The extraordinary optoelectronic performance of hybrid organic-inorganic perovskites has resulted in extensive efforts to unravel their properties. Recently, observations of ferroic twin domains in methylammonium lead triiodide drew significant attention as a possible explanation for the current-voltage hysteretic behaviour in these materials. However, the properties of the twin domains, their local chemistry and the chemical impact on optoelectronic performance remain unclear. Here, using multimodal chemical and functional imaging methods, we unveil the mechanical origin of the twin domain contrast observed with piezoresponse force microscopy in methylammonium lead triiodide. By combining experimental results with first principles simulations we reveal an inherent coupling between ferroelastic twin domains and chemical segregation. These results reveal an interplay of ferroic properties and chemical segregation on the optoelectronic performance of hybrid organic-inorganic perovskites, and offer an exploratory path to improving functional devices.

Memristive materials and devices, which enable information storage and processing on one and the same physical platform, offer an alternative to conventional von Neumann computation architectures. Their continuous spectra of states with intricate field-history dependence give rise to complex dynamics, the spatial aspect of which has not been studied in detail yet. Here, we demonstrate that ferroelectric domain switching induced by a scanning probe microscopy tip exhibits rich pattern dynamics, including intermittency, quasiperiodicity and chaos. These effects are due to the interplay between tip-induced polarization switching and screening charge dynamics, and can be mapped onto the logistic map. Our findings may have implications for ferroelectric storage, nanostructure fabrication and transistor-less logic.

Two-dimensional (2D) single-layer MoS2 nanosheets are demonstrated as efficient photocatalysts for hydrogen evolution reaction (HER) from water reduction, thanks to specific in-plane heterojunctions constructed in the MoS2 monolayer. These functional heterojunctions are formed among the different phases of chemically exfoliated MoS2 monolayers: semiconducting 2H, metallic 1T, and quasi-metallic 1T′ phases. The proportion of the three MoS2 phases can be systematically controlled via thermal annealing of the nanosheets. Interestingly, a volcano relationship is observed between the photocatalytic HER activity and the annealing temperature with an optimum activity obtained after annealing at 60 °C. First-principles calculations were integrated with experimental studies to shed light on the role of the multiphases of MoS2 and reveal that optimum photocatalytic HER activity results from the formation of the in-plane heterojunctions between 1T′ MoS2 and 2H MoS2. Importantly, this facilitates not only balanced light absorption and charge generation by the 2H phase, efficient charge separation at the 1T′/2H interface, but also favorable HER over the basal sites of 1T′ MoS2. Our work manifests how the confluence of the optical, electronic and chemical properties of 2D MoS2 monolayers can be fully captured for efficient photocatalytic water reduction.