Article

pubs.acs.org/IECR

Dynamical Analysis of Melt Flow in the Bridgman Process

Mojtaba Izadi, Youssef Belhamadia, and Stevan Dubljevic*,

Department of Chemical and Materials Engineering and Department of Biomedical Engineering, University of Alberta, Edmonton,
Alberta T6G 2R3, Canada

ABSTRACT: The Bridgman crystal growth process represents a prime example of a relevant industrial process in which uid
ow and mixing features impact desired process specications. In particular, we analyze the bulk mixing properties of the melt
ow in a vertical Bridgman process through the identication of Lagrangian coherent structures (LCS). The NavierStokes,
continuum, and heat transport equations are formulated in a mixed nite-element universal integration scheme to simulate the
multiphase problem using the nite-element method. The highly resolved time-varying accurate numerical solution of the
velocity eld is utilized to identify the transport barriers in terms of nite time Lyapunov exponent (FTLE) ridges whose
movements govern the mixing in the melt ow. The ridge structures are dynamically driven materials surfaces which provide the
insight into the eciency of mixing in two distinct operating regimes of the Bridgman crystal growth process.

1. INTRODUCTION
The dynamical analysis applied to uid ow systems has
attracted the interest of uid dynamicists and engineers for its
relevance in understanding fundamental uid ow features and
for providing practitioners with a new insight into a large
number of industrial processes (chemical, pharmaceutical,
petroleum, food). In particular, in the last two decades,
methods and quantities derived from dynamical system theory
emerged as Lagrangian or kinematic theory of transport and
mixing, and spread out as methodology to address features of
ow properties, laboratory equipment, static and stirred mixers,
and industrial-scale processes.1 One of the important crystal
manufacturing processes for the production and/or purication
of grown crystal is the Bridgman crystal growth process.
The Bridgman process is one of the common methods used
for the production of melt-grown crystals,2 where the material
is introduced in a crucible placed in a furnace. In the classical
vertical Bridgman method (see Figure 1), the upper zone of the
furnace has temperatures above the melting point of the
material and the lower zone with a temperature below melting
point separated by an adiabatic zone as a bae between the
two. The crucible is raised into the upper zone and solid
material is melted, possibly with a remaining nonmelted single-
crystal seed for the initiation of crystallization at the crucibles
bottom in the lower zone. After the temperature stabilizes, the
crucible is lowered slowly into the lower zone, so that the
crystal grows from the melt. In contrast, in an inverted
Bridgman process, the crucible is heated from the lower zone
and cooled from the upper zone of the furnace (see Figure 1).
In the melt-grown crystallization processes, thermal con-
vection of the melt ow plays an important role by aecting the
mixing properties, as well as the heat- and mass-transfer
phenomena.3 The consequence of incomplete mixing in the
melt is that a gradient of impurities concentration exists in the
melt near the grown-crystal/solid-melt interface.4 This aects
the crystal characteristics, such as compositional uniformity of
the grown crystal. In order to substantiate the inuence of the
melt ow on the grown crystal, Carruthers and Nassau,5 and
also Kobayashi and Arizumi,6 studied ow patterns and
stagnation surfaces that prevent complete mixing of the melt
in the crucible.
The Lagrangian coherent structures (LCS) approach, which
is conceptually formulated from the overlapping areas of
nonlinear dynamics and uid dynamics, is utilized in an analysis
of the bulk mixing of the melt ow in the Bridgman crystal
growth process. In other words, a novel way of understanding
transport in complex uid ows is given by identication of the
LCS structures that dene material transport across the
boundaries of the LCS structures over a selected period of
time. These structures are distinguished material lines, i.e.,
continuous smooth curves of uid elements advected by the
ow in a two-dimensional (2-D) space, that play the dominant
role in attracting and repelling neighboring uid elements.
Transport by material advection suggests the kinematic or
Lagrangian perspective of the uid ow description where

Received: July 30, 2014

Figure 1. Schematic conguration of the classical (left) and inverted
Revised: October 15, 2014
(right) vertical Bridgman process. Th and Tc are heating and cooling
temperatures, respectively. Accepted: October 17, 2014

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Industrial & Engineering Chemistry Research
individual uid elements are tracked as they are advected by the
ow through the ow domain. By contrast, the Eulerian point
of view considers the properties of a ow eld at each xed
point in space and time.
A detailed understanding of Lagrangian transport already
exists for time-independent ows such as the steady saddle-
point ow in Figure 2. Fluid parcels close to the saddle point
Figure 2. A (hyperbolic) saddle point in a time-independent two-
dimensional (2-D) ow, which constitutes the intersection of stable
(red) and unstable (blue) manifolds. A uid element close to the
saddle point on the two sides of the stable manifold (repelling LCS) is
drawn away along the unstable manifold (attracting LCS).
are drawn away from the stable manifold, that is the line of
owing material serving as a repulsive transport barrier, toward
a transverse unstable manifold, that is the material line
constituting an attractive transport barrier. The unstable
manifold acts as a core organizing structure in the vicinity of
the saddle point, attracting all nearby uid particles, which then
stretch out to adopt its shape. Also, one manifold (for > 0)
looks like the other with the time reversed (i.e., < 0).
In addition to steady ows, prominent material lines are also
known to exist in periodic and quasi-periodic ows, where they
serve as skeletons of observed tracer patterns. However, the
identication of dynamical skeletons for material patterns in
ows with complex spatial and temporal structure is an ongoing
challenge. Assuming that the velocity eld is observed for times
ranging over a nite interval, the LCSs of the ow during that
interval are the material lines that repel or attract nearby uid
trajectories at the highest local rate relative to other material
lines nearby. Overall, the repelling and attracting LCSs play
similar roles to the stable and unstable manifolds, respectively,
of the saddle point in Figure 2, where the repelling LCSs direct
particles to dierent domains of the attracting LCSs.
The framework of the dynamical systems theory to
demonstrate the existence of LCS as nite-time invariant
manifolds in the extended phase space for general time-
dependent ows is studied in the work of Haller and Yuan7 and
Haller.8 A pioneering insight into Lagrangian features of the
velocity eld data in these contributions is the landscape of the
nite time Lyapunov exponent (FTLE) eld. The Lyapunov
exponent is a scalar measure of how much initially adjacent
particles from a given location have separated. Regions of high
separation are locally of the strongest diverging ow.
Performing the same procedure in backward time, one
identies regions with high backward-time FTLE values with
strongest local convergence in forward time. The complex
patterns of FTLE distributions for physical ow elds were
connected to LCSs in ref 9, where the ridges of maxima in the
FTLE eld are dened as repelling LCSs in forward time and
attracting LCSs in backward time. This denition was later
explored by Shadden et al.10 and Lekien et al.11 in 2-D and n-
dimensional systems, showing that the ridges are almost
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Article
Lagrangian, i.e., the ux of the material across them is small. In
addition to nding LCSs from FTLE elds, Haller presented a
variational theory to identify LCSs that result in Lagrangian
material lines.12 Recently, the identication of these structures
has become an important tool for examining the transport
phenomena in uid mechanics, since they describe mixing
templates that govern the transport in a uid system (see the
works of Dabiri,13 Shadden et al.,14 Lekien and Ross,15 and
Izadi and Dubljevic16 for dierent applications). Although the
identication of the LCS structures denes objective indexes
(FTLE elds) that quantify the quality of the mixing process
within each of the invariant regions associated with the mixing
ow, it does not provide any information about how these
region-dependent indexes can be merged together to construct
some global measure of mixing in the entire ow domain. In
other words, the pure kinematic approach to the analysis of the
mixing templates in the Bridgman crystal growth process lacks
the presence of a diusive transport mechanism, and this
insight should be included in future research.
In this paper, we address the analysis of mixing features in
the melt ow in the vertical Bridgman crystal growth process
through the kinematic approach of identication of Lagrangian
coherent structures. In order to study the mixing templates of
the melt ow in the Bridgman process, a velocity eld is
obtained based on the mixed nite-element formulation of the
set of nonlinear governing equations, which include the
NavierStokes, continuity, and energy equations. Using the
obtained velocity eld data, forward and backward FTLE elds
for the uid ow system are computed to identify repelling and
attracting LCSs in the Bridgman crystal growth process. The
simulation and associated data reveal the relation between the
impurities distributions in two important operational settings of
the Bridgman crystal growth process. In particular, the two
process regimesone characterized with a low Rayleigh
number with two formed stable vortexes and less ecient
mixing, and another one characterized with a high Rayleigh
number and aperiodic uid ow and more ecient mixingare
presented from theoretical and practical perspectives.
2. FORMULATION
Kaenton et al. study the transition ow regimes for the
solidication of gallium in an inverted vertical Bridgman
conguration.17 Depending on the Rayleigh number (Ra),
steady symmetric ow with two counter rotating cells, steady
asymmetric ow with one dominant cell, symmetric periodic
motion with one or two frequencies, and asymmetric quasi-
periodic and nonperiodic regimes are reported for the 2-D
Cartesian melt ow simulation.
2.1. Governing Equations. Following the same geometry
as that given in ref 17 and shown schematically in Figure 3, a
velocity eld in the melt is obtained in this work for pure
gallium whose thermophysical properties in solid and liquid
states are the same. The uid is assumed to be Newtonian
incompressible, and the Boussinesq approximation is consid-
ered. The governing equationsincluding the NavierStokes,
continuity, and energy equationscan be written in a
dimensionless form as
v g
+ vv = Pr (v) p + Av + RaPr T
t g (1)
v = 0 (2)
Industrial & Engineering Chemistry Research Article

0 if T < Tf

= F (T ) =
1 if T > Tf

(4)

In applications, phase change is not always instantaneous and

may occur in a small temperature range [Tf , Tf + ]. The
relationship for F(T) can thus be replaced by a regularized
function F(T).
2.2. Finite Element Model. Solving the system dened by
eqs 14 is a challenging task. In this paper, we adopted the
numerical method used in Belhamadia et al.,18 which consists of
using a mixed formulation for NavierStokes (see eqs 1 and 2).
The nite-element discretization is based on quadratic
polynomials (written by using a hierarchical basis) for the
velocity and linear (continuous) polynomials for the pressure.
Using the test functions (u,q), the variational formulation can
be written as

Figure 3. Geometry of the inverted Bridgman process: W and L are vt u + (vv)u d

the width and height of the crucible and LT is the length of the
isolated bae. + (Pr vu pu A()vu) d

g
T 1 = RaPr Tu d
+ v T + (T ) = 0 g
t Ste t (3)


qv d = 0
where v is the velocity, p the pressure, and T the temperature.
The Boussinesq approximation, in common use, is used to A mixed formulation is also employed for the energy (see eqs
describe the melts convective motion. In the classical 3 and 4). The nite-element discretization is based on quadratic
Boussinesq model, the buoyancy term varies linearly with the polynomials for both temperature T and phase change variable
temperature and is given by RaPr(g/g)T. . Using the test functions (uT,u), the corresponding
The dimensionless formulation is obtained by using W as the variational formulation can be written as
scale factor for the length, W2/ for the time, /W for the
velocity, and 2/W2 for the pressure. Pr, Ra, and Ste are
dimensionless parameters. Pr is the Prandtl number, which is Tt uT + (vT )uT d + Ste1 t uT d


dened as
+ (T uT ) d = 0
v
Pr =


( F(T ))u d = 0
Ra is the Rayleigh number, which is dened as
In all our numerical simulations, a fully implicit backward
g(Th Tc)W 3 second-order scheme is used for time discretization. For
Ra = instance, given approximate solutions Tn1, Tn, and Tn+1 at
v times tn1, tn, and tn+1, respectively, the time derivative at time
Ste is the Stefan number, which is dened as tn+1 is approximated by
T n + 1 3T n + 1 4T n + T n 1
cp(Th Tc)W 3 (t )
Ste = t 2t
L
Therefore, the overall algorithm for solving the proposed model
In these dimensionless parameters, is the thermal expansion is described as follows.
coecient, the thermal diusivity, the kinematic viscosity, (1) Starting from (Tn,n), the solutions (vn+1,pn+1) are
and L the latent heat. The specic heat (cp) and the density () obtained by solving the system
are assumed to be equal in the liquid and solid phases. A is
dened as n+1
4v n + v n 1


3v 2t
u d

(1 )2
A = a 3
+b ((vn+1vn+1)u + Prvn+1u) d
+

+ ( p(n + 1) v A(n)v(n + 1)u) d
where b = 106 is a constant introduced to avoid division by
zero and a = 1015. In the uid domain (l), A is zero and has g (n)
= RaPr T u d
no inuence. However, in the totally solid region (s), A has a g
large value and forces the velocity to be zero. The function is
a phase change variable that satises a simple algebraic equation qvn+1 d = 0
of the form

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Industrial & Engineering Chemistry Research
and the Newtons method is used to solve for the zeros of a
large nonlinear system of algebraic equations.
(2) Starting from (vn+1,pn+1), the solutions (Tn+1,n+1) are
obtained by solving the system
(n + 1)
3T 4T (n) + T (n 1)
uT
2t
+
(v (n + 1)
T (n + 1)
)u T d
1 3(n + 1) 4(n) + (n 1)
Ste
+ uT d
2t
+
(T (n + 1)uT ) d = 0
(
(n + 1)
F(T (n + 1)))u d = 0
with Newtons method being used to obtain the solution.
(3) Return to step (1).
2.3. Lagrangian Coherent Structures. The standard
formulation of the Lagrangian Coherent Structures (LCS)
identication methodology usually assumes a general time-
dependent uid ow problem. Namely, the stationary uid ow
systems reveal time-invariant LCS structures, while periodic or
fully time-varying ows with possible transfer to chaotic ows
depict more interesting features of the LCS evolution. In the
following discussion, we describe the method of extracting the
LCS using the method of nite-time Lyapunov exponents
(FTLE). In particular, since the FTLE method is a kinematic
approach, we must compute a ow map that maps the particles
forward in time along their trajectories. Dierentiation of the
ow map will provide a measure of separation of two nearby
particles advected by the ow, so that we identify the LCS to be
a material surface in the ow on which separation is locally
maximal.
Let the uid ow system be considered as a dynamical
system of the form
dx
= v(x , t ), x(t0) = x0
dt
with x denoting the position in the uid domain, given as
x 1 n and the smooth velocity eld v(x,t) being dened
over the uid domain l. The system given by eq 5 is evolved
over a time interval of t = [t0,t0 + ]. Solution of the system
described by eq 5 is the trajectory x(t;x0, t0) of a particle at time
t initially (i.e., at t = t0), located at x0. By xing the initial time t0
and the nal time t of the dynamical system evolution, the ow
map tt0 is dened as the map which takes the point from its
initial position x0 in the uid domain at time t0 to its nal
position x in the uid domain at time t:
tt : l l : x0 tt (x0) = x(t ; x0 , t0)
0 0
The ow map, in essence, encodes the Lagrangian or kinematic
paths of the particles used to capture the local stretching in the
ow by which the particles are advected. By considering at time
t0 a point located at x0 l, which is advected by the ow to
tt00+ after a time interval , the symmetric nite-time Green
deformation tensor is obtained and dened by the following:
Ctt00+ = (tt0+ )tt0+ (7)
0 0
with two real positive eigenvalues in the case of 2-D uid ow
1(x0, t0, ) 2(x0, t0, ) and associated eigenvectors
Article
1(x0,t0,), 2(x0,t0,). The deformation tensor is positive
denite; therefore, it has positive eigenvalues. For the linearized
ow, if an innitesimal perturbation to the trajectory is dened
by x0, after the time interval , maximum stretching of this
perturbation occurs when x0 is aligned with 2(x0, t0, ) and
max x(x0 , t0 , ) = 2(x0 , t0 , ) x0
x0 (8)
where x0 is aligned with 2(x0,t0,). The aforementioned
expression for the maximal stretch perturbation of the uid
element (eq 8) can be written as
max x(x0 , t0 , ) = e t0
t0+
(2x0) | |
2(x0 , t0 , )
x0 (9)
where
1
tt00+ (x0) = ln 2 (x 0 , t 0 , )
| | (10)
where the tt00+(x0) represents the (largest) nite-time
Lyapunov exponent (FTLE) over integration time . Generally,
from the kinematic point of view, the FTLE scalar eld
describes how many particles initially located at x0 separate
after time interval by being advected by ow.
The Lagrangian coherent structures (LCSs) are dened as
ridges of the scalar FTLE eld.10 This implies that the intuitive
notion of the ridge suces to identify LCS; however, Haller
provided counterexamples for the LCSs dened as FTLE
ridges.12 In refs 12 and 19, variational theory is presented based
on the denition of the LCS as locally the strongest repelling or
attracting material surface. In this theory, the mathematically
given sucient and necessary conditions for extraction of LCS,
in terms of eigenvalues and eigenvectors of the Green strain
tensor eld, are presented. Application of these criteria to 2-D
ows denes an LCS as an one-dimensional (1-D) material
surface that is approximately normal to the eigenvector eld
associated with the largest eigenvalues of the Green strain
(5)
tensor eld. Therefore, the (hyperbolic) LCS is the strongest
repelling or attracting surface among all nearby material
surfaces. To dierentiate among repelling and attracting ones,
the repelling LCS at time t0 are obtained for going forward in
time ( > 0), while attracting LCS at t0 are obtained for going
backward in time ( < 0). In addition, Farazmand and Haller
provided a computational algorithm to capture the LCS in a 2-
D ow.20 The identication of the LCS is a useful tool to
provide assessment of transport uxes across the LCS
structures. In particular, integration of uxes over the LCS,
which is given by
(6) (t ) = LCS ddLt ds (11)
where the integral is taken over the length of the LCS, where
L(x,t) is the LCS material line (surface), which is obtained as
the level set L(x,t) = 0 and provides insight into quantitative
transport features.
In addition, as it will be demonstrated in the Results and
Discussion section, the intersection of repelling and attracting
LCS reveals a homoclinic tangle, and the time evolution of the
LCS describes the continuous motion of the lobes dened by
these intersections. In other words, some regions of the uid
are transported by the mechanism of lobe dynamics.
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Industrial & Engineering Chemistry Research
3. RESULTS AND DISCUSSION
In the general formulation, the nondimensional parameters that
dene the problem are given in Table 1 with the associated
Table 1. Nondimensional Parameters
parameter magnitude
Prandtl number, Pr 0.01
Stefan number, Ste 1 Ra value would be more desired; however, the problem is that
L/W 2 the thermal gradients across the same height of the solidied
LT/W 0.25
values used in this work. Theses parameters represent pure
gallium, whose properties in solid and liquid phases are the
same, and have been taken from ref 17, where the solidication
of this material in an inverted Bridgman apparatus have been
investigated. The computational domain is the rectangle [0,1]
[0,2]. A 64 128 grid is used for the simulation. Since we
use quadratic discretization, this grid leads to 74 691 and 66 306
degrees of freedom for the NavierStokes equation and the
continuity and energy formulations, respectively. Initial
conditions for the simulations include stationary uid with
temperature Th and solid with temperature Tc with a at
interface and Ra is applied at t = 0, leading to evolution of the
solution with a nondimensional time step of t = 6.8 104.
In order to compute the ow map and deformation tensor, a
discrete uniform grid of computational points over the melt
domain is dened. A rule of thumb is that the computational
grid for the FTLE eld should be ne enough to account for
the high FTLE growth rate near the LCS.10 Therefore, the
point uid element at each grid point in the computational
domain is advected by the ow map over the time interval
resulting in the ow map tt00+. The uid element trajectory is
determined from the velocity data (provided by the solution of
the nite-element model) using a fourth-order RungeKutta
explicit integration algorithm. For spatial interpolation of
discrete velocity data standard linear nite element interpola-
tion functions are used, while the gradients of the ow map
were computed by nite dierencing. Having the 2-D ow map,
computation of the deformation tensor and corresponding
eigenvalues is straightforward.
Figure 4 shows representatives of FTLE elds for dierent
Rayleigh numbers. As can be noticed, the numerical simulation
reveals two dierent processing congurations of the Bridgman
growth process. The rst one, which is less temperature and
heat-transfer intensive and is characterized by the lower
Figure 4. Representative backward FTLE eld for Ra = 4.5 104 and
= 150t (left) and forward FTLE eld for Ra = 106 and = 20t
(right).
Article
Rayleigh number (Ra = 4.5 104), yields a relatively uniform
planar (straight line) interface between solidliquid and
formation of two similar vortexes coexisting within the melt
domain. In contrast, the more thermally intensive process given
by the higher Rayleigh number (Ra = 106) is characterized by
the more intensive heat transfer, and yields completely time-
varying aperiodic ow with the parabolic type of solid/melt line
interface. From the crystal growth practitioner view, the higher
crystal are very large and may impact the grown crystal quality.
In other words, the material point at the solid/melt interface
and at x = 0.5 and corresponding solidied material points
along the horizontal direction and at the same height generate
very large temperature gradients, which might be detrimental
for the grown crystal. In this sense, there is a tradeo between
the mixing and the quality of produced grown crystal.
Along the same line, when the processing crystal operational
conditions favored a less-intensive process, Figure 5 depicts a
sequence of the attracting (blue) and repelling (red) LCS for
Ra = 4.5 104 for which ow regime is characterized by
symmetric partition of two vortexes. There is an LCS at the
symmetry line, as is expected, at which repelling and attracting
LCS material lines almost coincide. Another attracting LCS is
formed at the lower part of the crucible, and the repelling LCS
formed below the liquid/solid interface and expanded toward
the sides and bottom of the crucible; then, it moves downward
(see Figure 5). Since there is no melt ow across the LCS,
because of transport barriers, the movement of the LCS shown
in Figure 5 governs the mixing of the melt in a symmetric, less-
intensive thermal regime.
Figure 6 shows a sequence of attracting LCSs (denoted by
blue lines, which are obtained by integrating the ow map
backward in time) and repelling LCSs (denoted by red lines,
which are obtained by integrating the ow map forward in
time) for Ra = 106, for which the ow regime is asymmetric and
fully time-varying. Since the magnitude of velocity vectors is
larger than that in the previous case (Ra = 4.5 104), the
integration time () is smaller. In general, the value for is
selected in such a way that uid element separations reveal the
desired dynamics of the uid system.10 For this ow regime,
mixing is better accomplished, because of the fact that, initially,
the melt ow pattern is not symmetric and the middle LCS
does not exist. In this case, the dynamic lobe is formed and
mixing takes a set of particles by the ow from one side of the
crucible to the other one (see Figure 7), and, later, more
intersections of the lobe set occur, which characterizes
observable LCSs using the degree and extent of the melt
mixing.
4. CONCLUSION
In this paper, we demonstrate a novel approach for under-
standing the interplay between geometric features and
dynamics of mixing in the melt ow in the vertical Bridgman
process. In particular, the nite-element discretization of a
mixed formulation for the NavierStokes equation, and
continuity and energy balances, provide highly resolved velocity
data. These data are used to identify Lagrangian coherent
structures (LCSs) as ridges of the nite-time Lyapunov
exponent (FTLE) eld, representing time-dependent transport
barriers to the ow. The presence of attracting and repelling
LCSs in the melt during the Bridgman process shows the
existence of material surfaces that govern the mixing template
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Industrial & Engineering Chemistry Research
Figure 5. A sequence of attracting LCS (blue lines) and repelling LCS (red lines) for Ra = 4.5 104 and = 150t shown at t = 800, 925, ...,
1300t.
Figure 6. A sequence of attracting LCS (denoted by blue lines) and repelling LCS (denoted by red lines) for Ra = 106 and = 20t shown at t =
1101, 1104, ..., 1337t.
Figure 7. A sequence of attracting LCS (denoted by blue lines) and
repelling LCS (denoted by red lines) for Ra = 106 and = 20t,
which are enclosed by the red and green lobes, which evolve from one
side of the domain into another with constant intersections, with
attracting and repelling LCSs.
of the melt. Incomplete mixing of the melt results in
nonuniform distribution of the material in the manufactured
crystal. This fact highly aects the physical properties of the
product, which have signicant importance in the semi-
conductor industry.
AUTHOR INFORMATION
Corresponding Author
*E-mail: Stevan.Dubljevic@ualberta.ca.
Notes
The authors declare no competing nancial interest.
F dx.doi.org/10.1021/ie503030z | Ind. Eng. Chem. Res. XXXX, XXX, XXXXXX
Article
ACKNOWLEDGMENTS
The authors thank the anonymous reviewers for their valuable
comments and suggestions to improve the quality of the article.
Financial support by Natural Science and Engineering Research
Council of Canada (NSERC), through Discovery Grant No.
386508-2011, is gratefully acknowledged.
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