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The p-type amorphous boron carbon thin film alloy prepared by radio-frequency reactive sputtering/plasma-enhanced chemical vapor deposition and its applications for solar cells
|關鍵字:||碳基;Carbon-based;硼;薄膜合金;反應式濺鍍;電漿輔助化學氣相沉積法;填充因子;太陽能電池;Boron;Thin film alloys;Reactive sputtering;Plasma-enhanced chemical vapor deposition(PECVD);Fill factor;Solar cells||出版社:||材料科學與工程學系所||引用:|| J. Robertson. Diamond-like amorphous carbon. Materials Science and Engineering: R: Reports, 2002; 37 (4–6): 129–281.  H. Zhu, J. Wei, K. Wang, D. Wu. Applications of carbon materials in photovoltaic solar cells. Solar Energy Materials and Solar Cells, 2009; 93 (9): 1461–70.  K.S. Novoselov, A.K. Geim, S.V. Morozov, D. Jiang, Y. Zhang, S.V. Dubonos, I.V. Grigorieva, A.A. Firsov. Electric field effect in atomically thin carbon films. Science, 2004; 306 (5696): 666–9.  K.S. Novoselov, A.K. Geim, S.V. Morozov, D. Jiang, M.I. Katsnelson, I.V. Grigorieva, S.V. Dubonos, A.A. Firsov. Two-dimensional gas of massless Dirac fermions in graphene. Nature, 2005; 438 (7065): 197–200.  A.K. Geim, K.S. Novoselov. The rise of graphene. Nature Materials, 2007; 6 (3): 183–91.  H.W. Kroto, J.R. Heath, S.C. 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當在固定100 nm的薄膜厚度下，改變不同的射頻功率，其實驗結果指出：當射頻功率由100 W增加至500 W，非晶質硼碳薄膜合金的沉積速率受到B/C比例增加的影響，些微地由68.4 nm/min減少至60.0 nm/min，而其B/C比例由0.0031增加至1.03。當射頻功率為300 W時，非晶質硼碳薄膜合金具有最高的石墨化程度及sp2碳鍵結（其ID/IG值為0.80），所以具有最低1.83 eV的光學能隙值（Eg）與2.16×104 Ω•cm的電阻率。此外，所有的非晶質硼碳薄膜合金皆具p型半導體特性。當射頻功率為300 W時，a-BC/n-Si二極體具有最低279 Ω的串聯電阻與4.90的理想因子值。另一方面，非晶質硼碳薄膜合金的楊氏模數E和硬度H值會受到sp2碳含量的影響。因此，使用射頻反應式濺鍍/電漿輔助化學氣相沉積法透過控制射頻功率之沉積參數，預期能對非晶質硼碳薄膜合金的結構及特性進行改質。
當在固定623 K的退火溫度與30 nm的薄膜厚度下，改變射頻功率從100至500 W，其實驗結果亦顯示：非晶質硼碳薄膜合金在300 W的射頻功率時，具有最大的ID/IG值為1.49。因此，可以預期在射頻功率為300 W製備的非晶質硼碳薄膜合金具有最大的石墨化程度與sp2碳鍵結。
當在固定300 W的射頻功率和30 nm的薄膜厚度下，改變退火溫度從未退火至673 K，其實驗結果顯示：當退火溫度為623 K時，非晶質硼碳薄膜合金具有較少的懸掛鍵缺陷，而其光學能隙值為1.90 eV。此外，在退火623 K後，a-BC/n-Si二極體的串聯電阻和理想因子分別為98 Ω和2.43。而a-BC/n-Si元件在未退火和經623 K退火後的內建能障電壓分別為0.45 V與0.88 V。
在本研究中，可以發現經623 K退火後的a-BC/SiO2/n-Si接面元件，在20 mW/cm2的光強度照射後，具有高達93.4%的填充因子和6.3%的光電轉換效率，並且優於文獻上報導過的a-BC/Si接面元件的結果。當施加電壓為0.2 V時，a-BC/SiO2/n-Si二極體的理想因子為1.70。填充因子的增加是歸因於在高溫退火後，硼原子摻雜進入碳薄膜中造成sp2鍵結團簇增加的影響。此外，利用射頻反應式濺鍍/電漿輔助化學氣相沉積法於n型矽基材上製備非晶質硼碳薄膜合金，形成a-BC/SiO2/n-Si太陽能電池，及其有無原生氧化SiO2介面層之影響也在本論文中討論。薄的原生氧化SiO2介面層在Au/a-BC/SiO2/n-Si/Al太陽能電池效能上扮演了一關鍵的角色。因此，考量奈米級厚度、透明的、低成本，與容易大量製造的特點，非晶質硼碳薄膜合金可以被應用在光伏太陽能電池和其他光電元件上。
The effects of different process parameters on the characteristics of p-type amorphous boron carbon (a-BC) thin film alloys prepared by radio-frequency (RF) reactive sputtering/plasma-enhanced chemical vapor deposition (PECVD) are investigated. The process parameters, such as RF powers, different RF powers at the fixed annealing temperature of 623 K, and annealing temperatures, are considered. RF reactive sputtering/PECVD combines RF reactive sputtering and RF-PECVD; is not dangerous for boron doping, and has all of the advantages of chemical vapor deposition (CVD). Moreover, the p-type a-BC thin film alloys are deposited on n-type silicon (n-Si) substrates to fabricate photovoltaic devices, and their applications for solar cells are discussed.
When changing RF powers at a fixed film thickness of 100 nm, experimental results indicate that as the RF power increases from 100 to 500 W, the deposition rate of a-BC thin film alloys slightly decreases from 68.4 to 60.0 nm/min that is resulted from the increase of the B/C ratio, and the B/C ratio in the thin film alloys increases from 0.0031 to 1.03. The a-BC thin film alloy prepared at the RF power of 300 W has a maximum graphitization degree and sp2 carbon bonds (its ID/IG value is 0.80), so it has the lowest optical band gap (Eg) of 1.83 eV and electrical resistivity of 2.16×104 Ω•cm. All the a-BC thin film alloys prepared with different RF powers are p-type. As the a-BC thin film alloy prepared at the RF power of 300 W, the a-BC/n-Si diode possesses the lowest series resistance of 279 Ω and an ideality factor of 4.90. On the other hand, the trend of Young''s modulus (E) and hardness (H) of a-BC thin film alloys is consistent with the ID/IG and Eg values. This indicates that the E and H of a-BC thin film alloys are affected by the sp2 carbon content. Consequently, it is expected that the structure and property of a-BC thin film alloys can be modified by controlling the deposition parameter of RF powers using RF reactive sputtering/PECVD.
When changing RF powers from 100 to 500 W at the fixed annealing temperature of 623 K and film thickness of 30 nm, the experimental results also show that the a-BC thin film alloy prepared at the RF power of 300 W has the highest ID/IG value of 1.49. Hence, it is expected that the a-BC thin film alloy prepared at the RF power of 300 W has a maximum graphitization degree and sp2 carbon bonds.
When changing annealing temperatures from as-deposited to 673 K at the fixed RF power of 300 W and film thickness of 30 nm, experimental results suggest that as the annealing temperature is 623 K, there are less dangling bonds in the a-BC thin film alloy, and its Eg value is 1.90 eV. Alternatively, after annealed at 623 K, the series resistance and ideality factor of the a-BC/n-Si diode reduce to 98 Ω and 2.43, respectively. The built-in voltages of the a-BC/n-Si devices are 0.45 and 0.88 V for the a-BC thin film alloys before and after annealed at 623 K, respectively.
In this study, it is found that under light illumination of 20 mW/cm2 at room temperature, the a-BC/SiO2/n-Si junctions after annealed at 623 K has a high fill factor of 93.4% and the power conversion efficiency of 6.3%, which is much better than the a-BC/Si junctions reported before. The ideality factor of the a-BC/SiO2/n-Si diode was 1.70 under an applied voltage of around 0.2 V. The enhanced fill factor is ascribed to the B atoms incorporation and the increase in sp2-bonded carbon clusters in the carbon films caused by the high annealing temperature. Moreover, the effects of a-BC/SiO2/n-Si solar cells with or without a thin native SiO2 interfacial layer on n-Si substrates prepared by RF reactive sputtering/PECVD are also discussed. The thin native SiO2 interfacial layer plays a key role in the performance of Au/a-BC/SiO2/n-Si/Al solar cells. Consequently, considering the nanometer-thickness, transparent, low-cost, and easy to produce massively features of these a-BC thin film alloys, they may also find applications in areas of photovoltaic solar cells and other optoelectronic devices.
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