Journal of Luminescence 155 (2014) 2731

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Journal of Luminescence
journal homepage: www.elsevier.com/locate/jlumin

Shell to core carrier-transfer in MBE-grown GaAs/AlGaAs coreshell

nanowires on Si(1 0 0) substrates
Maria Herminia Balgos n, Rafael Jaculbia, Michael Defensor, Jessica Pauline Afalla, Jasher
John Ibaes, Michelle Bailon-Somintac, Elmer Estacio, Arnel Salvador, Armando Somintac
Condensed Matter Physics Laboratory, National Institute of Physics, University of the Philippines, Diliman, Quezon City 1101, Philippines

art ic l e i nf o a b s t r a c t

Article history: We report on the shell-to-core carrier-transfer in GaAs/Al0.1Ga0.9As core-shell nanowires grown on
Received 26 August 2013 Si(1 0 0) substrates via molecular beam epitaxy. The nanowires are dominantly zincblende and are tilted
Received in revised form with respect to the substrate surface. Photoluminescence (PL) excitation spectrosocopy at 77 K revealed an
2 June 2014
abrupt increase in the GaAs PL intensity at excitation above the Al0.1Ga0.9As shell bandgap which is attributed
Accepted 5 June 2014
Available online 16 June 2014
to shell to core carrier-transfer. More carriers from the Al0.1Ga0.9As transfer to the GaAs at T490 K, as
observed in the time-resolved PL and temperature dependence of the relative PL intensities of GaAs and
Keywords: Al0.1Ga0.9As due to the ionization of the traps within the Al0.1Ga0.9As. Using a coupled rate equation model
IIIV semiconductors that takes into account shell to core carrier-transfer, the average recombination time constants of Al0.1Ga0.9As
Carrier transfer
shell rec,s 400 ps (580 ps) and GaAs core rec,c 600 ps (970 ps) were obtained from the time-resolved PL at
Nanowires
300 K (77 K). Carrier-transfer time constants CT 50 ps (55 ps) at 300 K (77 K) were also obtained.
Time-resolved luminescence
& 2014 Elsevier B.V. All rights reserved.

1. Introduction The enhancement of the PL intensity in CSNWs is attributed

Semiconductor nanowires (NWs) are quasi-one dimensional
structures with diameters in nanometers and length in microns.
The wide range of base materials and the possible production of
highly crystalline structures from lattice-mismatched materials
make NWs a versatile alternative to its bulk counterpart [1-3]. In
fact, the integration of IIIV semiconductors to Si has been possible
through NW growth [47]. Due to its interesting properties, NWs
cover a wide range of applications such as in energy conversion,
sensors, electronics, and optoelectronics.
Application of NWs as light emitters such as light emitting
diodes [8,9] and lasers [10] has been previously demonstrated. Due
to their high surface-to-volume ratio, however, NWs are suscep-
tible to surface states that may degrade their light emission
capabilities [11,12]. To reduce the effects of surface states, NWs
are coated with high bandgap material (shell) that serves as a
passivation barrier from the surface states. Electrical and optical
investigations in these coaxial structures, commonly known as
core-shell NWs (CSNWs), show enhanced carrier mobility [13,14]
and photoluminescence (PL) intensity [1518], as compared to
bare NWs (no shell).
n
Corresponding author. Tel./fax: 63 99209749.
E-mail address: mbalgos@nip.upd.edu.ph (M.H. Balgos).
mainly to the reduced interaction of carriers with the surface
states which may act as nonradiative recombination sites, electro-
nic traps, and scattering sites [11,12,19]. However, the introduction
of the shell can also enhance the PL intensity by acting as another
source of carriers for the NW core [20]. The carriers from the shell
can transfer to the core and effectively increase the number of
recombining carriers thereby producing a more intense PL [21].
Carrier transfer (CT) has already been observed in quantum wells
[2223], laser structures [24], and type II coreshell heterostruc-
tures [20] using time resolved PL (TRPL).
In this work, we study in detail the shell-to-core CT in GaAs/
Al0.1Ga0.9As CSNWs by utilizing continuous wave (CW) and TRPL
for varying temperatures. The relatively low Al mole fraction
(x 0.1) of the AlxGa1  xAs allows us to observe a distinct PL signal
from GaAs and AlGaAs and at the same time, to pump both GaAs
and AlGaAs using a Ti:Sapphire CW laser. The effect of the CT on
the PL intensity is measured directly using PL excitation (PLE).
2. Methods
GaAs/Al0.1Ga0.9As CSNWs coated with n-doped GaAs cap layer
were grown on Si (1 0 0) substrates using a Riber 32P molecular
beam epitaxy (MBE) machine. The Si substrate was pre-patterned
with gold nanodots that serve as catalysts for the vaporliquidsolid
(VLS) growth of NWs [25]. GaAs was deposited at 580 1C for 30 min

http://dx.doi.org/10.1016/j.jlumin.2014.06.008
0022-2313/& 2014 Elsevier B.V. All rights reserved.
28 M.H. Balgos et al. / Journal of Luminescence 155 (2014) 2731
followed by Al0.3Ga0.7As at the same growth temperature and
duration. The thin lm equivalent thickness is 0.65 m and
0.84 m for GaAs and Al0.3Ga0.7As, respectively. Lastly, a 0.1 m Si-
doped GaAs cap ( 1017 cm  3) served as a protective coating for the
AlGaAs which readily oxidizes when exposed to air [26]. The n-
doping of
the GaAs cap decreases the width of the depletion region at the
airAlGaAs interface [13,14] preventing it from penetrating to
the AlGaAs. The formation of a depletion shell could narrow the
electronic channel producing PL [15] and decreases the carrier
lifetime [5].
CW-PL measurements were conducted at temperatures of
10300 K. The sample was mounted on the coldnger of a
closed-cycle He cryostat equipped with a Lakeshore temperature
controller. The excitation source was a 488 nm Ar laser and the
PL signal was dispersed by a SPEX 500 m monochromator and
detected by a Hamamatsu GaAs photomultiplier tube. PLE (at 77 K)
and TRPL (at 77 K and 300 K) measurements were conducted at a
separate -PL setup where a 10  objective was used to focus the
laser and collect the PL signal from the sample mounted inside a
continuous ow liquid nitrogen cryostat for 77 K measurements.
For the PLE, the GaAs PL peak intensity at 1.514 eV was monitored
using a Synapse Si CCD detector attached to an iHR550 Horiba
Jobin Yvon spectrometer. The excitation energy of a CW Ti:
Sapphire laser was tuned from 1.531.68 eV (810740 nm) corre-
sponding to below and above the Al0.1Ga0.9As shell bandgap,
respectively. For the TRPL measurements, a frequency doubled
Ti:Sapphire femtosecond laser (400 nm) with 100 fs pulses at
80 MHz repetition rate was used as excitation. The uence was
kept at 0.012 J/cm3 to ensure minimal, if any, nonlinear effects
[27]. The PL signal was fed to a streak camera system consisting of
Digikrm spectrometer and an Optronis streak camera. The
measured TRPL resolution is  10 ps. All measurements were
performed on the as-grown CSNW sample (i.e., on ensemble of
CSNWs) only. TRPL for bare GaAs NWs was not reported because
the signal was too weak to be detected by our TRPL setup.
3. Results
Fig. 1 shows a representative top view SEM micrograph of the
sample. The CSNWs are tilted with respect to the horizontal due to
the o1 1 1 4 preferential growth of GaAs NWs [28]. Close
inspection of the CSNWs show that they have a tapered tip, as
previously observed in Au-assisted GaAs NWs [29]. From various
SEM images, the diameter of the CSNWs is estimated to be
Fig. 1. Top view SEM micrograph of the coreshell nanowires (CSNWs) showing
high density formation. The CSNWs are predominantly tilted with respect to the
substrate surface due to the o 1 1 1 4 preferential growth of the nanowires.
Fig. 2. 300 K PL of GaAs/AlGaAs core-shell nanowires and bare GaAs nanowires.
The (  10) means that the PL spectrum of GaAs is multiplied by 10 for clarity. More
than an order of magnitude increase in the GaAs PL peak intensity of the coreshell
nanowires compared to bare nanowires is observed. The inset is a schematic of the
coreshellcap structure.
141 714 nm with a density of 1.68  108 cm  2. The GaAs core
diameter and the AlGaAs shell thickness is  100 nm and  19 nm,
respectively. These values were estimated using the diameter of a
bare GaAs NW (1037 25 nm) grown separately using the same
parameters as reference. For MBE-grown NWs via the VLS
mechanism, the growth elements are decomposed as they are
deposited on the substrate. Hence, a lm is also formed in areas
with no gold catalysts [30]. However, due to the high lattice
mismatch between GaAs and Si (4%) [31], this lm is defective
and emits very weak PL, if any.
Fig. 2 shows the 300 K PL spectrum of the CSNWs and bare
GaAs NWs. The sharp peaks in the 300 K spectra may be Ar laser
plasma lines. For the CSNWs, we identied distinct bands at
1.437 eV and 1.559 eV corresponding to the GaAs core and to the
Al0.1Ga0.9As shell transitions, respectively. The position of the GaAs
band is near the bandgap of bulk zincblende GaAs, suggesting that
our sample is predomintantly zincblende (ZB). To verify this
structure, we use x-ray diffraction and temperature dependent
PL [32]. The low Al mole fraction x 0.1 may be attributed to the
different kinetics between 2-D lm and NW growth, as observed
by Chen et al. [30]. In VLS, the growth depends on the rate at
which the adatoms diffuse along the NW sidewalls [30]. Compared
to the bare GaAs NWs, there is more than an order of magnitude
increase in the GaAs PL intensity for the CSNWs. The enhanced
GaAs PL signal in CSNWs may be due to (i) suppressed surface
recombination because of the passivation provided by the Al0.1
Ga0.9As shell [11,12,1519]; and (ii) increased number of recom-
bining electron-hole pairs via the shell to core CT [21].
The shell-to-core CT in our sample is observed via PLE at 77 K.
Fig. 3a shows the 77 K PLE spectrum of GaAs where the excitation is
varied from below to above the Al0.1Ga0.9As bandgap of 1.65 eV. An
abrupt increase in the PLE signal is observed at 1.65 eV which we
attribute to the CT. At excitations ho1.65 eV (Region I), the carriers
that contribute to the GaAs PLE in Region I are those optically excited
from the GaAs region only. At excitations h41.65 eV (Region II),
carriers optically excited from the Al0.1Ga0.9As can diffuse and
transfer to GaAs and can contribute to the PLE signal [33]. Since
the PLE spectrum follows absorption spectrum for CW excitation, we
expect the PLE spectrum to mimic the E bulk density of states. The
PLE spectrum follows the h dependence in Region I but deviates
drastically in Region II. The deviation can be explained by the added
absorption introduced by the Al0.1Ga0.9As. The CT mechanism
and band-to-band recombination are schematically shown in
Fig. 3b. However, it should be noted that aside from these two,
recombination via defects (not included in Fig. 3b) is also possible.
 M.H. Balgos et al. / Journal of Luminescence 155 (2014) 2731 29

Fig. 3. (a) GaAs core PLE spectrum at 77 K. Abrupt increase of PL at excitations above the Al0.1Ga0.9As bandgap indicates carrier transfer. (b) Mechanism for the shell to core
carrier transfer.

Fig. 4. Time resolved photoluminescence at 77 K and 300 K of the (a) GaAs core and (b) AlGaAs shell of the core-shell nanowires. Black solid lines are ts to the coupled rate
equation (Eqs. (1a) and (1b)). The recombination time constants rec and carrier transfer time constants CT obtained from the ts are included in the gure.

The n-doped GaAs cap is too thin to have a signicant effect on the
PLE signal.
We further investigated the CT mechanism using TRPL. Fig. 4a
and b shows the TRPL spectra of GaAs and Al0.1Ga0.9As, respec-
tively, at 300 K and 77 K. The spectra were obtained by taking a
horizontal segment in the streak image with height equal to the
full-width at half maximum of the PL signal. All spectra were tted
using a coupled differential rate equation model to represent the
temporal carrier evolution for the Al0.1Ga0.9As shell and GaAs core:
 
d N c t N ex;c Nc N s N max  N CT
 1a
dt rc rec;c CT N max
 
d N s t N ex;s Ns N s N max  NCT
 
dt rs rec;s CT Nmax
where the subscripts s and c denote shell and core, respectively.
N is the number of carriers, Nex is the initial number of excited
carriers due to the optical excitation, r is the rise time constant,
rec is the recombination time constant, CT is the transfer time
constant, Nmax is the maximum number of carriers that can
transfer, and NCT is the number of carriers that transferred. Eqs.
(1a) and (1b) are modied generationrecombination rate equa-
tions for NWs [34]. Generation manifests as the TRPL rise while
recombination manifests as the TRPL decay. The rst term in the
right-hand-side of Eqs. (1a) and (1b) indicates addition of carriers
via optical excitation and the subsequent thermalization of the
carriers to the band edges. The second term represents the
radiative (R) and nonradiative (NR) recombination with time
constant 1/rec 1/R 1/NR. The last term accounts for of the
CT mechanism. The term in brackets is to incorporate the nite
number of carriers Nmax from Al0.1Ga0.9As that can transfer.
Physically, only carriers near the Al0.1Ga0.9AsGaAs interface can
readily transfer; those away from the interface have to initially
diffuse before they can undergo CT. Simultaneously, in momentum
space, these carriers thermalize to reach the band edges before
they recombine. Since thermalization is a faster process (in the
order of femtoseconds [35]) than diffusion, then recombination is
favored at longer timescales. In our model, when NCT reaches Nmax,
the CT process stops (last term in Eqs. (1a) and (1b) goes to zero)
1b leaving recombination as the only carrier exit path in the shell and
the optical excitation as the only source of carriers in the core.
The black solid lines in Fig. 4a and b are the least square ts of
Eqs. (1a) and (1b), respectively. It is important to note that r is
xed at 10 ps equivalent to the resolution of our TRPL setup. This
value is reasonable since the thermalization of the carriers,
characterized by r is in the order of femtoseconds [34] and is
beyond the resolution of our TRPL setup.
For the GaAs core (Fig. 4a), the TRPL rise has a single rate. Since
carriers from Al0.1Ga0.9As transfer to GaAs, we expect a double rise
characterized by two different time constants one from the
optical excitation and one from the CT. The single TRPL rise may be
explained by the relative contribution to the number of carriers of
30 M.H. Balgos et al. / Journal of Luminescence 155 (2014) 2731
Fig. 5. (a) Integrated PL intensity versus inverse temperature of the AlGaAs shell. Activation energy Ea 31.4 meV corresponds to the ionization of traps within the AlGaAs.
(b) Temperature dependent GaAsAlGaAs PL intensity ratio showing an increase at  90 K.
the two processes. More carriers are produced via optical excita-
tion, hence, the TRPL rise from the CT is swamped and is not
observed. The TRPL of GaAs at both temperatures is characterized
by a single TRPL decay rate. We attribute the decay to carrier
recombination within the GaAs, The faster decay of 600 ps at
300 K is due to signicant NR recombination at 300 K. Since rec,c
which is a combined effect of R and NR recombination [36], that is,
1/rec 1/R 1/NR, we observe a longer time constant of 970 ps at
77 K where NR is minimized and 1/NR approaches zero. The
values obtained at 300 K and 77 K are within the range of reported
carrier lifetime values for nearly intrinsic exciton lifetimes of GaAs
NWs (0.051.1 ns) reported by Perera et al. [37].
For the Al0.1Ga0.9As shell (Fig. 4b), a single exponential TRPL
rise, due to the optical excitation, is observed at 77 K and 300 K.
The TRPL decay, however, is characterized by a single exponential
decay rate at 77 K and a double exponential (fast and slow) decay
rate at 300 K. We propose that the appearance of the double decay
is a consequence of the CT mechanism. We attribute the fast decay
to the combined effect of recombination and carrier transfer while
the slow decay is ascribed to the recombination. Numerical tting
using Eq. (1a) revealed rec,s of 400 ps at 300 K and 580 ps at 77 K.
A longer rec,s at 77 K is again attributed to the minimized NR
recombination at low temperatures. The transfer time constant CT
is 50 ps and 55 ps for at 300 K and 77 K, respectively. This is
similar to the CT time constants of GaAs/AlGaAs separate conne-
ment heterostructures reported by Morin et al. (19.2 ps at 300 K
and 22 ps at 80 K) [38]. Our values of CT show that the CT time is
almost independent of temperature and cannot explain the double
decay observed in the 300 K TRPL of Al0.1Ga0.9As.
As such, the the maximum number of transferred carriers Nmax
relative to the initial number of carriers Nex,s (t0) in the shell was
investigated. We obtain a value of Nmax/Nex,s(t0) of 0.24 at 77 K
and 0.69 at 300 K. These values show that a higher fraction of
excited carriers transfer at 300K than at 77 K. We believe that
defects in the Al0.1Ga0.9As affect the number of carriers that can
transfer. Using an Arrhenius plot of the integrated PL intensity vs
inverse temperature (Fig. 5a), we calculate an activation energy
Ea 31 meV for the defects within the AlGaAs at  90 K which can
be attributed to an electron trap E9 (30 meV) or a hole trap H4
(32 meV) [39]. At 77 K (o90 K), there is still efcient trapping of
carrier by the defects, thus there are not enough transferred
carriers to produce a double decay. At 300 K, the defects in the
shell are already ionized and are not as efcient at trapping
carriers. Thus, more carriers can diffuse until they nally transfer
to the GaAs.
The temperature dependence of the number of carriers avail-
able for transfer to GaAs is investigated using the relative PL
intensities of GaAs and Al0.1Ga0.9As at 10K300 K. Fig. 5b shows
the GaAsAl0.1Ga0.9As PL intensity ratio (PLIR) as a function of
temperature. Owing to the same growth conditions, the defects
incorporated in GaAs and AlGaAs have minimal difference. The PL
signal for GaAs and Al0.1Ga0.9As therefore should quench at almost
the same rate with temperature resulting to a constant PLIR if they
are to be treated independently. Constant PLIR is seen at 1070 K
as indicated by the horizontal dash line in Fig. 5b. At 90150 K,
however, there is an apparent increase in the PLIR as indicated by
the slanted dash line. At these temperatures, the GaAs PL intensity
increases relatively to the Al0.1Ga0.9As. More carriers from the
Al0.1Ga0.9As transferred to GaAs at T 490 K. We note that
the intersection of the horizontal and slanted line at  90K
coincides with the activation temperature of the defects within
the Al0.1Ga0.9As.
4. Conclusion
The shell-to-core CT mechanism of an ensemble of dominantly
zincblende GaAs/AlGaAs CSNWs is investigated through CW-PL,
TRPL and PLE spectroscopy for varying temperatures. PLE provides
strong evidence of the CT mechanism while CW-PL and TRPL
demonstrate that the CT process is dependent of temperature
mainly because a high number of carriers participate in the CT
process at T 490 K. Coupled rate equations are used to t the TRPL
at 300 K and at 77 K, thereby facilitating the evaluation of the
recombination and carrier transfer time constants. The 300 K
(77 K) average recombination time constants for GaAs core are
rec,c 600 ps (970 ps) while that of the AlGaAs shell are rec,
s 400 ps (580 ps). The CT time constant is determined to be
CT 50 ps (55 ps) for 300 K (77 K).
Acknowledgments
This work is supported in part by Grants from PCIEERD-DOST,
DOST-GIA, and University of the Philippines OVCRD. The authors
would also like to thank Intel for the donation of the streak
camera.
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