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AC conductivity and dielectric properties of Sb 2S 3 films

Article  in  Vacuum · December 2000

DOI: 10.1016/S0042-207X(00)00403-6

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 Vac1=1935=Susan=Venkatachala=BG

Vacuum 59 (2000) 932}939

AC conductivity and dielectric properties of Sb S "lms

 
A.M. Farid*, A.E. Bekheet
Physics Department, Faculty of Education, Ain Shams University, Roxy, Cairo, Egypt

Abstract

Stoichometric Sb S "lms were prepared by thermal evaporation technique. X-ray di!raction patterns
 
showed that the as-deposited Sb S "lms is in the amorphous state. The ac conductivity and dielectric
 
properties of the amorphous Sb S "lms has been investigated in the frequency range of 100}100 kHz. The
 
ac conductivity is found to be proportional to u1 where s(1. The temperature dependence of ac conductiv-
ity and the parameter s can be discussed with the aim of the correlated barrier-hopping (CBH) model. The
maximum barrier height = calculated from dielectric measurements according to Guintini equation agrees
+
with the theory of hopping of charge carriers over potential barrier as suggested by Elliot in the case of
chalcogenide glasses.  2000 Elsevier Science Ltd. All rights reserved.

1. Introduction

Sb S exists in nature in a crystalline form known as stibnite. Its structure reported by Arun et
 
al. [1] belongs to the orthorhombic system. Sb S in thin "lm form was prepared by several
 
methods, namely spray pyrolysis [2,3], chemical deposition [4,5], electrodeposition [5], dip try
method [7] and thermal evaporation [8,9]. It was found that amorphous "lms could be obtained
by thermal evaporation of the bulk material [8]. The electrical [2,3,7,10,11], thermoelectrical [7]
and optical [3,6,10,11] properties were studied for the Sb S "lms. No data concerning the ac
 
conductivity and/or dielectric properties of the obtained material are available in literature.
Measurement of ac conductivity of amorphous chalcogenide semiconductors has been extensive-
ly used to understand the conduction process in these materials. Various models, quan-
tum}mechanical tunneling model (QMT) [12,13], small polaron tunneling model [13,14], large
polaron tunneling model [14], atomic hopping model [14,15] and correlated barrier hopping
(CBH) model [16}18] have been proposed to explain the ac conduction mechanism for di!erent

* Corresponding author. Fax: #20-2-4552138.

E-mail address: ashraf}bekheet@hotmail.com (A.M. Farid).

0042-207X/00/$ - see front matter  2000 Elsevier Science Ltd. All rights reserved.
PII: S 0 0 4 2 - 2 0 7 X ( 0 0 ) 0 0 4 0 3 - 6
 Vac1=1935=SK=VVC

A.M. Farid, A.E. Bekheet / Vacuum 59 (2000) 932}939 933

materials. Measurements of dielectric properties of materials are used to understand the types of
polarization that exist in these materials.
In this paper the temperature and frequency dependence of ac conductivity and dielectric
properties are measured for Sb S "lms of di!erent thicknesses . Our results are discussed with the
 
basis of a di!erent theory of ac conductivity of amorphous semiconductors.

2. Experimental techniques

Thin "lms of di!erent thicknesses of Sb S were obtained by conventional thermal evaporation

 
technique using a high vacuum coating unit (Edwards-type E306 A). The substrate was "xed onto
a rotatable holder (up to 240 r.p.m.) to obtain homogeneous deposited "lms at a distance of 25 cm
above the evaporator. The "lm thickness was measured by Tolansky's interferometric method. The
"lm thickness ranged from 323 to 506 nm. X-ray di!raction analysis revealed the amorphous
nature of the investigated "lms.
For ac measurements, "lms were sandwiched between two Al electrodes as lower and upper
electrodes. A programmable automatic RLC bridge (PM 6304 Philips) was used to measure the
impedance Z, the capacitance C and the loss tangent (tan d) directly, since all samples could be
represented by a resistance R connected in parallel with a capacitance C. The total conductivity was
calculated from the equation: p (u)"d/ZA, where d is the thickness of the "lm and A is the

cross-sectional area. The dielectric constant was calculated from the equation: e "dC/Ae , where
 
C is the capacitance of the "lm and e is the permittivity of free space. The dielectric loss e was
 
calculated from the equation: e "e tan d, where (d"90!
).
 

3. Results and discussion

3.1. Frequency and temperature dependence of ac conductivity

A common feature of all the amorphous semiconductors is that the ac conductivity p (u)

increases with frequency according to the equation

p (u)"p (u)!p "AuQ, (1)

  
where u is the angular frequency, s is the frequency exponent and A is a temperature-independent
constant. Fig. 1 shows the frequency dependence of ac conductivity p (u) for Sb S "lm of
  
thickness 323 nm at di!erent temperatures as a representative example. It is clear from the "gure
that p (u) increases linearly with frequency. The same behavior of the frequency dependence of

p (u) was obtained for all investigated "lms. Values of the frequency exponent s were obtained

from the slopes of these lines of the "gure. The temperature dependence of s for the investigated
"lms is shown in Fig. 2. It is clear from this "gure that, s decreases with increasing temperature. The
discrepancy in the values of s for samples at each temperature indicated by vertical lines on the
obtained results lie within the experimental error of $6% on average. Accordingly, s is indepen-
dent of the "lm thickness in the investigated range.
 Vac=1935=SK=VVC

934 A.M. Farid, A.E. Bekheet / Vacuum 59 (2000) 932}939

Fig. 1. Frequency dependence of p (u) for Sb S "lm of thickness 323 nm at di!erent temperatures.
  

Fig. 2. The temperature dependence of the parameter s for Sb S "lms.

 

According to the quantum}mechanical tunneling (QMT) model [19], the exponent s is almost
equal to 0.8 and increases slightly with increasing temperature or independent of temperature.
Therefore, QMT model is considered not applicable to the obtained samples.
According to the overlapping-large polaron tunneling (OLPT) model [20], the exponent s is
both temperature and frequency dependent. s decreases with increasing temperature from unity at
room temperature to a minimum value at a certain temperature, then it increases with increasing
temperature. Therefore, OLPT model is considered not applicable to the obtained samples.
According to the correlated barrier-hopping (CBH) model, values of the frequency exponent s is
ranged from 0.7 to 1 at room temperature and is found to decrease with increasing temperature.
 Vac1=1935=SK=VVC

A.M. Farid, A.E. Bekheet / Vacuum 59 (2000) 932}939 935

Fig. 3. Temperature dependence of p (u) for Sb S "lm of thickness 506 nm at di!erent frequencies.
  

This is in good agreement with the obtained results, so the frequency dependence of p (u) can be

explained in terms of CBH model. The expression for s derived on the basis of this model is given by
Elliott [16,17] as

S"1!(6k¹/B), (2)

where k is Boltzmann constant, T is temperature in kelvin and B is the optical band gap of the
material. Using the previously [6] obtained value of the energy gap of Sb S "lms (1.74 eV), the
 
value of s at room temperature is calculated using Eq. (2). The calculated value (0.911) is in good
agreement with the experimental value (0.925) within 1.5%.
According to the Austin}Mott formula [21], ac conductivity p (u) can be explained in terms of

hopping of electrons between pairs of localized states at the Fermi level. p (u) is related to the

density of states N (E ) at the Fermi level by the equation

p (u)"(p/3)[N(E )]k¹ea\[ln(l /u)], (3)
  
where a is the exponential decay parameter of localized states wave functions, and l is the

phonon frequency. By assuming l "10 s\ and a\"10 As , the density of state is calculated. It

is found that it has values of the order of 10}10 eV\ cm\ and increases with frequency and
temperature.
The temperature dependence of p (u) for Sb S "lm of thickness 506 nm is shown in Fig. 3 as
  
a representative example. It is clear from the "gure that p (u) increases linearly with the reciprocal

of absolute temperature. This suggested that the ac conductivity is a thermally activated process
from di!erent localized states in the gap or in its tails. The activation energy of conduction is
calculated at di!erent frequencies using the well-known equation p"p exp(*E /k¹). The fre-
 N
quency dependence of activation energy for Sb S "lms of di!erent thicknesses is shown in Fig. 4.
 
It is clear that *E (u) decreases with increasing frequency. Such a decrease can be attributed to the
N
 Vac=1935=SK=VVC

936 A.M. Farid, A.E. Bekheet / Vacuum 59 (2000) 932}939

Fig. 4. The frequency dependence of ac activation energy for Sb S "lms.

 

Fig. 5. Frequency dependence of e for Sb S "lm of thickness 506 nm at di!erent temperatures.

  

contribution of the frequency applied to the conduction mechanism, which con"rms the hopping
conduction to the dominant mechanism. The discrepancy in the values of *E (u) for samples at
N
each frequency indicated by vertical lines on the obtained results lie within the experimental error
of $8% on average. Accordingly, *E (u) is independent on "lm thickness in the investigated
N
range.

3.2. Frequency and temperature dependence of dielectric constant

Fig. 5 shows the frequency dependence of dielectric constant e at di!erent temperatures for

Sb S "lm of thickness 506 nm as a representative example. It is clear from the "gure that
 
e decreases with increasing frequency and increases with increasing temperature. The decrease of

 Vac1=1935=SK=VVC

A.M. Farid, A.E. Bekheet / Vacuum 59 (2000) 932}939 937

e with frequency can be attributed to the fact that at low frequencies e for polar material is due to
 
the contribution of multicomponents of polarizibility, deformational (electronic, ionic) and relax-
ation (orientaional an interfacial). When the frequency is increased, the orientational polarization
decreases since it takes more time than electronic and ionic polarization. This decreases the value of
dielectric constant with frequency reaching a constant value at high frequency due to interfacial
polarization.
The increase of e with temperature can be attributed to the fact that the orientational polariza-

tion is connected with the thermal motion of molecules, so dipoles cannot orient themselves at low
temperatures. When the temperature is increased the orientation of dipoles is facilitated and this
increases the value of orientational polarization and this increases e with increasing temperature.


3.3. Frequency and temperature dependence of dielectric loss

The frequency dependence of dielectric loss e was studied at di!erent temperatures for Sb S
  
"lms of di!erent thicknesses. e is found to decrease with increasing frequency and increase with

increasing temperature. The obtained data of the frequency dependence of e for a "lm of thickness

223 nm is represented as ln e vs. ln u (Fig. 6) according to the equation e "Au , where A is
 

Fig. 6. Frequency dependence of e for Sb S "lm of thickness 323 nm at di!erent temperatures.

  
 Vac=1935=SK=VVC

938 A.M. Farid, A.E. Bekheet / Vacuum 59 (2000) 932}939

Fig. 7. Temperature dependence of the parameter m for Sb S "lms.

 

a constant. The power m, calculated from Fig. 6, is represented in Fig. 7 as m vs. T. It is clear from
the "gure that m decreases linearly with temperature according to the Guintini [22] equation:
m"!4k¹/= , where = is the maximum barrier height. Value of = obtained from the slope

of the line of the "gure (0.182 eV) which is in good agreement with the theory of hopping of charge
carriers over a potential barrier as suggested by Elliott [16,17] in the case of chalcogenide glasses.
The variation of e with temperature can be explained by Stevels [23] who divided the relaxation

phenomena into three parts, conduction losses, dipole losses and vibrational losses. At low
temperatures conduction losses have minimum value since it is proportional to (p/u). As the
temperature increases p increases and so the conduction losses increase. This increases the value of
e with increasing temperature.


4. Conclusion

Amorphous Sb S "lms were prepared by thermal evaporation technique. The ac conductivity,

 
dielectric constant and dielectric loss, is found to be frequency and temperature dependent. The
frequency and temperature dependence of ac conductivity suggested the applicability of correlated
barrier model (CBH) to the investigated material. Value of the maximum barrier height is estimated
from the data of dielectric loss which is in good agreement with the theory of hopping of charge
carriers over a potential barrier as suggested by Elliott in case of chalcogenide glasses.

References

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