Abstract In this work, we have investigated Cu2ZnSnS4 (CZTS) solar cells made from oxide, oxy-sulfide and sulfide precursors produced by pulsed laser deposition (PLD). Although sulfide precursors are widely used to fabricate CZTS solar cells, Sn loss is commonly observed due to the high volatility of SnxSy species during high temperature sulfurization. This can lead to a non-ideal absorber composition and a high density of detrimental Sn-related defects that severely affect the performance of the device. By using oxide precursors, we have shown that the Sn loss can be significantly reduced due to the higher thermal stability of SnxOy species when compared to their sulfide counterparts. However, the reaction mechanism for the oxide route results in rough CZTS films. We hypothesize that the SO2 gas that forms during the conversion from oxide to sulfide is trapped in the film during sulfurization, and can lead to grains with hollow cavities and thus increase the surface roughness. Therefore, we have developed an annealing route for the oxide precursors at lower annealing pressures, which leads to improved film morphology and device performance. As a result, we report a power conversion efficiency of 5.4% for solar cells made from oxide precursors. This is the highest value reported for a CZTS absorber produced by PLD.

中文翻译：

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脉冲激光沉积法制备Cu2ZnSnS4太阳能电池的氧化物路线

摘要 在这项工作中，我们研究了由脉冲激光沉积 (PLD) 产生的氧化物、氧硫化物和硫化物前驱体制成的 Cu2ZnSnS4 (CZTS) 太阳能电池。尽管硫化物前驱体被广泛用于制造 CZTS 太阳能电池，但由于 SnxSy 物质在高温硫化过程中的高挥发性，通常会观察到 Sn 损失。这会导致不理想的吸收体成分和高密度的有害 Sn 相关缺陷严重影响器件的性能。通过使用氧化物前体，我们已经表明，与硫化物对应物相比，SnxOy 物质具有更高的热稳定性，因此可以显着降低 Sn 损失。然而，氧化物路线的反应机制导致粗糙的 CZTS 薄膜。我们假设在从氧化物到硫化物的转化过程中形成的 SO2 气体在硫化过程中被困在薄膜中，并可能导致晶粒中空，从而增加表面粗糙度。因此，我们开发了一种在较低退火压力下对氧化物前体进行退火的路线，从而改善了薄膜形态和器件性能。因此，我们报告了由氧化物前体制成的太阳能电池的功率转换效率为 5.4%。这是 PLD 生产的 CZTS 吸收器报告的最高值。因此，我们报告了由氧化物前体制成的太阳能电池的功率转换效率为 5.4%。这是 PLD 生产的 CZTS 吸收器报告的最高值。因此，我们报告了由氧化物前体制成的太阳能电池的功率转换效率为 5.4%。这是 PLD 生产的 CZTS 吸收器报告的最高值。