透明導電膜兼具低電阻率及高可見光穿透率，為光電產業應用廣泛的透明電極材料。其中以ZnO為母材之薄膜，由於Zn蘊藏量豐富且薄膜圖形蝕刻容易，同時藉由施體摻雜可穩定及改善薄膜電性，故其在光電元件應用上極具發展潛力。此外，p型ZnO薄膜的製備帶動ZnO同質接面的研究風潮，使得ZnO薄膜在半導體材料的應用上更為廣泛。同時， ZnO與Cu2O所製備之異質接面，在太陽能電池的研究也是近年來ZnO應用熱門課題。
本研究以2wt%Al2O3-ZnO陶瓷為靶材，利用射頻磁控濺鍍法製備透明導電薄膜。全文共分三部分，第一部分為探討ZnO:Al薄膜結構及性質與製程參數及熱處理條件之關係，並應用於酒精氣體感測。第二部分探討p型ZnO之製作，以期增廣ZnO之應用性。利用N2O與Ar混合氣體作為反應氣體，探討不同體積分率與Al-N codoped ZnO薄膜對結構及光電性質之影響，並探討熱處理對性質改善之可行性。第三部分為在不同優選面氧化亞銅上製備ZnO:Al 薄膜作為異質接面，探討ZnO:Al製作之參數對於異質接面結構與光伏特性之影響。
研究結果得知，ZnO:Al薄膜沈積速率隨濺鍍功率的增加而加快，且利用濺鍍法製備之薄膜皆呈(0002)優先成長，並不因濺鍍功率與基板溫度而改變。基板加溫及鍍膜熱處理後，ZnO:Al薄膜之(0002)繞射峰往高角度位移，發現薄膜殘留應力釋放。此外由表面形態觀察亦發現因加熱晶粒成長現象。當濺鍍功率為120 W時，薄膜之電阻率較低，在基板溫度為250℃時，可獲得進一步的降低。500℃氫氣氛熱處理1 hr的ZnO:Al薄膜，具有最低之電阻率5.15×10-4 Ω•cm，電子濃度及移動率分別為8.03×1020 cm-3及15.1 cm2V-1s-1。在氧氣氛下熱處理，薄膜電阻率明顯升高。對於ZnO:Al薄膜穿透率之量測發現，在不同濺鍍功率及基板溫度下，薄膜之穿透率在可見光範圍(380 nm至760 nm)內平均達90%以上。而氫氣氛熱處理後之薄膜，短波長範圍之穿透率明顯提升，且其吸收端有往短波長藍移現象；在氧氣氛熱處理，薄膜穿透率則明顯下降，且吸收端有往長波長紅移之情況。在酒精氣體感測應用上，ZnO:Al薄膜具有快速反應及回復的特性，對不同濃度之酒精氣體皆具感測再現性。當酒精氣體濃度為400ppm操作溫度為250℃時，ZnO:Al薄膜之靈敏度約為20。
不同N2O/(N2O+Ar)體積分率，Al-N codoped ZnO薄膜沈積速率隨體積分率上升，速率明顯減緩，同時薄膜(0002)繞射峰強度降低且寬化，顯示薄膜結晶性降低，但薄膜仍具(0002)優先成長之特性，且並無其他繞射峰出現。薄膜之導電形態，隨N2O體積分率提高至20%，薄膜由n型轉為p型；體積分率為30%時，p型Al-N codoped ZnO薄膜有較低之電阻值2.57 Ω•cm，電洞濃度及移動率分別為2.53×1017 cm-3及9.6 cm2V-1s-1；體積分率提升至60%以上時，薄膜則由p型反轉為n型。不同體積分率所得之Al-N codoped ZnO薄膜之可見光穿透率平均皆在85%以上，通入N2O氣體時，吸收端有紅移現象。然而在Ar、O2及N2氣氛中熱處理後，薄膜之p型導電形態消失，可知N之摻雜並不穩定。
製備ZnO:Al/Cu2O異質接面時，因氧化亞銅之(111)與ZnO:Al薄膜間晶格失配程度較低，ZnO:Al薄膜成長以(0002)為優選面；而在氧化亞銅之(200)上，有當基板加溫時，ZnO:Al薄膜有(0002)優選生長之傾向。在光照條件為83.2 mW/cm2下，ZnO:Al/Cu2O異質接面之光伏特性的量測，在室溫時，ZnO:Al/(111)-orientated Cu2O因晶格失配較小而有較高之轉換效率。適當降低各薄膜之厚度，ZnO:Al(200 nm)/(111)-orientated Cu2O(1 μm)異質接面具有較佳之轉換效率0.22%，其開路電壓、短路電流密度及填充因子分別為0.15 V、4.3 mA/cm2及0.29。

Due to the low resistivity and high transmittance in visible spectrum, transparent conducting films are comprehensively applied in optoelectronics. Among them, ZnO is easily etched in process and the electrical properties can be further improved by donor doping as well as the abundance of Zn, making ZnO-based films more potential. Besides, the fabrication of ZnO-based homojunction using p-type ZnO films indicates the extensive applications of ZnO. In addition, the recent research of ZnO/Cu2O heterojunctions in solar cells also attracts many interesting attentions.
In this study, 2wt%Al2O3-ZnO is used as target to deposit transparent conducting films by RF magnetron sputtering system. Three issues investigated in this study are (1) the effects of deposition and annealing parameters on the structural, electrical and optical properties of ZnO:Al films as well as the applications of ZnO:Al films in the ethanol gas sensor detection; (2) the fabrication of p-type Al-N co-doped ZnO films by different N2O/(N2O+Ar) volume ratios and the effects of annealing condition on the structural, electrical and optical properties of Al-N co-doped ZnO; (3) the effects of deposition parameters on the structural and photovoltaic properties of ZnO:Al/Cu2O heterojunctions for (200) and (111)-orientation Cu2O.
From the results, the ZnO:Al film grows with the preferred (0002) plane and its deposition rate increases as the RF power increases. After the substrate heating and post-deposition annealing, the grain growth is observed and (0002) diffraction peak shifts to high 2θ position, indicating the relaxation of residual stress in the films. As the RF power used is 120 W, the ZnO:Al film has a low resistivity that can further be reduced with the substrate heating at 250℃. After annealing at 500℃ in H2 for 1 hr, the lowest resistivity of 5.15×10-4 Ω•cm is obtained with the electron concentration and mobility of 8.03×1020 cm-3 and 15.1 cm2V-1s-1, respectively. For various RF powers and substrate temperatures, the transmittance of ZnO:Al films is higher than 90% in average during the visible spectrum. After annealing in O2, the absorption edge has a red-shift; however, it has a blue shift for annealing in H2. For the application as a ethanol gas sensor, ZnO:Al films have a quick response-recovery characteristics and the sensitivity is about 20 with the ethanol concentration of 400 ppm at the operating temperature of 250℃.
For the fabrication of p-type Al-N co-doped ZnO films, the deposition rate decreases as the N2O/(N2O+Ar) volume ratio increases. At the same time, the (0002) diffraction peak broadens but decreases in intensity, indicating the degradation of the thin-film crystallinity. As the volume ratio increases to 20%, the conduction type turns from n type to p type. With the ratio of 30%, p-type Al-N co-doped ZnO film has a low resistivity of 2.57 Ω•cm with the hole concentration and mobility of 2.53×1017 cm-3及9.6 cm2V-1s-1, respectively. When the ratio is larger than 60%, the conduction type returns to n type. For various N2O volume ratios, the transmittance of Al-N co-doped ZnO films is higher than 85% and the absorption edge shows a red-shift with the introduction of N2O.
Using (111)-orientated Cu2O films as substrates for the fabrication of ZnO:Al/Cu2O heterojunctions, the ZnO:Al films deposited on Cu2O films with or without substrate heating show a preferred (0002) due to the small lattice mismatch. For (200)-orientated Cu2O films, substrate heating is helpful for the growth of ZnO:Al films with a preferred (0002). Under the illumination condition of 83.2 mW/cm2, the conversion efficiency of ZnO:Al/(111)-orientated Cu2O heterojunction is higher than that of ZnO:Al/(200)-orientated Cu2O heterojunction. With an appropriate modification of thickness, ZnO:Al(200 nm)/(111)-orientated Cu2O(1 μm) heterojunction has the best conversion efficiency of 0.22% in this study with the open-circuit voltage of 0.15 V, short-circuit current density of 4.3 mA/cm2 and fill-factor of 0.29.

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