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Off-lattice Kinetic Monte Carlo simulations of strained hetero-epitaxial growth
Theoretische Physik und Astrophysik
& Sonderforschungsbereich 410
Julius-Maximilians-Universität Würzburg
Am Hubland, D-97074 Würzburg, Germany
http://theorie.physik.uni-wuerzburg.de/~biehl {~much}
Mathematics and Computing Science
Intelligent Systems
Rijksuniversiteit Groningen, Postbus 800,
NL-9700 AV Groningen, The Netherlands
Michael Biehl Florian Much, Christian Vey, Martin Ahr, Wolfgang Kinzel
MFO Mini-Workshop on Multiscale Modeling in Epitaxial Growth, Oberwolfach 2004
Hetero-epitaxial crystal growth
- mismatched adsorbate/substrate lattice
- model: simple pair interactions, 1+1 dim. growth
- off-lattice KMC method
Stranski-Krastanov growth - self-assembled islands, SK-transition - kinetic / stationary wetting layer - mismatch-controlled island properties
Summary and outlook
Outline
Formation of dislocations - characteristic layer thickness - relaxation of adsorbate lattice constant
Molecular Beam Epitaxy ( MBE )
control parameters:deposition rate substrate temperature T
ultra high vacuumdirected deposition of adsorbatematerial(s) onto a substrate crystal
oven
UHV
T
Hetero-epitaxy
lattice constants A adsorbate
S substratemismatch
S
SA
σσσ
different materials involved in the growth process, frequent case:
substrate and adsorbate with identical crystal structure, but
initial coherent growth undisturbed adsorbate enforced in first layers far from the substrate
dislocations,lattice defects
S
A
strain relief
island and mound formationhindered layered growthself-assembled 3d structures
A
S
and/or
Modelling/simulation of mismatch effects
Ball and spring KMC models, e.g. [Madhukar, 1983]
activation energy for diffusion jumps: E = Ebond - Estrain
bond counting
elasticenergy
continuous variation of particle distances, but within
preserved (substrate) lattice topology, excludes defects, dislocations
e.g.: monolayer islands [Meixner, Schöll, Shchukin, Bimberg, PRL 87 (2001) 236101]
SOS lattice gas : binding energies, barriers continuum theory: elastic energy for given configurations
Lattice gas + elasticity theory:
Molecular Dynamics
limited system sizes / time scales, e.g. [Dong et al., 1998]
continuous space Monte Carlo
based on empirical pair-potentials,
rates determined by energies of the binding states
e.g. [Plotz, Hingerl, Sitter, 1992], [Kew, Wilby, Vvedensky, 1994]
off-lattice Kinetic Monte Carlo
evaluation of energy barriers in each given configuration
[D. Wolf, A. Schindler (PhD thesis Duisburg, 1999)
e.g. effects of (mechanical) strain in epitaxial growth,diffusion barriers, formation of dislocations
A simple lattice mismatched system
continuous particle positions, without pre-defined lattice
6
ij
o
12
ij
ooooij r
σrσ
U4σUU ,
equilibrium distance o
short range: Uij 0 for rij > 3 o
substrate-substrate US, S
adsorbate-adsorbate
substrate- adsorbate, e.g. 2σσσUUU ASASASAS ,
UA, A
lattice mismatch SSA σσσ
qualitative features of hetero-epitaxy, investigation of strain effects
example: Lennard-Jones system
KMC simulations of the LJ-system
- deposition of adsorbate particles with rate Rd [ML/s]
- diffusion of mobile atoms with Arrhenius rate TBk
ΔE
oi
i
e R
simplification: for all diffusion events -112
o s10
- preparation of (here: one-dimensional) substrate with fixed bottom layer
Evaluation of activation energies by Molecular Statics
virtual moves of a particle, e.g. along x
minimization of potential energy w.r.t. all other coordinates
(including all other particles!)
e.g. hopping diffusion
binding energy Eb (minimum)
transition state energy Et (saddle)
diffusion barrier E = Et - Eb Schwoebel barrier Es
possible simplifications: cut-off potential at 3 o
frozen crystal approximation
KMC simulations of the LJ-system
- deposition of adsorbate particles with rate Rd [ML/s]
- diffusion of mobile atoms with Arrhenius rate TBk
ΔE
oi
i
e R
simplification: for all diffusion events -112
o s10
- preparation of (here: one-dimensional) substrate with fixed bottom layer
- avoid accumulation of artificial strain energy (inaccuracies, frozen crystal)
by (local) minimization of total potential energy
all particles after each microscopic event with respect to particles in a 3 o neighborhood of latest event
n
1ijij
n
1itot UE
Simulation of dislocations
dislokationendislokationen
· deposition rate Rd = 1 ML / s
· substrate temperature T = 450 K
· lattice mismatch -15% +11%
· system sizes L=100, ..., 800 (# of particles per substrate layer)
· interactions US=UA=UAS diffusion barrier E 1 eV for =0
· 6 ... 11 layers of substrate particles, bottom layer immobile
= 6 % = 10 %
large misfits:
dislocations at the
substrate/adsorbate
interface
(grey level: deviation from A,S , light: compression)
Critical film thickness
small misfits: - initial growth of adsorbate coherent with the substrate
hc vs. ||
solid lines:
<0: a*=0.15
>0: a*=0.05
adsorbate under compression,earlier dislocations
=- 4 %
- sudden appearance of dislocations at a film thickness hc
experimental results (semiconductors):
misfit-dependence hc = a* ||-3/2
re-scaled film thickness
vert
ical
latt
ice
spac
ing
KMC
- Pseudomorphic growth up to film thickness -3/2
enlarged vertical lattice constant in the adsorbate
- Relaxation of the lattice constant above dislocations
qualitatively the same:6-12-, m-n-, Morsepotential
[F. Much, C. Vey]
ZnSe / GaAs, in situ x-ray diffraction
= 0.31%
[A. Bader, J. Geurts, R. Neder]SFB-410, Würzburg,in preparation
Critical film thickness
experimental results for various II-VI semiconductors
-3/2
Matthews, Blakeslee .hlnh c
1c const
Stranski-Krastanov growth
experimental observation ( Ge/Si, InAs/GeAs, PbSe/PbTe, CdSe/ZnSe, PTCDA/Ag)
deposition of a few ML adsorbate material
with lattice mismatch, typically 0 % < 7 %
PbSe on PbTe(111) hetero-epitaxy G. Springholz et al., Linz/Austria
potential route for the fabrication of self-assembled quantum dots
desired properties: (applications)
- dislocation free
- narrow size distribution
- well-defined shape
- spatial ordering
- initial adsorbate wetting layer of characteristic thickness- sudden transition from 2d to 3d islands (SK-transition) - separated 3d islands upon a (reduced) persisting wetting layer
Stranski-Krastanov growth
S-K growth observed in very different materials
hope: fundamental mechanism can be identified by
investigation of very simple model systems
L J pair potential, 1+1 spatial dimensions
modification: Schwoebel barrier removed by hand
single out strain as the cause of island formation
small misfit, e.g. = 4%
deposition of a few ML dislocation free growth
Simple off-lattice model:
US > UAS > UA favors wetting layer formation
Stranski-Krastanov growth
aspect ratio 2:1
- kinetic WL hw* 2 ML
growth: deposition + WL particles
splitting of larger structures
- stationary WL hw 1 ML
US= 1 eV, UA= 0.74 eV
Rd= 7 ML/s T = 500 K
AS
mean distance from neighbor atoms
= 4 %
self-assembled quantum dots
dislocation free multilayer islands
Nature of the SK-transition
-thermodynamic instability ? Island size ~ -2
- triggered by segregation and/or intermixing effects ?
e.g. InAs/GaAs [Cullis et al.] [Heyn et al.]
reduced effective misfit
concentrationand strain gradient
- kinetic effects, strain induced diffusion properties ?
PTCDA / Ag ? [Chkoda et al., Chem Phys. Lett. 371, 2004]
Adsorbate adatom diffusion on the surface
slow on the substrate fast on the wetting layer UAS
E
[eV
]
substrate
WL (1) (2)
- qualitatively as, e.g., for Ge on Si [B. Voigtländer et al.]
- stabilizing effect: favors existence of a wetting layer
- LJ-potential: no further decrease for more than 3 WL, limited (stationary) wetting layer thickness
Adsorbate adatom diffusion on the surface
single adatom on a (partially) relaxed island on top of 1 WL
base: 24 particles, height h ML
position above island base
diffusion bias towards the
center
stabilizes existing islands
energy barrier (hops to the left)
1
35
isla
nd
heig
ht
(on relaxed ads.)
(on 1 WL)
Determination of the kinetic wetting layer thickness
analogous to experiment:
end of layer-by-layer roughness oscillations or:
(3rd and 4th layer) island density vs. coverage
fit: = o ( – hw* )
simulations:
Rd=3.5 ML/s, T=500 K
= o ( – hw* )
1.5, hw* 2.1 ML
Rd=3.5 ML/s, T=500 K
= 4 %
[ Leonard et al., Phys. Rev. B 50 (1994) 11687 ]
experiment: InAs on GeAs
hw*=
[ML]
Kinetic wetting layer thickness
hw* grows with
- increasing flux
- decreasing temperature
US = 1 eV
UA = 0.74 eV
= 4 %
hw
*
[ML]
T= 480 KT= 500 K
hw* = ho ( Rd / Rup )
0.2
Fit (500K):
Rup
island formation triggered by
significant rate Rup for upward
moves at the 2d-3d transition
[ J. Johansson, W. Seifert, J. Cryst. Growth 234 (2002) 132 ]
Characterization of islands
saturation behavior: island properties depend only on
density base length bdistance d
become constant and T-independent
for large enough deposition rate Rd
T=500 K
T=480 K
= 4 %
b
b
dT=500 KT=480 K
0.0
10
.03
T=500 K
T=480 K 0
.02
30
50
70
Rd= 7 ML/s
T = 500 K #
of
isl
ands
Characterization of islands
saturation behavior: island properties depend only on
density base length bdistance d
become constant and T-independent
for large enough deposition rate Rd
T=500 K
T=480 K
= 4 %
b
b
b -1
length scale
-1 introduced
by S A
Summary
Method
off-lattice Kinetic Monte Carlo
Dislocations
characteristic length -1, critical layer thickness -3/2
Stranski-Krastanov growth
strain induced formation of mounds, kinetic / stationary wetting layer
large deposition rates: misfit controlled island density, size b -1
SK-transition:
slow diffusion on the substrate significant rate for upward jumps
fast diffusion on the wetting layer diff. bias towards island centers
application: simple model of hetero-epitaxy
Outlook
interaction potentials,lattices
universality (Morse, mn-Potentials)
material specific (e.g. RGL-Potentials) simulations
2+1 dimensional growth
Stranski-Krastanov growth:
- island formation mechanism for <0 ? - spatial distribution of islands
- long time behavior, e.g. annealing / ripening after
deposition
- kinetic vs. equilibrium dots, e.g. b -2 for Rd0 ?
Growth modes
- Volmer-Weber growth for
?
UAS < UA
- Layer-by-layer growth for small misfit ?