Micro-Patterned Organic Electroluminescent Devices
, Ivan T
, Masahiro G
, Akira K
, Tadashi T
, and Masahiro T
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.
-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
/tris(8-hydroxyquinoline) aluminum (Alq
)/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
, 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
) 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
has been demonstrated by Karthaus
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
-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,
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
. 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
Pa. An Alq
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
. 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
E-mail address: firstname.lastname@example.orgJapanese Journal of Applied PhysicsVol. 47, No. 2, 2008, pp. 1263–1265
2008 The Japan Society of Applied Physics