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2013 Semicond. Sci. Technol. 28 055002
(http://iopscience.iop.org/0268-1242/28/5/055002)
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The article was downloaded on 29/03/2013 at 05:23
IOP PUBLISHING
doi:10.1088/0268-1242/28/5/055002
1. Introduction
0268-1242/13/055002+07$33.00
A Bag et al
2. Experimental details
We used ITO-coated PET as flexible substrates for the
fabrication of GO-based MIM capacitors. The ITO-coated
PET film was purchased from Sigma-Aldrich. The surface
resistivity of the ITO is 60 /sq. and the thickness of
the ITO is 100 nm. Initially, the substrates were cleaned
sequentially with acetone and methanol in an ultrasonic
bath for about 5 min followed by DI water rinse. In this
work, ITO not only acts as the bottom electrode, but the
lower part also acts as a good adhesive layer with the
PET substrates. The GO layer was formed by the drop
casting method. The GO in aqueous solution (0.1 mg ml1)
was obtained from Nanocs Inc., USA (product: GO1-AQ-1,
graphene oxide, aqueous solution, 20 ml). However, before GO
layer formation, the ITO-coated PET substrate was exposed
to UV light for 1.5 h for better adhesion of GO. The
GO film thickness was measured by a surface profilometer
(Veeco Dektak 150) at five locations for three different
samples, and the average thickness of the film was found as
370 nm. Finally, as the top electrode, Pt was deposited by
dc sputtering in Ar ambient through a shadow mask (area
1.96 103 cm2). The CV measurements were performed
using an Agilent E4980A precision LCR meter. Before
CV measurements, open and short correction was carried
out to remove the parasitic series resistance and capacitance.
The constant current stressing (CCS) and constant voltage
stressing (CVS) were employed using an Agilent 4156C
semiconductor parameter analyser. Periodically, the stressing
and CV measurements were performed by switching the
measuring instruments automatically by an Agilent E5250A
low switching mainframe through a computer programming
controlled system.
Flexibility
RMS value of
roughness, Rq (nm)
Before
After
Before
After
Before
After
12.28
13.05
23.43
30.59
20.09
25.53
1
3
5
7
4
5
A Bag et al
(a)
(b)
(c)
(d )
(e)
(f)
Figure 2. Surface morphology study of the GO film, bottom electrode (ITO) and top electrode (Pt) during the flexibility study. Surface
condition of the GO, ITO and Pt before ((a), (c) and (e) respectively) and after 6000 times flexibility study ((b), (d) and ( f ) respectively).
A Bag et al
(1)
A Bag et al
figure 5). It may be due to the existence of the large charge traps
at the electrodeGO interface. Since different traps exhibit
different time constants, it is reasonable to expect that as the
frequency increases, fewer traps will be able to follow the
ac signal and hence a decrease in measured capacitance was
observed. Generally, the frequency dependence of quadratic
VCC implies a strong relationship with the relaxation time in
the GO layer. This frequency dispersion may also be due to the
electrode polarization effect. By electrode polarization, mobile
carriers form an accumulation layer at the electrodes, leading
to a voltage-dependent double layer capacitance, which can be
expressed as follows [28, 29]:
AD
C = Cm 1 +
,
(4)
1 + 2 2
2
8 q2
h 8 q
+
N
,
(5)
d3Ke
d3Kh
where q is the unit charge, d is the distance between the
molecules, is the atomic polarizability of the dielectric and
Ke/Kh and Ne/Nh are the potential energy profile of the trap
(spring constant) and the density of the trapped charges inside
the dielectric for the electron and the hole, respectively [31].
Thus, it may be concluded that the oxide-trapped charges
increase the local permittivity, leading to an increase in the
capacitance.
To further investigate the degradation mechanisms of
the GO-based MIM capacitors, the CVS was carried out
with different constant voltages. The effects of CVS on the
dielectric properties were evaluated by alternatively switching
CVS and CV measurements which allowed an investigation
into the stress-induced degradation exclusively for the GO
layer. Figure 7 shows that the capacitance increases with
stress time under different CVS measured at 1 MHz. The
change of capacitance occurs due to the charge trapping effect
between the GO film and the electrode. These traps affect
charge trapping of carriers in the dielectric materials, and
trapped carriers can generate new dipoles, which results in an
increase in capacitance density as a function of stress time,
and higher stress voltage can cause more charge trapping
at deep traps [32, 33]. Figure 7 shows the extrapolated
C/C0 for a 10 year lifetime as a function of the different
stress voltages. The good reliability characteristic with a small
C/C0 of less than 1.0% was obtained. The logarithmic
increase of C/C0 also signifies the voltage nonlinearity
in the capacitance characteristics as discussed above. This
nonlinearity may be due to the creation of oxygen vacancies
after stressing.
= GO + N e
A Bag et al
4. Conclusion
The objective of this work has been the evaluation and
feasibility study of fabricating graphene oxide-based MIM
capacitors for flexible electronic applications in which
reliability is the primary concern. In this study, a GO thin film
on plastic substrates was prepared successfully with the drop
casting method. The results of detailed physico-chemical and
electrical properties of GO thin films on flexible substrates
for possible flexible electronic applications are reported.
Acceptable capacitance density with low VCC- and a low
loss tangent was obtained. However, high frequency dispersion
in capacitance and VCC- has been observed. The relative
capacitance increases logarithmically as a result of both the
CCS and CVS. The origin of this increase may be related
to the oxygen vacancies and/or oxygen interstitials, which
may be formed after electrical stressing. Finally, the GO films
show reasonable mechanical flexibility in a repetitive bending
test owing to their high ductility and the low-temperature
process used. The process developed in this work may provide
a practical approach for the fabrication of flexible MIM
capacitors using GO.
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