J Mater Sci (2012) 47:3706–3712
DOI 10.1007/s10853-011-6219-8
Density and thermal expansion of liquid Al–Si alloys
Julianna Schmitz • Bengt Hallstedt •
Jürgen Brillo • Ivan Egry • Michael Schick
Received: 9 August 2011 / Accepted: 19 December 2011 / Published online: 14 January 2012
Ó Springer Science+Business Media, LLC 2012
Abstract The density of Al-rich liquid Al–Si alloys was
measured contactlessly on electromagnetically levitated
samples using optical dilatometry. Data were obtained for
samples covering compositions up to 50 at.% Si and in a
temperature range between 650 and 1500 °C. The densities
can be described as linear functions of temperature with
negative slopes. Moreover, they increase monotonically
with an increase of Si concentration. In a temperature range
between 1100 and 1400 °C, it can be deduced from the
composition dependence of the density that virtually no
excess volume arises during alloying of the pure elements.
For lower temperatures an excess volume is discussed,
considering the temperature dependence of Si density lit-
erature data. The density data were integrated in a ther-
modynamic model description of the Al–Si system. In this
way volume changes during solidification and changes in
phase equilibria as function of pressure can be calculated.
Introduction
Motivation
Ternary Al–Cu–Si alloys are technologically widely used as
lightweight casting alloys due to their good castability,
J. Schmitz (&)  J. Brillo  I. Egry
Institut für Materialphysik im Weltraum, Deutsches Zentrum
für Luft- und Raumfahrt (DLR), 51170 Cologne, Germany
e-mail: julianna.schmitz@dlr.de
B. Hallstedt  M. Schick
Materials Chemistry, RWTH Aachen University,
52074 Aachen, Germany
123
processability, and mechanical strength, which can be fur-
ther improved by heat treatment or additive elements [1].
In practice, mainly Al-based alloys are employed, which
contain small amounts of the other alloying components and
additives. However, there are also some investigations
dealing with Si richer alloys. These studies focus on
solidification [2–5] or thermodynamics [6–12] of the binary
or the ternary alloy [13, 14]. Those liquids’ thermophysical
properties have hardly been studied [15, 16].
To anticipate and optimize casting processes, a funda-
mental understanding of solidification is essential. Models
with a quantitative prediction capability are needed, based
on the thermodynamics of these processes. Using a
CALPHAD approach [17] the Gibbs free energy can pro-
vide this basis. If the Gibbs energies were accurately
known, all other thermophysical properties could be cal-
culated from basic thermodynamic relations. Vice versa
Gibbs energies can be determined from sound thermody-
namic data. However, for this approach to work, it is not
sufficient to explore the Al-rich part of the phase diagram
only; a strategy for covering the entire phase diagram must
be developed.
Of particular interest for solidification is the knowledge
of the density of the alloy melt. When these density data
are available, volume changes during solidification and
cooling can be calculated. This is a prerequisite for realistic
casting simulations and simulation of macro-segregation.
For the fairly small number of binary systems investi-
gated experimentally, the excess volume has been found to
be in the order of a few percent of the total volume and no
correlation has been found so far with e.g., excess enthalpy
(i.e., enthalpy of mixing). The excess volume is, thus, in
the same order of magnitude as the volume change
during solidification. Therefore, measured volumes, and in
particular excess volumes, are important.
J Mater Sci (2012) 47:3706–3712
Since the expected excess volume is only a few percent,
it is necessary to access as large part of the composition
range of the considered system as possible to gain highly
accurate measurements.
For ternary systems these data are generally sparse and
even data of binary alloys are often missing. Hence, our
objective is to systematically develop a reliable thermo-
dynamic dataset, first for the binary Al-alloys before
addressing the ternaries.
In the liquid Al–Cu system, density and surface tension
data have already been reported [18, 19], viscosities are in
preparation. With this article, we continue working on the
densities of Al–Si, which were measured contactlessly in
electromagnetic levitation (EML), a method which enables
us to handle high melting and reactive materials.
Density and molar volume of binary mixtures
Within a temperature interval, (T-TL), which is small
enough, the density, q(T), of a liquid metal can be con-
sidered as a linear function of temperature, T:
qðTÞ ¼ qL þ qT ðT  TL Þ ð1Þ
Here, TL is the liquidus temperature, qL is the density at TL
and qT its temperature coefficient qq/qT.
From these quantities, the volume expansion coefficient
b ¼ V1 oV
oT can be calculated:
q where G is the Gibbs energy, P is the pressure, P0 the
b¼ T ð2Þ
qL
In multicomponent mixtures, the different elements usually
establish additional interactions among each other. This is
the reason, why in alloying not only the sum of the
weighted molar volumes of the pure components, i, has to
be considered, but also an excess volume, which accounts
for these interactions.
In a binary liquid system (i = 1, 2) the molar volume, V,
can be written [20].
X
2
Mi
V¼ xi  þ VE ð3Þ
i¼1
qi
The molar volumes of the pure components are here
written by considering the molar masses, Mi, of each
component and their densities, qi, at a certain temperature.
These are weighted by the atomic concentrations xi.
Deviations of V from ideal mixing behavior are included by
the excess volume, VE. That means, for VE = 0 Eq. 3 is a
simple linear combination of pure component molar vol-
umes and describes an ideal mixing without volume
change.
From Eq. 3 the composition dependence of the binary
system’s density is deduced:
3707
P2
M xi  Mi
qðxi Þ ¼ ¼ P2 i¼1 M ð4Þ
V i¼1 xi  q þ V
i E
i
In most cases, VE does not vanish. When atoms are of similar
size and have no preferred coordination with either similar
or different atoms, they are stochastically distributed in the
solution. In this situation, the temperature and composition
dependence of VE can be split by an approximation, which is
symmetric in the alloy composition [20, 21]:
V E ðx1 ; x2 ; T Þ ¼ x1 x2 V0 ðTÞ ð5Þ
Here, the composition dependence is incorporated in the
product of the atomic concentrations xi (i = 1, 2) of the
alloy components. Hence, the whole system can be
described by a coefficient V0, which is a function of tem-
perature, but independent of composition.
Thermodynamic modeling
Volume data are usually not included in thermodynamic
databases so far. In the form of Eqs. 3 and 5, they can
easily be added to existing thermodynamic model
descriptions. To each Gibbs energy parameter in the ther-
modynamic description a term of the form (P–P0)V is
added;
GðP; TÞ ¼ GðTÞ þ ðP  P0 ÞV; ð6Þ
normal pressure (1 bar) and V the volume. The thermo-
dynamic description of the Al–Si system from Feufel et al.
[22] was used. Volume data for solid and liquid Al and Si
from [23] and excess volumes from the present work were
added to this description. The data for liquid Al were
adjusted to match the evaluation of Assael et al. [24]. The
modified volume used for liquid Al is V = 9.9044 ?
1.548 9 10-3T cm3/mol, where T is in K.
Experimental
Electromagnetic levitation (EML)
Experiments were performed in a stainless steel high vac-
uum chamber described in detail elsewhere [25, 26]. It was
evacuated to 10-7 mbar and then filled with 750 mbar Ar
(purity: 99.9999 vol.%). The pre-alloyed sample was
positioned in the center of a levitation coil to which an
alternating current of typically 300 kHz and about 200 A is
applied. Its inhomogeneous electromagnetic field induces
eddy currents inside the electrically conductive sample.
The forces arising from interaction of these currents with
the field levitate the sample stably against gravity.
123
3708
A detailed consideration of the EML-principle is given in
literature [27].
Beneficial effect of the inherent ohmic losses of these
currents is the heating and melting of the sample, which is
realized simultaneously with EML. As levitation and
heating are coupled, a certain desired temperature can only
be adjusted within narrow limits by changing the levitation
power. During our measurements, the forced cooling in a
laminar flow of Ar or even He gas could be avoided, since
reducing the levitation power was sufficient to cool the
samples to the desired temperatures. Only for solidification
additional cooling by He gas flow was needed.
The measurement procedure is to start at a certain lev-
itation power at high temperatures and reduce the power
stepwise to reach lower temperatures. Measurements are
then performed in thermal equilibrium.
The sample temperature is measured by an infrared
pyrometer. As the emissivity is generally not known, the
pyrometer output signal, TP, has to be recalibrated using
the known liquidus temperature, TL, of each sample as a
calibration point. For most liquid metals, the emissivity
within a limited wavelength band is almost independent of
the temperature [28]. Hence, for calibration a constant
emissivity within the operating wavelength range of the
pyrometer can be assumed. The exact calibration procedure
is described, for instance, in [29].
Optical dilatometry
Densities of the liquid droplets are determined by taking
side view shadowgraph images and calculating its volume
at different temperatures. The technique is thoroughly
described in [25].
In principle, the levitated sample is illuminated from the
back side by an expanded HeNe-laser beam. An interfer-
ence filter removes thermal radiation of the sample and a
pinhole eliminates scattered nonparallel light rays from the
beam. The images are recorded by a CCD-camera and
analyzed by an edge detection algorithm to determine the
edge curve of the 2D-projection of the sample. In order to
evaluate the liquid sample volume, 3D-information must be
gained from these images.
The surface of a levitated droplet performs oscillations
around its rest position, which is axially symmetric to the
symmetry-axis of the electromagnetic field providing the
levitating force. Since not every oscillation mode is sym-
metric to this axis, a single frame is not necessarily axially
symmetric, when it does not incidentally capture the rest
position of the sample. In averaging over 1000 of these
frames, these oscillations (usually in the order of 50 Hz)
are eliminated and one obtains an edge curve, which is
symmetric to the vertical sample axis [25]. This curve is
then fitted by Legendre polynomials and gives the sample
123
J Mater Sci (2012) 47:3706–3712
volume, when it is integrated over space assuming
rotational z-axis symmetry:
Zp
2
VP ¼ p \RðuÞ [ 3 sinðuÞdu ð7Þ
3
0
Here, R(u) is the fitted average 2D-edge curve and u is the
polar angle. The sample volume, Vp, is only obtained in
pixel units. It must be calibrated to the real volume, V, by a
comparison to reference volumes, which is also described
in [25]. From the mass, m, of the processed sample the
density is calculated, provided evaporation during the
measurement was negligible.
Sample preparation
Samples with a diameter of about 6 mm were made of Si
and Al metal with a purity of 99.999% (metals basis). Mass
adjustment and surface cleaning was achieved by pinching
off pieces and ultrasonic treatment. Despite the contact
with crucible material, the samples needed to be pre-
alloyed within an arc melting furnace, since otherwise the
solid semiconducting Si could not have been processed in
EML. Alloying was completed in the EML apparatus by
heating the samples to about 1500 °C. At the same step,
oxygen contaminations were removed by keeping the
sample at this temperature until no bright oxide spots could
be observed on the surface. After this alloying procedure
and the subsequent experiment, the mass loss of the about
300 mg samples was less than 3 mg. If this evaporation
affected only one component (Al), the change of the alloy
composition would amount 0.2 at.% at most. For compar-
ison and to check the reproducibility of the data, also
samples prepared in vacuum induction melting and in
electron beam melting were measured. The inductively
molten samples were obtained from our cooperation part-
ners in Jena1, the electron beam samples from Clausthal.2
Results
Measurements were performed at temperatures, where
evaporation was negligible. Levitation became more and
more unstable, the colder the samples got and the more Si
they contained. Hence, a limited temperature interval was
accessible, which, however, is quite broad for most sam-
ples (800–1400 °C).
1
M. Rettenmayr, A. Löffler, Institut für Materialwissenschaft und
Werkstofftechnologie, Friedrich-Schiller-Universität Jena, 07743
Jena, Germany.
2
R. Schmid-Fetzer, J. Gröbner, Institut für Metallurgie, TU Claus-
thal, 38678 Clausthal-Zellerfeld, Germany.
J Mater Sci (2012) 47:3706–3712 3709

Table 1 Fit parameters for the

Sample TL, °C qL, g cm-3 qT, 10-4 g cm-3K-1 b, 10-5 K-1
density and thermal expansion
of each of the investigated Al 660 2.36 ± 0.01 -3.0 ± 0.1 12.8 ± 0.1
Al–Si samples. The samples,
denoted by FSU or TUC were Al88Si12 576 2.46 ± 0.01 -2.1 ± 0.1 13.1 ± 0.3
obtained from Jena (see Al80Si20 697 2.44 ± 0.01 -2.3 ± 0.1 8.9 ± 0.1
footnote 1) or Clausthal (see Al70Si30 831 2.37 ± 0.02 -1.6 ± 0.2 6.8 ± 1.0
footnote 2), respectively
Al70Si30 (FSU) 831 2.40 ± 0.02 -1.7 ± 0.2 7.0 ± 0.9
Al70Si30 (TUC) 831 2.39 ± 0.02 -1.8 ± 0.2 7.0 ± 0.7
Al60Si40 (TUC) 952 2.42 ± 0.01 -2.9 ± 0.1 11.9 ± 0.3
Al50Si50 (TUC) 1061 2.46 ± 0.03 -3.2 ± 0.2 12.9 ± 1.0

The measured densities are displayed in Fig. 1. They
can be fitted linearly by Eq. 1. The obtained densities qL at
liquidus temperature, TL, and the slopes of the curves
(temperature coefficients), qT, are compiled in Table 1 for
each measured sample. There, also the volume expansion
coefficient, b, is calculated from Eq. 2.
Literature data of the pure components are denoted as
dashed lines in Fig. 1. The literature data for Al [23] were
adjusted to match those of [24] in temperature interval
660–920 °C. The ones of pure Si [23, 30] remained
unmodified. The data in [23] (dashed line in Fig. 1) are
fitted using a linear temperature dependence of the volume.
The measured Al-densities fit the reported data quite
well, except for the values measured above 1450 °C.
There, a steeper slope arises, leading to lower density
values. This effect must be due to evaporation of sample
material during measurement at these elevated tempera-
tures. In this temperature region, the mass loss of 3%
disturbs recalibrating sample volumes to densities with the
processed sample mass. Below 1450 °C no evaporation
occurs, so the mass during the lower T measurements stays
constant.
Measurements were started at high temperatures and
data were acquired after subsequent cooling steps. This
means that at high temperatures evaporation leads to a
change of sample mass between different data points. Later
on, at lower temperatures, no evaporation occurs, and the
sample mass stays constant. Since these data are evaluated
using the mass of the processed sample, the lower tem-
perature densities are determined correctly, while the val-
ues at higher temperatures are underestimated. For this
reason, recalibrated densities of Al up to 1450 °C are
reliable and only these data are evaluated in the linear
fitting.
In all the data of the other samples, where the overall mass
loss was less than 1%, this effect does not occur. In these
cases, the major evaporation was during the alloying and
surface cleaning step at more elevated temperatures. Hence,
for these samples the recalibration by the processed sample
mass is valid throughout the whole measurement range.
At first glance the value of the Al80Si20 sample seems to be
quite high. But the composition dependence depicted in
Fig. 2 visualizes that this scatter is within the small uncer-
tainties of the measurement principle which are of 1% [25].

Fig. 1 Density of liquid Al–Si versus temperature. The solid lines

represent linear fits to the data. The samples denoted by FSU or TUC Fig. 2 Composition dependence of the liquid Al–Si density at
were obtained from Jena (see footnote 1) or Clausthal (see footnote 1200 °C. The pure component data were taken from literature [23,
2), respectively. For comparison, literature data [23] (partly combined 24, 30]. The lines represent fits of Eq. 5 to the data, giving an excess
with [24], see text) of the pure components are also depicted volume, VE, of zero

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3710 J Mater Sci (2012) 47:3706–3712

The same holds for the Al70Si30 alloys, where we

compared samples created by different methods. Within the
measurement uncertainties, density values are the same.
The completely homogeneous samples, obtained from our
project partners, levitated more stably from the beginning.
The pre-alloyed samples only became stable after they
were heated above the melting temperature of pure Si. For
this reason, only fully alloyed initial samples were used for
Si-contents above 30 at.% .

Discussion

In Figs. 2, 3 and 4, the composition dependence of q is

depicted at different temperatures, together with literature
Fig. 4 Composition dependence of the liquid Al–Si density at
data [23, 24, 30] of the pure components. The density 800 °C with the extrapolated pure component data from literature
increases monotonically with increasing Si-content. The [23, 24, 30]. Considering the different existing datasets of Si, both fits
considered density range between pure Al and Si is quite to the data are equally good. In either case the excess volume, VE,
does only differ little from zero
narrow and scatter of the data is within the measurement
uncertainties of only 1%.
In Figs. 2, 3 and 4, the composition dependence of the
For liquid Si, there are two classes of datasets [23, 30].
alloy density is fitted by Eq. 4. The black lines are reduced
Starting from quite similar density values above TL, one
v2-fits to the data using one Si dataset [23] the grey curves
dataset [23] observes a linear behavior during undercooling
employ the other [30]. The full lines represent fits, where
to about 1100 °C. The other [30] reports a T2-behavior
qAl, qSi, and VE were varied. These fit parameters are
within the same temperature region and extrapolates a
compiled in Tables 2 and 3. As a guide to the eye, VE was
maximum around 900 °C.
set to zero in the dashed line fits.
Since our measurements were performed in this under-
The main difference in the fits originates from the single
cooled temperature range of pure Si and it is not trivial to
Si-datapoints. The fits start to deviate from each other at Si
select between those reported data, we checked the
extrapolations of both datasets with regard to composition- Table 2 Fit parameters for the excess volume and densities of Al and
dependent volume effects during alloying. Si at different temperatures, utilizing pure metal data from Ref. [23]
T, °C V0, cm3 mol-1 qAl, g cm-3 qSi, g cm-3

800 0.5 ± 0.6 2.31 ± 0.03 2.79 ± 0.03

900 0.6 ± 0.6 2.31 ± 0.03 2.74 ± 0.03
1000 0.2 ± 0.5 2.26 ± 0.02 2.70 ± 0.03
1100 0.0 ± 0.5 2.24 ± 0.02 2.66 ± 0.02
1200 -0.1 ± 0.3 2.21 ± 0.02 2.62 ± 0.01
1300 -0.2 ± 0.4 2.19 ± 0.02 2.58 ± 0.02
1414 -0.3 ± 0.4 2.17 ± 0.02 2.54 ± 0.02

Table 3 Fit parameters for the excess volume and densities of Al and
Si at different temperatures, utilizing pure Si data from Ref. [30]
T, °C V0, cm3 mol-1 qAl, g cm-3 qSi, g cm-3

800 -0.6 ± 0.4 2.30 ± 0.03 2.63 ± 0.04

900 -0.1 ± 0.6 2.30 ± 0.3 2.63 ± 0.04
1000 -0.3 ± 0.5 2.26 ± 0.02 2.63 ± 0.03
Fig. 3 Composition dependence of the liquid Al–Si density at
1100 -0.2 ± 0.4 2.24 ± 0.02 2.62 ± 0.02
1000 °C with the extrapolated pure component data from literature
[23, 24, 30]. There, in the undercooled region of Si different behavior 1200 -0.2 ± 0.4 2.21 ± 0.02 2.62 ± 0.02
is discussed and considered in the evaluation of our data. The lines 1300 0.0 ± 0.4 2.20 ± 0.02 2.60 ± 0.02
represent fits of Eq. 5 to each of the datasets. With the second, a slight 1414 0.01 ± 0.4 2.17 ± 0.02 2.58 ± 0.2
deviation of VE of from zero might occur

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J Mater Sci (2012) 47:3706–3712
concentrations of about 50 at.%. The Al50Si50 data seem to
be slightly higher than the fits, implying higher values for
Si-rich alloys. Since we focused on the Al-rich side of the
alloy, no final statement can be given about the Si-rich
densities.
Comparing fits with adjustable VE and those with
E
V = 0, one might observe slight differences between
them, intensifying with decreasing T. But even at 800 °C
the deviation of the measured molar volume from the ideal
one is only in the order of 2%, which is more due to the
scatter of the data. In Fig. 5, the temperature dependence of
the fitted VE is evaluated, considering V0 from Eq. 5.
There, for both of the evaluated Si-densities, V0 virtually
vanishes considering its uncertainty.
The observed simple additivity of molar volumes in the
Al–Si system implies comparable nearest–neighbor inter-
actions regardless of the kind of atoms involved. In literature
[15], at temperatures 20 K above TL and Si contents higher
than 40 at.%, a virtually instantaneous change in the average
coordination number of the Al–Si alloy atoms was observed
by neutron diffraction. This was explained by formation of
tetrahedrally coordinated Si atoms only in the Si-rich liquid.
For Si concentrations below 40 at.% the average coordina-
tion of the atoms stayed almost constant and decreased
to another constant value upon increasing the Si content by
10 at.% to 50 at.%. The mean distance of atoms within the
pure liquids and the alloys was comparable.
Considering this, for low Si contents, an ideal mixing
seems plausible. In case the Si tetrahedral short-range order
should establish in Si-rich Al–Si alloys, the atomic inter-
actions within the system cannot be equal. Against this
background the observed ideal mixing is not trivial and
should be examined in more detail by extending density
measurements to alloys with higher Si-contents.
Fig. 5 Temperature dependence of VE, visualized by the coefficient
V0 fitted with different Si densities [23, 30]. The dashed line is placed
at zero. Within the uncertainties, V0 and VE equal zero
3711
2.70
Al-6Si
2.65
2.60
Solid
2.55
[g/cm3 ]
2.50
2.45
2.40
Liquid
2.35
2.30
2.25
0 200 400 600 800 1000
T [°C]
Fig. 6 Calculated density as function of temperature for an Al–6
at.% Si alloy
Using the thermodynamic description for Al–Si includ-
ing volume data (with zero excess volume) with the
modified Gibbs energy expressions according to Eq. 6, the
density as function of temperature can be calculated with
standard thermodynamic software such as Thermo-Calc
[31] for any composition, including any phase transfor-
mations, such as solidification. An example for an Al–6
at.% Si alloy is shown in Fig. 6. Including volume data in
the thermodynamic description means, that pressure
dependence of the Gibbs energy is incorporated. This can
be used to calculate phase equilibria as function of pres-
sure. In Fig. 7, the Al–Si phase diagram is calculated at
different pressures. Such calculations can be considered
reasonably accurate at moderate pressure. High pressure
differences in compressibility, which is currently not
modeled, will lead to deviations from reality of such
‘‘simple’’ calculations. For pressures above about 1 GPa
(10 kbar), depending on material, it is probably necessary
to consider the compressibilities to reach acceptable
accuracy.
Summary
The density and thermal expansion of liquid Al–Si alloys
was determined experimentally as a function of tempera-
ture and composition up to Si-concentrations of 50 at.%.
The density can be described by a linear combination of the
pure metals’ molar volumes and hence, no pronounced
excess volume was found. On the other hand, there are
experiments [15], suggesting strong interactions in Al–Si
melts with Si-contents above 50 at.%. Addressing densities
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3712 J Mater Sci (2012) 47:3706–3712

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Acknowledgement Within the framework of PAK 461 this study 24. Assael MJ, Kakosimos K, Banish RM, Brillo J, Egry I, Brooks R,
was financially supported by the ‘‘Deutsche Forschungsgemeins- Quested PN, Mills KC, Nagashima A, Sato Y, Wakeham WA
chaft’’ under grant numbers EG 93/8-1 and HA 5382/3-1. This is (2006) J Phys Chem Ref Data 35:285
gratefully acknowledged. Further, we would like to thank our coop- 25. Brillo J, Egry I (2003) Int J Thermophys 24:1155
eration partners Rainer Schmid-Fetzer, Joachim Gröbner, Markus 26. Brillo J, Egry I, Giffard HS, Patti A (2004) Int J Thermophys
Rettenmayr, and Andrea Löffler for sharing their expertise and for the 25:1881
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Mat Prod Tech 26:247
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