Crystallinity and crystal orientation have a predominant impact on a materials’ semiconducting properties, thus it is essential to manipulate the microstructure arrangements for desired semiconducting device performance. Here, ultra‐uniform hole‐transporting material (HTM) by self‐assembling COOH‐functionalized P3HT (P3HT‐COOH) is fabricated, on which near single crystal quality perovskite thin film can be grown. In particular, the self‐assembly approach facilitates the P3HT‐COOH molecules to form an ordered and homogeneous monolayer on top of the indium tin oxide (ITO) electrode facilitate the perovskite crystalline film growth with high quality and preferred orientations. After detailed spectroscopy and device characterizations, it is found that the carboxylic acid anchoring groups can down‐shift the work function and passivate the ITO surface, retarding the interface carrier recombination. As a result, the device made with the self‐assembled HTM show high open‐circuit voltage over 1.10 V and extend the lifetime over 4,300 h when storing at 30% relative humidity. Moreover, the cell works efficiently under much reduced light power, making it useful as power source under dim‐light conditions. The demonstration suggests a new facile way of fabricating monolayer HTM for high efficiency perovskite devices, as well as the interconnecting layer needed for tandem cell.

中文翻译：

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高性能钙钛矿太阳能电池自组装功能化聚噻吩空穴传输层的简便制备

结晶度和晶体取向对材料的半导体性能有主要影响，因此控制微结构排列以获得所需的半导体器件性能至关重要。在这里，通过自组装COOH功能化P3HT（P3HT-COOH）制备了超均匀空穴传输材料（HTM），在其上可以生长接近单晶质量的钙钛矿薄膜。特别是，自组装方法有利于P3HT-COOH分子在氧化铟锡（ITO）电极顶部形成有序且均匀的单层，有利于钙钛矿晶体薄膜的高质量和择优生长。经过详细的光谱和器件表征后，发现羧酸锚定基团可以降低功函数并钝化 ITO 表面，从而延迟界面载流子复合。因此，用自组装 HTM 制成的器件表现出超过 1.10 V 的高开路电压，并且在 30% 相对湿度下存储时，使用寿命延长了 4,300 小时以上。此外，该电池在光功率大大降低的情况下也能高效工作，使其在弱光条件下可用作电源。该演示提出了一种新的简便方法来制造用于高效钙钛矿器件的单层 HTM，以及串联电池所需的互连层。