Thin Solid Films 517 (2009) 5318–5321

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Thin Solid Films

j o u r n a l h o m e p a g e : w w w. e l s e v i e r. c o m / l o c a t e / t s f

Preparation and characterization of pentacene-based organic thin-film transistors

with PVA passivation layers
G.M. Wu ⁎, Y.H. Lu, J.W. Teng, J.C. Wang, T.E. Nee
Institute of Electro-Optical Engineering, Department of Electronic Engineering, Chang Gung University, Kweisan, Taoyuan 333, Taiwan, ROC

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

Available online 29 March 2009 High-mobility organic thin-film transistors (OTFT) were fabricated with pentacene active layers and
passivated by polyvinyl acetate (PVA) in this study. The organic pentacene film showed a single phase
Keywords: structure with the interplanar spacing of 1.54 nm corresponding to the (001) diffraction. The initial field
Pentacene effect mobility of OTFT was 4.4 × 10− 2 cm2/Vs without the passivation. After the PVA passivation, the device
Organic thin-film transistor exhibited an improved field-effect mobility of 1.0 × 10− 1 cm2/Vs. It was decreased to 8.0 × 10− 2 cm2/Vs after
Passivation
35 days. The on/off current ratio has been at the order of 106. The device durability was also examined by 80°
bending cycle tests in tension. The transistors exhibited lower on/off ratio and higher turn-on voltage after
2500 bending cycles. The lifetime of the passivated OTFT was improved to more than 2 months in air. It has
been suggested that the PVA passivation layer could effectively protect the pentacene-based OTFT from
moisture and oxygen permeation.
© 2009 Elsevier B.V. All rights reserved.

1. Introduction the passivation material. We present high-performance pentacene

Flat panel displays (FPD) have been highly preferred due to their
characteristics of light weight, slim structure, and versatility in use.
The main applications of organic thin-film transistors (OTFT) would
be in the driving circuits for organic flat displays and switching
devices for organic light-emitting devices. The advantages include
lower cost, lower manufacturing temperature, more suitable for flex-
ible substrates, and being biodegradable [1–3]. However, the carrier
mobility values of OTFTs are relatively low to be useful for practical
high-speed electronics or integrated circuits. It is therefore desired to
improve the carrier mobility for OTFTs by enhancing the structural
order of the active layer. On the other hand, the organic thin films can
be easily degraded when exposed to water vapor, oxygen and various
chemical solvents. For example, atmospheric moisture alone can de-
grade the performance of OTFT with no encapsulation in ambient air.
The water molecules diffuse into the grain boundaries and crystal
lattice, where they capture charges generated in the channel because
of the polar nature [4–8].
In this study, pentacene material has been used as the active layers
of high-mobility organic thin-film transistors on plastic substrates.
The surface morphology and structures of the pentacene thin films
were examined by atomic force microscopy (AFM) and X-ray
diffraction (XRD). In addition, a protective passivation layer is applied
to keep the device from exposure to open environment during the
process of the upper layers. Polyvinyl acetate (PVA) has been used as
⁎ Corresponding author. Tel.: +886 3 2118800; fax: +886 3 2118668.
E-mail address: wu@mail.cgu.edu.tw (G.M. Wu).
OTFT on plastic substrates, both with and without the organic
passivation layer of PVA.
2. Experimental
The organic thin-film transistors were fabricated by thermal
evaporation, sputtering deposition, and lift-off process. The devices
were designed to have bottom gates and top contacts. Polyether
sulfone (PES) substrates of 100 by 100 mm were used for gate elec-
trode deposition. The substrates were sequentially cleaned in de-
ionized water, acetone, and isopropyl alcohol (IPA) for three minutes
in each step by an ultrasonic unit, and then dried by nitrogen gas. After
that, aluminum (Al) thin film of 100 nm in thickness was deposited for
gate electrodes by a thermal evaporation system. The gate oxide was
prepared by sputtering with 200-nm thick SiO2 layer. The surface of
the SiO2 insulator was treated by O2 plasma, and the organic pen-
tacene (Aldrich, purified at 220–240 °C) active layer was deposited by
vacuum evaporation at a rate of 0.05 nm/s. The final pentacene film
thickness was about 100 nm and the pressure was set at 10− 5 Torr
during evaporation. The source and drain electrodes were deposited
with 80-nm thick silver (Ag, 0.01 nm/s) by thermal evaporation, and
the channel width/length of 500/30 μm was patterned by the lift-off
process. In addition, some OTFT devices were encapsulated with a
protective polyvinyl acetate (PVA) cover film. The electrical char-
acteristics of the OTFT devices were evaluated by the drain current
versus gate voltage (Id–Vg) and drain current versus drain voltage
(Id–Vd) curves from HP4156B semiconductor parameter analysis [9–14].
The device durability was also examined by 80° bending cycle tests in

0040-6090/$ – see front matter © 2009 Elsevier B.V. All rights reserved.
doi:10.1016/j.tsf.2009.03.187
 G.M. Wu et al. / Thin Solid Films 517 (2009) 5318–5321
tension. The OTFTs were stressed for 10 s at a bending radius of 3 cm. The
flexing was performed at 2°/s and then repeated for up to 2500 times
before the measurements.
3. Results and discussion
Pentacene has very strong tendency to form crystalline structures.
The electrical characteristics of pentacene thin film layer are also
influenced by the structures of the crystalline lattice. The resistance of
pentacene, with a crystalline structure, is similar to that of
semiconductors. For amorphous pentacene, the electrical behavior is
more like an insulator. It is thus interesting to determine whether the
deposited pentacene thin film layer formed a crystalline structure. The
surface morphology of the 100-nm thick pentacene thin film by AFM
is shown in Fig. 1. The root-mean-square (RMS) for surface roughness
of the pentacene film has been estimated to be 8.2 nm when measured
over an area of 10 by 10 μm. No specific island structure and dendrite-
like crystal formation was observed. It would have formed smooth
active layer surface.
The characterization of the crystal structure for the as-deposited
pentacene thin films has been conducted using X-ray diffraction,
operated with Cu-Kα radiation in a symmetric reflection, coupled
θ–2θ mode. Fig. 2 displays the XRD spectrum of the pentacene thin
films with an average thickness of 100 nm, deposited on SiO2 in-
sulators at room temperature. The result indicates that pentacene
could form very ordered lattice, in single crystalline with sharp first-
order peaks [15]. The single lattice spacing parameter is 1.54 nm in
(001) diffraction. This is attributed to the thin-film order phase in the
device. The thermally evaporated pentacene thin film exhibited
single phase structure with 0.5–1.5 μm in grain size.
The electrical characteristics of OTFT devices without the passiva-
tion are shown in Fig. 3 at room temperature. The initial carrier
mobility (μ) was determined to be 4.4 × 10− 2 cm2/Vs. The mobility
value was decreased rapidly and reached 2.4 × 10− 2 cm2/Vs after
35 days in air. The current on/off ratio has been also seriously de-
Fig. 1. Surface morphology of the pentacene film (10 × 10 μm2) grown on SiO2 insulator
by AFM analysis.
5319
Fig. 2. XRD spectra of the pentacene film. It has been indicated of ordered lattice
structure with sharp diffraction peaks.
graded. On the other hand, Fig. 4 shows the electrical characteristics
for the OTFT devices with the PVA passivation layer. The initial carrier
mobility was improved to 1.0 × 10− 1 cm2/Vs, and it was decreased
to 8.0 × 10− 2 cm2/Vs after 35 days. The threshold voltage has been
−20 V, and the on/off current ratio was at the order of 106. The
excellent electrical characteristics are well preserved.
It was suggested that the PVA passivation layer effectively
blocked moisture, oxygen, and UV light, and that the stability of
the OTFT devices could be maintained for a long period of time. In
addition, the saturation currents and mobilities decreased with
ambient oxygen concentration. The O2 and H2O that diffused into
the charge accumulation region were mainly responsible for the
change in performance [16]. Fig. 5 summarizes the variations in
field-effect mobility and on/off ratio of organic pentacene OTFT
devices. After 35 days, the mobility for OTFT without passivation
became 2.4 × 10− 2 cm2/Vs, and the current on/off ratio was below
105. On the other hand, the OTFT with passivation exhibited a higher
mobility of 8.0 × 10− 2 cm2/Vs after 35 days, and the current on/off
ratio was above 2.0 × 106. The passivated sample even remained a
Fig. 3. Electrical characteristics of pentacene-based OTFT devices without passivation:
(a) drain current versus gate voltage curves (Vd = − 40 V) and (b) drain current versus
drain voltage curves at room temperature.
5320 G.M. Wu et al. / Thin Solid Films 517 (2009) 5318–5321
Fig. 4. Electrical characteristics of pentacene-based OTFT devices with the PVA
passivation layers: (a) drain current versus gate voltage curves and (b) drain current
versus drain voltage curves. The corresponding changes after 35 days are also shown.
good mobility value of about 5.5 × 10− 2 cm2/Vs for up to 63 days in
air. The current on/off ratio was then good at 1.0 × 106. The lifetime
of the passivated OTFT is thus as high as more than 2 months in the
Fig. 5. The variations in field-effect mobility and on/off ratio of the pentacene OTFT
devices.
Fig. 6. Flexibility of the OTFT devices with the PVA passivation layers using 80° bending
cycle tests in tension. The gate voltage ranged from 30 to −50 V.
ambient air environment when it is defined as the time required to
decrease the device mobility by one half. The field-effect mobility of
the OTFT devices was decreased exponentially without the passiva-
tion layer.
The flexibility of the pentacene OTFT devices after 80°bending
cycle tests in tension is described in Fig. 6. The gate voltage ranged
from 30 to −50 V. In the flexible tests, the device with 2500 bending
cycles exhibited a lower current on/off ratio (2.4 × 105) and higher
turn-on voltage (− 23.7 V). Some micro-cracks might have been
developed on the surface during the flexible tests, resulting in a higher
permeation rate for water vapor and oxygen. No catastrophic failure
has been encountered. Under constant bending moment condition,
because of the relaxation in the PES substrate, the surface strain was
increased with tension. It has the maximum value over a long period
of time and may cause fracture.
The encapsulation by a PVA passivation layer could improve the
resistance of water vapor and oxygen permeation into OTFT devices.
High-stiffness passivation layer induces less surface strain, which
would result in crazes and cracks. It is therefore suggested to use
moisture and oxygen barrier with higher Young's modulus to increase
structure stiffness and to reduce electrode strain. This can improve the
reliability and lifetime of the OTFT devices.
4. Conclusion
We prepared high-mobility pentacene organic thin-film transis-
tors on flexible plastic substrates using PVA passivation. The devices
exhibited good field-effect mobility of 0.08–0.1 cm2/Vs. The on/off
current ratio has been at the order of 106. PVA was shown to be quite
effective as a protecting passivation layer for pentacene-based OTFT,
because PVA prevented moisture and oxygen permeation. The lifetime
of the passivated OTFT is as high as more than 2 months in the
ambient air environment when it is defined as the time required to
decrease the device mobility by one half.
Acknowledgement
This work was supported in part by the National Science Coun-
cil under research grants NSC96-2221-E182-022 and NSC97-2221-
E182-005. The assistance received from ITRI was also gratefully
acknowledged.
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