Exchange Bias Effect in Ferro-/Antiferromagnetic van der Waals Heterostructures.

The recent discovery of magnetic van der Waals (vdW) materials provides a platform to answer fundamental questions on the two-dimensional (2D) limit of magnetic phenomena and applications. An important question in magnetism is the ultimate limit of the antiferromagnetic layer thickness in ferromagnetic (FM)/antiferromagnetic (AFM) heterostructures to observe the exchange bias (EB) effect, of which origin has been subject to a long-standing debate. Here, we report that the EB effect is maintained down to the atomic bilayer of AFM in the FM (Fe3GeTe2)/AFM (CrPS4) vdW heterostructure, but it vanishes at the single-layer limit. Given that CrPS4 is of A-type AFM and, thus, the bilayer is the smallest unit to form an AFM, this result clearly demonstrates the 2D limit of EB; only one unit of AFM ordering is sufficient for a finite EB effect. Moreover, the semiconducting property of AFM CrPS4 allows us to electrically control the exchange bias, providing an energy-efficient knob for spintronic devices.

Band gap, dielectric constant, and susceptibility of DNA layers as controlled by vanadium ion concentration.

Deoxyribonucleic acid (DNA) doped with transition metal ions shows great versatility for molecular-based biosensors and bioelectronics. Methodologies for developing DNA lattices (formed by synthetic double-crossover tiles) and DNA layers (used by natural salmon) doped with vanadium ions (V3+), as well as an understanding of the physical characteristics of V3+-doped DNA nanostructures, are essential in practical applications in interdisciplinary research fields. Here, DNA lattices and layers doped with V3+ are constructed through substrate-assisted growth and drop-casting methods. In addition, enhanced physical characteristics such as the band gap energy, work function, dielectric constant, and susceptibility of V3+-doped DNA nanostructures with varying V3+ concentration ([V 3+ ]) are investigated. The critical concentration ([V 3+ ]C ) at a given amount of DNA was predicted based on an analysis of the phase transition of DNA lattices from crystalline to amorphous with specific [V 3+ ]. Generally, the [V 3+ ]C provided crucial information on the structural stability and extremum physical characteristics of V3+-doped DNA nanostructures due to the optimum incorporation of V3+ into DNA. We obtained the optical absorption spectra for energy band gap estimation; Raman spectra for identifying the preferential coordination sites of V3+ in DNA; x-ray photoelectron spectra to examine the chemical state, chemical composition, and functional groups; and ultraviolet photoelectron spectra to estimate the work function. In addition, we addressed the electrical properties (i.e. current, capacitance, dielectric constant, and storage energy) and magnetic properties (magnetic field-dependent and temperature-dependent magnetizations and susceptibility) of DNA layers in the presence of V3+. The development of biocompatible materials with specific optical, electrical, and magnetic properties is required for future applications because they must have designated functionality, high efficiency, and affordability.

Electromagnetic and optical characteristics of Nb5+-doped double-crossover and salmon DNA thin films.

We report the fabrication and physical characteristics of niobium ion (Nb5+)-doped double-crossover DNA (DX-DNA) and salmon DNA (SDNA) thin films. Different concentrations of Nb5+ ([Nb5+]) are coordinated into the DNA molecules, and the thin films are fabricated via substrate-assisted growth (DX-DNA) and drop-casting (SDNA) on oxygen plasma treated substrates. We conducted atomic force microscopy to estimate the optimum concentration of Nb5+ ([Nb5+]O = 0.08 mM) in Nb5+-doped DX-DNA thin films, up to which the DX-DNA lattices maintain their structures without deformation. X-ray photoelectron spectroscopy (XPS) was performed to probe the chemical nature of the intercalated Nb5+ in the SDNA thin films. The change in peak intensities and the shift in binding energy were witnessed in XPS spectra to explicate the binding and charge transfer mechanisms between Nb5+ and SDNA molecules. UV-visible, Raman, and photoluminescence (PL) spectra were measured to determine the optical properties and thus investigate the binding modes, Nb5+ coordination sites in Nb5+-doped SDNA thin films, and energy transfer mechanisms, respectively. As [Nb5+] increases, the absorbance peak intensities monotonically increase until ∼[Nb5+]O and then decrease. However, from the Raman measurements, the peak intensities gradually decrease with an increase in [Nb5+] to reveal the binding mechanism and binding sites of metal ions in the SDNA molecules. From the PL, we observe the emission intensities to reduce them at up to ∼[Nb5+]O and then increase after that, expecting the energy transfer between the Nb5+ and SDNA molecules. The current-voltage measurement shows a significant increase in the current observed as [Nb5+] increases in the SDNA thin films when compared to that of pristine SDNA thin films. Finally, we investigate the temperature dependent magnetization in which the Nb5+-doped SDNA thin films reveal weak ferromagnetism due to the existence of tiny magnetic dipoles in the Nb5+-doped SDNA complex.

A Quenched Disorder in the Quantum-Critical Superconductor CeCoIn5.

Emergent inhomogeneous electronic phases in metallic quantum systems are crucial for understanding high-Tc superconductivity and other novel quantum states. In particular, spin droplets introduced by nonmagnetic dopants in quantum-critical superconductors (QCSs) can lead to a novel magnetic state in superconducting phases. However, the role of disorders caused by nonmagnetic dopants in quantum-critical regimes and their precise relation with superconductivity remain unclear. Here, the systematic evolution of a strong correlation between superconductive intertwined electronic phases and antiferromagnetism in Cd-doped CeCoIn5 is presented by measuring current-voltage characteristics under an external pressure. In the low-pressure coexisting regime where antiferromagnetic (AFM) and superconducting (SC) orders coexist, the critical current (Ic ) is gradually suppressed by the increasing magnetic field, as in conventional type-II superconductors. At pressures higher than the critical pressure where the AFM order disappears, Ic remarkably shows a sudden spike near the irreversible magnetic field. In addition, at high pressures far from the critical pressure point, the peak effect is not suppressed, but remains robust over the whole superconducting region. These results indicate that magnetic islands are protected around dopant sites despite being suppressed by the increasingly correlated effects under pressure, providing a new perspective on the role of quenched disorders in QCSs.

Giant coercivity enhancement in a room-temperature van der Waals magnet through substitutional metal-doping.

FexGeTe2 (x = 3, 4, and 5) systems, two-dimensional (2D) van der Waals (vdW) ferromagnetic (FM) metals with high Curie temperatures (TC), have been intensively studied to realize all-2D spintronic devices. Recently, an intrinsic FM material Fe3GaTe2 with high TC (350-380 K) has been reported. As substitutional doping changes the magnetic properties of vdW magnets, it can be a powerful means for engineering the properties of magnetic materials. Here, the coercive field (Hc) is substantially enhanced by substituting Ni for Fe in (Fe1-xNix)3GaTe2 crystals. The introduction of a Ni dopant with x = 0.03 can enhance the value of Hc up to ∼200% while maintaining the FM state at room temperature. As the doping level increases, TC decreases, whereas Hc increases up to 7 kOe at x = 0.12, which is the highest Hc reported so far. The FM characteristic is almost suppressed at x = 0.68 and a spin glass state appears. The enhancement of Hc resulting from Ni doping can be attributed to domain pinning induced by substitutional Ni atoms, as evidenced by the decrease in magnetic anisotropy energy in the crystals upon Ni doping. Our findings provide a highly effective way to control the Hc of the 2D vdW FM metal Fe3GaTe2 for the realization of Fe3GaTe2 based room-temperature operating spintronic devices.

High critical current density and high-tolerance superconductivity in high-entropy alloy thin films.

High-entropy alloy (HEA) superconductors-a new class of functional materials-can be utilized stably under extreme conditions, such as in space environments, owing to their high mechanical hardness and excellent irradiation tolerance. However, the feasibility of practical applications of HEA superconductors has not yet been demonstrated because the critical current density (Jc) for HEA superconductors has not yet been adequately characterized. Here, we report the fabrication of high-quality superconducting (SC) thin films of Ta-Nb-Hf-Zr-Ti HEAs via a pulsed laser deposition. The thin films exhibit a large Jc of >1 MA cm-2 at 4.2 K and are therefore favorable for SC devices as well as large-scale applications. In addition, they show extremely robust superconductivity to irradiation-induced disorder controlled by the dose of Kr-ion irradiation. The superconductivity of the HEA films is more than 1000 times more resistant to displacement damage than that of other promising superconductors with technological applications, such as MgB2, Nb3Sn, Fe-based superconductors, and high-Tc cuprate superconductors. These results demonstrate that HEA superconductors have considerable potential for use under extreme conditions, such as in aerospace applications, nuclear fusion reactors, and high-field SC magnets.

Author Correction: A peak in the critical current for quantum critical superconductors.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Giant proximity effect in single-crystalline MgB2 bilayers.

Although giant proximity effect (GPE) can shed important information on understanding superconducting pairing mechanisms and superconducting electronics, reports on the GPE are few because the fabrication of the junctions with GPE is technologically difficult. Here, we report a GPE in the single-crystalline MgB2 bilayers (S'/S), where the S' is the damaged MgB2 layer by cobalt (Co)-ion irradiation and the S is the undamaged MgB2 layer. Superconducting properties of the S' is remarkably degraded by the irradiation, whereas those of the S is uninfluenced by the irradiation. The degraded superconductivity in the S' is fully recovered by increasing the thickness of undamaged MgB2 layer S despite almost ten times larger thickness ~ 95 nm of S' than the superconducting coherence length ξab(0) ~ 8.5 nm of the S, indicating a presence of GPE in the S'/S MgB2 bilayers. A diffusion of electrons in the S' into the S can reduce a pair breaking scattering in the S', and the similar electronic structures of S' and S layers and a finite attractive electron-electron interaction in the S' are thought to be origins of unpredicted GPE between the same superconducting materials. Both upper critical field (µ0Hc2) and in-field critical current density (Jc) of S'/S bilayers show a significant enhancement, representing a strong correlation between S' and S. These discoveries provide the blue print to the design of the superconducting multilayers for fundamental researches on the mechanism of the GPE as well as their technological applications.

Thermal annealing and pressure effects on BaFe2-x Co x As2 single crystals.

We investigate the pressure and thermal annealing effects on BaFe2-x Co x As2 (Co-Ba122) single crystals with x = 0.1 and 0.17 via electrical transport measurements. The thermal annealing treatment not only enhances the superconducting transition temperature (T c) from 9.6 to 12.7 K for x = 0.1 and from 18.1 to 21.0 K for x = 0.17, but also increases the antiferromagnetic transition temperature (T N). Simultaneous enhancement of T c and T N by the thermal annealing treatment indicates that thermal annealing could substantially improve the quality of the Co-doped Ba122 samples. Interestingly, T c of the Co-Ba122 compounds shows a scaling behavior with a linear dependence on the resistivity value at 290 K, irrespective of tuning parameters such as chemical doping, pressure, and thermal annealing. These results not only provide an effective way to access the intrinsic properties of the BaFe2As2 system, but may also shed a light on designing new materials with higher superconducting transition temperature.

A peak in the critical current for quantum critical superconductors.

Generally, studies of the critical current Ic are necessary if superconductors are to be of practical use, because Ic sets the current limit below which there is a zero-resistance state. Here, we report a peak in the pressure dependence of the zero-field Ic, Ic(0), at a hidden quantum critical point (QCP), where a continuous antiferromagnetic transition temperature is suppressed by pressure toward 0 K in CeRhIn5 and 4.4% Sn-doped CeRhIn5. The Ic(0)s of these Ce-based compounds under pressure exhibit a universal temperature dependence, underlining that the peak in zero-field Ic(P) is determined predominantly by critical fluctuations associated with the hidden QCP. The dc conductivity σdc is a minimum at the QCP, showing anti-correlation with Ic(0). These discoveries demonstrate that a quantum critical point hidden inside the superconducting phase in strongly correlated materials can be exposed by the zero-field Ic, therefore providing a direct link between a QCP and unconventional superconductivity.

Origin of extremely large magnetoresistance in the candidate type-II Weyl semimetal MoTe2-x.

The recent observation of extremely large magnetoresistance (MR) in the transition-metal dichalcogenide MoTe2 has attracted considerable interest due to its potential technological applications as well as its relationship with novel electronic states predicted for a candidate type-II Weyl semimetal. In order to understand the origin of the MR, the electronic structure of MoTe2-x (x = 0.08) is systematically tuned by application of pressure and probed via its Hall and longitudinal conductivities. With increasing pressure, a monoclinic-to-orthorhombic (1 T' to Td) structural phase transition temperature (T*) gradually decreases from 210 K at 1 bar to 58 K at 1.1 GPa, and there is no anomaly associated with the phase transition at 1.4 GPa, indicating that a T = 0 K quantum phase transition occurs at a critical pressure (Pc) between 1.1 and 1.4 GPa. The large MR observed at 1 bar is suppressed with increasing pressure and is almost saturated at 100% for P > Pc. The dependence on magnetic field of the Hall and longitudinal conductivities of MoTe2-x shows that a pair of electron and hole bands are important in the low-pressure Td phase, while another pair of electron and hole bands are additionally required in the high-pressure 1 T' phase. The MR peaks at a characteristic hole-to-electron concentration ratio (nc) and is sharply suppressed when the ratio deviates from nc within the Td phase. These results establish the comprehensive temperature-pressure phase diagram of MoTe2-x and underscore that its MR originates from balanced electron-hole carrier concentrations.

Hard magnetic properties in nanoflake van der Waals Fe3GeTe2.

Two-dimensional van der Waals materials have demonstrated fascinating optical and electrical characteristics. However, reports on magnetic properties and spintronic applications of van der Waals materials are scarce by comparison. Here, we report anomalous Hall effect measurements on single crystalline metallic Fe3GeTe2 nanoflakes with different thicknesses. These nanoflakes exhibit a single hard magnetic phase with a near square-shaped magnetic loop, large coercivity (up to 550 mT at 2 K), a Curie temperature near 200 K and strong perpendicular magnetic anisotropy. Using criticality analysis, the coupling length between van der Waals atomic layers in Fe3GeTe2 is estimated to be ~5 van der Waals layers. Furthermore, the hard magnetic behaviour of Fe3GeTe2 can be well described by a proposed model. The magnetic properties of Fe3GeTe2 highlight its potential for integration into van der Waals magnetic heterostructures, paving the way for spintronic research and applications based on these devices.

Superconductivity at 7.4 K in few layer graphene by Li-intercalation.

Superconductivity in graphene has been highly sought after for its promise in various device applications and for general scientific interest. Ironically, the simple electronic structure of graphene, which is responsible for novel quantum phenomena, hinders the emergence of superconductivity. Theory predicts that doping the surface of the graphene effectively alters the electronic structure, thus promoting propensity towards Cooper pair instability (Profeta et al (2012) Nat. Phys. 8 131-4; Nandkishore et al (2012) Nat. Phys. 8 158-63) [1, 2]. Here we report the emergence of superconductivity at 7.4 K in Li-intercalated few-layer-graphene (FLG). The absence of superconductivity in 3D Li-doped graphite underlines that superconductivity in Li-FLG arises from the novel electronic properties of the 2D graphene layer. These results are expected to guide future research on graphene-based superconductivity, both in theory and experiments. In addition, easy control of the Li-doping process holds promise for various device applications.

Structural and Optical Properties of Single- and Few-Layer Magnetic Semiconductor CrPS4.

Atomically thin binary two-dimensional (2D) semiconductors exhibit diverse physical properties depending on their composition, structure, and thickness. By adding another element in these materials, which will lead to formation of ternary 2D materials, the property and structure would greatly change and significantly expanded applications could be explored. In this work, we report structural and optical properties of atomically thin chromium thiophosphate (CrPS4), a ternary antiferromagnetic semiconductor. Its structural details were revealed by X-ray and electron diffraction. Transmission electron microscopy showed that preferentially cleaved edges are parallel to diagonal Cr atom rows, which readily identified their crystallographic orientations. Strong in-plane optical anisotropy induced birefringence that also enabled efficient determination of crystallographic orientation using polarized microscopy. The lattice vibrations were probed by Raman spectroscopy and exhibited significant dependence on thickness of crystals exfoliated down to a single layer. Optical absorption determined by reflectance contrast was dominated by d-d-type transitions localized at Cr3+ ions, which was also responsible for the major photoluminescence peak at 1.31 eV. The spectral features in the absorption and emission spectra exhibited noticeable thickness dependence and hinted at a high photochemical activity for single-layer CrPS4. The current structural and optical investigation will provide a firm basis for future study and application of this kind of atomically thin magnetic semiconductors.

Enhanced critical current density in the pressure-induced magnetic state of the high-temperature superconductor FeSe.

We investigate the relation of the critical current density (Jc) and the remarkably increased superconducting transition temperature (Tc) for the FeSe single crystals under pressures up to 2.43 GPa, where the Tc is increased by ~8 K/GPa. The critical current density corresponding to the free flux flow is monotonically enhanced by pressure which is due to the increase in Tc, whereas the depinning critical current density at which the vortex starts to move is more influenced by the pressure-induced magnetic state compared to the increase of Tc. Unlike other high-Tc superconductors, FeSe is not magnetic, but superconducting at ambient pressure. Above a critical pressure where magnetic state is induced and coexists with superconductivity, the depinning Jc abruptly increases even though the increase of the zero-resistivity Tc is negligible, directly indicating that the flux pinning property compared to the Tc enhancement is a more crucial factor for an achievement of a large Jc. In addition, the sharp increase in Jc in the coexisting superconducting phase of FeSe demonstrates that vortices can be effectively trapped by the competing antiferromagnetic order, even though its antagonistic nature against superconductivity is well documented. These results provide new guidance toward technological applications of high-temperature superconductors.