本論文旨在以水熱法成長氧化鋅奈米結構與單晶/類單晶薄膜及其應用於相關光電元件之研究。於本研究中，已成功利用水熱法製備奈米結構於氮化鎵系列發光二極體與單晶矽太陽能電池表面，有效提升發光二極體之光析出效率與太陽能電池之光電轉換效率。本研究亦以簡易之水熱法成功製備出單晶/類單晶之氧化鋅薄膜於氮化鎵基板與氧化銦錫基板，並成功製備高性能UV光感測元件與UV光發光二極體，亦已完成退火製程開發，有效降低氧化鋅材料之氧空缺，改善薄膜應用於光電元件特性。
於藉由水熱法製備n型氧化鋅奈米錐於傳統氮化鎵發光二極體表面之研究方面，所開發技術具有低成本、低溫、設備簡易及折射係數調變之優勢，其中，操作電流為350 mA時，表面具奈米尖端結構之氮化鎵發光二極體相較於傳統氮化鎵發光二極體，其光輸出效率增加了36.1%。
於利用氮化矽包覆氮化鎵奈米線結構，進一步提升氮化鎵發光二極體之光析出效率之研究方面，利用水熱法成長氧化鋅奈米線於氮化鎵發光二極體表面作ICP蝕刻之遮罩，製備出表面具氮化鎵奈米結構之發光二極體，再進行PECVD沉積氮化矽薄膜，即完成具折射係數漸變(氮化鎵:2.5薄氮化矽:2矽空氣:1)及奈米結構之氮化鎵發光二極體元件，其中，具折射係數漸變及奈米結構之氮化鎵發光二極體元件於注入電流350 mA時，與傳統氮化鎵發光二極體相較，其光析出效率增加28.7%。
本論文亦利用水熱法製備氧化鋅奈米線於傳統太陽能電池表面，再利用室溫之蝕刻製程形成奈米管結構，最後使用PECVD沉積氮氧化矽作為折射係數漸變層，即完成具折射係數漸變及奈米結構之太陽能電池且與傳統太陽能電池比較，其光電轉換效率增加39.2%。
本研究藉由水熱法進行類單晶之氧化鋅薄膜之選擇性成長，以類單晶氧化鋅薄膜為基材搭配P型氧化亞銅半導體材料，進而製備出異質接面結構之紫外光感測器。此技術具有低溫低壓製程、製程容易、可避免傳統使用氧化鋅奈米線作為UV感測元件之絕緣製程(此製程技術複雜耗時，導致元件成本提高)、較大接面面積與較高之機械應力(與奈米結構比較)優勢。本研究所開發之氧化鋅薄膜/氧化亞銅異質接面結構之UV光感測器，具有數種不同氧化亞銅薄膜厚度調變(250~750 nm)，且擁有良好之整流電特性與優異的紫外光(365 nm)響應，其響應能力(光照與暗室環境下之電流比值)約為55.6倍，響應時間與復歸時間約為20秒與26秒。
為進一步提升氧化鋅薄膜品質，本論文另擇用晶格較匹配的p型氮化鎵基板成長單晶氧化鋅薄膜，並製備異質接面結構之紫外光發光二極體，此技術具有低溫低壓製程、製程簡易、元件製作成本低廉之優勢。所開發之紫外光發光二極體，發光主波長為375 nm。經由退火製程(於氮氣環境下，500oC，10 分鐘)，有效改善漏電流(降低約150%)及整流電特性。
本論文亦於n型氮化鎵基板表面製備具多孔隙結構之p型氧化鋅，且將其應用於紫外光感測器並深入研究。所開發之紫外光感測器，具有數種不同孔隙調變(50~500 nm)且擁有良好之整流電特性與優異的紫外光(365 nm)響應，其響應能力(光照與暗室環境下之電流比值)約為80倍，響應時間與復歸時間約為6秒與7秒。
本論文所開發與研製之氧化鋅奈米結構，已成功提高水平LED之光析出效率36.1%、垂直LED之光析出效率28.7%及傳統太陽能電池之轉換效率39.2%，亦已成功將所開發之單晶/類單晶氧化鋅薄膜及多孔隙結構之p型氧化鋅分別製備成紫外光發光二極體及紫外光感測元件，其中紫外光發光二極體之發光主波長為375 nm，且經由退火製程大幅改善了漏電流(約150%)，而製備之紫外光感測元件亦有極佳之光電響應能力，分別為55.6倍及80倍。根據本論文所建立的材料與元件製備技術基礎，預期於適度之製程參數調變下，將對未來發光二極體、太陽能電池及紫外光感測元件應用有相當之助益。

The dissertation aims at the preparation of ZnO nanostructures and crystalline/quasi-monocrystal films and theirs applications on related optoelectronic devices such as light emitting diodes (LEDs), solar cells (SCs), and ultraviolet photodetectors (UV-PDs). A surface roughening scheme with ZnO-based nanostructures is proposed to improve the light extraction efficiency of GaN-based LED and the energy conversion efficiency of crystalline Si-based SCs. The growth of crystalline (or quasi-monocrystal) ZnO film on p-GaN (or ITO) using the hydrothermal growth (HTG) methods also is proposed. A thermal annealing process for ZnO-based optoelectronic devices is developed together to reduce the amount of oxygen vacancies in the grown ZnO films for improving both the optical and electrical properties.
In the present study, ZnO nanotapers (ZnO-NTs) were grown on the regular horizontal LED (HLED) surface by HTG method. The surface roughening technology using ZnO-NTs offers advantages of low cost and low temperature processing, which facilitates a surface roughening structure with a graded refractive index. Through the use of ZnO-NTs, a considerable improvement in light output power (LOP) of LED by 36.15% at 350 mA as compared to regular HLED has been obtained.
A surface roughening scheme with SiNx-coated GaN nanowire (NW) arrays is also proposed in this work to further improve the LOP of GaN-based vertical LEDs (VLEDs). At first, ZnO NW arrays were grown on the VLEDs surface using HTG method. With ZnO NW as a mask, a dry etching using an inductively coupled plasma reactive ion etching process was conducted on the n-GaN surface with GaN NW arrays. Finally, a SiNx layer was coating on the GaN NW using a plasma-enhanced CVD system and the VLEDs with graded refractive index was obtained. Compared with that of regular VLEDs, the use of SiNx-coated GaN NW arrays leads to an improvement in LOP by 28.7% at 350 mA.
ZnO NWs were also grown on the regular SCs with a SiNx/micropyramid surface by HTG method and then the ZnO nanotubes were formed via the etching process at room temperature atmosphere. Then a SiON layer was coating on the ZnO nanotubes using a plasma-enhanced CVD system and the SCs with graded refractive index were fabricated. Note that the use of SiON-coated ZnO nanotubes increases the energy conversion efficiency by 39.2% under AM1.5G (100 mW/cm2) as compared to that of regular SCs with a SiNx/micropyramid surface.
The preparation of quasi-monocrystal ZnO film and deposition p-Cu2O-film heterojunction (HJ) for UV-PDs are studied and demonstrated. The HJ was formed via the sputtering deposition of p-type copper oxide onto HTG-ZnO-film that offers advantages of low cost, low temperature processing, effective prevention of the p-Cu2O from reaching the substrate during HJ formation and avoidance the possible short-circuit problem usually encountered for ZnO-NW-based UV-PDs. The prepared UV-PDs with different Cu2O thicknesses (250~750 nm) with thermal annealing at 600oC in nitrogen exhibit well-defined rectifying current-voltage characteristics, superior response to UV light illumination with UV light sensitivity as high as 55.6, and rise/fall time of ~20/26 s were obtained.
The growth of single crystalline ZnO film on p-GaN substrate which has small lattice mismatch of 1.8% with ZnO is proposed to further improve the quality of ZnO film. The proposed technology has advantages of low-pressure and low-temperature processing, ease of fabrication, and a relative low cost. A good rectifying diode behavior and 150 % improvement in leakage current at -4 V of n-ZnO/p-GaN UV-LED after thermal annealing was obtained. Strong ultraviolet lights emission from the annealed n-ZnO/p-GaN UV-LED at around 375 nm without defect-related emissions in the visible region are observed from electroluminescence (EL) spectra.
Porous p-ZnO films were grown on the n-GaN epilayer by hydrothermal growth method and the fabrication and characterization of UV-PDs based on p-ZnO/n-GaN HJ are presented. The prepared UV-PDs with different pores sizes of 300~600 nm exhibit well-defined rectifying current-voltage characteristics, superior response to UV light illumination with UV light sensitivity (IUV/Idark) as high as 80, and rise/fall time of ~6/7 s were obtained.
In this study, the surface roughening technology using ZnO-based nanostructures shows a considerable improvement in LOP of GaN-based LEDs by 36.15% and 28.7% as well as in energy conversion efficiency of Si-based SCs by 39.2%. Furthermore, the fabricated UV-LED with thermal annealing has the main lights emissions at around 375 nm and a 150 % improvement in leakage current. Moreover, the prepared p-Cu2O/n-ZnO and p-ZnO/n-GaN UV-PDs exhibit well-defined rectifying current-voltage characteristics, superior response to UV light illumination with UV light sensitivity as high as 55.6 and 80, respectively. According to these results, it is expected that the proposed ZnO nanostructure and crystalline/ quasi-monocrystal films based optoelectronic devices with a suitable fabrication processes tuning could be an effective vehicle for future LED, SCs, and UV-PDs applications.

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