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2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Adv. Mater. 2011, 23, 100–105 wileyonlinelibrary.com
Sangchul Lee, Gunho Jo, Seok-Ju Kang, Gunuk Wang, Minhyeok Choe, Woojin Park,
Dong-Yu Kim, Yung Ho Kahng,* and Takhee Lee*
Enhanced Charge Injection in Pentacene Field-Effect
Transistors with Graphene Electrodes
S. Lee, G. Jo, S.-J. Kang, G. Wang, M. Choe, W. Park,
Prof. D.-Y. Kim, Dr. Y. H. Kahng, Prof. T. Lee
Department of Nanobio Materials and Electronics
Department of Materials Science and Engineering
Gwangju Institute of Science and Technology
Gwangju 500–712, Korea
E-mail: yhkahng@gist.ac.kr; tlee@gist.ac.kr
Dr. Y. H. Kahng
Research Institute for Solar and Sustainable Energies
Gwangju Institute of Science and Technology
Gwangju 500–712, Korea
DOI: 10.1002/adma.201003165
Organic electronic devices have generated a great deal of
research interest because of their low-cost fabrication, limitless
material variety, and the myriad of potential applications.
[1–9]
Sig-
nificant research efforts have been directed towards improving
the performance of devices such as organic field-effect transis-
tors (OFETs).
[4–9]
One important approach for improving this
performance is to select contact-electrode materials that yield
efficient charge injection into the active channels.
[7–9]
Con-
tact electrodes affect the device performance by determining
the carrier type from the energy-level alignment and by gov-
erning charge injection, which is related to the quality of the
contacting interface.
[10,11]
Noble metals and doped metal-oxide
films have conventionally been used as electrode materials.
However, problems with metal-oxide films include their inflex-
ibility and high cost.
[12]
In addition, Au, which is predominantly
used as an electrode in OFETs, has shown a significant charge-
injection barrier because of unfavorable interface dipole layer
formation.
[13,14]
Therefore, alternative electrode materials must
be found to avoid such shortfalls.
[7–9,15–17]
Recently, graphene-based thin films have attracted great
attention as an alternative electrode material for organic elec-
tronic devices.
[18]
Graphene, a two-dimensional conducting
sheet, is transparent and conducting and has good mechan-
ical stability and flexibility.
[19,20]
Large samples of multilayer
graphene (MLG) films have been synthesized by chemical
vapor deposition (CVD) or solution-based methods, rendering
them realistic prospects as electrodes.
[21–23]
To date, MLG films
have exhibited a promising performance as electrodes for many
organic devices such as organic transistors,
[15–17]
light-emitting
diodes,
[24,25]
and photovoltaics.
[26–29]
However, to establish MLG
films as viable alternative electrodes for organic devices and to
provide fundamental engineering routes for better perform-
ances, detailed studies on the interface between the MLG film
and organic materials are necessary. Because the interfacial
characteristics such as contact resistance, dipole effect, and
charge injection barrier height strongly dominate the charge-
injection properties, these characteristics need to be analyzed.
In this work, we report on the efficient charge injection in
pentacene OFETs with graphene electrodes. Pentacene OFETs
are an excellent choice to investigate the properties of the
interface because they are known to be reliable, exhibit a high
mobility, and have been studied for many years as organic sem-
iconductor devices.
[30,31]
We show that the OFET performance
was significantly improved by using MLG electrodes; the output
and transfer currents and mobility increased in comparison to
conventional OFETs with Au electrodes. Detailed investigations
on the contact resistance and charge-injection barrier height
revealed that such improvements were a result of the superior
interfacial contact between the MLG electrode and the penta-
cene organic channels. Our findings will aid in establishing
graphene-based thin films as an efficient electrode material for
improving OFETs and other types of organic electronic devices.
The fabrication process of pentacene OFETs with patterned
MLG electrodes is illustrated in Figure 1. The graphene syn-
thesis is explained in the Experimental section. The grown
MLG film was detached from the growth substrate by using
a catalyst-etching and scooping-up technique with aqueous
iron chloride (FeCl
3
) solution (around 1 M) as the etchant
(Figure 1a),
[21,32]
and transferred onto a 300-nm-thick SiO
2
layer
on a heavily doped Si wafer (Figure 1b). Then, a 50-nm-thick
Ni layer was evaporated through a shadow mask onto the MLG
film (Figure 1c), and the substrate was exposed to oxygen
plasma at 200 mTorr and 50 W to remove the MLG film from
the unprotected regions (Figure 1d). The Ni mask patterns were
then etched away in FeCl
3
solution (Figure 1e). The patterned
graphene electrodes were coated with poly(methylmethacrylate)
(PMMA). Subsequently, the PMMA-coated graphene electrodes
were detached from the SiO
2
substrate by etching the SiO
2
layer
with buffered oxide etchant. Then, the detached graphene elec-
trodes were transferred onto an octadecyltrichlorosilane (OTS)-
treated substrate. After this, the PMMA was removed by ace-
tone. Finally, a pentacene layer (ca. 60 nm thick) was deposited
using a thermal evaporator under vacuum through a shadow
mask onto the patterned MLG electrodes (Figure 1f). The fab-
ricated OFETs had a width of 1000 μm and channel lengths of
50, 100, 200, and 300 μm.
Figure 2 shows the typical characteristics of the graphene-elec-
trode pentacene OFETs (denoted as GR-pentacene OFETs). Also
shown are the characteristics of Au-electrode pentacene OFETs
(denoted as Au-pentacene OFETs) for comparison. Figure 2a
presents the output characteristics, that is, the drain current
versus drain voltage ( I
D
– V
D
) curves at a fixed gate voltage ( V
G
)
of -50 V for GR-pentacene and Au-pentacene OFETs with