Imaging Thermally Fluctuating Néel Vectors in van der Waals Antiferromagnet NiPS3.

Studying antiferromagnetic domains is essential for fundamental physics and potential spintronics applications. Despite their importance, few systematic studies have been performed on antiferromagnet (AFM) domains with high spatial resolution in van der Waals (vdW) materials, and direct probing of the Néel vectors remains challenging. In this work, we found multidomain states in the vdW AFM NiPS3, a material extensively investigated for its unique magnetic exciton. We employed photoemission electron microscopy combined with the X-ray magnetic linear dichroism (XMLD-PEEM) to image the NiPS3's magnetic structure. The nanometer-spatial resolution of XMLD-PEEM allows us to determine local Néel vector orientations and discover thermally fluctuating Néel vectors that are independent of the crystal symmetry even at 65 K, well below the TN of 155 K. We demonstrate that an in-plane orbital moment of the Ni ion is responsible for the weak magnetocrystalline anisotropy. The observed thermal fluctuations of the antiferromagnetic domains may explain the broadening of magnetic exciton peaks at higher temperatures.

Possible Persistence of Multiferroic Order down to Bilayer Limit of van der Waals Material NiI2.

Realizing a state of matter in two dimensions has repeatedly proven a novel route of discovering new physical phenomena. Van der Waals (vdW) materials have been at the center of these now extensive research activities. They offer a natural way of producing a monolayer of matter simply by mechanical exfoliation. This work demonstrates that the possible multiferroic state with coexisting antiferromagnetic and ferroelectric orders persists down to the bilayer flake of NiI2. By exploiting the optical second-harmonic generation technique, both magnitude and direction of the ferroelectric order, arising from the cycloidal spin order, are successfully traced. The possible multiferroic state's transition temperature decreases from 58 K for the bulk to about 20 K for the bilayer. Our observation will spur extensive efforts to demonstrate multifunctionality in vdW materials, which have been tried mostly by using heterostructures of singly ferroic ones until now.

Terahertz Spectroscopy and DFT Analysis of Phonon Dynamics of the Layered Van der Waals Semiconductor Nb3 X 8 (X = Cl, I).

We have conducted a terahertz spectroscopic study and a density functional theory analysis of the phonon dynamics of the layered van der Waals semiconductors Nb3Cl8 and Nb3I8. Several infrared-active phonon modes were observed in the terahertz region, and their frequencies were found to be in excellent agreement with our first-principles lattice dynamics calculations. For Nb3Cl8, the observed phonon spectra are consistent with a structural transition at 90 K from the high-temperature P3̅m1 phase to the low-temperature R3̅m phase. Also, our study confirmed that the structural and magnetic transitions were coupled in Nb3Cl8. For Nb3I8, which is nonmagnetic at and below room temperature, no significant temperature or magnetic field dependence was observed in the phonon spectra. Our study provides an intriguing connection between the structural properties and the paramagnetic-nonmagnetic transitions in Nb3Cl8 and Nb3I8.

Multiferroic-Enabled Magnetic-Excitons in 2D Quantum-Entangled Van der Waals Antiferromagnet NiI2.

Matter-light interaction is at the center of diverse research fields from quantum optics to condensed matter physics, opening new fields like laser physics. A magnetic exciton is one such rare example found in magnetic insulators. However, it is relatively rare to observe that external variables control matter-light interaction. Here, it is reported that the broken inversion symmetry of multiferroicity can act as an external knob enabling magnetic excitons in the van der Waals antiferromagnet NiI2 . It is further discovered that this magnetic exciton arises from a transition between Zhang-Rice-triplet and Zhang-Rice-singlet fundamentally quantum-entangled states. This quantum entanglement produces an ultrasharp optical exciton peak at 1.384 eV with a 5 meV linewidth. The work demonstrates that NiI2 is 2D magnetically ordered with an intrinsically quantum-entangled ground state.

Gigantic Current Control of Coercive Field and Magnetic Memory Based on Nanometer-Thin Ferromagnetic van der Waals Fe3 GeTe2.

Controlling magnetic states by a small current is essential for the next-generation of energy-efficient spintronic devices. However, it invariably requires considerable energy to change a magnetic ground state of intrinsically quantum nature governed by fundamental Hamiltonian, once stabilized below a phase-transition temperature. Here, it is reported that, surprisingly, an in-plane current can tune the magnetic state of the nanometer-thin van der Waals ferromagnet Fe3 GeTe2 from a hard magnetic state to a soft magnetic state. It is a direct demonstration of the current-induced substantial reduction of the coercive field. This surprising finding is possible because the in-plane current produces a highly unusual type of gigantic spin-orbit torque for Fe3 GeTe2 . In addition, a working model of a new nonvolatile magnetic memory based on the principle of the discovery in Fe3 GeTe2 , controlled by a tiny current, is further demonstrated. The findings open up a new window of exciting opportunities for magnetic van der Waals materials with potentially huge impact on the future development of spintronic and magnetic memory.

Exciton-driven antiferromagnetic metal in a correlated van der Waals insulator.

Collective excitations of bound electron-hole pairs-known as excitons-are ubiquitous in condensed matter, emerging in systems as diverse as band semiconductors, molecular crystals, and proteins. Recently, their existence in strongly correlated electron materials has attracted increasing interest due to the excitons' unique coupling to spin and orbital degrees of freedom. The non-equilibrium driving of such dressed quasiparticles offers a promising platform for realizing unconventional many-body phenomena and phases beyond thermodynamic equilibrium. Here, we achieve this in the van der Waals correlated insulator NiPS3 by photoexciting its newly discovered spin-orbit-entangled excitons that arise from Zhang-Rice states. By monitoring the time evolution of the terahertz conductivity, we observe the coexistence of itinerant carriers produced by exciton dissociation and a long-wavelength antiferromagnetic magnon that coherently precesses in time. These results demonstrate the emergence of a transient metallic state that preserves long-range antiferromagnetism, a phase that cannot be reached by simply tuning the temperature. More broadly, our findings open an avenue toward the exciton-mediated optical manipulation of magnetism.

Air-Stable and Layer-Dependent Ferromagnetism in Atomically Thin van der Waals CrPS4.

Ferromagnetism in two-dimensional materials presents a promising platform for the development of ultrathin spintronic devices with advanced functionalities. Recently discovered ferromagnetic van der Waals crystals such as CrI3, readily isolated two-dimensional crystals, are highly tunable through external fields or structural modifications. However, there remains a challenge because of material instability under air exposure. Here, we report the observation of an air-stable and layer-dependent ferromagnetic (FM) van der Waals crystal, CrPS4, using magneto-optic Kerr effect microscopy. In contrast to the antiferromagnetic (AFM) bulk, the FM out-of-plane spin orientation is found in the monolayer crystal. Furthermore, alternating AFM and FM properties observed in even and odd layers suggest robust antiferromagnetic exchange interactions between layers. The observed ferromagnetism in these crystals remains resilient even after the air exposure of about a day, providing possibilities for the practical applications of van der Waals spintronics.

Tuning dimensionality in van-der-Waals antiferromagnetic Mott insulators TMPS3.

We present an overview of our recent work in tuning and controlling the structural, magnetic and electronic dimensionality of 2D van-der-Waals antiferromagnetic compounds (Transition-Metal)PS3. Low-dimensional magnetic systems such as these provide rich opportunities for studying new physics and the evolution of established behaviours with changing dimensionality. These materials can be exfoliated to monolayer thickness and easily stacked and combined into functional heterostructures. Alternatively, the application of hydrostatic pressure can be used to controllably close the van-der-Waals interplanar gap and tune the crystal structure and electron exchange paths towards a 3D nature. We collect and discuss trends and contrasts in our data from electrical transport, Raman scattering and synchrotron x-ray measurements, as well as insight from theoretical calculations and other results from the literature. We discuss structural transitions with pressure common to all materials measured, and link these to Mott insulator-transitions in these compounds at high pressures. Key new results include magnetotransport and resistivity data in the high-pressure metallic states, which show potentially interesting qualities for a new direction of future work focussed on low temperature transport and quantum critical physics.

Hard ferromagnetic van-der-Waals metal (Fe,Co)3GeTe2: a new platform for the study of low-dimensional magnetic quantum criticality.

The widely-studied ferromagnetic van-der-Waals (vdW) metal Fe3GeTe2 has great promise for studies of quantum criticality in the 2D limit, but is limited by a relatively high Curie temperature in excess of 200 K. To help render the quantum critical point achievable in such a system within the reach of practically possible tuning methods, we have grown single crystals of a variant of (Fe,Co)3GeTe2 with useful physical properties for both this purpose and the wider study of low-dimensional magnetism and spin transport. (Fe,Co)3GeTe2 is found through x-ray diffraction and electron microscopy to have an equivalent crystal structure to Fe3GeTe2, with a random distribution of the cobalt dopant sites. It exhibits a sharp ferromagnetic transition at a value below 40 K, a stronger anisotropy and a coercive field ten times larger than that of Fe3GeTe2. The transport properties and specific heat show the electronic properties and strong correlations of Fe3GeTe2 to be near-unchanged in this doped material. We demonstrate that (Fe,Co)3GeTe2 can be cleanly exfoliated down to monolayer thickness. This unprecedented hard metallic vdW ferromagnet is a valuable new addition to the limited range of materials available for the study of 2D magnetism.