Quantum efficiency of ambipolar light-emitting polymer field-effect

transistors
Jana Zaumseil, Christopher R. McNeill, Matt Bird, Darryl L. Smith, P. Paul Ruden et al.

Citation: J. Appl. Phys. 103, 064517 (2008); doi: 10.1063/1.2894723

View online: http://dx.doi.org/10.1063/1.2894723
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 JOURNAL OF APPLIED PHYSICS 103, 064517 共2008兲

Quantum efficiency of ambipolar light-emitting polymer

field-effect transistors
Jana Zaumseil,1 Christopher R. McNeill,1 Matt Bird,1 Darryl L. Smith,2 P. Paul Ruden,3
Matthew Roberts,4 Mary J. McKiernan,5 Richard H. Friend,1 and Henning Sirringhaus1,a兲
1
Cavendish Laboratory, Department of Physics, University of Cambridge, J J Thomson Ave.,
Cambridge CB3 0HE, United Kingdom
2
Los Alamos National Laboratory, Los Alamos, New Mexico 87545, USA
3
University of Minnesota, Minneapolis, Minnesota 55455, USA
4
Sumation Co. Ltd., 2020 Cambourne Business Park, Cambourne, Cambridgeshire CB23 6DW,
United Kingdom
5
Cambridge Display Technology Ltd., Building 2020, Cambourne Business Park,
Cambridgeshire CB3 6DW, United Kingdom
共Received 15 October 2007; accepted 8 January 2008; published online 28 March 2008兲
The emission characteristics and external quantum efficiencies of ambipolar polymer light-emitting
field-effect transistors are investigated as a function of applied voltage, current density, and ratio of
hole to electron mobility. Green-emitting poly共9,9-di-n-octylfluorene-alt-benzothiadiazole兲 共F8BT兲
with balanced electron and hole mobilities and red-emitting poly共共9,9-dioctylfluorene兲-2,7-
diyl-alt-关4,7-bis共3-hexylthien-5-yl兲-2,1,3-benzothiadiazole兴-2⬘ , 2⬙-diyl兲 共F8TBT兲 with strongly
unbalanced hole and electron mobilities as semiconducting and emissive polymers are compared.
The current-voltage and light output characteristics of the two types of light-emitting transistors
were found to be fundamentally alike independent of mobility ratio. Device modeling allowing for
a single 共Langevin-type兲 charge recombination mechanism was able to reproduce the device
characteristics for both cases but could not replicate the experimentally observed dependence of
external quantum efficiency on current density. The increase of quantum efficiency with current
density up to a saturation value could be indicative of a trap-assisted nonradiative decay mechanism
at the semiconductor-dielectric interface. Optical output modeling confirmed that the maximum
external quantum efficiency of F8BT light-emitting transistors of 0.8% is consistent with complete
recombination of all charges and a singlet exciton fraction of 25%. © 2008 American Institute of
Physics. 关DOI: 10.1063/1.2894723兴

I. INTRODUCTION
Organic light-emitting field-effect transistors 共LFETs兲
are a new type of bifunctional organic electronic devices
combining the switching behavior of transistors with the
emissive behavior of light-emitting diodes 共LEDs兲. Due to
their planar structure allowing spatial resolution of the re-
combination and emission zone and properties such as higher
charge carrier mobilities and current densities compared to
LEDs, they have received increased attention in recent
years.1 A number of LFETs have been demonstrated using a
wide range of materials from small molecules to conjugated
polymers and blends thereof. Some of the demonstrated
LFETs operate solely as unipolar transistors, being only ca-
pable of conducting either holes or electrons.2–4,4,5 Injection
and recombination of opposite charges occurs only in the
direct vicinity of the drain electrodes and is often inefficient.
Recently, however, a number of ambipolar LFETs were
reported.6–11 For suitable biasing conditions, these ambipolar
FETs can accumulate both positive and negative charge car-
riers in spatially separate regions of the device. They allow
observation of a narrow recombination and emission zone
where the hole and electron accumulation layers meet. This
zone can be moved and positioned from the source electrode
a兲
Electronic mail: hs220@cam.ac.uk.
through the channel to the drain electrode and vice versa by
changing the applied gate 共Vg兲 or source-drain voltage
共Vds兲.7–9,11 Theoretical models supported by optical reso-
lution of the emission zone showed that this ambipolar re-
gime can be thought of as a saturated electron channel and a
saturated hole channel in series within the overall transistor
channel. In the simplest case, an infinite recombination rate
and, thus, an infinitesimal width of the recombination zone
are assumed such that the hole 共Ih兲 and electron current 共Ie兲
equal the source-drain current Ids = Ih = Ie.10,12–14 Even for a
finite recombination rate, for example, based on Langevin-
type recombination and, hence, a certain interpenetration of
holes and electrons,15,16 this assumption holds true, if the
channel length is sufficiently long compared to the width of
the recombination zone. As long as light is emitted from well
within the channel, the external quantum efficiency 共EQE兲 of
ambipolar light-emitting transistors is expected to be con-
stant and should only depend on the singlet-triplet ratio, ra-
diative yield of formed excitons, and light outcoupling effi-
ciency irrespective of, for example, the ratio of hole to
electron mobility or voltage conditions.
In this paper, we test this assumption and investigate the
emission characteristics and EQEs of ambipolar LFETs in
bottom contact/top gate geometry, illustrated in Fig. 1共a兲,
based on two different conjugated polymers. One of them,

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064517-2 Zaumseil et al.
FIG. 1. 共a兲 Schematic device structure of a bottom contact/top gate transis-
tor with gold electrodes, PMMA as the gate dielectric, and F8BT or F8TBT
as the semiconducting layer on a glass substrate. 共b兲 Chemical structures and
photoluminescence spectra of F8BT 共left兲 and F8TBT 共right兲 thin films after
annealing.
poly共9,9-di-n-octylfluorene-alt-benzothiadiazole兲 共F8BT兲
关Fig. 1共b兲, left兴, is a green-emitting, semiconducting polymer
关emission wavelength of ⬃550 nm, photoluminescence 共PL兲
efficiency of ⬃54%兴,17 which we previously demonstrated to
exhibit efficient ambipolar transport and light emission in
FETs with balanced hole and electron mobilities on the order
of 共7 – 8兲 ⫻ 10−4 cm2 V−1 s−1.9 The other conjugated polymer
is poly共共9,9-dioctylfluorene兲-2,7-diyl-alt-关4,7-bis共3-hexyl-
thien-5-yl兲-2,1,3-benzothiadiazole兴-2⬘ , 2⬙-diyl兲 共F8TBT兲
关Fig. 1共b兲, right兴, which emits in the red 共emission wave-
length of ⬃670 nm, PL efficiency of ⬃34%兲. F8TBT can be
used both as the hole or as the electron transporting layer in
photovoltaic cells and also shows ambipolar transport and
light emission in bottom contact/top gate FETs.18 The hole
mobility in F8TBT transistors, however, is found to be an
order of magnitude higher than the electron mobility. In this
paper, we compare the emission characteristics and EQEs for
these two types of polymer LFETs and demonstrate their
fundamental similarity both experimentally and using an
analytical device model. We will show that the quantum ef-
ficiency 共QE兲 of these ambipolar LFETs increases with cur-
rent density before saturating at values consistent with com-
plete charge recombination and about 25% singlet excitons,
pointing toward a trap-assisted mechanism for nonradiative
recombination in these devices.
II. DEVICE PREPARATION AND EXPERIMENTAL
METHODS
The schematic device structure of bottom contact/top
gate LFETs is shown in Fig. 1共a兲. Low sodium glass 共Corn-
ing 1737F兲 served as the substrate on which interdigitated
gold electrodes 共thickness of 15– 30 nm兲 were photolitho-
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J. Appl. Phys. 103, 064517 共2008兲
graphically patterned by a standard two-layer liftoff process
共LOR 5B/Shipley 1813, MicroChem Corp.兲. Vapor treatment
with 共3-mercaptopropyl兲trimethoxysilane 共Aldrich兲 before
metal evaporation improved adhesion of the gold to the
glass. Spinning 8 – 10 mg ml−1 solutions of F8BT or F8TBT
in anhydrous m-xylene gave films of 50– 70 nm thickness.
Annealing at 290 ° C removed residual solvent and induced
polycrystallinity in F8BT films,17 while F8TBT films re-
mained amorphous. A 450– 520 nm thick poly共methyl meth-
acrylate兲 共PMMA兲 共M n = 350 kg mol−1, Polymer Source,
Inc., dielectric constant ␧PMMA = 3.6兲 gate dielectric was de-
posited by spin coating from an anhydrous n-butyl acetate
solution 共35– 40 mg ml−1兲. Shadowmask evaporation of
15 nm of gold as a semitransparent gate electrode completed
the devices.
All processing steps after liftoff as well as device char-
acterizations were carried out in a dry nitrogen glovebox
excluding oxygen and moisture. Current-voltage characteris-
tics of the fabricated transistors were measured using an Agi-
lent semiconductor parameter analyzer HP4155C. The ca-
pacitance Ci of the gate dielectric was determined for each
sample using a capacitor structure and a Hewlett–Packard
impedance analyzer HP4192A. Saturation field-effect mo-
bilities were extracted from the unipolar parts of the transfer
characteristics applying Ids sat
= 共WCi␮sat / 2L兲共Vg − VTh兲2 共W,
sat
channel width; L, channel length; Ids , source-drain current in
saturation; VTh threshold voltage; and ␮sat, saturation mobil-
ity兲 and assuming gate voltage independent mobilities. The
light output of LFETs was recorded with a silicon photodi-
ode 共Hamamatsu S1133-01, maximum dark current of 5 pA兲,
which was much larger than the device and placed in close
proximity to the device surface at a reverse bias of 4 V. For
calculations of EQEs, it was assumed that all photons emit-
ted from the surface 共that is, through the gold gate electrode兲
were collected by the photodiode, which gave a lower bound
for the total EQE..
PL spectra and efficiencies of annealed F8BT and
F8TBT thin films were measured at room temperature in a
nitrogen-purged integrating sphere with excitation from an
argon ion laser at 457 nm. PL efficiencies were calculated as
described by de Mello et al.19
III. RESULTS AND DISCUSSION
Typical transfer and output characteristics of an ambipo-
lar F8TBT transistor are displayed in Fig. 2. The transfer
characteristics 关Figs. 2共a兲 and 2共b兲兴 exhibit the characteristic
source-drain voltage dependence expected for ambipolar
FETs and are similar to those previously reported for ambi-
polar F8BT transistors.9 The significant difference between
the hole and electron mobilities is clearly reflected by the
asymmetry of the hole 共at low gate voltages兲 and electron 共at
high gate voltages兲 currents. The hole mobility 共5
⫻ 10−4 cm2 V−1 s−1兲 in saturation is about an order of mag-
nitude larger than the electron mobility 共3
⫻ 10−5 cm2 V−1 s−1兲. This large disparity of hole and electron
mobilities compared to F8BT can be rationalized when as-
suming that electrons are largely localized on the benzothia-
diazole 共BT兲 unit of the polymer chain, whereas holes are
064517-3 Zaumseil et al.
expected to be delocalized along the backbone. Such a dif-
ference between the electron and hole polaron wavefunctions
has been predicted by quantum chemical calculations on
F8BT,20 and a similar behavior is expected for F8TBT.21 The
distance between BT units in F8TBT is much larger than in
F8BT due to the additional thiophene units in the polymer
backbone. This increased hopping distance is likely to be
responsible for lowering the electron mobility in F8TBT sig-
nificantly, while in F8BT, the hopping distance for electrons
is sufficiently small so that electron and hole mobilities re-
main approximately balanced.
In our device configuration containing gold source-drain
electrodes, ambipolar F8TBT transistors exhibit high contact
resistance indicated by suppressed drain currents at low
source-drain voltages as seen in the output characteristics
关Fig. 2共c兲 and 2共d兲兴. The contact resistance for hole injection,
however, is notably lower than that of F8BT transistors 共see
Ref. 9兲. This is due to the smaller bandgap of F8TBT 共Egap
= 2.2 eV兲 共Ref. 18兲 compared to F8BT 共Egap = 2.6 eV兲 and
the improved alignment of the F8TBT highest occupied mo-
lecular orbital 共HOMO兲 level 共⬃5.4 eV兲 to the work func-
tion of the injecting gold electrodes 共␸Au ⬃ 4.8 eV兲 and, thus,
lower injection barrier compared to F8BT 共HOMO level of
⬃5.9 eV兲. The injection barrier for electrons into F8TBT is
only slightly lower, due to the more similar lowest unoccu-
pied MO levels of F8TBT 共3.15 eV兲 and F8BT 共3.3 eV兲.
Both F8BT and F8TBT ambipolar FETs show light
emission from within the channel region, as shown in Figs.
3共a兲 and 3共b兲. For both transistors, the position of the emis-
sion zone can be adjusted from close to the source electrode
through the entire channel to the drain electrode by changing
the applied gate or source-drain voltage as previously re-
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J. Appl. Phys. 103, 064517 共2008兲
FIG. 2. Current-voltage characteristics of an ambipolar
F8TBT transistor with L = 20 ␮m, W / L = 500, and Ci
= 7.1 nF cm−2. Transfer characteristics at different 共a兲
negative and 共b兲 positive source-drain voltages. Output
characteristics for gate voltages 共c兲 from 0 to − 80 V
and 共d兲 from 20 to 100 V in steps of 10 V. The hole
and electron mobilities at saturation for this device are
5 ⫻ 10−4 and 3 ⫻ 10−5 cm2 V−1 s−1, respectively.
ported for F8BT 共Ref. 9兲 and other ambipolar LFETs.7,8,11
Figure 3共c兲 shows the position of the emission zone and
source-drain current 共Ids兲 of a F8BT LFET during a transfer
scan with respect to the applied gate voltage and at constant
source-drain voltage. The symmetric form of the sigmoidal
position curve centered around the current minimum ob-
served in the transfer characteristics is expected for a device
with balanced hole and electron mobilities.10 Light-emitting
carbon nanotube FETs show an equivalent dependence of the
emission spot position on gate voltage.22 The shift of the
center point of the curve away from the ideal condition of
Vg = Vds / 2 is due to the somewhat different threshold volt-
ages for holes 共−29 V兲 and electrons 共25 V兲 and the reduced
effective Vds due to contact resistance. For the F8TBT LFET,
on the other hand, a very asymmetric position-versus-gate-
voltage curve is observed reflecting the disparity of mobili-
ties 关Fig. 3共d兲兴. Since electrons exhibit a lower mobility than
holes in F8TBT, a larger voltage drop across the electron
accumulation layer is needed to obtain an electron current
equivalent to the hole current. For equivalent voltage condi-
tions the electron channel must be shorter than in the case of
balanced mobilities. Hence, for a wide range of gate volt-
ages, the emission zone is located closer to the electron in-
jecting electrode, and only for a very narrow voltage range, it
remains closer to the hole injecting electrode 关Fig. 3共d兲兴.
Note that in both cases, there is a wide range of gate voltages
for which the emission zone is located away from the inject-
ing electrodes and, thus, complete recombination of holes
and electrons is expected. This notion is further supported by
the narrow shape of both emission zones. In the case of
F8BT LFETs, the width at half maximum is about 4 ␮m. The
intensity profile along the recombination zone shows a
064517-4 Zaumseil et al.
grainy texture reflecting the polycrystalline morphology of
the F8BT film. This polycrystalline texture also leads to
some broadening of the emission zone. In contrast, the amor-
phous F8TBT films shows a much narrower emission zone
with a width at half maximum of about 2 ␮m with no visible
asymmetry. The correlation of emission images and micro-
structure of the polymer films suggests that the linewidth
observed by optical microscopy reflects the true width of the
recombination zone and is not determined by limited reso-
lution of the microscope setup.
Figure 4 shows the current-voltage and corresponding
light output characteristics of F8BT and F8TBT LFETs to-
gether with their EQEs as a function of gate and source-drain
voltages. The EQE of the F8BT LFET reaches a plateau at
around 0.55% centered around the source-drain current mini-
mum for Vds = −100 V. However, at Vds = −80 V, the maxi-
mum efficiency is lower than that by almost 20%. The EQE,
thus, seems to increase with increasing Vds. Furthermore, for
Vds = −80 and −90 V, a dip in efficiency coincident with the
current minimum is evident where the emission zone should
be in the middle of the channel, as shown in Fig. 3共c兲.
A similar behavior of the external efficiency has been
described recently by Smits et al. for a bottom-gate near-
infrared light-emitting ambipolar FET based on a solution-
processable small-bandgap squarylium dye.10 This suggests
that this dependence is a common feature among ambipolar
LFETs irrespective of their geometry or organic semiconduc-
tor. A similar apparent increase of efficiency with source-
drain voltage can be found for F8TBT light-emitting transis-
tors 关Fig. 4共f兲兴. F8TBT transistors show generally lower QEs
compared to F8BT LFETs due to the lower PL efficiency of
F8TBT 共34%兲 and the maximum EQE is reached at 0.4%. In
contrast to the F8BT case, however, this maximum is not
centered around the current minimum but shifted toward
lower Vds and higher Ids. There is also no clear plateau of
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J. Appl. Phys. 103, 064517 共2008兲
FIG. 3. 共Color online兲 Optical images of light emission
from 共a兲 F8BT and 共b兲 F8TBT light-emitting FETs with
interdigitated source-drain electrodes 共dark areas兲 with
L = 20 ␮m. The emission zone of the F8BT LFET re-
flects the polycrystallinity of the polymer film, while
the emission from the amorphous F8TBT is featureless.
Position of emission zone with respect to source
共grounded兲 electrode and source-drain current vs gate
voltage during a transfer scan of an ambipolar 共c兲 F8BT
and 共d兲 F8TBT transistor with L = 20 ␮m.
efficiency but rather a peak that becomes broader as Vds in-
creases. From Fig. 3共d兲, one would expect the emission zone
of the F8TBT LFET to be located within the channel, away
from the electrodes, for a gate voltage range from about
50 to 80 V for Vds = 100 V. Thus, complete recombination of
holes and electrons should take place resulting in a constant
QE. However, clearly in Fig. 4共f兲, the efficiency is already
significantly lowered at about 65 V even before the drain
current reaches its minimum and, thus, before the emission
zone has reached the drain electrode. There is, however, a
kink in the efficiency curve at the gate voltage with the low-
est drain current and the emission efficiency decreases less
steeply from there. Notably, as the source-drain voltage in-
creases, the shape of the efficiency curve becomes broader
and seems to approach a plateau. While the maximum QE at
each Vds remains unchanged, the efficiency at higher gate
voltages increases with respect to the maximum value lead-
ing to a more plateaulike curve shape.
It is highly unlikely that a hole or electron can pass
through several micrometers of an accumulation layer of op-
posite charge without recombining, and the narrowness of
the emission zone supports the assertion that all charges are
recombining in a LFET with sufficient channel length. Thus,
as long as the emission is located within the channel, hole
and electron currents must be balanced irrespective of the
source-drain voltage or mobility ratio. Increased gate leakage
as a possible source of additional emission can be excluded.
The gate-source current in these LFETS is always two to
three orders of magnitude lower than the source-drain cur-
rent, and there is no correlation between gate leakage and
emission. The origin of the changing EQE must, therefore,
be due to a change of either outcoupling efficiency or radia-
tive yield. An effect of source-drain voltage on the outcou-
pling efficiency is unlikely as the lateral position of the emis-
sion zone is always far away from the source-drain
064517-5 Zaumseil et al. J. Appl. Phys. 103, 064517 共2008兲

FIG. 4. 共a兲 Source-drain current, 共b兲 light output, and 共c兲 external quantum efficiency vs gate voltage 共forward and reverse兲 of a light-emitting F8BT 共green兲
transistor with L = 20 ␮m, W / L = 500, Ci = 5.9 nF cm−2, ␮e = 5 ⫻ 10−4 cm2 V−1 s−1, ␮h = 6 ⫻ 10−4 cm2 V−1 s−1. 共d兲 Source-drain current, 共e兲 light output, and 共f兲
external quantum efficiency vs gate voltage 共forward and reverse兲 of a light-emitting F8TBT 共red兲 transistor with L = 20 ␮m, W / L = 1000, Ci = 6.8 nF cm−2,
␮e = 3 ⫻ 10−5 cm2 V−1 s−1, ␮h = 6 ⫻ 10−4 cm2 V−1 s−1.

electrodes and remains localized at the gate dielectric inter-
face excluding interference effects.23 A dependence of the
radiative yield on applied field and, thus, Vds could be pos-
sible at very high fields; however, no corresponding correla-
tion of efficiency with the channel length and, thus, field
could be found. The pronounced dip of efficiency for the
F8BT LFETs at lower Vds and the lowered efficiency at lower
drain currents in the case of F8TBT LFETs suggest that the
observed changes of EQE might be caused by different cur-
rent densities rather than source-drain voltage or lateral field.
Before looking more closely at a possible charge density
dependence of the QE, we will compare the experimental
device characteristics to a recently developed analytical
model for organic ambipolar LFETs.16,14,24 We calculated the
salient device characteristics using the gradual channel ap-
proximation based approach described in Ref. 16 and in-
cluded the effects of nonvanishing contact resistances. The
contact resistance values were chosen to be Re = 3
⫻ 106 ⍀ cm and Rh = 105 ⍀ cm for both F8BT and F8TBT
devices, reflecting the expected larger contact resistance for
electron injection compared to hole injection from the gold
contacts. Carrier density dependent and, hence, gate voltage
dependent, mobilities for electrons and holes were modeled
as in Refs. 16 and 14, with threshold 共VT,e and VT,h兲 and
slope 共Ve and Vh兲 parameters given by VT,e = 15 V, VT,h =
−20 V and Ve = 100 V, Vh = 200 V for F8BT, and by VT,e
= 20 V, VT,h = −20 V and Ve = 100 V, Vh = 100 V for F8TBT.
Saturation mobilities corresponded to the experimental satu-
ration mobilities 共Fig. 4兲, as did the other independently de-
termined device parameters, i.e., gate-channel capacitances
and channel lengths and widths. With the “source” grounded,
the source is the electron injecting contact 共large contact re-
sistance兲 and the drain injects holes for positive drain and
gate biases, while negative drain and gate biases imply that
the source is the hole injecting contact 共smaller contact re-
sistance兲 and the drain injects electrons.
First, we explore the dependence of the recombination
position as a function of gate voltage for fixed Vds in com-
parison with the experimental data in Figs. 3共c兲 and 3共d兲.
Figures 5共a兲 and 5共b兲 show results for F8BT and F8TBT
devices with Vds = 100 and −120 V, respectively. Evidently,
the model reproduces well the qualitative differences in the
shapes of these curves that are directly attributable to the
significantly different electron and hole mobility ratios of the
two materials as described above.
Next we examine the drain current, light output, and QE
results for the two different devices. For both F8BT and
F8TBT devices, the calculated transfer curves shown in Figs.
6共a兲 and 6共d兲 are in satisfactory agreement with the measured
data 关Figs. 4共a兲 and 4共d兲兴. Qualitative differences, i.e., the

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064517-6 Zaumseil et al.
FIG. 5. Calculated source-drain current and position of recombination zone
vs Vg at constant Vds for ambipolar transistors with 共a兲 F8BT 共␮h / ␮e = 1.2,
Vds = 100 V兲 and 共b兲 F8TBT 共␮h / ␮e = 20, Vds = −120 V兲 as in Fig. 3.
FIG. 6. 共a兲 Calculated source-drain current, 共b兲 light output, and 共c兲 quantum efficiency vs gate voltage of a light-emitting F8BT 共green兲 transistor with
balanced hole and electron mobilities 共␮h / ␮e = 1.2兲. 共d兲 Calculated source-drain current, 共e兲 light output, and 共f兲 quantum efficiency vs gate voltage of a
light-emitting F8TBT 共red兲 transistor with unbalanced hole and electron mobilities 共␮h / ␮e = 20兲.
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J. Appl. Phys. 103, 064517 共2008兲
strong asymmetry of the F8TBT transfer curves compared
with those of the F8BT device, can be traced back to the very
different electron/hole mobility ratios.
In order to reproduce the light output and QE character-
istics, we extended the model by evaluating the total recom-
bination rate and QE. This was done by integrating the spa-
tial recombination profile between the source and drain
contacts, suppressing emission from regions very close to the
contacts 共about 1 / 50th of the channel length兲 to account for
the low probability of radiative recombination in close prox-
imity of the metal contacts. The integrated recombination
probability, which is assumed to be proportional to the light
output, is plotted in Figs. 6共b兲 and 6共e兲. The model repro-
duces well the overall 共twin peak兲 shape of the experimental
curves 关Figs. 4共b兲 and 4共e兲兴. In the case of the F8TBT device,
the high-voltage peak is largely suppressed because the cur-
rent in that voltage range is electron dominated and, due to
the low electron mobility, significantly smaller than the cur-
rent in the hole-dominated low-voltage range. Finally, Figs.
6共c兲 and 6共f兲 show the calculated QEs as a function of the
gate voltage. The calculated QEs, in agreement with the
measured data, display less structure than the light output
versus gate voltage curves. In particular, the strong asymme-
try of the light output results is not found in the QEs of the
F8TBT device because the effect of the lower electron mo-
bility is largely cancelled out in the QE. The present model is
limited to a single 共Langevin兲 recombination mechanism,
which is interpreted as a radiative process and leads to a
constant efficiency 共that is, a flat efficiency plateau兲 for both
064517-7 Zaumseil et al.
F8BT and F8TBT in contrast to the experimental efficiency
curves. Competing mechanisms, possibly with different car-
rier density dependencies,25 may reduce the internal QE. The
slopes of the calculated total recombination rate and QE
curves are steeper than those of the experimental results for
light output and EQE. We attribute this difference primarily
to the width of the calculated recombination profile
共⬃0.5 ␮m兲, which is significantly narrower than the experi-
mentally observed width of the light emission zone here
共2 – 4 ␮m兲 and in other LFETs.26 The width of the calculated
recombination profile is underestimated in the present model,
primarily because the use of the gradual channel approxima-
tion throughout the recombination region neglects the carrier
spreading away from the semiconductor/insulator interface
and the associated lowering of the longitudinal electric field
in that region.
Evidently, device models that include only a single 共ra-
diative兲 recombination mechanism cannot reproduce the in-
crease of QE with Vds and the dip of efficiency at the plateau
demonstrated in Figs. 4共c兲 and 4共f兲, which again suggests
that other charge density dependent recombination processes
could play a role. In order to deconvolute the influences of
Vds and source-drain current on QE in LFETs, we performed
constant current measurements on both types of polymer
transistors. For these measurements, the source-drain current
was kept constant while sweeping the gate voltage, adjusting
the source-drain voltage accordingly and recording the emit-
ted light. Figure 7 shows the corresponding Vds 关共a兲 and 共c兲兴
and light output 关共b兲 and 共d兲兴 versus Vg characteristics of a
F8BT and F8TBT LFET.
During a gate voltage sweep with constant source-drain
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J. Appl. Phys. 103, 064517 共2008兲
FIG. 7. Constant current measurements of LFETs in
Fig. 4: 共a兲 Source-drain voltage and 共b兲 light output vs
gate voltage for various fixed negative source-drain cur-
rents of a F8BT-LFET. 共c兲 Source-drain voltage and 共d兲
light output vs gate voltage for various fixed positive
source-drain currents of a F8TBT-LFET. The voltage
range for which a plateau of the light output is observed
corresponds to the emission zone moving away from
the source electrode through the channel before reach-
ing the opposite drain electrode.
current, the emission zone is again moved through the entire
channel; for a certain gate voltage range, the emission zone
must be located within the channel away from either elec-
trode and complete charge recombination should take place.
For both polymer transistors, this regime is indicated by a
nearly constant maximum light output and, hence, QE 关pla-
teau region in Figs. 7共b兲 and 7共d兲兴. For values of Vg at the
edges of the plateau 共corresponding to lower and higher Vg兲,
the efficiency is reduced as the emission zone is located next
to the source or drain electrode resulting in incomplete re-
combination and/or luminescence quenching by energy
transfer. At the plateau, the light output is nearly constant for
a range of Vg and Vds, as shown in Figs. 7共b兲 and 7共d兲, unlike
in the transfer curves of Figs. 4共c兲 and 4共f兲. For example,
while in Fig. 4共c兲, a change of Vds from −80 to − 100 V
causes an increase of QE of about 20%, in Fig. 7共b兲, the light
output and, hence, the QE for a constant source-drain current
of 500 nA remains unchanged for source-drain voltages be-
tween 80 and 100 V. This suggests again that Vds is not
directly responsible for the increasing QE in Figs. 4共c兲 and
4共f兲 but rather indirectly through increasing the current den-
sity.
From these constant current measurements, one can ex-
tract the light output and QE for a range of source-drain
currents encompassing more than two orders of magnitude
from 20 nA cm−1 up to 8 ␮A cm−1, as shown in Fig. 8共a兲 for
F8BT and from 20 nA cm−1 up to 1.5 ␮A cm−1 in Fig. 8共b兲
for F8TBT. In Fig. 8, the source-drain current was normal-
ized against channel width in order to be able to compare
devices with different W / L ratios and give a measure of cur-
rent density. The QE of both types of LFETs initially in-
064517-8 Zaumseil et al.
FIG. 8. Light output 共squares兲 and external quantum efficiency 共triangles兲 vs
channel-width-normalized source-drain current of 共a兲 F8BT 共W = 1 cm兲 and
共b兲 F8TBT 共W = 2 cm兲 transistors. Data points were extracted from plateau
part of light output vs Vg of constant current measurements, as shown in Fig.
7.
creases strongly with increasing source-drain current and
then starts to saturate approaching a constant efficiency at
source-drain currents exceeding 1.5 ␮A cm−1.
The maximum EQE of F8BT LFET at high source-drain
currents is about 共0.8⫾ 0.1兲%. In order to estimate the light
outcoupling efficiency for our LFETs, we carried out optical
modeling of the multilayer structure of glass/F8BT/
PMMA/Au with light collected above the gold electrode as
follows. The power loss spectrum P共k储 , ␭ , ␪ , d兲 of a single
dipole source with fixed free space wavelength ␭, orientation
␪, and position d within a multilayer structure is calculated
using a scattering matrix approach to solving Maxwell’s
equations.27 Couplings to surface emission modes, substrate
guided modes, surface plasmon-polariton modes, and lossy
surface waves28 are all included in this treatment. Intrinsic
nonradiative losses of the material are estimated from the PL
efficiency of thin films and included in the calculation as
described by Lu and Sturm29 The outcoupling efficiency is
obtained by calculating the ratio of the power lost to the
surface emission modes to the total loss rate. This calculation
is weighted over a realistic distribution of dipole positions,
orientations, and emission wavelengths. The distribution of
dipole positions 共or exciton formation zone profile兲 is taken
as an exponentially decaying function peaking at the F8BT-
PMMA interface with decay width of 15 nm. The average
dipole orientation 共x , y , z兲 = 共0.44, 0.44, 0.11兲 is estimated
from the ratio of in-plane to out of plane extinction coeffi-
cients obtained from spectroscopic ellipsometry 共kz / kx
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J. Appl. Phys. 103, 064517 共2008兲
FIG. 9. 共a兲 Experimental 共open circles兲 and modeled 共lines兲 transmission
spectra of a multilayer stack of glass/F8BT 共60 nm兲/PMMA 共420 nm兲/gold
with different modeled thicknesses of gold 共13 nm, dashed line; 15 nm,
solid line; and 17 nm, dash-dot line兲. Calculated external quantum efficien-
cies based on the multilayer stack in 共a兲 for different thicknesses of 共b兲
F8BT, 共c兲 PMMA, and 共d兲 gold assuming 55% PL efficiency, 25% singlet
exciton fraction, and an emitting dipole orientation of kz / kx = 0.25.
= 0.25兲.30,31 The emission wavelength distribution is esti-
mated from the PL spectrum of a F8BT film on quartz.
Figure 9共a兲 shows experimental and simulated transmis-
sion spectra of the multilayer optical structure for different
thicknesses of the gold gate electrode. The model is found to
reproduce the experimental transmission spectrum well and
is, therefore, expected to allow accurate calculation of out-
coupling efficiencies and expected EQEs depending on the
thicknesses of F8BT, PMMA, and Au, as shown in Figs.
9共b兲–9共d兲. The EQE is obtained by multiplying the outcou-
pling efficiency by the singlet yield, estimated here to be
25%. We find that an experimental EQE of 0.8% is well
within the range of the expected values. The thicknesses of
F8BT and PMMA affect this value only slightly. Both the
outcoupling efficiency and the absolute transmittance are
shown to be the most sensitive to the gold thickness, as
might be expected. The best fit is obtained for 15 nm gold,
suggesting an EQE of ⬃0.75%. We note that due to the
complete recombination of charges in ambipolar LFETs, they
could be used to determine the singlet-triplet ratio of organic
electroluminescent materials, which has been a matter of de-
bate for some time.32 Our results here are consistent with at
least 25% singlets being formed in F8BT. More detailed ef-
ficiency measurements and optical modeling will be needed
to give a more reliable estimate. The optical modeling shows
that the experimentally measured EQE of 0.8% is evidence
of very efficient LFET operation. What might at first appears
to be a low EQE value is, in fact, entirely due to the chosen
detection geometry because only relatively little light is out-
coupled through the gate electrode.
Based on the observed dependence of QE on Ids in Fig.
064517-9 Zaumseil et al.
8, we can now easily explain the observed variations of ef-
ficiency shown in Fig. 4. The source-drain current for which
the emission zone is located within the transistor channel
increases with Vds, explaining the concomitant increase in
EQE. As experimentally observed at very high Vds, the effi-
ciency increases less with Vds than at lower values because it
starts to saturate at higher currents. Likewise, when the
source-drain current reaches its minimum during a transfer
scan 关for example, −230 nA for Vds = −80 V in Fig. 4共a兲兴, the
efficiency goes down as well, causing the dip in the effi-
ciency plateau 关Fig. 4共c兲兴. When the source-drain voltage is
increased to −100 V and, thus, the minimum source-drain
current increases to about −1 ␮A, this dip becomes less pro-
nounced because EQE already approaches saturation.
In this way, the asymmetric efficiency plots for the
F8TBT transistors become comprehensible as well. Because
the electron mobility is so much lower than the hole mobil-
ity, the source-drain currents at high Vg in Fig. 4共d兲 are much
lower than at lower Vg, which leads to a lower light output
but also lower QE at this point despite total charge recombi-
nation. The maximum QE of 0.4% for the F8TBT LFET in
Fig. 4共f兲 is achieved for source-drain currents of about
8 – 10 ␮A 共that is, 4 – 5 ␮A cm−1兲 and is almost independent
of source-drain voltage. As the source-drain current increases
with increasing source-drain voltage in Fig. 4共f兲, the QE also
starts to approach this maximum value in the high Vg region
leading to a more plateaulike efficiency curve shape.
This behavior is reminiscent of the increasing QE of
polymer LEDs at low forward bias and, thus, current
densities.33 This increase of efficiency in single layer poly-
mer LEDs, however, was explained with nonradiative recom-
bination losses when the emission is predominantly located
next to the metal cathode at low biases.34 This effect can be
ruled out for ambipolar light-emitting transistors where emis-
sion takes place far away from the source-drain electrodes.
The distance of 400– 500 nm to the gate electrode given by
the thickness of the gate dielectric excludes emission
quenching by energy transfer to the metal. However, light
emission in a LFET is anticipated to predominantly take
place close to the interface between the gate dielectric and
the emitting polymer. Nonradiative recombination processes
at this interface could, thus, play a large role.
Hsieh et al. investigated the influence of nonradiative
recombination processes on the QE of light-emitting carbon
nanotube transistors and found that a trap-assisted Shockley–
Read–Hall-type nonradiative recombination mechanism
would lead to an increase of efficiency with current density.25
A similar process could be responsible for the increasing QE
in polymer LFETs. If a charge is trapped at the interface or at
a defect in the bulk of the emitting polymer, recombination
with an opposite charge is likely to be nonradiative assuming
that a charged trap is also a luminescence quenching site. As
the source-drain current increases the number of defects at
the interface, or in the bulk, thus, the fraction of nonradiative
recombination events become less significant compared to
the number of radiative recombination events between mo-
bile charge carriers resulting in increased QE. The exact na-
ture of such traps, however, remains unclear. The relatively
large threshold voltages for both hole and electron transport
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J. Appl. Phys. 103, 064517 共2008兲
in F8BT and F8TBT as well as the hysteresis of the current-
voltage characteristics in Figs. 2 and 4 indicate that there is a
significant number of charge traps present at the interface.
Whether those charge traps or other chemical or structural
defects of the polymer chains at the interface are responsible
for non-radiative recombinations remains to be investigated,
for example, by means of temperature-dependent QE mea-
surements. The fact that there is always a perfect balance
between holes and electrons and a known position of the
recombination zone within the devices will be helpful to
study the nature of this nonradiative recombination process.
In order to compare the observed QEs of F8BT and
F8TBT LFETs and their dependence on the source-drain cur-
rent to those of other LFETs and polymer LEDs, one needs
to determine the current density within the emission zone.
Calculating the actual current density in a light-emitting tran-
sistor is not straightforward. It is not known how much holes
and electrons remain confined to the interface within the re-
combination zone compared to their respective accumulation
regions 共within about 1 – 2 nm of the interface35兲 or how
much they spread out away from the interface and, if so, how
this depends on voltage conditions. Nevertheless, it is helpful
to estimate a lower and an upper limit for the current density
in light-emitting transistors taking into account the current
flow through an area that is defined by the channel width and
the height of the emission zone. For a normalized source-
drain current of 1 ␮A cm−1, the corresponding upper limit is
10 A cm−2 共assuming all charges are confined to within 1 nm
at the active interface兲, while the lower limit of current den-
sity is calculated to be 0.2– 0.14 A cm−2 using the thickness
of the polymer film 共50– 70 nm兲. However, this calculation
does not yet take into account the finite width of the emission
zone in LFETs 共2 – 4 ␮m兲, which indicates that charge re-
combination is less spatially confined in a LFET than in a
polymer LED,15,16 and that the exciton concentration within
the recombination zone of the LFET is not as high as indi-
cated by the calculated current densities. Therefore, one
could expect the QE to be noticeably affected by a fixed
number of quenching sites as described above and, thus, to
increase with increasing source-drain current. Higher current
densities at which such a quenching mechanism ceases to be
predominant are possible in LFETs with shorter channel
lengths and thinner gate dielectrics. The upper limits of QE
in polymer LFETs, peak brightness, and possible quenching
mechanisms at high current densities are currently under in-
vestigation.
IV. CONCLUSIONS
We have demonstrated experimentally and using an ana-
lytical device model that ambipolar LFETs based on two
conjugated polymers with either balanced 共F8BT兲 or strongly
unbalanced 共F8TBT兲 hole and electron mobilities show fun-
damentally the same emission characteristics. The emission
zone of both transistor types can be moved through the chan-
nel by changing the applied gate voltage, thus, adjusting the
point at which recombination of charge carriers takes place.
Balanced hole and electron mobilities are not necessary for
achieving a well-controlled ambipolar regime in organic
064517-10 Zaumseil et al. J. Appl. Phys. 103, 064517 共2008兲

9
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Adv. Mater. 共Weinheim, Ger.兲 18, 2708 共2006兲.
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ACKNOWLEDGMENTS 23
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The authors thank Cambridge Display Technologies Ltd. P. P. Ruden and D. L. Smith, Organic Thin-Film Electronics—Materials,
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