*Corresponding author. Tel.

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E-mail address: Liuhy@red.semi.ac.cn (H.Y. Liu).
Journal of Crystal Growth 220 (2000) 216}219
E!ects of interdi!usion on the luminescence of InAs/GaAs
quantum dots covered by InGaAs overgrowth layer
H.Y. Liu*, X.D. Wang, Y.Q. Wei, B. Xu, D. Ding, Z.G. Wang
Laboratory of Semiconductor Materials Science, Institute of Semiconductors, Chinese Academy of Sciences, P.O. Box 912,
Beijing 100083, People's Republic of China
National Laboratory for Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences,
P.O. Box 912, Beijing 100083, People's Republic of China
Received 4 August 2000; accepted 22 August 2000
Communicated by M. Schieber
Abstract
We have studied the e!ects of postgrowth rapid thermal annealing on the optical properties of 3-nm-height InAs/GaAs
quantum dots covered by 3-nm-thick In
V
Ga
V
As (x"0, 0.1, and0.2) overgrowth layer. At higher annealing temperature
(*7503C), the photoluminescence peak of InGaAs layer has been observed at lower-energy side of the InAs quantum-dot
peak. In addition, the blueshift in photoluminescence (PL) emission energy is found to be similar for all samples with
increasing the annealing temperature from 650 to 8503C. However, the trend of narrowing of photoluminescence linewidth
is signi"cantly di!erent for InAs quantum dots with di!erent In mole fractions in InGaAs overgrowth layer. These results
suggest that the intermixing in the lateral direction plays an important role in helping to understand the modi"cation of
optical properties induced by rapid thermal annealing. 2000 Elsevier Science B.V. All rights reserved.
PACS: 81.05.Ea; 78.55.Cr; 68.55.Jk
Keywords: Rapid thermal annealing; InAs quantum dots; InGaAs overgrowth layer; Photoluminescence
1. Introduction
The postgrowth thermal treatments have been
recently used to modify the optical properties and
tune the intersubband energy spacing of self-assem-
bled quantum dots (QDs) [1}9]. The strong nar-
rowing of photoluminescence (PL) linewidth, the
large blueshift in the intersubband transition en-
ergy, and the signi"cant reduction in intersublevel
spacing energy induced by rapid thermal annealing
(RTA) have been observed [1}8]. These experi-
mental results indicate that the postgrowth thermal
treatments provide a promising method for the
application of quantum-dot structure in semicon-
ductor QD lasers and detectors. The structural and
optical properties of InAs/GaAs QDs subjected to
RTAhave been widely investigated by transmission
electron microscopy and PL techniques. Although
the strong narrowing and signi"cant blueshift of
QD luminescence emission can be described by the
In}Ga interdi!usion between InAs QDs and GaAs
barrier layer, the detailed mechanisms are still rela-
tively poorly understood. In particular, the invest-
igation into the intermixing in the lateral direction
0022-0248/00/$- see front matter 2000 Elsevier Science B.V. All rights reserved.
PII: S 0 0 2 2 - 0 2 4 8 ( 0 0 ) 0 0 7 7 3 - 9
Fig. 1. Low-temperature PL spectra (at 77 K) obtained from the
InAs QDs with InGaAs overgrowth layer (sample C) unannealed
and annealed at di!erent temperatures (700}8503C) for 60 s.
is rarely reported. Such information is directly rel-
evant to understanding the optical changes of QDs
subjected to RTA.
In this paper, we propose and demonstrate a QD
structure for estimating the e!ects of intermixing in
the lateral direction. The 3-nm-height InAs/GaAs
QDs covered by 3-nm-thick In
V
Ga
V
As (x"
0, 0.1, 0.2, and 0.3) overgrowth layer have been
fabricated [10]. The atomic force microscopy
measurements indicate that the surface topography
of InAs islands covered by In
V
Ga
V
As (x)0.2)
becomes #atter [10]. Because the thickness of In-
GaAs overgrowth layers equals the QD height, the
lateral intermixing will be suppressed during RTA
process and the InGaAs overgrowth layer will have
a little in#uence on the intermixing in the vertical
direction. Therefore, the in#uence of lateral inter-
mixing on the QD optical characteristics can be
studied using these samples. Our experimental re-
sults indicate that the In}Ga intermixing in the
lateral direction has a strong in#uence on the re-
duction of PL linewidth and a minute e!ect on the
blueshift in QD emission energy. In addition, we
have observed the photoluminescence peak of In-
GaAs layer at lower-energy side of InAs quantum-
dot PL peak for the samples annealed at higher
temperature.
2. Experimental procedure
The samples studied here were grown on GaAs
(1 0 0) substrates by a conventional solid source
molecular beam epitaxy system (MBE) using Riber
32P machine. The growth order of our sample
structure is a 500-nm GaAs bu!er layer, a 2.0-ML
InAs QDs layer, a 3-nm In
V
Ga
V
As layer (x"0
for sample A, 0.1 for sample B, 0.2 for sample C,
and 0.3 for sample D), and a 100-nm GaAs cap
layer. The InAs and InGaAs layers were grown at
5003Cand the GaAs bu!er and cap layers at 5803C.
The formation of 3D islands was signalled by the
abrupt change from a streaky re#ection high-en-
ergy electron di!raction pattern to a spotty one.
A detailed account of the growth and structural
information of these samples has been published
elsewhere [10]. After deposition of 100-nm SiO
`
,
the samples were subjected to RTA in an argon
ambient at the temperature range from 650 to
8503C for 60 s. Then the SiO
`
layers were removed
by dipping the samples in HF solution for PL
measurements, which were performed in closed-
cycle He cryostat under the exciton of 514.5-nm
line of an Ar> laser. The luminescence spectra were
detected with a Fourier transform infrared spec-
trometer operating with an InGaAs photodetector.
3. Results and discussion
Fig. 1 shows the low-temperature PL spectra (at
77 K) obtained from sample C unannealed and
annealed at di!erent temperatures (700}8503C).
The post-growth RTA treatments lead to a blue-
shift (up to 140 meV) in the emission energy and
a narrowing of the full-width at half-maximum
(FWHM) from 35 meV of the as-grown sample to
17 meV of the samples annealed at 8503C. The
changes induced by RTA are similar to those re-
ported for InAs/GaAs QDs. However, a lower-
energy PL shoulder appears at 1.28 eV for sample
C annealed at 7503C, which has not been observed
for In(Ga)As QDs subjected to RTA. Moreover, the
H.Y. Liu et al. / Journal of Crystal Growth 220 (2000) 216}219 217
Fig. 2. Low-temperature PL spectra (at 77 K) obtained from the
InAs QDs with In
V
Ga
V
As (x"0, 0.1, 0.2, and 0.3) overgrowth
layer annealed at 8003C for 60 s.
Fig. 3. Annealing temperature dependence of the PL energy of
samples A, B, and C.
increment of annealing temperature induces a red-
shift in the emission energy of lower peak.
The low-energy peak has also been detected in
the PL spectra of InAs QDs covered by In
"
Ga
""
-
As and In
"`
Ga
"`
As layers. Fig. 2 shows the
emission from InAs/GaAs QDs with InGaAs layer
annealed at 8003C. However, the broad PL peak
has not been observed at lower-energy side of InAs
emission peak for sample A.
These results indicate that the broad lumines-
cence peak cannot be attributed to InAs QDs, due
to the redshift in the PL energy with increasing the
RTA temperature shown in Fig. 2 [1}8]. Here, we
believe that this peak corresponds to the emission
of InGaAs overgrowth layer. The band gap of In-
GaAs overgrowth layer is larger than that of InAs
QDs in as-grown samples. Thus, the PL peak of
InGaAs in unannealed sample has not been detec-
ted. For InAs/GaAs QDs, the RTA treatments will
result in a larger blueshift of QD peak energy.
However, the e!ects of RTA on the optical proper-
ties of quantum wells (QWs) are much smaller than
those for QDs. The blueshift induced by pos-
tgrowth thermal treatments in PL energy of QWs
cannot be clearly observed at low annealing tem-
perature ((8003C) [2,8]. Therefore, with in-
creasing the annealing temperature, the band gap
of InAs QDs will become larger than that of In-
GaAs quantum well. With further increasing the
annealing temperature, the interdi!usion of In}Ga
will lead to the increment of In mole fraction in the
InGaAs overgrowth layer, resulting in the redshift
of PL energy.
Next we will discuss the relative changes of optical
properties induced by RTA for InAs/GaAs QDs
with the di!erent-In-mole-fraction InGaAs over-
growth layer. Fig. 3 shows the annealing temper-
ature dependence of the peak position of PL spectra
for samples A, B, and C. It can be clearly seen that
the trend of blueshift in emission energy is similar for
all samples. However, the reduction of PL linewidth
depends strongly on the composition of InGaAs
overgrowth layer, as shown in Fig. 4. The reduction
of PL linewidth decreases with increasing the In
mole fraction in the InGaAs overgrowth layer.
Even at the annealing temperature of 8503C, the
FWHM of sample C is the largest. This result is
unexpected for us, because the PL linewidth of
sample C is the least in the as-grown samples [10].
In general, the blueshift in emission peak and the
reduction of PL linewidth of InAs/GaAs QDs in-
duced by RTA have been explained by the In}Ga
interdi!usion between InAs QDs and GaAs barrier
layer [6,9]. Since the height of QDs is much smaller
than the QD lateral size, the blueshift in PL peak
energy induced by RTA process will mainly result
from the change in the vertical direction [6]. Al-
though InAs/GaAs QDs are covered by InGaAs in
our samples, the InGaAs overgrowth layer will
have a weak in#uence on intermixing in the vertical
direction. Therefore, the trend of blueshift in PL
218 H.Y. Liu et al. / Journal of Crystal Growth 220 (2000) 216}219
Fig. 4. Annealing-temperature-dependent FWHM of PL peaks
of samples A, B, and C.
energy shown in Fig. 3 is similar for all samples. On
the other hand, the e!ective increment in the QD
height and the reduction of con"ning potential
have been proposed to explain the reduction of PL
linewidth of QDs induced by RTA [6,9]. However,
the relative changes of PL linewidth shown in Fig.
4 cannot be explained only in terms of the reduc-
tion of con"ning potential, because the PL peak
positions of samples B and C are similar at every
annealing temperature (indicated in Fig. 3). Here,
we propose that the relative changes of PL
linewidth can be explained in terms of the in#uence
of lateral intermixing between InAs QDs and bar-
rier layer. For the InAs QDs covered by GaAs, the
In}Ga intermixing in the lateral direction is larger
than that in the vertical direction, due to the anisot-
ropic strain distribution at the interface [7,8,11].
Therefore, the relative quantum e!ects in the lateral
direction of QDs will become weaker, when the QD
samples are annealed at higher temperature. How-
ever, the lateral intermixing will be suppressed for
the samples covered by InGaAs, resulting in the
relative increment of quantum e!ects in the lateral
direction. For the samples subjected to RTA, the
e!ects of the lateral size distribution on the PL
linewidth will be enhanced upon increasing the In
mole fraction in the overgrowth layer. Therefore,
the changes of InAs/GaAs QD PL linewidth in-
duced by RTA will decrease with increment of the
In mole fraction in InGaAs overgrowth layer.
4. Summary
In conclusion, the e!ects of lateral intermixing
between QDs and barrier layer have been investi-
gated by the RTA treatments of InAs/GaAs QDs
covered by InGaAs overgrowth layer. It is found
that the trend of blueshift in PL QD energy is
similar for all samples. However, the changes of PL
linewidth decrease with increasing the In mole frac-
tion in the overgrowth layer. Even at the annealing
temperature of 8503C, the FWHM of InAs/GaAs
QDs covered by In
"`
Ga
"`
As layer is the largest,
although its value is the least in the as-grown sam-
ples. We attribute the changes of PL linewidth
observed here to the suppression of lateral inter-
mixing. In addition, at higher annealing temper-
ature (*7503C), the photoluminescence peak of
InGaAs layer has been observed at the lower-en-
ergy side of InAs quantum-dot peak.
Acknowledgements
This work was supported by the National Natu-
ral Science Foundation of China under contract
No. 69736010 and by the National Advanced Ma-
terials Committee of China.
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