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as solidified alloys
J. A. Spittle*
The generally reported observations pertinent to any proposed interpretation of the columnar to
equiaxed transition (CET) in as solidified alloys are initially considered. The review then proceeds
to consider the proposed mechanisms of equiaxed grain formation, the influence of alloy and
processing conditions on the CET, criteria for the termination of columnar growth and, finally,
deterministic/stochastic models for predicting the CET. In conclusion, the present level of
understanding of the CET and current modelling capabilities are summarised and assessed.
Published by Maney Publishing (c) IOM Communications Ltd
Introduction
As solidified metals (shaped castings, ingots, continuously cast alloys, directionally solidified materials,
welds, etc.) consist of grains (single phase or multiphase) formed during solidification by one or more of
the various types of phase transformation that can occur
on cooling, e.g. primary phase freezing from the melt,
eutectic solidification and peritectic transformation.
Subsequent to nucleation, these grains either continue
to grow preferentially in a direction normal to the
liquidus isotherm in the solidifying system (i.e. they
become elongated in one dimension and are termed
columnar) or they grow in suspension in supercooled
liquid (termed equiaxed).
To manufacture useful products, most alloys are
fabricated either by solid state deformation of simple
cast forms such as sheet, billet or slab (wrought alloys)
or by filling complex shaped moulds/dies with molten
metal (casting alloys). The as cast microstructures of
wrought alloys (which are often continuously or semicontinuously cast) consist predominantly of solid solution grains of the initial primary phase. However, this is
not always the case, e.g. in low carbon steels, the initial
primary phase d ferrite is transformed to single-phase c
austenite at a lower temperature. On the other hand,
casting alloys, in most alloy systems, often deliberately
contain large volume fractions of eutectic (e.g. aluminium and zinc-base alloys and cast irons). Therefore, if
the alloy compositions lie close to the eutectic value, the
microstructures will be dominated by eutectic grains
(cells). However, other casting alloys, e.g. hypoeutectic
AlSi alloys, may contain significant amounts of
primary solid solution phase.
In as solidified structures, growth of columnar grains
often terminates with the appearance of an equiaxed
zone or, possibly, a band of equiaxed grains (which then
undergoes a further transition back to columnar
Materials Research Centre, School of Engineering, University of Wales
Swansea, Swansea SA2 8PP, UK
*Email j.a.spittle@swansea.ac.uk
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G=RvmC0 (1k)=kD
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(1)
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2 Schematic series (ae) illustrating change of liquidus temperature and actual temperature in bulk liquid ahead of
advancing columnar front and origin of constitutional supercooling13
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Alloy parameters
Omni-directional freezing
(2)
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3 Variation of relative grain size of Al1 at.-% solute alloys as a function of parameter P 21
(3)
Unidirectional solidification
Instead of trying to experimentally quantify the influence of different alloy parameters on the CET, for a
given set of casting conditions, during omni-directional
solidification, an extensively used alternative approach
has been to try to determine the conditions existing at
the location of the CET for a given alloy system. Studies
of this type involve unidirectional solidification.
Plaskett and Winegard27 examined the unidirectional
solidification of AlMg alloys under non-steady conditions. The alloys were melted in situ in a graphite
crucible held in a furnace and directionally solidified
from a cooled chill. For each alloy, the values of G and
R were determined at the location of the breakdown of
columnar growth. Over the composition range investigated, 010%Mg, an almost linear relationship was
obtained between C0 and the value of G/R1/2 at
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4 Experimental
plot
illustrating
linear
relationship
between wt-%Sn and G/R for columnar to equiaxed
transition in PbSn alloys28
Spittle
form by heterogeneous nucleation ahead of the columnar front due to CS. Tiller predicted that the equiaxed
zone would form when the maximum undercooling
exceeded a critical value.
The significant renewed interest in the CET since the
1980s has resulted from the emergence of new modelling
approaches to investigate the transition which, as a
consequence, have prompted further experimental studies. The studies have been performed on a variety of
alloy systems and the data have often been compared to
the predictions of models. Alternatively, modellers have
used experimental data to assess the general validity of
their models.
Mahapatra and Weinberg30 and Ziv and Weinberg,31
using a 1D finite difference heat transfer model,
investigated the CET, under non-steady freezing conditions, for in situ melted and directionally solidified
alloys of Sn containing 5, 10 and 15 wt-%Pb and, Al
3 wt-%Cu, respectively. In the case of the SnPb alloys,
they reported that the CET occurred when the
temperature gradient ahead of the advancing dendrite
tips for each alloy fell below a critical value. The values
(which were determined from a finite difference heat
transfer model of the solidifying ingot) were 1.0, 1.1 and
1.3 K cm1, respectively. The CET could not be directly
related to dendrite tip velocity. For the Al3 wt-%Cu
alloy, the CET occurred when the gradient fell to
0.6 K cm1 which was found to be in agreement with a
gradient prediction from Hunts analytical model of the
CET (see the subsection Analytical models below).32
From adding different amounts of nominally Al5Ti1B
grain refiner to the AlCu alloy, it was found that a
definite amount was required in order to effect the CET.
They suggest this indicates that a critical high density of
nuclei is required to form a fine-grained structure.
Suri et al.33 again using a 1D heat transfer model to
determine the values of G and V at the positions of the
CET, studied Al4.5%Cu alloys directionally solidified
under non-steady conditions for different superheats
and conditions of heat extraction. They reported that
the transition occurred if
:
Gv0:74V 0 64
(4)
34
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Superheat
Numerous authors have reported that increasing superheat increases columnar grain length, i.e. suppresses the
CET (Fig. 7).13,19,4751 Although this is true for laboratory scale experiments, frequently performed on cylindrical cast shapes of less than 500 cm3 in volume, the
observation cannot be extrapolated to larger volumes.
Morando et al.50 examined the solidification of a
series of Al2%Cu cylindrical ingots, varying in volume
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Fluid flow
Investigations of the significance of fluid flow to the
CET have centred on two aspects. First, determination
of the influence of natural convection/pouring turbulence on the transition and, second, application of forced
flow to promote equiaxed grain formation. Much of this
work, which has been qualitative in nature, was carried
out by Cole and Bolling.19,48,49,54,55
Considering the role of natural convection, a variety
of techniques have been used to reduce/remove convection in the melt.19,47,49,50,56 Cole and Bolling inserted
grids across the mould diameter19 or slowly rotated the
mould about its vertical axis during solidification.49
Others have solidified alloys in a static magnetic
field,47,50,56 either applying the field at all times or, over
selected time periods during solidification in order to
differentiate between potential mechanisms of equiaxed
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stirring current at a fixed Si content. Electromagnetic stirring therefore promotes the CET.
Electromagnetic stirring resulted in the rapid removal
of the bulk liquid superheat and liquid velocities up to
0.25 m s1 were predicted. The investigators concluded
that their results support the contention that forced fluid
flow promotes the equiaxed region and the CET by
fragmentation of the solidifying front. The role of
heterogeneous nucleation was also investigated by
comparing ingots of Al2.5 wt-%Si made from base
materials of different purities solidified under conditions
of natural convection (no forced stirring). The equiaxed
zone in the higher purity alloy (lower Ti and B levels)
contained fewer and larger grains than in the commercial purity alloy. This suggested that, under conditions
of natural convection, the CET is influenced by the
number of heterogeneous nuclei. With stirring, the
number of heterogeneous nuclei becomes less important
because of the creation of dendrite fragments from
which growth of equiaxed dendrites can proceed.
Willers et al.58 carried out an experimental study to
investigate the influence of bulk flow in the melt on the
unidirectional solidification of cylindrical samples of
alloys of Pb and Sn. The bulk flow was generated by a
rotating magnetic field. The alloys studied were Sn
15 wt-%Pb, Sn38 wt-%Pb and Pb25 wt-%Sn. The
second alloy corresponds to the eutectic composition.
These compositions were chosen to provide different
density ratios between interdendritic liquid, bulk liquid
and primary crystals and, also, to provide an alloy
(eutectic) that is not subject to macro solute rejection at
the solidifying front or grows dendritically. The alloys
were preheated in cylindrical moulds 50 mm internal
diameter by 100 mm in height to a superheat of 90 K.
The alloys were then solidified upwards by placing the
mould on a water-cooled copper chill, the whole
assembly being located inside a magnetic inductor.
Stirring of the melt was initiated simultaneously with
the cooling. Temperatures were recorded along the
central axis of the cylinder and experiments were
conducted with variations of the magnetic field strength.
In the absence of a magnetic field, the alloys were
completely columnar. Melt agitation promoted grain
refinement. The present study revealed, in all cases
including the eutectic alloy, that increasing field strength
displaced the CET towards the bottom of the cylinder.
The CET appears for critical values of the cooling rate
of about 0.4 K s1 and for temperature gradients
between 0.6 and 1.0 K mm1. These are about an order
of magnitude greater than those reported for non-stirred
melts.30,40 Measurements revealed the existence of
remarkable temperature fluctuations in the mushy zone
lending support to thermal melting of dendrites. Solute
accumulation at a CET was considered to be responsible
for obstruction of columnar growth, in accordance with
Ref. 45, see the section Proposed mechanisms/criteria
for the termination of columnar growth below. The
origin and the effect of magnetic field strength on the
CET in eutectic alloys are unclear. It appears that
dendrite fragmentation and solutal interaction between
columnar and equiaxed growth cannot be responsible
and the investigators simply suggest that stirring leads to
a multiplication of nuclei.
In a continuation of the research described in the
previous paragraph using the same experimental
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Deterministic models
Analytical models
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(5)
(6)
and of the mean dwell time in the melt. The model does
not take into account the latent heat released by the
growing equiaxed grains. As stated in the section
Proposed mechanisms/criteria for the termination of
columnar growth above, they assumed that the criterion
for the CET was that an equiaxed grain had grown to
one-tenth of the spacing between two adjacent equiaxed
grains and that convective flow equalises the temperature in the bath and controls the heat transfer to the
solid shell. The model showed that two parameters
controlled the CET, undercooling of the interface and
the thickness of the undercooled layer.
Fredriksson and Olsson61 have used a similar
.
approach assuming, again, a velocity t0 5 relationship
for the columnar front, that the front undercooling is
dependent on velocity, that convective flow equalises the
temperature in the bath and that there are a specified
number of growing equiaxed crystals. They assume that
the equiaxed grains grow with a spherical shape, having
an internal solid fraction of 0.3, and that the growth rate
is dependent on the square of the undercooling. Their
model accounts for the latent heat evolved by the
equiaxed grains. However, the growth rate and undercooling of the columnar interface are not affected by the
growth of the equiaxed grains. Best values were chosen,
for a growth constant and the number of equiaxed
dendrites per unit volume, to give a best fit between a
measured cooling curve recorded at the centre of a steel
ingot and a curve predicted from the model. Both curves
displayed recalescence and, as stated in the section
Proposed mechanisms/criteria for the termination of
columnar growth above, they predicted that the CET
occurred at the time corresponding to the minimum
temperature preceding recalescence. Their model predicts an increase in the columnar zone the larger the
superheat, the smaller the number of free crystals, the
lower the solute content, the higher the cooling rate and
the greater the height and/or width of the ingot.
Flood and Hunt69,70 were the first to simultaneously
model the growth of both the columnar and equiaxed
grains. This was achieved using a 1D finite difference
thermal model. The model takes into account both
conduction and convection in the bulk, the latent heat
liberated by the equiaxed grains and the thermal
interaction between the solidifying columnar and
equiaxed grains. In this way, the velocity and undercooling of the columnar front are calculated dynamically
throughout the simulation and are not fixed a priori.
Convection is treated with a simple boundary layer
approximation, it being assumed that there is complete
mixing ahead of a conducting boundary layer and that
the bulk is isothermal. It is assumed that the velocities of
the columnar and equiaxed grains are governed by a
parabolic velocity undercooling relationship. The liquid
fraction in the columnar grains is assumed to be related
to temperature by the Scheil equation,71 truncated at
an undercooling determined by the heat flow at the
dendrite tips.69 The spherically shaped equiaxed grains
ahead of the columnar front either grow as soon as some
critical undercooling is exceeded or are nucleated at a
temperature dependent rate. The equiaxed grains are
assumed to be isothermal and to also have a solid
fraction governed by the Scheil equation. Equiaxed
grain impingement is allowed for using an Avrami
treatment and the CET is assumed to occur when the
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9 Comparison of data in Fig. 8 with that predicted from numerical model of Gaumann et al., where DTn is undercooling
at heterogeneous nucleation temperature, N0 is total number of heterogeneous nucleation sites per unit volume and
C0 is wt-%Cu80
10 Contours of equal grain size shown on plot of solidification velocity versus thermal gradient together with
locus for CET calculated from Hunts analysis2
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Stochastic models
Simulating the solidification of individual grains provides the potential for examining more precisely the
local conditions controlling the CET. Modelling at this
scale has, in more recent models, enabled the solution of
solute diffusion equations and microscopic tracking of
the movement of the solid/liquid interface of the grains.
This has removed the need to include dendrite tip
growth models for the grains and has resulted in the
simulation of dendritic grain morphologies that have a
realistic appearance. However, assumptions are still
required regarding the nucleation of the grains. The
models are also severely limited by the grain number
densities that can be handled in a simulation. The
significant feature of the models is that they are capable
of creating computed micrographs of grain structures
that closely resemble those found in castings, etc.
Various researchers have reported the use of 2D
stochastic models to simulate the evolution of grain
structures and the CET during solidification.
Brown and Spittle,83 using a Monte Carlo computer
simulation technique previously applied to a number of
solid-state processes such as recrystallisation and grain
growth, were the first to use the method for solidification
transformations. The technique employs a lattice of
sites, squares or triangles, which are initially designated
as liquid. The transformation of these sites to solid is
then simulated according to a set of rules governing
nucleation and growth. Individual grains are identified
and tracked during solidification and the final grain
structure can be drawn as a micrograph. Using
appropriate densities and locations of nuclei, realistic
pictures of CETs were generated (Fig. 11). The model
does not use real temperatures, actual phase diagram
parameters or any thermophysical properties data. It
was found that the CET occurred, in agreement with the
probabilistic argument of Hunt,32 when the actual
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CET in welds
Several reviews have been published that consider the
detailed relationship between solidification parameters
and weld structures9396 and one of these96 concentrates
on the CET. It is recognised that equiaxed grain
structures at the centres of welds would be of benefit
in reducing/eliminating susceptibility to centreline cracking. They would also improve the ultrasonic inspection
of certain alloys, e.g. austenitic stainless steels. In
practice, columnar equiaxed transitions are rarely
observed in welds and obtaining an equiaxed structure
is often not achievable or difficult to optimise.96 As
would be expected, equiaxed regions are found, if at all,
at the centreline where the solidification rates are fastest
and the temperature gradients lowest. The nature of
welding processes and the cooling rates involved (102
107 K s1) make quantitative experimental evaluation of
the CET virtually impossible. Also, because of weld pool
shape, care must be taken to ensure that an apparent
CET is real and that the equiaxed grains are not
simply transverse sections through columnar grains. The
mechanisms proposed to account for the CET (in the
absence of inoculants) are those previously suggested in
the section Mechanisms of equiaxed grain formation
for castings, with the added possibility of grain detachment in the partially molten region (see the section
Overall consideration of proposed mechanisms of
equiaxed grain formation above). Since the fusion zone
boundary in a weld is at the freezing temperature, weld
(7)
Summary
The probable origins of the equiaxed grains associated
with a CET (in the absence of added inoculants) are now
well defined and accepted. During solidification, one or
more of them will operate and which ones become active
or dominant will depend on factors such as cooling rate,
freezing time, the temperature distribution ahead of the
columnar front, thermal and constitutional supercooling, and the number and efficiency of potential nucleants
in the melt. In turn, these are governed by the alloy
system, the amount of solute present, section size, type
of solidification process (e.g. casting/welding/directional
solidification) and processing conditions (e.g. superheat,
mould temperatures, extent of fluid flow, etc.). It is
evident that the manner of termination of columnar
growth will differ according to the number and rate of
growth of the equiaxed grains and the degree of
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