黃銅礦結構的銅銦鎵硒(CuIn1-xGaxSe2, CIGS)具有高光吸收係數等優點，特別適合應用於可撓式薄膜型太陽能電池。但是CIGS成份複雜，薄膜成長較爲困難，目前還沒有一種成長方法可以完全達到高純、快速、廉價等要求。本研究嘗試利用脈衝雷射沉積技術(Pulsed Laser Deposition, PLD)成長CIGS薄膜，由於雷射具有超快加熱速率與超高溫的特性，可將靶材的成份按原比例蒸鍍到基板上，即所謂的同成分蒸發，因而特別適合用來成長多組元成份的CIGS薄膜。本論文探討PLD成長參數、元素摻雑對薄膜的相純度、結構以及光電性質的影響，主要結論依薄膜成份分為三個部分概括如下：
(1)未摻雑之CIGS: 以純元素粉末製作比例為Cu:In:Ga:Se=1:0.7:0.3:2的靶材，在燒結溫度500oC持溫10小時，可獲得結晶性良好的CIGS (x0.3)純相。隨後利用PLD在鈉玻璃基板上成長CIGS薄膜，在基板溫度300oC時成長的CIGS薄膜可獲得良好的黃銅礦結構，且EDS成份分析結果證實靶材成分基本上按原比例沉積到基板。在調整雷射能量密度時發現，當能量密度過高(12 J/cm2)時會有氣相成核的情況發生，而且會造成靶材表面有明顯的刻痕，本實驗最合適的雷射能量約為5.5 J/cm2。將脈衝雷射光頻率從1 kHz降低至5 Hz時，薄膜表面會出現大顆微粒，直徑約為100~200 nm。1 kHz與5Hz成長的CIGS薄膜在製作成簡易太陽能電池後，初步測得的光電轉換效率分別為0.23%與0.11%，開路電壓分別為0.32及0.16 V。
(2)摻Na之CIGS: 利用添加Na到自製CIGS靶材的方式，可直接成長CIGS:Na薄膜，以便解決PI基板無法像鈉玻璃基板那樣，在高溫時能提供微量Na離子來增加CIGS的轉換效率。實驗結果發現，添加Na元素(1~10 at%)的CIGS靶材在燒結溫度500oC持溫12小時的製作條件下，可以得到CIGS純相。在基板溫度300oC時，利用CIGS:1 at%Na靶材在可撓式PI基板上成長的薄膜，其結晶性較好且具有純的CIGS相，但如果靶材Na含量過高(>1 at%)，則會有二次相出現或薄膜結晶性明顯變差。隨著薄膜中Na含量從1.8 at%增加到7.8 at%，薄膜的能隙會從1.2 eV 增加到1.6 eV，同時載子濃度也隨著增加(10161018 cm-3)，進而導致電阻率降低。藉由拉曼光譜分析得知，這是因為用含Na 5 at% 或10 at%靶材成長的薄膜中有二次相CuSe存在的緣故。
(3)過渡金屬取代Ga之CIGS，即CuIn1-xMxSe2 (M=Cr、V、Ti): 利用過渡金屬元素添加進入CuInSe2 方式製作Cu(In0.8M0.2)Se2 (CIMS)靶材，在燒結溫度700oC持溫8小時可獲得CIMS純相靶材。在室溫下PLD成長可以獲得具有微結晶的CIMS薄膜，隨後在200~500oC對薄膜進行退火處理，其中400oC退火可以獲得最佳的結果，晶粒大小從3 nm(室溫成長)增大為19 nm且成份不會因爲在高溫過度揮發而偏離化學計量比太多，在拉曼光譜分析中僅觀察到屬於黃銅礦結構的振動特徵峰，而之前在室溫成長薄膜中出現的CuSe特徵峰已消失。經實驗分析，CIMS薄膜實際成份分別為CuIn0.91Cr0.09Se2、CuIn0.86V0.14Se2與CuIn0.92Ti0.08Se2，其對應的能隙值依序為1.23、1.30與1.36 eV，此結果顯示摻雜微量過渡金屬元素對於優化CuInSe2能隙的效果要比傳統的CuIn0.7Ga0.3Se2來得更加明顯。

Pulsed laser deposition (PLD) was used to grow the chalcopyrite-structured CuIn0.7Ga0.3Se2 (CIGS) films for photovoltaic applications. All the targets for PLD were synthesized from pure elements of Cu, In, Ga and Se by the solid state reaction method. CIGS films grown at 300 oC on the soda-lime-glass (SLG) substrates showed a pure phase with the chalcopyrite structure, which had the bandgap of about 1.25 eV. The films grown with the laser fluence of 5.5 J/cm2 and pulse repetition rate of 1 kHz exhibited best phase-purity and surface morphology (i.e. fewest numbers of large particulates). Because Na diffusion from SLG substrates to the CIGS films was known to enhance the photovoltaic efficiency, sodium was added into the homemade CIGS targets for the growth of CIGS:Na films on the flexible PI substrates which did not contain Na. 1-at% Na doped CIGS films deposited on PI at 300 oC showed a pure phase with a fairly good crystallinity. Higher Na doping led to a poorer crystallinity as well as the occurrence of the secondary phase CuSe. Transition-metal (TM) substituted films, i.e. CuIn1-xMxSe2 (CIMS, M=Cr, V and Ti), were also grown by PLD on SLG at room temperature, which showed the right phase with a very small grain size of 3 nm. The grain size was increased to 19 nm by a post-deposition annealing at 400 oC, which also improved the homogeneity of film composition. Hall-effect measurements revealed that the CIMS films had lower carrier concentration but higher mobility than CIGS films. The bandgap of CIMS films was increased, varying from 1.08 eV in CuInSe2 (CIS) to 1.23 eV in CuIn0.91Cr0.09Se2, 1.30 eV in CuIn0.86V0.14Se2 and 1.36 eV in CuIn0.92Ti0.08Se2. Compared to Ga in CIGS, the TM elements studied in this work were much more effective to increase the bandgap of CIS.

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