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標題: 以原子層沉積系統製備氧化鋁鈍化薄膜應用於射極鈍化背接觸太陽電池
Preparation of Al2O3 Thin Films by Atomic Layer Deposition Applied to Passivated Emitter and Rear Cell
作者: 楊智翔
Chih-Hsiang Yang
關鍵字: 射極鈍化背接觸太陽能電池;空間陣列式原子層沉積系統;固定負電荷;介面缺陷;表面形貌;高分子球;二甲基甲酰胺;Passivated Emitter and Rear Cells;Non-vacuum Spatial ALD;Interfacial Trap Density;Negative Charge;Surface Morphologies;Polystyrene Spheres;Dimethylformamide
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本研究改變水流量、製程溫度及退火溫度製備氧化鋁薄膜得到不同的材料結構特性與電性。氧化鋁薄膜帶電的原因是來自於薄膜內不同配位數的氧鋁結構所致,當四面體的四氧化鋁離子結構與八面體的六氧化鋁結構比值越高時,氧化鋁較傾向帶負電。介面的化學鈍化則跟氧化鋁與矽晶片之間的二氧化矽及反應時所產生的氫原子有關,當氧原子與氫離子能有效填補表面的懸浮鍵時表面缺陷能有效降低介面缺陷密度,研究結果發現當水流量為500 sccm時,固定負電荷為-2.7×1012 cm-2、介面缺陷為7.15 ×1012 eV-1cm-2,此時表面複合速率為40.5 cm/s; 當製程溫度升至170°C時固定負電荷為-4.59×1012 cm-2、介面缺陷為6.98 ×1012 eV-1cm-2,表面複合速率為41.55 cm/s; 當退火溫度為450°C時固定負電荷為-1.25×1012 cm-2、介面缺陷為6.71 ×1012 eV-1cm-2, 表面複合速率為37.5 cm/s。為了解決在沉積氧化鋁時因氫氣或水氣的流動所產生的氣泡,我們採用感應耦合電漿化學氣相沉積系統沉積一層薄氧化矽作為界層及減薄氧化鋁厚度同時沉積氮化矽薄膜作為氧化鋁的保護層兩種方法,最終優化的太陽電池開路電壓為0.647 V、短路電流為38.2 mA/cm2、填充因子為0.776,而效率為19.18 %。在此章節中,我們歸納出主要影響少數載子生命週期表現的是介面缺陷的多寡,其次才是固定負電荷的強弱。
本論文也改變蝕刻時間,讓矽晶片的背面產生不同的形貌變化,接著沉積氧化鋁薄膜,研究背表面形貌對於超量少數載子行為的影響。結果發現當氧化鋁沉積在幾乎平坦的背表面會與氧化鋁形成良好的披覆,獲得較高的載子生命週期,長波長頻譜響應也微量增加,最終以平坦背表面所製成的太陽電池可得到開路電壓0.662 V、短路電流為36.69 mA/cm2、填充因子為0.793,轉換效率為19.27 %。
有別於傳統的雷射開孔技術,本研究採用旋轉塗佈方式將球狀高分子聚合物均勻分散在基板背表面,透過後續氧化鋁薄膜的後退火製程將高分子球氣化並留下孔洞,相較於雷射技術,此開孔方法能有效減少因雷射高能量所造成的基板損傷,微幅提升開路電壓,將不同分佈比例的試片製成電池後比較其電性特性發現當孔洞覆蓋率為2.88 %時可得到最佳效能為開路電壓0.622 V、短路電流為36.9 mA/cm2、填充因子為0.779,轉換效率為17.88 %,略低於雷射開孔製程的17.99 %,主要是因為雷射製程較能均勻地排列孔洞得到較高的填充因子所致。
本研究也利用低成本的旋轉塗佈技術將氧化矽與氧化鈦混合溶液均勻地噴塗在太陽電池前表面,取代原有的氮化矽作為抗反射層,在退火過程中因為薄膜應力分佈不均容易造成膜裂而影響光學特性。為改善薄膜品質,我們在溶液中滴入二甲基甲酰胺,可有效改善混和薄膜膜裂問題,使得其平均反射率下降約9 %。經過50次的再現性測試中發現,雖然混合膜應用於太陽電池元件所得到之平均效率約16.3 % 略低於市售電池的16.8 %,但生產成本卻可大幅下降。此結果顯示旋轉塗佈製備抗反射層技術有其潛力應用於現行的太陽能電池產線上。
最終我們將上述優化過後的參數與結構整合並製備成大面積的射極鈍化背接觸太陽能電池,轉換效率約為20.5 %, 其開路電壓為0.66 V、短路電流為39.16 mA/cm2、填充因子為0.793;而目前市售的射極鈍化背接觸太陽電池平均轉換效率約為21.2 %, 開路電壓0.667 V、短路電流為40.32 mA/cm2、填充因子為0.788。兩者相比可發現開路電壓與填充因子差距很小,主要的差距在於短路電流,業界的電流較高主要原因為電池入光面的粗電極條數較多,易於取出自由載子。

Compared to traditional monocrystalline silicon solar cells, passivated emitter and rear cells (PERC) feature as its rear-side passivation stacks of aluminum oxide and silicon nitride (Al2O3/SiNx), which can reduce the recombination velocity and enhance the absorption of long-wavelength incident light. Currently plasma-enhanced chemical vapor deposition (PECVD) technique becomes a good choice instead of plasma-assisted atomic layer deposition system (ALD) for depositing Al2O3 films due to capacity requirement. In this thesis, high quality Al2O3 films are prepared by using self-developed non-vacuum spatial ALD with deposition rate of 0.16 nm/cycle. The deposition and annealing conditions are investigated to estimate properties of Al2O3 films. We also have investigated other structural topics such as rear-side surface morphologies, novel rear-side opening technique and the antireflective coating (ARC) material. Finally all the concepts are merged to fabricate a PERC.
The passivation effect of Al2O3 films could be divided into chemical passivation and field effect passivation, which are mainly related to interfacial trap density (Dit) and negative charge (Qf) of Al2O3 films, respectively. The interfacial SiO2 films and hydrogen atoms can effectively passivate dangling bonds to prevent carriers being trapped. The root cause for the charges of Al2O3 is determined by fourfold-coordinated AlO4 tetrahedral configuration. Another stable sixfold-coordinated AlO6 octahedra also exist within the Al2O3 bulk. The more the ratio of AlO4 sites to AlO6 sites, the higher the negative charges. Experimental result shows that as H2O carrier flow reaches 500 sccm, the Qf and Dit are -2.7×1012 cm-2 and 7.15 ×1012 eV-1cm-2, respectively, leading to the surface recombination velocity (Smax) 40.5 cm/s; When deposition temperature is 170°C, the Qf and Dit are -4.59×1012 cm-2 and 6.98 ×1012 eV-1 cm-2, with a corresponded Smax of 41.55 cm/s; The Qf and Dit are -1.25×1012 cm-2 and 6.71 ×1012 eV-1cm-2, the corresponded Smax is 37.5 cm/s, after the post-annealing treatment was performed to Al2O3 films. The blisters which form at the Si/Al2O3 interface occur under an external load in the presence of a tensile residual stress due to the effusion of H2 and H2O. Two approaches are proposed to solve it. First a stoichiometric silicon is deposited on silicon surface by inductively coupled plasma chemical vapor deposition to block blisters. The other method is to reduce the thickness of Al2O3 as well as increase the post-annealing temperature to out-gassing the interior gases. The optimized PERC with the improved triple-layer SiO2 /Al2O3 /SiNx:H stacked passivation film has an obvious gain in open-circuit voltage (Voc) and short-circuit current (Jsc). The electrical performance of the optimized PERC with the Voc of 0.647 V, Jsc of 38.2 mA/cm2, fill factor of 0.776, and the efficiency of 19.18 % can be achieved.
Various rear-side surface morphologies were obtained through different etching treatments. We compare the PERCs with standard etching treatment and further polishing processes on rear-side surfaces. Experimental results show that compared with the unpolished cell, the polished cell attains superior electrical performance, particularly in Voc and Jsc, because of the more effective rear-side surface passivation and reabsorption of long-wavelength light. Both improvements raise the conversion efficiency to 19.27 %, with the Voc of 0.662 V, Jsc of 36.69 mA/cm2, and FF of 0.793.
Instead of using the traditional laser ablation process, this thesis demonstrates spin-coated polystyrene spheres (PS) to create local openings on the rear side of PERCs. Effects of PS concentration and post-annealing temperature on PERC performance are investigated. The experimental results show that the PS are randomly distributed on wafers and no PS are joined together at a spin rate of 2000 rpm. The PS can be removed at a temperature of 350°C, leaving holes on the passivation layers without damaging the wafer surfaces. As compared to the laser opening technique with the same contact fraction, the PS opening technique can yield a higher minority effective lifetime, a higher Voc, and a slightly higher Jsc. Although the fill factor of the PS opening technique is lower owing to non-optimized distribution of the openings, the conversion efficiency of the devices is comparable to that of devices prepared via the laser opening process.
Composite silicon dioxide-titanium dioxide (SiO2-TiO2) films are deposited on a large area of 15.6 × 15.6 cm2 textured multicrystalline silicon solar cells to increase the incident light trapped within the device. For further improvement of the antireflective coatings (ARCs) quality, dimethylformamide (DMF) solution is added to the original SiO2-TiO2 solutions. DMF solution solves the cracking problem, thus effectively decreasing reflectance as well as surface recombination. The ARCs prepared by sol-gel process and PECVD on multicrystalline silicon substrate are compared. The average efficiency of the devices with improved sol-gel ARCs is 16.3 %, only 0.5 % lower than 16.8 % of devices with PECVD ARCs.
Eventually a PERC based on all concepts mentioned above is realized on a 15.6 × 15.6 cm2 p-type solar grade silicon wafer. The conversion efficiency is 20.5 %, slightly lower than 21.2 % of the PERC from the industrial. The main factor in around 0.7 % difference can be attributed to the amounts of front side bus bars, which collect minority carrier lifetime. The results represents that the spatial ALD utilized in this thesis has high potential to be used in industrial production line.
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