Formation of CuInSe_2 and CuGaSe_2 Thin Films Deposited by Three-Stage Thermal Co-Evaporation: A Real-Time X-Ray Diffraction and Fluorescence Study

Humberto Rodriguez-Alvarez; Alfons Weber; Jakob Louche; Christian Alexander Kaufmann; Thorsten Rissom; Dieter Greiner; Manuela Klaus; Thomas Unold; Christoph Genzel; Hans-Werner Schock; Roland Mainz

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Formation of CuInSe_2 and CuGaSe_2 Thin Films Deposited by Three-Stage Thermal Co-Evaporation: A Real-Time X-Ray Diffraction and Fluorescence Study

机译：三阶段热共蒸发沉积CuInSe_2和CuGaSe_2薄膜的形成：实时X射线衍射和荧光研究

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Thin film solar cells based on co-evaporated Cu(In,Ca)Se_2 absorber films present the highest efficiencies among current polycrystalline thin-film technologies. Thanks to the development of a novel experimental setup for in situ growth studies, it was possible to follow the formation of the crystalline phases during such deposition processes for the first time. This synchrotron-based energy-dispersive X-ray diffraction and fluorescence setup is suited for real-time studies of thin film vapor deposition processes. Focusing on the growth of CuInSe_2 and CuCaSe_2 fabricated by three-stage processing, we find that the phase transitions in the Cu-In-Se system follow the reported pseudo-binary In_2Se_3-Cu_2Se phase diagram. This requires a transformation of the Se sublattice during the incorporation of Cu-Se into the In_2Se_3 precursor film from the first process stage. In the Cu-Ca-Se system, besides an increase in the lattice spacings, we observe no transformation of the Se sublattice. Furthermore, the structural defects of the Ca-Se precursor film are preserved until the CuCaSe_2 stoichiometry is reached. By means of model calculations of the fluorescence signals, we confirm in both systems the segregation of Cu_2Se at the surface near a concentration of 25 at.% Cu shortly after the recrystallization of the films. The modeling also reveals that Cu_2Se penetrates into the CuInSe_2 film, whereas it remains at the surface of the CuCaSe_2 film.

机译：在目前的多晶薄膜技术中，基于共蒸发Cu（In，Ca）Se_2吸收膜的薄膜太阳能电池具有最高的效率。由于开发了用于原位生长研究的新型实验装置，因此有可能首次在这种沉积过程中追踪结晶相的形成。这种基于同步加速器的能量色散X射线衍射和荧光设置适用于薄膜气相沉积过程的实时研究。着眼于通过三阶段工艺制造的CuInSe_2和CuCaSe_2的生长，我们发现Cu-In-Se系统中的相变遵循报道的伪二进制In_2Se_3-Cu_2Se相图。这要求从第一工艺阶段开始将Cu-Se掺入In_2Se_3前驱体膜中，然后将Se子晶格转变。在Cu-Ca-Se系统中，除了晶格间距的增加之外，我们没有观察到Se亚晶格的转变。此外，保留了Ca-Se前体膜的结构缺陷，直到达到CuCaSe_2化学计量比为止。通过荧光信号的模型计算，我们在两个系统中都确认了薄膜重结晶后不久，Cu_2Se在浓度接近25 at。％Cu的表面偏析。该模型还揭示了Cu_2Se渗透到CuInSe_2膜中，而仍保留在CuCaSe_2膜的表面。

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《Advanced energy materials》 |2013年第10期|1381-1387|共7页
作者
Humberto Rodriguez-Alvarez; Alfons Weber; Jakob Louche; Christian Alexander Kaufmann; Thorsten Rissom; Dieter Greiner; Manuela Klaus; Thomas Unold; Christoph Genzel; Hans-Werner Schock; Roland Mainz;
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Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany,International Iberian Nanotechnology Laboratory Avenida Mestre Jose Veiga s, 4715-330 Braga, Portugal;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

Helmholtz-Zentrum Berlin Hahn-Meitner Platz 1, 14109 Berlin, Germany;

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机译：原位光散射和原位X射线衍射研究Cu_2ZnSnSe_4薄膜的共蒸发过程
2. Effects of Se Flux on the Microstructure of Cu(In,Ga)Se_2 Thin Film Deposited by a Three-Stage Co-evaporation Process [J] . Ki Hwan Kim, Kyung Hoon Yoon, Jae Ho Yun Electrochemical and solid-state letters . 2006,第8期

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3. In-situ Raman spectroscopy and X-ray diffraction studies of the structural transformations leading to the SrCu_2O_2 phase from strontium-copper oxide thin films deposited by metalorganic chemical vapor deposition [J] . A. Khan, C Jimenez, O. Chaix-Pluchery, Thin Solid Films . 2013,第AUGa31期

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4. Bandgap gradients in (Ag,Cu)(In,Ga)Se2 thin film solar cells deposited by three-stage co-evaporation [C] . Thompson Christopher P., Chen Lei, Shafarman William N., IEEE Photovoltaic Specialists Conference . 2015

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5. In situ X-ray diffraction based investigation of crystallization in solution deposited PZT thin films [D] . Nittala, Krishna 2012

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6. High energy x-ray diffraction∕x-ray fluorescence spectroscopy for high-throughput analysis of composition spread thin films [O] . John M. Gregoire, Darren Dale, Alexander Kazimirov, -1

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7. Scanning X-Ray Diffraction: A Technique With High Compositional Resolution for Studying Phase Formation in Co-Deposited Thin Films [O] . T.I. Selinder, D.J. Miller, K.E. Gray, 1994

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8. Scanning x-ray diffraction: A technique with high compositional resolution for studying phase formation in co-deposited thin films [R] . Selinder, TI, Miller, D J, Gray, KE, 1994

机译：扫描X射线衍射：一种具有高成分分辨率的技术，用于研究共沉积薄膜中的相形成

Formation of CuInSe_2 and CuGaSe_2 Thin Films Deposited by Three-Stage Thermal Co-Evaporation: A Real-Time X-Ray Diffraction and Fluorescence Study

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