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Register a new userNearly room temperature ferromagnetism in pressure-induced correlated metallic state of van der Waals insulator CrGeTe$_3$
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A complex interplay of different energy scales involving Coulomb repulsion, spin-orbit coupling and Hunds coupling energy in two-dimensional (2D) van der Waals (vdW) material produces novel emerging physical state. For instance, ferromagnetism in vdW charge transfer insulator CrGeTe$_3$, that provides a promising platform to simultaneously manipulate the magnetic and electrical properties for potential device implementation using few layers thick materials. Here, we show a continuous tuning of magnetic and electrical properties of CrGeTe$_3$ single crystal using pressure. With application of pressure, CrGeTe$_3$ transforms from a FM insulator with Curie temperature, $T_{rm{C}} sim $ 66 K at ambient condition to a correlated 2D Fermi metal with $T_{rm{C}}$ exceeding $sim$ 250 K. Notably, absence of an accompanying structural distortion across the insulator-metal transition (IMT) suggests that the pressure induced modification of electronic ground states are driven by electronic correlation furnishing a rare example of bandwidth-controlled IMT in a vdW material.
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The bosonic analogues of topological insulators have been proposed in numerous theoretical works, but their experimental realization is still very rare, especially for spin systems. Recently, two-dimensional (2D) honeycomb van der Waals (vdW) ferromagnets have emerged as a new platform for topological spin excitations. Here, via a comprehensive inelastic neutron scattering study and theoretical analysis of the spin-wave excitations, we report the realization of topological magnon insulators in CrXTe$_3$ (X=Si, Ge) compounds. The nontrivial nature and intrinsic tunability of the gap opening at the magnon band-crossing Dirac points are confirmed, while the emergence of the corresponding in-gap topological edge states is demonstrated theoretically. The realization of topological magnon insulators with intrinsic gap-tunability in this class of remarkable 2D materials will undoubtedly lead to new and fascinating technological applications in the domain of magnonics and topological spintronics.
Layered van-der-Waals 2D magnetic materials are of great interest in fundamental condensed-matter physics research, as well as for potential applications in spintronics and device physics. We present neutron powder diffraction data using new ultra-high-pressure techniques to measure the magnetic structure of Mott-insulating 2D honeycomb antiferromagnet FePS$_3$ at pressures up to 183 kbar and temperatures down to 80 K. These data are complemented by high-pressure magnetometry and reverse Monte Carlo modeling of the spin configurations. As pressure is applied, the previously-measured ambient-pressure magnetic order switches from an antiferromagnetic to a ferromagnetic interplanar interaction, and from 2D-like to 3D-like character. The overall antiferromagnetic structure within the $ab$ planes, ferromagnetic chains antiferromagnetically coupled, is preserved, but the magnetic propagation vector is altered from $(0:1:frac{1}{2})$ to $(0:1:0)$, a halving of the magnetic unit cell size. At higher pressures, coincident with the second structural transition and the insulator-metal transition in this compound, we observe a suppression of this long-range-order and emergence of a form of magnetic short-range order which survives above room temperature. Reverse Monte Carlo fitting suggests this phase to be a short-ranged version of the original ambient pressure structure - with a return to antiferromagnetic interplanar correlations. The persistence of magnetism well into the HP-II metallic state is an observation in seeming contradiction with previous x-ray spectroscopy results which suggest a spin-crossover transition.
The van der Waals ferromagnet Fe5GeTe2 has a Curie temperature TC of about 270 K, which can be raised above room temperature by tuning the Fe deficiency content. To achieve insights into its ferromagnetic exchange, we have studied the critical behavior by measuring the magnetization in bulk Fe5GeTe2 crystal around the ferromagnetic to paramagnetic phase transition. The analysis of the magnetization by employing various techniques including the modified Arrott plot, Kouvel-Fisher plot and critical isotherm analysis achieved a set of reliable critical exponents with TC = 273.7 K, beta = 0.3457, gamma = 1.40617, and delta = 5.021, suggesting a three-dimensional magnetic exchange with the distance decaying as J(r) ~ (r)$^-4.916, which is close to that of a three-dimensional Heisenberg model with long-range magnetic coupling.
The individual building blocks of van der Waals (vdW) heterostructures host fascinating physical phenomena, ranging from ballistic electron transport in graphene to striking optical properties of MoSe2 sheets. The presence of bonded and non-bonded cohesive interactions in a vdW heterostructure, promotes diversity in their structural arrangements, which in turn profoundly modulate the properties of their individual constituents. Here, we report on the presence of correlated structural disorder coexisting with the nearly perfect crystallographic order along the growth direction of epitaxial vdW heterostructures of Bi2Se3/graphene/SiC. Using the depth penetration of X-ray diffraction microscopy and scattering, we probed their crystal structure from atomic to mesoscopic length scales, to reveal that their structural diversity is underpinned by spatially correlated disorder states. The presence of the latter induces on a system, widely considered to behave as a collection of nearly independent 2-dimensional units, a pseudo-3-dimensional character, when subjected to epitaxial constraints and ordered substrate interactions. These findings shed new light on the nature of the vast structural landscape of vdW heterostructures and could enable new avenues in modulating their unique properties by correlated disorder.
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 NiPS$_3$ 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 the 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.
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