Isostructural Mott transition in 2D honeycomb antiferromagnet V 0.9 PS 3

Abstract: The MPX3 family of magnetic van-der-Waals materials (M denotes a first row transition metal and X either S or Se) are currently the subject of broad and intense attention for low-dimensional magnetism and transport and also for novel device and technological applications, but the vanadium compounds have until this point not been studied beyond their basic properties. We present the observation of an isostructural Mott insulator–metal transition in van-der-Waals honeycomb antiferromagnet V0.9PS3 through high-pressure x-ray diffraction and transport measurements. We observe insulating variable-range-hopping type resistivity in V0.9PS3, with a gradual increase in effective dimensionality with increasing pressure, followed by a transition to a metallic resistivity temperature dependence between 112 and 124 kbar. The metallic state additionally shows a low-temperature upturn we tentatively attribute to the Kondo effect. A gradual structural distortion is seen between 26 and 80 kbar, but no structural change at higher pressures corresponding to the insulator–metal transition. We conclude that the insulator–metal transition occurs in the absence of any distortions to the lattice—an isostructural Mott transition in a new class of two-dimensional material, and in strong contrast to the behavior of the other MPX3 compounds

Strongly adhesive dry transfer technique for van der Waals heterostructure

That one can stack van der Waals materials with atomically sharp interfaces has provided a new material platform of constructing heterostructures. The technical challenge of mechanical stacking is picking up the exfoliated atomically thin materials after mechanical exfoliation without chemical and mechanical degradation. Chemically inert hexagonal boron nitride (hBN) has been widely used for encapsulating and picking up vdW materials. However, due to the relatively weak adhesion of hBN, assembling vdW heterostructures based on hBN has been limited. We report a new dry transfer technique. We used two vdW semiconductors (ZnPS3 and CrPS4) to pick up and encapsulate layers for vdW heterostructures, which otherwise are known to be hard to fabricate. By combining with optimized polycaprolactone (PCL) providing strong adhesion, we demonstrated various vertical heterostructure devices, including quasi-2D superconducting NbSe2 Josephson junctions with atomically clean interface. The versatility of the PCL-based vdW stacking method provides a new route for assembling complex 2D vdW materials without interfacial degradation.Comment: Accepted for publication in 2D Material

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 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.Comment: 24 pages, 23 figure

Electronic and vibrational properties of the two-dimensional Mott insulator V0.9PS3 under pressure

We present a Raman spectroscopic study of the layered antiferromagnetic Mott insulator V(0.9)PS(3 )and demonstrate the evolution of the spectra with applied quasihydrostatic pressure. Clear features in the spectra are seen at the pressures identified as corresponding to a structural transition between 20 and 80 kbar and the insulator-metal transition at 120 kbar. The feature at 120 kbar can be understood as a stiffening of interplanar vibrations, linking the metallization to a crossover from two- to three-dimensionality. Theoretical ab initio calculations, using the previously determined high-pressure structures, were able to reproduce the measured spectra and map each peak to specific vibration modes. We additionally show calculations of the high-pressure band structure in these materials, where the opening of a band gap with an included Hubbard U term and its subsequent closing with pressure are clearly demonstrated. This little-studied material shows great promise as a model system for the fundamental study of low-dimensional magnetism and Mott physics. ©2019 American Physical Societ

Observation of plateau-like magnetoresistance in twisted Fe3GeTe2/Fe3GeTe2 junction

© 2020 Author(s). Controlling the stacking of van der Waals (vdW) materials is found to produce exciting new findings, since hetero- or homo-structures have added the diverse possibility of assembly and manipulated functionalities. However, so far, the homostructure with a twisted angle based on the magnetic vdW materials remains unexplored. Here, we achieved a twisted magnetic vdW Fe3GeTe2 (FGT)/Fe3GeTe2 junction with broken crystalline symmetry. A clean and metallic vdW junction is evidenced by the temperature-dependent resistance and the linear I-V curve. Unlike the pristine FGT, a plateau-like magnetoresistance (PMR) is observed in the magnetotransport of our homojunction due to the antiparallel magnetic configurations of the two FGT layers. The PMR ratio is found to be similar to 0.05% and gets monotonically enhanced as temperature decreases like a metallic giant magnetoresistance. Such a tiny PMR ratio is at least three orders of magnitude smaller than the tunneling magnetoresistance ratio, justifying our clean metallic junction without a spacer. Our findings demonstrate the feasibility of the controllable homostructure and shed light on future spintronics using magnetic vdW materials. Published under license by AIP Publishing11sciescopu

Observation of plateau-like magnetoresistance in twisted Fe3GeTe2/Fe3GeTe2 junction

© 2020 Author(s). Controlling the stacking of van der Waals (vdW) materials is found to produce exciting new findings, since hetero- or homo-structures have added the diverse possibility of assembly and manipulated functionalities. However, so far, the homostructure with a twisted angle based on the magnetic vdW materials remains unexplored. Here, we achieved a twisted magnetic vdW Fe3GeTe2 (FGT)/Fe3GeTe2 junction with broken crystalline symmetry. A clean and metallic vdW junction is evidenced by the temperature-dependent resistance and the linear I-V curve. Unlike the pristine FGT, a plateau-like magnetoresistance (PMR) is observed in the magnetotransport of our homojunction due to the antiparallel magnetic configurations of the two FGT layers. The PMR ratio is found to be similar to 0.05% and gets monotonically enhanced as temperature decreases like a metallic giant magnetoresistance. Such a tiny PMR ratio is at least three orders of magnitude smaller than the tunneling magnetoresistance ratio, justifying our clean metallic junction without a spacer. Our findings demonstrate the feasibility of the controllable homostructure and shed light on future spintronics using magnetic vdW materials. Published under license by AIP Publishing11sciescopu

Isostructural Mott transition in 2D honeycomb antiferromagnet V 0.9 PS 3

Abstract: The MPX3 family of magnetic van-der-Waals materials (M denotes a first row transition metal and X either S or Se) are currently the subject of broad and intense attention for low-dimensional magnetism and transport and also for novel device and technological applications, but the vanadium compounds have until this point not been studied beyond their basic properties. We present the observation of an isostructural Mott insulator–metal transition in van-der-Waals honeycomb antiferromagnet V0.9PS3 through high-pressure x-ray diffraction and transport measurements. We observe insulating variable-range-hopping type resistivity in V0.9PS3, with a gradual increase in effective dimensionality with increasing pressure, followed by a transition to a metallic resistivity temperature dependence between 112 and 124 kbar. The metallic state additionally shows a low-temperature upturn we tentatively attribute to the Kondo effect. A gradual structural distortion is seen between 26 and 80 kbar, but no structural change at higher pressures corresponding to the insulator–metal transition. We conclude that the insulator–metal transition occurs in the absence of any distortions to the lattice—an isostructural Mott transition in a new class of two-dimensional material, and in strong contrast to the behavior of the other MPX3 compounds

Local nuclear and magnetic order in the two-dimensional spin glass Mn0.5Fe0.5PS3

© 2020 American Physical Society. We present a comprehensive study of the short-ranged nuclear and magnetic order in the two-dimensional spin glass, Mn0.5Fe0.5PS3. Nuclear neutron scattering data reveal a random distribution of Mn2+ and Fe2+ ions within the honeycomb layers, which gives rise to a spin glass state through inducing competition between neighboring exchange interactions, indicated in magnetic susceptibility data by a cusp at the glass transition, T-g = 35 K. Analysis of magnetic diffuse neutron scattering data collected for both single-crystal and polycrystalline samples gives further insight into the origin of the spin glass phase, with spin correlations revealing a mixture of satisfied and unsatisfied correlations between magnetic moments within the honeycomb planes, which can be explained by considering the magnetic structures of the parent compounds, MnPS3 and FePS3. We found that, on approaching T-g from above, an ensemble-averaged correlation length of xi = 5.5(6)angstrom developed between satisfied correlations, and below T-g, the glassy behavior gave rise to a distance-independent correlation between unsatisfied moments. Correlations between the planes were found to be very weak, which mirrored our observations of rodlike structures parallel to the c* axis in our single-crystal diffraction measurements, confirming the two-dimensional nature of Mn0.5Fe0.5PS311sci