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Micro-Patterned Organic Electroluminescent Devices

Micro-Patterned Organic Electroluminescent Devices

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Micro-Patterned Organic Electroluminescent Devices
Yuriy P
IHOSH
Ã
, Ivan T
URKEVYCH
, Masahiro G
OTO
, Akira K 
ASAHARA
, Tadashi T
AKAMASU
, and Masahiro T
OSA
 National Institute for Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki 305-0047, Japan
(Received April 6, 2007; accepted June 18, 2007; published online February 15, 2008)
Laser induced molecular implantation technique (LIMIT) has been used for site-controlled fabrication of pixel arrays of organic light-emitting diodes in a form of dots with a diameter of several micrometers.
,
 N 
0
-Bis(3-methylphenyl)-
 N 
,
 N 
0
-diphenylbenzidine (TPD) dots, which were implanted into the poly(3,4-ethylene dioxythiophene)–poly(styrene sulphonate)(PEDOT–PSS) layer, act as recombination centers between the hole- and electron-transport layers in the indium tin oxide(ITO)/PEDOT–PSS/TPD
dots
/tris(8-hydroxyquinoline) aluminum (Alq
3
)/Mg–Ag sandwich structure, and illuminate intensegreen light. We studied fluorescence spectra of the implanted TPD dots and the dependence of their size and morphology onthe intensity of a laser pulse, as well as the electroluminescence resulted from the organic light-emitting device (OLED)arrays. The site-controlled fabrication of such small OLEDs opens up an opportunity for production of electroluminescentdevices with ultrahigh resolution.[DOI:10.1143/JJAP.47.1263]
KEYWORDS: laser implantation, TPD, Alq
3
, organic light-emitting device, micro-patterning
Organic light-emitting devices (OLEDs) have become avery promising technology for electronic displays andlighting. Since electroluminescence (EL) has beenobservedin antracene crystals by Helfrich and Schneider
in 1965,OLEDs based on organic semiconductors havebeen exten-sively studied. In 1987 Tang and Van Slyke
fabricatedtwo-layer heterostructure devices based on electron- andhole-transport organic semiconductors tris(8-hydroxyquino-line) aluminum (Alq
3
) and diamine, respectively. Since thenOLEDs have been extensively developed in the area of flatpanel displays applications.
Fabrication of full colordisplays requires site-controlled patterning of red, blue andgreen emitting compounds. Since the usage of conventionallithography is a rather complicated process for the patterningof organic layers, the most widely used patterning tech-niques today are screen-printing (ink-jetprinting)
andevaporation through a shadow mask.
However bothtechniques have low resolution limited to several tens of microns, and therefore can hardly be used for fabrication of micron-sized OLED devices. The pattering of the EL layerswith the formation of micrometer size EL dots can be used toprevent degradation of the OLED device. Since degradationof EL layers spreads through the whole OLED devicetypically from one defect point, the confinement of thedefect to a small EL dot can prevent the destruction of thewhole device. Although an excellent method for theformation of monochrome EL dots with the diameterof 0.5–2
m
m
has been demonstrated by Karthaus
et al.
,
their technique is based on a self-organized dewettingprocess and therefore can not control the position of the dots.Here we report the development of a novel method forthe site-controlled fabrication of micron-sized OLED dotsby using laser induced molecular implantation technique(LIMIT). Recently, LIMIT has been developed as a highlyefficient method to transfer and implant organic moleculesinto polymer films producing space selective patterning.
This technique involves laser activated transfer and implan-tation of molecules from a doped polymer source film to anundoped polymer target film placed in proximity to eachother. The energy of laser pulse is absorbed by molecules of the source film and converts into heat, which generates aplume of ejected molecules flowing along the direction of the incident laser beam. The collision of the ejected plumewith the target polymer leads to the formation of a dot whichconsists of the source organic molecules implanted into thetarget polymer film.In our previous work 
we used the same method totransfer coumarin-6 molecules from a doped polymer film toan undoped one. The main advantages of the LIMIT are thatthe process is clean and space selective, and, moreover, thefunctionality of implanted organic molecules survives thelaser implantation. Besides providing high resolution, thismethod can also be used for the implantation of a wide rangeof organic materials by simply changing the material of asource film, which is important for the fabrication of fullcolor OLED displays with ultra-high resolution.The details of our experimental set up have beendescribed previously.
Figure 1(a) shows the conceptualsketch of our apparatus (conventional fluorescence micro-scope, Olympus IX70), which was used for the fabrication of the micro-patterned EL devices. The TPD source films wereprepared by thermal evaporation of 
,
 N 
0
-bis(3-methylphen-yl)-
 N 
,
 N 
0
-diphenylbenzidine (TPD) from a Knudsen cell(Kitano Seiki KTC 20A) in a vacuum, and the filmdeposition rate was controlled by a quartz crystal micro-balance monitor.A single focused laser pulse (4ns pulse,
¼
440
nm) wasused to irradiate the source TPD films, which were broughtinto the direct contact with the target poly(3,4-ethylenedioxythiophene)–poly(styrene sulphonate) (PEDOT–PSS)/indium tin oxide (ITO)/glass structure. The target structurewas fabricated on the ITO-coated glass substrates with thesize of 
20
Â
20
mm
2
. The ITO substrates were first ultra-sonically cleaned in ethanol for 25min. When dry, thecleaned ITO substrates were spin coated by PEDOT–PSSwith the thickness of about 50nm, and then transferred to avacuum chamber for drying for 4h at 70
C. The ablationtransfer of the TPD material was controlled by the laserfluence, and the implanted position was predetermined bycomputer control
stage. The target structure with theimplanted TPD dots was put into the evaporation system andpumped out to
1
Â
10
À
4
Pa. An Alq
3
layer with the thicknessof 80nm was evaporated on the target system and the devicewas completed by evaporating an Mg/Ag top electrode withthe thickness of about 1
m
m
. A schematic sketch of theprepared device is shown in Fig. 1(b). The fluorescencespectra from the source film and the target surface wereobserved with the USB-2000-FLG spectrometer (Ocean
Ã
E-mail address: yuriy.pihosh@nims.go.jpJapanese Journal of Applied PhysicsVol. 47, No. 2, 2008, pp. 1263–1265
#
2008 The Japan Society of Applied Physics
1263
Communication 
 
Optics Incorporated) before the thermal evaporation of Alq
3
and the Mg/Ag top electrode. The electroluminescencespectra were measured using a fluorescence spectrophotom-eter (Hitachi F-7000). The micro-images of EL microdotswere obtained by an Andor high speed charge coupleddevice (CCD) camera (Tokyo Instruments Incorporated),which was connected to a fluorescence microscope, and theemitted light was collected by a
40
Â
microscope lens atdriving voltage of 11.5V.The TPD spots were successfully formed on the surface of the PEDOT–PSS film by using LIMIT. In order to explorepossible ways to control the size and morphology of the TPDspots, we performed experiments on two TPD source filmswith different thickness at various laser fluences. Figure 2(a)shows the size of the TPD spots implanted on the PEDOT–PSS layer versus the laser intensity for two TPD source filmswith the thickness of 1.8 and 0.73
m
m
. It is clearly seen thatboth the thickness of the TPD source film and the laserfluence strongly affect the size of the implanted spots. Thereis almost linear increase of the spots size with the increasingof the laser fluence for both source films. The minimum sizeof the implanted spots was achieved when the thickness of the source film was 1.8
m
m
and estimated to be
2
:
5
Æ
0
:
5
m
m
at the laser fluence of 687.9J/cm
2
. In the case of a thinnersource film, the implanted spots on PEDOT–PSS film arelarger and acquire a donut shape at any laser fluence. The1.8
m
m
source film gives smaller spots and their shapeundergoes transformation near the threshold at intermediatelaser fluence of about 800J/cm
2
where the shape of theimplanted spots transforms to the dot type. After reachingthe minimum at 687.9J/cm
2
the diameter of the implantedspots slightly increases again with the decreasing of the laserfluence and below 470J/cm
2
the implanted TPD materialdisperses on the surface of the target film without spotsformation. Although it is difficult to reveal the factors whichinfluence formation of the ejected plume and its shape, theexistence of the above mentioned minimum indicates that atlower laser fluences the main fraction of the laser pulse isabsorbed in the thick source film without ejection of thematerial in the form of the highly directed plume. Due to thelocal increase in temperature some of the molecules are stillejected from the surface of the source film, but they disperseon surface of the target film without a compact spotformation.In order to check what happens with the TPD materialafter the implantation we measured the fluorescence spectraof the implanted spots. Figure 2(b) indicates the fluores-cence spectra of the pristine TPD source film and the spotsimplanted on the PEDOT–PSS/ITO/glass target system atthe highest and the lowest laser fluences. The intensity of thefluorescence correlated with the amount of the implantedmaterial while the fluorescence spectral peaks of theimplanted spots appeared at the same position as that of the source film, which indicates that the implanted TPDmaterial was transferred without decomposition.Figure 3(a) shows the fluorescence micrograph of theimplanted TPD dots on the PEDOT–PSS/ITO target systemafter the excitation at wide-band wavelength from 330 to385nm. This photo had been taken before the evaporation of the Alq
3
and Mg/Ag layers. Figure 3(b) shows the ELmicrograph of the prepared OLED device at the operatedvoltage of 11.5V. The possibility to control the size and theposition of the implanted dots allowed us to compare thefluorescence and the EL micro-images and therefore we canconclude that all the implanted TPD dots emit green light.The cross section profile of four TPD dots is shown inFig. 3(c). The brightness of all the dots, which emitted greenlight and had the size of about
2
:
3
Æ
0
:
3
m
m
is almost thesame and the spacing between the dots centers is 50
m
m
.
(a)(b)
Fig. 1. (a) Conceptual sketch of the setup used for the laser implantationof TPD material and (b) sketch of the prepared devices.
200400600800100012001400246810121416182022242628303234
   D   i  a  m  e   t  e  r  o   f   i  m  p   l  a  n   t  e   d  s  p  o   t  s   [
     µ
  m   ]
Laser fluence [J/cm
2
]
Thickness of the source film is 730 nm
Thickness of the source film is 1.8
µ
m
dispersion of TPD material
(a)
Threshold
350400450500550600650700
   F   l  u  o  r  e  s  c  e  n  c  e   i  n   t  e  n  s   i   t  y   [  a  r   b .  u  n   i   t   ]
Wavelength [nm]
imlanted spot at 1361.9 J/cm
2
implanted spot at 687.9 J/cm
2
source TPD film
(b)
Fig. 2. (a) Dependence of the size of the TPD spots implanted onPEDOT–PSS layer, upon the laser intensity at two different thicknesses of the TPD source film and (b) fluorescence spectra of the pristine TPDsource film and the prepared spots.Jpn. J. Appl. Phys., Vol. 47, No. 2 (2008) Y. P
IHOSH
et al.
1264

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