Bulk CsEuBr₃ and CsEuCl₃ are experimentally shown to be magnetic semiconductors that order antiferromagnetically at Néel temperatures of 2.0 K and 1.0 K, respectively. Given that nanoparticles and thin films of CsEuCl₃ have been reported to order ferromagnetically at a similar temperature, our observation of antiferromagnetic ordering in CsEuBr₃ and CsEuCl₃ expands the possible applications of halide perovskites to now include spintronic devices where both ferromagnetic and antiferromagnetic devices can be fabricated from a single material. The conclusion that CsEuCl₃ can be used as a switchable magnetic material is also supported by our density-functional theory calculations.

The ability to continuously tune the band gap of a semiconductor allows its optical properties to be precisely tailored for specific applications. We demonstrate that the band gap of the halide perovskite CsPbBr₃ can be continuously widened through homovalent substitution of Sr²⁺ for Pb²⁺ using solid-state synthesis, creating a material with the formula CsPb_1-xSr_xBr₃ (0 ≤ x ≤ 1). Sr²⁺ and Pb²⁺ form a solid solution in CsPb_1-xSr_xBr₃. Pure CsPbBr₃ has a band gap of 2.29(2) eV, which increases to 2.64(3) eV for CsPb_0.25Sr_0.75Br₃. The increase in band gap is clearly visible in the color change of the materials and is also confirmed by a shift in the photoluminescence. Density-functional theory calculations support the hypothesis that Sr incorporation widens the band gap without introducing mid-gap defect states. These results demonstrate that homovalent B-site alloying can be a viable method to tune the band gap of simple halide perovskites for absorptive and emissive applications such as color-tunable light-emitting diodes, tandem solar cells, and photodetectors.

We synthesize and characterize the magnetic and thermodynamic properties of the quasi one-dimensional organic–inorganic hybrid ANiCl₃ compounds [A = N(CH₃)₄⁺, CH₃NH₃⁺, (CH₃)₂NH₂⁺, C(NH₂)₃⁺, and CH(NH₂)₂⁺]. Additionally, the crystal structure of (CH₃)₂NH₂NiCl₃ is reported. These materials possess chains of face-sharing NiCl₆ octahedra in a triangular array. The chains run in one direction and are separated from one another by organic cations of different sizes and geometries. In accordance with the 90° superexchange model, we find that the nature of the magnetic coupling within chains can be predicted by the value of the Ni–Cl–Ni angle. As the Ni–Cl–Ni angle decreases from 90°, the magnetic interactions become increasingly antiferromagnetic. These findings provide a foundation for predicting the magnetic properties of quasi one-dimensional organic–inorganic hybrid ANiCl₃ compounds.

The design of new chiral materials usually requires stereoselective organic synthesis to create molecules with chiral centers. Less commonly, achiral molecules can self-assemble into chiral materials, despite the absence of intrinsic molecular chirality. Here, we demonstrate the assembly of high-symmetry molecules into a chiral van der Waals structure by synthesizing crystals of C₆₀(SnI₄)₂ from icosahedral buckminsterfullerene (C₆₀) and tetrahedral SnI₄ molecules through spontaneous self-assembly. The SnI₄ tetrahedra template the Sn atoms into a chiral cubic three-connected net of the SrSi₂ type. Our results represent the remarkable emergence of a self-assembled chiral material from two of the most highly symmetric molecules, demonstrating that almost any molecular, nanocrystalline, or engineered precursor can be considered when designing chiral assemblies.

Despite the tremendous interest in halide perovskite solar cells, the structural reasons that cause the all-inorganic perovskite CsPbI₃ to be unstable at room temperature remain mysterious, especially since many tolerance-factor-based approaches predict CsPbI₃ should be stable as a perovskite. Here single-crystal X-ray diffraction and X-ray pair distribution function (PDF) measurements characterize bulk perovskite CsPbI₃ from 100 to 295 K to elucidate its thermodynamic instability. While Cs occupies a single site from 100 to 150 K, it splits between two sites from 175 to 295 K with the second site having a lower effective coordination number, which, along with other structural parameters, suggests that Cs rattles in its coordination polyhedron. PDF measurements reveal that on the length scale of the unit cell, the PbI octahedra concurrently become greatly distorted, with one of the IPbI angles approaching 82° compared to the ideal 90°. The rattling of Cs, low number of CsI contacts, and high degree of octahedral distortion cause the instability of perovskite-phase CsPbI_3. These results reveal the limitations of tolerance factors in predicting perovskite stability and provide detailed structural information that suggests methods to engineer stable CsPbI₃-based solar cells.