Light enhancement by the formation of an Al-oxide honeycomb nano-structure on the n-gan surface of thin-gan light-emitting diodes

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1 Light enhancement by the formation of an Al-oxide honeycomb nano-structure on the n-gan surface of thin-gan light-emitting diodes C. L. Lin, P. H. Chen Department of Chemical and Materials Engineering, National Central University, Jhong-Li, 32001, Taiwan, Republic of China Chia-Hua Chan, C. C. Lee, Chii-Chang Chen, Jeng-Yang Chang Department of Optics and Photonics, National Central University, Jhong-Li, 32001, Taiwan, Republic of China C. Y. Liu Institute of Materials Science and Engineering, National Central University, Jhong-Li, 32001, Taiwan, Republic of China Abstract By using micron poly-styrene ball array as a template, an Al-oxide honeycomb structure was produced on the n-gan surface of a thin-gan LED (Light Emitting Diode). The Al-oxide honeycomb structure consists of networking hexagonal Al-oxide nano-wall. With the Al-oxide honeycomb nano-structure, the total lighting output of thin-gan LED was enhanced by 35%. We believe that the networking nano-wall of the Al-oxide honeycomb structure acted as wave guide to extract the light emitted to the outer medium effectively. 1

2 GaN-based light-emitting diodes (LEDs) have lately attracted serious attention due to their numerous applications, particularly in the area of outdoor display panel and general illumination. However, the reported external quantum efficiency of GaN-based LEDs (around 30%) still leaves plenty of room for improvement. One of major reasons for the low external quantum efficiency is the low light extraction efficiency, which is mainly due to the loss of total internal reflection (TIR) at the GaN/outer medium. To increase the light extraction efficiency, the TIR issue has to be solved. Many reports have shown that roughening the emitting surface can reduce the TIR effect. Various ways have been used to texture the emitting p-gan surface in conventional p-side up LEDs. A 29.4% to 80% enhancement of the entire light output can be achieved. 1-3 Recently, vertical thin-gan LED structures have been identified as the most promising structure to improve high-power LEDs over other traditional LED structures. Unlike the conventional LED structures, the thin-gan LED is an n-side up structure with the light emitted from the n-gan layer to the outer medium. From the view-point of light extraction, the n-side up thin-gan LED has a great many merits over the traditional p-side up LED structures, such as (1) a slightly larger so-called escape cone which occurs due to the smaller refraction index of the n-gan layer compared to the p-gan layer. Note that the refractive index of n-gan and 2

3 p-gan are 2.42 and 2.45, respectively. (2) The thicker n-gan layer (2-3 µm) is better for the subsequent texturing process on the n-gan surface. The thickness of the p-gan layer is only about few hundred nanometers, so the roughening process, say plasma, can easily cause damage during surface texturing process. 4 To reduce the TIR effect, roughening of the surface of the n-gan top layer is needed. Various dry and wet etching techniques, such as, photoelectrochemical (PEC) and Inductively Coupled Plasma (ICP) techniques have been used to roughen the n-gan surface of thin-gan LED structures, to improve the light extraction efficiency. With proper roughening, the total out-put power can be enhanced. 5-6 In recent years, photonic crystals (PhCs) with an ordered array structure have been implemented in LEDs. The light out-put of the conventional type of LED can be enhanced by the placing of a photonic crystal structure on the p-gan surface. 7 In this work, we study the light enhancement by forming the Al-oxide honeycomb nano-structure on the n-gan top layer of a thin-gan LED. Metalorganic chemical vapor deposition (MOCVD) was used to grow GaN LED epi-layers on sapphire wafers for the fabrication of thin-gan LED chips. Fig. 1 (a) shows the entire LED epi-layer structure, which consists of a 200 nm buffer-gan layer, a 2 µm undoped GaN layer, a 2 µm Si-doped n-gan layer, five pairs of InGaN/GaN multi-quantum well layers, and a 300 nm Mg-doped p-gan layer. The 3

4 wave length of the emitting light is about 465 nm. First, a GaN epi-layer was defined onto 40-mil LED chips; then an e-gun evaporation process was used to deposit Ni (5 nm) / Au (5 nm) / Al (300 nm) metallization onto the p-gan surface of the thin-gan chips. The Ni/Au served as the p-type contact layer, and Al layer as the reflector layer. For wafer bonding metallization structure, i.e., Cr (50 nm)/ Pt (30 nm)/ Au (2 µm), was deposited on the top Al layer by the sputtering process. Using Au-Si bonding, the metallized GaN epi-wafer was bonded with a Si substrate. 8 The bonding process was performed at 400 in a vacuum furnace. After wafer bonding, a 248 nm wavelength KrF excimer laser was used to strip off the original sapphire substrate. The thin-gan LED chips were then transferred onto the Si substrate. The n-pad on the n-gan layer of the thin-gan LED chip was 300 µm in diameter: Ti/ Al/ Ti/ Au (30 nm/ 120 nm/ 50 nm/ 200 nm). After fabricating thin-gan LED chips on the Si substrate, a latex solution (a mixture of dispersive polystyrene (PS) micro-spheres and Al-contained solution) was coated onto the n-gan surface. The two-µm PS balls formed a uniform two-dimensional closely-packed array on the n-gan surface 9, as seen in the OM image in Fig. 1 (b). This PS ball array served as a template for the formation of the Al-oxide honeycomb nano-structure. The space between the PS balls was filled with Al-containing solution. Then, the samples were annealed at 350 for 5 minutes. 4

5 During annealing, the PS balls thermally decomposed in the ambient air and the Al content in the Al-containing solution oxidized to form Al-oxide between the PS balls. As a result, the Al-oxide honeycomb structure was produced on the n-gan surface, as sketched in Fig. 1 (c). Fig. 2 shows a SEM image of the enlarged top-view of the Al-oxide honeycomb structure. The insert in the upper right corner of Fig. 2 is a tilted SEM image. From the titled SEM image, we notice that the thickness and height of the Al-oxide honeycomb wall are in the nano-scale regime, which are about 20 nm and 300 nm, respectively. Image of photons emitting on the top surface of the Al-oxide honeycomb nano-structure is shown in Fig. 3. The average power intensity emitted from the Al-oxide honeycomb nano-structure thin-gan LED surface was larger than that emitting on the blank thin-gan LED. The power density was found to be enhanced especially at the position of perfect Al-oxide honeycomb array. Fig. 4 shows the lighting intensity of thin-gan LEDs with and without the Al-oxide honeycomb nano-structure. We found that the light output of the thin-gan LED chip with the Al-oxide honey-comb nano-structure was enhanced by 35%, compared with thin-gan LED without this structure. Note that the refraction index of Al-oxide is in between the values of the refraction index of n-gan and air ambient. To clarify the reduction of TIR effect by 5

6 using the low refraction-index of Al-oxide on the n-gan surface, a layer of Al-oxide was produced on the n-gan surface of a thin-gan LED chip by using the same process as in the case for the Al-oxide honeycomb nano-structure. Hence, the quality and thickness of the Al-oxide layer is same as the Al-oxide honeycomb nano-structure. Surprisingly, we found that no obvious light enhancement could be observed after a complete Al-oxide layer formed on the thin-gan LED; see the solid square marks in Fig. 4. The implications are: (1) the light extraction enhancement has very little to do with the effect of the medium refractive index of the Al-oxide layer. (2) the fabricated Al-oxide has a high transmittance for the 460nm wave-length. From the above discussions and observations, the major contribution to the light enhancement should thus be due to the structure-effect of the Al-oxide honeycomb nano-structure. We believe that the networking Al-oxide nano-wall on the n-gan surface acts as a wave guide. Light rays, generated from the active LED epi-layers, entering the Al-oxide honeycomb nano-structure are guided in the networking Al-oxide nano-wall and emitted to the outer medium effectively. In conclusion, an Al-oxide honeycomb nano-structure was produced on the n-gan surface of a thin-gan LED. The total lighting output of the honeycomb nano-structure thin-gan LED was enhanced by 35%. The networking Al-oxide nano-wall on the n-gan surface acts as a wave guide to extract light emitted to the 6

7 outer medium. Acknowledgements: The authors are grateful for the support of the Taiwan National Science Council, the MOE Lab in the Optical Sciences Research Center, and the Ministry of Economic Affairs, R.O.C. program for the new generation solid-state lighting, under grant number 95-EC-17A-07-S1-043, and also for the measurement equipment supplied by Professor Gou-Chung Chi. (Department of Physics, NCU, Taiwan). 7

8 References: 1. C.H. Liu, R.W. Chuang, S.J. Chang, Y.K. Su, L.W. Wu, C.C. Lin, Mater Sci Eng B 112, 10 (2004) 2. Seok-In Na, Ga-Young Ha, Dae-Seob Han, Seok-Soon Kim, Ja-Yeon Kim, Jae-Hong Lim, Dong-Joon Kim, Kyeong-Ik Min, Seong-Ju Park, IEEE Photon. Technol. Lett. 18, 1512 (2005) 3. Hung-Wen Huang, J. T. Chu, C. C. Kao, T. H. Hseuh, T. C. Lu, H. C. Kuo, S. C. Wang, C. C. Yu, Nanotechnology 16, 1844 (2005) 4. X. A. Cao, S. J. Pearton, A. P. Zhang, G. T. Dang, F. Ren, R. J. Shul, L. Zhang, R. Hickman, J. M. Van Hove, Appl. Phys. Lett. 75, 2569 (1999) 5. T. Fujii, Y. Gao, R. Sharma, E. L. Hu, S. P. DenBaars, S. Nakamura, Appl. Phys. Lett. 84, 855 (2004) 6. D. W. Kim, H. Y. Lee, M. C. Yoo, G. Y. Yeom, Appl. Phys. Lett. 86, (2005) 7. Dong-Ho Kim, Chi-O Cho, Yeong-Geun Roh, Heonsu Jeon, Yoon Soo Park, Jaehee Cho, Jin Seo Im, Cheolsoo Sone, Yongjo Park, Won Jun Choi, Q-Han Park, Appl. Phys. Lett. 87, (2005) 8. S. C. Hsu and C. Y. Liu, Electrochemical and Solid-State Letters 9, G171 (2006) 9. C. H. Chan, C. C. Chen, C. K. Huang, W. H. Weng, H. S. Wei, H. Chen, H. T. Lin, 8

9 H. S. Chang, W. Y. Chen, W. H. Chang, and T. M. Hsu, Nanotechnology 16, 1440 (2005) 9

10 Figure Captions: Fig. 1 (a) Structure of the GaN LED epi-layer. (b) 2-D array of Polystyrene (PS) balls on the n-gan surface. (c) Sketch of 3-dimension Al-oxide honeycomb nano-structure on thin-gan LED. Fig. 2 Al-oxide honeycomb nano-structure on the n-gan surface. Fig. 3 (a) Images of photons of the blank thin-gan LEDs and (b) the thin-gan LEDs with Al-oxide honeycomb nano-structure with 350 ma current. Fig. 4 Lighting performance of the thin-gan LED with Al-oxide honeycomb nano-structure. 10

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