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)

Web Site: www.ijaiem.org Email: editor@ijaiem.org, editorijaiem@gmail.com

Volume 2, Issue 5, May 2013 ISSN 2319 - 4847

Volume 2, Issue 5, May 2013 Page 418

ABSTRACT

Ab-initio Density function theory (DFT) method coupled with Large Unit Cell (LUC) method has been used to simulate

electronic structure of InxGa1-xAs nanocrystals alloy for three Indium concentrations x=0.25, 0.50, and 0.75. Gaussian 03

package has been used throughout this study to calculate some of the physical properties such as energy gap , lattice constant ,

valence and conduction band as well as density of state . Results show that the lattice constant increases with the increasing in

the Indium concentration in the alloy, while the energy gap deceases due to the size effect. The total energy, cohesive energy,

electron affinity and ionization as well as ionicity for these concentrations have been reported.

Keywords: In

X

Ga

1-X

As nanocrystals, Ab-initio (DFT) , (LUC)

1. INTRODUCTION

A nanomaterial is a term that includes all nanosized materials. Nanomaterials semiconducting materials have been a

subject of intense study for last several years due to their size dependent physical and chemical properties [1-4].InGaAs

belongs to the InGaAsP quaternary system that consists of indium arsenide (InAs), gallium arsenide (GaAs), and

gallium phosphate (GaP). These binary materials and their alloys are all III-V compound semiconductors. A

comprehensive of band parameters for the technologically important III-V zinc blende compound semiconductor is

given in ref. [5].

In general III-V semiconductors provide the materials basis for a number of well-established commercial technologies.

Energy gap and whether the bandgap is “direct” or ”Indirect” is the main factor that gives semiconductors the optical,

electrical, and magnetic properties. The energy bandgap of the quaternary system (InGaAsP) range from 0.33eV

(InAs) to 2.25eV (GaP), with InP (1.29eV) and GaAs (1.43 eV) falling between. A semiconductor will only detect light

with photon energy larger than the band gap, in other word, with the wavelength shorter than the cutoff wave length

associated with the band gap. This wavelength cutoff works out to 3.75 µm for InAs and 0.55 µm for GaP with InP at

0.96 µm and at 0.87 µm for GaAs. The progress made in physics and technology of semiconductors depends mainly on

two families of materials, the group IV elements and the III-V compounds. For all of the ternary alloys, such as

InGaAs, the dependence of the energy gap on alloy composition is assumed to fit the quadratic form [6]

2

1

] ) ( [ ) ( ) 1 ( ) ( bx b BC E AC Eg x C B A E

g X X g

+ ÷ + ÷ =

÷

The value of (b) is a measure of the deviation from the linear interpolation curve and is often referred to be as the

bowing parameter.

In

x

Ga

1-x

As alloy has been of great interest for short wave infrared (SWIR) detector applications [7]. The SWIR InGaAs

cameras are a good complement to thermal imaging cameras, SWIR cameras can be used to identify and recognize

objects in cooler environment than those cameras which detect only warm bodies (cars, people, etc...) [8]. Indium

gallium arsenide (InGaAs) is used in high-power and high-frequency electronics [9] because of its superior electron

velocity with respect to the more common semiconductors silicon and gallium arsenide. InAs single and multiple

quantum dot (QD) layers have been explored for their potential use in the implementation of GaAs-based optical

devices such as Lasers, semiconductor optical amplifiers (SOAs) and saturable absorber mirrors operating at

telecommunication wavelengths (1300-1550nm) which is the same InGaAs band gap, also makes it

the detector material of choice in optical fiber communication at those mentioned wavelengths [10-13].

2. THEORY

One of the most important goals of physics is to describe the physical properties of interacting many-particle systems.

This can be done by deriving the properties of many-particle systems from the quantum mechanical laws this requires

the solution of the Schrödinger equation in 3N spatial variables and N spin variables. Solutions of the Schrödinger

Electronic structure of In

x

Ga

1-x

As nanocrystals

alloy using Ab-initio Density functional theory

calculation coupled with LUC method

Mohammed T. Hussien

1

, Akram H. Taha

2

and Thekra Kasim

3

1&3

Department of Physics,

College of Science, University of Baghdad

2

Department of Physics,

Faculty of Science & Health, Koya University,

International Journal of Application or Innovation in Engineering& Management (IJAIEM)

Web Site: www.ijaiem.org Email: editor@ijaiem.org, editorijaiem@gmail.com

Volume 2, Issue 5, May 2013 ISSN 2319 - 4847

Volume 2, Issue 5, May 2013 Page 419

equation yield the electron state and their characteristic for a given arrangement of the atoms [14]. The non-relativistic

Hamiltonian for a system consisting n electrons and N nuclei is given by (all equations are expressed in atomic units)

¿¿ ¿ ¿ ¿ ¿

< >

+ + ÷ V ÷ V ÷ =

n

i

N

I

n

j i ij

N

J I IJ

J I

Ii

I

n

i

i

N

I

I

r r

Z Z

r

Z

H

1

2

1

2

1

2 2

(1)

Where the lower case indexes the electron and the upper case indexes the nuclei. r is a distance between the objects

specified by the subscripts.

After applying the Born-Oppenheimer approximation, the Hamiltonian is obtained and neglecting relativity is

¿¿ ¿ ¿

<

+ ÷ V ÷ =

n

i

N

I

n

j i ij Ii

I

n

i

i

el

r r

Z

H

1

2

1

2

(2)

Now the expectation value of Hamiltonian operator due to the Hartree-Fock representation is given by

¿ ¿

= =

÷ + = =

N

j i

ij ij

N

i

i HF HF HF

K J H H E

1 , 1

) (

2

1

ˆ

Where

i

H defines the contribution due to the kinetic energy and the electron-nucleus attraction i.e

x d x x V x H

i eff i i

) ( ) (

2

1

) (

2 *

} (

¸

(

¸

÷ V ÷ ÷

the coulomb integrals

ij

J is given by

2 1 2 2

*

12

1

*

1

) ( ) (

1

) ( ) ( x d x d x x

r

x x J

j j i i ij

}}

=

And the exchange integrals

ij

K is

2 1 2

*

2

12

1 1

*

) ( ) (

1

) ( ) ( x d x d x x

r

x x K

j i j i ij

}}

=

All these integrals are real, and 0 > >

ij ij

K J .

The unrestricted Hartree-Fock is based upon the use of a single determinant total wavefunction in which orbitals of the

same n, L, and m

L

values but different m

s

. values are regarded as being independent [15]. This method is the most

common molecular orbitals method for open shell molecules where the number of electrons of each spin is not equal. It

is an extremely convenient method because it is a very natural extension of the conventional Hartree-Fock method, and

the many-electron wave function is written in the form of a single determinant so that calculations are relatively easy.

However, because the unrestricted Hartree-Fock method allows the α and β spins to have different wave functions the

total wave function obtained is not an eigenfunction of S

2

and hence the validity of the method must be questioned. It

has been suggested that [16-18] this objection may be overcome by determining the one-electron functions by the

unrestricted Hartree-Fock method and then eliminating by means of the appropriate projection operators those parts of

the function corresponding to the unwanted values of S2.

Density functional theory predicts a great variety of molecular properties: molecular structure, atomization energies,

vibrational frequencies, electrical and magnetic properties as well as ionization energies….etc. The central quantity in

DFT is the electron density ρ(r), it is defined as the integral over the spin coordinates of all electrons and over all but

one of the spatial variables (x=r,s)

N N

x d x d ds x x x N r

...... ) ....., , , ( ...... ) (

2 1

2

2 1

} }

=

(3)

Kohn and Sham introduced the following separation of the functional F[ρ]

] [ ] [ ] [ ] [

xc s

E J T F + + = (4)

Where T

s

do not equal to the true kinetic energy of the system, and E

xc

is the exchange-correlation energy and can be

defined through equation (4) as

{ } { } ] [ ] [ ] [ ] [ ] [ J E T T E

ee s xc

÷ + + = (5)

. Then the energy of the interacting system will be

International Journal of Application or Innovation in Engineering& Management (IJAIEM)

Web Site: www.ijaiem.org Email: editor@ijaiem.org, editorijaiem@gmail.com

Volume 2, Issue 5, May 2013 ISSN 2319 - 4847

Volume 2, Issue 5, May 2013 Page 420

¿

}

¿

¿¿

}}

¿

} }}

÷

+ + V ÷ =

+ + + =

+ + + =

N

i

N

A

i

A

A

xc

i i i

N

i

i

Ne xc s

Ne xc s

r d r

r

Z

E

r d r d r

r

r

r d r V E r d r d

r

r r

T

E E J T E

1

2

1

2 1

2

2

12

2

1

2

2 1

12

2 1

) ( ] [

) (

1

) (

2

1

2

1

) ( ] [

) ( ) (

2

1

] [

] [ ] [ ] [ ] [ ] [

(6)

The generalized gradient approximation (GGA) coupled with large unit cell method is used to evaluate the electronic

structure of In

x

Ga

1-x

As.

3.RESULTS AND DISCUSSION

The stoichiometry of In

x

Ga

1-x

As using geometrical optimization is shown in figure (1,2) for 16 and 64 core atoms. It is

found that all our samples with all concentrations x(=0.25, 0.50, and 0.75) have the prralelpiped shape for 16 and 54

core atoms, while for 8 and 64 core atoms the shape was cubic (primitive cell).

The lattice constant optimization of 16 and 64 core atoms is illustrated in fig. (3, 4) for one concentration only

In

0.5

Ga

0.5

As noting that we found lattice optimization for them but we will just review the optimization for only

In

0.5

Ga

0.5

As. The results for the value of lattice constant for the different concentration is in good agreement with Ref.

[19].

The total energy versus number of core atoms for the concentrations x=0.25, 0.50, and 0.75 is shown in figures (5). The

linearity is the main characteristic for all concentrations. The energy decrease as the number of core atom increase. For

each concentration the total energy decreases with the increasing of the number of core atoms [20].

Density of states for In

x

Ga

1-x

As core atoms 16 and 64 and for the concentrations x=0.50 are shown in figures (6,7).

The density of state increases with the increasing of the number of core atoms which is due to the increasing of the

number of orbital hence the degenerates of energy state. The dense of line become more with increasing the number of

atoms.

The density of states as a function of number of core atoms is shown in figure (8) for the three concentrations of

In

25

Ga

75

As, In

50

Ga

50

As and In

75

Ga

25

As respectively. The increase in the density of states is obvious as the number of

core atom increase for each concentration. On the other hand as the concentration of indium in the alloy increases the

density of states increases also. The variation of bands width (conduction & valence) with the number of core atoms

and the concentration is shown in fig.(9,10).

Finally the dependency between the energy gap and the concentration is illustrated in fig. (11). The effect of changing

of the concentration of Indium in the InxGa1-xAs alloy on the energy gap is shown in fig. (3.52). Three concentration

has been taken x=0.25, 0.50, and 0.75 the energy gap is decreasing with increasing In concentration in the alloy due to

the occurrence of exciton in the band gap which give rise to a new energy level to be there in the “forbidden region”.

When the size of the nanoparticle approaches that of an exciton, size quantization occurs. Each band has a width that

reflects the interaction between atoms, with a bandgap between the conduction and the valence bands that reflects the

original separation of the bonding and antibonding states. When the size of the nanoparticle approaches that of an

exciton, size quantization occurs.

Conclusions:

Using Ab-initio density functional theory (DFT) coupled with large unit cell (LUC) approximation to estimate the

electronic properties of In

X

Ga

1-X

As alloy give the main conclusions summarized as follow:

1. The total energy and cohesive energy depends on the number of core atoms , it decreases with increasing the number

of core atom. Also the total energy decrease with increasing the indium concentration in InXGa1-XAs alloy.

2. The energy gap varies with the indium concentration in the InXGa1-XAs alloy as well as the number of core atoms.

3. The valence and conduction bands decreases with increasing the number of core atoms.

4. The results show a strong shape that 8 and 64 core atoms have a cubic structure (Bravais cells) while (16 and54) core

atoms have a parallelepiped structure (primitive cell).

5. The density of states become more intense when the number of core atoms increase also the degeneracy increase.

Figure (1): 16 In

0.5

Ga

0.5

As core atoms Figure (2): 64 In

0.5

Ga

0.5

As core atoms

International Journal of Application or Innovation in Engineering& Management (IJAIEM)

Web Site: www.ijaiem.org Email: editor@ijaiem.org, editorijaiem@gmail.com

Volume 2, Issue 5, May 2013 ISSN 2319 - 4847

Volume 2, Issue 5, May 2013 Page 421

Figure (3): Total energy Vs lattice constant for 16 atom of In

50

Ga

50

As core nanocrystal

Figure (4): Total energy Vs lattice constant for 64 atom of In

50

Ga

50

As core nanocrystal

Figure (5): The total energy as a function of the number of core atoms for different concentrations

x=0.25, 0.50, and 0.75

Figure (6): Density of states of 16 core atoms for In

50

Ga

50

As. The bold lines represent the conduction

band while the ordinary lines represent the valence band, E

g

=1.353 eV

International Journal of Application or Innovation in Engineering& Management (IJAIEM)

Web Site: www.ijaiem.org Email: editor@ijaiem.org, editorijaiem@gmail.com

Volume 2, Issue 5, May 2013 ISSN 2319 - 4847

Volume 2, Issue 5, May 2013 Page 422

Figure (7): Density of states of 64 core atoms for In

50

Ga

50

As. The bold lines represent the conduction

band while the ordinary lines represent the valence band, E

g

=1.45 eV

Figure (8): The density of states vs the number of core atoms for In

25

Ga

75

As,

In

50

Ga

50

As and In

75

Ga

25

As

Figure (9): The relationship between the band width (conduction and valence) with the number of core atoms of

In

50

Ga

50

As nanocrystals

Figure (10): variation of band width (conduction & valence) with the concentration x=0.0, 0.25, 0.50, 0.75, and 1.0 of

In

X

Ga

1-X

As

International Journal of Application or Innovation in Engineering& Management (IJAIEM)

Web Site: www.ijaiem.org Email: editor@ijaiem.org, editorijaiem@gmail.com

Volume 2, Issue 5, May 2013 ISSN 2319 - 4847

Volume 2, Issue 5, May 2013 Page 423

Figure(11): The energy gap versus the number of core atoms for different concentrations of In, 25, 50, and 75%.

References

[1.] J. Woltersdorf, A. S. Nepijko and E Pipple, “The Synthesis of Nano Hybrid CNTs/TiO2 Materials” Surf. Sci. 106,

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[2.] S. B. Qadri , J. Yang, B. R. Ratna, E. F. Skelton, " Pressure induced structural transitions in nanometer size

particles of PbS" Appl. Phys. Lett., 69, pp 2205 (1996)

[3.] Norman Henon, Y ing Wang, and Hellmut Eckert, “Synthesis and Characterization of Surface-Capped, Size-

Quantized CdS Clusters. Chemical Control of Cluster Size” J. Am. Chem. Soc. 112, pp1322-1326 (1990)

[4.] R. Rosseti, S. Nakahara, and L. E. Brus, ” Quantum size effects in the redox potentials, resonance Raman spectra,

and electronic spectra of CdS crystallites in aqueous solution ” J. Chem. Phys. 79, 1086 (1983)

[5.] I. Vurgaftman, J. R. Meyer, and L. R. Ram-Mohan, “Band parameters for III– V compound semiconductors and

their alloys”, J. App. Phys. 89, 5815 (2001)

[6.] J. A. Van Vechten and T. K. Bergstreeer, “Electronic Structures of Semiconductor Alloys”, Phys. Rev. B1,

3351(1970)

[7.] Ruud W.M Hoogeveen, Ronald J van der A, Albert P.H Goede, “ Extended wavelength InGaAs infrared (1.0-2.4

μm) detector arrays on SCIAMACHY for space-based spectrometry of the Earth atmosphere”, Infrarad Physics &

technology, Volume 42, Issue 1, February, pp1–16(2001)

[8.] R. Guntupali and R. Allen, “Evaluation of InGaAs camera for scientific near infrared imaging and applications”

Proc. Of Spie, Vol. 6294

[9.] Tom Pearsall, T. P., “ Quantum Semiconductor Devices and Technologies”, Springer.

[10.] D. L. Huffaker, G. Park, Z. Zou, O. B. Shchekin, and D. G. Doppe, “Structural and optical properties of

GaInNAs/GaAs quantum structures ”, Appl. Phys. Lett. 73, 2564 (1998)

[11.] N. N. Ledenstov, A. R. Kovish, A. E. Zhokov, N. A. Maleev, S. S. Mikhrin, A. P. Vasil’ev, E. S. Semenova, M.

V. Maximov, Yu. M. Shernyakov, N. V. Kryzhanoviskaya, N. M. Ustinov, and D. Bimberg, “High performance

quantum dot lasers on GaAs substrates operating in 1.5 μm range”, Electron Lett. 39, 1126 (2003)

[12.] S. Dommers, V. V. Temnov, U. Woggon, J. Gomis, J. Martinez-Pastor, M. Laemmlin, and D. Bimberg,

“Complete ground state gain recovery after ultrashort double pulses in quantum dot based semiconductor optical

amplifier” Appl. Phys. Lett. 90, 33508 (2007)

[13.] M. P. Lumb, P. N. Stavrinous, E. M. Clark, R. Murray, C. G. Leburn, C. Jappy, N. K. Metzger, C. T. A. Brown,

and W. Sibbet, “Dispersionless saturable absorber mirrors with large modulation depths and low saturation

fluences” Appl. Phys. B 97,53(2009)

[14.] David J. Griffiths, "Introduction to quantum mechanics" , Prentice Hall.

[15.] Pratt G. W., “Unrestricted Hartree-Fock Method”, Phys. Rev. Vol. 102, issue 5, pp 1303-1307(1956)

[16.] R. K.Nesbet, “Magnetic Hyperfine Structure of the Ground State of Lithium”,Phys. Rev., 118, pp681-683

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[17.] A. J. Freeman, and R. E. Watson, “Contribution of the Fermi Contact Term to the Magnetic Field at the Nucleus

in Ferromagnets”, Phys. Rev. Letters, 5, 498 (1960)

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Factors for Spin Polarized Ni++”, Phys. Rev., 120, 1125, 1134 (1960)

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[21.] M. Born, and K. Huang, “Dynamical theory of crystal lattice”, (Oxford, London) 1954

International Journal of Application or Innovation in Engineering& Management (IJAIEM)

Web Site: www.ijaiem.org Email: editor@ijaiem.org, editorijaiem@gmail.com

Volume 2, Issue 5, May 2013 ISSN 2319 - 4847

Volume 2, Issue 5, May 2013 Page 424

AUTHOR

Dr.Mohammed T.Hussein completed his Ph.D. at the physics department in laser spectroscopy from

Complutense University – Madrid-Spain in 1995. His research interests lie in the field of organic

semiconductor and molecular spectroscopy. He is currently a member of the Nanotechnology &

Optoelectronics Research Group at the Physics department of Baghdad University.

Akram H.Tahacompleted his M.Sc. in solid state physics/ Yarmouk university (HKJ), His work Assistant

lecture at university of science and technology then lecturer at Sau's university (Republik of Ymen) and

lecturer at Faculty of science and health.-physics dep-koya university.

Thekra Kasim her M.Sc. Solid state Physics/ University of Baghdad , her work Assist. Lecturer at physics

department /college of science / University of Baghdad then lecturer at physics department./University of

Baghdad, now Ph.D. Postgraduate student at physics department, college of science /University of Baghdad

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