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Accessing vertical orientation of two-dimensional (2D) perovskite films is key to achieving high-performance solar cells with these materials. Herein, we report on solvent-vapor annealing (SVA) as a general postdeposition strategy to induce strong vertical orientation across broad classes of 2D perovskite films. We do not observe any local compositional drifts that would result in impure phases during SVA. Instead, our experiments point to solvent vapor plasticizing 2D perovskite films and facilitating their surface-induced reorientation and concomitant grain growth, which enhance out-of-plane charge transport. Solar cells with SVA 2D perovskites exhibit superior efficiency and stability compared to their untreated analogs. With a certified efficiency of (18.00 ± 0.30) %, our SVA (BDA)(Cs 0.1 FA 0.9 ) 4 Pb 5 I 16 solar cell boasts the highest efficiency among all solar cells with 2D perovskites ( n ≤ 5) reported so far.

We demonstrate the generation of block copolymer (BCP) line patterns oriented orthogonal to a very small (minimal) topographic trench pattern over arbitrarily large areas using solvent-vapor annealing. Increasing the thickness of BCP films induced an orthogonal alignment of the BCP cylindrical microdomains, where full orthogonal alignment of the cylindrical microdomains with respect to the trench direction was obtained at a film thickness corresponding to 1.70 L 0 . A capillary flow of the solvent across the trenches was a critical factor in the alignment of the cylindrical microdomains. Grazing incidence small-angle X-ray scattering was used to determine the orientation function of the microdomains, with a value of 0.997 being found reflecting a nearly perfect orientation. This approach to produce orthogonally aligned BCP line patterns could be extended to the nanomanufacturing and fabrication of hierarchical nanostructures.

Two twisted singly linked perylene bisimide (PBI) dimers with chalcogen bridges in the PBI cores, named C4,4-SdiPBI-S and C4,4-SdiPBI-Se, were synthesized as acceptors for nonfullerene all-small-molecule organic solar cells (NF all-SMSCs). A moderate-band-gap small-molecule DR3TBDTT used as the electron donor displayed complementary absorption with C4,4-SdiPBI-S and C4,4-SdiPBI-Se. It was found that solvent-vapor annealing (SVA) played a critical role in the photovoltaic performance in NF all-SMSCs, which improves the crystallinity of the donor and acceptors, promotes the proper phase segregation domain size, and therefore enhances charge transport. The power conversion efficiencies (PCEs) of NF all-SMSC devices based on DR3TBDTT/C4,4-SdiPBI-S and DR3TBDTT/C4,4-SdiPBI-Se increased from 2.52% to 5.81% (J SC = 11.12 mA cm -2 , V OC = 0.91 V, and FF = 57.32%) and from 2.65% to 6.22% (J SC = 11.55 mA cm -2 , V OC = 0.92 V, and FF = 58.72%), respectively, after exposure to chloroform vapor. The best efficiency of 6.22% is one of the highest PCEs for NF all-SMSC-based PBI acceptors so far. The studies illustrate that highly efficient NF all-SMSCs can be achieved by using a PBI acceptor with a suitable SVA process.