, (b1) 4 s, (c1) 6 s, and (d1) 40 s. (a2) transverse slice
at z = 150 µm, t = 2 s, (b2) transverse slice at z = 450 µm, t
= 4 s, (c2) transverse slice at z = 750 µm, t = 6 s, and (d2)
transverse slice at z = 750 µm, t = 40 s.
metrical development along both the x and y direc-
tions (see Fig. 11(b2)). As solidification continues,
the growth velocities of the 15 dendrites begin to
vary, leading to some of the dendrites to slow
down (see Fig. 11(c1)). This competitive growth
results in only 10 dendrites surviving after 40 s
of solidification (see Fig. 11(c1)), which gives an
average primary dendrite spacing along x direction
of about 75 µm.
 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
4.2. Effect of perturbation on pulling velocity
Perturbations of the withdrawal velocity were
also added to the three 3D simulations. All the 3D
simulations were subjected to the same cycle of
perturbations as described for the 2D simulations.
Fig. 12 shows the change of the dendritic structure
in the simulation starting with 15 seeds. When the
velocity is increased, the tip undercooling also
increases, thus the tip position falls back relative
Fig. 12. 3D simulation results for 15 seeds under perturbation
of withdrawal velocity at a solidification time of (a1) 40 s, (b1)
43 s, (c1) 60 s and (d1) 75 s. (a2) transverse slice at z = 750
µm, t = 40 s, (b2) transverse slice at z = 625 µm, t = 50 s, (c2)
transverse slice at z = 875 µm, t = 60 s, and (d2) transverse
slice at z = 750 µm, t = 750 s.
2985
to the reference frame, as shown in Fig. 12(b1).
Since the primary dendrite spacing along the x and
y directions are already very small, no branching
was observed. On the contrary, two dendrites slow
down and die out, as shown in Fig. 12(b1). It is
because of the decrease in the pulling velocity that
the relatively stable state the dendrites have achi-
eved at 40 s has broken down and introduced devi-
ations in spacings that lead the dendrites to select
a more stable spacing. When the pulling velocity
is decreased 10 s later, one more dendrite slows
down, as shown in Fig. 12(c1). Finally, 7 of the
10 dendrites survive the perturbation of the pulling
velocity, and the average primary dendrite spacing
along x direction increases to 107 µm
In 3D simulations, the partitioned solute at the
dendrite tip can diffuse away more efficiently than
in 2D simulations; therefore the primary dendrite
spacing in 3D is also smaller than in 2D. The upper
and lower limits of dimensionless primary spacing
l⬘1 against dimensionless solidification rate V⬘ in
3D may be obtained simply through modification
of the predicted limit lines in 2D (Eq. (12)) by mul-
tiplying by a factor, which is chosen as a factor of
√2 / 2 in this work:
l⬘1max ⫽ 8.63 ⫻ 103(V⬘)⫺0.291
. (13)
l⬘1min ⫽ 3.70 ⫻ 103(V⬘)⫺0.291
These two lines are plotted in Fig. 13, together
with the predicted average primary dendrite spac-
Fig. 13. Predicted 3D upper and lower limits of the distri-
bution of primary dendrite spacing, with the 3D simulation
results. They are compared with Hunt–Lu model [12] and pre-
vious experimental results [7,29,30].
2986 W. Wang et al. / Acta Materialia 51 (2003) 2971–2987
ing direction in the 3D simulations both without
and with perturbation. The Hunt–Lu prediction
[12] and previous experimental results [7,29,30]
are also shown for comparison. It can be seen that
the Hunt–Lu prediction is nearly a midline between
the prediction upper and lower limit lines, and the
predicted 3D results and the experimental values
fit well.
This result suggests that for applications such as
single crystal turbine blades, where as consistent a
spacing as possible is desirable, then perturbation
in the process parameters early on in the formation
of the dendritic microstructure might result in an
improved product. Defects may also be reduced if
the spacing is in the center of the range. For
example, if the spacing is near the upper limit of
the stable range, the solute fields interact less, and
hence the region of undercooling between the den-
drites is larger, which may lead to defects such as
stray grains, since any heterogeneous nuclei are
more likely to be activated.
5. Conclusions
A combined CA-FD model was developed to
simulate the solidification process of binary alloys.
The velocity of the solid/liquid interface, determ-
ined by the equilibrium conditions at the interface,
was calculated by considering both the solute and
curvature undercooling terms. A modified decent-
ered square/octahedron growth technique was
implemented to account for the effect of crystallo-
graphic anisotropy.
Two and three dimensional simulations were
carried out for the directional solidification of a
binary alloy with properties approximating a
nickel-based superalloy. The initial seed density
had a direct effect on the initial growth stage of
columnar dendrites, but had little effect on the pri-
mary dendrite arm spacing and tip undercooling
after the dendrite growth reached a stable state. It
was found that the dendrite spacing selection had
a hysteresis whose value in dendrite branching is
larger than that of dendrite competition. Pertur-
bation on the growth velocity affects both the pri-
mary dendrite arm spacing and tip undercooling.
The primary dendrite arm spacing has a much nar-
rower distribution after perturbation. The upper
limit of the distribution of primary dendrite arm
spacing is about two times of the lower limit. The
average primary spacing was found to be depen-
dent not only on the current growth conditions, but
also on the way in which those conditions were
reached.
Acknowledgements
The authors would like to thank Special Metals
Wiggin Ltd, Rolls-Royce plc, Wyman-Gordon Ltd,
QinetiQ and the EPSRC (GR/N14132) for financial
support together with the provision of both
materials and information. The authors gratefully
acknowledge the assistance of their colleagues in
the Materials Processing Group, ICSTM,
especially Drs A. Kermanpur and R. Atwood.
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