Journal of Alloys and Compounds 872 (2021) 159470

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Journal of Alloys and Compounds

journal homepage: www.elsevier.com/locate/jalcom

Effect of GaAs insertion layer on the properties improvement of

InGaAs/AlGaAs multiple quantum wells grown by metal-organic ]]
]]]]]]
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chemical vapor deposition

⁎
Bin Zhang, Haizhu Wang , Xu Wang, Quhui Wang, Jie Fan, Yonggang Zou, Xiaohui Ma
State Key Laboratory of High Power Semiconductor Laser, Changchun University of Science and Technology, Changchun, Jilin, China

a r t i cl e i nfo a bstr ac t

Article history: Multiple quantum wells (MQWs) are commonly employed in InGaAs/AlGaAs semiconductor materials for
Received 7 October 2020 devices such as semiconductor lasers and solar cells. However, the Indium atoms’ problems of segregation
Received in revised form 16 February 2021 and large surface roughness, due to the different growth temperatures of well and barrier layers, have not
Accepted 7 March 2021
yet been solved. In the present work, a GaAs material was designed as an insertion layer (ISL) and used in
Available online 18 March 2021
the structure of the InGaAs/AlGaAs MQWs. The study found that when the thickness of the GaAs ISL was
6 nm, the maximal properties of the InGaAs/AlGaAs MQWs were achieved. Various theoretical and
Keywords:
InGaAs/AlGaAs experimental studies were performed to measure the crystal’s purity to elucidate the reasons for improving
GaAs insertion layer the InGaAs/AlGaAs MQWs. The measurements indicated that the AlGaAs barrier guaranteed more radiative
MQWs recombination in the MQWs’ structure while simultaneously ensuring the GaAs ISL diminished surface
roughness and the Indium atoms’ segregation. The design of the InGaAs/AlGaAs MQWs creates new
opportunities for innovative applications of next-generation diode lasers with optimized integration.
© 2021 Elsevier B.V. All rights reserved.

1. Introduction a lattice-mismatch-induced compressively strained quantum well

InGaAs/GaAs multiple quantum wells (MQWs) have been
extensively used for laser diodes, photodetectors, and various op­
toelectronic devices [1–3]. However, there is a problem that the
potential barrier height of GaAs is not sufficiently higher than the
InGaAs wells when InGaAs/GaAs MQWs are used as the lasers’ active
region with an emitting wavelength near 900 nm. Additionally, to
obtain ideal high-temperature optoelectronic device performance, it
is essential to have very deep quantum wells to reduce carrier
leakage [4–7]. Compared to the GaAs barrier, the AlGaAs material
has a higher potential barrier with nearly the same lattice constant.
Therefore, the InGaAs/AlGaAs MQWs can be effectively employed in
semiconductor lasers with a wavelength between 880 and 940 nm.
InGaAs/GaAs mismatched strained MQWs have been intensively
investigated, suggesting that it leads to defects and deterioration in
the epitaxial structure’s crystal quality, influencing device perfor­
mance [8,9]. However, a relatively small level of strain can change
the energy band structure. It has been demonstrated that a laser’s
optical gain and threshold current could be improved by introducing
⁎
Corresponding author.
E-mail address: whz@cust.edu.cn (H. Wang).
(QW) as the active region [10]. Theoretically, the strain induces a
change in the band-gap, while heavy-hole and light-hole states split
at the top of the valence band [11]. When the compressive strain due
to lattice mismatch is incorporated, one may obtain the growth of
high-quality dislocation-free InGaAs/AlGaAs MQWs structure in
which the InGaAs materials are entirely under elastic strain [12,13].
There are still numerous outstanding questions about the
InGaAs/AlGaAs MQWs grown by metal-organic chemical vapor
deposition (MOCVD) [14–16]. First, the AlGaAs layer’s growth needs
a higher temperature to reduce unintentional carbon and oxygen
impurity and promote the Al atoms migration over the surface
[17,18]. A large temperature difference exists in the epitaxy process
since the appropriate growth temperature of AlGaAs layers is higher
than that of InGaAs. Meanwhile, the higher temperature for InGaAs
layers growth may result in the Indium atoms surface segregation
[19–21]. Second, the InGaAlAs alloy is probably formed at the in­
terface between the InGaAs well layers and the AlGaAs barrier
layers. Both factors are believed to be unfavorable for optical and
crystal performance. Thus, much research has been dedicated to
solving these problems. Shi et al. had reported the technological
approach that “Lower temperature grows AlGaAs capping layer” for
improving the barrier upper surficial planeness and QW interfacial
quality by molecular beam epitaxy (MBE) [16]. However, there is

https://doi.org/10.1016/j.jallcom.2021.159470
0925-8388/© 2021 Elsevier B.V. All rights reserved.
B. Zhang, H. Wang, X. Wang et al. Journal of Alloys and Compounds 872 (2021) 159470

limited research on the method of InGaAs/AlGaAs MQWs grown via

MOCVD [22]. The main reason is that the AlGaAs layer needs to be
prepared at a higher temperature, influencing the overall crystal
quality. The insertion layer (ISL) is proposed as a structural design
method and used in the InGaAs/AlGaAs MQWs. Considering the In­
GaAs/AlGaAs MQWs, AlAs and GaAs can be selected as the ISL. It is
found that the AlAs submonolayer inserted into GaAs/AlGaAs QWs
can not only efficiently modify the intersubband transition between
the ground state and the first excited state, but also change the
electron-phonon scattering and effective mass of electrons [23].
However, for the AlAs material, the band-gap is much greater than
that of the InGaAs quantum well, which leads to a capacity reduction
in pump absorption and carrier transport. Meanwhile, the AlAs
materials are easily oxidized, and the segregation of Indium atoms
will occur at high temperature, which will have a significant impact
on crystal quality and device performance. So, the AlAs material will
not be studied as the InGaAs/AlGaAs MQWs ISL in this paper. Since
the GaAs material does not contain randomly situated impurities,
there is a decrease in the probability of carrier scattering in MQWs.
Furthermore, it has been demonstrated in numerous studies that
this could decrease interface roughness [24] and lead to stronger
photoabsorption (promote carrier escape) [25,26]. Therefore, the Fig. 1. The schematic structure of InGaAs/AlGaAs MQWs.

GaAs material as ISL is an ideal choice.

In this paper, the GaAs as the ISL was designed and used between Table 1
InGaAs and AlGaAs layers, and the InGaAs/AlGaAs MQWs were The details of the MQWs growth process.
prepared via MOCVD technology. Furthermore, the growth tem­ Materials Growth temperature (°C)
peratures of InGaAs and AlGaAs layers were optimized in the growth Al0.3Ga0.7As 680
process to solve the problems mentioned above. The effect of the GaAs 600
GaAs ISL thicknesses on the performance of MQWs was studied. The In0.15Ga0.85As 600
research showed considerable potential for applications controlling GaAs 680
Al0.3Ga0.7As 680
the InGaAs/AlGaAs MQW structure with GaAs ISL as the lasers’ active
region in the 880–940 nm range.

2. Experiment
The InGaAs/AlGaAs MQWs were grown on an (001) n-type GaAs
substrate in a low-pressure horizontal MOCVD reactor produced by
Aixtron (AIXTRON 200/4) in Germany. Trimethylgallium (TMGa),
trimethylindium (TMIn), trimethylaluminum (TMAl), and arsine
(AsH3) were used as the precursor. The reactor pressure was fixed at
100 mbar. All the MO sources were carried by high-purity hydrogen
(H2) gas. Before the growth process started, the substrate was baked
for 5 min at 650 °C, and a 300 nm GaAs buffer layer was grown on a
GaAs substrate. Fig. 1 shows a schematic of the InGaAs/AlGaAs
MQWs structure, which comprised a 300 nm GaAs buffer layer, 8 nm
Al0.3Ga0.7As barrier layer, x nm GaAs ISL, 6 nm In0.15Ga0.85As well
layer, x nm GaAs ISL, 8 nm Al0.3Ga0.7As barrier layer, and 150 nm
GaAs capping layer.
The MQWs structure, with thickness x for the GaAs ISL (where
x = 0, 2, 4, 6, and10 nm), was grown, and the samples were defined
from A to E, respectively. The MQWs structure contained three
periods of InGaAs/AlGaAs MQWs, a 6 nm InGaAs quantum well, and
an 8 nm AlGaAs barrier to prevent dislocation caused by excessive
strain. The details of the MQWs’ growth process are shown in
Table 1. In order to avoid the Indium atoms segregation at a higher
temperature, different growth temperatures were chosen for
GaAs ISL at 600 °C and 680 °C. A thickness of 0 nm represents the
InGaAs/AlGaAs MQWs without a GaAs ISL. Typically, a thickness of
10 nm represents the InGaAs/GaAs MQWs with a GaAs ISL; the
whole structure was grown at 600 °C.
To estimate the optical properties, crystalline quality, and inter­
face roughness for all samples, the surficial morphology, and the root
mean square (RMS) surface roughness were analyzed by atomic
force microscopy (AFM). The optical properties of MQWs were
measured by photoluminescence (PL) spectroscopy (RPM 2000) at
room temperature (RT), and the wavelength and power density of
the light source were 532 nm and 2.05 W/cm2, respectively.
The heterogeneous interfacial quality was characterized by high-
resolution X-ray diffraction (HRXRD) Omega-2Theta scanning at
40 kV and 40 mA using Cu 2Kα X-rays with a 1.5418Ȧ wavelength,
0.05° step, and 0.3°/min scanning speed between 60° and 70°. The
thickness of each layer of the sample was probed by high-resolution
scanning electron microscopy (SEM).
3. Results and discussion
3.1. PL spectra analysis of the InGaAs/AlGaAs MQWs
In order to verify the effect of GaAs ISL in the InGaAs/AlGaAs
MQWs, all samples were measured by PL at RT; the results are
shown in Fig. 2. In Fig. 2, two peaks are observed at 870 and 930 nm
corresponding to GaAs substrate material and the InGaAs/AlGaAs
MQWs (ground state electron-heavy hole band), respectively.
Meanwhile, a shoulder peak, located at about 900 nm, is also
observed when the GaAs ISL thickness is 2, 4, and 6 nm. To further
analyze the shoulder peak, the PL spectra of the 6 nm thick GaAs ISL
was selected and fitted; the result is shown in the inset of Fig. 2.
According to eight-band Kane-type k·p Hamiltonian analysis and the
different quantization conditions (spin-orbit coupling, different
eigenstates) in the InGaAs/AlGaAs MQWs, the quantum confinement
energies create heavy-hole (HH) and light-hole (LH) bands valence
band splits [27]. Consequently, the band structure is composed of
two twice-degenerate isotropic valence bands with heavy-hole
effective masses mhh and light-hole effective masses mlh, with the
heavy-hole band at the valence band maximum. It is demonstrated
that the strain and quantum-confinement effects play an in­
dependent role in determining the subband energy spacings in
compressively strained wells [28]. Furthermore, the reduction of

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B. Zhang, H. Wang, X. Wang et al. Journal of Alloys and Compounds 872 (2021) 159470

Fig. 2. PL spectra of InGaAs/AlGaAs MQWs grown on (001) GaAs substrate with Fig. 3. The FWHM with different thicknesses of GaAs insertion layer.
different thicknesses of GaAs insertion layer at RT. The inset shows the PL spectra of
6 nm-thick GaAs insertion layer with a Gaussian line shape fitting.
MQWs [29,34]. However, when the GaAs ISL thickness exceeds a
mave (averaged effective mass of the lowest subband) tends to special value, the GaAs layers will replace the AlGaAs layer as actual
saturate as the compressive strain exceeds 1.0%. The subband energy barriers and promote carriers escape [25].
spacing (△E) between the HH1 and LH1 slightly increases when a The model of recombination process of photoexcited carriers was
small amount of strain is applied. However, it also tends to saturate established to explain why the PL intensity of the InGaAs/AlGaAs
as the compressive strain exceeds 1.0%. This energy spacing is the MQWs increases with the change of thickness of the GaAs ISL, as
main reason that the LH subbands move away from the band edge shown in Fig. 4. The model consists of three relaxation processes: (i)
when compressive strain is considerable, which weakens its influ­ thermal escape from InGaAs well, (ii) non-radiative, and (iii) radia­
ence on ΔE and mave. Therefore, quantum confinement is a dominant tive carrier recombination within the InGaAs well [35]. According to
factor in determining the amount of ΔE in compressively strained the model, the probability of thermal escape of electrons from an
wells. Moreover, from the inset of Fig. 2, it can be seen that the InGaAs quantum well is reduced based on the AlGaAs barrier,
shoulder peak is considered as the recombination of the ground increasing the radiation recombination of photoexcited carriers.
state electron-light hole band (1e-1lh) in the InGaAs MQWs [29]. According to the PL spectral image, the InGaAs/AlGaAs MQWs
Fig. 2 shows the PL peak wavelength of MQW blue shifts with with the GaAs ISL, such as samples B–D, exhibit a significant increase
increasing thickness of the GaAs ISL, attributed to the Indium in the PL intensity. It can be concluded that the higher PL intensity
segregation. The Indium segregation appears in the InGaAs/AlGaAs results from fewer thermal escapes in the MQWs. Because of the
interface, predominating at the higher growth temperature, lower GaAs potential barriers, the probability of thermal escape of
resulting in reducing the Indium composition in the InGaAs layer. carriers from the InGaAs well increases. However, the probability of
When the segregation length exceeds the ISL thickness, the Indium non-radiative recombination predominates for sample A with the
atoms will enter the AlGaAs layers to form the quaternary com­ thinner GaAs ISL. The proper GaAs ISL thickness (x = 6 nm, sample D)
pound of InGaAlAs. The InGaAlAs compound will become a
non-radiative recombination center, which results in the reduction
of the PL intensity [30,31]. For sample E (InGaAs/GaAs MQWs), the
Indium diffusion is limited inside the GaAs layers, comparable to
when GaAs barriers encapsulate the InGaAs well layers; the
InGaAlAs compound is also not formed. However, the PL intensity of
sample E is much lower than other samples and is insufficient.
Additionally, it is observed that the PL intensity of sample D is the
strongest of all the samples.
Subsequently, to further evaluate the crystal quality of InGaAs/
AlGaAs MQWs, the full width at half maximum (FWHM) of PL as a
function of GaAs ISL thicknesses was extracted and plotted in Fig. 3.
It is found that the FWHM of the PL spectrum broadens with the
decreasing thickness of the GaAs ISL, indicating the deterioration of
interface quality, the uniform incorporation of Indium into the
AlGaAs layers, and more scattering losses at heterogeneous interface
fluctuation [32,33]. The confined energy level of the potential barrier
height increases utilizing AlGaAs as the barrier so that more carriers
are trapped in the InGaAs wells [6,31]. Furthermore, the GaAs ISL can
decrease the Indium atoms composition fluctuation and alloy
broadening effects. In particular, the condition that some carriers Fig. 4. Three proposed carrier relaxation processes based on the van Roosbroeck
involved in the processes of non-radiative recombination formed by Shockley treatment: the signal generation efficiency for thermal escape, non-radiative,
the InGaAlAs compound diminish the PL intensity of InGaAs/AlGaAs and radiative recombination.

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B. Zhang, H. Wang, X. Wang et al. Journal of Alloys and Compounds 872 (2021) 159470

increases the PL intensity of the InGaAs/AlGaAs MQWs, which may

be closely related to raising the probability of radiative recombina­
tion. Theoretical formulas and testing data were discussed to
support the result that the GaAs ISL can decrease the probability of
non-radiative recombination and further enhance the optical
performance. The PL signal generation efficiency can be defined by
the following equation, according to the van Roosbroeck-Shockley
treatment [36]:
1/ R
PL = ,
1/ R + 1/ NR + 1/ th (1)
where τth, τNR, and τR are the thermal escape, non-radiative, and
radiative recombination times, respectively. Furthermore, τNR and τth
are temperature-dependent, as denoted by the following
equations [37]:
1 ENR
= C0 exp and
NR KT (2)

1 1 KT Ebarr. (F) Fig. 5. Schematic illustration of MQWs structure.

= exp ,
th W 2 mW KT (3)
where mw is the effective carrier mass in the quantum well, mb is the by AFM; the results are shown in Fig. 7. Accordingly, the value of
effective carrier mass in the barrier, W is the well width, b is the RMS surface roughness of samples A, D, and E was calculated to be
barrier width, and Ebarr.(F) is the barrier height for the nth energy 0.683, 0.263, and 0.473 nm, respectively [39].
subband. In the presence of an electric field F, the barrier height can According to the AFM measurement results, it is evident that the
be written as growth mode completely follows the two-dimensional step flow
mode with the introduction of the GaAs ISL. Even though the lattice
FW
Ebarr. (F) = ECB Ee1 q , mismatch between InGaAs and GaAs is merely 1.07%, the surface
2 (4)
morphology’s deterioration is caused by the accumulation of com­
where ΔECB is the conduction or valence band offset, Ee1 the energy pressive strain in each layer. Fig. 7(a) shows when the terrace height
of the first energy subband measured from the center of the well, fluctuation and bulges are much more apparent than other fluc­
and q the electron charge. tuations, the terrace edges become bent, and the interface crystal
Furthermore, the IQE (internal quantum efficiency) ƞIQE is, by quality of the InGaAs/AlGaAs has been deteriorated [9]. Furthermore,
definition, the ratio between the radiative recombination rate and while the thickness of the GaAs ISL reaches 6 nm, the surface mor­
the total carrier generation rate [38]: phology improves; the surface of sample D flattens, and the RMS
1/ R value is 0.263 nm, which is significantly enhanced compared to the
IQE = . other samples, as shown in Fig. 7(b). The main reason is that the
1/ NR + 1/ R (5)
thickness of GaAs ISL exceeds the segregation length of the Indium
According to these formulas, both ƞPL and ƞIQE are affected by atoms and the lower fluctuation of Indium compositions. Combined
radiative recombination and non-radiative recombination. with the PL measurement result of sample D, sample D’s crystal
Significantly, the effects are beneficial to ƞPL and ƞIQE when non- quality is excellent, making the FWHM modulation narrow and the
radiative recombination is reduced. To further confirm that the IQE PL intensity increase. For sample A, the AFM image and the PL
and radiative recombination are enhanced by weakening the spectrum show poor results due to the deterioration of crystal
non-radiative recombination caused by defects and interface quality rather than barrier height reduction. Simultaneously, it
roughness, the AFM and XRD will be used to test the quality of suggests that an increased interface roughness generated by the
crystal growth, and the thickness of the GaAs ISL can be precisely deterioration of crystal quality could increase the probability of
determined via SEM testing in the following work.

3.2. Description of surface and cross-section

A special epitaxial structure was devised and grown to accurately

calibrate the thickness of GaAs ISL, as shown in Fig. 5. The structure,
which consists of a 150 nm GaAs layer, an MQWs structure, and
another 150 nm GaAs layer, is grown three cycles on the 300 nm
GaAs buffer layer. The MQW structure contains an 8 nm Al0.3Ga0.7As
barrier layer, 2 nm GaAs ISL, and 6 nm In0.15Ga0.85As. The SEM
measurement shows much higher contrast among the InGaAs well
layer, GaAs ISL, and the AlGaAs barrier layer, as shown in Fig. 6,
suggesting that the interfaces are discrete and without any thickness
fluctuation. In order to reduce the experimental error, the entire
thickness of Al0.3Ga0.7As and GaAs layers, the Al0.3Ga0.7As, GaAs, and
InGaAs layers, and the whole three cycles of MQWs were as 10.25,
15.66, and 75.54 nm, respectively. The SEM measurements show the
targeted thickness is reasonably accurate.
To analyze the surface roughness of the InGaAs/AlGaAs MQWs,
the surface morphologies of samples A, D, and E were characterized Fig. 6. The image of the cross-section of the grown MQWs sample.

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B. Zhang, H. Wang, X. Wang et al. Journal of Alloys and Compounds 872 (2021) 159470

Sample E’s roughness is relatively high, with measured surface

roughness it is as large as RMS = 0.683 nm. Distinctly parallel and
straight periodical stripes are observed, as shown in Fig. 7(c), where
the terraces’ height is comparable to 2 monolayers (MLs). It is
speculated that the increased roughness in surface topography is
attributed to the different migrant lengths of Ga and Al atoms
[40,41]. Moreover, the increased surface roughness and the lower
GaAs barrier would weaken the PL intensity for sample E, as shown
in Fig. 2.

3.3. XRD rocking curves discussion

To get an evaluation of the hetero-interface quality for the

InGaAs/AlGaAs MQWs, the XRD Omega-2Theta (degree) diffraction
patterns for different thicknesses of the GaAs ISLs are shown in
Fig. 8. The strongest and narrowest peak is the GaAs (400) substrate.
The diffraction patterns of all samples show distinctly periodical
diffraction peaks, indicating their periodical structures and highly
crystallization quality, which is in accordance with the three-period
InGaAs/AlGaAs MQWs structure.
Nevertheless, many disturbances, such as thickness fluctuations,
composition nonuniformity, interface roughness, and strain relaxa­
tion in the MQWs structure, broaden each order satellite peaks
[35,42]. From the measurement results of Fig. 8 and Fig. S1, it can be
seen that the higher-order satellite peaks and the narrower FWHM
of each order satellite peak corresponded to sample D. When the
thickness of the GaAs ISL was 6 nm, the number of satellite peaks
reached a maximum (about six satellite peaks). Notably, compared
to sample D, the FWHMs of each order satellite were irregular and
exhibited inferior structure quality for the other samples [43].

Fig. 7. The AFM images of InGaAs/AlGaAs MQWs in 3 × 3 µm2 scanning area with
different GaAs insertion layer thicknesses: (a) 0, (b) 6, and (c) 10 nm.

carriers’ scattering and lower the radiative recombination that can

only contribute to optical gain, which is in close agreement with the
Fig. 8. XRD Omega-2Theta(ω-2θ) scans measured patterns for different GaAs inser­
PL characteristic. tion layer thicknesses.

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B. Zhang, H. Wang, X. Wang et al.
Therefore, all the measurement results indicate that the crystal
quality and luminescence properties of the InGaAs/AlGaAs MQWs with
the 6 nm GaAs ISL were optimal. Moreover, it was generally accepted
that non-radiative recombination decreases as the interface defects
decrease; thus, high internal quantum efficiency (IQE) and excellent PL
performance are promising [38]. The superior crystal quality could be
ascribed to the higher growth temperature for the AlGaAs layer, which
would effectively reduce the impurity concentration, and the GaAs ISL
could separate the well and barrier layer.
4. Conclusion
According to the analysis and discussion of the samples’
measurements, the InGaAs/AlGaAs MQWs with a 6 nm GaAs ISL
were superior to the other samples with or without the different
thicknesses of the GaAs ISL. The optimal GaAs ISL could significantly
increase the PL intensity and narrow the FWHM, which indicated it
had excellent crystal and hetero-interface quality. In addition, the
AFM and XRD measurements also revealed that crystal perfection
and surface smoothness of MQWs had been achieved. It could be
attributed to the GaAs ISL and higher AlGaAs barrier, which made it
possible to avoid the impact of the InGaAlAs compound and improve
the radiative recombination performance in the wells. Therefore,
this technology could be widely used in the epitaxial growth of
semiconductor devices.
CRediT authorship contribution statement
Bin Zhang: Investigation, Formal analysis, Writing - original
draft, Writing - review & editing. Haizhu Wang: Writing - original draft,
Writing - review & editing, Formal analysis, Supervision. Xu Wang:
Writing - original draft. Quhui Wang: Formal analysis. Jie Fan: Funding
acquisition. Yonggang Zou: Funding acquisition. Xiaohui Ma: Project
administration, Supervision, Funding acquisition.
Declaration of Competing Interest
The authors declare that they have no known competing fi­
nancial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgment
This work is supported by the National Science Foundation for
Young Scientists of China (Grant No. 21707010), the 13th Five-Year
Science and Technology Research Foundation of Education
Department of Jilin Province (Grant No. JJKH20181114KJ), Jilin
Science and Technology Development Plan (Grant Nos.
20180519018JH, 20190302052GX), Excellent Youth Foundation of
Jilin Province (Grant No. 20180520194JH), and Changchun University
of Science and Technology Youth Science Foundation (Grant No.
XQNJJ-2017–20).
Appendix A. Supporting information
Supplementary data associated with this article can be found in
the online version at doi:10.1016/j.jallcom.2021.159470.
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