本實驗使用濺鍍機製程，透過不同的氧氣流量作為參數，交互鍍製多層富矽氧化物/二氧化矽薄膜，進行三道黃光微影之後，即可完成多層富矽氧化物/二氧化矽發光二極體。
　　在多層富矽氧化物/二氧化矽薄膜當中進行光致發光的量測，可以發現光譜隨著氧氣流量的變化呈現奈米矽晶尺寸效應，在較高的激發能量下，更可以發現薄膜主要的發光來源為奈米矽晶或是輻射復合缺陷，包括E’δ center和NOV。另外，在不同的激發能量下，更是發現光譜的發光強度隨激發能量增加而下降的趨勢，以及奈米矽晶尺寸選擇效應。最後，經過鈍化的薄膜在發光強度上有大幅度的增加。
　　在多層富矽氧化物/二氧化矽發光二極體當中進行電致發光的量測，可以發現光譜隨著氧氣流量的變化而異，元件的發光來源非常多，包括奈米矽晶、NBOHC、E’δ center和NOV。在較強的電場激發下，甚至出現能帶填充效應，也可以發現奈米矽晶的第一激發態發光。另外，隨著氧氣流量的變化，可以發現奈米矽晶和輻射復合缺陷的貢獻發光有消長的趨勢。最後，隨著氧氣流量的不同，光致發光與電致發光的結果不一定一致。

In this study, silicon-rich oxide/silicon dioxide multilayers (SRO/SiO2 MLs) were synthesized by reactive magnetron sputtering in a gas mixture of argon and oxygen. In particularly, the variation from 0 to1.0 sccm in the oxygen flow was used. The structural, optical, and electrical properties of the SRO/SiO2 MLs were investigated by TEM, PL, XPS and EL measurements, where the excitation laser was employed by the 325, 532 and 633 nm for the PL analysis. The PL emission was originated from the band-to-band transition within the Si-NCs and the radiative recombination centers at the Si-NCs/SiO2 interface. The results demonstrate that size of Si-NCs was decreased due to quantum-size effect as increasing the oxygen flow. The enhancement of EL in the visible range was achieved by using oxygen flow of 0.15 sccm. Relationship between PL and EL in the SRO/SiO2 MLs has been examined. The blueshift in the EL was attributed to the band filling effect under high current injection mode. The EL spectra at different oxygen flows were recorded, and the correlation between charge transport mechanisms and EL properties was discussed.

[1] A. Parisini, R. Angelucci, L. Dori, A. Poggi, P. Maccagnani, G.C. Cardinali, G. Amato,G. Lerondel, D. Midellino,” TEM characterisation of porous silicon”, Micron,vol 31,pp 223–230(2000).
[2]A.G. Cullis, and L. T. Canham,”Visible light emission due to quantum size effect in highly porous crystalline silicon”, Nature,vol.353,pp 335-338(1991)
[3]Z. H. Lu,D.J. Lockwood,and J.M.Baribeau,”Quantum confinement and light emission in Si/SiO2 supperlattice”,Nature ,vol. 378,pp.258(1995).
[4] B. Averboukh, R. Huber, K. W. Cheah, Y. R. Shen, G. G. Qin, Z. C. Ma, and W. H. Zong,” Luminescence studies of a Si/SiO2 superlattice”, JOURNAL OF APPLIED PHYSICS, vol. 92, pp. 3564(2002)
[5] Chih-Hsien Cheng, Yu-Chung Lien, Chung-Lun Wu, and Gong-Ru Lin,” Mutlicolor electroluminescent Si quantum dots embedded in SiOx thin film MOSLED with 2.4% external quantum efficiency”, Opt Express, Vol. 21,pp392-403(2013).
[6]Mark Fox”Optical Properties of Solids” ch.3 5 6(2009)
[7]陳亞孚, 萬春明, 盧俊”超晶格量子井物理” ch6(2002)
[8] S K Ray, S Maikap, W Banerjeeand S Das” Nanocrystals for silicon-based
light-emitting and memory devices” JOURNAL OF APPLIED PHYSICS, vol. 46, pp.153001(2013)
[9] Roushdey Salh” Defect Related Luminescence in Silicon Dioxide Network: A Review”, In Crystalline Silicon - Properties and Uses, Sukumar Basu (ed.), pp. 135-172(2011)
[10] Felice Friedrich, Christoph Boehme, and Klaus Lips” Triplet recombination at Pb centers and its implications for capture cross sections” JOURNAL OF APPLIED PHYSICS, vol. 97, pp. 056101(2005)
[11] S. GODEFROO, M. HAYNE, M. JIVANESCU, A. STESMANS, M. ZACHARIAS, O. I. LEBEDEV,G. VAN TENDELOO AND V. V. MOSHCHALKOV” Classification and control of the origin of
photoluminescence from Si nanocrystals” nature nanotechnology, vol. 3, pp174-178(2008)
[12] R. A. B. Devine and D. Mathiot, W. L. Warren and D. M. Fleetwood, B. Aspar” Point defect generation during high temperature annealing of the Si-Si02 interface” Appi. Phys. Let, vol. 63, No. 21, 22(1993)
[13] Gong-Ru Lin, Chun-Jung Lin, and Kuo-Chen Yu” Time-resolved photoluminescence and capacitance–voltage analysis of the neutral vacancy defect in silicon implanted SiO2 on silicon substrate” JOURNAL OF APPLIED PHYSICS, vol. 96, pp. 3025(2004)
[14] Gong-Ru Lin, Chun-Jung Lin, and Chi-Kuan Lin, Li-Jen Chou and Yu-Lun Chueh” Oxygen defect and Si nanocrystal dependent white-light and near-infrared electroluminescence of Si-implanted and plasma-enhanced chemical-vapor deposition-grown Si-rich SiO2” JOURNAL OF APPLIED PHYSICS vol. 97, 094306(2005)
[15] M. Ya. Valakh, V. A. Yukhimchuk, V. Ya. Bratus’, and A. A. Konchits, P. L. F. Hemment, T. Komoda” Optical and electron paramagnetic resonance study of light-emitting Si+ ion implanted silicon dioxide layers” JOURNAL OF APPLIED PHYSICS, vol. 85, pp.168(1999)
[16]陳紹平,”氫離子源輔助濺鍍多層富矽氧化物/二氧化矽發光二極體之研究”,國立成功大學, 2014
[17] Timur Nikitin and Leonid Khriachtchev “Optical and Structural Properties of Si Nanocrystals in SiO2 Films” nanomaterials, vol.5, pp.614-655(2015)
[18] Z TKang, B Arnold, C J Summers and B K Wagner “Synthesis of silicon quantum dot buried SiOx films with controlled luminescent properties for solid-state lighting” Nanotechnology, vol.17, pp. 4477-4482(2006)
[19] D. Riabinina, C. Durand, F. Rosei, and M. Chaker ” Luminescent silicon nanostructures synthesized by laser ablation” phys. stat. sol. (a), vol. 204, pp.1623-1638(2007)
[20] Mallar Ray, Samata Sarkar, Nil Ratan Bandyopadhyay, Syed Minhaz Hossain, and Ashit Kumar Pramanick “Silicon and silicon oxide core-shell nanoparticles: Structural and photoluminescence characteristics” Journal of Applied Physics, vol.105, pp.074301(2009);
[21] Benjamin G. Lee, Daniel Hiller, Jun-Wei Luo, Octavi E. Semonin, Matthew C. Beard, Margit Zacharias, and Paul Stradins ”Strained Interface Defects in Silicon Nanocrystals” Adv. Funct. Mater., vol. 22, pp.3223-3232(2012)
[22]Jong-Ick Son, Hee-Jong Nam, and Nam-Hee Cho “Nanostructural, Chemical, and Mechanical Features of nc-Si:H Films Prepared by PECVD” International Journal of Photoenergy, pp.643895(2012)
[23]Asuha, Takuya Kobayashi, Osamu Maida, Morio Inoue, Masao Takahashi, Yoshihiro Todokoro, and Hikaru Kobayashi ”Ultrathin silicon dioxide layers with a low leakage current density formed by chemical oxidation of Si ” Applied Physics Letters, vol. 81, pp. 3410(2002)
[24]L Palacios-Huerta, S A Cabañas-Tay, J A Luna-López, M Aceves-Mijares, A Coyopol and A Morales-Sánchez “Effect of the structure on luminescent
characteristics of SRO-based light emitting capacitors” Nanotechnology, vol. 26, pp.395202(2015)
[25]Byoung Youl Park, Sol Lee, Kyoungwan Park, Chang Hyun Bae, and Seung Min Park “Enhancement of light emission from silicon nanocrystals by post-O2–annealing process” Journal of Applied Physics, vol.107, pp.014314(2010)
[26]Gong-Ru Lin, Senior Member, IEEE, Chung-Hsiang Chang, Chih-Hsien Cheng, Student Member, IEEE, Chih-I Wu, and Po-Sheng Wang “Transient UV and Visible Luminescent Dynamics of Si-Rich SiOx Metal-Oxide-Semiconductor Light-Emitting Diodes” IEEE Photonics Journal, vol.4, pp1351-1363(2012)
[27]Bo-Han Lai, Chih-Hsien Cheng, and Gong-Ru Lin “Multicolor ITO/SiOx/p-Si/Al Light Emitting Diodes with Improved Emission Efficiency by Small Si Quantum Dots” IEEE JOURNAL OF QUANTUM ELECTRONICS, vol.47, pp.698-704(2011)
[28] W. D. A. M. de Boer, D. Timmerman1, K. Dohnalova, I. N.Yassievich, H. Zhang, W. J. Buma and T. Gregorkiewicz “Red spectral shift and enhanced quantum efficiency in phonon-free photoluminescence from silicon nanocrystals” NATURE NANOTECHNOLOGY, vol. 5, pp.878-884(2010)