研究和优化替代MBE沉积的金属前驱体，以制备高效的Kesterite CZTSe：Ge太阳能电池,Progress in Photovoltaics

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研究和优化替代MBE沉积的金属前驱体，以制备高效的Kesterite CZTSe：Ge太阳能电池
Progress in Photovoltaics ( IF 8.0 ) Pub Date : 2019-06-19 , DOI: 10.1002/pip.3147
Sergio Giraldo ₁ , Shinho Kim ₂ , Jacob Antonio Andrade‐Arvizu ₁ , Xavier Alcobé ₃ , Claudia Malerba ₄ , Matteo Valentini ₄ , Hitoshi Tampo ₂ , Hajime Shibata ₂ , Victor Izquierdo‐Roca ₁ , Alejandro Pérez‐Rodríguez _{1,

5} , Edgardo Saucedo ₁

Affiliation

如今，Cu ₂ ZnSn（S，Se）_4的大多数最佳效率（CZTSSe）太阳能电池是从吸收器层获得的，这些吸收器层是使用顺序工艺制造的，包括典型地通过溅射沉积金属堆叠前驱体，然后在硫属元素气氛下进行反应性退火。溅射技术因易于生长金属层而广为人知，尽管有时沉积速率，生长形态和成核或粗糙度有时会成为导致最终层不均匀的问题。尽管如此，由于超高真空条件和高纯度，MBE（分子束外延）技术可能具有一些优点，可以获得高质量的金属层，并且可以精确地控制生长。在这项工作中，我们研究了使用先进的MBE系统来生长金属堆叠前体的方法，以替代溅射或热蒸发技术，获得高质量的CZTSe：Ge吸收体。由于每种前驱物的性质不同，因此通过修改一些关键的硒化参数（例如温度或硒含量）来提出热退火优化方法，以获得结晶良好的吸收剂。详细的形态，组成和结构表征显示了每种前体的相关特征，主要与MoSe的形成有关₂在背面的界面上，硒化后的硒和锡组成处于不同的条件下。关于太阳能电池装置，主要的效率限制来自V _OC和FF，这可能暂时与不受控制的硒化有关。不同的前体反应性，孔隙率或组成；反应性退火过程中碱扩散不同。最后，在第一个优化中，已经实现了9.2％效率的设备，并为未来的改进提供了有希望的前景。

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Study and optimization of alternative MBE‐deposited metallic precursors for highly efficient kesterite CZTSe:Ge solar cells

Nowadays, most of the best efficiencies of Cu₂ZnSn(S,Se)₄ (CZTSSe) solar cells are obtained from absorber layers fabricated using sequential processes, including the deposition of metallic stack precursors, typically by sputtering, and followed by reactive annealing under chalcogen atmosphere. The sputtering technique is widely known for the easy growth of metallic layers, although the deposition rates, growth morphology and nucleation, or the roughness can sometimes be an issue leading to inhomogeneities in the final layers. Nevertheless, MBE (molecular beam epitaxy) technique could have some advantages to obtain high‐quality metallic layers, with accurate control of the growth due to ultra‐high vacuum conditions and high purity. In this work, we study the use of advanced MBE systems to grow metallic stack precursors, alternatively to sputtering or thermal evaporation techniques, to obtain high‐quality CZTSe:Ge absorbers. Due to differences in the nature of each type of precursor, thermal annealing optimizations are presented by modifying some critical selenization parameters, such as the temperature or the selenium amount in order to obtain well‐crystallized absorbers. Detailed morphological, compositional, and structural characterizations show relevant features of each precursor, mainly related to the formation of MoSe₂ at the back interface, and Se and Sn composition after selenization in different conditions. Regarding the solar cell devices, main efficiency limitations come from V_OC and FF, which could be tentatively related to a noncontrolled selenization; different precursor reactivity, porosity, or composition; and different alkali diffusion during the reactive annealing. Finally, in the first optimization, a 9.2% efficiency device has been achieved with promising perspectives for future improvements.

更新日期：2019-06-19

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