Preliminary study on multiscale optimal control: Chemical

Deposition Reactor
Estudio preliminar en control ptimo multiescalar: Reactor de
deposicin qumica
David Esteban Bernal-Neiraa, Federico Lozano-Santamaraa, Watson Lawrence VargasEscobara & Jorge Mario Gmez-Ramreza
a

Departamento de Ingenera Qumica, Universidad de los Andes, , Colombia. de.bernal531@uniandes.edu.co, f.lozano396@uniandes.edu.co,

wvargas@uniandes.edu.co,jorgomez@uniandes.edu.co
Received:

Abstract
The dynamic optimization of multiscale systems requires the appropriate and efficient integration between the models of the different
scales, as the description of discrete and continuum phenomena. The optimal control of a chemical vapor deposition (CVD) reactor using
a multiescalar model to describe the phenomena present in the system is studied in this article. The gaseous phase is modelled by
differential balances that make a system of partial differential equations (PDE) and the surface phenomena are modelled using a
kinematic Monte-Carlo (kMC) simulation. The flow of information between the models is bidirectional and is given by the boundary
conditions on the substrate surface. With this representation of the problem the injection velocity and the surface temperature as time
functions are obtained. The results obtained are the ones that allowed the film height with minimal rugosity.
Keywords: Multiscale optimization; optimal control; kinematic Monte-Carlo simulation; chemical vapor deposition reator.
Resumen
La optimizacin dinmica de sistemas multiescalares requiere la integracin apropiada y eficiente entre los modelos de las diferentes
escalas, como la descripcin de fenmenos continuos y discretos. En este trabajo se estudia el control ptimo de un reactor de deposicin
qumica de vapor utilizando un modelo multiescalar para describir los fenmenos presentes en el sistema. La parte continua de la fase
gaseosa se modela por medio de balances diferenciales que forman un sistema de ecuaciones diferenciales parciales; mientras que los
fenmenos de la superficie se modelan por medio de una simulacin cinemtica de Monte-Carlo. El flujo de informacin entre los
modelos es bidireccional y se da en las condiciones de frontera presentes en la superficie del sustrato. Con esta representacin del
problema se obtiene la velocidad de inyeccin de sustrato en funcin del tiempo y la temperatura de superficie, las cuales permiten
alcanzar altura de pelcula deseada con mnima rugosidad.
Palabras clave: Optimizacin multiescala; control ptimo; simulacin cinemtica de Monte-Carlo; reactor de deposicin qumica.
1 Introduction
The transport phenomena have been usually seen from the
macroscale, where the conservation equations are applied over
black boxes, or the mesoscale point of view, that considers the
matter as a continuum and applies the conservation equations over
differential elements of matter making a system of partial
differential equations. In certain cases, these levels of description
may not be enough for certain application in chemical engineering,
which have inherent discrete characteristics as the emulsions,
suspension, porous media, surface phenomena, advanced material
processing and nanotechnology applications. On the other hand,
the transport phenomena in molecular or microscopic scales
consider the discrete characteristics of matter in an atomic,

molecular or molecular clusters level [1]. The processes in

microscopic scales may be modelled by molecular dynamics,
where one solves the Newton motion equations associated to the
multiple bodies under intermolecular or interatomic forces defines
by an interaction potential; kinematic Monte-Carlo evolution, that
selects the execution of different events based on probability
distributions that are related to the occurrence frequency of the
events defined pf physical parameters; among others [2].
Nevertheless, the application of these models requires a high
computational load which makes almost impossible its application
for studying phenomena of a larger scale (meso/macro scale),
leaving the multiescalar integration as a possible choice that allows
to describe with a higher precision specific parts of the studied
system using models of different scales in time and/or length.

The authors; license Universidad Nacional de Colombia.

DYNA

Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

The way the different scales are coupled is the main limit of
the multiescalar study of different processes because there is not a
systematic and valid way to do it [1, 3]. One way to integrate the
different scales is using reduced order models or models obtained
by data fitting that allow relating the variables from the different
scales [4]. Although these fitting models relate the variables of the
microscale and the mesoscale in the operations ranges where they
were determined, the physical description of the phenomenon and
the capacity of predicting the behavior of the process outside the
fitting range are lost.
This multiscale approximation in order to model the processes
leads to consider the operation, design and control problems using
optimization algorithms. Nevertheless, its application is not direct
because of the difference in the lime and length scales, besides of
the high computational cost associated with the microscale models.
Because of this, the coupling between the different scales must be
done in an efficient way with a bidirectional flow of information
so that the optimization is not limited by the computational
demand of a large-scale problem [5]. The mesoscale processes are
described using partial differential equations (PDE) that after being
discretized using finite differences, finite elements of collocation
methods lead to large scale algebraic problems. These problems
can be solved using deterministic nonlinear gradient-based
optimization algorithms. The microscale description can not be
included directly into the large-scale problems because of its
stochastic nature and the high computational cost that is required
by only one integration step. On the other hand, by using an in-out
model for the microscale, determined outside of the optimization
algorithm, the limitation of the multiscale optimization is
overcome provided that polytopic restrictions are added in the
states to guarantee the validity of the fitted model [6].
The modelling and multiscale dynamic optimization of the
film growth phenomenon in a chemical deposition vapor (CVD)
reactor is studied in this article.
The section 2 presents a theoretical revision about the present
phenomena in the CVD reactor and about multiescalar
optimization. The section 3 describes the modelling in the
mesoscale and the microscale of the reactor, the approximation
used to relate these two scales and the study case proposed to
analyze this phenomenon. The section 4 describes the dynamic
optimization problem, the handle of the PDE and the objective
function. The results obtained are discussed in the section 5 and
the last section concludes the study.

exposed to one or more volatile precursors which react in the

substrate surface in order to produce the desired deposition.
Because of the versatility of the CVD processes there is a wide
range of possible products. Among these products there are two
large application areas, the semiconductor industry and the
metallurgical coatings; whose applications may cover from
electrical, optical, mechanical and chemical uses [7]. As prominent
examples are the production of silicon wafers with or without
doping for the microelectronic industry, coatings of synthetic
diamond for utilization of this material properties which without
this technology would be economically inviable [8, 9], among
others.
The factors that control a CVD process are the
thermodynamics, kinetics, mass transport, chemical reaction and
process parameters such as pressure, temperature and chemical
activity. Most of the CVD processes can be classified as thermic
CVD processes, although recently several variations of it have
emerged such as the plasma CVD, the laser CVD or the photo
CVD. The main difference between these kinds of processes is the
application method of the energy required for the CVD reaction to
take place.
The thermic CVD requires that the necessary energy for the
CVD reaction activation is by means of temperature, which is
between 500 and 2000C according to the necessary application.
The reactor used for this process can be classified as closed (batch
production, generally used for coatings) or open (with continuous
flow of reactants); of hot walls (where the whole reactor is heated
to the necessary temperature) or of cold walls (where just the
substrate is heated); and of low pressure operation or atmospheric
pressure operation [7].
The plasma, laser and photo CVD are innovative versions of
the thermic CVD where using energy transfer method different to
temperature gradients, the reaction is supplied with the energy to
be conducted. These different versions offer advantages compared
to the traditional thermic CVD (lower operation temperatures and
precision of deposition writing) but are still on development
phases and their actual cost make them attractive just for very
specific cases.
2.2 Multiscale optimization
The modelling and for instance the optimization of the CVD
reactors involves two scales of length. The microscale includes the
response variables as the deposited amount, the deposition rate and
the surface rugosity. The measurable variables (e.g. injection
velocity, operation temperature) or design variables (e.g. rotation
velocity, number of injectors) belong to the mesoscale. The
optimization of multiscale processes; either with design, operation
or control objectives; is limited by the size of the model or by the
stochastic nature of the microscopic models.
The integration of the multiple scales is often made using
reduced order models in order to simplify the optimization
problem [6]. These models are a simplification of the original
detailed models that are still able to keep the physical description
of the phenomenon until certain level pf precision. The order
reduction may be carried by several different ways, among them
two stand out: reduction of the number of equations from the
original model and reduction of order directed by data [4, 10]. In
the first case a simplified model is developed so that it retains the
structure of the original equations in order that it generates a more
efficient and less expensive representation of the detailed original
model. Among the methods to reduce the order of PDE systems
one can name: multi grid methods and proper orthogonal
decomposition [11]. The second approximation leads to the
construction of a substitute model in four steps: a) selection of a
design of experiments for the data acquisition, b) selection of a

2. Theoretical framework
The topic of this article is the optimal control of a CVD
reactor. For instance, in the next section the theoretical framework
of such kind of reactors and of multiescalar optimization will be
developed. As mentioned before, the phenomenology of this kind
of process requires the integration of phenomena in molecular
scales (that are mainly the surface phenomena in the reactor) and
continuum scales (that include the reactor momentum, mass and
energy transport along the reactor). The first part of this section
will develop the description of CVD reactors and the next part of it
will focus on the multiscale optimization.
2.1 Chemical vapor deposition (CVD) reactors
The chemical vapor deposition (CVD) process is a chemical
process used to produce solid materials of high purity and
performance. This kind of process is very versatile and allows the
production of coating, powders, fibers and monolithic components
of practically any metallic and non-metallic material such as
carbides, nitrides, oxides, carbon and silicon compounds, among
others [7]. In a typical CVD process, a wafer of substrate is
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Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

representation model, c) data fitting to the observed data, and d)

validations and verification of the model. Nevertheless, this
approximation requires a high off-line computational demand [4].
The usage of reduced order models in the multiscale
optimization does not guarantee that the optimal solution of the
original detailed model is found because the gradient information
does not match, which just guarantee first order optimality
conditions to be satisfied for the detailed model. In order to tackle
this difficulty adaptive strategies can be used, which can be
compared with the closed-loop operation of a controller, using
filters or other additions to match the gradients of the reduced and
the original models [12]. Another choice is using methodologies
that correct the reduced order model on-line. This on-line
correction is being made in every iteration of the optimization
algorithm, like for example the optimization in a trust-region
scheme with the gradients of the detailed model [4] or the in-situ
adaptive tabulation [2]. Nevertheless, these options require the
periodic evaluation of the original model in order to correct the
reduced model. This can be avoided if the reduced models have the
characteristic of being -exact. An -exact model is the one where
the absolute difference between the gradients of the two models is
inferior to a specified tolerance [4].

The reaction to be carried in the surface is described in the eq.

(1).
(1)
SiH4 Si + 2H2
This reaction is irreversible and for temperatures between 1000
and 1040C generates epitaxial silicon although between 650 and
1100C generates polycrystalline silicon. Among the applications
of the epitaxial silicon are the integrated circuits and other
semiconductor devices. The polycrystalline silicon is used in
thermal and mechanical sensors, and in photovoltaic cells [7].
The simulated reactor in this study case is a CVD reactor with
axial symmetry described schematically in the Figure 2. This
reactor has as feed stream a mixture of silane and molecular
nitrogen (inert) and over the surface is carried that dissociation
reaction of silane into silicon and hydrogen where the silicon
deposits over the surface. The temperature of the substrate can be
manipulated using the heaters under it. The reactor disposition is
based on the work of Christofides, et al [14].

3 Modelling and description of the study case

In the development of this article the study case chosen is a
chemical vapor deposition reactor used for the production of
polycrystalline or epitaxial silicon from silane in a thermic, open
low pressure operation and cold walls CVD reactor. The silicon is
a semiconductor material called as the structural material of the
current electronic industry. It has a tetrahedral crystalline structure
(as the diamond) and its properties are strongly influenced by this
structure [13].
3.1 General model
The epitaxial wafer layers, where the crystalline structure of
the substrate is equal to the one of the layer above it, have superior
transmission layers, but its application is limited by the high
deposition temperatures (higher than 1000C). Despite of the
numerous silicon precursors under hydrogen-rich atmospheres
(SiH4, SiH2Cl2, SiHCl3 or SiCl4) the silane SiH4 has been chosen
because of the reported larger wafer growth under high
temperatures [13] as shown in the Figure 1.

Figure 2. Schematic of the simulated chemical deposition reactor

Based on: Christofides, (2008)

The description of a CVD reactor requires multiscale models.

From the modelling point of view, the major challenge is the
integrations of the large range of scales of length and time that the
process requires. Specifically in the gaseous phase, it is needed to
model the behavior of mass, momentum and energy transfer
according to a continuum model describing for example the
temperature into the reactor chamber and the concentration of the
different species there. On the other hand by studying the
microstructure of the surface the molecular adsorption, desorption
and migration phenomena become important and the length and
time scales reduce drastically.
Although the two different models are required, there is an
important interaction between them; for example the concentration
of the precursor in the feed stream has an effect over the
adsorption rates on the surface, or the desorption rate affects the
concentration of the precursor in the continuum phase. In order to
integrate both models it has been decided to carry a multiscale
integration. As shown in the Figure 2, the continuum simulation of
the reactor will be made for almost the whole domain and the
concentration and temperature parameters are provided to the
microscopic simulation, which returns boundary conditions for the
macroscopic simulation.

Figure 1. Ahrrenius plot for the vapor deposition os silicon using different
precursors.
Source: Pearce, (1983).

3.2 Continuum model

A partition in time and space was performed in order to
discretize the differential equations describing the continuum
simulation. From this discretization three sets arise, which
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Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

determine the description of the equations. Apart of these three

sets, there is another set that contains the substances involved in
the reaction. In the general case one has:
= {0, , }: Set of radius finite elements.
(2)

temperature

= {0, , }: Set of length finite elements.

(3)

= {0, , }: Set of time finite elements.

= {0, , }: Set of substances.

Continuity equation
1

( ) + ( ) = 0
+

3.2.2 Energy equation

( +

+ )

2
= [
(( )) + 2 ]

( , , , ) = 0; = 0; = {0, , }:
symmetry
= ; { , , }; = :
Side
temperature
= ; { , , }; = :
Upper

(21)
(22)
(23)
(24)

The geometrical and operation parameters used for the

modelling of the reactor are reported in the Table 1.
Table 1.
Geometrical and operation parameters used for the CVD reactor [14].
Parameter
Amount
2 in
Reactor radius
1.5 in
Substrate radius
1.5 in
Feed inlet radius
3 in
Distance from the substrate to the feed inlet
Reactor pressure
0.1 atm
300 K
Feed temperature
300 K
Wall temperature
0.6
Silane feed mole fraction 4,
0.4
Nitrogen feed mole fraction 2,
80 cm/s
Feed velocity 0

(6)

(7)

(8)

The transport and thermodynamic properties were obtained

with the software Aspen Properties.

(9)

3.2 Microscopic model

The las boundary condition is the one tha couples the macro
and microscopic models. The function of concentration and
temperature on the surface must be determined using molecular
models. The model used in this article has three different
controlling steps: adsorption of molecules from the gaseous phase
to the surface, desorption of molecules from the surface to the
gaseous phase, and migration of molecules in the surface. These
processes are schematically showed in the Figure 3.

(20)

= 0; = ; = {0, , }: Side wall heat isolation

the substrate interphase.

3.2.3 Mass balance per component

(
+
+
)

2
(10)
= [
((
)) + 2 ]

.
The resolution of this set of differential equations is subject to
certain boundary conditions described below.
= 0 ; {0, , }; = : Feed flow.

(11)
(12)
= ; { , , }; = 0: Effluent flow
= 0; { , , }; = : No-slip upper wall
(13)

(19)

= 0; { , , }; = : Upper Wall heat

isolation

= 0; = ; = {0, , }: Solid (without mass

transfer) side wall

= 0; ; { , , }; = : Solid (without mass

transfer) upper wall

= , (, , ): Mass flow in

= 0; = ; = {0, , }: No-slip side wall

= , ; {0, , }; = : Feed composition

(5)
By solving the equations of the continuum phase the values of
temperature, concentration and velocity will be found inside the
reactor. Each one of them will depend on its position and moment
of time. In order to determine the value of these variables the mass,
momentum and energy conservation equations will be solved.
Because of the symmetry of the system, the analysis is reduced
into a two-dimensional analysis, such that the conservation
equations are:

Motion equation in the longitudinal direction.

(
+
+
)

2
=
+[
( ( )) + 2 ].

(18)

(4)

3.2.1 Equations of motion

Motion equation in the radial direction.

(
+
+
)

1
2
( )) + 2 ].
=
+[ (

= ; {0, , }; = : Feed temperature

(14)
Axial

(15)

wall

(16)

wall

(17)

Figure 3. Schematic of surface microscopic controlling steps

In the construction of this model the supposition that the

growth in different layers exist was made. It was also supposed

Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

that each site is available for the adsorption, making the adsorption
rate independent of the site.
According to the kinetic theory of gases, for an ideal gas, the
adsorption rate is:
0
=
(25)
22
Where s0 is the sticking coefficient, is the Botzmann
constant, the partial pressure of the precursor, is the total
concentration of sites in the surface, is the molecular mass of
the precursor, is the temperature of the gaseous phase just over
the surface and is the strain rate.
To model the desorption, the local microenvironment of the
molecule and its local activation energy must be considered. Under
the consideration of only first-nearest neighbors interactions, the
desorption rate is given by:
0

(26)
=
exp ( )
2

Where is the energy of a single bond, the number of

considerable neighbors in the microenvironment and 0 is the
frequency of the events, determined by:

(27)
0 = 0 exp ( )

Where 0 is an event-frequency constant and is the

energy associated with desorption.
Finally the migration in a surface is modelled as a desorption
followed by a readsorption, where the migration rate is given by:
0

(28)
=
exp ( )
2

Where is the difference of energy associated to the one

that a molecule must overcome to move from one lattice site to an
adjacent one. This difference is given by:

(29)
= exp (
)

Where is the energy associated to the migration.

This sort of process is determined as stochastic because the
place and time of the events is unknown and the only known
feature is the probability that these events may occur. Given this
case, this process can be modelled as a Poisson series of events,
which have as valid suppositions that the occurrence probability of
an event in independent of the events that happened in the past and
from the events that happen in a not infinitesimal time difference.
The probability of an event happening in an infinitesimal time
differential is equal to where is the mean counting rate of
the event and the probability that other event happens in the same
time differential is negligible.
With these supposition emerges the master equation of a
stochastic process, which one seeks to solve by the proposed
model. That equation states that:
(, )
= (, ) (, )
(30)

For the simulation of a thin film in a superficial microstructure

a kMC model described below.
An squared grid is defined so that it satisfies periodic boundary
conditions. The molecules that are on the surface will be classified
in 5 groups, according to the number of first-nearest neighbors at
the same height (0, 1, 2, 3 or 4). The choice of the happened event
is given by logic tests evaluated over a random generated number.
In order to generate the logic tests, the total rates for each
microprocess must be determined by the following way:
= 2
(31)
4

; = ()

(32)

; = ()

(33)

=0
4
=0

Where the subscripts , and are referred to adsorption,

desorption and migration respectively, is the rate of each
microprocess, the total rate of each microprocess, the grid
size analized and the number of molecules in the lattice of each
kind.
With the rated calculated, a random number between 0 and 1
is generated, which enters into the following logic tests:

If 0 < <
then a molecule is adsorbed.
(34)
If

+ +

+ +

desorbed.
+
If

<

+
+ +

then a molecule is

(35)

< 1 then a molecule migrates.

(36)
After determining the controlling step that will happen, in
the case of the adsorption a random place on the lattice is chosen
to determine where the molecule will be absorbed. For the
desorption, a random number will be generated in order to
determine the class of molecule that will be desorbed and then
another random number will determine which of the molecules of
this class will be desorbed. In a similar way, a random number will
determine which molecule will migrate in the case it had to and
then randomly a direction of migration will be determined.
Once the event is determined, the increase in real time is
calculated by the following equation:
ln
(37)
=
+ +
Where is another random generated number between 0 and
1.
Finally, the classes into the lattice must be updated and the
kMC simulation must be continued until reaching a stopping
criteria, which was determines as an amount of events.
The parameters used for the modelling of this system are
reported in the Table 2.
+ +

Table 2.
Parameters used for microscopic simulation [14]
Parameter
Precursor molar mass
Precursor diameter
Strain rate
Sticking coefficient 0
Single bond surface energy
Desorption event-frequency constant 0
Desorption associated energy
Migration associated
Lattice size

Where and are system configurations, that for this

specific case is the height of each lattice site, and is the
probability of occurence of a transition event between a
configuration and a configuration .
The model mentioned above is based on the work made by
Christofides, et al [14].
Due to the large number of configurations and variables, the
direct resolution of the master equation is practically impossible,
for instance a model that approximates its solution must be used.
The selected model is a kinetic Monte Carlo (kMC), where the
events are created through Monte Carlo simulations that follow the
probability function based on the same suppositions necessary to
find the master equation.

Amount
32.06 g/mol
3.7*10-10m
5 1/s
0.1
0.74 eV
1.86*106
0.74 eV
0.4608 eV
50

As output parameters the microscopic simulation has the

following variables as time, temperature and pressure functions:

Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

: Total number of molecules on the lattice. [-]

(38)

: Average Surface height.[]

(39)

= max (
=

()2

): Rugosity constant. []

: Growth rate. [/s]

(51)
= 0 ; = {0, , }; = {0, , } .
The temperature profile is defined by the gradient of the
temperature between the surface and the feed inlet and
does not have radial effects. The walls of the reactor are
heated in such way that the radial temperature gradients
are avoided.

2
( ) = [
(52)

].

(53)

( ) = 0.
2

(54)
=
>0

1 exp()
(55)
=
+ 2

( = 0) = = 1 + 2 2 = 1 .
(56)
1 exp( )
( = ) = =
+ 2 1

(57)

=
1 exp()

exp (
)

() =
+

1 exp (
)

(58)

1 exp (
)

Radial temperature in the Surface boundary

1

(59)
0 = [
(( ))].

(60)
( ) = 0.

= 1 ln + 2
(61)
( = ) = 2 = 1 ln .
(62)
( = ) = 2 = 1 ln .
(63)


() =
ln +
.
(64)

ln
ln

Under these suppositions, the mesoscale phenomenon

description is reduced to the mass transfer equations in steady
state, compared with the original detailed model with the mass,
momentum and energy dynamic balances to be solved
simultaneously.
In order to solve the optimization problem with Non Linear
Programming (NLP) algorithms it is necessary to discretize the
partial differential equations so that a large scale algebraic problem
is obtained. This makes possible to exploit the dispersion and
structure of the PDE problems [11, 12]. Finite differences are used
so that the first order derivatives are represented as in eq. (65) and
the second order derivatives are represented as in eq. (66).
( + ) ()
(65)

2
( + ) 2() + ( )
(66)

2
2
The equality constraints of the optimization problem are the
reduced order models corresponding to the reduced order by
physical simplifications model in the mesoscale and the reduced
order directed by data model in the microscale. The inequality
constraints correspond to the operation conditions shown in the
section 3, which are basically polytopic constraints in the rugosity
and temperature states. The manipulated variables in this problem

(40)
(41)

Where is the number of molecules in each site of the

lattice.
4 Formulation of the optimal control problem
The general formulation of a dynamic optimization problem
may be represented as:

min = ( ) + ( (), (), ())

s.t.

(42)

= ( (), (), (), )

(0)

= 0

( (), (), (), ) = 0

(43)
(44)
(45)

( (), (), (), ) 0

(46)
Where the subscript represents the differential variables
and the subscript the algebraic variables. The objective function
is composed by two terms, a terminal cost ( ) and a mobile
cost, represented in the integral, which takes into account the time
variations.
According to the section 2.2 is not possible to include
directly the microscale model that describes the growth of the
surface by the molecule deposition because of it stochastic nature
and its large computational times. In order to tackle this problem a
reduced order model directed by data is constructed in order to
substitute the original detailed model. The design of experiments
used for the construction of the model consists in a factorial design
where the factors are the temperature and the partial pressure of
the precursor, both limited by the conditions described in the
section 3. The response variables are the change in the surface
height, the growth rate and the surface rugosity. The models used
for the phenomenon description have the form of the eq. (47) and
will be determined by the minimization of the quadratic error.
However, the rugosity depends on the surface configuration,
meaning the amount of particle adsorbed in the last time, making
necessary the use of another approximation as the one in eq. (48)
in order to consider this factor.
= + + +
(47)
(48)
)(, ) (,) + (, )
= (,
Where is any of the following variables: change in the
surface height, growth rate and number of molecules in the lattice.
The description of the phenomena that happen in the
mesoscale is made through a PDE system presented in the section
3. In order to reduce the problem size, the next suppositions are
applied [15].

Pseudo-stable state: The phenomena that happen in the

fluid are much faster than the ones occurring on the
boundaries. This allows considering just the temporal
effects in the boundary conditions.

2
(49)
0 ( ) = [
((
)) + 2 ].

(50)

=
;

The velocities profile is only defined by the injection

velocity and is not affected by the concentration changes.
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Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

are the surface temperature as a function of the radius and the time
and the inlet precursor feed velocity as a function of the time.
The objective control function is formulated as a tracking
function of the average film height compared to the set-point while
penalizing the average rugosity of the surface eq. (67).

2
()]
min = [(() ) +

(67)

5 Results and discussion

There are several categories for the results obtained in this
article. In first place the results of the kinetic Monte Carlo model
aiming to obtain the condition dependent models of the
microscopic properties will be shown. With these results a
optimization problem was implemented in GAMS based on the
formulation presented in the section 4 and the results obtained are
reported here. Finally the optimization problem was reformulated
leaving the inlet reactor velocity parameter as a variable.

Figure 5. Kinematic Monte Carlo simulation results with T=1000K,

P=101.325Pa, t=0.1s

The Figure 6 shows the results obtained by the kMC

simulation for the change of the adsorbed particles, the surface
height change and the growth rate. The behavior is linear
compared to both the pressure and the temperature which shows
that the proposed model (eq. 47) is a good fitting for the analyzed
operation range. In order to simplify the problem and avoid
inconsistencies from the prediction of the fitted models, the change
in the surface height and the growth rate are related through a
fitting, reducing then the number of variables.

5.1 Results of the kMC model

For the black-box model construction that is used to
describe the phenomena of the microscale a factorial design of
experiments is formulated in which the temperature is evaluated
between 900 and 1300K, and the precursor partial pressure
between 0 and 0.1 bar, which are the limiting operating conditions
of the process. The total number of events is fixed as 7e4 so that
there are enough to observe the behavior of the variables.
However, this makes that the simulated time of each case to be
different, requiring the standardization of the results compared to
the temporal duration of each analyzed level. The Figure 4shows
the evolution of the surface, as the number of molecules deposited
in the 50x50 lattice after 0.1 seconds. The change in the height of
the surface and the large dispersion of height which cause the
increase in the rugosity can be observed. A typical response of the
microscale that are used in the experimental design are presented
in the Figure 5 that shows a lineal evolution of the number of
deposited molecules and the height change against time, whereas
the growth rate oscillates around a constant value due to the
variability introduced by the migration and desorption events.
There is a growth of the rugosity against time, but this growth is
lower as the time (amount of particles deposited) increases,
reaching eventually a constant value.

Figure 6. Fitting of an in-out model from eq. (47) for the growth rate and
the changes of the surface height. The points represent the obtained data by
the kMC and the lines represent the adjusted model.

In the case of the rugosity, exponential or power functions

are used to fit the parameters of the eq. (48). The Figure 7 presents
the results obtained. These results show a high variability from the
data, and for instance a good prediction can not be guaranteed
outside of the operation range. In the optimization problem,
polytopic restrictions are added to the parameters of the rugosity
model that match with the ranges observed in the Figure 7 so that
erroneous predictions are avoided.
Figure 4. Kinematic Monte Carlo simulation results for a 50x50 lattice with
T=1000K, P=101.325Pa, t=0.1s

Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

Figure 7. Fitting of an in-out model (Ec. 44) for the rugosity coefficients.
The points represent the obtained data by the kMC and the lines represent
the adjusted model.

Figure 9. Precursor partial pressure and temperature on the surface profiles

for constant precursor feed

It can be observed that the optimal control algorithm, after

obtaining a fall in the inlet velocity, regulated the temperature on
the surface such that the adsorption on it increased. The
phenomenon resulted in the minimization of the rugosity even
after the perturbation in less than two seconds without affecting the
constant growth rate as seen in the Figure 10.

5.1 Results of the optimization with constant inlet velocity

Once the models of average height, rugosity, growth rate and
number of particles against temperature, pressure and time were
developed from the kMC simulation, the interface necessary for
the continuum simulation was available with the boundary
conditions and the control specified functions. After programming
the equations shown in the section 3 applying the simplifications
and suppositions shown in the section 4 in the optimization
software GAMS (General Algebraic Modeling System). The
dynamic optimization problem was also programmed on this
software. The problem was solved using the NLP optimization
algorithm CONOPT and the results are shown below.
For the original formulation of the problem the optimization
software after minimizing the rugosity and after 5 seconds of
operation reaching 0.04mm of thin film height was forced to
modify the inlet velocity reaching almost zero after 1.6 seconds as
shown in the Figure 8.

Figure 10. Rugosity and thin film height profiles for constant precursor
feed

5.1 Results of the optimization with variable inlet velocity

Following the results presented in Figure 8, the optimal control
algorithm forced a change in the inlet velocity against an
specification of this parameter. For this reason, it was decided to
study the behavior of the system when the inlet velocity was not a
fixed constant, but a control variable inside the reactor. After
reformulating the optimization program with this degree of
freedom the following results were obtained.

Figure 8. Inlet velocity profile for constant precursor feed

After achieving the minimization of the rugosity the results of

the multiscale coupling variables obtained, such as the partial
pressure of precursor on the surface, surface temperature, the thin
film height and the rugosity as seen in the Figure 9 andFigure 10.

Figure 11. Inlet velocity profile for variable precursor feed

Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

It can be noted that the optimal velocity inlet profile is one

order or magnitude smaller that the specified as a constant, besides
that it behaves as a pulse of feed flow. This inlet accomplishes the
specifications given by the optimization problem, which are the
minimization of the rugosity and a constant growth rate of the
substrate layer. The silane partial pressure profile and the surface
temperature are reported in the Figure 12 and the silicon wafer
height and the rugosity profiles are shown in the Figure 13.

and models is made through a molar flux boundary condition. Due

to the size of the original detailed problem and the amount of
computational time required for the solution of the microscale
model, reduced order models obtained through physical
simplifications and data fitting were used in order to describe the
phenomenon in the optimization problem.
The optimal control problem was solved for two different
cases. The first one treated the inlet velocity as a fixed constant,
and the second one considered it as a variable. The second case is
the only that satisfies the control objective of the seeked surface
height The variation in the inlet velocity allowed to control the
precursor partial pressure on the surface, controlling then the thin
film growth rate. The variation of the radial surface temperature
allows to homogenize the thin film height and control the rugosity.
As future work in this investigation are several routes to
follow: the refinement of the reduced order models of the
microscale, the consideration of other definition of rugosity, the
application of a Computational Fluid Dynamics (CFD) model, the
implementation of stochastic optimization algorithms, the
extension of the study case, and the study of more advanced
control strategies. The refinement of the reduced order models can
be done by feeding them with the data obtained after solving the
optimal control model until observing no improvement in the
objectives. The rugosity can be redefined as the number of broken
bonds and not as the standard deviation of the lattice heights. The
used of CFD models for describing the mesoscale directly into the
optimization algorithm can be considered either by implementing
them directly or by reduction techniques as the Proper orthogonal
decomposition (POD). The implementation of stochastic
optimization algorithms can be used to include directly the
microscale model into the optimization problem. The study case
can be extended to the growth of multiple thin films
simultaneously. The more advanced control strategies that can be
proposed from this work are closed-loop control or model
predictive control (MPC).

Figure 12. Precursor partial pressure and temperature on the surface

profiles for variable precursor feed

The profiles obtained with a variable precursor feed velocity

are considerably different to the ones reported in the Figure 9. The
partial pressure of the silane is less than the one obtained on the
last simulation, this because the inlet flow is also less. The
temperature reached the operational limit of 1300K after 0.9
seconds. This behavior is the optimal answer found using the
CONOPT algorithm are the ones reported in the Figure 12 and
Figure 13.

References
[1] W. Vargas, Introduction to Multiscale Transport Phenomena,
Bogot: Universidad de los Andes, 2014.
[2] A. Varshney y A. Armaou, Multiscale optimization using
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[3] Z. Jaworski y B. Zakrzewska, Towards multiscale modelling
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[5] M. Salciccioli, M. Stamatakis, S. Caratzoulas y D. Vlachos,
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Albuquerque: Noyes Publications, 1992.
[8] M. Costello, D. Tossell, D. Reece, C. Brierley y J. Savage,

Figure 13. Rugosity and thin film height profiles for variable precursor
feed

Notice that the rugosity obtained with this new control scheme
(velocity with variable velocity) is higher to the one obtained with
the constant inlet velocity and the deposition height is less in
almost all the range of times but an uniform surface in the radial
direction is desirable for the final product. This shows that the
operation from the point of view of product quality is more
convenient the results obtained taking the inlet velocity as a
variable.
5 Conclusions and perspectives
This article describes the implementation of an open loop
control to a CVD reactor using dynamic optimization. The model
that describes the operation of the reactor has a multiscale
integration. The description of the adsorption reaction in the
surface is simulated through kMC; and the mass, energy and
momentum transfer in the gaseous phase is described by
differential balances. The integration of the two different scales
9

Bernal-Neira, Lozano-Santamara, Vargas-Escobar, Gmez-Ramrez / DYNA.

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D.E: Bernal-Neira is a Teaching Assistant at Universidad de los Andes

(Bogot, Colombia). He received a BS in Chemical Engineering from
Universidad de los Andes and is a M.Sc. in Chemical Engineering ans BS
in Physics student at Universidad de los Andes. Currently he lectures on
Optimization of Chemical Processes complementary sections. His research
interests include dynamic optimization, stochastic simulations and process
control.
F. Lozano-Santamara is a Teaching Assistant at Universidad de los
Andes (Bogot, Colombia). He received a BS in Chemical Engineering
from Universidad de los Andes and is a M.Sc. in Chemical Engineering
student at Universidad de los Andes. Currently he lectures on Industrial
Processes Fundamentals complementary sections. His research interests
include dynamic optimization, MPC and process control.
W.L. Vargas-Escobar is Assistant Professor at the Chemical Engineering
Department, Universidad de los Andes. He was educated as the
Universidad de America (Bogot, Colombia), Colombia National
University (Bogot, Colombia) and University of Pittsburgh (Pittsburgh,
PA). He has worked at Colombia National University, Nueva Granada
Military University and University of Pittsburgh. He is a member of the
American Institute of Chemical Engineers, American Chemical Societies
(Colloids division), and American Institute of Physics. Currently, he
lectures on Chemical Reaction Engineering, Advanced Trasnport
Phenomena and Fundamental aspects of Nanotechnology. His current
research interests are in the areas of transport phenomena in complex
systems including: suspensions, emulsions, granular media and more
recently nanoparticles. He is also concerned with the general topic of
research and education on Chemical Engineering.
J.M. Gmez-Ramrez is Associate Professor and former head of the
Chemical Engineering Department at Universidad de los Andes (Bogot,
Colombia). He received a BS and M.Sc. in Chemical Engineering from
Universidad Nacional de Colombia, a M.B.A. from Universidad de los
Andes and a Ph.D. from Universit de Pau et de Pays de lAdour, France.
Currently he lectures on Optimization of Chemical Processes and Industrial
Processes Fundamentals. His research interests include dynamic
optimization with integer variables, energy optimization and optimal

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