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            Abstract Recently, layered transition metal thiophosphate MPX3(M= transition metals,X= S or Se) have gained significant attention because of their rich magnetic, optical, and electronic properties. Specifically, the diverse magnetic structures and the robustness of magnetism in the two-dimensional (2D) limit have made them prominent candidates to study 2D magnetism. Numerous efforts such as substitutions and interlayer intercalations have been adopted to tune the magnetic properties of these materials, which has greatly deepened the understanding of the underlying mechanisms that govern the properties. In this work, we focus on modifying the magnetism of Ising-type antiferromagnet FePS3using electrochemical lithium intercalation. Our work demonstrate the effectiveness of electrochemical intercalation as a controllable tool to modulating magnetism, including tuning magnetic ordering temperature and inducing low temperature spin-glass state, offering an approach for implementing this material into applications.more » « lessFree, publicly-accessible full text available February 14, 2026
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            Free, publicly-accessible full text available April 1, 2026
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            Encapsulating Cs4PbBr6 quantum dots in silicon nano-sheets not only stabilizes the halide perovskite, but also takes advantage of the nano-sheet for a compatible integration with the traditional silicon semiconductor. Here, we report the preparation of un-passivated Cs4PbBr6 ellipsoidal nanocrystals and pseudo-spherical quantum dots in silicon nano-sheets and their enhanced photoluminescence (PL). For a sample with low concentrations of quantum dots in silicon nano-sheets, the emission from Cs4PbBr6 pseudo-spherical quantum dots is quenched and is dominated with Pb2+ ion/silicene emission, which is very stable during the whole measurement period. For a high concentration of Cs4PbBr6 ellipsoidal nanocrystals in silicon nano-sheets, we have observed Förster resonance energy transfer with up to 87% efficiency through the oscillation of two PL peaks when UV excitation switches between on and off, using recorded video and PL lifetime measurements. In an area of a non-uniform sample containing both ellipsoidal nanocrystals and pseudo-spherical quantum dots, where Pb2+ ion/silicene emissions, broadband emissions from quantum dots, and bandgap edge emissions (515 nm) appear, the 515 nm peak intensity increases five times over 30 min of UV excitation, probably due to a photon recycling effect. This irradiated sample has been stable for one year of ambient storage. Cs4PbBr6 quantum dots encapsulated in silicon nano-sheets can lead to applications of halide perovskite light emitting diodes (PeLEDs) and integration with traditional semiconductor materials.more » « less
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            Abstract Antiferromagnetic van der Waals‐typeM2P2X6compounds provide a versatile material platform for studying 2D magnetism and relevant phenomena. Establishing ferromagnetism in 2D materials is technologically valuable. Though magnetism is generally tunable via a chemical way, it is challenging to induce ferromagnetism with isovalent chalcogen and bimetallic substitutions inM2P2X6. Here, we report co‐substitution of Cu1+and Cr3+for Ni2+in Ni2P2S6, creating CuxNi2(1‐x)CrxP2S6medium‐entropy alloys spanning a full substitution range (x= 0 to 1). Such substitution strategy leads to a unique evolution in crystal structure and magnetic phases that are distinct from traditional isovalent bimetallic doping, with Cu and Cr co‐substitution enhancing ferromagnetic correlations and generating a weak ferromagnetic phase in intermediate compositions. This aliovalent substitution strategy offers a universal approach for tuning layered magnetism in antiferromagnetic systems, which along with the potential for light‐matter interaction and high‐temperature ferroelectricity, can enable multifunctional device applications.more » « less
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