Superlattices and Microstructures, Vol. 26, No.

4, 1999
Article No. spmi.1999.0770
Available online at http://www.idealibrary.com on

Lineshape analysis of photoreflectance spectra from InGaAs/GaAs

quantum wells

N. M. S. C HOQUE , D. B ELIAEV , J. A. N. T. S OARES , L. M. R. S COLFARO ,

A. L. S PERANDIO , A. A. Q UIVY , J. R. L EITE
Instituto de Física da Universidade de São Paulo, Caixa Postal 66318, 05315-970 São Paulo, SP, Brazil

(Received 26 April 1999)

The fundamental optical transitions in In0.15 Ga0.85 As/GaAs single symmetric quantum
wells (QWs) are studied through photoreflectance (PR) measurements and their depen-
dence on the well distance from the surface. A phase rotation of the lineshape of the PR
signal is observed as was predicted in our previous works. PR spectra of several samples,
measured at 77 K, are compared with results of PR lineshape calculations, and a fairly
good agreement is found. The quantum-confined Stark effect is shown to be the dominant
modulation mechanism in the QW. Pronounced interference effects make PR spectra from
QWs sensitive to the cap layer thickness.
c 1999 Academic Press
Key words: photoreflectance, quantum wells, lineshape analysis.

1. Introduction
InGaAs/GaAs quantum wells (QWs) have attracted a great interest as important material systems for opto-
electronic devices. They have been the subject of several experimental and theoretical investigations [1–4].
Although photoreflectance (PR) measurements have been widely conducted in these types of systems for
the determination of the material parameters associated with the energies of spectral singularities, the phys-
ical origin of the PR lineshapes displayed behavior in the optical spectra that still deserves to be addressed
more precisely [4–6]. For example, the interpretation of the experimental PR data can be complicated by the
superposition of spectral structures provenient from different regions of the sample. In particular, interfer-
ence of light from the QW and the top surface plays a crucial role in determining the spectral lineshape. In
the case of reflectance (R) experiments on a Al0.3 Ga0.7 As/GaAs/Al0.3 Ga0.7 As 100 Å QW, this was already
observed experimentally and compared to the electron heavy-hole transition lineshapes fitted neglecting the
Fabry–Perot-type multiple reflections [7]. For the case of planar-doped QWs, the variation of the PR (not
R) spectra was already investigated theoretically [8] by depicting the changes in the PR signal as a function
of the geometry of the relative well positions in the samples. A similar investigation, also from the point of
view of modulation spectroscopy needs, was performed later for AlGaAs/GaAs/AlGaAs QWs, for which the
PR spectra for different QW widths and surface barrier thicknesses were calculated in a rigorous way [9].
The spectral features related to transitions within the QW have been shown to depend on the phase shifts
varying according to the cap layer thickness. These phase-shifting effects lead to a ‘rotation’ of the spectrum
lineshape. Nevertheless, such rotation-like experimental data, as far as PR spectra are concerned, were not
previously reported.

0749–6036/99/100243 + 08 $30.00/0 c 1999 Academic Press

244 Superlattices and Microstructures, Vol. 26, No. 4, 1999

GaAs
cap layer d

In0.15Ga0.85As QW 100 Å

GaAs buffer layer 1 µm

GaAs
semi-insulating 450 µm
substrate

Fig. 1. Composition of the samples used for which the cap layer thicknesses were: d = 500, 1000, 2500, 7500, and 10000 Å.

The aim of the present work is to experimentally confirm the theoretical prediction of the lineshape ‘ro-
tation’ for the case of InGaAs/GaAs QWs by performing a systematic study of the lineshape behavior as a
function of the cap layer thickness and analyzing the influence of interference effects on the QW transition
energy values to be extracted from PR spectra. To the best of our knowledge, this is the first time that rig-
orously calculated PR lineshapes from InGaAs/GaAs heterostructures are compared with the experimental
lineshapes for a set of samples with different cap layer thicknesses. The theoretical spectra are obtained by
the original hybrid matrix method, developed in our previous works [10, 11]. This method enables us to rig-
orously calculate the PR spectra. That was not achieved in [7] (the simplified approach only permitted a fit of
the R spectra lineshapes) and remained a subject for further study. We observe not only a qualitative, as in the
above-mentioned paper, but also quantitative agreement between theoretical and experimental curves. In our
work, besides the extention of the method to include confined carriers’ contributions accounting in this way
for the modulation of the dielectric function (DF) inside the QW [9], the excitonic features of the transitions
have also been properly taken into account. The Stark effect is used to describe the changes in oscillator
strengths and transition energies between the QW confined levels. Radiative recombination mechanisms are
analyzed by comparing the experimental and theoretical results. The excellent agreement between theory and
experiment demonstrates the applicability and advantages of our approach to the study of quantum-confined
systems and, in particular, modulation spectroscopy spectra from InGaAs/GaAs QWs.

2. Experimental details
We report PR spectra from a set of six different samples, each containing a single undoped symmetric
QW of a fixed width of 100 Å, with varying surface barrier thickness (d). The samples were grown in a
VARIAN GEN II MBE machine, on a (001)-oriented semi-insulating GaAs substrate. They consist of a
10000 Å undoped buffer layer followed by a 100 Å thick In0.15 Ga0.85 As layer (QW) and an undoped barrier
GaAs cap layer with d = 500, 1000, 2500, 5000, 7500, and 10000 Å, as schematically illustrated in Fig. 1.
The substrate, in all samples, was heated to 580 ◦ C in order to grow the buffer layer, then the temperature
was lowered to 520 ◦ C to grow the well and the cap layer.
The PR spectra were taken by a standard PR setup. It consists of a halogen lamp, a monochromator and
a Si detector using a lock-in technique. As a pump beam, an argon laser with power output of 3 mW mm−2
was used.
Superlattices and Microstructures, Vol. 26, No. 4, 1999 245

3. Results and discussion

In Fig. 2, we present the detailed PR spectra for the six samples in the energy region close to the
In0.15 Ga0.85 As fundamental transition. The spectra are dominated by a PR resonance at about 1.355 eV
which is due to the e1–hh1 transition involving the first confined electron (e1) and heavy-hole (hh1) states
of the QW. The broadening of the lines indicates the Gaussian character of the dielectric susceptibility. One
can clearly see in these spectra that the phase of the resonance line depends on the thickness of the cap layer
d. The phase changes by π if the thickness of the cap layer increases by an amount which is equal to 1/4 of
the optical path of the probe light inside GaAs, λm /4. This behavior can be understood bearing in mind that
the PR lineshape is determined by a composition of the real and imaginary parts of the DF inside the QW.
This mixture is modified by the phase change of light travelling from the surface to the QW and then back
to the surface. Thus we experimentally observe the effect of lineshape ‘rotation’ predicted theoretically in a
previous paper [9]. The concept of ‘rotation’ can be understood as a projection of the lineshape curve, rotated
in a space around ‘photon energy’ axis, onto the plane defined by the ‘1R/R’ and the ‘photon energy’ axis.
The one-circle rotation corresponds to the increase in the cap layer thickness by 1/2 of the material optical
path, λm /2. Although none of our samples corresponds to the case of (λm (1.355 eV))/4 ≈ 650 Å multiple
thicknesses, it is clear from the spectra shown in this work, and it was verified through theoretical calcula-
tions, that the lineshapes corresponding to n × λm /2 and (n + 1) × λm /2 cap layer thicknesses differ only
in amplitude due to the probe light absorption inside the sample; peak positions remain the same; however,
the shapes may change only slightly as the λm -related accumulated phase change is slightly different for
different photon energies since the probe light optical path λm (ω) and the photon energy are inter-related.
Therefore, the conclusions of the present work are valid for any thickness between the surface and QW.
In order to understand the radiative recombination and interference mechanisms associated with our ex-
perimental PR spectra, a rigorous theoretical lineshape analysis is performed. Our samples consist of various
layers of either macroscopic (GaAs buffer layer and substrate) or mesoscopic (QW In0.15 Ga0.85 As layer)
widths. While the optical constants of these layers may be assumed to be spatially constant parallel to the
interfaces, weak inhomogeneities occur perpendicularly to them due to the presence of inhomogeneous elec-
tric fields in the depletion region. In any case, such intralayer inhomogeneities arise from the modulating PR
perturbations. The weak intralayer inhomogeneities are superimposed by the generally much stronger varia-
tions of optical constants between different layers. In previous works, we developed and applied a method to
calculate PR spectra from heterostructures which treats each kind of inhomogeneity in its own way [10, 11].
The intralayer inhomogeneity is treated by means of a generalization of the perturbation approach, developed
for the case of an infinite half space [12]. The interlayer inhomogeneity is included in the calculations by
means of the transfer matrix method [13].
First, as they have already been published, we only discuss briefly our methods of calculation [10, 11]. The
problem of PR spectra calculations is the problem of the reflection coefficient calculations in the presence
and in the absence of modulating light, taking into account an influence of the modulated and unmodulated
built-in electric field profiles on the dielectric function ε(ω, z). Our structure is described by a generalized
transfer matrix M including both inter- and intralayer inhomogeneities, given by the matrix product

M = Mn Mn−1 . . . M1 , (1)

where Mn is a transfer matrix of the nth layer, incorporating the intralayer inhomogeneities in an integral
way. The first layer contacts vacuum and the nth layer contacts the substrate. In terms of M, the reflection
coefficient may be expressed as
|(e R |M|e0 )|2
R= , (2)
|(e R |M|e∗0 )|2
where the vectors e0 = (1, −ik0 ), e R = (−iksub , 1) defined through wavevectors of the vacuum (k0 ) and of
246 Superlattices and Microstructures, Vol. 26, No. 4, 1999

d = 500 Å

d = 1000 Å

d = 2500 Å
1R/R (a.u.)

d = 5000 Å

d = 7500 Å

d = 10000 Å

1.32 1.33 1.34 1.35 1.36 1.37 1.38 1.39

Photon energy (eV)

Fig. 2. Measured PR spectra of InGaAs/GaAs QWs of 100 Å width at the energy region close to the fundamental QW transition hh1–e1
showing the lineshape rotation for different cap layer thicknesses d.

the substrate (ksub ) are used. The transfer matrix Mn may be formed as follows
E + (z) E − (z)
 
Mn =
E+0 (z) E 0 (z) . (3)
−
Here, the two linearly independent solutions of the wave equation are taken in the form
E + (z) = 12 [eiφ+ (z) + eiφ− (z) ], (4)
i
E − (z) = [eiφ+ (z) − eiφ− (z) ], (5)
2kn
where φ± (z) follows from the equation
(n)
dz 0 [e±2ikn (z−z ) − 1] 1 (n)(z ) .
Rz 0 0
φ± (z) = ± 12 kn z n−1 (6)
To account for the electric field induced change in the DF 1(z) of bulk-like GaAs layers we used the well-
known Airy function expression [10, 11], following the Franz–Keldysh oscillations theory. The changes in
Superlattices and Microstructures, Vol. 26, No. 4, 1999 247

the QW DF were described using the quantum-confined Stark effect theory and bearing in mind that we are
dealing with the excitonic transitions. Thus, to account for the DF modulation within the In0.15 Ga0.85 As layer
with respect to the fundamental transition with frequency ωt , we employ the following expression [14]:
1
1ε (ω) = Ct 1ωt , (7)
(ω − ωt + i0t )2
where 1ωt , 0t and Ct are the Stark shift of an oscillator frequency, damping parameter and scaling coefficient
related to the matrix element, respectively.
Thus, each matrix Mn is a functional of the electric field profile ϕ 0 (z); the latter should be determined. The
electric potential ϕ(z) obeys an integral form of Poisson’s equation:
Z z0
ρ(z 00 )
Z 0
ϕ(z) = Vs + 4π dz 0
dz 00 , (8)
z ∞ (z 00 )
with ρ(z) being a total charge density and (z) being a static dielectric constant of the structure at z. The
boundary conditions ϕ(0) = Vs and ϕ 0 (∞) = 0 are automatically guaranteed by this relation. Since ρ(z)
depends on ϕ(z), eqn (3) has to be solved self-consistently.
To calculate the electric field profile determining the spatial distribution of the DF changes, we assumed
that the potential is constant far inside the samples and takes a certain surface value at the sample/vacuum
boundary [10, 11]. In the case of undoped systems, this surface potential is not determined by the surface-
localized states’ density but by the occupation of the available states by free carriers which have migrated
to the surface from the MBE grown layers. Since in our samples the undoped layers are usually p-type with
a residual background concentration of about 1 × 1014 cm−3 due to unintentional carbon, one could easily
verify that the total charge of free carriers in our system does not allow us to employ the hypothesis of the
surface Fermi level pinning. Henceforth, we calculate the surface potential barrier values self-consistently
for the different widths of the epitaxial layers, assuming that the position of the Fermi level is exactly in
the middle of the fundamental energy gap in the semi-insulating, practically intrinsic, GaAs substrate. Since
the potential profile depends on the free carrier concentrations and on the confined QW level positions, the
coupled Poisson and Schrödinger equations have to be solved self-consistently. We keep our method for
solving the Poisson equation [10, 11], but after each iteration, the Schrödinger equation is solved and the
new level positions are determined. Figure 3 shows the calculated electric field profiles at zero excitation.
The average unmodulated electric field value within the QW was found to be 1.33 kV cm−1 for all the
samples. It is consistent with the fact that as there are not enough carriers to fill all the surface states, the
value of the electric field is determined by the thickness of the buffer layer, which for all the samples is
constant and equal to 1 µm.
In Fig. 4, the results of our spectral calculations for the QW fundamental transition are depicted. The
calculated PR spectra exhibit the same lineshape rotation ‘around the energy axis’ as observed experimentally
(Fig. 2), and are in good quantitative agreement. It is worth mentioning that the angle of this so-called
‘rotation’ is not the same for different parts of a spectrum, as the phase factors depend not only on the
cap layer thickness but also on the probe light photon energy. This is due to the frequency dependence
of the GaAs DF, and, consequently, of its refractive index. This dependence is automatically taken into
consideration by means of our method. In our PR spectra calculation, we used Gaussian broadening resulting
in a spectral form, which decays exponentially and approaches zero closer than Lorentzian lineshapes. That
is why we did not observe the interference maxima and minima predicted earlier for the case of Lorentizian
broadening [9] for the whole set of our samples. The lineshape calculations based on a Lorentzian type of
broadening were undertaken too. No similarity with the experimental spectra was found. We also do not find
any indication of interference effects between light reflected at the two heterointerfaces of the QWs. This is
consistent with the fact that the QW width is small in comparison with the optical wavelength of the incident
light. The calculated transition energies also vary slightly for each sample due to the small variations of the In
248 Superlattices and Microstructures, Vol. 26, No. 4, 1999

0.2
0.0
–0.2
–0.4
Electric field (KV cm–1)

–0.6
–0.8
–1.0
–1.2 F = –1.33 KV cm–1
–1.4
–1.6 T = 77 K
d = 500 Å
–1.8
d = 1000 Å
–2.0
d = 2500 Å
–2.2
d = 5000 Å
–2.4
d = 7500 Å
–2.6 d = 10000 Å
–2.8

0 5000 10000 15000 20000 34000

z (Å)

Fig. 3. Calculated nonmodulated built-in electric field profiles for samples with cap layer thicknesses: d = 500, 1000, 2500, 7500, and
10000 Å.

composition within the QW layer. The In concentration was independently determined by PL measurements
and taken into account in our calculations in an appropriate way.
Comparing the experimental transition energies with the calculated energies, one can find a difference
of less than 1 meV. A variation of the PR lineshape is seen due to the rotation of the phase of the light at
different capping layer thicknesses. Many-body effects, such as exchange and correlation interactions, were
also taken into account in the local density approximation as explained in our previous publications [15, 16].
The band discontinuities have been assumed to be 1E c /1E v = 58/42 in accordance with results found
in our previous PR measurements for the undoped QWs [1]. The effective masses used were 0.060 m 0 ,
0.470 m 0 , and 0.061 m 0 for electrons, and heavy and light holes, respectively, where m 0 is the free electron
mass. The average binding energy of confined excitons was taken as 7 meV [17]. For comparison, we also
performed calculations for 1E c /1E v = 70/30, as suggested by other authors. In this case, the calculated
transition energies vary by less than 1%. This provides further evidence that the excitonic transitions between
QW confined states are responsible for the spectral features observed below the GaAs fundamental gap. The
small discrepancies between our theoretical (Fig. 4) and the experimental (Fig. 2) curves could be attributed
to the fact that modulation effects due to the electric field induced changes in the broadening parameters 0t
are not included in our calculations.

4. Conclusion
We have reported experimental and theoretical results for PR spectra of InGaAs/GaAs QWs located at
different positions relative to the surface (cap layer thickness). A rotation of the PR lineshapes is observed
in the measured spectra as well as in the theoretical calculations. Since the effect is of purely interferential
origin, such a phase rotation does not affect the exact determinations of transition energies by means of PR
measurements. On the other hand, the transition energy itself is independent of the surface barrier thickness
for the samples investigated here. Fairly good agreement between theory and experiment is found for both
the PR spectra lineshape and transition energies. It should be noted that, to our knowledge, this is the first
Superlattices and Microstructures, Vol. 26, No. 4, 1999 249

d = 500 Å

d = 1000 Å

d = 2500 Å
1R/R (a.u.)

d = 5000 Å

d = 7500 Å

d = 10000 Å

1.32 1.33 1.34 1.35 1.36 1.37 1.38 1.39

Photon energy (eV)

Fig. 4. Calculated PR spectra of an InGaAs/GaAs QW of 100 Å width for different cap layer thicknesses d for the vicinity of hh1–e1
well transition. Broadening parameters 0hh1–e1 were taken as 2 meV, as estimated from the experimental data.

study that definitively detects the phase rotation by modulation spectroscopy techniques, which also exibits
a remarkable agreement with the theoretical spectra calculations. Our work also provides us with a better
understanding of the lineshape behavior in the modulation spectra in general, obtained by means of PR,
electroreflectance (ER), piezoreflectance (PZR), etc.
Acknowledgements—The authors are grateful to Professor Dr Donat J. As for fruitful discussions and sug-
gestions, and to CAPES/DAAD/PROBAL project for supporting his stay in Brazil. The authors would also
like to thank CNPq, FINEP, and FAPESP (Brazilian funding agencies) for partial financial support of this
work.

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