See discussions, stats, and author profiles for this publication at: https://www.researchgate.

net/publication/316941595

Donor Impurity States in Semiconductor Zincblende Nitride Quantum

Systems as a Source of Nonlinear Optical Response

Article  in  Journal of Nanoscience and Nanotechnology · February 2017

DOI: 10.1166/jnn.2017.13062

CITATIONS READS

0 88

3 authors:

Julian Correa M. E. Mora-Ramos

Universidad de Medellín Universidad Autónoma del Estado de Morelos
47 PUBLICATIONS   734 CITATIONS    281 PUBLICATIONS   2,333 CITATIONS   

SEE PROFILE SEE PROFILE

C. A. Duque
University of Antioquia
326 PUBLICATIONS   3,982 CITATIONS   

SEE PROFILE

Some of the authors of this publication are also working on these related projects:

optical properties of type II quantum dots for photovoltaic applications View project

Nonlinear optical properties in low dimensional systems. View project

All content following this page was uploaded by M. E. Mora-Ramos on 30 May 2017.

The user has requested enhancement of the downloaded file.

Correct cite: Vol. 17, No. 2, pp. 1517-1524 (2017)

Article
Journal of
Copyright © 2016 American Scientific Publishers
Nanoscience and Nanotechnology
All rights reserved Vol. 16, 1–8, 2016
Printed in the United States of America www.aspbs.com/jnn

Donor Impurity States in Semiconductor

Zincblende Nitride Quantum Systems as a
Source of Nonlinear Optical Response
J. D. Correa1 , M. E. Mora-Ramos2
∗ , and C. A. Duque3
1
Departamento de Ciencias Básicas, Universidad de Medellín, Medellín, Colombia
2
Centro de Investigación en Ciencias-IICBA, Universidad Autónoma del Estado de Morelos. Av. Universidad 1001,
CP 62209, Cuernavaca, Morelos, Mexico
3
Grupo de Materia Condensada-UdeA, Instituto de Física, Facultad de Ciencias Exactas y Naturales,
Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín, Colombia

The optical absorption and the optical rectification coefficients associated to hydrogenic impurity
interstate transitions in zincblende GaN-based nanostructures of the quantum wire type are investi-
gated. The system is assumed to have cylindrical shape and the influence of external tuning probes
such as hydrostatic pressure and static electric fields is particularly taken into account. The elec-
tron states are obtained within the effective mass approximation, via the exact diagonalization of
the donor-impurity Hamiltonian with parabolic confinement. The nonlinear optical coefficients are
calculated using a nonperturbative solution of the density-matrix Bloch equation. Our results show
that the resonance-related features of the optical response become shifted in the frequency range
of the incident radiation due to the effect of the hydrostatic pressure, the strength of the applied
field and the change in the impurity center position.
Keywords: Zincblende GaN, Quantum Wire, Nonlinear Optics, Hydrostatic Pressure.

1. INTRODUCTION zincblende substrates such as GaAs.8 It is known that

The III–V nitride compounds have attracted more attention
in their wurtzite allotropic form. But cubic nitrides actu-
ally exhibit interesting properties from the point of view
of electronics and optoelectronics applications. Zicblende
nitride semiconductor films have been grown with high
crystal quality.1–4 A review of the basics and applica-
tions in optoelectronics of cubic III-nitride-based nano-
structures can be found in Ref. [5]. The cubic symmetry
avoids the presence of high spontaneous polarizations in
the crystal, which are partially responsible for the pres-
ence of large built-in fields in polar wurtzite-based het-
erostructures. This phenomenon causes the impairing of
the carrier recombination leading to drops in efficiency in
light emitting diodes.6, 7 On the other hand, the zincblende
(ZB) structure in nitrides is associated with higher car-
rier mobilities, larger optical gain and lower threshold cur-
rent density because of its smaller effective mass, whereas
it has mirror facets compatible with non-nitride III–V
∗
Author to whom correspondence should be addressed.
structures based on cubic III–V nitride semiconductors
do not suffer from the problem of strong internal elec-
tric fields. Recent reports show the increasing interest in
the fabrication of ZB-nitride-based devices. For instance,
it has been demonstrated that high-quality cubic GaN can
be grown on silicon substrates, overcoming the challenge
of obtaining in a commercial way this material, character-
ized by a thermodynamically unstable crystal structure.9
Then, the development of nanostructures using ZB GaN
semiconductor is relevant for the production of short wave-
length optoelectronic devices, high temperature devices
and high frequency high power devices.10 The use of
dry chemical etching allowed to obtain cubic GaN quan-
tum dots embedded in zincblende AlN microdisks.11 Fur-
thermore, the growth of ZB GaN quantum dot has been
reported demonstrating the versatility of the so called layer
transfer method to fabricate a large variety of ZB III-
nitride photonic structures operating at short wavelengths,
including photonic crystal nanocavities and waveguides.12
However, only few reports on zincblende-nitride-based

J. Nanosci. Nanotechnol. 2016, Vol. 16, No. xx 1533-4880/2016/16/001/008 doi:10.1166/jnn.2016.13062 1

Correct DOI: 10.1166/jnn.2017.13062

Donor Impurity States in Semiconductor Zincblende Nitride Quantum Systems
quantum wires (QWs) have been published in the recent
years.13–17
In general, the optoelectronic properties of semicon-
ductor low-dimensional systems can be affected by mod-
ifying the geometrical and compositional configurations
(shape, size, alloying), and by applying external probes
which are mainly electromagnetic fields, strain or hydro-
static pressure, or both. The issue of the combined effects
of an externally applied field and the hydrostatic pressure
is worth of investigating because those combined effects
can induce new response ranges, such as the appear-
ance of blue-shifts or red-shift in the optical response
of the structures, thus opening the way to the develop-
ment of new applications. In particular, the influence of
hydrostatic pressure in cubic nitride QDs has been con-
sidered by by Baser et al.15 and by Xia et al.18 On the
other hand, the production of electronic and optoelectronic
devices based on semiconductor materials usually requires
the doping of the material with the inclusion of either
donor or acceptor atoms in the crystal. Besides, in spite
of the high levels of purity obtained during the crystal
growth processes of nowadays, there is always a degree
of non-intentional doping in the semiconductor matrix.
In consequence, it turns out that the study of donor impu-
rities in ZB GaN based nanostructures is fundamental to
understand the physical behavior of this kind of systems.19
In particular, the reference15 studies the hydrogenic impu-
rity states in InGaN/GaN cylindrical quantum well wires,
whereas Wang and collaborators investigated the impurity
states under hydrostatic pressure in ZB InGaN/GaN quan-
tum wells.20
Among the different manifestations of the optical
response of a nanostructure under applied electric field,
the optical absorption is one of the most studied.21 In
a seminal paper dealing with quantum wells, Ahn and
Chuang reported on the linear and nonlinear absorption
coefficients via a perturbative formalism for solving the
density matrix equation.22 Afterwards, the same approach
has been widely used to calculate the nonlinear optical
absorption in different semiconductor heterostructures (for
a few examples see, for instance, Refs. [23–26]).
, with 0 being the distance between the wire’s
The nonlinear optical rectification (NOR) effect (also
named as dc effect) was discovered by Bass et al. in
1962.27 It is detected as a static polarization of the nonlin-
ear system that is proportional to the second power of the
incident field amplitude. Among its applications one may
list the measurements of nonlinear crustal susceptibilities
as well as of the power, polarization and profile of laser
pulses; excitation of electromagnetic waves in resonators
and waveguides, generation of infrared radiation, and non-
linear spectroscopy28 and, more recently, the generation of
THz radiation with the use of ultrafast laser pulses.29 In
semiconducting nanostructures, it is possible to mention-
for instance-the experimental observation of large NOR
in compositionally asymmetric quantum wells,30 whereas
2 J. Nanosci. Nanotechnol. 16, 1–8, 2016
Correa et al.
giant NOR was found in asymmetric coupled double
quantum wells.31 From the theoretical point of view, a key
reference is the work by Rosencher and Bois in quantum
wells.32
Recently, Paspalakis et al. reported new expressions for
the nonlinear optical absorption and optical rectification
coefficients.33 Their formalism is based in the two-level
model an the rotating wave approximation. One of the fea-
tures of this scheme is that the problem of saturation of
the optical absorption is properly addressed.
Motivated by the above commented elements, in this
work we report a study on the nonlinear optical suscep-
tibility associated to hydrogenic impurity interstate tran-
sitions in GaN quantum wires of cylindrical shape taking
into account the effects of externally applied static elec-
tric field and hydrostatic pressure. We make use of the
effective mass approximation, via the exact diagonaliza-
tion of the donor-impurity Hamiltonian with parabolic con-
finement and external field effects. The nonlinear optical
properties are then calculated using the model put forward
in Ref. [33]. The next section will be devoted to com-
ment the theoretical framework whereas in section 3 the
results obtained will be presented and discussed. Finally,
the section 4 contains the conclusions of the work.
2. MODEL THEORY
In the framework of the effective mass approximation, the
Hamiltonian of the system is given by



2  1  e2
−
·
−  + V   + eF  cos 
2 m∗ ∗ 2 + z2
(1)
where m∗ P  and P  are the pressure dependent con-
duction band effective mass and static dielectric constant,
respectively, e is the absolute value of the electron charge
and g =
/m∗ R2  is the frequency associated with the
lateral confinement. The wire’s cross section has a cir-
cular shape with radius R, and we choose to model the
confining conduction band potential energy profile via the
parabolic function V   = 1/2m∗ 2g  cos  +0 2 +
 sin 2
axis and the impurity position. We have defined a QW
radius in terms of  the expectation
 value of the in-plane
coordinate 2 : R = 2  =
/m∗ g . The external elec-
tric field (F ) is applied perpendicularly to the QW axis.
For the purpose of the calculation, the position of the
impurity atom can be considered both on-axis or off-axis.
Given the geometry of the structure, we choose the set of
cylindrical coordinates with the center placed at the impu-
rity position. In order to obtain the energy spectrum of the
system we need to solve the eigenvalues equation:
Ĥ = E (2)
With this purpose, we propose the wavefunction  as
an expansion in a Gaussian-like basis set. As a result,
Correa et al. Donor Impurity States in Semiconductor Zincblende Nitride Quantum Systems
we obtain the eigenstates by direct diagonalization of the
resulting Hamiltonian matrix. Details of this specific solu-
tion are quite extensively given in our previous works.14, 17
The effects of the hydrostatic pressure in the electronic
properties of the QW are included through the pressure
dependence of the different input parameters. That is,
effective mass, dielectric constant and QW radius. The
specific dependencies, in the case of ZB GaN are taken
from previous works on the subject.15, 34–36 Then, the effec-
tive mass, as a function of the hydrostatic pressure is
given by
m0 C appear with a significant mixing of both longitudinal and
= 1+ (3)
m∗GaN Eg P 
where C is a constant and Eg P  is the bandgap energy as
a function of the hydrostatic pressure, given by
In this expression, fi is the ionicity of the material, and
BP  is the bulk module pressure dependence given by

BP  = B0 + B0 P (11)
The use of the bulk phonon information is a convenient
approximation aiming at providing a suitable qualitative
description of an otherwise troublesome problem. In a sys-
tem like the one here investigated, the phonon spectrum
is largely modified from its bulk features due to the pres-
ence of interfaces. Confined and interface vibration modes
transversal polarizations (see Ref. [37]). In consequence,
a more complicated relation between the frequencies of
the phonon modes would appear. Thus, the only way for
a proper description of the hydrostatic pressure effects
Eg P  = Eg 0 + P +
P 2  (4) would be a microscopic-first principles-calculation of  in
our particular system. Clearly, this lies beyond the scope
The dependence of the radius on the hydrostatic pres- of the present work.
sure can be written as Once we know the eigenvalues and eigenstates of the

RP  = R0 1 − 2P S11 + S12  (5) impurity in the QW, we can derive analytical expressions
for the diagonal and off-diagonal matrix elements of the
where S11 and S22 are the elastic compliance constants. We electric dipole moment operator, M̂ , in the system (for
evaluate them using the relation of these particular tensor details view17 ). Then, according to Paspalakis et al.,33
elements with those of its inverse one—the elastic stiffness the inter-state nonlinear optical absorption coefficient as
tensor—which are no other than the elastics constants of a function of the incident light frequency near the reso-
the medium C11 and C12 . In the cubic symmetry case, they nance is
are given by
C11 + C12 I 
S11 = (6) e2 ii Mfi 2 Efi
C11 − C12 C11 + 2C12 
=
and 0
nr c
C12  2   
S12 = − (7) J eMff −Mii Ẽ/
 −J 2 eMff −Mii Ẽ/
 
0 2
C11 − C12 C11 + 2C12  ×
fi ii +ii /fi 
−Efi 2 +
fi I
To deal with the pressure effect on the dielectric screen-
ing we shall make the following simplifying assump- (12)
tion: The static dielectric constant is determined from
where
the Lyddane-Sachs-Teller relation, involving the pressure


dependence of the longitudinal and transversal long wave- ce2 I Mfi 2 eMff −Mii Ẽ
length optical phonon modes:
fi I  = J0
2nr




LO 2 eMff −Mii Ẽ 2
P  =  P  (8) +J2 (13)
TO

Here, LO and TO are the longitudinal optical and
In these expressions, J0 x and J2 x are the Bessel
transversal optical zone-center phonon frequencies, respec-
functions of the first kind. In addition, fi =
/Tfi , and
tively, and  P  is the pressure-dependent high frequency
ii =
/Tii . The quantity Tfi is the transverse relaxation
dielectric constant. With the help of the mode-Grüneisen
(or dephasing) time of the transition, whilst Tii is the lon-
parameter (i ) we can calculate LO P  and TO P 
gitudinal relaxation (or population decay) time. Besides,
through the expression
Efi = Ef − Ei is the transition energy difference,  is
1 i P  the magnetic permeability of vacuum, 0 is the free-space
i = B0 (9)
i P dielectric permittivity, and c is the speed of light in the free
where, B0 is the bulk module at P = 0. Finally the pressure space. On the other hand, Mfi = f  cos i  are the
dependence of the high frequency dielectric constant is matrix elements of the projection of the electron-impurity
given by distance along the incident light polarization direction.
 5 − 1 Additionally,  is the 3D √ density of carriers involved in
≈ 09 − fi  (10) the transition and nr =  is the refractive index of the
P 3B
J. Nanosci. Nanotechnol. 16, 1–8, 2016 3
Donor Impurity States in Semiconductor Zincblende Nitride Quantum Systems Correa et al.

material. The quantity I is the intensity of the incident (a) 0.23

light, which relates with the amplitude of the incoming
electromagnetic radiation (Ẽ) through the relation 0.22

nr 0 cẼ2 0.21
I= (14)

m*(P)
2
0.2
In addition, from the real part of the nonlinear suscep-
tibility one extracts the expression for the coefficient of 0.19
relative change of the refraction
nI  Efi −
 ii 0.18
= 0 5 10 15 20 25 30
nr cnr 0 I fi
(b)

fi I 
× 9.6
fi ii +ii /fi 
−Efi 2 +
fi I 
(15) 9.4

ε∗(P)
whilst an independent procedure leads to the coefficient of
9.2
NOR which is given by
4nr eMff −Mii  ii
0 I  = 9
c0 I fi

fi I  0 5 10 15 20 25 30
× (16) P(GPa)
fi ii +ii /fi 
−Efi 2 +
fi I 
Figure 1. Effective mass (a) and static dielectric constant (b) of the
bulk-GaN as a function of hydrostatic pressure.
3. RESULTS AND DISCUSSION
To study the effects of the hydrostatic pressure on the zero applied electric field. It is possible to observe that as
optical properties of zincblende GaN QW, we consider a long as the hydrostatic pressure augments the energy of the
QW of radius 6 nm. The numerical results are obtained ground impurity state decreases. This behavior is mainly
using the following values of the involved parameters: caused by the reduction in the value of ∗ P  as shown in
For the calculation of the effective mass the C constant the Figure 1(b). This trend is also detected in the case of
is 13.73 eV, the band gap at zero pressure is Eg 0 = the ground state energy in the situations with off-center—
322 eV. To describe the hydrostatic pressure dependence at 3 nm—impurity position and zero field and with on-
of the band gap we have used  = 40 meV/GPa and
= center donor atom and F = 20 kV/cm (Figs. 2(b and c),
−038 meV/GPa2 . The hydrostatic pressure dependence respectively).
of elastic constants and the bulk module values are taken On the other hand, at the zero field, on-center donor
from Ref. [35], and are such that C11 = 252 + 417P − impurity configuration, the excited energy states decrease
0019P 2, C12 = 131 + 350P − 0011P 2, B0 = 1713, and with the pressure until reaches a minimum value. Then, the

B0 = 372. The high frequency dielectric constant at P = 0 ulterior increment of the hydrostatic pressure leads to the
is  0 = 53, the mode-Grüneisen parameters are LO = increase of the energies, and this also occurs to a greater
12 and TO = 14, the longitudinal optical and transver-
sal optical zone-center phonon frequencies at P = 0 are
respectively LO 0 = 743 cm−1 and TO 0 = 553 cm−1 ,
and finally the material ionicity is taken as fi = 05. For
illustration, the Figure 1 shows the variation of both the
electron effective mass and the static dielectric constant as
functions of the hydrostatic pressure.
The functional dependencies m∗ P  and ∗ P  have the
typical behaviors occurring in the III–V semiconductor
compounds. They mean that as long as the pressure grows,
the confined electron states become more localized and the
strength of its Coulombic interaction with a charged center
will be stronger.
The Figure 2(a) shows the impurity energies as func-
tions of the hydrostatic pressure with on-axis impurity at
4 J. Nanosci. Nanotechnol. 16, 1–8, 2016
or lesser extent in the other two configurations considered.
All this behavior is a result of the competition between the
different pressure-dependent influences—effective mass,
dielectric constant, wire radius—in the system as com-
mented. Clearly, the effect of the pressure-induced reduc-
tion in the radial size will be more strongly felt by the
excited energy levels—greatly due in our case to the rather
large energy separation between them and the ground state.
The consequence is the predominance of the increment in
the degree of confinement and thus the rise of the corre-
sponding energy values.
The localization of the donor impurity atom out of the
QW axis (0 = 3 nm) as well as the application of a
Dc electric field (F = 20 kV/cm) along the radial direc-
tion are both causes of symmetry breaking in the system
Correa et al. Donor Impurity States in Semiconductor Zincblende Nitride Quantum Systems

(a) (b) (c) (a) 10 (b) 1

10
8
0.5

|M1i|2(nm2)
6

Mii(nm)
0
0
4

–0.5
2

–10 0 –1
0 5 10 15 20 25 30 0 5 10 15 20 25 30
P(GPa) P(GPa)
E(meV)

(c) 10 (d) 10

8
–20 8

6 M11

|M1i|2(nm2)
6 M22

Mii(nm)
M33
|M12|2 4 M44
4 |M13|2
|M14|2 2
–30
2 |M15|2
0

0 –2
0 5 10 15 20 25 30 0 5 10 15 20 25 30

–40 P(GPa) P(GPa)

0 10 20 30 0 10 20 30 0 10 20 30
P(GPa) P(GPa) P(GPa) Figure 3. Dipole matrix elements in a cylindrical GaN quantum wire
with parabolic confinement potential as a function of the hydrostatic pres-
Figure 2. Calculated hydrogenic impurity energies in a zincblende GaN sure. In (a and c) are depicted the squared dipole off-diagonal matrix
quantum wire with parabolic confinement potential as functions of hydro- elements for the transitions between the ground state and the first four
static pressure. The wire radius has been set to 6 nm. (a) for on-axis excited states, whereas (b and d) correspond to the dipole diagonal matrix
impurity position and zero applied electric field (b), the radial impurity elements. Different configurations are include: (a and b) are for on-axis
position is 0 = 3 nm and zero applied electric field, and (c) the electric impurity and zero applied electric field, whereas (c and d) are for off-axis
field intensity is 20 kV/cm for on-axis impurity position. impurity (0 = 3) and F = 20 kV/cm.

as was discussed in a previous work.14 Such an effect
gives rise to changes in the confining potential which
modify the energy spectrum in comparison with the com-
pletely symmetrical structure as can be seen from the
Figures 2(b and c). Under both circumstances, the ground
state behaves much alike. It exhibits a slight increase
which can be explained by the presence of the linear term
in the -dependent potential function.
At zero pressure, the upper states behave in different
manners. For instance, the first excited state has a small
decrease related with the enhancement of the Coulombic
attraction that occurs because of the reduction in the aver-
age electron-impurity distance, whereas the-split-second
one shifts upwards due-in this case-to the combined effect
of the stronger confinement and the change in the prob-
ability density distribution that moves the electron farther
away from the donor center, and so on. All such displace-
ments are mostly governed by the changes in the corre-
sponding confining potential configurations.
The graphics in Figure 3 show the variation of the
dipole moment matrix elements as functions of the
hydrostatic pressure. Off-diagonal dipole moment matrix
elements having the ground state as the initial one
appear in Figures 3(a and c). Permanent dipole moments
(diagonal elements) are depicted as functions of P in
Figures 3(b and d). The role played by the system’s
symmetry is readily noticed. In the on-axis donor cen-
ter plus zero electric field case the selection rules lead to
the quenching of the permanent polarization, keeping as
nonzero quantities the contributions of the non-permanent
polarization coming from transitions between states with
different parities. However, the shift of the impurity atom
away from the center together with the application of an
electric field cause the loss of the central symmetry giving
rise to additional possibilities for the dipole polarization in
the structure.
In Figure 4 we show the linear (when I ≡ 0), non-
linear and total optical absorption coefficient for different
values of hydrostatic pressure. The absorption process
implies the—allowed—transition from the ground to a
given excited state. In the column (1) the obtained results
correspond to the on-axis impurity configuration and the
external electric field is set to zero. We can observe a
blue-shift of the main linear and nonlinear absorption—
related with the transition from the ground to the second
excited state—peak as the hydrostatic pressure increases.

J. Nanosci. Nanotechnol. 16, 1–8, 2016 5

Donor Impurity States in Semiconductor Zincblende Nitride Quantum Systems Correa et al.

(1) (2) absorption coefficient is smaller compared with the case

(a) 40 (a) 40
35 in which the impurity locates on-axis. Symmetry reasons
30 30 are responsible for a significant reduction of the ampli-
αl(104m–1)

25 tude of this particular contribution. Moreover, one notices

20 20
15 that the pressure acts as an optical response quencher for
10 10 this nonlinear part. This means that the pressure acts in a
5 way that maximizes the contribution of
fi  I . In other
0 0
0 20 40 60 80 0 20 40 60 80 words, the radial asymmetry associated to the displacement
(b) 0 (b) 0
of the impurity center away from the cylinder’s axis causes
–5 –5
a change in the permanent dipoles of the system in such
a way that the element Mff − Mii  approaches zero-the
αn1(104m–1)

–10 –10
value at which the factor J0 x + J2 x2 reaches its max-
–15 –15
imum value. This combines with the strong fall of the non-
–20 –20
permanent dipole moment Mfi and leads the nonlinear part
–25 –25
to practically vanish. Then, the optical absorption response
–30 –30
0 20 40 60 80 0 20 40 60 80 of the QW when the impurity is off-axis is approximately
(c) 40 (c) 40
equal to the lineal optical response.
35 35 The Figure 5 contains the same results as the Figure 4
αTotal(104m–1)

30 30 but, in this case, the applied electric field is set at

25 25
20 20
20 kV/cm. When the impurity is on-axis (left-hand
15 15
10 10
(1) (2)
5 5 (a) 30 (a) 40
0 0 25
0 20 40 60 80 0 20 40 60 80 30
αl(104m–1)

EPhoton(eV) EPhoton(eV) 20
15 20
Figure 4. The impurity-related optical absorption coefficient in a cylin-
10
drical GaN quantum wire with parabolic confinement as a function of the 10
incident photon energy, the incident radiation intensity is I = 1010 W/m2 . 5
Each line corresponds to a different value of hydrostatic pressure, with P 0 0
0 20 40 60 80 100 0 20 40 60 80 100
ranging from 0 to 285 GPa. The column (1) is for the on-axis impurity
and zero applied electric field configuration whereas column (2) contains (b) 0 (b) 0
the results for the off-axis impurity-0 = 3 nm and zero electric field –5 –5
αn1(104m–1)

case. The filled lines correspond to the zero pressure case. (a) Linear –10 –10
optical response, (b) nonlinear optical response, and (c) total absorption
–15 –15
coefficient.
–20 –20
–25 –25
This behavior is due to the variation of the previously dis-
–30 –30
cussed impurity states. Additionally, it is possible to notice 0 20 40 60 80 100 0 20 40 60 80 100
an increment in the amplitude of the optical response (c) 30 (c) 30
as a consequence of the rising pressure hydrostatic pres- 25 25
αTotal(104m–1)

sure. The main reason for this phenomenon is, initially, 20 20

the increase of the off-diagonal dipole moment matrix 15 15
element-due to a greater degree of wavefunction overlap 10 10
at higher values of the radial position, associated to the 5 5
influence of the hydrostatic pressure-, combined with the
0 0
increment of the transition energy difference Efi . At higher 0 20 40 60 80 100 0 20 40 60 80 100
pressures, the contribution of Mfi 2 slightly decreases and EPhoton(eV) EPhoton(eV)
the reason from the amplitude growth relates mostly with
Figure 5. The impurity-related optical absorption coefficient in a cylin-
the blueshift mentioned. drical GaN quantum wire with parabolic confinement as a function of the
When the impurity atom is located off-axis at 3 nm, the incident photon energy, the incident radiation intensity is I = 1010 W/m2 .
results for the optical absorption coefficient [Fig. 4, col- Each line corresponds to a different value of hydrostatic pressure, with
umn (2)] show the appearance of two absorption peaks P ranging from 0 to 285 GPa. The column (1) is for on-axis impurity
and applied electric field intensity of 20 kV/cm applied electric field.
around 29 meV and 42 meV. When the hydrostatic pressure
Column (2) is for off-axis impurity at 0 = 3 nm and F = 20 kV/cm. The
increases, the positions of these peaks are blue-shifted— filled lines correspond to the zero hydrostatic pressure case. (a) Linear
just under 10 meV when P = 285 GPa. In this case, optical response, (b) nonlinear optical response, and (c) total absorption
the amplitude of the non-linear contribution to the optical coefficient.

6 J. Nanosci. Nanotechnol. 16, 1–8, 2016

Correa et al. Donor Impurity States in Semiconductor Zincblende Nitride Quantum Systems

column), we can observe two pronounced transition peaks, (a) 30

that are blue-shifted as long as the hydrostatic pressure 25
increases. This effect is due to the changes induced by the

χ(10–6m/V)
20
hydrostatic pressure in the impurity energy excited states. 15
In addition, it can be seen that the electric field also causes
10
the reduction of the non-linear optical absorption coeffi-
5
cient compared with the case when the impurity is on-axis
and the electric field is zero. The intensity of the nonlinear 0
0 20 40 60 80
optical absorption coefficient decreases progressively with (b) 30
the increment of the hydrostatic pressure. The physical
25
explanation to this behavior follows the same arguments

χ(10–6m/V)
20
given above in the discussion of the Figure 4.
The calculated nonlinear relative refractive index change 15

related with transitions between electron-impurity states 10

appears in Figure 6. It is possible to detect once again the 5
blueshift effect associated with the influence of the hydro- 0
0 20 40 60 80
static pressure. As discussed, this phenomenon as well as
the behavior of the signal’s amplitude are modulated by the (c) 30

change in the properties of the electron states when dealing 25

with the symmetry-breaking cases of off-center impurity
χ(10–6m/V)
20
and applied electric field. 15
10

(a) 0.1 5
0
0.05 0 20 40 60 80

0 EPhoton(meV)
∆n/nr

–0.05 Figure 7. Nonlinear optical rectification coefficient as a function of the

incident photon energy. Each line corresponds to a different value of
–0.1
hydrostatic pressure (0 ≤ P ≤ 285 GPa. The wire radius is taken equal
to 6 nm. (a) For on-axis impurity position and zero electric field, (b) the
0 20 40 60 80 radial impurity position is 0 = 3 nm and the electric field is zero, and
(b) 0.1 (c) configuration with 0 = 3 nm and F = 20 kV/cm.

0.05
Finally, the coefficient of nonlinear optical rectifica-
∆n/nr

0 tion in a cylindrical zincblende GaN QW is shown in the

–0.05
Figure 7. The calculation has considered the same setups
taken into account in obtaining the above discussed results.
–0.1 Clearly, the case with complete symmetry leads to zero
0 20 40 60 80
NOR response due to the fact that in this case the involved
(c) 0.1 permanent polarization vanish identically. However, non-
0.05 symmetrical configurations can lead to a nonlinear rectifi-
cation response that exhibits the pressure-induced blueshift
0
∆n/nr

and the resonant peak amplitudes of the same order of

–0.05 magnitude already detected in previous reports.38
–0.1

0 20 40 60 80
EPhoton(meV)
Figure 6. Nonlinear relative refractive index change as a function of
the incident photon energy. Each line corresponds to a different value of
hydrostatic pressure, with P ranging from 0 to 285 GPa. The wire radius
has been set to 6 nm. (a) For on-axis impurity position and zero electric
field, (b) the radial impurity position is 0 = 3 nm and the electric field
is zero, and (c) the radial impurity position is 0 = 3 nm and the electric
field intensity is 20 kV/cm.
4. CONCLUSIONS
In this work, we investigated the nonlinear optical
response associated with the electron-donor-impurity states
in zincblende GaN quantum wires of cylindrical shape
under the influence of hydrostatic pressure. The study also
takes into account the possible application of an external
static electric field. The properties under consideration are
the optical absorption, the relative change of the refrac-
tive index and the optical rectification. For each case we

J. Nanosci. Nanotechnol. 16, 1–8, 2016 7

 Donor Impurity States in Semiconductor Zincblende Nitride Quantum Systems
calculate the corresponding coefficient and determine their
features as long as the different system’s parameters are
changed.
In general, the influence of the hydrostatic pressure
causes a shift of the different optical signals towards higher
frequencies. This fact is modulated by the effects of the
electric field and the change of the radial position of the
impurity atom. According to our findings, the dominant
influence among the different effects analyzed is that asso-
ciated with the hydrostatic pressure. One may conclude
that GaN quantum wires with the zincblende crystal struc-
ture may be considered a source for nonlinear optical
response with the associated technological applications.
Up to our knowledge, experimental reports on light
absorption and nonlinear optical rectification in cubic GaN
quantum wire/quantum dot systems are not yet available in
the literature. Therefore, it is not possible to make here a
comparison of our theoretical results. As mentioned in the
introductory section, the methods for obtaining good qual-
ity, thermodynamically stable cubic nitride structures are
developing at a fast pace. Epitaxial layers are now obtained
at relatively low cost. It could be expected that within few
years, quantum dots and even quantum nanopillars made
of c-GaN are obtained. Then, models like the one here
presented would provide a suitable tool for the description
of their optical response.
Acknowledgments: J. D. Correa thanks the Research
Office of Universidad de Medellín by financial sup-
port through the project No. 709. CAD is grateful to
the Colombian Agencies CODI-Universidad de Antio-
quia (Estrategia de Sostenibilidad de la Universidad de
Antioquia), Facultad de Ciencias Exactas y Naturales-
Universidad de Antioquia (CAD-exclusive dedication
project 2015–2016), and El Patrimonio Autónomo Fondo
Nacional de Financiamiento para la Ciencia, la Tecnología
y la Innovación, Francisco José de Caldas.
References and Notes
1. M. Mizuta, S. Fujieda, Y. Matsumoto, and T. Kawamura, J. Appl.
Phys. 25, L945 (1986).
2. S. Yoshida, Physica E 7, 907174 (2000).
3. C.-L. Hsiao, T.-W. Liu, C.-T. Wu, H.-C. Hsu, G.-M. Hsu, L.-C.
Chen, W. Y. Shiao, C. C. Yang, A. Gallstrom, P.-O. Holtz, C.-C.
Chen, and K.-H. Chen, Appl. Phys. Lett. 92, 111914 (2008).
4. S. V. Novikov, N. M. Stanton, R. P. Campion, R. D. Morris,
H. L. Geen, C. T. Foxon, and A. J. Kent, Semicond. Sci. Technol.
23, 015018 (2007).
5. D. J. As, Microelectron. J. 40, 204 (2009).
6. A. D. Andreev and E. P. O’Reilly, Phys. Rev. B 62, 15851 (2000).
8 J. Nanosci. Nanotechnol. 16, 1–8, 2016
View publication stats
Correa et al.
7. S. Schulz, S. Schumacher, and G. Czycholl, Phys. Rev. B 73, 245327
(2006).
8. S. Li, J. Schormann, D. J. As, and K. Lischka, Appl. Phys. Lett.
90, 071903 (2007).
9. In News: Semiconductor Today, Compounds and Advanced Silicon
11, 46 (2016).
10. Y. Dub, B. Changa, X. Fua, X. Wanga, and M. Wang, Optik
123, 2208 (2012).
11. M. Bürger, R. M. Kemper, C. A. Bader, M. Ruth, S. Declair,
C. Meier, J. Förstner, and D. J. As, J. Cryst. Growth 378, 287 (2013).
12. S. Sergent, S. Kako, M. Bürger, S. Blumenthal, S. Iwamoto, D. Josef,
and Y. Arakawa, Appl. Phys. Express 9, 9 (2016).
13. E. Caetano, V. Freire, G. Farias, and E. Da Silva, Appl. Surf. Sci.
234, 5017 (2004).
14. J. Correa, Z. Barticevic, and M. Pacheco, Solid State Commun.
150, 788 (2010).
15. P. Baser, S. Elagoz, and N. Baraz, Physica E 44, 356 (2011).
16. M. Pattammal, A. J. Peter, and C. Yoo, Superlattice Microst. 50, 181
(2011).
17. J. D. Correa, M. E. Mora-Ramos, and C. A. Duque, J. Appl. Phys.
115, 213105 (2014).
18. C. Xia, T. Wang, and S. Wei, Superlattice Microst. 46, 840 (2009).
19. S. Wei and Q. Chang, Physica E 43, 354 (2010).
20. T. Wang, Z. Zeng, C. Xia, and S. Wei, Superlattice Microst. 49, 365
(2011).
21. D. A. B. Miller, D. S. Chemla, T. C. Damen, A. C. Gossard,
W. Wiegmann, T. H. Wood, and C. A. Burrus, Phys. Rev. B 32, 1043
(1985).
22. D. Ahn and S. L. Chuang, IEEE J. Quantum Elect. 23, 2196
(1987).
23. I. Karabulut and S. Baskoutas, J. Appl. Phys. 103, 073512 (2008).
24. E. C. Niculescu and L. M. Burileanu, Eur. Phys. J. B 74, 117 (2010).
25. S. Baskoutas, C. Garoufalis, and A. F. Terzis, TEur. Phys. J. B
84, 241 (2011).
26. M. Sabaeian, M. Shahzadeh, and M. Farbod, AIP Adv. 4, 127105
(2014).
27. M. Bass, P. A. Franken, J. F. Ward, and G. Weinreich, Phys. Rev.
Lett. 9, 446 (1962).
28. B. N. Morozov and Y. M. Aĭvazyan, Sov. J. Quantum Electron. 10, 1
(1980).
29. J. Ahn, A. Efimov, R. Averitt, and A. Taylor, Opt. Express 11, 2486
(2003).
30. E. Rosencher, P. Bois, J. Nagle, E. Costard, and S. Delaitre, Appl.
Phys. Lett. 55, 1597 (1989).
31. E. Rosencher, P. Bois, B. Vinter, J. Nagle, and D. Kaplan, Appl.
Phys. Lett. 56, 1822 (1990).
32. E. Rosencher and P. Bois, Phys. Rev. B 44, 11315 (1991).
33. E. Paspalakis, J. Boviatsis, and S. Baskoutas, J. Appl. Phys.
114, 153107 (2013).
34. C. Xia, Z. Zeng, Q. Chang, and S. Wei, Physica E 42, 2041 (2010).
35. S. P. Łepkowski, J. A. Majewski, and G. Jurczak, Phys. Rev. B
72, 245201 (2005).
36. A. R. Goñi, H. Siegle, K. Syassen, C. Thomsen, and J.-M. Wagner,
Phys. Rev. B 64, 035205 (2001).
37. C. Trallero-Giner, R. Pérez-Álvarez, and F. García-Koliner, Long
Wave Modes in Semiconductor Heterostructures, Elsevier (1998).
38. I. Karabulut, M. E. Mora-Ramos, and C. A. Duque, J. Lumin.
131, 1502 (2011).
Received: 16 December 2015. Accepted: 24 April 2016.