APPLIED PHYSICS LETTERS 101, 222112 (2012)

High electron mobility in Ga(In)NAs films grown by molecular beam epitaxy

Naoya Miyashita,1,a) Nazmul Ahsan,1 Makoto Inagaki,2 Muhammad Monirul Islam,1
Masafumi Yamaguchi,1,2 and Yoshitaka Okada1

1
Research Center for Advanced Science and Technology (RCAST), The University of Tokyo, 4-6-1 Komaba,
Meguro-ku, Tokyo 153-8904, Japan
2
Toyota Technological Institute, 2-12-1 Hisakata, Tempaku-ku, Nagoya 468-8511, Aichi, Japan

(Received 4 October 2012; accepted 12 November 2012; published online 28 November 2012)
We report the highest mobility values above 2000 cm2/Vs in Si doped GaNAs film grown by
molecular beam epitaxy. To understand the feature of the origin which limits the electron mobility
in GaNAs, temperature dependences of mobility were measured for high mobility GaNAs and
referential low mobility GaInNAs. Temperature dependent mobility for high mobility GaNAs is
similar to the GaAs case, while that for low mobility GaInNAs shows large decrease in lower
temperature region. The electron mobility of high quality GaNAs can be explained by intrinsic
limiting factor of random alloy scattering and extrinsic factor of ionized impurity scattering.
C 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4768949]
V
Since the proposal of the GaInNAs as a material for
high-efficiency multi-junction tandem solar cells1,2 and
GaAs-based long-wavelength optoelectronic devices,3,4
dilute nitride semiconductor alloy systems have received
much interest for their fundamental research. Both the properties of large bandgap reduction and decrease of lattice constant with incorporation of a small amount of nitrogen into
GaAs open their potential application for infrared devices
grown on GaAs substrate. However, both the optical and
electrical characteristics are generally degraded even if only
a few atomic percent of nitrogen are added to (In)GaAs, typically accompanied with compositional fluctuation.5 Therefore, usually one need to accurately control and optimize the
growth parameters such as the growth temperature,6 growth
rate, as well as the As/III flux ratio.7
Since the minority carrier properties of GaInNAs are inferior to the conventional III-V semiconductor materials,8,9
carrier collection in a GaInNAs sub-cell is generally insufficient for application to GaInP/GaAs/GaInNAs/Ge quadruple
junction solar cell. One tentative solution is to employ an
n-i-p structure with undoped i-GaInNAs absorber layer
which needs to possess very low carrier concentration. This
structure enables to increase photocurrent from GaInNAs
layer by field-aided carrier collection.9,10 For an effective solution, minority carrier diffusion length and hence both the
carrier mobility and the carrier life time need to be
improved. In this work, we report the highest mobility values
in Si-doped GaNAs films compared to those reported to
date.8,1115 We present the material properties of these films.
The 1.0 lm thick-Si doped GaNxAs films (x 0.009 and
0.013) were grown on semi-insulating GaAs (001) substrates
by radio frequency-molecular beam epitaxy (RF-MBE). The
GaNAs layers were grown under As2 flux of 2  105 Torr at
the growth temperature of 520  C and the growth rate of
1.0 lm/h. The amount of Si donor was set to 5  1017 cm3. As
for the N plasma condition, the N2 flux of 0.61  105 Torr
a)

Author to whom correspondence should be addressed. Electronic mail:

miyashita@mbe.rcast.u-tokyo.ac.jp. Tel.: 81-3-5452-6514. Fax: 81-35452-6504.

0003-6951/2012/101(22)/222112/4/$30.00

and RF power of 6580 W were used. Compared to our past

works,6 we have chosen a low N2 flux and decreased RF
power for the growth of present GaNAs samples. A post
growth annealing treatment of 250  C, which is low
enough not to change crystalline quality, was carried out to
obtain ohmic contact in a van der Pauw geometry for Hall
measurements.
From atomic force microscope observation, the rootmean square values of the surface morphologies were
0.33 nm (x 0.009) and 0.32 nm (x 0.013), respectively,
which are almost as smooth as 1 mono-layer of GaAs in
thickness. Reflection high energy electron diffraction
(RHEED) pattern was also observed during MBE growth
and it appeared (2  4) streak pattern throughout the growth
of GaNAs layer. These results support that the growth surfaces maintain a two dimensional growth mode. The GaNxAs
(004) diffraction peaks observed by high resolution x-ray diffraction measurement for both samples reveal that 1.0 lm
thick-GaNAs layers can be grown coherently on GaAs substrate, although the diffraction spots, compared to nearly
lattice-matched GaIn0.054N0.016As reference sample,13 are
slightly diffused due to increase of lattice mismatch between
GaAs substrate with incorporating N atoms.
Figure 1 shows photoreflectance (PR) spectra for GaNx
As films, which reveal transition energies from valence band
(EV) to E and E bands as can be explained by the band
anticrossing model.16 Here, we treat transition energy from
EV to E as the bandgap (Eg) of GaNAs, and Eg clearly redshifts with increasing N composition. The PR features at
760840 nm originate from spin-orbit splitted EV D0 to
E transitions.
First, Hall measurements were performed for both samples at room temperature. The free electron concentrations
were 5.2  1016 cm3 and 4.4  1016 cm3 for x 0.009 and
0.013, respectively. Compared to Si donor concentration of
5  1017 cm3 introduced during growth, ratio of electron
activation from Si donor levels was found to be lowered by a
factor of 10. To correctly characterize the incorporation of
Si atoms into Ga(In)NAs, we carried a separate experiment
by secondary ion mass spectroscopy. We found that Si

101, 222112-1

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Miyashita et al.

FIG. 1. Room temperature photoreflectance spectra of GaNxAs films.

donors are incorporated regardless of whether N atoms are

incorporated in Ga(In)As or not. This low activation of Si
donor is usually observed in this alloy.13,14 Compared to the
situation of Si donor, Voltz et al. reported that the Te donors
can supply free electrons in GaInNAs material as the same
level as in GaAs.14 They suggest that N and Si may connect
to form the stable N-Si bond, which can suppress the free
electron supply from Si donor levels. On the other hand, Te
is a group VI donor and cannot form nearest neighbor connection with N atoms, and hence, Te is thought to supply
free electrons as much as the amount of Te atoms introduced.
Another possibility is that Si might play the role of an amphoteric dopant in Ga(In)NAs, resulting in a low net electron
concentration.
The electron mobilities of GaNxAs samples are found to
be 2115 cm2/Vs and 1867 cm2/Vs for x 0.009 and 0.013,
respectively. As shown in Fig. 2, these mobility values are
significantly higher than those previously reported on Si
doped Ga(In)NAs films.8,1115 It is thought that one of the
major origin of low mobility in Ga(In)NAs is random alloy
scattering, which dominates the mobility and considered as
an intrinsic limiting factor.17 In our present study, the mobility values are almost same as this intrinsic limit on electron
mobility in dilute nitrides. It should also be noted that such
any factor as lowering mobility is independent on the

FIG. 2. Plots of mobility vs. electron concentration of n-type Ga(In)NAs

films at 300 K.

Appl. Phys. Lett. 101, 222112 (2012)

magnitude of lattice strain, because high mobility GaNxAs

films have more lattice mismatch to GaAs substrate than
GaIn0.054N0.016As. Therefore, we consider that piezoelectric
effect has less impact on limiting mobility in dilute nitride
films studied here.
Next, the temperature dependences of these parameters
were investigated to clarify the differences with the reference
sample showing low electron mobility. The temperature
dependence of electron mobility is shown in Fig. 3. The mobility for GaIn0.054N0.016As reference sample shows large
decrease in lower temperature region. In contrast, the mobility for both x 0.009 and 0.013 sample shows a less temperature dependence over the whole temperature range and is
similar to the GaAs case shown in the same figure.
The temperature dependence of the electron mobilities
can generally be explained by different scattering components
such as ionized impurity scattering (lII / T3/2), space charge
scattering (lSC / T1/2),18 alloy scattering (lAL / T1/2),17
and polar optical phonon scattering (lPO / T3/2). If each
scattering mechanism contributes independently, then the
resultant mobility can be given by Mattiessens rule,
X
li 1 ;
(1)
l1
where li is the mobility limited by the ith scattering mechanism. Here, we take into account three components shown
below for the parameter fitting,
lII C3=2 T3=2 ;

(2)

lSC C1=2 T1=2 ;

(3)

and
lAL

( p 
)1
 

m 2 dEC 2 3
3m kB T
p

a0 x
;
e
dx
2ph2

(4)

where m* is the effective mass, kB is the Boltzmanns constant, e is the electronic charge, h is the Plancks constant,
EC is the conduction band energy, x is the N composition,
and a0 is the lattice constant. As for the dEC/dx term, we
adopt 10.2 eV,17 while m*/m0 0.088 for the effective
mass of electrons in Ga(In)NAs was deduced from Eq. (4)
and fitting the mobility result of GaN0.013As sample. This
effective mass value is the lowest possible mass for the best

FIG. 3. Temperature dependence of electron mobilities of n-GaNxAs films.

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Miyashita et al.

fit. Good fitting results were achieved even though the

lPO C3/2 T3/2 component is not considered. This is due
to its high limiting mobility values compared to the intrinsic
alloy scattering at high temperature region.
Our fits show that, in addition to the intrinsic alloy scattering, the degree of extrinsic scattering processes by the ionized impurities and space charges distinguishes the
magnitude of mobility in the samples. Figure 4 show experimental data and the fits. The ionized impurity scattering limited mobility, lII, depends on the concentration of ionized
impurities NI ND NA, here ND and NA are the concentration of ionized donor and acceptor, respectively.
Because the Si doping level is fixed, some kind of unintentionally introduced charged scattering centers can increase
the influence of lII. From the results of temperature dependent electron concentration shown in Fig. 5, GaIn0.054N0.016As
sample shows significant drop in electron concentration toward the low temperature region, which suggests the existence of acceptor-like electron trap levels. On the other hand,
the electron concentration values in high mobility GaNxAs
films maintain an order of 1016 cm3 even at 50 K. Then, we
estimated the activation energy of each sample using
r 

NC ND
Ea
exp 
;
(5)
n
2
2kB T
where NC, ND, and Ea are effective density of state in conduction band, donor concentration, and activation energy

FIG. 4. Mobility fitting curves for (a) high mobility GaNxAs (x 0.009 and
0.013) and (b) low mobility GaIn0.054N0.016As films.

Appl. Phys. Lett. 101, 222112 (2012)

FIG. 5. Temperature dependence of electron concentration in GaNxAs

(x 0.009 and 0.013) and GaIn0.054N0.016As films.

from donor level to conduction band, respectively. Ea values

of GaNxAs and GaIn0.054N0.016As samples are 11.4 meV
(x 0.009), 13.5 meV (x 0.013), and 75.6 meV, respectively. Compared to GaNxAs samples, it can be seen that a
new deeper state is obviously introduced in GaIn0.054
N0.016As sample, and it captures electrons emitted from Si
donor level at lower temperature. If capturing electrons, it
can also act as ionized impurity like scattering center.
Because it should influence more in lower temperature
region, this assumption is consistent with the large reduction
of mobility in GaIn0.054N0.016As at low temperature. Up to
date, several groups reported on the electron trap levels in
Ga(In)NAs resulting probably from nitrogen related defects
such as Nint, (N-As)As, and (N-N)As.1921 Such electron traps
can act as acceptor-like levels, although their activation energies were reported 0.250.33 eV below the conduction band
edge. Another possibility is the conduction band fluctuation
caused by inhomogeneous distribution of N atoms, which
leads formation of localized states below the conduction
band of GaNAs.2225 In a separate study using temperature
dependent photoluminescence characterization,22,23 carrier
thermal redistribution among the localized states were discussed. Then, if these localized states also act as acceptorlike center, deepened donor levels observed in GaIn0.054
N0.016As sample can be explained.
In general, for the lSC component, the formation of
some space-charge region can be considered due to the presence of spatially inhomogeneous incorporation of Si dopants,
uneven distribution of N atoms,22 indium segregation, and/or
introduction of anti-site or interstitial defects such as AsGa,
Nint, (N-N)As, and (N-As)As. We think that optimization of
growth condition6,26 or post growth thermal treatments24 can
improve the homogeneity of the material with reduced effect
of lSC component. The improved homogeneity in GaNxAs
samples compared to GaIn0.016N0.054As resulted in reduced
lSC and lII component in Eq. (1) and consequently in higher
mobility.
In summary, high mobility above 2000 cm2/Vs have
been obtained in Si doped GaNAs films grown by MBE.
From the analysis of temperature dependent mobility plot, it
was experimentally shown that both intrinsic limiting factor

222112-4

Miyashita et al.

of random alloy scattering and extrinsic introduced ionized

impurity scattering limit the electron mobility of high quality
GaNAs alloy.
This work was performed under SOLAR QUEST program supported by the Incorporated Administrative Agency
New Energy and Industrial Technology Development Organization (NEDO) under Ministry of Economy, Trade and
Industry (METI), Japan.
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