Structure-Performance Relationship Pentacene-Based Thin-Film Transistors

Structure-performance relationship in pentacene-based thin-film transistors
Gilles Horowitz1, Wolfgang Kalb2, Mohammad Mottaghil and Philippe Lang'

'ITODYS, CNRS-UMR 7086, Universitv Demis-Diderot. Paris, France, e-mail: (horowitz, lang)(,f,paris7.jussieu.fr
-. Physikalisches Institut, RWTH Aaclhen, Aachen. German+, e-mail: wolfgang_kalb(a,yahoo.de
ion beam deposition with an average thickniess of 80 mm, as

Abstract- Pentacene-based thin-film transistors were determined by ellipsometrv, and a capacitance of 90
fabricated on Si:n+/alumina substrates with gold top-contact nF/cm2. Pentacene was purchase to Aldrich and used with-
source and drain electrodes. The growth mechanism of the out further purification. The pentacene layer was evaporated
pentacene layer was followed by atomic force microscopy
(AFMO. On some devices, the alumina surface was modicfied bv heating in a molybdenum boat at a base pressure of 10-
with fatty- acid self-assembled monolayers (SAM) prior to Torr. Gold source and drain electrodes were also vacuum
pentacene deposition. The first stage of the deposition was evaporated through electron microscope grids used as
found two-dimensional on bare alumina and three- shadowz masks, thus defining a series of regularlv spaced
dimensional on the SAM treated substrates. This has impor- adjacent squares. The respective clhannel length and width
tant implications on the depth dependent mobility, as e'vi-
denced fiom a modeling of the current-voltage characteris- were 10 and 74, and 25 and 54 gim.
tics. It is found that SAM treated samples present higher per- Prior to pentacene deposition. samples were cleaned with
formance with thick film, while the reverse is true for thin fil an UV-ozone treatment. Additional cleaning and activation
Index Terms-organic thin-film transistors, self- were carried out by- dropping sulfuric acid (98%) on the sur-
assembled monolayers, growth mechanism face for 15 s and rinsing the substrate with ultra pure water
right after. The self-assembled monolayers (SAMs) were
L. INTRODUCTION grown by dipping the substrates in a solution of eicosanoic
Organic thin-film transistors are widely studied because acid (Aldrich. 99% pure) in distilled heptane at a concentra-
of their potential applications in large area, lowN-7 cost elec- tion of 5x 10-4 moleAL during 45 min. The qualitv of the
tronics and their compatibilitv with flexible plastic sub- SAM was checked by contact angle measurements. Typical
strates [1]. The carrier mobility of pentacene is now compa- contact angles ranged from 1060 to 10°.
rable to, and in some cases higher than that of hydrogenated Electrical measurements were perfonred in air with a
amorphous silicon [2-5]. Vapor deposited pentacene films manual probe station and a semiconductor parameter ana-
present a polvcrvstalline morphology, with a grain size that lvzer (Keithlev 4200-CSV).
critically depends on the nature of the substrate and the
conditions of deposition [4]. Carrier transport in these films II. RESULTS
depends less on the intrinsic properties of the material than
on grain boundaries and electrode interfaces. It is now well A. Field-effect mobility
accepted that large gmin size is a prerequisite to high mobil- In these preliminary experiments. the field-effect mobil-
ity [6]. Furthermore, because most of the induced charge is itV RIFE was determined from the transconductance
located close to the insulator-semiconductor interface [7],
the morphologp of the film at this interface is of primary gm = OID/01' at low drain voltage. Eq. (1).
importance.
In this conununication, we repoit on pentacene tliin-film AFE= gm L/( ffC,j D) (1)
transistors grown on alumina substrates that serve as the Here, ID is the drain current. VD and I 'G the drain and gate
insulator. Some of the substrates have been modified by a voltages. Ci the insulator capacitance and L and Wr- the
fatty acid self-assembled monolayer (SAM). The mobility channel width and length. Note that as will be discussed in
was estimated as a function of film growth rate, thickness the following, the field-effect mobility is gate voltage de-
of the pentacene layer and the presence or absence of a pendent. The values reported in Fig. 1 and Table 1 corre-
SAM. We also present an analysis of the depth dependence spond to an absolute gate voltage of 4.5 V.
of the mobility, which gives us a better access to the struc- Fig. 1 shows the variation of the field-effect mobility as
ture-properties relationship. a function of pentacene growth rate, for both bare and modi-
fied surfaces. Although the scattering of the data does not
II. EXPERIMENTAL DETAILS allow a definitive conclusion, the curves bring strong evi-
The structure of the thin-film transistors was as follows. dence for an optimum rate at around 0.1 A/s.
The devices were made on highly doped silicon wafers that
serve as gate electrode. The insulator was alumina grown by
0-7803-8304-4/04/$20.00 C02004 IEEE 1409

0.08
0.07 o with SAM
* wihout SAM
0.06
I {
(6
C-
0.05
0.04
0
Q
-0 0.03
E
0.02
0.01
I I
O L
0.001 0.01 0.1 I
evaporation rate (A/s)
Fig. 1 Variation of the field-effect mobility! as a function of growth
rate.
The variation of the mobilitAy with thickness for films

grown at a rate of 0.1 A/s is shown in Table 1. Two
prominent features can be noted. First, the mobilitv in-
Table 1. Field etfect mobilitv (in cm-,Vs) of transistors with various
thickness Fig. 2 AFM images of pentacene films grown on alumina. Left rowv:
non treated substrate: right roxv: SAM modified surface. Thickness
of the filnm: upper line, lnm: lower line, 6 nm.
Thickness (mn) Without SAM With SAM
11)
0.0007 No field-effect
6 .0.0010 0.015 first monolayer, growth on bare alumina turns to a more
30 1 0.0026 0.11 -
I complicated three-dimensional mechanism.
creases by more than one order of magnitude upon modifi- C. Analysis of the depth dependent niobilitv
cation of the insulator surface by a SAM. Next. the mobil- The evolution of the structure of the film during the
itv also increases wlhen the thickness of the pentacene layer deposition process. as evidenced form the above analysis.
increases. Note that these values were estimated at an abso- infers that the charge transport in these films might be
lute gate voltage of 1.5 V. As will be shown in the follow- depth dependent. To verify this hypothesis, we conducted a
ing. mobility, substantially increases when the gate voltage depth analysis of the mobilitv in the conducting channel of
is increased. Also note that no field-effect could be detected the thin-film transistors. Suclh an analysis rests on the fact
on a 3 nm thick film deposited on a SAM modified sub- that when the gate bias increases. the charge distribution in
strate. This feature will be discussed below. the conducting clhannel tends to concentrate near the insula-
tor-semiconductor interface. Accordingly. the mobility is
B. Structure of the pentacene fihns gate voltage dependent. and at least part of this dependence
Fig. 2 shows AFM images of pentacene films at two dif- mirrors the depth dependence.
ferent thicknesses. The low thickness cofresponds to a sub- The analysis was conducted by making use of the Trans-
monolayer coverage formed of not connected grains. These fer Line Method (TLM). which consists of measuring the
images give access to the initial stage of the initial stage of drain current on several devices wAith various channel length.
the growth. The image profile (not shown) clearly; indicates The variation of the drain current is given by Eq. (2)
that the initial growth is two-dimensional on the surface not
treated by- a SAM. The average thickness of the grain is IVD/ID = LI[WjiCi (1 G- I 'T)] + Rc (2)
around 1.5 mm, which correspond to one monolayer of pen-
tacene. By contrast. the tliickness of the grains on ths SAM The method allows one to get rid of the source and drain
modified surface amounts to several monolavers. which contact resistance Rc. The gate bias dependent mobility can
clearly indicates a three-dimensional growth. then be estimated from the slope of the clannel length de-
Further evidence for 3D growth on the SAM modified pendent resistance. A more detailed description of the
surface is brought by the AFM image of a 6 nm thick film method can be found in [8, 91. Results for two 30 nm thick
(lower right image in Fig. 2). This image closely resembles devices, one witlhout and the other one with SAM treat-
that of the 1 nm thick fihns, thus indicating that the growth ment, are shown in Fig. 3. We note that the mobility in-
mechanism does not change from that observed in the ini- creases at low gate voltages. This has been attributed to the
tial stage of the deposition. polv-cnrstalline character of the film [6]. Because grain
The image of a 6 nm thick film on a bare alumina sur- boundaries are likely to contain charge traps. clarge tmns-
face (lower right image) looks strongly different. Here, one port is mainly limited by these traps. As gate voltage in-
recognizes the well-documented dendritic growth of penta- creases. traps are filled, resulting in an increase of the effec-
cene. This clearly indicates that after the completion of the tive mobility.
1410
At higher gate voltages, we note a revers al of the trend: [2] S.F. Nelson. Y.'. Liin D.J. Gundlach and T.N. Jackson. "Tempera-
that is. mobility now decreases. This can t ture-independent transport in high-mobility pentacene
Phvs. Lett.. 72. 1998. 1854-1856. transistors.-
A4ppl.
H. Klauk. M. Halik U. Zschieschlang. G.
[3] Schmid, W. Radlik and W.
0.5 Weber, "High-mobility polvmer gat.e dielectric pentacene thin film
transistors." J. Appl. Phys.. 92, 2002. 5259-5263.
[4] D. Knipp, R.A. Street. A. V6lkel and J. Ho. "Pentacene thin film
0.4 transistors on inorganic dielectrics: Morphology, structural proper-
En ties, and electronic transport ."J. Appl. Phys.. 93. 2003. 347-355.
[5] T.W. Kelley. L.D. Boardman, T.D. Dunbar. D.V. Muyres. M.J.
c 0.3 Pellerite and T.P. Sniith. "High-performance OTFTs using surface-
modified alumina dielectrics," J. Phvs. Cheim. B. 107. 2003, 5877-
E.
._ 0.2 5881.
0 [6] G. Horowitz and M.E. Hajlaoui, "Grain size dependent mobilitv in
polycrystalline organic field-effect transistors," Synth. Metal.. 122.
0.1 2001, 185-189.
[7] A. Dodabalapur. L. Torsi and H.E. Katz, "Organic transistors: Two-
dimensional transport and improved electrical characteristics." Sci-
0
0 5 10 15 20Dence. 268. 1995. 270-271.
[8] H. Klauk. G. Schmidt XX. Radlik. W. Weber, L. Zhou. C.D. Sheraw.
gate voltage (V) J.A. Nichols and T.N. Jackson. "Contact resistance in organic thin
film transistors" Solid-State Electron.. 47. 2003. 297-301.
Fig. 3 Gate voltage dependent mobilitv of devices vvith and without [9] G. Horowitz. "Organiic thiln film transistors: From theory to applica-
SAM treatmenet. In both cases, the pentacene film is 30 nm thick. tions, 'J. Mater. Res.. in press.
the accumulation of the charge close to the insulator-
semiconductor interface where trap centers are likely to be
more abundant. Note that this effect is more pronounced in
the SAM modified device. This can be related to the struc-
ture of the film in that region. On bare alumina, two-
dimensional growth leads to the formation of a continuous
film with a minimum amount of defects. By contrast. the
three-dimensional growth of the film on SAM modified
alunina induces the formation of holes between the grains.
The filling of these holes occurs during the subsequent
stage of the deposition. However, it is likelv that the filling
does not go down to the aluminia surface. so that charge
transport in this region remains largelyIhindered bv the
holes. We finally note that furtlher evidence for the above
statement is brouglht by that transistors made with very thin
films of pentacene (3 nm) do not show any current on
SAM modified samples. while a small current is detected
on devices with bare alumina.
IV. CONCLUSIONS
The growth mechanism of pentacene on bare and SAM
modified alumina shows significant differences. On bare
alumina, the deposition is first two-dimensional and turns
to three-dimensional after the completion of the first layer.
On the modified substrate, film growth remains three-
dimensional all along the deposition process. The present
study brings evidence for the inference of these features on
the behavior of field-effect transistors made on these sub-
strates. A depth dependent analysis of the mobility slhows
that more efficient charge transport is found in the bulk of
the fllm for the SAM modified device, wlhile a reverse trend
is observed for charge transport at the insulator-
semiconductor interface.
V. REFERENCES
[1] C.D. Dimitrakopoulos and P.R.L. Malenfant, "Organic thin film
transistors for large area electronics."' Ad". Mater., 14. 2002, 99-
117.
1411

Structure-Performance Relationship Pentacene-Based Thin-Film Transistors

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Structure-Performance Relationship Pentacene-Based Thin-Film Transistors

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Structure-performance relationship in pentacene-based thin-film transistors

Gilles Horowitz1, Wolfgang Kalb2, Mohammad Mottaghil and Philippe Lang'

ion beam deposition with an average thickniess of 80 mm, as

0-7803-8304-4/04/$20.00 C02004 IEEE 1409

The variation of the mobilitAy with thickness for films

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