Materials Science and Engineering B93 (2002) 131
/134

www.elsevier.com/locate/mseb

Structural and optical characterization of thick InGaN layers and

InGaN/GaN MQW grown by molecular beam epitaxy
F.B. Naranjo a,*, S. Fernández a, M.A. Sánchez-Garcı́a a, F. Calle a, E. Calleja a,
A. Trampert b, K.H. Ploog b
a
ISOM and Departamento de Ingenierı́a Electrónica, ETSI Telecomunicación, Universidad Politécnica de Madrid, Ciudad Universitaria, 28040 Madrid,
Spain
b
Paul-Drude-Institut fuer Festkoerperelektronik, Hausvogteiplatz 5-7, D-10117 Berlin, Germany

Abstract

Thick Inx Ga1x N (0.20B x B 0.27) layers and InGaN/GaN multiple quantum wells (MQWs) are grown by plasma-assisted
molecular beam epitaxy on GaN/Al2O3 templates. The strain and In-content is estimated from high-resolution X-ray diffraction,
showing that the bulk samples are not fully relaxed. A bowing parameter of 3.6 eV is obtained from absorption measurements of
Inx Ga1x N layers. Strong In-dependent excitonic localization is observed in these bulk layers, leading to an increase in the
absorption band edge with the In content. Regarding the MQWs structures, high-resolution transmission electron microscopy
reveals an increase in the interface roughness for high In content. The dominant PL emission of the MQWs shows a red-shift when
increasing the well thickness for a given In-content, due to internal piezoelectric field. The excitonic localization is studied and
compared between thick layers and MQWs structures. # 2002 Elsevier Science B.V. All rights reserved.

Keywords: InGaN; Molecular beam epitaxy; Transmission electron microscopy; Localization; Strain

1. Introduction
InGaN-based light emitting diodes (LED) and laser
diodes (LD) grown on sapphire substrates by metal
/
organic chemical vapor deposition (MOCVD) techni-
ques have been demonstrated in the recent years [1].
However, there are many aspects of the growth of this
material that are still not well understood. In particular,
the thermodynamical unstability of the GaN
/InN alloy
has been a subject of many reports [2]. This effect, and
the segregation of In at the surface during growth, are
some reasons that make the growth conditions of this
material so critical [3]. Molecular beam epitaxy (MBE)
has attracted much attention, due to the in situ control
of the growth using reflection high energy electron
diffraction (RHEED) and the possibility of achieving
abrupt interfaces. The lower temperature decomposition
* Corresponding author. Tel.: 34-91-549-5700x420; fax: 34-91-
336-7323.
E-mail address: naranjo@die.upm.es (F.B. Naranjo).
0921-5107/02/$ - see front matter # 2002 Elsevier Science B.V. All rights reserved.
PII: S 0 9 2 1 - 5 1 0 7 ( 0 2 ) 0 0 0 3 2 - 6
of InN (630 8C) compared with GaN (850 8C) [4] gives
rise to the need of lower growth temperatures for
InGaN layers (around 580 8C). In this aspect, MBE
allows the use of these low temperatures. On the other
hand, the quality of the GaN grown by MBE on
sapphire is generally not as good as MOCVD-grown
samples. With the use of MOCVD-GaN templates for
MBE (homoepitaxy), this problem could be avoided [5].
The study of InGaN-based multiple quantum wells
(MQW) is necessary to improve the performance of
the devices. In this paper we report on the growth and
characterization of bulk InGaN layers and InGaN/GaN
MQW by MBE on GaN templates. The characterization
is performed in order to compare the emission mechan-
ism in both kinds of samples.
2. Experiment
InGaN layers and MQWs were grown on 2-mm thick
MOCVD-GaN templates. The growth was performed in
132 F.B. Naranjo et al. / Materials Science and Engineering B93 (2002) 131
/134

a commercial MECA2000 MBE system. Active nitrogen 3. Results

was provided using a RF plasma source from Oxford
Applied Research while conventional Knudsen cells
were employed for In, Ga and Al sources. More details 3.1. InGaN bulk layers
about the system configuration can be found elsewhere
[6]. Fig. 1 shows the low temperature (8 K) PL from
The templates were Ti coated (back side) and cleaned different InGaN bulk layers, an emission energy in-
with organic solvents before loading in the MBE system. crease is observed when decreasing the In content.
Prior to the growth, the substrates were outgassed in the Multiple peak emission is due to Fabry
/Perot oscilla-
growth chamber at 650 8C during 30 min. The growth tions in the whole structure (InGaNGaN buf-
ferGaN MOCVD 2.72 mm).
temperature was monitored using an optical pyrometer
To study the excitonic localization effect and its
focused at the surface of the sample.
dependence with the In content, temperature-dependent
A 300-nm thick MBE-GaN buffer layer was grown to
PL measurements were carried out. The results were
avoid the template surface contamination at 700 8C.
compared to absorption data, which were derived from
The temperature was then decreased for the growth of
the measured transmission using the relation
the InGaN/GaN MQW and bulk layers to 560
/600 8C.
a (E )8 ln(T ). The effective band gap, EG,eff, and an
Five periods of Inx Ga1x N/GaN were grown with the
estimation of the band edge broadening, DE , were
In mole fraction (x ) in the range 0.06
/0.16. The
calculated within a sigmoidal absorption approxima-
quantum well and barrier thickness were changed
tion,
between 3
/5 and 5
/9 nm, respectively. For comparison,
a set of 300-nm InGaN bulk layers were grown on a a0
a(E) (1)
similar GaN buffer layer. The amount of active nitrogen EG;eff  E
1  exp
was kept constant using a RF power of 400 W and a DE
nitrogen flow of 1.0 sccm for all the layers, quantum
wells and barriers. Fig. 2a and b shows the PL emission evolution with
For all the samples, a 2 2 surface reconstruction is temperature for two samples with 20 and 27% In,
observed after the growth of the initial GaN layer and respectively. The layers are not fully relaxed with this
cooling down of the sample, right before the InGaN thickness (300 nm) and a relaxation degree of 0.51 and
growth, indicating a smooth (2D) GaN surface. 0.86, respectively, was estimated using HRXRD. In
High resolution X-ray diffraction (HRXRD) was both samples, a clear red-shift is observed for tempera-
employed to assess the amount of strain and the In tures below 200 and 150 K, respectively, while for higher
temperatures the emission energy suffers a blue-shift.
content of the samples. For InGaN bulk layers, the
This behavior is explained in terms of carrier localiza-
symmetric (0002) and the asymmetric (105) reflections
tion in a distribution of local minima formed in higher
were used, assuming the validity of Vegard’s law for the
In content than the surrounding InGaN matrix [8]. At
lattice parameter [7] and taking the In-content depen-
low temperatures, photo-generated carriers are ran-
dent elastic coefficients C13 and C33 from Ambacher [4].
domly distributed among the different minima, but
The quantum well and barrier thickness, the In content
when increasing temperature, electron
/hole pairs have
and the strain state were obtained in the MQWs by
enough energy to reach the lower energy minima, and
fitting the measured (0002) symmetric reflection using a
the emission red-shifts. Temperature-induced blue-shift
dynamical simulation program.
To investigate the interface roughness in the layers,
transmission electron microscopy (TEM) measurements
were carried out in a Jeol JEM 3010 microscope
working at 300 kV accelerating voltage. The TEM
cross-sectional samples were conventionally prepared
by mechanical thinning and polishing followed by Ar-
ion beam milling using a cold stage at liquid nitrogen.
Transmission data were obtained using a Perkin
/
Elmer Lambda 9 spectrophotometer, while photolumi-
nescence (PL) measurements were performed in a
double cycle He-flow cryostat using a He
/Cd (325
nm) laser as excitation source with 1 mW. The emission
was dispersed by a high-resolution THR1000 Jobin-
Yvon spectrometer, detected by a GaAs photomultiplier Fig. 1. Low temperature PL spectra for different In content layers.
and processed using lock-in techniques. The In content and strain degree is specified for each layer.
 F.B. Naranjo et al. / Materials Science and Engineering B93 (2002) 131
/134 133

Fig. 2. PL emission energy and FWHM for samples with 20% In (a) and 27% In (b).

for temperatures above 200 K (20% In) and 150 K (27%

In) is attributed to filling of higher-energy minima with
electron and hole pairs due to the thermal energy. This
effect is clearer for the sample with the 27% In, where
the PL emission energy at room temperature is higher
than at low temperature. The distribution of carriers at
the different minima explains the behavior of the
emission FWHM with the temperature. At room
temperature, the PL FWHM and the absorption band-
edge broadening is observed to increase with the In
content. Absorption band edge from 153 to 210 meV
were calculated for In contents from 20 to 27% In,
respectively, which support the hypothesis of an In
content localization present in these layers [9].
Fig. 3. HRXRD (0002) reflection for two different MQWs, fitting
The calculated effective band-gap was extrapolated to results are described in the text.
the corresponding relaxed band-gap for each In content
estimated from HRXRD measurements considering the XRD diffraction data, as it has been observed by
dEG/do Š  14.5 eV [10], leading to a bowing parameter other authors [12]. High-resolution TEM image is
for relaxed InGaN of 3.6 eV, in agreement with the data
shown in Fig. 4 for sample (b), as it can be observed,
in the literature [11].
the quantum well and barriers thicknesses are in good
agreement with HRXRD simulations.
3.2. InGaN MQW

The HRXRD (0002) symmetric reflection is shown

for two different MQW structures in Fig. 3. Using the
simulation program, the best fitting leads to: sample (a),
with barrier and well thickness of 6 and 5 nm,
respectively; and sample (b), with 5 and 3 nm of barrier
and well thickness, respectively. The fully strained
InGaN has an In content of 0.16 for sample (a) and
0.12 for sample (b).
As it can be observed in Fig. 3, the satellite peaks are
clearly visible in sample (b). For samples with high In
content (as sample (a)), cross-section TEM images
reveals an increase of the interface roughness, which is
consistent with the broadening of the satellite peaks in Fig. 4. HRTEM image of sample (b).
134 F.B. Naranjo et al. / Materials Science and Engineering B93 (2002) 131
/134
Fig. 5. (a) Evolution of PL emission energy and FWHM of the emission for the sample (a). (b) Evolution of PL emission energy and FWHM of the
emission for the sample (b).
Fig. 5 shows the temperature dependent photolumi-
nescence evolution of samples (a) and (b). The S-shape
of the PL emission energy with the temperature reveals
the existence of localization, more important in the
sample (b) (thinner wells), which has a blue-shift of 30
meV for temperatures above 250 K. For sample (a), with
thicker wells, the effect of the localization is lower; it is
well known that the piezoelectric field increases with the
In content, and the total potential drop in the well is
proportional to the well thickness and the polarization
field. In fact, in sample (a) both mechanisms (localiza-
tion and piezoelectric fields) are responsible for the
emission energy, a decrease of the well thickness from 5
to 4 nm, maintaining the In content and barrier
thickness, lead to an emission blue-shift of 165 meV
(not shown). From this shift, a field of 1.6 MV cm 1 is
estimated in the well, lower than the theoretical predic-
tions [13] probably due to contribution by localization
effect.
4. Conclusions
InGaN bulk layers and MQWs were grown on GaN
templates to study the effect of the In localization in the
samples. HRXRD reveal that the thick layers (300 nm)
are not fully relaxed within the range of In contents
studied. From absorption measurements, an increase of
the absorption band-edge was observed, being depen-
dent on the In content. Localization is present in MQW
and an increase of the PL emission energy is observed
when decreasing the well thickness, showing an impor-
tant effect of piezoelectric fields in thick quantum wells.
Acknowledgements
The authors acknowledge the contribution of B.
Beaumont for the MOCVD GaN templates. Thanks
are due to B. Jenichen for his help in XRD measure-
ments and to O. Brandt for the HRXRD simulation
program. Partial financial support was provided by IST
ESPRIT 1999-10292 ‘AGETHA’ Project.
References
[1] S. Nakamura, Semicond. Sci. Technol. 14 (1999) R27.
[2] T. Takayama, M. Yuri, K. Itoh, T. Baba, J.S. Harris, Jr., J. Appl.
Phys. 88 (2000) 1104.
[3] H. Chen, A.R. Smith, R.M. Feenstra, D.W. Greve, J.E.
Northrup, MRS Internet J. Nitride Semicond. Res. 4S1 (1999)
G9.5.
[4] O. Ambacher, J. Phys. D: Appl. Phys. 31 (1998) 2653.
[5] M.A. Sánchez-Garcı́a, F.B. Naranjo, J.L. Pau, A. Jiménez, E.
Calleja, E. Muñoz, S.I. Molina, A.M. Sánchez, F.J. Pacheco, R.
Garcı́a, Phys. Status Solidi A176 (1999) 447.
[6] M.A. Sánchez-Garcı́a, E. Calleja, E. Monroy, F.J. Sánchez, F.
Calle, E. Muñoz, R. Beresford, J. Cryst. Growth 183 (1998) 23.
[7] M. Schuster, P.O. Gervais, B. Jobst, W. Hösler, R. Averbeck, H.
Riechert, A. Iberl, R. Stömmer, J. Phys. D: Appl. Phys. 32 (1999)
A56.
[8] L.P.D. Schenk, M. Leroux, P. de Mierry, J. Appl. Phys. 88 (2000)
1525.
[9] R.W. Martin, P.G. Middlenton, K.P. O’Donnell, W. Van der
stricht, Appl. Phys. Lett. 74 (1999) 263.
[10] S. Pereira, M.R. Correia, T. Monteiro, E. Pereira, E. Alves, A.D.
Sequeira, N. Franco, Appl. Phys. Lett. 78 (2001) 2137.
[11] C. Wetzel, T. Takeuchi, S. Yamaguchi, H. Katoh, H. Amano, I.
Akasaki, Appl. Phys. Lett. 73 (1998) 2566.
[12] Ig-Hyeon Kim, Hyeong-Soo Park, Yong-Jo Park, Taeil Kim,
Appl. Phys. Lett. 73 (1998) 1634.
[13] F. Della Sala, A. Di Carlo, P. Lugli, F. Bernardini, V. Fiorentini,
R. Scholz, Jean-Marc Jancu, Appl. Phys. Lett. 74 (1999) 2002.