APPLIED PHYSICS LETTERS 91, 203508 共2007兲

Contact-metal dependent current injection in pentacene thin-film

transistors
S. D. Wang, T. Minari, T. Miyadera, K. Tsukagoshi,a兲 and Y. Aoyagi
RIKEN, Wako, Saitama 351-0198, Japan and CREST-JST, Kawaguchi, Saitama 332-0012, Japan
共Received 24 July 2007; accepted 26 October 2007; published online 13 November 2007兲
Contact-metal dependent current injection in top-contact pentacene thin-film transistors is analyzed,
and the local mobility in the contact region was found to follow the Meyer-Neldel rule. An
exponential trap distribution, rather than the metal/organic hole injection barrier, is proposed to be
the dominant factor of the contact resistance in pentacene thin-film transistors. The variable
temperature measurements revealed a much narrower trap distribution in the copper contact
compared with the corresponding gold contact, and this is the origin of the smaller contact resistance
for copper despite a lower work function. © 2007 American Institute of Physics.
关DOI: 10.1063/1.2813640兴

Large contact resistance 共RC兲 in organic thin-film tran- ⫻ 10−5 Pa兲 system equipped with temperature controller.
sistors 共OTFTs兲 is one of the serious problems for practical Figure 1共b兲 shows the transfer characteristics of the pen-
applications,1–3 and the fundamental origin of RC is still un- tacene TFTs. The drain current 共ID兲 in the Cu TFT is much
clear. Since the energy difference between the Fermi level larger at low gate bias 共VGS兲 compared with the Au TFT; this
共EF兲 of metal electrode and the highest occupied molecular feature is highly reproducible in about 100 TFTs. The tran-
orbital 共HOMO兲 of organic semiconductor is commonly con- sistor total resistance 共Rtot兲 in the linear regime can be ex-
sidered as an origin of RC in p-type OTFTs, gold 共Au兲 has pressed as
been widely used as source and drain electrodes due to its
high work function. On the other hand, RC can be treated as L
Rtot = Rch + RC = + RC , 共1兲
two parts in series 关see Fig. 1共a兲兴,4 the part due to the metal/ WCi共VGS − VT兲␮ch
organic hole injection barrier 共Rint兲 and the other part for
charge accessing from the metal/organic interface to the where Rch and ␮ch are the channel resistance and channel
channel 共Racc兲. In particular, the charge transport in the latter mobility, respectively, Ci is the capacitance per unit area of
part was found to follow the Meyer-Neldel rule,4 indicating SiO2 layer, and VT is the threshold voltage. In the linear
regime 共VGS − VT ⬎ ⬎ VDS兲, we have Rsource ⬇ Rdrain = RC / 2,
that trap distribution in the contact region has great contri-
bution to RC. where Rsource and Rdrain are the resistances at source and drain
In this letter, we present that copper 共Cu兲, which is one contacts, respectively. The transfer line method 共TLM兲 was
of the low-cost metals and highly desirable in device manu- employed here to estimate RC based on Eq. 共1兲.3,4 As an
facturing, can produce smaller RC than Au in top-contact example, normalized Rtot of a set of Cu TFTs is plotted as a
function of L in Fig. 1共c兲.
pentacene TFTs despite a lower work function. The
temperature-varying measurements revealed that RC is domi-
nated by the accessing resistance rather than the hole injec-
tion barrier, and small RC for Cu is ascribed to the narrow
trap distribution at the Cu contact.
The heavily doped silicon wafers, with 200 nm silicon
dioxide 共SiO2兲 layers, were employed as the transistor sub-
strates. The substrates were coated with a self-assembling
monolayer of beta-phenethyltrichlorosilane 共␤-PTS兲 共Ald-
rich, 95%兲 prior to the deposition of pentacene.5 Pentacene
共Aldrich, purified with temperature gradient sublimation兲
thin films with 40 nm thickness were deposited at 0.1 Å s−1
under 6 ⫻ 10−5 Pa. Cu and Au top electrodes were subse-
quently deposited by thermal evaporation at 0.3 Å s−1 in the
same chamber, where a shadow mask was used to define
seven transistors 关see Fig. 1共a兲兴 with the same channel width
共W = 750 ␮m兲 and varied channel lengths 共L = 50– 350 ␮m
with 50 ␮m interval兲 on an identical pentacene film. Note
that all the processes except the final metal deposition were
performed at the same time for all the devices. The transistor
characteristics were measured in a high vacuum 共8 FIG. 1. 共Color online兲 共a兲 Optical micrograph of a set of Cu TFTs 共left兲 and
schematic transistor cross section describing RC 共right兲. 共b兲 Transfer charac-
teristics in the linear regime of pentacene TFTs 共L = 50 ␮m, 300 K兲 with Cu
a兲
Author to whom correspondence should be addressed. Electronic mail: and Au top electrodes. VDS is drain bias. 共c兲 W-normalized transistor total
tsuka@riken.jp resistance vs L 共TLM plots兲 of a set of Cu TFTs.

0003-6951/2007/91共20兲/203508/3/$23.00 91, 203508-1 © 2007 American Institute of Physics

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 203508-2 Wang et al. Appl. Phys. Lett. 91, 203508 共2007兲

FIG. 2. 共Color online兲 共a兲 Experimental data of W-normalized contact resis-
tance as a function of gate bias at 300 K 共markers兲. Solid line denotes
calculation data based on the theory in Ref. 10, using RC = C共VGS − VT兲−␣−1 in
which ␣ = EMN / kT − 1 and C is an adjustable constant. 共b兲 W-normalized
contact resistance vs gate bias at different temperatures from 160 to 300 K
with 20 K interval. Each line contains 20 data of RC obtained from TLM
plots.
FIG. 3. 共Color online兲 Arrhenius plots of contact mobility for 共a兲 Cu and 共b兲
Au contacts. The activation energy is calculated from the slope of fitting
straight line, EMN and ␮C00 are derived from the intersection point.
3共b兲 show a common intersection point in both cases, imply-
ing that ␮C follows the Meyer-Neldel rule11,12

Figure 2共a兲 shows that RC for Cu at 300 K is smaller

compared with Au, especially at low VGS. On the other hand,
␮C = ␮C0 exp − 冉 冊 EA
kT
= ␮C00 exp
EA
EMN
冉 冊 冉 冊
exp −
EA
kT
the Rch values of the both TFTs 共data not shown兲 are very
close, indicating the similarity of the channel region. The
temperature dependence of RC is shown in Fig. 2共b兲. It is
= ␮C00 exp EA 冋冉 1
EMN
−
1
kT
冊册 , 共4兲

clear that the charge transport at both contacts is thermally
activated. These results suggest that RC is not dominated by
the hole injection barrier. The reasons are as follows. 共1兲 The
reported hole injection barrier height at the Cu/pentacene
interface 共0.95 eV兲 is higher than that at the Au/pentacene
共0.47 eV兲 interface.6,7 Therefore, if RC is dominated by the
hole injection barrier, the Cu contact should have larger RC.
共2兲 If RC is determined by the tunneling process across
the hole injection barrier, RC should be temperature
independent.8
According to the above discussion, we define the local
mobility in the contact region as contact mobility 共␮C兲,
which satisfies
2D
RC = , 共2兲
WCi共VGS − VT兲␮C
where D is the thickness of pentacene films, and the factor 2
comes from RC = Rsource + Rdrain. As expected from Eq. 共2兲, an
approximately linear increase of RC with D was observed
when the pentacene films are not very thin 共D ⬎ 10 nm兲. In
order to precisely extract VGS-dependent ␮C, we define a
VGS-dependent function ⌽共VGS兲 = ⳵共1 / RC兲 / ⳵VGS, which can
be obtained from the data in Fig. 2共b兲. Assuming ␮C follows
the empirical VGS dependence,9,10 that is,
␮C = ␬共VGS − VT兲␣ ,
␣+1
we have 1 / RC ⬃ 共VGS − VT兲 and ⌽共VGS兲 ⬃ 共␣ + 1兲␮C from
Eqs. 共2兲 and 共3兲, and accordingly 共1 / RC兲 / ⌽共VGS兲 = 共VGS
− VT兲 / 共␣ + 1兲. We derived the exponent ␣ from the linear
plots of 共1 / RC兲 / ⌽共VGS兲 vs VGS, whose values are tempera-
ture dependent 共about −0.2 and 1.0 at 300 K for Cu and Au,
respectively兲. Eventually, ␮C is calculated from ⌽共VGS兲 and
␣. It is worth pointing out that the present method for mo-
bility extraction is quite general. For instance, in the case of
constant mobility 共␣ = 0兲 this method is equivalent to the
conventional extrapolation of transfer curve.
The Arrhenius plots of ␮C and the corresponding activa-
tion energy 共EA兲 for Cu and Au are shown in Figs. 3共a兲 and
3共b兲, respectively. The fitting straight lines in Figs. 3共a兲 and
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where ␮C0 共Y intercept兲 and ␮C00 共intersection point兲 are the
exponential prefactors, EMN is the Meyer-Neldel energy, k is
the Boltzmann constant, and T is the temperature. EMN can
be calculated from the intersection point. EMN for Cu is as
low as 22 meV, which is lower than kT at room temperature
共26 meV兲. From Eq. 共4兲, ␮C is expected to increase and de-
crease with EA when kT ⬎ EMN and kT ⬍ EMN, respectively.
This behavior is clearly presented in Fig. 3共a兲 for Cu. The
effect of the ␮C decrease with increasing VGS 共for instance,
Cu at 300 K兲 may counteract the effect of the charge density
increase, and result in a weak VGS dependence of RC as dem-
onstrated in Fig. 2共a兲. In contrast, the high EMN 共55 meV兲 for
Au will lead to a strong VGS dependence of RC at all mea-
sured temperatures 关Fig. 2共b兲兴.
The observation of the Meyer-Neldel rule in the present
study can be interpreted with an exponential distribution of
trap states in the contact region.4,10,13 The physical meaning
of EMN is the width of trap distribution. Thus the trap distri-
bution at the Cu contact is much narrower compared with the
Au contact 共see Fig. 4兲. On the other hand, ␮C00
共3兲
FIG. 4. 共Color online兲 Schematics of trap distribution and trap filling in the
contact region at 共a兲 low gate bias and 共b兲 high gate bias. NT共E兲
= 共NT0 / EMN兲exp共−E / EMN兲 denote exponentially distributed density of trap
states 共solid line兲, where EMN is derived from Fig. 3 and NT0 is estimated
from ␮C00. nT共E兲 = NT共E兲f共E兲 denote density of trapped charges 共broken
line兲, where f共E兲 is the Fermi-Dirac distribution at 300 K. The EF position
共vertical dotted line兲 is selected for setting the total density of trapped
charges 共integration of nT兲 equal in both cases of Cu and Au.
 203508-3 Wang et al.
= ␮ f NHOMO / NT0 based on the multiple trapping and release
model,10,14 where ␮ f is the free carrier mobility along the
vertical direction, and NHOMO and NT0 are the density of
HOMO states and the total density of trap states 共integration
of trap distribution兲 in the contact region, respectively. There
are two factors that may lead to the low ␮C00
⬃ 10−3 cm2 / V s as observed in Figs. 3共a兲 and 3共b兲. One is the
relatively low ␮ f in the present case because the vertical
direction is perpendicular to the ␲-overlap direction. The
other one is high NT0. For instance, assuming ␮ f
= 0.1 cm2 / V s and NHOMO = 1018 cm−3, NT0 is in the order of
1020 cm−3 for both contacts.
Using the derived EMN and estimated NT0, the density of
trap states 共NT兲 in the contact region is schematically plotted
in Fig. 4. The trapped charges density 共nT兲 is dependent on
NT and the EF position, that is, nT共E兲 = NT共E兲f共E兲, where E is
the energy and f共E兲 is the Fermi-Dirac distribution. At low
VGS, there are much fewer deep traps for Cu, so that EF is
closer to the HOMO as shown in Fig. 4共a兲. As a conse-
quence, the Cu TFT shows smaller RC and accordingly larger
ID. The increase of VGS will move EF toward the HOMO by
trap filling, leading to an increase of both the free carrier
density 共n f 兲 and nT 关see Fig. 4共b兲兴. However, ␮C ⬇ ␮ f n f / nT is
determined by the ratio n f / nT,10,14 and the change of this
ratio with EF is strongly dependent on the trap distribution
profile. If the trap distribution is very steep 共EMN ⬍ kT兲, as
the situation of Cu at 300 K, the nT increase due to the EF
shift will be in excess of the corresponding n f increase. Con-
sequently, ␮C will decrease with increasing VGS as shown in
Fig. 3共a兲. Finally, an exponential trap distribution actually
implies a VGS-dependent mobility with the same form of Eq.
共3兲, where ␣ = EMN / kT − 1.10 According to this theory, the
calculation for RC at 300 K is shown in Fig. 2共a兲, and a good
consistency is seen. Therefore, the physical picture in Fig. 4
can well interpret the experimental results.
High NT0 in the contact region might arise from the
dense structural defects close to the metal/organic interface.
The possible causes of the defects include original surface
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Appl. Phys. Lett. 91, 203508 共2007兲
defects before the metal deposition, vacancy and distortion
after the metal deposition, and molecular polarization due to
the image force. More experiments are needed to clarify the
underlying mechanism of the different trap distributions be-
tween the Cu and Au contacts.
In conclusion, top-contact pentacene TFTs with Cu elec-
trodes show smaller RC in comparison with the correspond-
ing Au TFTs. We suggest that the large RC in OTFTs is due
not to the hole injection barrier but to a low mobility region
close to the metal/organic interface. Different exponential
distributions of trap states at the Cu and Au contacts are well
defined by our analysis, and the small RC of the Cu contact is
attributed to the narrow trap distribution.
This work was supported in part by the Grant-In-Aid for
Scientific Research 共Nos. 16GS50219, 17069004, and
18201028兲 from the Ministry of Education, Culture, Sport,
Science and Technology of Japan.
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