Hybrid lead halide perovskites have emerged as high-performance photovoltaic materials with their extraordinary optoelectronic properties. In particular, the remarkable device efficiency is strongly influenced by the perovskite crystallinity and the film morphology. Here, we investigate the perovskites crystallisation kinetics and growth mechanism in real time from liquid precursor continually to the final uniform film. We utilize some advanced in situ characterisation techniques including synchrotron-based grazing incident X-ray diffraction to observe crystal structure and chemical transition of perovskites. The nano-assemble model from perovskite intermediated [PbI6]4− cage nanoparticles to bulk polycrystals is proposed to understand perovskites formation at a molecular- or nano-level. A crystallisation-depletion mechanism is developed to elucidate the periodic crystallisation and the kinetically trapped morphology at a mesoscopic level. Based on these in situ dynamics studies, the whole process of the perovskites formation and transformation from the molecular to the microstructure over relevant temperature and time scales is successfully demonstrated.

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Solid ferromagnetic materials are rigid in shape and cannot be reconfigured. Ferrofluids, although reconfigurable, are paramagnetic at room temperature and lose their magnetization when the applied magnetic field is removed. Here, we show a reversible paramagnetic-to-ferromagnetic transformation of ferrofluid droplets by the jamming of a monolayer of magnetic nanoparticles assembled at the water-oil interface. These ferromagnetic liquid droplets exhibit a finite coercivity and remanent magnetization. They can be easily reconfigured into different shapes while preserving the magnetic properties of solid ferromagnets with classic north-south dipole interactions. Their translational and rotational motions can be actuated remotely and precisely by an external magnetic field, inspiring studies on active matter, energy-dissipative assemblies, and programmable liquid constructs.

In this work, a nonfullerene polymer solar cell (PSC) based on a wide bandgap polymer donor PM6 containing fluorinated thienyl benzodithiophene (BDT-2F) unit and a narrow bandgap small molecule acceptor 2,2'-((2Z,2'Z)-((4,4,9,9-tetrahexyl-4,9-dihydro-s-indaceno[1,2-b:5,6-b']dithiophene-2,7-diyl)bis(methanylylidene))bis(3-oxo-2,3-dihydro-1H-indene-2,1-diylidene))dimalononitrile (IDIC) is developed. In addition to matched energy levels and complementary absorption spectrum with IDIC, PM6 possesses high crystallinity and strong π-π stacking alignment, which are favorable to charge carrier transport and hence suppress recombination in devices. As a result, the PM6:IDIC-based PSCs without extra treatments show an outstanding power conversion efficiency (PCE) of 11.9%, which is the record value for the as-cast PSC devices reported in the literature to date. Moreover, the device performances are insensitive to the active layer thickness (≈95-255 nm) and device area (0.20-0.81 cm ) with PCEs of over 11%. Besides, the PM6:IDIC-based flexible PSCs with a large device area of 1.25 cm exhibit a high PCE of 6.54%. These results indicate that the PM6:IDIC blend is a promising candidate for future roll-to-roll mass manufacturing and practical application of highly efficient PSCs.

Successfully interfacing enzymes and biomachineries with polymers affords ondemand modification and/or programmable plastic degradation during manufacture, utilization, and disposal, but requires controlled biocatalysis in solid matrices with macromolecular substrates. [1][2][3][4][5][6][7] Embedded enzyme microparticles have sped up polyester degradation, but compromise host properties and unintentionally accelerate microplastics formation with partial polymer degradation. 6,8,9 Here, by nanoscopically dispersing enzymes with deep active sites, semi-crystalline polyesters can be degraded primarily via chain-end mediated processive depolymerization with programmable latency and material integrity, akin to polyadenylationinduced mRNA decay. 10 It is also feasible to realize the processivity with enzymes having surface-exposed active sites by engineering enzyme/protectant/polymer complexes.Polycaprolactone and poly(lactic acid) containing less than 2 wt.% enzymes are depolymerized in days with up to 98% polymer-to-small molecule conversion in standard soil composts or household tap water, completely eliminating current needs to separate and landfill their products in compost facilities. Furthermore, oxidases embedded in polyolefins retain activities. However, the hydrocarbon polymers do not closely associate with enzymes like their polyester counterparts and the reactive radicals generated cannot chemically modify the macromolecular host. The studies described here provide molecular guidance toward the enzyme/polymer pairing and enzyme protectants' selection to modulate substrate selectivity and optimize biocatalytic pathways. They also highlight the need for in-depth research in solid-state enzymology, especially in multi-step enzymatic cascades, to tackle chemically dormant substrates without creating secondary environmental contamination and/or biosafety concerns.

Nanoparticle-surfactants (NPSs) assembled at water−oil interfaces can significantly lower the interfacial tension and can be used to stabilize liquids. Knowing the formation and assembly and actively tuning the packing of these NPSs is of significant fundamental interest for the interfacial behavior of nanoparticles and of interest for water purification, drug encapsulation, enhanced oil recovery, and innovative energy transduction applications. Here, we demonstrate by means of interfacial tension measurements the high ionic strength helps the adsorption of NPSs to the water−oil interface leading to a denser packing of NPSs at the interface. With the reduction of interfacial area, the phase transitions from a "gas"like to "liquid" to "solid" states of NPSs in two dimensions are observed. Finally, we provide the first in situ real-space imaging of NPSs at the water−oil interface by atomic force microcopy.

The unidirectional extension of a smaller fused-ring system into a larger one in a single direction will increase the conjugation length, allowing a fine-tuning of electronic properties. Here, we designed and synthesized a unidirectionally extended fused-8-ring-based nonfullerene acceptor, AOIC, and a bidirectionally extended fused-11-ring electron acceptor, IUIC2, and compared these with the parent fused-5-ring electron acceptor, F5IC. They share the same electron-accepting groups and alkylphenyl side chains but have different fused-ring electrondonating units. Core extension from 5 to 11 rings up-shifts the energy levels, red shifts the absorption spectra, and reduces bandgaps. The unidirectionally extended AOIC has the highest mobility (2.1 × 10 −3 cm 2 V −1 s −1) relative to the parent F5IC (1.0 × 10 −3 cm 2 V −1 s −1) and the bidirectionally extended IUIC2 (4.7 × 10 −4 cm 2 V −1 s −1). Upon blending with the donor PTB7-Th, AOIC-based organic photovoltaic cells show an efficiency of 13.7%, much better than that of F5IC-based cells (5.61%) and IUIC2-based cells (4.48%).

The benefits of excess PbI 2 on perovskite crystal nucleation and growth are countered by the photoinstability of interfacial PbI 2 in perovskite solar cells (PSCs). Here we report a simple chemical polishing strategy to rip PbI 2 crystals off the perovskite surface to decouple these two opposing effects. The chemical polishing results in a favorable perovskite surface exhibiting enhanced luminescence, prolonged carrier lifetimes, suppressed ion migration, and better energy level alignment. These desired benefits translate into increased photovoltages and fill factors, leading to high-performance mesostructured formamidinium lead iodide-based PSCs with a champion efficiency of 24.50%. As the interfacial ion migration paths and photodegradation triggers, dominated by PbI 2 crystals, were eliminated, the hysteresis of the PSCs was suppressed and the device stability under illumination or humidity stress was significantly improved. Moreover, this new surface polishing strategy can be universally applicable to other typical perovskite compositions.