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標題: | P-型非晶型鈣摻雜銅鋁氧化物及大氣噴射電漿氧化亞錫薄膜製程之研究 A study on P-type amorphous Ca doped CuAlOx and atmospheric-pressure-plasma-jet processed SnO thin films |
作者: | Guan-Wei Lin 林冠葦 |
指導教授: | 陳建彰(Jian-Zhang Chen) |
關鍵字: | 濺鍍,銅鋁氧化物,氧化亞錫,大氣電漿, sputter,copper aluminum oxide,tin monoxide,APPJ, |
出版年 : | 2014 |
學位: | 碩士 |
摘要: | 銅鋁氧化物以及氧化亞錫為具有潛力的P型透明導電材料。本實驗主要分為兩大部分,第一部分探討鋁/銅比例對鈣摻雜銅鋁氧化物薄膜性質之影響,並進一步將其應用在異質接面二極體。第二部分則將大氣噴射電漿系統應用於氧化亞錫薄膜製程。
第一部分的實驗中,使用室溫磁控濺鍍的方法沉積鈣摻雜銅鋁氧化物薄膜(CuAlx-0.2Ca0.2O, x=1, 1.25, 1.5, 1.75, 2)於玻璃基板及可撓性PET基板上,接著分析其組成成分、結晶結構、電性、光學性質、表面粗糙度及紫外光響應度。 室溫濺鍍之鈣摻雜銅鋁氧化物薄膜為非晶態,其光學穿透率以及電阻率皆隨著鋁/銅比例的增加而提升。適量的鈣摻雜下,CuAl0.8Ca0.2O薄膜之電阻率較無鈣摻雜的CuAlO2薄膜小了105倍。沉積在PET基板上之薄膜的電阻率稍高於沉積在玻璃基板上,且光學穿透率也較低。鈣摻雜銅鋁氧化物薄膜的表面都相當平整,大部分薄膜之方均根粗糙度皆不超過1 nm。而沉積於PET基板上的CuAl0.8Ca0.2O薄膜隨著紫外光強度增強其電阻率降低,且其電阻率在向外彎的狀態下會下降,向內彎時則上升。 在元件方面,我們成功製作鈣摻雜銅鋁氧化物與氧化鋅之異質接面二極體。鈣的摻雜對於提升二極體特性有相當明顯的幫助,且其電流密度隨著鋁/銅比例上升而變小。當鋁/銅比例為1.3時,其整流比達到25.37,啟動電壓為4.97 V,而崩潰電壓為-11.24 V。實驗中成功將此異質接面二極體製作於PET基板上,其電流密度會隨著紫外光強度以及試片彎曲程度上升。當向外彎的程度越大時,二極體對紫外光的響應度越高。 第二部分實驗主要研究大氣噴射電漿系統於氧化亞錫薄膜之製程。分別以濺鍍沉積不同氧通量比例的氧化亞錫薄膜以及金屬錫薄膜,接著以大氣噴射電漿系統進行不同時間的處理。氧化亞錫薄膜於大氣噴射電漿處理後呈現氧化亞錫的結晶結構,且隨氧通量比例提升主要結晶相從(1 1 0)相轉換為(1 0 1)的相。其薄膜穿透率與薄膜含氧比例皆隨氧通量比例以及電漿處理時間而提升。從霍爾量測以及Seebeck係數皆顯示其為N型導電性。而金屬錫薄膜於大氣噴射電漿後,有、無側孔之大氣電漿處理之結果並沒有太大的差異。薄膜之結晶結構以(1 0 1)之氧化亞錫為主,其晶粒粒徑約在20-30 nm之間,但大小隨電漿處理時間沒有明顯的規律。薄膜穿透率隨處理時間上升。由Tauc’s plot可觀察到其直接能隙有隨處理時間越長變大的趨勢,且在長時間電漿處理後,其值約固定在2.7 eV左右。金屬錫薄膜表面具有相當多的孔隙,且在電漿處理後結構並沒有明顯的變化,但可以觀察到隨電漿處理時間越長,出現越來越多黑色區塊以及顆粒,此現象在有側孔之電漿處理的薄膜上特別明顯。從霍爾量測之結果,薄膜呈現不穩定的導電性質。而Seebeck之量測結果則顯示薄膜在電漿處理前為N型導電性,長時間無側孔之電漿處理後轉變成P型導電性。 This thesis focuses on two parts. First part is the study on p-type amorphous Ca-Cu-Al-O thin films and diodes. The second part is the fabrication of SnO thin film using atmospheric pressure plasma jets. In the first part of the experiment, sputtering is used to deposit CuAlx-0.2Ca0.2O, x=1, 1.25, 1.5, 1.75, 2; target compositions) thin films on glass and PET substrates. The composition, microstructure, crystallinity, electrical properties, optoelectronic properties are investigated. Room-temperature sputtered CuAlx-0.2Ca0.2O is amorphous. The transmittance and resistivity increase with the Al/Cu ratio. The resistivity of CuAl0.8Ca0.2O is about 5 orders of magnitude below that of CuAlO2. The surfaces of as-deposited are rather smooth with Rrms < 1 nm. The resistance decreases with the UV illumination. The outward bending (tensile strain on the film) reduces the resistance but inward bending (compressive strain on the film) increases the resistance. The photocurrent also increases with UV intensity. CuAlx-0.2Ca0.2O/ZnO are also used for the p-layer/n-layer of the diodes. Ca doping significantly improves the diode characteristics. The current density decreases with Al/Cu ratio. As Al/Cu composition ratio reaches 1.3, the diode exhibits a rectifying ratio of 25.37, a threshold voltage of 4.97 V, and a reverse breakdown voltage of -11.24 V. We also successfully implement this diode on PET substrate. The photocurrent increases with UV intensity and bending curvature. The second part of the experiment is concerning the fabrication processes of SnO thin films using atmospheric pressure plasma jets. SnOx is sputter-deposited with oxygen partial pressure in sputtering gas; pure Sn metal film is deposited with pure Ar sputtering atmosphere. After APPJ treatment, SnOx film reveals SnO crystal structure; the preferred orientation changes from (1 1 0) to (1 0 1). The transmittance and oxygen content of the SnOx film increase with APPJ treatment duration. Although SnO phase is identified, but n-type conductivity is confirmed by Hall measurements and Seebeck coefficient measurements. The direct bandgap increases with APPJ treatment time and levels off at 2.7 eV. Longer APPJ treatment time causes the precipitate the Sn. Hall measurement shows unstable sign of carrier type, indicating the complication of material properties. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/56815 |
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