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標題: 表面後處理之銅銦鎵硒薄膜太陽能電池之研究
Surface modification of Cu(In,Ga)Se2 thin films for solar cells by post deposition treatment
作者: 陳俊宇
Chun-Yu Chen
關鍵字: 後處理;銅銦鎵硒硫;銅銦鎵硒硫太陽能元件;post deposition treatment;CIGS;CIGS solar cell
引用: [1] [2] [3] [4] [5],' Current Applied Physics, vol. 18, pp. S28-S32, 2018/08/01/ 2018. [6]'Claims for solar cell efficiency put to test at NREL,' 2016. [7]A. Chirilă et al., 'Potassium-induced surface modification of Cu (In, Ga) Se 2 thin films for high-efficiency solar cells,' Nature materials, vol. 12, no. 12, p. 1107, 2013. [8]'' [9]'' [10] '' [11] F. Hergert, S. Jost, R. Hock, M. Purwins, and J. Palm, 'Formation reactions of chalcopyrite compounds and the role of sodium doping,' Thin Solid Films, vol. 515, no. 15, pp. 5843-5847, 2007. [12] M. Ruckh, D. Schmid, M. Kaiser, R. Schäffler, T. Walter, and H. Schock, 'Influence of substrates on the electrical properties of Cu (In, Ga) Se2 thin films,' Solar Energy Materials and Solar Cells, vol. 41, pp. 335-343, 1996. [13] T. Wada, N. Kohara, S. Nishiwaki, and T. Negami, 'Characterization of the Cu (In, Ga) Se2/Mo interface in CIGS solar cells,' Thin Solid Films, vol. 387, no. 1-2, pp. 118-122, 2001. [14] A. M. Gabor et al., 'Band-gap engineering in Cu (In, Ga) Se2 thin films grown from (In, Ga) 2Se3 precursors,' Solar Energy Materials and Solar Cells, vol. 41, pp. 247-260, 1996. [15] M. Omar and M. M. Shaltout, 'Solar net radiation over water in a class 'A' evaporation pan at Giza, estimated on the base of its close relationship with global radiation,' Solar energy, vol. 41, no. 3, pp. 247-253, 1988. [16] V. Alberts, J. Titus, and R. Birkmire, 'Material and device properties of single-phase Cu (In, Ga)(Se, S) 2 alloys prepared by selenization/sulfurization of metallic alloys,' Thin Solid Films, vol. 451, pp. 207-211, 2004. [17] J. Yang et al., 'Influence of surface properties on the performance of Cu (In, Ga)(Se, S) 2 thin-film solar cells using Kelvin probe force microscopy,' RSC Advances, vol. 5, no. 51, pp. 40719-40725, 2015. [18] S. Ishizuka et al., 'Fabrication of wide-gap Cu(In1−xGax)Se2 thin film solar cells: a study on the correlation of cell performance with highly resistive i-ZnO layer thickness,' Solar Energy Materials and Solar Cells, vol. 87, no. 1-4, pp. 541-548, 2005. [19] T. Feurer et al., 'Progress in thin film CIGS photovoltaics–Research and development, manufacturing, and applications,' Progress in Photovoltaics: Research and Applications, vol. 25, no. 7, pp. 645-667, 2017. [20] P. Jackson, R. Wuerz, D. Hariskos, E. Lotter, W. Witte, and M. Powalla, 'Effects of heavy alkali elements in Cu(In,Ga)Se2solar cells with efficiencies up to 22.6%,' physica status solidi (RRL) - Rapid Research Letters, vol. 10, no. 8, pp. 583-586, 2016. [21] P. Jackson, D. Hariskos, R. Wuerz, W. Wischmann, and M. Powalla, 'Compositional investigation of potassium doped Cu (In, Ga) Se2 solar cells with efficiencies up to 20.8%,' physica status solidi (RRL)–Rapid Research Letters, vol. 8, no. 3, pp. 219-222, 2014. [22] T. M. Friedlmeier et al., 'Improved photocurrent in Cu (In, Ga) Se2 solar cells: From 20.8% to 21.7% efficiency,' in Photovoltaic Specialist Conference (PVSC), 2015 IEEE 42nd, 2015, pp. 1-3: IEEE. [23] T. M. Friedlmeier et al., 'Improved photocurrent in Cu (In, Ga) Se 2 solar cells: from 20.8% to 21.7% efficiency with CdS buffer and 21.0% Cd-free,' IEEE Journal of Photovoltaics, vol. 5, no. 5, pp. 1487-1491, 2015. [24] E. Handick et al., 'Formation of a K-In-Se Surface Species by NaF/KF Postdeposition Treatment of Cu (In, Ga) Se2 Thin-Film Solar Cell Absorbers,' ACS applied materials & interfaces, vol. 9, no. 4, pp. 3581-3589, 2017. [25] I. Khatri, K. Shudo, J. Matsuura, M. Sugiyama, and T. Nakada, 'Comparative study of water and ammonia rinsing processes of potassium fluoride-treated Cu (In, Ga) Se2 thin film solar cells,' Japanese Journal of Applied Physics, vol. 56, no. 8S2, p. 08MC12, 2017. [26] P. Reinhard et al., 'Alkali-templated surface nanopatterning of chalcogenide thin films: a novel approach toward solar cells with enhanced efficiency,' Nano letters, vol. 15, no. 5, pp. 3334-3340, 2015.
銅銦鎵硒硫太陽能元件(Cu(In,Ga)SSe, CIGSSe solar cell)是在多種太陽能電池中具非常有潛力的吸收層材料,除其展現的高轉換效率性能外,亦具備有製備為軟性基板的潛力,有利於未來卷對卷(roll to roll)的生產製程,能於大面積製造下降低成本。然而,CIGSSe所展現的高轉換效率十分仰賴介面特性的調控。有鑑於此,本論文透過於CIGSSe吸收層與緩衝層中,進一步探討介面改質與生成一寬能隙的化合物之影響;論文中,第一部分透過自行設計的裝置以對CIGSSe表面進行硫化銨後處理,結果顯示CIGSSe硫化銨後處理後,能使元件轉換效率從15%提升至16%,並透過成分、光學與電性分析以了解元件轉換效率提升之關鍵。第二部分則是探討藉由氟化銫沉積後做硫化銨處理,於吸收層表面上生成一寬能隙的化合物,並利用成分、元件及模擬進行分析,結果顯示CIGSSe開路電壓有所提升,但因為介面屏障能隙過大導致電流及填充因子皆下降,使得整體元件轉換效率並無提升,最後透過元件分析的方式以說明潛在機制,以利未來元件效能改善提供方向。

CIGSSe thin film solar cell is an attractive absorber material among a varity of solar cells because of its high conversion efficiency and enabled felxibility fabrication via the roll-to-roll process, effectively offering the possibility of reducing the low cost during large-scale manufacturing. However, high conversion efficiency of CIGSSe strongly relies on the interfacial condition. Accordingly, we focus on the interface between the absorber and the buffer in this study. The CIGSSe surface is exposed to ammonium sulfide atmosphere before the buffer deposition. Our result shows that 1% improvement of the conversion efficiency can be achieved by such the treatment. The related anayses such as the composition , optical and electrical properties are carried out in oder to understand the relaionship between the treated interface and the conversion efficiency.
In addition, we further deposit CsF film on CIGSSe before ammonium sulfide treatment to form a compound with larger band gap located at the interafce between the CIGSSe and buffer layer. Composition analysis, device performance and simulations have been conduced for the discussion as well. It can be found that Voc can be significantly improved by this method, but large barrier coccured at the interface causes much lower fill factor and short circuit current, leading to a reduced conversion efficiency. This experimental result could match the trend of our simulation for alkali metals' doping. Accordingly, this study is allowed to provide an insight into the future alkali metal-induced surface modification, and thereby further improve the CIGSSe conversion efficiency.
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