APPLIED PHYSICS LETTERS 94, 083309 共2009兲

Contact resistance instability in pentacene thin film transistors induced

by ambient gases
S. D. Wang,1,2,a兲 T. Minari,2,3,4 T. Miyadera,2,3 K. Tsukagoshi,2,3,5,b兲 and J. X. Tang1
1
FUNSOM, Soochow University, Suzhou, Jiangsu 215123, People’s Republic of China
2
CREST-JST, Kawaguchi, Saitama 332-0012, Japan
3
AIST, Tsukuba, Ibaraki 305-8568, Japan
4
RIKEN, Wako, Saitama 351-0198, Japan
5
MANA, NIMS, Tsukuba, Ibaraki 305–0044, Japan
共Received 19 January 2009; accepted 5 February 2009; published online 27 February 2009兲
Top-contact pentacene thin film transistors show the strong susceptibility of the contact resistance to
ambient gases. Moisture and oxygen lead to the increase and decrease in the contact resistance,
respectively. The phenomenon is interpreted by the local conductivity change in the contact region
induced by the adsorption/desorption of ambient gases. The present works suggest that the current
injection in the pentacene thin film transistors is strongly correlated with the charge transport
property in the contact region, where the contact resistance is mainly controlled by the charge trap
states. © 2009 American Institute of Physics. 关DOI: 10.1063/1.3089246兴

Pentacene-based organic thin film transistors 共OTFTs兲
have been extensively investigated over the last decade, be-
cause of the promising applications such as integrated
circuits1 and sensors.2 The electrical characteristics of penta-
cene OTFTs,3–5 as well as pentacene single-crystal field ef-
fect transistors6 and polymer OTFTs,7,8 have been reported to
be susceptible to ambient gases such as moisture 共H2O兲 and
oxygen 共O2兲. The ambience induced instability is on one
hand a severe problem that needs to be solved for producing
highly stable and reliable OTFTs, on the other hand, it hints
the potential of using OTFTs as gas sensors. The instability
studies have often focused on the channel properties such as
the channel mobility 共␮ch兲 and threshold voltage 共VT兲. How-
ever, it lacks of probing the influence of ambient gases on the
contact resistance 共RC兲, which is typically large and cannot
be neglected in OTFTs. This issue is significant not only for
the comprehensive understanding on the ambient gas effects,
but also for the attempt to effectively reduce RC in OTFTs.
We report that the top-contact pentacene OTFTs show a dra-
matic change in RC in different environment, which is attrib-
uted to the adsorption/desorption of ambient gases. The ex-
perimental observations indicate that H2O and O2 play the
opposite roles in the RC change, and suggest that the funda-
mental origin of large RC is the trap-rich low-mobility nature
of the contact region.
The heavily doped silicon wafers were employed as the
common gate electrodes, with 200 nm thick silicon dioxide
共SiO2兲 as the gate insulating layers. The SiO2 surface was
cleaned and coated with a self-assembling monolayer of
␤-phenethyltrichlorosilane 共Aldrich, 95%兲 in glove box,9
prior to the pentacene 共Aldrich, purified with temperature
gradient sublimation兲 deposition in high vacuum 共HV兲. The
thickness and the deposition rate of pentacene are about 40
nm and 0.1 Å/s, respectively. As copper 共Cu兲 top contacts
show smaller RC 10,11 and lower bias stress instability12 com-
pared with conventional gold 共Au兲 contacts, both Cu and Au
electrodes 共40 nm兲 were thermally evaporated and tested.
a兲
Electronic mail: wangsd@suda.edu.cn.
b兲
Electronic mail: kazu.tsukagoshi@aist.go.jp.
The top electrode pattern produces a set of OTFTs with an
identical channel width 共W = 750 ␮m兲 and varied channel
lengths 共L = 50– 350 ␮m with 50 ␮m interval兲, realizing the
precise RC extraction by the transfer line method 共TLM兲.13,14
The method is based on the following linear regime
equation:15
L
Rtotal = Rch + RC = + RC , 共1兲
WCi共VGS − VT兲␮ch
where Rtotal, Rch, Ci, and VGS are the transistor total resis-
tance, the channel resistance, the capacitance per unit area of
the SiO2 layer, and the gate bias, respectively. From the lin-
ear plot of Rtotal versus L, RC can be attained at the intercept
of the Y-axis 共L = 0兲.
A series of RC measurements of the pentacene OTFTs
were performed in different environment, with a sequence of
measuring 共1兲 in air, 共2兲 intermittently from hours up to days
in HV about 0.0001 Pa, 共3兲 successively in nitrogen 共N2兲 and
O2 atmosphere, and 共4兲 in air again. This process is sche-
matically described in Fig. 1共a兲, where the TLM plots mea-
sured in air and in HV are shown in Figs. 1共b兲 and 1共c兲,
respectively. Between the adjacent measurements, the
samples were stored in dark without any bias application.
Figure 2 shows the same trend of the RC change with the
storing time no matter the magnitude of VGS nor the materi-
als of the metal electrodes, and the phenomenon is highly
reproducible for different sets of pentacene OTFTs. It is ap-
parent that RC is unstable and easily influenced by the ambi-
ent conditions, indicating the strong ambient gas effects on
RC. The first feature in Fig. 2 is the RC decrease after pump-
ing to HV from air, which should be due to the desorption of
ambient gases from the pentacene films. Furthermore, Fig. 2
shows the second feature that RC is slowly increasing in HV,
though the increasing rate is gradually decreased. Note that
this feature has no relevance to the so-called bias stress
effect12,16 because of the fact that neither VGS nor the drain
bias 共VDS兲 were applied during the storage. The opposite
changing direction of RC in HV may arise from the different
adsorption effects of different gases, whose desorption rates
may be also different. In order to check this hypothesis and

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 083309-2 Wang et al.
FIG. 1. 共Color online兲 共a兲 Schematics of measuring environment change,
measuring sequence are described in detail in the text. TLM plots of a set of
pentacene OTFTs 共b兲 initially measured in air, and 共c兲 measured just after
pumping to HV, where straight lines are linear fittings, and arrows point at
channel-width normalized contact resistance.
distinguish the different gas effects, the pentacene OTFTs
were subsequently exposed to N2 atmosphere, and only the
small change in RC were observed. However, the subsequent
exposure to O2 atmosphere results in the dramatic RC de-
crease, and afterwards the RC values are close to the mini-
mum ones in HV. Thus it is reasonable to attribute the RC
increase in HV mainly to the O2 desorption, which might be
slower than the other gas desorption. Finally, the devices
were exposed to air again, and RC is promptly increased to
the same level as the initial measurements before the vacuum
pumping. This demonstrates that H2O can lead to an increase
in RC, and that the H2O desorption may be responsible for
the rapid RC decrease at the starting stage of the vacuum
pumping. As the reference, a group of the Rch data are shown
in Fig. 3, where the behavior of the Rch change are very
similar with that of the corresponding RC change in Fig. 2共b兲.
FIG. 2. 共Color online兲 Channel-width normalized contact resistance vs stor-
ing time of pentacene OTFTs measured in different environment, where zero
time represent starting of vacuum pumping, and gray area represent situation
in air. Solid, open, open-with-plus, and open-with-cross squares represent
data measured in air, HV, N2, and O2 atmosphere, respectively. Cu contact
共a兲 at VGS = −20 V and 共b兲 at VGS = −40 V, Au contact 共c兲 at VGS = −20 V
and 共d兲 at VGS = −40 V.
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Appl. Phys. Lett. 94, 083309 共2009兲
FIG. 3. 共Color online兲 Channel-width normalized channel resistance vs stor-
ing time of pentacene OTFTs measured in different environment, where the
measuring conditions are as same as those in Fig. 2共b兲.
Therefore, it is suggested that the current injection and trans-
port properties are correlated. The results above provide im-
portant information on the origin of RC and on the ambient
gas effects in pentacene OTFTs, and the insights are dis-
cussed in the following.
We have argued that RC in pentacene OTFTs is domi-
nated not by the hole injection barrier, but by the access
resistance from the metal/pentacene interface to the channel
arising from the high density of trap states in the contact
region.10,17,18 The trap-rich picture of the contact region is
schematically shown in Fig. 4, where the local charge mo-
bility 共␮C兲 is much lower compared with ␮ch in the channel.
This argument is based on several experimental observa-
tions: 共1兲 the RC change in Fig. 2 is reversible, implying that
the irreversible strong chemical reaction, such as the penta-
cene oxidation and the Cu oxidation at the Cu/pentacene
interface, if any, do not have remarkable influence on RC; 共2兲
although the lower work function of Cu which may lead to a
higher hole injection barrier, the Cu top contacts show
smaller RC than the corresponding Au contacts;10,11 共3兲 RC is
strongly dependent on the pentacene film morphology, for
example, on the grain size,14 suggesting the high sensitivity
of RC to the defect density; and 共4兲 if there is a barrier for the
hole injection at the source contact, no barrier is expected for
the hole extraction at the drain contact 共assuming same en-
ergy level alignment at both contacts in linear regime兲. How-
ever, RC of the drain contact is reported to be comparable
with that of the source contact.18 Therefore, the RC instability
may result from the local conductivity change in the contact
region caused by the ambient gas adsorption/desorption,
rather than from the modification of the hole injection bar-
rier. The ambient gas molecules can diffuse into the contact
region from the top electrode edges, and the diffused gas
molecules may interact with the pentacene molecules and
FIG. 4. Schematic energy diagram of contact region in pentacene OTFTs,
where EF represent Fermi level of metal electrode. Short lines and open-
with-plus circles represent hole trap states and trapped holes, respectively.
 083309-3 Wang et al.
introduce the electronic states within the highest occupied
molecular orbital 共HOMO兲 and lowest unoccupied molecular
orbital gap. As a consequence, the transport property in the
contact region and accordingly RC is changed depending on
the environmental conditions.
It is interesting that the adsorption of H2O and O2 affect
RC oppositely, as demonstrated in Fig. 2. The H2O adsorp-
tion leads to the RC increase, corresponding to the decrease
in mobile charge density in the contact region. The H2O
molecules may induce the occupied 共donorlike兲 states above
the HOMO, which act as the hole traps and decrease the
local conductivity. ␮ch in the linear regime measured in air,
about 0.4 cm2 / V s, is lower compared with that measured in
HV. In addition, the devices show much stronger bias stress
effect in air than that in HV 共data not shown兲, in consistency
with the consideration of H2O inducing the hole traps in
pentacene.4,6 Furthermore, H2O seems easier to desorb from
pentacene than O2, as shown in Fig. 2, which might be re-
lated to the lighter weight of H2O and its larger dipole mo-
mentum.
On the other hand, the O2 adsorption leads to the RC
decrease after keeping the devices in HV for a long time,
corresponding to the increase in mobile charge density in the
contact region. As opposite to H2O, the O2 molecules may
induce the unoccupied 共acceptorlike兲 states above the
HOMO and generate holes, which is consistent with the elec-
tron attraction nature of O2. Consequently the slow desorp-
tion of O2 in HV gradually decreases the local conductivity
in the contact region, where the deceleration of the RC in-
creasing rate 共see Fig. 2兲, can be interpreted by the decreas-
ing O2 desorption rate due to the lower O2 density inside the
pentacene films. The exact O2 effect in pentacene is still
under debate,3–6 more efforts are needed to fully clarify this
issue.
From the application point of view, the RC instability
should be suppressed, for instance by encapsulation, to
achieve high performance OTFTs with high stability and re-
liability. On the other hand, it is demonstrated that the ap-
propriate gas adsorption can remarkably reduce RC, similar
with the reports utilizing the doping techniques.19,20
The pentacene OTFTs show the RC instability dependent
on the environmental conditions; thus it is significant to take
the contact into account for the stability investigation of OT-
FTs. The RC change due to the adsorption/desorption of am-
bient gases is reversible to a large extent, and the study might
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Appl. Phys. Lett. 94, 083309 共2009兲
be extended to other gases for the OTFTs-based sensor ap-
plications. The present results support the physical picture
that the current injection in the pentacene OTFTs is limited
by the high density of traps in the contact region, which can
be affected by the adsorption/desorption of ambient gases.
The authors would like to thank K. Nomoto for valuable
discussions. This work was supported in part by the Grant-
In-Aid for Scientific Research 共Grant Nos. 16GS50219,
17069004, and 18201028兲 from the Ministry of Education,
Culture, Sport, Science and Technology of Japan.
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