MEASUREMENTS OF CELL AND PRIMARY DENDRITE

ARM SPACINGS IN DIRECTIONALLY SOLIDIFIED

ALUMIN~UM ALLOYS
D. G. MCCARTNEY

and J. D. HUNT

Department of Metallurgy and !Science of Materials, University of Oxford,

Oxford, U.K.
(Rcceired 16 February

1981)

Abstract-Ceil and primary dendrite arm spacings have been measured in AI-& and Al-Mg-Si alloys
directionally solidified at steady state over a very large range of growth conditions. The Al-Mg-Si alloys
have been chosen so as to minimize gravitational fluid flow in the liquid. A spacing parameter, 1, has
been correlated with the liquid temperature gradient GL, the growth velocity, V and the bulk alloy
composition, C,.
It has been found that for dendrites in the ALMg-Si system
j.

272G;o.S

V-o.8

Cafe

where C&r is the atom fraction of Si in the alloy.

It has also been observed that there is a discontinuous change in the spacing relationship, as measured
by L, when the growth morphology changes from cellular to dendritic, Cells were found to form a
roughly hexagonal array whereas dendrites adopted a much less regular pattern. This discontinuous
change in I is explained by considering how the nature of an array affects its average nearest neighbour
spacing I*.
RCsum&-Nous avons mesure les espacements des cellules et des bras des dendrites primaires dans des
alliages Al-t3 et Al-Mg-Si 8 ~Iidifi~tion orient& en regime permanent, pour me gamme t&s &endue
de conditions de croissance. Nous avons choisi le systeme Al-Mg-Si afin de minimiser ICcoulement
gravitationnel dans le liquide. Nous avons corr& un parametre despacement avec le gradient de
temperature du liquide GL, la vitesse de croissance V et la composition massive de lalliage C, .
Dans le cas des dendrites du sy&me Al-Mg-Si
1 f 272Gie.5 V-.~s Cakes
oil CmsI est la tencur atomique de lailiage en silicium.
Nous avons egalement observe un changement discontinu darts lespacement mesure par 2, lorsque ia
morphologje de la croissance de cellulaim devient dendritique: Les cellulcs forment grossi&ement des
hexagones alors que les dendrites adoptent une configuration beaucoup moins r#gttliere. Nous expliquons ce changement discontinu de L en considCrant comment la nature dun arrangement affecte
lespaccment moyen P des premiers voisins.
Zusammanfaaaung-Die Abstiinde von Zellen und prim&en Dettdriten wurden in Ai-Cu- und ACMgSiLegierungen gemessen; die Legierungen waren unter stationiiren Bedingungen crstarrt in einem
groBen Bereich von Wachstumsbedingungen.
Die Al-Mg-Si-Lcgierungen
wurden gewghlt, urn
~a~~tions~in~e
Bewegnngen in der Riissigkeit zu ~~i~er~.
Ein A~~ds~ra~t~
d wurde
mit dem Temperaturgradienten Gr, in der Fhissigkeit, der Wachstumsgeschwindigkeit V und der Legierungsznsammensetzung C, korreliert.
Fiir die Dendriten in dem Al-Mg-Si-System ergab sich:
2 = 272GiO.sS V-O.%3p~32
t

wobei CIDsiden Atombruchteil des Si in dcr Legicrung bedqptet.

AuDerdem wurde beobachtet, dal3 eine diskontinuierliche Anderung in der Abstandsheziehung, gemessen mit .J, at&rat, wenn die W~hstumsmo~holo~e
vom zeUuBiren in den dendritischen Charakter
umschlug. Die ZeUen bilden eine etwa hexagonale S$uktur, wohingegen die Dendriten eine vie1 regellosere Struktur einnehmen. Diese diskontinuierliche Anderung in wird erkltirt, indem die Beeinflussung
des mittleren Abstandes ntichster Nachbarn I* durch die Strukturart betrachtet wird.

INTRODUCTION
There has been considerable experimental work in the
past number of years on the measurement of cell and
primary dendrite arm spacings in a variety of alloy
systems [l-11]. Much of this has, however, been carried out under conditions in which the temperature

gradient and growth velocity have not been measured

inde~ndendy and instead the spacing of the primary
arms has been correlated with a parameter such as
frtning rate or cooling rate [l-3,5]. Of the work h
which the primary spacings have been correlated with
gradient and velocity separately much has been car-

1851

1852

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DIRECTIONALLY SOLIDiFIED ALUMINIUM

ALLOYS

value. That is in a two component

system to make

-crucible
~=(~)c~~(~)~~
flow of solute
/rich liquid.

/isotherm
/macroscopic
S/L interface shape
during growth

Fig. I. Jkiation of the macroscopic interface shape (solid

line) from the shape of the isotherm (dotted line) due to
fluid flow. Dense solute rich liquid flows in the directions
shown by the arrows.

ried out over relatively small ranges of velocity,

gradient and composition, and/or in systems in which
convective mixing may have been an important factor
[4, G-11]*
It is sometimes assumed that one method of eliminating gravitational convection in the melt is to maintain a negative vertical density gradient in the interdendrite liquid by solidifying vertically upwards in a
system in which the solute being rejected at the interface is denser than the bulk liquid. Burden et al. Cl23
have shown, however, that this is not so. If at any
stage the macroscopic interface shape becomes
slightly non-planar the densest solute flows into the
retarded region and the resulting increase in solute
content will cause it to drop still further behind forrning a steeple as shown in Fig 1,
Preliminary experiments on an Al-6 wt.% Cu alloy
showed that specimens solidified at growth rates of
less than 8 x 10-3mms-
with a temperature
gradient of 6 K mm- exhibited severe macroscopic
interface curvature indicating significant fluid flow.
This curvature was not the result of changes in the
heat flow pattern since pure Al and an Al-01 specimen of eutectic composition solidified with near
planar interfaces indicating that the isotherms of the
system were also of this near planar shape.
In a dendritic specimen the liquid composition
between the dendrites varies with temperature as it
does along the liquidus line of the phase diagram, and
it has been suggested [13] that the average liquid
composition just ahead of the dendrites varies in a
similar way. Thus one method of eliminating or at
least reducing flow in this region is to reduce the
density change along the liquidus line, dp/dl; where p
is the density and T the temperature, to a very low

tend towards zero, where Ca is the alloy composition

and m is the liquidus slope. Previous work [I21 has
shown that it is very difficult to find a two component
system where the temperature density change is
sufficiently accurately balanced by the composition
density change to eliminate the flow.
It has, however, been possible to eliminate the flow
in a tin based system where zinc is the main alloying
element by adding small amounts of lead. A tin alloy
containing 0.19 at .% Pb and 3.85 at. Y. Zn showed no
fluid flow, a Sn-3.85 at.%Zn
alloy showed the
characteristic macrosegregation of a system where the
liquid gets lighter on cooling, whereas a Sn-3.37 at.%
Zn-0.35 at .% Pb alloy showed the characteristics of a
system where the liquid becomes denser [I45 A ternary alurn~i~
based alloy was developed having
similar properties. Increasing amounts of magnesium
were added to an aluminium-silicon
alloy until the
steeple effect was just eliminated. It was found that
provided the atomic ratio of Mg to Si was kept constant in alloys of different total solute content flow
did not appear to occur. The Al-Mg-Si system whose
phase diagram is shown in Fig 2 is suitable for other
reasons as welL The Al-Si and A?-Mg bmaries have
similar liquidus and solidus slopes. The ternary alloys
might thus be expected to behave as pseudo-binaries,
with the solid-liquid tie lines lying along the lines of
constant Mg to Si ratio and freeze in a similar fashion
to simple binary alloys in which aluminium is rejecting a single solute.
The main object of this work was thus to measure
primary arm spacings over a wide range of growth
velocity, temperature gradient, and alloy composition
in the Al-Mg-Si system, under conditions in which
solute diffusion was the dominant mechanism of mass
transfer.

EXPERIMENTAL

METHOD

Apparatus
The aluminium alloy specimens contained in
graphite crucibles were directionally solidified in three
different types of furnace arrangements in order to
cover the required ranges of growth velocity and
temperature gradient.
Low temperature gradients of between 0.2 and
1.5K mm- at growth rates ranging from 4 x 10-s
to lo- mm s-i were obtained by using a thermal
valve furnace [16] which is shown schematically in
Fig. 3. The alloy was contained in a graphite crucible
of 9.0mm O.D. and 300mm total length which was
drilled out to a depth of 180mm with an I.D. of
7.3 mm. The furnace consisted of three separate heating zones each of which was controlled independently,
and the crucible was held in a fixed position. The

MCCARTNEY

Al

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DIRECTIONALLY SOLIDIFIED ALUMINIUM ALLOYS

1853

At %

Si

Fig. 2. Al rich corner of the Al-Mg-Si phasq diagram showing eutcctic valleys (solid lines) and isotherms

on the liquidus surface (dotted lines). Taken from reference [16].

middle zone was kept as near as possible (within

about one degree) to the temperature of the freezing
interface, and the top and bottom zones were controlled by thermocouples inserted in the specimen.
Temperature measurements in the specimen were
made using four transverse Pt/Pt, 13%Rh thermocouples placed 10 mm apart, made from 0.15 mm dia.
wire and insulated from the specimen using alumina
tubing of 0.2 mn I.D. 0.5 mm O.D. By feeding linearly
increasing D.C. voltages into the top and bottom
zone thermocouple circuits, the temperature of both
ends of the specimen could be made to decrease
linearly and a constant growth rate and temperature
gradient could be obtained. The temperature vs time
trace for each of the four thermocouples was recorded
in turn, enabling the growth velocity and temperature
gradient to be measured and their linearity checked.
The specimen was then rapidly quenched into a water
bath after it had grown approximately 10 mm past the
fourth measuring thermocouple. Only specimens in
which the velocity and temperature gradient changed
by less than 5% were used for spacing measurements.
Intermediate temperature gradients of between
at growth rates ranging from
2.5 and lOKmm-
4 x lo- 3 to 1 mm s- were obtained using a Bridgman type of furnace arrangement which is shown in
Fig. 4. The furnace temperature was controlled by a
thermocouple placed between the heating element
and the alumina tube. Improved stability was
achieved for low velocity runs by filling the interior of
the furnace tube with an insulating material; a 13 mm
diameter hole being left down the centre. The alloy
was contained in a graphite crucible 6.3 mn O.D.,
4.3 mn I.D., and 220mm long held in a stainless steel

rod. Unidirectional growth was achieved by withdrawing the specimen at a constant rate into a water
bath contained in a water-cooled brass jacket which
was inserted into the hot zone of the furnace. Preliminary experiments were carried out to check that the
withdrawal rate was qua1 to the growth rate of the
interface over the entire range of growth conditions.
control

thermocouple.

top furnace.

_ _._tirmocouDle
iiikple.

Fig. 3. Sectional view of the thermal valve furnace.

1854

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SOLIDIFIED

ALUMINIUM

ALLOYS

The

master alloy was prepared by melting

in a vacuum furnace, carefully adding
99.99% Mg in such a way as to prevent any loss by
99.99%Al

oxidation,

mixing the molten alloy well and then prq-

ducing a rapidly solidified cast rod of 10.5 mm diameter and 150 mm long. Slices of this cast rod were
chemically analyzed using atomic absorption spectrophotometry. Slices taken from either end were found
to be of slightly different composition from those
taken from the central 140 mm of the rod which were
of uniform composition and within 5% of the made
up composition. Thus 1Omm were discarded from
each end of the master alloy rod and only the central
130 mm was used in making up the Al-Mg-Si alloys.
water
bath.

minsulation.
Fig. 4. Sectional view of intermediate temperature gradient
furnace.

The temperature of the specimen was recorded using

a single transverse pt/Pt, 13% Rh thermocouple of the
same size as before, and from the temperature versus
time trace the temperature gradient in the liquid at
the growth front was measured. The specimen was
rapidly quenched into water after it had grown at
least 10mm past the thermocouple and after at least
50 mm of steady state growth had taken place.
The arrangement of the high temperature gradient
furnace was essentially the same as that shown in
Fig. 4 except that the water bath was replaced by a
liquid metal coolant (LMC) which was held at 65C
by pumping hot water around the water jacket. Using
this apparatus gradients of up to 20 K mm- at velocities ranging from lo- to 1 mm s- were obtained.
Alloy Preparation

Al-Cu alloys were prepared by melting together the

required amounts of 99.99%Al and 99.99x01 in a
vacuum, mixing well and charging the molten alloy
directly into the graphite crucible already in position
in the unidirectional growth apparatus and held at a
sufficiently high temperature to prevent the molten
charge solidifying. By filling the graphite crucibles in
this way macrosegregation, which would otherwise
occur due to the freezing and remelting of the alloy, is
avoided.
Al-Mg-Si alloys were prepared from 9.990/,Al
99.99/,Si and an Al-Mg alloy containing a known
amount of Mg (usually about 4 wt.%). The melting
and charging technique was identical to that for the
Al-Cu alloy.

Measurement of primary spacings

The quenched unidirectionally grown specimens

were removed from their graphite crucibles and a
longitudinal section which included the quenched
interface was cut from the solidified rod. This was
ground and polished to reveal the quenched interface
and a transverse section which contained
the
quenched interface was then prepared. This was carefully ground from the quenched liquid side until the
tips of the primary arms just became visible. This
ensured that the primary spacing at the growth front
was measured rather than the final spacing obtained
after coarsening. These spacings have been shown to
be very different in cellular specimens [a].
An area counting method was used to obtain a
measure of the cell/dendrite primary spacings. A spao
ing parameter, 2, was calculated by counting the
number of primary arm centres, N, inside a known

Table 1. Measurements of primary arm spacing parameter,

5 in Al-6 wt.% Cu specimens

1
Irm
128
76
72
66
158
118
96
475
310
280
200
175
471
415
349
251
398
380
355

Morphology
D
::
::
D
::
D
D
D
D
D
D
D
:
C
C

Growth
Rate mm s-l

Liquid
temperature
gradient
K mm-

1.0
1.0
1.0
1.0
5 x 10-l
5 x 10-l
5 x 10-I
5 x 10-z
5 x 10-z
5 x 10-f
5 x lo-*
5 x 10-f
1.67 x IO-*
1.67 x IO-
1.67 x IO-*
1.67 x IO-*
4.3 x lo-
4.3 x lo-
4.3 x 1o-3

3.40
11.0
12.1
15.5
4.85
8.70
13.9
2.05
5.50
7.90
11.8
16.7
3.67
4.86
6.70
13.0
4.2
6.0
8.4

The morphology is indicated as dendritic (D) or cellular

0.

MCCARTNEY

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DIRECTIONALLY

Table 2. Measurements of primary arm spacing parameter,

i, in Al-O.63 at.% Mg-1.39 at.% Si specimens
I
/tn1

Growth rate
mms-

Liquid temperature
gradient K mm-

444
439
320
320
290
390
231
302
176
300
151
140
198
87
210
70
870
630
1034
1270
860
800
1055

1.73 x
1.73 x
1.73 x
1.73 x
1.73 x
3.30 x
5 x
6.67 x
6.67 x

4.10
5.20
9.40
9.70
11.7
4.20
9.20
4.80
14.2
3.95
14.7
17.0
3.74
14.7
2.92
15.5
1.64
1.10
1.12
1.14
0.92
0.84
0.45

10-z
10-l
1o-z
10-z
10-2
10-l
10-Z
IO-*
lo-*
10-l
10-l
10-l
5 x 10-l
5 x 10-l
1.0
1.0
1.18 x lo-*
10-I
1.45 x 10-z
7.70 x lo-
3.67 x 1O-2
6.45 x 1O-2
1.08 x 10-l

All specimens had dendritic morphologies.

126
133
220
340
616
434
895
614
532
380
612
48.0
60.5
76.4
55.3

Morphology

Growth rate
mm s-l

Liquid
temperature
gradient
K mm-

5 x

D
M

10-l
5 x 10-l
10-l
1.05 x 10-l
1.50 x 10-l
6.91 x lo-
4.60 x 10-2
3.33 x 10-2
3.85 x lo-
3.17 x 10-z
1.83 x 1O-2
5 x 10-l

3.15
2.30
2.35
1.08
0.35
0.92
0.30
0.66
0.81
1.67
0.76
11.0

5 x 10-l
5 x 10-l
10-l

8.82
6.05
18.5

72.1
99.0
158
66.0

89.7
85.0
154
175
98.0
154
130
173

M
C
C

C
C

3.33 x
3.33 x
3.33 x
3.33 x
3.33 x
1.67 x
1.67 x
8.3 x
8.3 x

10-l
10-l
10-l
10-2
10-2
10-2
10-2
10-2
lo-
1O-2
1O-3
lo-

ALUMINIUM

ALLOYS

1855

Table 4. Measurements of primary arm spacing parameter,

1. in alloys of various total solute contents with a constant
atomic ratio of Mg to Si equal to 0.45.

i
/tm

C,Si
at./,

Growth rate
mms-

Liquid
temperature
gradient
K mm-

145
190
239
275
338

0.35
0.83
I .39
2.61
4.68

lo-
10-l
10-l
10-l
10-l

5.85
5.80
6.05
5.50
6.23

C,Si is the atomic percent silicon in the alloys.

area, A, at four different locations on the transverse

section and setting 1 equal to &%. Each measurement given in Tables 14 is the average value of
JX/N taken over the different locations. The error
bars on all the graphs were obtained by plotting the
smallest and largest values of I measured on a particular transverse section.
RESULTS
Since a significant amount of work was carried out
on both the Al-& and Al-Mg-Si systems the results
are presented separately.

Table 3. Measurements of primary arm spacing parameter

d in Al-O.15 at.% Mg-0.33 at.% Si specimens.

1
Itm

SOLIDIFIED

11.0
4.20
6.3
18.0
10.0
9.65
5.55
4.43
11.0
5.48
8.43
4.40

Morphologies are indicated as cellular (C), Dendritic (D)

or mixed (M)

Al-6wt.% Cu
The measurements of the primary spacing parameter, k on A1-6 wt.% Cu are listed in Table 1 and
presented graphically in Fig. 5 in which log 1 is
plotted against log GL for various different growth
velocities Y
All the closed points represent specimens which
solidified dendritically with macroscopically planar
solid-liquid interfaces. The open points represent
those specimens which solidified with a cellular
morphology and with macroscopically curved solid
liquid interfaces. A longitudinal section through the
quenched interface of such a specimen is shown in
Fig. 6. Electron microproble analysis of this specimen
revealed that the composition of the quenched liquid
20 mm from the interface was uniform and equal to
the made up composition of 6wtP/,Cu. The composition of the quenched liquid was also analyzed just
ahead of the leading part of the macroscopic interface
and down the right hand side of the specimen. Ahead
of the leading edge it was found to contain
6.5 wt.%Cu whereas down the side the Cu content
rose to approximately 11.5 Wt.% Cu, indicating severe
segregation due to gravitational fluid flow.
A best fit double linear regression analysis on all
the data at 1.67 x lo- mm s-l and above shows
that
~ = K Gi0.55 V-o.28
where K is a constant and there is a standard error in
both exponents of f0.02. The primary spacings in

1856

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DIRECTIONALLY

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ALUMINIUM

ALLOYS

AL-6wt/oCu

2.7 2-b 2.5 2.4 2.3 -

2.1 2.0 -

0.2

I
03

I
0.1

I
05

1
0.6

I
0.7

I
08

I
09

I
1.0

1
14

I
1.2

-I
1.3

h(GJ
Fig. 5. Plot of log 1 vs log GLfor Al-6 wt.% Cu at various different growth velocities, I! Closed points
represent dendritic specimens. Open points represent cellular specimens solidified at V = 4.3 x lo-
mms-. Lines of slope -0.5 are drawn through the dendritic points.

specimens grown at 4.3 x lo-mms-

are smaller
than would be predicted from the above equation (as
can be seen from Fig. 5) and are almost independent
of gradient. It would seem that this is most probably
due to the convective flow which is observed to occur
and is discussed further later.
Al-Mg-Si

Fig. 6. Longitudinal section showing the quenched interface of an AI-6 wt.,, Cu specimen with Y = 4.3 x
IO- mm s-I and GL = 5.5 K mm-. Magnification =
23 x .

In order to reduce the macroscopic interface curvature due to fluid flow (see Fig. 1) it is necessary to
eliminate, or reduce to a small value, density changes
with composition and temperature ahead of the dendrite tips and in the interdendritic liquid. This can be
done by choosing a ternary alloy containing one solute element which is denser than the solvent and one
which is less dense. If the composition of an alloy is
adjusted there will be one particular atomic ratio of
Mg to Si which just eliminates density changes with
composition and temperature along the liquidus. A
series of unidirection growth experiments was carried
out at a growth rate of 4.3 x lo- mms- with a
temperature gradient of 5.5 K mm- in order to determine the Mg to Si ratio which produced a minimal
amount of fluid flow (as assessed by the macroscopic
interface curvature of a quenched specimen).
A number of alloy specimens each containing a
known amount of solute but with different Mg to Si
ratios weie directionally frozen at steady state for approximately 50mm and rapidly quenched. A longitudinal section containing the quenched interface was
then examined and its macroscopic curvature com-

MCCARTNEY

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DIRECTIONALLY SOLIDIFIED ALUMINIUM ALLOYS

1857

(b)
Fig. 7. (a) Longitudinal section showing the quenched interface of an Al-Cu eutectic specimen. V = 4.3
x 10-3nuns;GL = 6.8 Kmm-. Magnification = 23 x . @)L.ongitudinal section showing the quenched

inte~a~ofanAl=0.61at.~M~l.3Qat.~gis~men.
V=4.3 x 10-mns-;
Magnification = 23 x .

pared with that of the freezing isotherm for an Al-Cu

eutectic specimen under the same conditions. When
the liquid at the dendrite tips is much denser than
that of the bulk liquid severe macroscopic curvature
develops (as shown in Fig. 6 for Al-6 wtp/,Cu)
whereas if it is only slightly denser the macroscopic
curvature is greatly reduced. It was found that an
alloy containing 1.39 at.% Si and 0.63 at.% Mg (a Mg
to Si ratio of 0.45) exhibited only a small deviation
from the isotherm shape indicating a minimal amount
of fluid flow due to the liquid at the dendrite tips
being only slightly denser than the bulk liquid.
Figures 7(a) and (b) compare the quenched interfaces
of an Al-Cu eutectic and Al-O.63 at.% Mg-1.39 at.%
Si solidified under the conditions described above.
The Al-Mg-Si phase diagram is shown in Fig. 2. It
is apparent that because of the similar slopes of the
binary Al-MB and Al-Si liquidus lines, the ternary
alloy of the above composition might be expected to
behave like a pseudo-binary system. Hence all alloys
subsequently used were made up to lie in this pseudobinary system (that is with a Mg to Si ratio of 0.45)
and none appeared to exhibit fluid flow.

GL=5.5Kmm-.

The measurements of the spacing parameter, J,, in

Al-Mg-Si alloys of two different compositions are
listed in Tables 2 and 3 and the growth morphology is
also indicated. From the results obtained for the alloy
containing 0.63 at.% Mg, 1.39 at .% Si it is possible to
relate I for dendrites to GL and V using a double
linear regression analysis on the 23 data points. It is
found that
L = 346 (3EO.S6 y-O.28
with a standard error in both exponents of f0.02.
By carrying out a similar analysis for the specimens
containing 0.15 at .% Mg 0.33 at.% Si and using 10
data points from fully dendritic specimens we find
that
2 = lgl

Gi0.54

V-O.8

with a standard error of f0.03 in the GL exponent

and i-0.02 in the V exponent.
By considering the 9 data points from cellular
specimens with the same ~m~sition
and applying a
similar analysis we find that
J. = 145 GLO46

v-0.20

1858

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DIRECIIONALLY SOLIDIFIED ALUMINWM

ALLOYS

WX)
t

dendrites
f-----.

Fig. 8. Plot of log A vs log (C, Y.) for cells and dendrites. Circles represent dendritic specimens, squares
cellular ones. &St fit lines are drawn through the points and a line of slope -0.5 is indicated for
comparative purposes.

are for

with standard errors of f0.04 and 20.03 in the Cr.

and V exponents respectively.
One way of representing these results graphically is
by plotting log (It) against log (GLVi*) and this is
done in Fig 8 for dendrites grown at both tempositions and for cells produced from the alloy of lower
solute content. The error bars indicated were
obtained as previously described, best fit lines are
drawn through the data points, and a line of slope
-0.5 is included for comparative purposes.
It can be seen from Fig. 8 that although the spacing
of cells and dendrites grown from alloys of the same
composition follow a similar functional dependence
on Gt and V over the range considered, the two best
fit lines are displaced from one another. This effect is
better illustrated by Plotting log (2) vs log (GL) for
four different growth velocities as shown in Fig. 9.
Lines of slope -0.5 are drawn through both the cellular and dendritic points, and the error bars have been
obtained as previously described. For each growth
rate the two lines are displaced relative to one
another and specimens of mixed morphology lie on
neither line. (Specimens are defined as being of
mixed morphology when a transverse section contains primary stalks both with and without sidearms).
It would thus seem that this effect is in some way
related to the transition from dendritic to cellular
growth.
These results clearly show that there is a break
going from a cellular to a dendritic structure when the
spacing is measured as *1= @j%. There has been
some doubt about this in the past 163.
in order to determine the composition dependence
of the primary dendrite arm spacing parameter 1, a

number of specimens of &&rent totat solute contents

but with the same atomic ratio of Mg to Si were
solidified at the same growth rate at gradients of ap
proximately 6.0 K mm- * and the results are listed in
Table 4. The actual spacings were then corrected for
the small differences in actual gradient from one
specimen. to another assuming a Gii* relationship
before being plotted graphically.
Figure 10 is a plot of log (A) vs log (Cas& where
Cmsi is the atomic percent of silicon in the alloy, for a
constant growth rate and temperature gradient+ The
error bars were determined as before and a best fit
line of slope 0.32 k 0.04 is drawn through the points.
A line of slope +0.33 is included for comparative
purposes.

SUNNY

OF RESULI3

The extensive data on Al-h4gSi alloys directionally solidified at steady state vertically upwards and
stable against fluid flow give the following main
results:
(i) 1 ==346 GLO*ss Y-oP2s for dendrites grown from
alloys of composition Al-O.61 at.% Mg-1.39 at.% Si
with a standard error &0.02 in both exponents.
(ii) A = 181 Gi** Y-o.zs for dendrites grown
from alloys of composition Al - 0.15 at.% Mg - 0.33
at.%Si with standard errors of f0.03 and f0.02 in
the GL and V exponents respectively.
1 = 145 GL0*46V-o*2ofor cells grown from the
same composition with standard errors of &0.04 and
f 0.02 respectively.

MCCARTNEY

AND

HUNT:

DIRECTIONALLY

SOLlDlFIED

ALUMINIUM

ALLOYS

1859

Dendrites
f
:,a&ufvs.
+

v =3.3&&n/$.

f
4

v=W&ulvs.

v =ti?n*

Fig. 9. Plot of log 1 vs log GL for cells and dendrites grown from Al-O.15 at.% Mg-0.33 at.% Si at four

different growth rates.

(iii) At a f&d grow&h rate of 10-t mms-t and
temperature gradient of approximately 6.0 K mm-
the composition dependence of the primary dendrite
arm spacing is given by 1 a (C,S1)0~32*0~04.Where
Cmsi is the atomic percent of silicon in the alloy, the
Mg to Si ratio has been fixed at 0.45 and d has been

+-O-45l

-036I

-0.26
I

-096-046
t
1 0 I

corrected for small deviations of Gt from the nominal

value.
(iv) By combining the results on Al-Mg-Si
dendrites from (i) (ii) and (iii) above we obtain a
combined relationship which is given by
1 = 272 G;O.ss V-0.28 -0,32.

I
*O-l0

,
l

I
0-x

I
+ 0-u

I
* OIL

Log(&&if

Fig. 10. Plot of log I vs log (CT,,,) at a constant temperature gradient (6 K mm-), growth rate
(lo- mm s- *), and atomic ratio of Mg to Si (0.45). A best fit line is drawn through the points and one of
slope 0.33 is included for comparison.

186@

MCCARTNEY

AND

HUNT:

DIRE~lONALLY

DISCUSSION
Comparison with theoretical models

The problem to be modelled is the growth of an

array of dendrites in a positive temperature gradient.
Most of the detailed theoretical treatments of dendritic solidification have considered the growth of an
isolated dendrite into an undercooled bath [17-231,
and are not readiIy appli~ble to the growth of an
array. The most complete treatments of the array
problem to date which relate dendrite spacings to
growth variables are those due to Hunt [24] and
Kutz and Fisher [25].
Both predict a primary spacing relationship of the
form
;, = K G-o.5 y-0.2$ Cto.25
m
where G is the temperature gradient, I/ is the growth
velocity and Ic is a constant for a binary alloy whose
solute content is C, providing the critical conditions
for plane front breakdown are sufficiently exceeded.
It is clear that our results on primary dendrite spao
ings are in good agreement with the G and V exponents predicted by these models, although agreement
with the composition exponent is less good. A more
detailed comparison is to be made in due course when
the constants needed in the analyses have been
obtained from work presently being carried out.
Both models indicate a change in the alone
relationship when the growth rate is no longer much
greater than that which would just produce planar
front growth, and the predictions of the two models
are shown in Fig. 11 using data from reference [25J
for an Al-2 wt .% Cu alloy. Figure 11 illustrates the
variation of primary spacing with growth rate (at a
constant gradient) predicted by the two models. KUR

SOLIDIFIED

ALUMINIUM

ALLOYS

and Fishers model [25] predicts that at sufficiently

low growth rates the cell spacing initially becomes
larger than that which would be expected by extrapolating the dendrite measurements at higher velocities. Our results provide no evidence for this and we
have found, to the contrary, that the spacing parameter, j,, for cells is less than would be predicted
from the ~asuremen~
on dendrites grown from
alloys of the same ~m~sition.
Other more approximate models have been put
forward by other workers[26-295, but our results,
obtained over wide ranges of GL and K show significant discrepancies from the predicted exponents.
Cellular-dendritic

transition

Figure 8 illustrates the discontinuous nature of the

relationship between the spacing parameter 11 and
(G Y) for cells and dendrites grown from alloys of
the same ~m~sition.
The graph of log I vs log GL
for various different growth rates shown in Fig. 9
indicates that for both oells and dendrites I = KGE
where a is approximately 0.5 for both 8;rowth forms,
that K is smaller for cells than for dendrites and that
the change in K is associated with a change in morphology both of the primary stalks and of the array
adopted by the growing primary arms. (Those specimens defined as mixed contain primary arms both
with and without secondary arms.)
As was mentioned earlier, the spacing parameter 1
is defined as J&%. The actual spa&g in a regular
array depends on the form of the array. If we define
the nearest neighbour spacing as 1+ then for a hexagonal array we find that ,I: = 1.075 &@I. For a
square array 12 = J7ii. For a completely random
array of points it has been shown [30] that the average nearest neighbour distance is given by 5+ = 0.5

x
8

VCS

Al-Zwt%Cu.

io*

Fig. Ii. I as a function of Y in an Al-2 wt.% Cu alloy at a temperature gradient of IOK mm- as
predicted by the models of Hunt (241 and Kurz and Fisher [25] (Iabelled Hand K-F respectively). The
data is taken from Ref. [253, and V,, is the constitotiona1 supercooling velocity for planar front growth.

MCCARTNEY
h

AND HUNT:

is defined as J1AIN) where N

number of primary arm centres

SQUARE

ARRAY
.
.

DIRECTIONALLY

is the
in an area A

AL
.
.

ALUMINHJM

ALLOYS

1861

It is concluded therefore that the discontinuity in

% = JAjiij can be a result of the form of the array
and a value of B z 0.8 leads to no discontinuity in rl*
which is the average nearest neighbour distance.

Discussion o~prL,~io#s experimental

X-l;,-?KiZ

SOLlDlFIED

ARRAY
l

$=,.OKiW$

Fig. 12.Schematic representatious of three different arrays

of points. k$ is the nearest aeighbour spacing for a cubic
array, 4 is for a hexagonal array, I$ is the average nearest
neighbour spacing for a random array. N is the number of
points in an area A.

@R. These three cases are illustrated schematically

in Fig. 12. The above expressions can all be written in
the form d* = B,/&@
where B depends on the
nature of the array.
It was observed that the c&~lar structure had a
well defined hexagonaI array whereas the dendritic
structure was much iess regular. These two cases are
illustrated by the micrographs of Figs 13(a) and (b).
Essentially the dendrites form a regular rectangular/
square pattern over small regions but there appears to
be little long range order. There is also considerable
evidence from the results of other workers [4,31 f that
these types of patterns arc generally observed.
It could be argued that what is important in an
analysis of the growth is the average nearest neighbour distance since this is the term which d&es the
diffusion distance. Thus when comparing results on
cells and dendrites the parameter rt*, defined as the
average nearest neighbour distance, should perhaps
be used.
For the hexagonal array of cells B = 1.075. The
value of B necessary to bring the dendrite measurements in Fig. 8 into the same fine as that for cells,
thus leading to no discontinuity in A*, is approximately 0.8. It can be seen that this value of B for
dendrites lies between the value of B for completely
random and the regular square array.

work

There has been considerable experimental work on

the measurement of primary arm spacings and most
of this has been reviewed by Hunt [24] and Klaren, et
al. [ll J. It is of interest, however, to compare our
results with the most recent work. This was carried
out by Klaren et al. [ll J on Pb-Sn and Pb-Au alloys.
The bulk of their results were obtained on lead-tin
alloys containing between 10 and 50 wt .% Sn.
As they pointed out the tin which is being rejected
is lighter than the bulk liquid and since the specimens
were frozen vertically upwards this means that the
density of the interdendritic liquid increases in the
vertical direction giving an unstable hydrodynamic
situation, It seems possible therefore that in these
experiments con~ion
currents occur in the liquid,
that these interact with the solute diffusion process
and affect the dendrite spacings. One would thus
expect little agreement between either their results
and those obtained in alloys in which a denser solute
is being rejected at the interface or the predictions of
a diffusion controlled model. Moreover as the growth
velocity is decreased convection will become relatively
more important in inserting
solute and it is not
unexpected that a critical velocity is observed below
which the spacing becomes independent of velocity.
Presumably at this stage convection has become the
dominant mass transfer mechanism.
Burden and Hunt [32] have in fact observed the
significant effect of convection on the dendrite spacings in the ammonium chforidewater system. They
found that ammonium chtoride dendrites grown vertically downwards had a much coarser spacing than
those grown vertically upwards. In the former case
the interdendritic density gradient was stable whereas
in the latter case it was potentially unstable.
The results of Klaren at al. [l l] on Pb-Au also
need to be treated with caution in that although there
is a stable vertical interdendritic density gradient,
ffuid flow of the type observed by Burden et al. [12]
(and described in the In~~uction) may still be occurring. This type of flow becomes serious when there is
a large density difference between the solute and soivent atoms, and when there is a large solute boundary
layer ahead of the dendrite type. Various workers
[15,33,34] have found that this boundary layer
depends on G/V where G is the temperature gradient
and V the growth rate.
Pb-Au is a system in which the liquid densities
differ considerably (liquid density of Pb = 10.68 x lo3
kg/m3 [35]; liquid density of Au = 17.36 x lo3 kg/m3
[35]) and so under conditions of high gradient and
IOW velocity significant fluid flow might be expected
and could account for the existence of a critical vel-

1862

MCCARTNEY

AND

HUNT:

DIRECTIONALLY

SOLiDPIED

ALUMINJUM

ALLOYS

(a)

Fig. 13. (a) Cell ular array in an Al-O.15 at.% Mg-0.33 at.% Si alloy. Magnification = 90x : . (b) Dendritic
array in an Al-O.63 at.% Mg-l.39at./0 Si alloy. Magnification = 75 x .

ocity below which thbe dendrite spacing is apparently

independent of rate.
In conclusion then the results of Kiaren et nl. [ 11J
must be treated wit1h caution because of the possibility of tluid flow in the bulk and interdendritic
liquid.

SUMMARY

AND Cf3INCLUSIONS

been obtained
in the ACMg-S i systern which exhibit little fluid flopw in the interden dritic
or bulk liquid, These have been obtained over a wide
Experimental

results

have

alloys of various compositions

MCCARTNEY

AND

HUNT:

DIRECTIONALLY

range of liquid temperature gradient, GL, growth velocity, V and alloy composition, C,. The parameter A,
which is a measure of the primary arm spacing has
been related to GL, V and C, using linear regression
analyses. It has been found that for dendrites the
relationship is of the form

where K is a constant and C,Si is the atomic percent

of silicon in the alloy. This shows good preliminary
agreement with the models presented by Hunt [24],
and Kurz and Fisher [25].
It has also been observed that the spacing relationship for cells and dendrites, for specimens grown from
alloys of the same composition, is discontinuous when
,I is taken as a measure of the primary arm spacing.
If, however, the average nearest neighbour spacing,
A*, is taken to be the important parameter in assessing cellular or dendritic growth instead of 1 (which
simply equals m)
then the discontinuous change
in I can be explained in terms of the different arrays
adopted by cells and dendrites. It has been shown
that A* = Bm
where the value of B depends on
the array. To eliminate a discontinuity in A* a value
of B for dendrites of 0.8 is required and this value
is between that for a square array and a completely
random array.
Acknowledgements-The
authors would like to thank Professor Sir Peter Hirsch F.R.S. for the provision of laboratory facilities which has made this work possible. One of us
(D. G. McC.) would like to acknowledge financial support
from the Department of Education for Northern Ireland.

SOLIDIFIED

ALUMINIUM

ALLOYS

1863

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(1971).
7. K. P. Young and D. H. Kirkwood. Mecull. Trans. A 6,

197 (1975).
8. T. Okamoto,

K. Kishitake and I. Bcssho, J. Cryst.

Growth 29, I31 (1975).
9. H. Jacobi and K. Schwerdtifeger, MadI Trans. A 7,
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IO. J. A. Spittle and D. M. Lloyd, Solidrjcation and Casting
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