Magnetism in two-dimensional materials is not only of fundamental scientific interest but also a promising candidate for numerous applications. However, studies so far, especially the experimental ones, have been mostly limited to the magnetism arising from defects, vacancies, edges or chemical dopants which are all extrinsic effects. Here, we report on the observation of intrinsic antiferromagnetic ordering in the two-dimensional limit. By monitoring the Raman peaks that arise from zone folding due to antiferromagnetic ordering at the transition temperature, we demonstrate that FePS3 exhibits an Ising-type antiferromagnetic ordering down to the monolayer limit, in good agreement with the Onsager solution for two-dimensional order-disorder transition.The transition temperature remains almost independent of the thickness from bulk to the 2 monolayer limit with TN ~118 K, indicating that the weak interlayer interaction has little effect on the antiferromagnetic ordering. KEYWORDSIsing model, Antiferromagentism, Magnetic ordering in 2 Dimension, FePS3, Iron phosphorus trisulfide, Raman spectroscopy 3 Magnetism has played an important role in advancing our understanding of the quantum nature of materials. Especially, low-dimensional magnetism has been a fertile playground, in which novel physical concepts have been learned and thereby moved the frontiers of the modern understanding of materials science. Most of the three-dimensional magnetic systems, other than some exceptional cases of quantum spin and/or strong frustration, host a magnetic order. On the other hand, fluctuations are so strong and easily destroy stabilization of order parameters in onedimensional systems as pointed out in the seminal work by Bethe. 1 Two-dimensional (2D) systems, on the other hand, have attracted much attention because the presence or absence of long-range order depends on the type of spin-spin interactions, which themselves compete with intrinsic fluctuations of either quantum and/or thermal nature.The XXZ Hamiltonian reads 2 ( )where XY J and I J are spin-exchange energies on the basal plane and along the c-axis, respectively; using an order-converting dual transformation that unlike the 1D system there is a phase transition at a finite temperature in the 2D Ising system. 4 Therefore, ferromagnetic or antiferromagnetic ordering in the 2D limit is possible only in the Ising model. There has been some indirect test of this prediction including the most notable one by Kim and Chan using CH4 molecules adsorbed 4 on graphite. 5 However, despite its fundamental importance, there has been no experimental work using a real 2D magnetic material.2D van der Waals (vdW) materials could be an ideal system for the study of 2D magnetism. 6 Unfortunately, however, finding suitable vdW materials and producing atomically thin magnetic materials have been a challenge. Although there have been a few reports of producing atomically thin samples of magnetic materials, 7-10 observation of magnetic ordering in the atomically thin limit has been l...

Emergent phenomena driven by electronic reconstructions in oxide heterostructures have been intensively discussed. However, the role of these phenomena in shaping the electronic properties in van der Waals heterointerfaces has hitherto not been established. By reducing the material thickness and forming a heterointerface, we find two types of charge-ordering transitions in monolayer VSe on graphene substrates. Angle-resolved photoemission spectroscopy (ARPES) uncovers that Fermi-surface nesting becomes perfect in ML VSe. Renormalization-group analysis confirms that imperfect nesting in three dimensions universally flows into perfect nesting in two dimensions. As a result, the charge-density wave-transition temperature is dramatically enhanced to a value of 350 K compared to the 105 K in bulk VSe. More interestingly, ARPES and scanning tunneling microscopy measurements confirm an unexpected metal-insulator transition at 135 K that is driven by lattice distortions. The heterointerface plays an important role in driving this novel metal-insulator transition in the family of monolayer transition-metal dichalcogenides.

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