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Abstract Quasi‐2D perovskite made with organic spacers co‐crystallized with inorganic cesium lead bromide inorganics is demonstrated for near unity photoluminescence quantum yield at room temperature. However, light emitting diodes made with quasi‐2D perovskites rapidly degrade which remains a major bottleneck in this field. In this work, It is shown that the bright emission originates from finely tuned multi‐component 2D nano‐crystalline phases that are thermodynamically unstable. The bright emission is extremely sensitive to external stimuli and the emission quickly dims away upon heating. After a detailed analysis of their optical and morphological properties, the degradation is attributed to 2D phase redistribution associated with the dissociation of the organic spacers departing from the inorganic lattice. To circumvent the instability problem, a diamine is investigated spacer that has both sides attached to the inorganic lattice. The diamine spacer incorporated perovskite film shows significantly improved thermal tolerance over maintaining a high photoluminescence quantum yield of over 50%, which will be a more robust material for lighting applications. This study guides designing quasi‐2D perovskites to stabilize the emission properties. 

Abstract Developing novel lead‐free ferroelectric materials is crucial for next‐generation microelectronic technologies that are energy efficient and environment friendly. However, materials discovery and property optimization are typically time‐consuming due to the limited throughput of traditional synthesis methods. In this work, we use a high‐throughput combinatorial synthesis approach to fabricate lead‐free ferroelectric superlattices and solid solutions of (Ba_0.7Ca_0.3)TiO₃(BCT) and Ba(Zr_0.2Ti_0.8)O₃(BZT) phases with continuous variation of composition and layer thickness. High‐resolution x‐ray diffraction (XRD) and analytical scanning transmission electron microscopy (STEM) demonstrate high film quality and well‐controlled compositional gradients. Ferroelectric and dielectric property measurements identify the “optimal property point” achieved at the composition of 48BZT–52BCT. Displacement vector maps reveal that ferroelectric domain sizes are tunable by varying {BCT–BZT}_Nsuperlattice geometry. This high‐throughput synthesis approach can be applied to many other material systems to expedite new materials discovery and properties optimization, allowing for the exploration of a large area of phase space within a single growth. image 

Abstract 2D hybrid organic–inorganic perovskites (HOIPs) are commonly found under subcritical cyclic stresses and suffer from fatigue issues during device operation. However, their fatigue properties remain unknown. Here, the fatigue behavior of (C₄H₉‐NH₃)₂(CH₃NH₃)₂Pb₃I₁₀, the archetype 2D HOIP, is systematically investigated by atomic force microscopy (AFM). It is found that 2D HOIPs are much more fatigue resilient than polymers and can survive over 1 billion cycles. 2D HOIPs tend to exhibit brittle failure at high mean stress levels, but behave as ductile materials at low mean stress levels. These results suggest the presence of a plastic deformation mechanism in these ionic 2D HOIPs at low mean stress levels, which may contribute to the long fatigue lifetime, but is inhibited at higher mean stresses. The stiffness and strength of 2D HOIPs are gradually weakened under subcritical loading, potentially as a result of stress‐induced defect nucleation and accumulation. The cyclic loading component can further accelerate this process. The fatigue lifetime of 2D HOIPs can be extended by reducing the mean stress, stress amplitude, or increasing the thickness. These results can provide indispensable insights into designing and engineering 2D HOIPs and other hybrid organic–inorganic materials for long‐term mechanical durability. 

Understanding and exploiting material flexibility through phenomena such as the bending and twisting of molecular crystals has been a subject of increased interest owing to the number of applications that benefit from these properties, such as optoelectronics, mechanophotonics, soft robotics, and smart sensors. Here, we report the growth of spontaneously bent and twisted ammonium urate crystals induced by the keto–enol tautomerism of the urate molecule. The major tautomer is native to biogenic crystals, whereas the minor tautomer functions as an effective crystal growth modifier to induce naturally bent and twisted ammonium urate crystals. We show that the degree of curvature can be tailored based on the judicious selection of growth conditions. A combination of state-of-the-art microscopy and spectroscopy techniques are used to characterize the origin of bending. Spatially resolved nano-electron diffraction and high-resolution electron microscopy of naturally bent crystals show nearly single crystallinity with local lattice deformations generated by a combination of screw and edge dislocations. These observations are consistent with photoinduced force microscopy and contact resonance atomic force microscopy, which confirmed spatially resolved changes in the intermolecular interactions and the mechanical properties throughout the cross-sectional and axial regions of bent crystals. A mechanism of bending involving the generation of regionally specific dislocations is proposed as an alternative to more commonly reported models. These findings highlight a unique characteristic of tautomeric crystals that may have broader implications for other biogenic materials.