Search

Conventional ligands for CsPbBr3 perovskite nanocrystals (NCs), composed of polar, coordinating head groups (e.g., ammonium or zwitterionic) and aliphatic tails, are instrumental in stabilizing the NCs against sintering and aggregation. Nonetheless, the aliphatic (insulating) nature of these ligands represents drawbacks with respect to objectives in optoelectronics, and yet removing these ligands typically leads to a loss of colloidal stability. In this paper, we describe the preparation of CsPbBr3 NCs in the presence of discrete conjugated oligomers that were prepared by an iterative synthetic approach and capped at their chain ends with sulfobetaine zwitterions for perovskite coordination. Notably, these zwitterionic oligofluorenes are compatible with the hot injection and ligand exchange conditions used to prepare CsPbBr3 NCs, yielding stable NC dispersions with high photoluminescence quantum yields (PLQY, >90%) and spectral features representative of both the perovskite core and conjugated ligand shell. Controlling the chain length of these capping ligands effectively regulated inter-NC spacing and packing geometry when cast into solid films, with evidence derived from both transmission electron microscopy (TEM) and grazing incidence X-ray scattering measurements.

As a class of semiconductor nanocrystals that exhibit high photoluminescence quantum yield (PLQY) at tunable wavelengths, perovskite nanocrystals (PNCs) are attractive candidates for optoelectronic and light‐emitting devices. However, attempts to optimize PNC integration into such applications suffer from PNC instability and loss of PL over time. Here, we describe the impact of organic and polymeric N‐oxides when used in conjunction with PNCs, whereby a significant increase in PNC quantum yield is observed in solution, and stable PL emission is obtained in polymeric nanocomposites. Specifically, when using aliphatic N‐oxides in ligand exchange with CsPbBr3 PNCs in solution, a substantial boost in PNC brightness is observed (~40% or more PLQY increase), followed by an alteration of the perovskite chemistry. When N‐oxide substituents are positioned pendent to a poly(n‐butyl methacrylate) backbone, the optically clear flexible nanocomposite films obtained have bright PL emission and maintain optical clarity for months. X‐ray diffraction is useful for characterizing the PNC crystalline structure following exposure to aliphatic N‐oxides, while electron microscopy (EM) and small‐angle X‐ray scattering (SAXS) measurements of the PNC‐polymer nanocomposites show this polymeric N‐oxide platform to cleanly disperse PNCs in flexible polymer films. [ABSTRACT FROM AUTHOR]

Organic solar cells (OSCs) and perovskite solar cells (PVSCs) are promising candidates for next-generation thin film photovoltaic technologies. The integration of OSCs with PVSCs in tandem devices is now attracting significant attention due to their similar fabrication procedures and the potential to afford a higher device performance. Here, a thickness-insensitive and solvent-resistant interconnecting layer is developed to efficiently connect perovskite and organic subcells with low contact resistance. The resultant perovskite-organic tandem devices maintain high efficiencies over a wide thickness range of the interconnecting layer, from ∼20 nm to ∼50 nm, providing an easily fabricated, solvent-resistant platform to integrate perovskite and organic active layers with low-temperature solution processing techniques. The tandem devices containing an ultrathin PVSC and a typical non-fullerene OSC give a maximum efficiency of 19.2%, which is much higher than those of the single-junction devices. Moreover, highly reproducible 1 cm 2 perovskite-organic tandem devices are achieved using the thickness-insensitive and solvent-resistant interconnecting layer, and an efficiency of 17.8% is realized. These 1 cm 2 tandem solar cells are used successfully in solar-to-hydrogen systems to afford a solar-to-fuel conversion efficiency of 11.2%. Overall, these advances represent significant progress in the design of ultrathin and facile solution processed perovskite-organic tandem solar cells.