Search

Abstract Lately, carbazole‐based self‐assembled monolayers (SAMs) are widely employed as effective hole‐selective layers (HSLs) in inverted perovskite solar cells (PSCs). Nevertheless, these SAMs tend to aggregate in solvents due to their amphiphilic nature, hindering the formation of a monolayer on the ITO substrate and impeding effective passivation of deep defects in the perovskites. In this study, a series of new SAMs including DPA‐B‐PY, CBZ‐B‐PY, POZ‐B‐PY, POZ‐PY, POZ‐T‐PY, and POZ‐BT‐PY are synthesized, which are employed as interfacial repairers and coated atop CNph SAM to form a robust CNph SAM@pseudo‐planar monolayer as HSL in efficient inverted PSCs. The CNph SAM@pseudo‐planar monolayer strategy enables a well‐aligned interface with perovskites, synergistically promoting perovskite crystal growth, improving charge extraction/transport, and minimizing nonradiative interfacial recombination loss. As a result, the POZ‐BT‐PY‐modified PSC realizes an impressively enhanced solar efficiency of up to 24.45% together with a fill factor of 82.63%. Furthermore, a wide bandgap PSC achieving over 19% efficiency. Upon treatment with the CNph SAM@pseudo‐planar monolayer, also demonstrates a non‐fullerene organic photovoltaics (OPVs) based on the PM6:BTP‐eC9 blend, which achieves an efficiency of 17.07%. Importantly, these modified PSCs and OPVs all show remarkably improved stability under various testing conditions compared to their control counterparts.

Abstract Using a transfer printing technique, we imprint a layer of a designated near-infrared fluorescent dye BTP-eC9 onto a thin layer of Pt(II) complex, both of which are capable of self-assembly. Before integration, the Pt(II) complex layer gives intense deep-red phosphorescence maximized at ~740 nm, while the BTP-eC9 layer shows fluorescence at > 900 nm. Organic light emitting diodes fabricated under the imprinted bilayer architecture harvest most of Pt(II) complex phosphorescence, which undergoes triplet-to-singlet energy transfer to the BTP-eC9 dye, resulting in high-intensity hyperfluorescence at > 900 nm. As a result, devices achieve 925 nm emission with external quantum efficiencies of 2.24% (1.94 ± 0.18%) and maximum radiance of 39.97 W sr−1 m−2. Comprehensive morphology, spectroscopy and device analyses support the mechanism of interfacial energy transfer, which also is proved successful for BTPV-eC9 dye (1022 nm), making bright and far-reaching the prospective of hyperfluorescent OLEDs in the near-infrared region.

Inverted perovskite solar cells (PSCs) mainly adopt polytriarylamine (PTAA) for the hole transport material (HTM), which usually brings about inferior interfacial contact owing to their hydrophobicity, high‐lying highest occupied molecular orbital energy level, and deficiency of passivation groups. Herein, a series of donor–π–acceptor (D–π–A) type small molecules is demonstrated based on 2,2′:6′,2″‐terpyridine (TPy) as the acceptor moiety, benzene ring as the π‐linker, and incorporating various donors to act as HTMs. These TPy‐based molecules coated atop PTAA manipulate the energy level and surface wettability, but the incorporation of the phenoxazine (POZ) donor can be prominent for enhancing charge transport and defect passivation, thereby simultaneously addressing the above‐mentioned issues. The highest power conversion efficiency of 22.36% can be achieved with an open‐circuit voltage (VOC) of 1.15 V, a short‐circuit current density (JSC) of 23.96 mA cm−2, and a fill factor (FF) of 81.16% for the optimized POZ‐TPy‐modified device. Moreover, the power PCE of a large POZ‐TPy‐modified device (1.96 cm2) can still reach more than 21%. These results are among one of the highest efficiencies for inverted PSCs, indicating the enormous potential of POZ‐TPy HTM in future perovskite applications.