Journal of the Korean Physical Society, Vol. 38, No. 1, January 2001, pp. L1∼L3 Letters Transient Electroluminescence Study of Enhanced Recombination Mobility in a Bilayer Organic Light-Emitting Diode Jae Won Jang, Dong Keun Oh, Chang Hoon Lee and Cheol Eui Lee∗ Department of Physics, Korea University, Seoul 136-701 Kyungkon Kim and Jung-Il Jin Division of Chemistry and Molecular Engineering and Center for Electro- and Photo-Responsive Molecules, Korea University, Seoul 136-701 (Received 20 September 2000) Transient electroluminescence (EL) measurements were carried out on indium-tin-oxide (ITO)/poly[2-(2’-ethylhexyloxy)-5-methoxy-1,4-phenylenevinylene] (MEH-PPV)/tris(8-hy droxyquinoline)aluminum (Alq3 )/Al bilayer and ITO/MEH-PPV/Al monolayer organic light-emitting diode devices. Significantly enhanced recombination mobility and EL lifetime were obtained in the bilayer device, explaining the greater EL efficiency in comparison to that of the monolayer device. trode with a thickness of 100 nm was used for the holeinjecting contact. To remove the solvent, we dried the spin-coated MEH-PPV layer at 150 ◦ C for 2 hours, and Alq3 (280 nm) was thermally evaporated on the MEHPPV layer for the bilayer device. The Al (100 nm) electrode was deposited on top of the MEH-PPV/Alq3 layer by using thermal evaporation at a pressure about 10−6 Torr. The active area of the devices was 1.54 mm2 . The devices were mounted onto a strip transmission line with a copper board, and indium solder was used to make contacts between the device electrodes and the strip line [8]. One side of the strip line had a 50-Ω termination to prevent input pulse distortion, and the other side was connected to the pulse generator. For the transient EL measurements, voltage pulses with 1-µs widths from a Hewlett-Packard 214B pulse generator were applied to the device, and the emitted light was collected by a photomultiplier tube (Hama- In the last ten years, π-conjugation organic polymers have attracted much attention as light-emitting materials. The organic light-emitting diodes (OLEDs) are very attractive for development of large-area flat panel displays and possess tunable electrical and optical characteristics, as well as flexibility [1,2]. Since the electroluminescence (EL) properties of poly(p-phenylenevinylene) (PPV) were reported, many researchers have made efforts to improve the optical and the electrical properties. The greatest obstacle to the better EL efficiency is the mobility imbalance of charge carriers [3,4]. PPV and most of its derivatives have hole mobilities superior to the electron mobilities, and charge-carrier mobility balancing is a very important factor for better EL efficiency. Thus, many attempts have been made to improve mobility balancing by using low work-function metals for the cathode [5], blending the light-emitting polymer with an electron transport material [6], and fabricating bilayer device structures [7]. In this letter, we report transient EL measurements of the charge-carrier recombination mobility and the EL lifetime in an ITO/MEH-PPV/tris(8hydroxyquinoline)aluminum (Alq3 )/Al bilayer device with an Alq3 electron-transport layer in comparison to those in an ITO/MEH-PPV/Al monolayer device where the poly(p-phenylenevinylene) (PPV) derivative, MEHPPV, was used as the light-emitting polymer. The structures of MEH-PPV and Alq3 are shown in Fig. 1. The MEH-PPV (62 nm) was spin coated on indiumtin-oxide (ITO) glass in an Ar atmosphere. An ITO elec∗ E-mail: rscel@korea.ac.kr Fax: +82-2-927-3292 Fig. 1. The structures of the the MEH-PPV and Alq3 . -L1- -L2- Journal of the Korean Physical Society, Vol. 38, No. 1, January 2001 Fig. 4. Transient EL decays for the MEH-PPV/Alq3 bilayer and the MEH-PPV monolayer devices, which are well fitted by a double-exponential function. to occur. Then, the drift mobility, or the recombination mobility, is given by Fig. 2. Typical transient EL signals for the MEH-PPV monolayer and the MEH-PPV/Alq3 bilayer devices. The inset shows how the delayed response time tr is defined. matsu R928 PMT). The input pulse shape was monitored by a digital oscilloscope (HP 54600B), and the PMT signal was recorded by a communication signal analyzer (Tektronix CSA 803A). In transient EL measurements, the delayed response time tr is defined as the time between the rising edge of the voltage pulse and the occurrence of EL (Fig. 2). This is the time for the radiative recombination of e-h pairs Fig. 3. Recombination mobilities obtained from transient EL measurements of the MEH-PPV/Alq3 bilayer and the MEH-PPV monolayer devices. µ= d2 , tr · (V − Von ) (1) where d is the carrier transit distance, V is the applied voltage, and Von = 0.6 V the is turn-on voltage, which is the work-function difference between the ITO and the Al [9]. Tunneling of carriers can take place when the conduction and the valance bands are in the so-called “flatband” condition, for which Von is necessary. For the MEH-PPV monolayer device, the light-emission region will be located near the cathode because of the mobility imbalance as the hole mobility is much greater than the electron mobility. Thus, the transit distance d corresponds to the thickness of the polymer film. For the MEH-PPV/Alq3 bilayer device, the light-emission region will be located near the MEH-PPV/Alq3 interface. Because the HOMO (highest occupied molecular orbit) level of Alq3 lies lower than that of MEH-PPV and in Alq3 the electron mobility is superior to the hole mobility, it is difficult for holes to cross the Alq3 layer. In our bilayer device, the Alq3 layer is thicker than the MEHPPV layer, so holes will wait near the MEH-PPV/Alq3 interface until electrons arrive. Thus, the time taken by electrons dictates the time for the recombination process to occur, and d can be taken to be the thickness of the Alq3 layer for the MEH-PPV/Alq3 bilayer device. Figure 2 shows the EL signals for the MEH-PPV monolayer and the MEH-PPV/Alq3 bilayer devices. For the bilayer device, a spike is noticed at the beginning of the EL signal in contrast to the case of the monolayer device, and is ascribed to the charges accumulated at the MEH-PPV/Alq3 interface [10]. The recombination mobilities of the e-h pairs in the MEH-PPV monolayer and the MEH-PPV/Alq3 bilayer devices obtained from our transient EL measurements Transient Electroluminescence Study of Enhanced Recombination Mobility· · · – Jae Won Jang et al. and Eq. (1) are shown in Fig. 3. It is noted that the bilayer device has an order of magnitude greater mobility than that of the monolayer device, indicating that the recombination process in the bilayer device is considerably faster than that in the monolayer device. The faster recombination process arises from the electron mobility being enhanced by the electron transport layer. The effect of the mobility balancing is reflected in the EL lifetime as well. Figure 4 shows the expansion plot of the tails of the transient EL signals, which were well fitted by a double-exponential function. The shorter time constant of the EL decay corresponds to the RC time constant of the devices, and the longer part of the EL decay corresponds to the EL lifetime of the e-h pairs. The EL lifetime in the MEH-PPV/Alq3 bilayer device ('1.9 µs) is found to be much longer than that of the MEH-PPV monolayer device ('0.3 µs), which is compatible with its EL efficiency being greater than that of the monolayer device [11,12] due to the mobility balancing. In this work, by using EL technique, we found the recombination mobility and the EL lifetime of a MEHPPV/Alq3 bilayer device to be significantly greater than those of a MEH-PPV monolayer device. Our results are compatible with a greater EL efficiency in the bilayer device, which can be attributed to the improved mobility balancing achieved by introducing an Alq3 electrontransport layer. ACKNOWLEDGMENTS This work was supported by the Korea Ministry of Science and Technology (National Research Laboratory and through the Center for Photo- and Electro-Responsive Molecules at Korea University) and by the Korea Re- -L3- search Foundation (D00064). Measurements at the Korea Basic Science Institute (KBSI), Seoul Branch, are acknowledged. REFERENCES [1] G. Gustafsson, Y. Cao, G. M. Treacy, F. Klavetter, N. Colaneri and A. J. Heeger, Nature 357, 477 (1992); K. Ziemelis, Nature 399, 408 (1999). [2] S. Cho, E. K. Kim and S-K. Min, J. Korean Phys. Soc. 32, 584 (1998); Y-K. Ha, C. Lee, J-E. Kim, H. Y. Park, S. B. Kim, H. Lim, B-C. Kim and H-C. Lee, J. Korean Phys. Soc. 36, 42 (2000); J. Lee, J. Korean Phys. Soc. 36, 60 (2000). [3] H. Autoniadis, M. A. Abkowitz and B. R. Hsieh, Appl. Phys. Lett. 65, 2030 (1994). [4] A. Kraft, P. L. Burn, A. B. Holmes, D. D. C. Bradley, R. H. Friend and J. H. F. Martens, Synth. Metals 55-57, 4136 (1994). [5] I. D. Parker, J. Appl. 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