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The layered crystal structure of Cr2Ge2Te6 shows ferromagnetic ordering at the two‐dimensional limit, which holds promise for spintronic applications. However, external voltage pulses can trigger amorphization of the material in nanoscale electronic devices, and it is unclear whether the loss of structural ordering leads to a change in magnetic properties. Here, it is demonstrated that Cr2Ge2Te6 preserves the spin‐polarized nature in the amorphous phase, but undergoes a magnetic transition to a spin glass state below 20 K. Quantum‐mechanical computations reveal the microscopic origin of this transition in spin configuration: it is due to strong distortions of the CrTeCr bonds, connecting chromium‐centered octahedra, and to the overall increase in disorder upon amorphization. The tunable magnetic properties of Cr2Ge2Te6 can be exploited for multifunctional, magnetic phase‐change devices that switch between crystalline and amorphous states. [ABSTRACT FROM AUTHOR]

While metals can be readily processed and reshaped by cold rolling, most bulk inorganic semiconductors are brittle materials that tend to fracture when plastically deformed. Manufacturing thin sheets and foils of inorganic semiconductors is therefore a bottleneck problem, severely restricting their use in flexible electronic applications. It is recently reported that a few single‐crystalline 2D van der Waals (vdW) semiconductors, such as InSe, are deformable under compressive stress. Here it is demonstrated that intralayer fracture toughness can be tailored via compositional design to make inorganic semiconductors processable by cold rolling. Systematic ab initio calculations covering a range of van der Waals semiconductors homologous to InSe are reported, leading to material‐property maps that forecast trends in both the susceptibility to interlayer slip and the intralayer fracture toughness against cracking. GaSe is predicted, and experimentally confirmed, to be practically amenable to being rolled to large (three quarters) thickness reduction and length extension by a factor of three. The fracture toughness and cleavage energy are predicted to be 0.25 MPa m0.5 and 15 meV Å−2, respectively. The findings open a new realm of possibility for alloy selection and design toward processing‐friendly group‐III chalcogenides for practical applications. [ABSTRACT FROM AUTHOR]

B Deformable Inorganic Semiconductors b In article number 2203776, Wei Zhang, En Ma, and co-workers achieve inorganic semiconductors that can be shaped via cold-rolling, advocating adequate fracture toughness in their design. The cracking-resistant van der Waals crystal, depicted here in the form of a highly deformed Mobius ribbon, is amenable to use in flexible thermoelectric, neuromorphic and optoelectronic devices. Designing Inorganic Semiconductors with Cold-Rolling Processability (Adv. Sci. 30/2022). [Extracted from the article]