Optics Communications 282 (2009) 3999–4004

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Optics Communications
journal homepage: www.elsevier.com/locate/optcom

Computation of the oscillator strength and absorption coefficients for the

intersubband transitions of the spherical quantum dot
Ayhan Özmen a, Yusuf Yakar b,*, Bekir Çakır a,*, Ülfet Atav a
a
Physics Department, Faculty of Sciences, Selcuk University, Campus 42031 Konya, Turkey
b
Physics Department, Faculty of Arts and Sciences, Aksaray University, Campus 68100 Aksaray, Turkey

a r t i c l e i n f o a b s t r a c t

Article history: The electronic structure and optical properties of one-electron Quantum Dot (QD) with and without an
Received 27 May 2009 on-center impurity were investigated by assuming a spherically symmetric confining potential of finite
Accepted 22 June 2009 depth. The energy eigenvalues and the state functions of QD were calculated by using a combination
of Quantum Genetic Algorithm (QGA) and Hartree–Fock Roothan (HFR) method. We have calculated
the binding energy for the states 1s,1p,1d,1f, oscillator strengths, the linear and third-order nonlinear
Keywords: optical absorption coefficients as a function of the incident photon energy and incident optical intensity
Spherical quantum dot
for the 1s–1p, 1p–1d and 1d–1f transitions. The existence of the impurity has great influence on the opti-
Binding energies
Oscillator strength
cal absorption spectra and the oscillator strengths. Also we found that the magnitudes of the total absorp-
Linear and third-order nonlinear absorption tion coefficients of the spherical QD increase for transitions between higher states.
coefficients Ó 2009 Elsevier B.V. All rights reserved.
QGA and HFR method

1. Introduction
The semiconductor structures have found various application
areas as electronic and electrooptical devices such as infrared
photo detectors, light emitting diodes, single-electron transistors
and quantum computers. Some authors have been focused on the
electronic structure and some other physical properties of the
zero-dimensional quantum dot, which is also called an artificial
atom, because it exhibits the atomic properties like discrete energy
levels and shell structures. Therefore, many authors have studied
to the electronic structure, the ground and excited energy states,
the binding energy, the relativistic effects etc. of the spherical
QDs by using various methods such as perturbation [1], variational
[2–5], exact solution [6,7], QGA [8–10] and a combination of QGA
and HFR method [11,12].
In low-dimensional system, the physical properties of the
spherical QD such as the dipole transition, the oscillator strength,
the linear optical absorption coefficient and the photoionization
cross section are studied by many authors using various computa-
tional techniques [13–18]. Besides, Wang and Guo [19] and Zhang
et al. [20] investigated the linear and third-order nonlinear optical
absorption coefficients in disk-like and one-dimensional parabolic
QDs. In very recently, Xie [21–23] calculated the linear and third-
order nonlinear optical absorption coefficients for a hydrogenic do-
* Corresponding authors.
E-mail addresses: yuyakar@yahoo.com (Y. Yakar), bcakir@selcuk.edu.tr
(B. Çakır).
nor in the spherical parabolic QD. Karabulut and Baskoutas [24] for
a case of spherical QD with parabolic confining potential, Huang
and Libin [25] for a parabolic QD with two-electrons, Chen et al.
[26] for an asymmetric double triangular quantum well, Yuan
[27] for an off-center hydrogenic donor confined by a spherical
QD with a parabolic potential performed the linear and third-order
nonlinear optical absorption coefficients. All studies mentioned
above are focused on the calculation of the transitions between
the lowest energy states, 1s–1p transition for the ground (L = 0)
and the first excited (L = 1) states of the QD.
The QGA method has been used investigation of electronic
structure and other physical properties of QDs. The QGA method
is a version of the Genetic Algorithm (GA) method. The QGA meth-
od is based on the principle of energy minimization just like in var-
iational method. The conventional linear variational method used
in atomic and molecular structure calculations assumes the non-
linear parameters known as a priori and determines only linear
expansion coefficients, whereas in the QGA method both the linear
and nonlinear parameters can be determined from the principle of
energy minimization. We combined the QGA procedure and HFR
method to determine the parameters cpk and fk in Eq. (5) to mini-
mizing the total energy over Slater Type Orbitals (STOs).
In the present paper, we calculated the ground and excited en-
ergy states and the binding energy of the spherical QD with and
without impurity, assuming a spherical symmetric confining po-
tential of finite depth. Moreover, we performed the optical dipole
transition, the oscillator strength, the linear and third-order non-
linear optical absorption coefficients for the 1s–1p, 1p–1d and

0030-4018/$ - see front matter Ó 2009 Elsevier B.V. All rights reserved.
doi:10.1016/j.optcom.2009.06.043
4000 A. Özmen et al. / Optics Communications 282 (2009) 3999–4004

1d–1f transitions in a spherical QD with and without impurity. On is the kinetic energy,
the other hand, the linear and third-order nonlinear optical absorp- Z R   Z 1  
Z Z
tion coefficients for all transitions investigated as a function of the hV i i ¼ ð/ir<R Þ  r<R /ir<R ds þ ð/ir>R Þ  r>R /ir>R ds;
incident photon energy and dot radius. 0 e r R e r
ð9Þ
2. Theory and formulations is the coulomb energy between the electron and the impurity, and
D E Z 1
We consider a shallow hydrogenic impurity located at the cen- V conf
i ¼ V0 ð/ir>R Þ /ir>R ds; ð10Þ
ter of a spherical QD confined by a finite spherical potential well R

with radius R. The Hamiltonian of this system can be written in is the energy due to the confining potential. When the wave func-
the effective mass approximation as tion given in Eq. (5) is substituted in Eqs. (8)–(10), these integrals
r2 Z are obtained in terms of the expansion coefficients and new inte-
H¼  þ VðrÞ; ð1Þ grals over STO’s. The integrals over STO’s have been extensively
2m er r
studied long before by many authors for the calculation of atomic
where Z is impurity charge, r is the distance between the electron to
system properties [28–30]. For QDs, the integrals given in Eqs.
the impurity, m* is the effective mass of the electron and er denotes
(8)–(10) can be easily evaluated by modifying the expressions for
the real part of the relative dielectric constant of the medium. The
atomic systems by appropriate consideration of the boundaries.
confinement potential is assumed in a form of the spherical poten-
The expansion coefficients cr<R r>R
ik , c ik and the screening constants
tial well, i.e. V(r) = 0 for r < R and V(r) = V0 for r > R. The time inde-
fr<R
ik , fr>R
ik are determined by using the QGA and HFR method from
pendent Schrödinger equation for this system is given by
the minimization of total energy Ei. Details of the method are given
Hwi ¼ Ei wi ; ð2Þ in Ref. [11].
In the electric dipole approximation, if the polarization of the
in which Ei is the energy and wi is the wave function for ith eigen-
electromagnetic radiation is chosen in z-direction, the dipole tran-
state of the system. The wavefunctions wi are orthonormalized, and
sition matrix element between ith state (lower) and fth state
the wavefunction and the probability flux should be continues at
(upper) is given by
the interface between GaAs and AlGaAs (r = R), i.e
Z R Z 1 
Z R Z 1
hM z ifi ¼ e ð/r<R Þ r cos h/r<R ds þ ð/r>R Þ r cos h/r>R ds :
ðwir<R Þ wjr<R d sþ ðwr>R
i Þ wjr>R d s ¼ dij f
0
i
R
f i
0 R
ð11Þ
and
  The matrix element is important for the calculation of different



r>R  1 dwir<R  1 dwir>R 
wr<R
i ¼ wi r¼R   ¼   : ð3Þ optical properties of the system related to electronic transitions. In
r¼R mr<R dr  mr>R dr 
r¼R r¼R spherical QD dipole transitions are allowed only between states
The eigenstates of the system can also be determined from the satisfying the selection rules D‘ = ±1, where ‘ is the angular
variational principle by minimizing the energy of the system corre- momentum quantum number.
sponding to the trial wave function /i The oscillator strength is a very important physical quantity in
the study of the optical properties which are related to the elec-
Ei ¼ h/i jHj/i i=h/i j/i i: ð4Þ tronic dipole-allowed transitions, and it is a dimensionless quan-
Within the HFR approach the wavefunction /i are written as lin- tity. The oscillator strength Pfi is expressed as follows
eal combinations of STOs, called basis set. We have used two differ- 2m  2
ent basis sets for inner and outer parts of the QD. As a result our Pfi ¼ 2
DEfi Mfi  ; ð12Þ
h
wave function is of the form
where DEfi = Ef  Ei denotes difference of the energy between lower
/i ¼ HðR  rÞ/r<R
i þ f1  HðR  rÞg/r>R
i and upper states. The oscillator strength can offer additional infor-
rr<R
X rr>R
X mation on the fine structure and selection rules of the optical
r<R r>R
¼ HðR  rÞ cr<R
ik vk ðfik ; rÞ þ f1  HðR  rÞg
~ r>R
cik vk ðfik ;~rÞ; absorption [31].
k¼1 k¼1 Photoabsorption process may be defined as an optical (inter-
ð5Þ subband) transition in low dimensional quantum mechanical sys-
where H(x) is the Heviside step function, r (r ) is the size of the r<R r>R tems. The photoabsorption occurs from a lower state to an upper
basis set used for the inner (outer) part of the wave function, state with absorbing a photon. The absorption computations for
cr<R r>R r<R r>R intersubband are based on Fermi’s golden rule, and the total optical
ik ðcik Þ are the expansion coefficients and fik ðfik Þ are the
screening parameters for the inner (outer) part of the wave function absorption coefficient is given [19,20,25]
of i.th eigenstates. The unnormalized complex spherical STO’s has aðx;IÞ ¼ a1 ðxÞþ a3 ðx;IÞ
the general form 8 9
rffiffiffiffiffiffiffiffiffi>
<  2  4 >
=
l h M  q h C 2I  M  q hC
vnk ‘k mk ðfk ; rh/Þ ¼ rnk 1 efk r Y ‘k mk ðh; /Þ; ð6Þ ¼x 
fi

o
i h 
fi

o
i ;
er e0 > 2
: Efi hx þ ðhCo Þ 2 2
nr eo c Efi hx þ ðhCo Þ ;
2
2>

where nk ; ‘k ; mk are the quantum numbers of basis functions and

Y‘m(h,u) are well-known complex spherical harmonics in Condon– ð13Þ
Shortley Phase convention. The energies of the system is given by where the term a1(x) and a3(x, I) denote the linear and third-order
D E
Ei ¼ hT i i þ hV i i þ V conf ; ð7Þ nonlinear optical absorption coefficients, I is the incident optical
i
hx is the incident photon energy, l is the permeability
intensity, 
where of the system defined as l = 1/e0c2, the q is the electron density
! ! pffiffiffiffi
Z Z in the QD, C0 is the relaxion ratio for states f and i, nr ¼ er repre-
R
r2 1
r2
hT i i ¼ ð/ir<R Þ  /r<R
i ds þ ð/r>R
i Þ  /r>R
i ds; sents the refraction index of the semiconductor, c is the speed of
0 2mr<R R 2mr>R
light in vacuum and e0 is the electrical permittivity of the vacuum,
ð8Þ respectively.
 A. Özmen et al. / Optics Communications 282 (2009) 3999–4004 4001

Since the third-order nonlinear optical absorption coefficient 24

a3(x, I) is negative and is proportional to the incident optical inten-
21 1s
sity I, the total absorption coefficient a(x,I) is decreases as I in-
1p
creases. Therefore, a(x,I) is reduced by one-half when I reaches a 1d
18
value, called the saturation intensity. 1f

eV)
15
3. Computational technique

STOs are preferred in the quantum mechanical analysis of the
electronic structure of a QD as they represent correct behaviour
of the electronic wavefunctions. Therefore, we have chosen a linear
combination of s (or p, d) STOs having different screening param-
eters for a s (or p, d) type atomic orbital. To maintain the orthogo-
nality of orbital the same set of screening parameters was used for
all the one-electron spatial orbital with the same angular momen-
tum, and took five basis sets (r = 5) to calculate the expectation va-
lue of the energy.
The QGA method used in our calculation is based on three basic
genetic operations: these are reproduction, crossover and muta-
tion. The method starts up with an initial random population of
possible solutions of the problem. A fitness value is assigned to
each individual in the population. In the reproduction process
the individuals of current population are copied to the next gener-
ation, according to their fitness values. Therefore, in performing
reproduction process, a selection procedure is necessary to choose
the individuals to be copied to the next generation. In the crossover
operation two individuals randomly selected from the present are
combined to obtain two new individuals of the next generation
population. Another operation in QGA, the mutation process plays
an important role in getting out of local minima and is imple-
mented at lower probabilities than other operations. In this pro-
cess, the genetic information is changed randomly. Here we have
given only the outline of the procedure. The details of the QGA
used in this study are given in our previous work [11].
4. Results and discussion
In the production of quantum nanostructures GaAs and AlGaAs
are extensively used for the well and barrier regions respectively.
Also the physical parameters of these materials are well known.
Therefore, we have used these material parameters in this study
and assumed that the confining potential is a spherical well of fi-
nite depth. The atomic units (a.u.) have been used in the determi-
nation of electronic energies and wave functions, in which the
electron charge e, the Planck constant  h, the electron mass m0
and 4pe0 are assumed as unit. The effective Rydberg energy
2 2
Ry ¼ 
h =mr<R a and the effective Bohr radius a ¼  h er<R =mr<R e2 .
We have used the material parameters mGaAs = 0.067m0, mAl-
GaAs = 0.088m0, eGaAs = 13.18, eAlGaAs = 12.24, V0 = 228 meV and
-2
Energy (10
12
9
6
3
0
0 1 2 3 4 5 6
*
Rdot(a )
Fig. 1. The ground and excited state energies of the QD with (with solid circles) and
without (without solid circles) the impurity as a function of dot radius.
with impurity lies under the 1s energy state of the case without
impurity about R > 2.6a* because of the impurity attractive cou-
lomb potential. In the same way, the 1d and 1f energy states of
the QD with impurity lie under the 1p and 1d energy state of the
case without impurity about 3.8a* and 5a*, respectively. This is be-
cause that the electrons become less confined when the dot radius
increases and their kinetic energies therefore decrease. For the case
with impurity the contribution of the coulomb interaction be-
comes dominant for large dot radii.
The effect of the attractive coulomb potential of the impurity on
the total energy can be more clearly seen in Fig. 2, which the differ-
ence between the total energies of the cases with and without
impurity is given. This difference can be regarded as the binding
of the electron to the impurity. This binding energy increases with
decreasing dot radius. At some critical radius it reaches to a max-
imum value and then it rapidly decreases with decreasing dot ra-
dius. For smaller dot radii the contribution of confinement
becomes dominant resulting in a rapid decrease of the binding en-
ergy, eventually forcing the electron to be unbound. This results
are in good agreement with the previous studies [2,6,18].
The oscillator strength is a useful parameter to obtain informa-
tion on electronic structure and optical properties of a QD. The
50 1s
1p
Binding energy (10 eV)

1
C0 ¼ 1:4 ps. The effective Rydberg energy and Bohr radius corre- 40 1d
sponding to these material parameters are Ry ¼ 5:72 meV,
-3

1f
a ffi 100 Å.
Fig. 1 shows the energies of ground (1s), first (1p), second (1d) 30
and third (1f) excited states of the spherical QD with and without
the impurity as a function of dot radius. As seen from Fig. 1, the
20
energies of electronic levels decrease with increasing dot radius.
The energies approach a value corresponding to the energy of a
free space hydrogen when the dot radius is large enough. For 10
example, for R = 25a*, we obtained the energy values (1,
 0.2499, 0.1106 and 0.0551) in effective Rydberg units for
1s-, 1p-, 1d- and 1f- states which can be compared to Hydrogen en- 0
ergy eigenvalues (1, 1/4, 1/9 and 1/16) in terms of Rydberg. 0 1 2 3 4 5
There is a critical dot radius for each state below in which the elec- Rdot(a* )
tron becomes unbound. These critical radii are very close for the
cases with and without impurity, but the radii are slightly smaller Fig. 2. Binding energy of the spherical GaAs/AlGaAs QD as a function of the dot
when there is an impurity. In Fig. 1, the 1p energy state of the QD radius.
4002 A. Özmen et al. / Optics Communications 282 (2009) 3999–4004

In Fig. 4 we show the linear a1(x), third-order nonlinear a3(x, I)

1.8
and total a(x,I) optical absorption coefficients for transitions be-
1.6 tween various states of the QD with and without impurity as a
function of the incident photon energy h  x. As seen from Fig. 4,
1.4
the linear absorption coefficient a1(x) is positive, whereas the
Oscilator strength

1.2 third-order nonlinear optical absorption coefficient a3(x, I) is neg-

1.0
0.8
0.6
0.4
1s-1p
0.2
0.0
0 5 10
Rdot (a* )
Fig. 3. The ground and excited state energies of the QD with and without the
impurity (line with and without solid circles respectively) as a function of dot
radius.
oscillator strength involves two parameters, One of them is the di-
pole matrix element and the other is difference between energy
states. The matrix element is very small although the energy differ-
ences are very high in small QDs.
The oscillator strengths for various transitions are shown in
Fig. 3. In the absence of an impurity the oscillator strength rapidly
increases with dot radius and then reach to a limit value for all
transitions. When there is an impurity, the rapid increase of the
oscillator strengths for small dot radii is similar to that of without
impurity. However, for the larger dot radii the oscillator strength
goes through a maximum and then it decreases to a value corre-
sponding to that of free hydrogen. The effect of the impurity on
the oscillator strengths is larger for transitions between lower
states and it decreases as the levels go up. For the 1s–1p transi-
tions, our results are good in agreement with the previous studies
[16,18].
ative. So the total optical absorption coefficient a (x,I) is signifi-
cantly reduced by the nonlinear contribution. Therefore, the
contributions of both the linear and third-order nonlinear absorp-
tion terms should be considered in calculation of absorption spec-
trum of the QDs especially for those operating under high incident
optical intensity I. Also we can see from Fig. 4 that the strengths of
both the linear and nonlinear terms are larger for transitions be-
1p-1d 1d-1f
tween higher levels.
The total optical absorption coefficients a(x,I) of the QD for 1s–
15 20 25 1p, 1p–1d and 1d–1f transitions are displayed as a function of the
incident photon energy  hx for six different values of the incident
optical intensity in Fig. 5. It can be seen from this figure that the
maximum of absorption coefficient corresponds to the threshold
photon energy, i.e. Efi   hx. This maximum value decreases with
increasing incident optical intensity I, and the absorption is
strongly bleached at sufficiently high-incident optical intensities.
Therefore, the nonlinear optical absorption coefficient a3(x, I)
should be taken into account when the incident optical intensity
I is comparatively strong, which can reduce total absorption coef-
ficient. When the incident optical intensity I exceeds a critical va-
lue Ic, the nonlinear term causes a collapse at the center of the total
absorption peak splitting it into two peaks. It is clearly seen that
this critical intensity Ic is smaller for transitions between higher
states while the intensity of the total absorption spectra increases
for the transitions between higher states.
For 1s–1p, 1p–1d and 1d–1f transitions we display the total
optical absorption spectra of the spherical QD as a function of
the photon energy  hx at three different dot radii in Fig. 6. The total
optical absorption coefficients for small dot radii are much stron-
ger than that for large dot radii since the absorption spectrum de-
pends on the QD volume. Also it is seen obviously from Fig. 6 that
existence of the impurity causes a shift on absorption spectra

15
Z=0 1p-1d 1d-1f
10 1s-1p

5
Absorption coefficient α (10 /m)

0
9

-5

-10
15
Z=1 1p-1d 1d-1f
10 1s-1p

-5 Lineer
Nonlineer
-10 Total

6. 5 7 .0 7. 5 8 .0 8. 5 9 .0 9. 5 10. 0 10. 5 11. 0

Photon energy (R y* )

Fig. 4. The linear (dashed), third-order nonlinear (dashed–dotted) and total optical (solid) absorption coefficients of the QD with and without impurity versus the incident
photon energy  hx for I = 10 MW/m2 and R = 1a*.
 A. Özmen et al. / Optics Communications 282 (2009) 3999–4004 4003

10
1d-1f
Z=0
8 1p-1d

6 1s-1p

Total absorption coefficient α (10 /m)

4
9

0
8 Z=1 1d-1f

1p-1d
2 1s-1p
I=20 MW/m
6 I=30 MW/m
2

2
I=38 MW/m
2
I=45 MW/m
4 2
I=55 MW/m
2
I=65 MW/m
2

6.5 7.0 7.5 8.0 8.5 9.0 9.5 10. 0 10.5 11.0

Photon energy (R*y)

hx for six different values of the incident optical

Fig. 5. The total optical absorption coefficients of the QD with and without impurity versus the incident photon energy 
intensity I and R = 1a*.

1d-1f
14 *
R=0.9 a Z=0
* 1p-1d
12 R=1 a
* 1d-1f
R=1.2 a 1s-1p
10 1p-1d
Total absorption coefficient α (10 /m)

8 1s-1p
9

1d-1f
6 1p-1d
1s-1p
4
2
0
14 1d-1f
Z=1
1p-1d
12 1d-1f
1s-1p
10 1p-1d

8 1s-1p
1d-1f
6 1p-1d
1s-1p
4
2
0
5 6 7 8 9 10 11 12 13
*
Photon eneregy(R y)

hx for three dot

Fig. 6. The total optical absorption coefficients of 1s–1p, 1p–1d and 1d–1f transitions in the QD with and without impurity versus the incident photon energy 
radii and I = 10 MW/m2.

towards higher energies (blue shift) for all transitions and dot radii. with the results for the spherical QD with parabolic confinement
This blue shift is more enhanced in the transitions between lower potential in Refs. [19,20,22,23,25].
states where the electron is more localized near the impurity. On
the other hand, the intensity of the total absorption spectra in- 5. Conclusion
creases for the transitions between higher levels. This is because
that the electronic dipolar transition matrix elements are very high We calculated the energies and wave functions of the spherical
for the transitions between higher levels. Optical absorption coef- QD with and without impurity for the ground and the excited
ficients obtained for the 1s–1p case are qualitatively consistent states. The binding energies of the electron to the impurity were
4004 A. Özmen et al. / Optics Communications 282 (2009) 3999–4004

also calculated. Moreover, we computed the oscillator strength Pfi, References

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