Applied Surface Science 127129 1998.

159163

Monte Carlo simulations of epitaxial growth: comparison of

pulsed laser deposition and molecular beam epitaxy
M.E. Taylor ) , Harry A. Atwater
Thomas J. Watson Laboratories of Applied Physics, California Institute of Technology 128-95, Pasadena, CA 91125, USA

Abstract
The influence of epitaxial growth method on surface morphology was explored using a solid-on-solid, rate equation,
Monte Carlo simulation whose parameters were chosen to approximate 1 = 1. Si 001.. In simulations corresponding to
molecular beam epitaxy, films of 10 monolayer thickness were deposited with a steady-state flux of 0.25 monolayersrs and
an adatom energy of 0.3 eV. In simulations corresponding to pulsed laser deposition, films of 10 monolayer thickness were
deposited with a pulsed flux of 0.5 monolayersrpulse and 0.5 pulsesrs and adatom energies ranging from 10 to 135 eV.
Surface morphology was characterized using surface images, surface height standard deviations, and heightheight
correlation functions. In comparison to molecular beam epitaxy, pulsed laser deposition was found to result in smaller
surface roughness at substrate temperatures below approximately 4008C and larger surface roughness at higher temperatures.
This behavior is attributed to a balance between roughening associated with pulsed deposition and smoothening associated
with energetic deposition. q 1998 Elsevier Science B.V.
PACS: 68.55.Jk; 81.15.Fg; 82.20.Wt; 81.15
Keywords: Pulsed laser deposition; Molecular beam epitaxy; Energetic deposition; Pulsed deposition; Surface morphology; Surface
roughness

1. Introduction
Pulsed laser deposition is a growth technique that
has emerged in the last decade as a feasible means of
producing materials from superconductors w1x to
semiconductors w26x. In molecular beam epitaxy,
growth is characterized by a steady-state temporal
profile and a narrow adatom energy distribution with
a mean of a few tenths of an eV. In pulsed laser
deposition, growth is characterized by a pulsed temporal profile and a broad adatom energy distribution
with a mean of a few eV. Films grown by pulsed
)

Corresponding author. Tel.: q1-626-395-3826; fax: q1-626795-7258; e-mail: maggie@daedalus.caltech.edu.

laser deposition have been observed to have reduced

surface roughness in comparison to films grown by
molecular beam epitaxy w5x. This result has been
qualitatively attributed to effects related to energetic
deposition w7x. The objective of this research was to
evaluate the effect of a pulsed energetic flux on the
growth process using an atomistic simulation.
2. Experimental
The simulation developed for this study is a solidon-solid, rate equation, Monte Carlo simulation w8
10x. Atoms are defined as point objects that occupy a
simple cubic lattice. The site of each deposition
event is chosen randomly from the set of lattice sites

0169-4332r98r$19.00 q 1998 Elsevier Science B.V. All rights reserved.

PII S 0 1 6 9 - 4 3 3 2 9 7 . 0 0 6 2 6 - 0

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M.E. Taylor, H.A. Atwaterr Applied Surface Science 127129 (1998) 159163

that define the surface. Morphologies such as voids

and overhangs are prohibited. Surface diffusion
events are assumed to follow Arrhenius kinetics.
Atoms are allowed to diffuse if they have less than
four lateral neighbors and lie on the surface. These
atoms are assigned four activation energies, one for
each possible diffusion direction. Each activation
energy is Qadatom , the barrier associated with an
adatom on a level surface, to which Qcoor and Qstep ,
the barriers associated with lateral coordination and
diffusion across a step edge, are added if appropriate.
Barrier values were chosen to correspond approximately to 1 = 1. Si 001.. A scanning tunneling
microscopy study of growth on Si 001. led to the
selection of values for Qadatom and the rate prefactor
of 0.55 eV and 600 jumpsrm s w11x. Values of 0.30
eV per lateral neighbor for Q coor and of 0.15 eV for
Qstep for single-height steps were selected to reflect
molecular dynamics simulation results for Si 001.
w12x. Since double-height steps microscopically resemble Si 111. surfaces, a value of 0.40 eV for
Qstep for double-height steps was selected to reflect
molecular dynamics simulation results for Si 111.
w13x. To reduce computation time, vertical movement
of more than two step heights in a single diffusion
event is prohibited. The boundary conditions are
periodic across the simulation cell.
Two temporal profiles are modeled. In the
steady-state mode, the time intervals between deposition events are exponentially distributed random deviates. In the pulsed mode, deposition events occur
in pulses of 5 m s, a pulse length observed experimentally for pulsed laser deposition of Si at an
energy density of 3 Jrcm2 and a targetsubstrate
distance of 3 cm by ion probe time of flight measurements w14x. Within a given pulse, the deposition
events follow the time interval distribution described
for the steady-state mode. Surface diffusion continues during the deposition pulse provided that the
diffusion rate is sufficient to allow diffusion events
to occur between deposition events.
Two adatom energy distributions are modeled. In
the thermal mode, all adatoms are assigned an energy of 0.3 eV, a typical energy for Si molecular
beam epitaxy. In the energetic mode, adatoms are
assigned energies according to a distribution observed for pulsed laser deposition of Si under the
experimental conditions previously described w14x.

This distribution ranges from 10 to 135 eV and

peaks at 20 eV. The simulation incorporates two
energy effects. The first energy effect is transient-enhanced surface diffusion. Following a deposition
event, the deposited adatom is allowed to retain its
deposition energy for a thermalization period of 5 ps,
after which it is assigned an energy corresponding to
the substrate temperature. During the thermalization
period, the adatom has an enhanced rate of diffusion
due to its kinetic energy. The second energy effect is
cluster size reduction. If a depositing adatom impacts
a surface atom that is lying on the edge of a cluster,
the collision may result in diffusion of the surface
atom and usurpation of its original site by the adatom.
A probability distribution for this type of event as a
function of Si adatom energy was obtained by extrapolation from molecular dynamics calculations of
Si atom displacement yield under Arq bombardment
w15x. Between 10 eV and 62 eV, the extrapolated
distribution varies linearly from 0.08 to 1.0. For
energies lower than 10 eV and higher than 62 eV,
values of 0.0 and 1.0 were assumed.
The majority of the simulations presented in this
paper fall into two categories. The first type, which
corresponds to molecular beam epitaxy, combines
the steady-state and thermal modes. The second type,
which corresponds to pulsed laser deposition, combines the pulsed and energetic modes. Each pulse
contains an identical distribution of adatom energies
arranged in order of descending energy to simulate
the temporal separation of adatoms that occurs between ablation and deposition. For temperatures of
1004008C, a 128 = 128 atom simulation cell size
was used. For temperatures of 5008C and 6008C, a
64 = 64 atom cell size was used to reduce computation time. In the steady-state mode, a deposition rate
of 0.25 monolayersrs was used. In the pulsed mode,
a deposition coverage of 0.5 monolayersrpulse was
used in conjunction with a pulse repetition rate of 0.5
pulsesrs to give the same time-averaged deposition
rate. In all simulations, 10 monolayers of material
were deposited on an initially flat substrate.

3. Results and discussion

Fig. 1 shows simulated surface images for a.
steady-state thermal growth at 2008C, b. pulsed

M.E. Taylor, H.A. Atwaterr Applied Surface Science 127129 (1998) 159163

161

representative of the set. For temperatures below

4008C, the pulsed energetic films appear smoother
than the steady-state thermal films. At 4008C, the
pulsed energetic films appear smoother than the
steady-state thermal films on length scales longer
than approximately twenty atoms. For temperatures
of 5008C and 6008C, the pulsed energetic films
appear rougher than the steady-state thermal films.
In a more quantitative approach, surface roughness was analyzed using heightheight correlation
functions w1618x. The heightheight correlation
function M k . for each simulation is the square of
the Fourier transform of the distribution of surface
atom heights. Fig. 2 shows M k . functions for
steady-state thermal growth and pulsed energetic
growth at 2008C, 4008C, and 6008C. Each M k .
function shown represents an average of the M k .
functions for ten simulations with identical input
parameters. At temperatures below 4008C, the pulsed
energetic curve lies below the steady-state thermal
curve for all k values, indicating smaller surface
roughness over length scales equal to and shorter
than the cell size. At 4008C, the pulsed energetic
curve lies below the steady-state thermal curve for
k F 0.06 and coincides with the steady-state thermal
curve for k G 0.06. This indicates that pulsed energetic growth is less subject than steady-state thermal
growth to formation of clusters of 16 atoms or more
Fig. 1. Simulated surface images of 10 monolayers of Si deposited on an initially flat 1=1. Si 001. substrate by a.
steady-state thermal growth at 2008C, b. pulsed energetic growth
at 2008C, c. steady-state thermal growth at 4008C, d. pulsed
energetic growth at 4008C, e. steady-state thermal growth at
6008C, and f. pulsed energetic growth at 6008C. The steady-state
films were deposited at 0.25 monolayersrs; the pulsed films were
deposited at 0.5 monolayersrpulse and 0.5 pulsesrs to give the
same time-averaged deposition rate. The films deposited at 2008C
and 4008C have an area of 128=128 atoms; the films deposited at
6008C have an area of 64=64 atoms. Black and white represent
thickness of 2 monolayers and 18 monolayers, respectively.

energetic growth at 2008C, c. steady-state thermal

growth at 4008C, d. pulsed energetic growth at
4008C, e. steady-state thermal growth at 6008C, and
f. pulsed energetic growth at 6008C. Each of these
images was selected from a set of ten simulations
with identical input parameters and is considered

Fig. 2. Heightheight correlation curves for simulated films deposited by steady state thermal growth and pulsed energetic
growth at 2008C, 4008C, and 6008C. Filled and open symbols
represent steady-state thermal deposition and pulsed energetic
deposition, respextively. Squares, circles, and diamonds correspond to growth at 2008C, 4008C, and 6008C, respectively.

162

M.E. Taylor, H.A. Atwaterr Applied Surface Science 127129 (1998) 159163

in diameter, and equally subject to formation of

smaller clusters. At temperatures above 4008C, the
pulsed energetic curve lies above the steady-state
thermal curve for all k values, indicating larger
surface roughness over length scales equal to and
shorter than the cell size.
These observations can be explained as a balance
between the effects of pulsed deposition and the
effects of energetic deposition. Pulsed deposition
should produce rougher surfaces than steady-state
deposition because the former, having higher instantaneous growth rates, is a more stochastic process
than the latter. Energetic deposition should produce
smoother surfaces than thermal deposition because
of the smoothening effects of transient-enhanced surface diffusion and cluster size reduction, provided
that lattice damage does not occur. At low temperatures, where surface diffusion rates are low,
smoothening due to energetic deposition should
dominate over roughening due to pulsed deposition.
At higher temperatures, roughening due to pulsed
deposition should dominate over smoothening due to
energetic deposition.
To test this hypothesis, a small number of simulations of two additional types were performed to
independently evaluate the effects of pulsed deposition and energetic deposition. The first type combines the steady-state and energetic modes. The
adatom energies are randomly distributed with time.
The second type combines the pulsed and thermal
modes.
Fig. 3 shows the standard deviation R in surface
atom height for each temperature and simulation
type. Each R value shown represents an average of
the R value for ten simulations with identical input
parameters. At 1008C and 2008C, the two thermal
curves have nearly identical values. At higher temperatures, the steady-state thermal curve lies below
the pulsed thermal curve. At 1008C, 2008C, and
3008C, the two energetic curves have nearly identical
values. At higher temperatures, the steady-state energetic curve lies below the pulsed energetic curve.
Below 5008C, the energetic curves lie below the
thermal curves. At 5008C, the steady-state thermal
and pulsed energetic curves have nearly identical
values intermediate between the pulsed thermal and
steady-state energetic values. Above 5008C, the
steady-state curves lie below the pulsed curves. These

Fig. 3. Surface height standard deviation curves for simulated

films deposited by steady-state thermal growth, pulsed energetic
growth, steady-state energetic growth, and pulsed thermal growth,
represented by squares, circles, up triangles, and down triangles,
respectively.

results indicate that at low temperatures, smoothening due to energetic deposition plays a larger role
than roughening due to pulsed deposition, and that at
high temperatures, roughening due to pulsed deposition plays a larger role than smoothening due to
energetic deposition.

4. Conclusion
A solid-on-solid, rate equation, Monte Carlo simulation was developed and used to investigate the
differences in morphological evolution between
pulsed laser deposition and molecular beam epitaxy
of material approximating 1 = 1. Si 001.. Simulation films of 10 monolayer thickness were grown by
molecular beam epitaxy at 0.25 monolayersrs and
by pulsed laser deposition at 0.5 monolayersrpulse
and 0.5 pulsesrs to give the same time-averaged
deposition rate. Simulated surface images, surface
height standard deviations, and heightheight correlation functions indicate that in comparison to
molecular beam epitaxy, pulsed laser deposition produces smoother films for substrate temperatures below approximately 4008C and rougher films for temperatures above approximately 4008C. This is attributed to a balance between smoothening due to
energetic deposition and roughening due to pulsed
deposition.

M.E. Taylor, H.A. Atwaterr Applied Surface Science 127129 (1998) 159163

Acknowledgements
E. Chason provided assistance with algorithm development. D. Goodwin, T. Tombrello, W. Goddard,
B. Crill, S. Glade, R. Beach, M. Ragan, and the
Engineering Computing Facility provided computational resources. This work was supported by the
National Science Foundation and by the Intel Foundation.
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