Oblique alignment of columns of self-organized Ge/Si(001) islands in multilayer

structure
C. J. Huang, D. Z. Li, B. W. Cheng, J. Z. Yu, and Q. M. Wang

Citation: Applied Physics Letters 77, 2852 (2000); doi: 10.1063/1.1322372

View online: http://dx.doi.org/10.1063/1.1322372
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 APPLIED PHYSICS LETTERS VOLUME 77, NUMBER 18 30 OCTOBER 2000

Oblique alignment of columns of self-organized GeÕSi„001… islands

in multilayer structure
C. J. Huang,a) D. Z. Li, B. W. Cheng, J. Z. Yu, and Q. M. Wang
State Key Laboratory on Integrated Optoelectronics, Institute of Semiconductors, Beijing 100083,
People’s Republic of China
共Received 31 May 2000; accepted for publication 12 September 2000兲
Ge/Si multilayer structures with a bimodal distribution of the island spacing in the first layer have
been investigated by atomic-force microscopy and transmission electron microscopy. Besides the
vertical alignment, some oblique alignments of stacked islands are observed. The presence of the
elastic interaction between islands is responsible for the oblique alignment of stacked islands.
© 2000 American Institute of Physics. 关S0003-6951共00兲04644-1兴

Strain-driven self-assembly of defect-free islands in the
Stranski–Krastanov growth mode has attracted a lot of atten-
tion during the last few years, as these structures are ex-
pected to be potential candidates for the realization of quan-
tum electronic and optoelectronic devices. In particular, the
lattice-mismatched material systems Ge/Si and InAs/GaAs
are currently under intense investigation.1 Although self-
organized islands can be unexpectedly uniform in size, they
are still not sufficiently for most practical application. The
other major drawback of the self-organized islands is the
lack of macroscopic periodic order in spatial distribution,
which limited them in some applications such as quantum
automata.2 A widely used approach to improve the homoge-
neity and periodicity of islands is to stack several island lay-
ers separated by a spacer layer.3 The spacer layers act like a
bandpass filter for the spatial frequency leading to a progres-
sively more uniform island spacing and size distribution. A
remarkable feature of these multilayer arrays of islands is
that buried islands in successive layers are spatially corre-
lated if the thickness of the spacer layer is kept thin enough.
To our knowledge, there are two main ways of correlation of
multilayer arrays of islands. One is vertical correlation for
three-dimensional islands in Ge/Si 共Ref. 4兲 and InAs/GaAs
共Ref. 5兲 systems; the other is vertical anticorrelation for two-
dimensional islands in the CdSe/ZnSe 共Ref. 6兲 system. The
origin of the two correlation ways has been attributed to the
interaction between buried and surface islands by the anisot-
ropy strained field, by neglecting the elastic interaction be-
tween islands in the same layer.3,7 However, such an elastic
interaction must be considered to explain the phenomena
here.
In this letter, we investigate the Ge island growth behav-
ior in the Ge/Si共001兲 multilayer structure by cross-sectional
transmission electron microscopy 共TEM兲 and atomic-force
microscopy 共AFM兲. We find that both the island size and
height increase with the increase of the number of deposited
layers, which results from the accumulation of strain relax-
ation due to the correlation of three-dimensional islands. By
TEM images, we find that there are some oblique alignments
of stacked islands besides the vertical alignment, giving di-
a兲
Electronic mail: cjhuang@red.semi.ac.cn
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rect evidence that there exists an elastic interaction between
islands in the same layer.
All samples were grown by ultra-high-vacuum 共UHV兲
chemical-vapor deposition on a 共001兲-oriented Si substrate
from pure disilane and germane (Si2H6 and GeH4). The Si
substrates were cleaned in an ex situ chemical etch process
and loaded into an UHV growth chamber with basic pressure
lower than 10⫺8 Pa, and then heated up to 950 °C to deoxi-
dize. The multilayer structures underwent the following
growth procedure: growth of ⬃250 nm Si buffer layer at
850 °C, followed by ten bilayers consisting of 5.8 ML Ge
and 35-nm-thick Si at 650 °C. Two reference samples with
the same 5.8 ML Ge layers were grown without the Si cap
layer for AFM analysis: one consisted of a single Ge layer
and the other consisted of ten Ge/Si periods. The thicknesses
of the Ge and Si layers were obtained by Rutherford back-
scattering combined with double-crystal x-ray diffraction
analysis, which were in good accordance with the results
from the TEM images. AFM images were recorded with a
Digital Instrument AFM setup operating in contact mode.
TEM measurements were performed on cross sections using
a 200 kV microscope. The TEM samples were thinned to an
average thickness of the order of 20 nm by tripod polishing
follow by brief ion milling.
Figure 1 shows the 5⫻5 ␮ m2 AFM topographs 共inset兲
and the nearest-spacing histograms of two reference samples.
The deposited Ge amount was kept at 5.8 ML in all layers of
both samples. The AFM images in Figs. 1共a兲 and 1共b兲 cor-
respond to the morphology of the first and the tenth Ge layer
in the multilayer sample, respectively. The island shapes in
both the AFM images are rounded domes, and no pyramidal-
shape islands are observed. Two types of island size are
found in the first layer. Large-dome heights are about 14 nm
and the base dimensions are around 140 nm, and the heights
and base dimensions of the small domes are 11 and 100 nm,
respectively. As shown in the Fig. 1共a兲 inset, several small
domes surround a large dome over large denuded areas,
which results in a bimodal distribution of the nearest-island
spacing with peaks at 180 and 300 nm. The former corre-
sponds to the spacing between the small domes, while the
latter corresponds to the spacing between the large and small
domes. Having grown nine Ge/Si bilayers on the first Ge
layer, the morphology of the tenth Ge layer changes strik-
2852 © 2000 American Institute of Physics
 Appl. Phys. Lett., Vol. 77, No. 18, 30 October 2000
FIG. 1. 5 ␮ m⫻5 ␮ m AFM topographs 共inset兲 and histograms of the nearest
spacing 共center to center兲 between islands from 共a兲 the single-Ge-layer
sample and 共b兲 the ten-bilayer Ge/Si sample without the Si cap layer. Note
that the deposited Ge amount was kept 5.8 ML in all layers.
ingly. The islands become larger and more uniform with a
base width of ⬃180 nm and a height of ⬃17 nm, as well as
the nearest-island spacing, exhibits a single modal distribu-
tion with the peak at 260 nm 关Fig. 1共b兲兴. In addition, the
density of islands in the tenth layer has decreased slightly
from 11⫻108 cm⫺2 in the first layer to 8⫻108 cm⫺2.
Two typical cross-sectional TEM images taken along the
关110兴 azimuth of the sample with ten Ge/Si bilayers are
shown in Fig. 2. Figure 2共a兲 is the bright-field image of two
columns of vertical-correlation islands where their spacing
along 关110兴 in the first layer is larger than 400 nm. There-
fore, one of the two islands in the first layer corresponds to
the large dome shown in the Fig. 1共a兲 inset and the other
corresponds to the small dome.8 A dark-field image of the
same sample but at a different region is shown in Fig. 2共b兲.
Due to the effect of strain, the gray contrast does not well
correspond to the Ge-content distribution. However, because
the contour of islands is clear, the position and shape of the
islands can still be distinguished. The spacing of each of the
two nearest islands in the first layer is less than 200 nm and
all of four islands in the first layer belong to the small type of
domes. For both situations, the size of the islands increases
with the number of bilayers, which is in accordance with the
previous results.3,4,9
By linking the middle points of the bases of the islands
in one column, we use white lines to indicate the directions
of alignment of the correlated islands. As shown in Fig. 2共a兲,
where the island spacing in the first layer is larger, the left
column is vertically aligned and the right column is oblique
to the left. Therefore, the spacing of the two islands in the
same layer decreases with increasing the number of bilayers,
which exhibits an attractive interaction between the islands.
However, the spacing in the first layer increases with increas-
ing the number of bilayers at the region where the island
spacing in the first layer corresponds to the small value, as
shown in Fig. 2共b兲. Column A is vertically aligned from the
first to the third layer and then oblique from the fourth layer
on. Column B only contains islands in the first three layers
and its alignment is vertical. The alignments of columns C
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and D are whole oblique and vertical, respectively. Such ob-
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Huang et al. 2853
FIG. 2. Two typical cross-sectional TEM images of the same sample with
ten Ge/Si bilayers but at different regions. 共a兲 A bright-field image with two
columns of Ge islands, their island spacing in the first layer corresponds to
the large value in the bimodal distribution of island spacing. 共b兲 A dark-field
image with four columns of Ge islands, their island spacings correspond to
the small value. The white lines are guides to the eye.
lique alignments of stacked islands as in Fig. 2 result in the
changeover of the island spacing from a bimodal distribution
to a single modal one 共Fig. 1兲.
Tersoff, Teichert, and Lagally3 pointed out that nucle-
ation of islands of the second sheet occurs preferentially
above buried islands by consideration of the local strain on
the surface due to the buried islands. They explained the
enhancement of the uniformity of the island spacing by in-
creasing new islands at the region with widely spaced islands
buried and merging10 at the region with closely spaced is-
lands buried. However, their preferential nucleation theory
cannot predict the oblique alignment of stacked islands as
depicted here. An elastic interaction between islands in the
same layer must be considered, besides the interaction be-
tween islands in different layers. According to the theory of
spontaneous ordering of arrays of strained islands,6,11 the
elastic interaction consists of two parts: attraction and repul-
sion and both of them depend on the volume and spacing of
the islands. If the volumes of interacting islands are kept
constant, two parts balance each other by changing the criti-
cal spacing between the islands to a critical value. Therefore,
the different sizes of the islands correspond to the different
spacings, which results in the bimodal distribution of the
spacing in the first layer where there are two sizes of islands.
In the stacked island structure, the size of the islands in-
creases and becomes more uniform with increasing the num-
ber of bilayers. On one hand, the more uniform size of the
islands results in the more uniform spacing between islands.
 2854 Appl. Phys. Lett., Vol. 77, No. 18, 30 October 2000
On the other hand, if the spacing between islands is kept
constant, the increase of size of islands makes an enhance-
ment of the elastic interaction. At the initial stage of island-
ing, small islands preferentially nucleate directly vertically
above the buried islands and their spacing is kept the same as
that of the buried islands. Then, as the islands become large
gradually, the enhanced elastic interaction cannot be bal-
anced. Therefore, the spacing of islands has to change by an
asymmetrical development of island shape that can be found
in some islands at the obliquely aligned columns. In particu-
lar, the interaction exhibits attraction at the region with a
wide spacing and exhibits repulsion at the region with a
close spacing. This induces the oblique alignment of the is-
land column.
Although the theory predicts that the elastic interaction
between islands in one layer is direction related, no obvious
preferential direction is observed in the arrangement of is-
lands, as shown in the AFM images. Therefore, we believe
that the oblique alignment of stacked islands exists not only
in the direction that the TEM images are taken along, but
also in other directions. Due to the cooperation of several
island columns nearby, some island columns still preserve
vertical alignment as the left column in Fig. 2共a兲 and column
D in Fig. 2共b兲.
In conclusion, we have investigated the alignments of
columns of self-organized Ge islands in a multilayer struc-
ture, where the spacing between islands is a bimodal distri-
bution in the first layer. Some obliquely aligned columns
have been observed in TEM images taken along the 关110兴
azimuth. The oblique alignment makes larger spacings re-
duce and smaller spacings increase, resulting in a single dis-
tribution of the island spacing in the tenth layer. The pres-
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132.174.255.116 On: Mon, 01 Dec 2014 21:32:39
Huang et al.
ence of the elastic interaction between islands is responsible
for the oblique alignment of stacked islands, a deviation
against the vertical alignment formed in the preferential
nucleation effect.
The AFM measurements were performed at Institute of
Physics, Chinese Academy of Sciences. The authors grate-
fully acknowledge Professor Ju Wu for helpful discussion.
This work was supported by ‘‘863’’ Research Plan Grant
No. 863-307-06-05共03兲, and the National Natural Science of
China Foundation under Grant Nos. 69787004, 69746001,
69990540, and 69896260.
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