Observation of Three-State Nematicity and Domain Evolution in Atomically Thin Antiferromagnetic NiPS3.

Nickel phosphorus trisulfide (NiPS3), a van der Waals 2D antiferromagnet, has received significant interest for its intriguing properties in recent years. However, despite its fundamental importance in the physics of low-dimensional magnetism and promising potential for technological applications, the study of magnetic domains in NiPS3 down to an atomically thin state is still lacking. Here, we report the layer-dependent magnetic characteristics and magnetic domains in NiPS3 by employing linear dichroism spectroscopy, polarized microscopy, spin-correlated photoluminescence, and Raman spectroscopy. Our results reveal the existence of the paramagnetic-to-antiferromagnetic phase transition in bulk to bilayer NiPS3 and provide evidence of the role of stronger spin fluctuations in thin NiPS3. Furthermore, our study identifies three distinct antiferromagnetic domains within atomically thin NiPS3 and captures the thermally activated domain evolution. Our findings provide crucial insights for the development of antiferromagnetic spintronics and related technologies.

Synthesis of 2D layered transition metal (Ni, Co) hydroxides via edge-on condensation.

Layered transition metal hydroxides (LTMHs) with transition metal centers sandwiched between layers of coordinating hydroxide anions have attracted considerable interest for their potential in developing clean energy sources and storage technologies. However, two-dimensional (2D) LTMHs remain largely understudied in terms of physical properties and applications in electronic devices. Here, for the first time we report > 20 µm α-Ni(OH)2 2D crystals, synthesized from hydrothermal reaction. And an edge-on condensation mechanism assisted with the crystal field geometry is proposed to understand the 2D intra-planar growth of the crystals, which is also testified through series of systematic comparative studies. We also report the successful synthesis of 2D Co(OH)2 crystals (> 40 µm) with more irregular shape due to the slightly distorted octahedral geometry of the crystal field. Moreover, the detailed structural characterization of synthesized α-Ni(OH)2 are performed. The optical band gap energy is extrapolated as 2.54 eV from optical absorption measurements and the electronic bandgap is measured as 2.52 eV from reflected electrons energy loss spectroscopy (REELS). We further demonstrate its potential as a wide bandgap (WBG) semiconductor for high voltage operation in 2D electronics with a high breakdown strength, 4.77 MV/cm with 4.9 nm thickness. The successful realization of the 2D LTMHs opens the door for future exploration of more fundamental physical properties and device applications.