surface science

ELSEVIER Applied Surface Science 92 (1996) 589-597

Electroluminescence in thin films

Reiner H. M a u c h *
Heinrich-Hertz-lnstitut fiir Nachrichtentechnik Berlin GmbH, AG Elektrolumineszenz, Hausvogteiplatz 5-7, D-10117 Berlin, Germany
Received 12 December 1994; accepted for publication 4 March 1995

Abstract

The three most important technologies for future display applications where electroluminescence (EL) in thin films is
used for light generation are discussed. These technologies are firstly, Alq- and PPV-based organic light emitting diodes
(LED); secondly, inorganic a-SiC LED and thirdly, at-driven thin film electroluminescent devices based on II-VI
compounds. The last of these is of the high-field EL-type whereas the first two utilise low-field injection type EL. The basic
principles and the current status of the respective technologies are summarised. Recent developments in ac thin film
electroluminescence for full colour display applications are emphasised.

1. Introduction must be formed, whereas in high-field EL a thin film

Electroluminescence in solids can be generated by
one of two basically different physical principles. In
the injection type electroluminescence (EL) like that
occurring in light emitting diodes (LED), electrons
and holes are injected by low electrical fields into n-
and p-type doped regions. In the simplest situation,
direct band to band recombination of the carders
near the p - n junction generates the emission. By
contrast, in high-field EL electrons are accelerated in
electrical fields as high as 2 M V / c m gaining enough
energy to impact excite impurities. In the first case,
the bandgap of the host material determines the
emission spectrum; in the second, the impurities
which act as luminescent centres determine the spec-
tral distribution. A further difference is found in the
device structure. In typical LEDs a p - n junction
* Tel.: +49 30 20377326; fax: +49 30 20377405; e-mail:
mauch@hhi.de.
MISIM structure in which the light emitting layer (S)
is embedded between insulator (I) and metal (M) is
utilised. For practical use as high information con-
taining displays, in particular for high-resolution flat
panel displays, only high-field inorganic thin film EL
is used at present since classical III-V LEDs are
based on expensive single crystalline material. Such
LEDs are only found in low-resolution, low informa-
tion containing, small screen or low-resolution, very
large screen displays.
Recently, two new classes of thin film injection
type EL devices have been introduced. One is based
on a thin film p - i - n LED structure made from
a-SiC. The other utilises various organic materials.
Both have attracted attention because of improved
luminance and efficiency of as-fabricated devices.
However, the main problem which hinders rapid
application is the limited stability under operation
conditions.
Hence, this paper shall emphasise products using
inorganic high-field EL for high-resolution mono-

0169-4332//96/$15.00 © 1996 Elsevier Science B.V. All fights reserved

SSD! 01 6 9 - 4 3 3 2 ( 9 5 ) 0 0 3 0 1 - 0
590 R.H. Mauch / Applied Surface Science 92 (1996) 589-597
chrome and full colour displays. The other types of
thin film EL devices will be described briefly.
2. Organic electroluminescence
Organic electroluminescence is a low-field injec-
tion type EL utilising a structure similar to that in
inorganic light emitting diodes. The advantage of
organic EL among all other types of solid state light
emitters lies in the possibility of realising low-volt-
age devices on large areas deposited at room temper-
ature. Even low-cost flexible substrates can be used.
Furthermore, is has been demonstrated that structur-
ing in the submicron range is possible in such de-
vices. Many papers about this class of devices have
been published in the last few years. In this paper we
shall only summarise a few important issues.
The invention of the double-layer organic EL
structure by Tang and Van Slyke [1] initiated a new
age of organic based EL research. The novel EL
device consisted of a light emission layer (EML) of
8-quinolinol aluminum complex (Alq) and a hole
transporting layer (HTL). Higher luminance, higher
efficiency and lower drive voltage than those en-
countered in earlier devices were obtained with this
structure. Since that time, many investigations on
organic type EL have been conducted. They have led
to a variety of experimental structures. In Fig. 1, the
three major types are displayed. As shown in this
figure, even three or more layers are currently used
to improve transport and luminescent properties.
In structure (a), an electron transport layer (ETL)
is used in conjunction with the emission layer (EML)
whereas in structure (b) a hole transport layer (HTL)
acts as the emission layer. Finally, in (c) the emis-
sion takes place neither in the ETL nor in the HTL
but in a dedicated emission layer. In all cases ITO is
used as the transparent contact and a MgAg elec-
I
Ill Jim
I I irro
~w J
U~Ao
El'l.
tro
Fig. 1. Typical organic EL device structures [2].
trode as the low work function metal electrode for
electron injection. Typical device thicknesses are
about 200 nm implying that the thicknesses of the
single layers are only around 50 rim. Therefore,
vacuum deposition techniques are necessary to con-
trol the film growth. Usually, even UHV deposition
is used in order to avoid contamination of the layers.
Both, doped and undoped Alq and 9,10-bis-styry-
lanthracene derivatives (BSAs) have been applied as
efficient light emission layers [2,3]. These materials
make it possible to produce EL emission over a
broad range of the visible spectrum. However, emis-
sion with the high colour purity required in display
applications is difficult to obtain.
Very recently, an efficiency level of 7.4%, the
highest observed so far, has been reported by Waki-
moto et al. [4]. Despite the fact that such excellent
initial performance was realised with this type of
organic EL device, it turned out that stability is the
major problem for practical applications. For exam-
ple, the high-efficiency device described above driven
at an initial luminance of 300 c d / m 2 reached 150
c d / m 2 at end of life; i.e., after 400 h aging in
vacuum. However, some progress has been reported
by Tang et al. [5]. They found that the degradation is
strongly dependent on the current flow through the
device. If the device is driven at higher currents than
l0 m A / c m 2 even perfect sealing or aging in vacuum
result in lifetimes below 1000 h, whereas lower
currents increase the device lifetime to more than
5000 h.
Since 1990 a new class of organic EL materials
based on conjugated polymers (polypropylenviny-
lene: PPV) is under investigations. The first report
by Burroughes et al. [6] was the starting point of
significant research activities. A major advantage of
this type of organic EL is that in principle cheap
deposition techniques can be used to form the exper-
imental structure. Even the doctor plate technique
results in reasonable devices [7]. Either a simple heat
treatment in vacuum or an UV treatment causes the
formation of the conjugated polymer. The experi-
mental structures under investigations are compara-
ble to those displayed in Fig. 1. Also other similari-
ties are found.
For instance, as is found for other types of or-
ganic EL almost all emission colours can be ob-
tained, in this instance by chemical modification of
 R.H. Mauch / Applied Surface Science 92 (1996) 589-597
fjAL
--.
- - ~ ~-sic
I:~-':':I - - p a-SiC
g,o- . ". " ¢ ( . C - " '," rro/ o
Fig. 2. Schematic structure of a p - i - n - T F L E D based on a-SiC:H
[12l.
the PPV material [8-10]. The most recent work
resulted in a quantum efficiency of 4% for PPV-based
EL as reported by Bradley [11]. Since only rare data
on the stability of PPV devices are available it has
not been possible to foresee whether these films will
be useful.
3. Inorganic electroluminescence
3.1. a-SiC light emitting diodes
Amorphous silicon carbide a-SiC can be fabri-
cated with bandgaps from 1.7 to 3 eV by adjusting
the deposition parameters, in particular, the ratio of
Si and C precursors during the glow discharge depo-
sition process. This property enables the fabrication
of p-i-n-type thin film light emitting diodes
(TFLED) with various emission coiours if an experi-
mental structure as shown in Fig. 2 [12] is used.
Even blue emitting TFLEDs have been fabricated by
utilising a hydrogenated amorphous carbon [13].
Under forward bias, electrons and holes are in-
jected from the n- or p-type a-SiC, respectively, into
the i layer where they recombine. The emission can
be enhanced by introducing quantum well structures
for improved electron injection or to obtain a con-
finement in the i layer [14].
Although attractive properties are expected for
this type of devices, very little data on stability have
been published so far. Hence, it is not clear whether
this approach is a promising candidate for future
display applications.
591
3.2. Ac thin film EL
Ac-driven high-field thin film electroluminescent
1300 (TFEL) displays based on inorganic light emitting
layers have reached a general acceptance in demand-
(250-1000~
o
ing display applications where excellent performance
(150A) is required. It is believed that this type of display
could be the ultimate flat panel display because of its
all solid state structure which is an advantage over
all competing technologies. This strong feature is
accompanied by a robust construction, a wide opera-
tion temperature range, wide viewing angle, high
contrast ratio, video capability and high lifetime.
Additionally, the possibility of variable pixel sizes is
another major advantage of this technology. The
pixel resolution can range from a few /xm up to
several mm covering different display demands.
Moreover, thanks to thin film technology almost all
screen diagonals from a few inches up to TV or
HDTV screen sizes are possible. During the past
several years, ac-driven monochrome TFEL displays
based on a yellow emitting ZnS:Mn phosphor layer
have increased their market share steadily. However,
to open new markets for TFEL technology a pre-
requisite is full colour capability.
Hence, the research and development activities
nowadays are mainly concentrated on the realisation
of multi and full colour displays. Furthermore, while
ZnS:Mn can play only a limited role in full colour
displays, new light emitting materials and new mate-
rial combinations as well as new device structures
are under investigation.
Presently, alkaline earth sulphides and alkaline
earth thiogallates as SrS and (Sr,Ca)Ga2S 4 are very
promising candidates. One reason is the high solubil-
ity for rare earth doping. Doping with rare earth ions
makes it possible to cover the whole visible spec-
trum. In particular, doping with Ce results in an
efficient blue TFEL emitter.
We shall first introduce the basic principle of the
high-field EL mechanisms exemplified in the case of
ZnS:Mn. Afterwards, recent achievements in devel-
oping new phosphor materials will be discussed.
Emphasis will be given to the state of the art of both
major display concepts.
3.2.1. Basic principles
Despite the fact that more than 20 years have
passed since the invention of thin film based electro-
592 R.H. Mauch /Applied Surface Science 92 (1996) 589-597

o. 100-200V
metal electrode ~ . . . ~ • insulatorl phosphor layer insula~ electrode
insulator ~ 5 0 0 n r n ~ . : : : ' : : - ' : ' - ' t i
I
phosphor layer luminescent
centre
insulator ~ 3 0 0 n r ~ ~ ; . : : . - ' : : ' : ~
l f f f .l
transparent~,-
-fi$--
~,,~,~o o *gioss,~

light cathode
Fig. 3. Experimental structureof a TFEL device after Inoguchi
[]9].

Fig. 4. Simplified band structure of a TFEL device under opera-

luminescence, research on the physics of such kind tion.
of devices continues, which show, that a conclusive
model is still not available [15-18]. However, as a
basics for understanding the phenomenon, a crude Some parameters are decisive for high performing
model for the light production is discussed below. EL devices: The host material should allow high-field
The typical device structure proposed by Inoguchi conduction, the dopant should fit into the lattice of
et al. [19] is displayed in Fig. 3. The whole device the host material without severe distortion (high
consists of five sequentially deposited layers. The solubility); the cross section for impact excitation of
light emitting phosphor layer is embedded between the dopant (luminescent centre) should be large; the
two insulators and two electrodes where one of the emission spectrum of the luminescent centre has to
electrodes is transparent. Because of this structure, be located in the visible. In addition, the luminescent
the device is highly symmetrical and is of a capaci- centres must be stable in the high-field environment
tive nature. Therefore, the device requires an alter- associated with the EL phenomenon. Hence, donor-
nating driving voltage. If the external voltage is acceptor centres which are efficiently used in
below a certain value, the so-called threshold voltage cathodoluminescent phosphors are usually not useful
Vth, the device behaves like a capacitive divider in high-field EL. It turns out, that in particular II-VI
where the voltage is split according to the capaci- compounds doped with some transition metals or
tances of the insulators and the phosphor layer. rare earth ions satisfy these basic requirements best.
Voltage levels exceeding Vth result in a high-field The classical EL phosphor material is ZnS:Mn which
conduction of the phosphor layer (typically F > 1
MV/cm) accompanied by the onset of the light
emission. A simplified hand diagram sketched for 10 3
this case is shown in Fig. 4. Electrons which are able /
/
to move in this high fields can originate either at the 2
10
interface between the insulating and the phosphor
layers or from bulk states. These electrons are accel- E
1 1 v
erated in the electrical field and gain enough energy 10 10
8
r,- O
¢-
to impact excite luminescent centres which are incor-
porated into the host with doping levels below 1 at%. _= 10
0 100~
The electrons move further to the opposite interface
threshold
where they build up a polarisation field. When the
next pulse of the excitation voltage is applied, the 10"1 i ~ I I 10 -1
same process occurs but in the opposite direction. 100 200 3oo
The described mechanism leads to a typical lumi- voltage (V)
nance and efficiency versus voltage characteristic as Fig. 5. Typical luminance and efficiency versus voltage character-
shown in Fig. 5. istics of an ac-TFEL device.
 R.H. Mauch/ Applied Surface Science 92 (1996)589-597 593

HIGH LUMINANCE

Lumi. : 200 cd/rnZt

J
/

Power 11 W |
Pixel 640x480 J
Pitch 0.33x0.33J
i
LOW POWER J LARGE SIZE
/

i II Pix=l (199o)
: 640x480
lI : ,7 inch
Power : 6W J LumL : 100 cd/m21 J Pixel : 640x480 I
LumL I00 ¢d/m 2 = Power : 18 W ] >l LumL : 170 =d/m2I
eixel 640x480 I
I
Pitch : o.~3x0.33 I
Groy'sco!a : 16 J ioo i
,l
Pixel : 1280x1024
Pitch : 0.2x0.2
Size : 13 inch

HIGH RESOLUTION
Fig. 6. Recent progress of commercial monochrome EL displays [20].
allows efficient electroluminescence with luminous
efficiencies as high as 8 lm/W. As already men-
tioned, for full colour applications new phosphor
materials as SrS:Ce and (Ca,Sr)GazS4:Ce are under
investigation.
3.2.2. Monochrome thin film EL
One of the major advantage of TFEL displays is
that no active thin film transistor matrix is required.
The pixel is simply defined by the crossing area of
the rectangular patterned top and bottom electrodes.
Hence, the technology leads to a high production
yield, large display sizes and low power consump-
tion. This is demonstrated by the recent progress of
commercial ZnS:Mn-based monochrome EL (Fig. 6).
As a basis for comparison a standard display product
of 1990 is used. Various developments towards high
luminance, high resolution, low power and finally
large sizes have been summarised by Mikami [20].

Viewing Direction

L I
Electrodes _ _ ~ ITO -- ,- r
Electrodes
Insulator
RGB White __ J
Phosphors Phosphor
Insulator
Metal __
Electr°de~ -''~(-~,(-'~ J / J
Subslrafe I ~ "~"

v iewing TDirection
Fig. 7. Structured and "colour by white" display approach.
594

still remarkable improvements can be obtained in

monochrome EL, in particular, by optimising the
driving electronics.
t::

•~ 50
I00~
R.H. Mauch/ Applied Surface Science92 (1996)589-597

Although the ZnS:Mn material properties are well

understood and the thin film processes are optimised

3.2.3. Full colour thin film EL ~ o

In contrast to the monochrome case where the 370 442 514 586 658
greatest gain in performance can be achieved by Wavelength (nm)
adjusting the electronics, full colour EL requires new
Fig. 8. Emissionspectraof the CaGa2S4:CeEL device[25].
phosphor materials which need to be optimised, es-
pecially, in terms of stoichiometry and crystallinity
[21-24].
display, a double substrate solution has been intro-
Besides the new materials, different display struc-
duced by Planar America. The red and green pixels
tures and display concepts are also subject of the
are fabricated on the first transparent substrate
present investigation. The two concepts displayed in
whereas on the second substrate the whole pitch area
Fig. 7 turn out to be the most promising for future
is used for the blue pixel. This solution gives rise to
full colour TFEL displays. The first is the classical
luminance gain simply by geometry but also by
approach of structured phosphor layers where the
driving the blue display at higher frequencies [25].
three primary colours are achieved by three dedi-
Recently, the production of the first full colour EL
cated phosphor materials. A more recent idea is the
panel was announced for sale in 1995 by Planar
so-called "colour by white" concept, where the
America [27]. This 5" display will have 320 X 256
active layer is a broad band white emitter. The
colour pitches and is able to provide an areal white
different colours are substractively generated by re-
luminance of 30 c d / m 2.
spective colour filters. While structured phosphor
"Colour by white" EL display. For a number of
devices are characterised by high luminance levels
years alkaline earth sulphides (AES) like SrS and
the advantages of the latter solution are found in
CaS have been under investigation because of their
production, since in addition to a standard
cation radii are a good fit to the rare earth ions. If the
monochrome process only the colour filter matrix
"colour by white" concept is considered, SrS:Ce is
has to be developed. Both options show promise of
the most promising material because of its broad
realising high-quality information displays in the near
emission band in the blue-green. However, for a long
future. time the reported luminance and efficiency data were
Structured phosphor EL display. The basis for the
not high enough for application. Several reasons for
realisation of this type of display was the develop-
the substandard performance have been identified.
ment of an active layer is emitting in the deep blue.
First the purity of the material which is used for the
It has been demonstrated by Planar Systems, that
thin film deposition is low ( ~ 99.9%) compared to
Ce-doped Ca- and Sr-thiogallates are able to satisfy
typical semiconductor high-purity precursors. Sec-
these requirements. The researchers from Planar
America were also able to demonstrate a full colour
VGA-EL panel at the SID'93 conference [25].
Table 1
In Fig. 8 a typical spectrum of a CaGa2S4:Ce Luminancelevelsfor the structuredphosphorEL display [25]
TFEL device is shown. The corresponding CIE coor- Colour Material Luminance CIE coordinates
dinates are x = 0.15; y = 0.19. The replacement of at 60 Hz 60 Hz (cd/m 2)
Ca by Sr leads to a further shift into the blue (cd/m2) x y
resulting in coordinates x = 0.1; y = 0.1 [26].
Red FilteredZnS:Mn 68 0.65 0.34
Table 1 summarises the luminance data which Green ZnS:Tb 100 0.31 0.60
have been obtained for the structured phosphor con- Blue CaGa2S4:Ce 10 0.15 0.19
cept. To improve the blue luminance of the VGA
 R.H. Mauch/ Applied Surface Science 92 (1996) 589-597 595

~ 0.6 at% Mn .~.

~_,,I~.~E
oo0 %
0 , 4 at% Mn rr ~.At
=
J=
/,,,
10o
v

o=
t.-
o
.__. 10 =
E

=1
400 450 500 550 600 650 700
200 250 300 350 400 wavelength (rim)
voltoge(V)
Fig. 10. Emission spectra of various doped ZnS:Mn/SrS:Ce
Fig. 9. Luminance versus voltage characteristics of a nine multi-
multilayer EL devices [29].
layer and a conventional SrS:Ce EL device driven at 1 kHz [28].

Therefore, the task was and still is to develop new

ond, the alkaline earth sulphides require more com-
plex deposition processes than the classical ZnS.
Furthermore, since the physical processes leading to
emission are not well understood, it seems that the
conventional EL device structure is not best for
reaching the highest performance of AES-type elec-
troluminescence.
Thus, besides further optimisation of the fabrica-
tion processes also new device structures are under
investigation. For the latter, a first approach has been
reported in 1992. The homogeneous SrS:Ce phos-
phor layer was replaced by a multilayer package of
alternatingly deposited ZnS and SrS:Ce sublayers
[28]. In the case of undoped ZnS, a multilayer device
resulted in more than a twofold increase of lumi-
nance compared to a conventional SrS:Ce device as
shown in Fig. 9.
This development is the basis for a further step
towards "colour by white". The additional doping
of the ZnS layers with Mn leads to a superposition of
processes allowing the fabrication of SrS:Ce phos-
phor layers of higher quality. The application to EL
devices should result in an advanced performance
even in the conventional EL structure.
As was already mentioned, stoichiometry and
crystallinity are decisive for EL performance. It is
well known that, besides an optimised substrate tem-
perature, the control of sulphur during or after the
deposition is the key to successful SrS growth. In the
case of reactive evaporation where pure elements
(Sr, S) are used as sources, only low reactive S
molecules are observed in the flux. Hence, other
source materials which supply highly reactive atomic
S may improve the thin film growth. On the basis of
these considerations a new process has been devel-
oped where a S source supplying atomic S was used.
The XRD spectra (Fig. 11) and the L - V character-
istics (Fig. 12) are compared for a SrS:Ce fabricated
12000 m rtew pt'o~m

the emissions as demonstrated in Fig. 10 [29]. In this FWHM: 0.16"

10000 . . . . .F. I ~~ M :1 0.16"
case, three different Mn doped ZnS layers were
incorporated in a ZnS:Mn/SrS:Ce multilayer struc- 8O00
ture. The contribution of the Mn emission depends "E
strongly on the doping level as is known for conven- ~ 600o
tional ZnS:Mn EL devices.
4000
The multilayer approach resulted in lab-sample
performance of SrS:Ce-based EL which has the pos- 2000
sibility of application. However, if the results have to
be transferred to a production process more stringent 0
n

29.5 30.0
i

requirements have to be fulfilled. Hence, further 20 (DEG)

improvements in luminance and efficiency and also Fig. I 1. Improvement in crystalline perfection for SrS:Ce,CI
in process simplicity are needed. fabricated with elemental S and the new process [24,30].
596 R.H. Mauch / Applied Surface Science 92 (1996) 589-597

2000
mixed ~ j, have been reported for samples in which the share of
elemental IRJffur
.z. ,°
the ZnS:Mn emission is increased [34]. However, the
1500 colour coordinates are worse for green and blue and
hence, not comparable with the data given above.
While the colour coordinates in Table 2 for red and
" 1000
c
green are in perfect agreements with EBU standards,
those for blue (0.13, 0.26) still need some improve-
E
=, SO0 ment to satisfy the requirements of EBU. This can be
done by replacing S with Se [35]. Nevertheless, the
achieved performance allows immediate application
0 "
100 120 140 160 in various products where multi to full colour imag-
Voltage (V)
ing is required.
Fig. 12. Comparisonof the L - V characteristics of SrS:Ce,CI EL
devices fabricated according to the standard and the new process
[24,30].
4. S u m m a r y

with elemental S and for a sample produced accord-
ing to the new recipe. Since the FWHM of the (200)
peak and the luminance are superior for the new
process the close correlation between EL perfor-
mance and crystalline perfection is demonstrated.
Furthermore, values of 1.6 l m / W measured at 1
p , C / c m 2 and 1 kHz driving frequency are the high-
est efficiency ever reported for SrS-based EL. The
new process applied to the growth of a
ZnS:Mn/SrS:Ce multilayer phosphor resulted in lu-
minance levels at 60 Hz driving as high as: L = 340
c d / m 2, L r = 39 c d / m 2, Lg = 90 c d / m 2, L b = 18
c d / m 2.
In Table 2 the state of the art for the "colour by
white" concept is summarised. It shows the tremen-
dous improvements obtained within the last seven
years. In terms of luminance the gain is about seven-
teen times. If the best data are considered for red,
green and blue, a full colour display with an areal
white luminance of at least 40 c d / m 2 can be re-
alised. Even higher luminance levels up to 470 c d / m 2
The basic principles and the status of various thin
film light emitter technologies for future display
applications have been summarised. Thin film elec-
troluminescence in organic and a-SiC LEDs are of
the low-field injection type. These approaches have
interesting prospects. Organic EL is more advanced
in terms of luminance and efficiency. In addition, in
the case of organic EL the realisation of different
colours in more straightforward. Both technologies
have reliability problems which are serious obstacles
to application.
In contrast, in the case of high-field thin film
electroluminescence of the MISIM type stability is-
sues have been successfully solved as demonstrated
in a variety of products. The major problem of the
past, the lack of reasonably good blue emitting mate-
rials has been solved since several options have been
found. Further optimisation is the subject of present
investigations. Never the less, it is expected that the
first full colour EL flat panel displays will be avail-
able in the very near future.

Table 2
History and state of the art for the "colour by white" EL display
Phosphor layer Technology Year Laboratory Luminance at 60 Hz (cd/m 2)
Unfiltered Red Green Blue
ZnS:Mn/SrS:Ce/ZnS:Mn E-beam 1987 Tottori [31] 20 - - -

ZnS:Mn/SrS:Ce/ZnS:Mn MSD 1992 Komatsu[32] - 23 37 6

ZnS:Mn/SrS:Ce 9 ML React. evap. 1993 HHI/IPE [29] 226 22 53 10
ZnS:Mn/SrS:Ce ALE 1993 Planar [33] 220 29 62 5.5/14
ZnS:Mn/SrS:Ce 9 ML React. evap. 1994 HHI [24] 340 39 90 18
 R.H. Mauch / Applied Surface Science 92 (1996) 589-597
Acknowledgements
The author wishes to thank his colleagues of the
AG Elektrolumineszenz of the Heinrich-Hertz-In-
stitut. This work has been supported by the Bun-
desministerium f'tir Forschung und Technologie un-
der contract 01 BK 202/7.
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