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研究生： 洪敏皓
Hong, Min-Hao
論文名稱： 氧化鋅奈米柱/氧化亞銅異質介面應用在太陽能電池及PVK 緩衝層光檢測器
A study of ZnO nanorods/Cu2O heterojunction applications to solar cells and to photodetectors with a poly-(N-vinylcarbazole) intermediate layer
指導教授： 彭洞清
Perng, Dung-Ching
學位類別： 博士
Doctor
系所名稱： 電機資訊學院 - 微電子工程研究所
Institute of Microelectronics
論文出版年： 2018
畢業學年度： 106
語文別： 英文
論文頁數： 139
中文關鍵詞： 太陽能電池 、氧化亞銅 、氧化鋅奈米柱 、化學水浴法 、高短路電流密度 、氧化鋅 、PVK 、氧化亞銅 、紫外光 、光二極體
外文關鍵詞： solar cells, cuprous oxide, ZnO nanorods, Mirror, Heterojunction, PVK, ultraviolet detection, visible-blind photodetector
相關次數： 點閱：111  下載：2 
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    • 本研究探討氧化鋅奈米柱/氧化亞銅異質介面應用在太陽能電池其短路電流特性及使用PVK 緩衝層之光檢測器其光響應能力。首先在太陽能電池部分,以低成本電鍍製成之半透明氧化亞銅/ 氧化鋅奈米柱太陽能電池達成高短路電流密度（Jsc）9.53 mA/cm2. 首先利用化學水浴法合成高品質氧化鋅奈米柱藉以取代傳統電鍍的氧化鋅薄膜作為載子收集之路徑，如此短路電流密度（Jsc）從1.63到 6.41 mA/cm2，幾乎增加了四倍。接下來減少氧化亞銅吸收層電鍍的厚度來彌補因少數載子漂移及擴散的複合損失(二者長度大約為 100 nm)，因此短路電流密度（Jsc）更進一步的被提高到7.77 mA/cm2。最後將銀鏡沉積於玻璃基板背面來產生額外的光生載子以加強太陽能電池的光吸收，進而達到迄今為止利用低成本電鍍製程之氧化亞銅/ 氧化鋅太陽能電池的最高短路電流密度（Jsc）9.53 mA/cm2。其二在光檢測之應用是以PVK薄膜作為電子阻擋與電洞傳輸層並鑲入具低成本的氧化亞銅薄膜與氧化鋅奈米柱之間，作為具高性能紫外光探測器。氧化亞銅/PVK/氧化鋅奈米柱光探測器在波長360 nm其光響應度為13.28 A/W，在-0.1V的低偏壓低紫外光強度24.9 μW/cm2下具有高偵測率1.03×1013 Jones。紫外光探測器有無 PVK 中間層在-0.5 V偏壓下光暗電流比分別為1.34 × 102和3.99，而可見光拒斥比(R360 nm / R450 nm) 則分別為350 和1.735。在上述的結果中，展示幾個新穎的特徵:(a) 紫外光在氧化鋅奈米柱上所產生的電洞載子能夠穿越PVK層傳輸至氧化亞銅層;(b) PVK緩衝層具有顯著地抑制逆偏漏電流,致使有較大的光電流放大效果;(c) 利用PVK層大幅改善紫外光對可見光拒斥比並在極低的光強度下達到高靈敏度的紫外光偵測能力。

    In solar cell, this study reports the achievement of a high short-circuit current density (Jsc) of 9.53 mA/cm2 for low cost electrodeposited (ED) semi-transparent Cu2O/ZnO nanorod (NR) solar cells. High-quality chemicalbath-deposited ZnO NRs that align with the carrier collection path were used to replace the traditionalsputtered ZnO film. An almost four-fold increase (from 1.63 to 6.41 mA/cm2) in Jsc was obtained with the NRs compared to the level obtained with a sputtered ZnO thin film cell. Decreased the ED Cu2O absorber film thickness is able to compensate for the recombination loss that results from Cu2O's short minority carrier drift and diffusion length (both on the order of 100 nm), further boosting Jsc to 7.77 mA/cm2. Additional photo-generated carriers were created for the semi-transparent solar cells when a silver mirror was deposited on the backside of the glass; this further enhanced absorption and improved Jsc to 9.53 mA/cm2. This is the highest Jsc value reported to date for a low-cost ED Cu2O/ZnO solar cell.
    In photodetector, this study reports a high-performance hybrid ultraviolet (UV) photodetector with visible-blind sensitivity fabricated by inserting a poly-(N-vinylcarbazole) (PVK) intermediate layer between lowcost processed Cu2O film and ZnO nanorods (NRs). The PVK layer acts as an electron-blocking/ hole-transporting layer between the n-ZnO and p-Cu2O films. The Cu2O/PVK/ZnO NR photodetecto exhibited a responsivity of 13.28 A/W at 360 nm, a high detectivity of 1.03×1013 Jones at a low bias of -0.1V under a low UV light intensity of 24.9 μW/cm2. The photo-to-dark current ratios of the photodetector with and without the PVK intermediate layer at a bias of -0.5V are 1.34×102 and 3.99, respectively. The UV-to-visible rejection ratios (R360 nm/R450 nm) are 350 and 1.735, respectively. Several features are demonstrated: (a) UV photo-generated holes at the ZnO NRs can effectively be transported through the PVK layer to the p-Cu2O layer; (b) the insertion of a PVK buffer layer significantly minimizes the reverse-bias leakage current, which leads to a larger amplification of the photocurrent; and (c) the PVK buffer layer greatly improves the UV-to-visible responsivity ratio, allowing the device to achieve high UV detection sensitivity at a low bias voltage using a very low light intensity.

    Contents 中文摘要 I Abstract III ACKNOWLEDGEMENTS V Contents VI TABLE CATIONS IX FIGURE CATIONS X Chapter 1 Introduction 1 §1.1 Introduction of Solar Cell 1 § 1.2 Review of relevant ZnO and Cu2O properties 1 1.2.1 Cu2O thin film and its properties 1 1.2.2 ZnO thin film and its properties 5 §1.3 Introduction of Photodector 8 § 1.4 Review of relevant PVK and ZnO nanorod properties 9 1.4.1 Material properties of PVK thin film 9 1.4.2 ZnO nanorod array thin films as an absorber in solar-blind UV photodetectors 10 Chapter 2 12 Theory and Literature Reviews 12 §2.1 Solar Energy Spectrum 12 §2.2 PN Junction 13 §2.3 Principle of Solar Cell 14 §2.4 PN Junction Photovoltaic I-V Characteristics 16 §2.5 Metal-semiconductor contact 20 §2.6 p-n junction principles 21 2.6.1 p-n junction under equilibrium and various bias conditions 21 2.6.2 The series resistance (Rseries) 24 §2.7 Semiconductor photodector 25 2.7.1 Principle of operation 25 2.7.2 P-n junction photodiodes 25 2.7.3 Photoconductive detectors 26 2.7.4 Responsivity and Detectivity 28 § 2.8 Motivation of the studies 29 2.8.1 Motivation of solor cell 29 2.8.2 Motivation of photodector 33 Chapter 3 Solar Cell Experimental Scheme 35 § 3.1 Experimental materials 35 3.1.1 Substrate 35 3.1.2 Chemicals 35 3.1.3 Target 35 3.1.4 Gas 36 § 3.2 Process Equipments 36 3.2.1 Sputter system 36 3.2.2 Electrochemical Plating System 39 § 3.3 Analytical Instruments 42 3.3.1 SEM and Energy Dispersive X-ray Spectroscope (EDX) 42 3.3.2 X-ray Diffraction (XRD) 46 3.3.3 Alpha-step 49 3.3.4 Solar simulator 50 § 3.4 Process Flow 51 3.4.1 Cleaning of substrate of Indium Tin Oxide (ITO) glass 52 3.4.2 Cuprous oxide electrodeposition 52 3.4.3 ZnO seed sputtering 53 3.4.4 ZnO nanorods chemical bath deposition 55 3.4.5 Transparent electrode of indium tin oxide (ITO) sputtering 55 3.4.6 Metal electrode of silver sputtering 55 Chapter 4 Photo Detector Experimental Scheme 57 §4.1 Experimental materials 57 §4.2 Process equipment 57 4.2.1 Electrochemical deposition system 57 4.2.2 Spin coater 62 4.2.3 Square furnace 63 4.2.4 RF/DC sputtering system 64 §4.3 Analytical instruments 66 4.3.1 Scanning Electron Microscope (SEM) 66 4.3.2 X-ray Diffraction (XRD) 69 4.3.3 Electrical measurement system 70 §4.4 Experimental Flow 72 4.4.1 Indium-tin-oxide (ITO) coated glass substrate 73 4.4.2 Electrodeposition of p-Cu2O thin films 73 4.4.3 Spin-coated PVK layers 74 4.4.4 Sputtered i-ZnO thin films 74 4.4.5 ZnO nanorod arrays (NRAs) grown by chemical bath deposition 75 4.4.6 Sputtered transparent ITO top electrodes 75 Chapter 5 Results and Discussion 76 §5.1 Cu2O/ZnO heterojunction solar cells 76 5.1.1 Analysis of SEM image and XRD pattern 77 5.1.2 Effect of seed thickness for solar cells 80 5.1.3 Effect of zinc oxide thin film and nanorods for solar cells 82 5.1.4 Effect of sparse nanorods 85 5.1.5 Effect of Cu2O thickness for solar cells 87 5.1.6 Silver mirror 91 5.1.7 Summary 92 §5.2 Photodetector based on Cu2O/ZnO nanorods with PVK intermediate layer 97 5.2.1 X-ray diffraction patterns of stacked films 98 5.2.2 Surface morphology and cross-sectional view of Cu2O and ZnO 101 5.2.3 Electrical measurement 105 5.2.4 Photoresponse and detectivity 114 5.2.5 Summary 119 Chapter 6 Conclusions 125 §6.1 Cu2O/ZnO heterojunction solar cells 125 §6.2 Photodetector based on Cu2O/ZnO nanorods with PVK intermediate layer 125 Bibliography 127

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