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Rare-earth chalcogenide compounds ARECh2 (A = alkali or monovalent metal, RE = rare earth, Ch = O, S, Se, Te) are a large family of quantum spin liquid (QSL) candidate materials. NaYbS2 is a representative member of the family. Several key issues on NaYbS2, particularly how to determine the highly anisotropic spin Hamiltonian and describe the magnetism at finite temperatures and the ground state, remain to be addressed. In this paper, we conducted an in-depth and comprehensive study on the magnetism of NaYbS2 from finite temperatures to the ground state. Firstly, we successfully detected three crystalline electric field (CEF) excitation energy levels using low-temperature Raman scattering technique. Combining them with the CEF theory and magnetization data, we worked out the CEF parameters, CEF energy levels, and CEF wavefunctions. We further determined a characteristic temperature of ∼40 K, above which the magnetism is dominated by CEF excitations while below which the spin-exchange interactions play a main role. The characteristic temperature has been confirmed by the temperature-dependent electron spin resonance (ESR) linewidth. Low-temperature ESR experiments on the dilute magnetic doped crystal of NaYb0.1Lu0.9S2 further helped us to determine the accurate g-factor. Next, we quantitatively obtained the spin-exchange interactions in the spin Hamiltonian by consistently simulating the magnetization and specific heat data. Finally, the above studies allow us to explore the ground state magnetism of NaYbS2 by using the density matrix renormalization group. We combined numerical calculations and experimental results to demonstrate that the ground state of NaYbS2 is a Dirac-like QSL. [ABSTRACT FROM AUTHOR]

The physical properties of most 2D materials are highly dependent on the nature of their interlayer interaction. In-depth studies of the interlayer interaction are beneficial to the understanding of the physical properties of 2D materials and permit the development of related devices. Layered magnetic NiPS3 has unique magnetic and electronic properties. The electronic band structure and corresponding magnetic state of NiPS3 are expected to be sensitive to the interlayer interaction, which can be tuned by external pressure. Here, we report an insulator-metal transition accompanied by the collapse of magnetic order during the 2D-3D structural crossover induced by hydrostatic pressure. A two-stage phase transition from a monoclinic (C2/m) to a trigonal (P 3 ¯ 1 m) lattice is identified via ab initio simulations and confirmed via high-pressure X-ray diffraction and Raman scattering; this transition corresponds to a layer-by-layer slip mechanism along the a-axis. Temperature-dependent resistance measurements and room temperature infrared spectroscopy under different pressures demonstrate that the insulator-metal transition and the collapse of the magnetic order occur at ∼20 GPa, which is confirmed by low-temperature Raman scattering measurements and theoretical calculations. These results establish a strong correlation between the structural change, electric transport, and magnetic phase transition and expand our understanding of layered magnetic materials. Moreover, the structural transition caused by the interlayer displacement has significance for designing similar devices at ambient pressure. [ABSTRACT FROM AUTHOR]