Elimination of interfacial charge accumulation and inhibition of ion migration are still challenging for promoting both efficiency and operational stability of perovskite solar cells (PVSCs) with 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenyl-amine)-9,9′-spiro bifluorene (spiro-OMeTAD). Here an innovative interface engineering, self-assembled cocrystal layer (SAM-CL) for PVSCs is constructed from a 1-pyrenemethylamine hydrochloride (PRMA) monolayer on the perovskite surface and 2,3,5,6-tetrafluoro-7,7′,8,8′-tetracyanoquinodimethane (F4TCNQ) doped in spiro-OMeTAD through intermolecular π–π interactions and hydrogen bonds. SAM-CL optimizes interfacial energy level alignment by a strong charge-transfer effect, thereby eliminating interfacial charge accumulation. Moreover, the excellent barrier effect of large pyrene rings and fluorine atoms in SAM-CL effectively hinders ion migration and moisture invasion, thus significantly improving the stability of PVSCs. The resulting PVSCs yield a power conversion efficiency (PCE) of 24.03% with a high open circuit voltage of 1.21 V and deliver impressive stability, which can maintain 85% of initial PCE after over 1800 h in air with a relative humidity of 70–80% without encapsulation.

中文翻译：

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通过自组装共晶中间层消除电荷积累，实现高效稳定的钙钛矿太阳能电池

消除界面电荷积累和抑制离子迁移对于提高2,2',7,7'-四( N , N-二-对甲氧基苯基- )钙钛矿太阳能电池(PVSC)的效率和运行稳定性仍然具有挑战性。胺）-9,9'-螺二芴（spiro-OMeTAD）。这里，一种创新的界面工程，用于 PVSC 的自组装共晶层 (SAM-CL) 由钙钛矿表面上的 1-芘甲胺盐酸盐 (PRMA) 单层和 2,3,5,6-四氟-7,7' 构建而成， 8,8′-四氰基醌二甲烷（F4TCNQ）通过分子间π-π相互作用和氢键掺杂在spiro-OMeTAD中。SAM-CL通过强大的电荷转移效应优化界面能级排列，从而消除界面电荷积累。此外，SAM-CL中大的芘环和氟原子的优异阻隔作用有效阻碍了离子迁移和水分入侵，从而显着提高了PVSC的稳定性。由此产生的 PVSC 的功率转换效率 (PCE) 为 24.03%，开路电压为 1.21 V，并具有令人印象深刻的稳定性，在相对湿度为 70-80 的空气中经过 1800 小时以上后仍可保持初始 PCE 的 85% % 无封装。