Interface regulation for efficient and stable inverted perovskite solar cells

Organic-inorganic halide perovskite solar cells (PSCs), an emerging photovoltaic technology, have received widespread attention in the past several years due to their low cost and high power conversion efficiency (PCE). The highest certified PCE has reached 25.7%, exceeding those of most traditional photovoltaic devices. PSCs can be divided into two types: regular PSCs (n-i-p) and inverted PSCs (p-i-n). Compared to regular PSCs, inverted PSCs show great promise for large-scale commercialization because of the easily scalable fabrication process, good stability against moisture, and wide application for integrating with other narrow-bandgap solar cells. However, their power conversion efficiency (PCE) is yet reported lower than that of regular PSCs due to their different interface contacts; these lead to poor film quality, unfavorable charge transport, and mismatched energy level. Besides, there are high concentrations of trap states at the interfaces between the charge transport layers (CTL) and the perovskites. Especially in inverted PSCs, defects at the HTL/perovskite interface are particularly abundant. Therefore, my works in this thesis focus on the realization of efficient and stable inverted PSCs by interface regulation, which can greatly reduce interfacial defect density, improve interface contact, and optimize energy levels between CTLs and perovskites.
First, an efficient antisolvent-assisted crystallization strategy was adopted to modify the top interface of perovskite. Specifically, the 1,3,5-tris(1-phenyl-1H-benzimidazol-2-yl)benzene (TPBi) facilitated the crystallization of perovskites along (100) orientation and enhanced the hole-blocking capability of the top interface of perovskite. Upon the incorporation of TPBi, the champion inverted PSCs exhibited a high PCE of 21.79% and good long-term stability.
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Then, [2-(9H-carbazol-9-yl)ethyl]phosphonic acid (2P) was used to modify the HTL/perovskite interface by a pre-wetting process; it can improve crystallinity, enhance interface contact, and accelerate hole extraction. Upon the incorporation of 2P, inverted PSCs delivered a high PCE of 22.17% with superior stability.
Finally, an interfused interface was constructed to graft the bottom of the formamidinium lead triiodide (FAPbI3) and the NiOx HTL. This unique interface structure effectively stabilized the α phase of FAPbI3, reduced interfacial defects, and facilitated carrier transport. As a result, FAPbI3 inverted PSC exhibited the highest power conversion efficiency of 23.56% (certified 22.58%) and excellent thermo-optical stability.

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