Exotic Magnetic Anisotropy Near Digitized Dimensional Mott Boundary.

The magnetic anisotropy of low-dimensional Mott systems exhibits unexpected magnetotransport behavior useful for spin-based quantum electronics. Yet, the anisotropy of natural materials is inherently determined by the crystal structure, highly limiting its engineering. The magnetic anisotropy modulation near a digitized dimensional Mott boundary in artificial superlattices composed of a correlated magnetic monolayer SrRuO3 and nonmagnetic SrTiO3 , is demonstrated. The magnetic anisotropy is initially engineered by modulating the interlayer coupling strength between the magnetic monolayers. Interestingly, when the interlayer coupling strength is maximized, a nearly degenerate state is realized, in which the anisotropic magnetotransport is strongly influenced by both the thermal and magnetic energy scales. The results offer a new digitized control for magnetic anisotropy in low-dimensional Mott systems, inspiring promising integration of Mottronics and spintronics.

Hybridization-Controlled Pseudogap State in the Quantum Critical Superconductor CeCoIn_{5}.

The origin of the partial suppression of the electronic density states in the enigmatic pseudogap behavior, which is at the core of understanding high-T_{c} superconductivity, has been hotly contested as either a hallmark of preformed Cooper pairs or an incipient order of competing interactions nearby. Here, we report the quasiparticle scattering spectroscopy of the quantum critical superconductor CeCoIn_{5}, where a pseudogap with energy Δ_{g} was manifested as a dip in the differential conductance (dI/dV) below the characteristic temperature of T_{g}. When subjected to external pressure, T_{g} and Δ_{g} gradually increase, following the trend of increase in quantum entangled hybridization between the Ce 4f moment and conduction electrons. On the other hand, the superconducting (SC) energy gap and its phase transition temperature shows a maximum, revealing a dome shape under pressure. The disparate dependence on pressure between the two quantum states shows that the pseudogap is less likely involved in the formation of SC Cooper pairs, but rather is controlled by Kondo hybridization, indicating that a novel type of pseudogap is realized in CeCoIn_{5}.

High mobility field-effect transistors based on MoS2crystals grown by the flux method.

Two-dimensional (2D) molybdenum disulphide (MoS2) transition metal dichalcogenides (TMDs) have great potential for use in optical and electronic device applications; however, the performance of MoS2is limited by its crystal quality, which serves as a measure of the defects and grain boundaries in the grown material. Therefore, the high-quality growth of MoS2crystals continues to be a critical issue. In this context, we propose the formation of high-quality MoS2crystals via the flux method. The resulting electrical properties demonstrate the significant impact of crystal morphology on the performance of MoS2field-effect transistors. MoS2made with a relatively higher concentration of sulphur (a molar ratio of 2.2) and at a cooling rate of 2.5 °C h-1yielded good quality and optimally sized crystals. The room-temperature and low-temperature (77 K) electrical transport properties of MoS2field-effect transistors (FETs) were studied in detail, with and without the use of a hexagonal boron nitride (h-BN) dielectric to address the mobility degradation issue due to scattering at the SiO2/2D material interface. A maximum field-effect mobility of 113 cm2V-1s-1was achieved at 77 K for the MoS2/h-BN FET following high-quality crystal formation by the flux method. Our results confirm the achievement of large-scale high-quality crystal growth with reduced defect density using the flux method and are key to achieving higher mobility in MoS2FET devices in parallel with commercially accessible MoS2crystals.

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.

Pressure-tuned quantum criticality in the antiferromagnetic Kondo semimetal CeNi2-δAs2.

The easily tuned balance among competing interactions in Kondo-lattice metals allows access to a zero-temperature, continuous transition between magnetically ordered and disordered phases, a quantum-critical point (QCP). Indeed, these highly correlated electron materials are prototypes for discovering and exploring quantum-critical states. Theoretical models proposed to account for the strange thermodynamic and electrical transport properties that emerge around the QCP of a Kondo lattice assume the presence of an indefinitely large number of itinerant charge carriers. Here, we report a systematic transport and thermodynamic investigation of the Kondo-lattice system CeNi2-δAs2 (δ ≈ 0.28) as its antiferromagnetic order is tuned by pressure and magnetic field to zero-temperature boundaries. These experiments show that the very small but finite carrier density of ~0.032 E-/formular unit in CeNi2-δAs2 leads to unexpected transport signatures of quantum criticality and the delayed development of a fully coherent Kondo-lattice state with decreasing temperature. The small carrier density and associated semimetallicity of this Kondo-lattice material favor an unconventional, local-moment type of quantum criticality and raises the specter of the Nozières exhaustion idea that an insufficient number of conduction-electron spins to separately screen local moments requires collective Kondo screening.

Fermi surface reconstruction and multiple quantum phase transitions in the antiferromagnet CeRhIn5.

Conventional, thermally driven continuous phase transitions are described by universal critical behavior that is independent of the specific microscopic details of a material. However, many current studies focus on materials that exhibit quantum-driven continuous phase transitions (quantum critical points, or QCPs) at absolute zero temperature. The classification of such QCPs and the question of whether they show universal behavior remain open issues. Here we report measurements of heat capacity and de Haas-van Alphen (dHvA) oscillations at low temperatures across a field-induced antiferromagnetic QCP (Bc0 ≈ 50 T) in the heavy-fermion metal CeRhIn5. A sharp, magnetic-field-induced change in Fermi surface is detected both in the dHvA effect and Hall resistivity at B0* ≈ 30 T, well inside the antiferromagnetic phase. Comparisons with band-structure calculations and properties of isostructural CeCoIn5 suggest that the Fermi-surface change at B0* is associated with a localized-to-itinerant transition of the Ce-4f electrons in CeRhIn5. Taken in conjunction with pressure experiments, our results demonstrate that at least two distinct classes of QCP are observable in CeRhIn5, a significant step toward the derivation of a universal phase diagram for QCPs.

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.

Reemergent superconductivity and avoided quantum criticality in Cd-doped CeIrIn(5) under pressure.

We investigated the electrical resistivity and heat capacity of 1% Cd-doped CeIrIn_{5} under hydrostatic pressure up to 2.7 GPa, near where long-range antiferromagnetic order is suppressed and bulk superconductivity suddenly reemerges. The pressure-induced T_{c} is close to that of pristine CeIrIn_{5} at 2.7 GPa, and no signatures of a quantum critical point under pressure support a local origin of the antiferromagnetic moments in Cd-CeIrIn_{5} at ambient pressure. Similarities between superconductors CeIrIn_{5} and CeCoIn_{5} in response to Cd substitutions suggest a common magnetic mechanism.

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.

Evidence for charge delocalization crossover in the quantum critical superconductor CeRhIn5.

The nature of charge degrees-of-freedom distinguishes scenarios for interpreting the character of a second order magnetic transition at zero temperature, that is, a magnetic quantum critical point (QCP). Heavy-fermion systems are prototypes of this paradigm, and in those, the relevant question is where, relative to a magnetic QCP, does the Kondo effect delocalize their f-electron degrees-of-freedom. Herein, we use pressure-dependent Hall measurements to identify a finite-temperature scale Eloc that signals a crossover from f-localized to f-delocalized character. As a function of pressure, Eloc(P) extrapolates smoothly to zero temperature at the antiferromagnetic QCP of CeRhIn5 where its Fermi surface reconstructs, hallmarks of Kondo-breakdown criticality that generates critical magnetic and charge fluctuations. In 4.4% Sn-doped CeRhIn5, however, Eloc(P) extrapolates into its magnetically ordered phase and is decoupled from the pressure-induced magnetic QCP, which implies a spin-density-wave (SDW) type of criticality that produces only critical fluctuations of the SDW order parameter. Our results demonstrate the importance of experimentally determining Eloc to characterize quantum criticality and the associated consequences for understanding the pairing mechanism of superconductivity that reaches a maximum Tc in both materials at their respective magnetic QCP.

Textured superconducting phase in the heavy fermion CeRhIn5.

When antiferromagnetism and unconventional superconductivity coexist in CeRhIn(5) there is a significant temperature difference between resistively and thermodynamically determined transitions into the superconducting state. In this state, anisotropic transport near the superconducting transition reveals the emergence of textured superconducting planes that appear without a change in translational symmetry of the lattice. CeRhIn(5) is not unique in exhibiting these behaviors, indicating that textured superconductivity may be a general consequence of coexisting orders in correlated electron materials.

Hidden magnetism and quantum criticality in the heavy fermion superconductor CeRhIn5.

With only a few exceptions that are well understood, conventional superconductivity does not coexist with long-range magnetic order (for example, ref. 1). Unconventional superconductivity, on the other hand, develops near a phase boundary separating magnetically ordered and magnetically disordered phases. A maximum in the superconducting transition temperature T(c) develops where this boundary extrapolates to zero Kelvin, suggesting that fluctuations associated with this magnetic quantum-critical point are essential for unconventional superconductivity. Invariably, though, unconventional superconductivity masks the magnetic phase boundary when T < T(c), preventing proof of a magnetic quantum-critical point. Here we report specific-heat measurements of the pressure-tuned unconventional superconductor CeRhIn5 in which we find a line of quantum-phase transitions induced inside the superconducting state by an applied magnetic field. This quantum-critical line separates a phase of coexisting antiferromagnetism and superconductivity from a purely unconventional superconducting phase, and terminates at a quantum tetracritical point where the magnetic field completely suppresses superconductivity. The T --> 0 K magnetic field-pressure phase diagram of CeRhIn5 is well described with a theoretical model developed to explain field-induced magnetism in the high-T(c) copper oxides, but in which a clear delineation of quantum-phase boundaries has not been possible. These experiments establish a common relationship among hidden magnetism, quantum criticality and unconventional superconductivity in copper oxides and heavy-electron systems such as CeRhIn5.

Study on superconducting properties of CeIrIn5thin films grown via pulsed laser deposition.

We report the growth of CeIrIn5thin films with different crystal orientations on a MgF2(001) substrate using pulsed laser deposition technique. X-ray diffraction analysis showed that the thin films were either mainlya-axis-oriented (TF1) or a combination ofa- andc-axis-oriented (TF2). The characteristic features of heavy-fermion superconductors, i.e. Kondo coherence and superconductivity, were clearly observed, where the superconducting transition temperature (Tc) and Kondo coherence temperature (Tcoh) are 0.58 K and 41 K for TF1 and 0.52 K and 37 K for TF2, respectively. The temperature dependencies of the upper critical field (Hc2) of both thin films and the CeIrIn5single crystal revealed a scaling behavior, indicating that the nature of unconventional superconductivity has not been changed in the thin film. The successful synthesis of CeIrIn5thin films is expected to open a new avenue for novel quantum phases that may have been difficult to explore in the bulk crystalline samples.

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.

Transport and calorimetry study of 20% La-doped CeIn3.

CeIn3, a prototypical antiferromagnet, is an ideal candidate for investigating the relationship between magnetism and superconductivity, as superconductivity is induced as the magnetic transition temperature (T N) is lowered to 0 K by applying pressure. When La is substituted for Ce, T N of CeIn3 decreases to 0 K owing to the Ce dilution effects, thereby providing an alternative route to the zero-temperature quantum phase transition. In this study, we report a combinatorial approach to gain access to the critical point by applying external pressure to 20% La-doped CeIn3. Electrical resistivity measurements of La0.2Ce0.8In3 show that the T N of 8.4 K at 1 bar is gradually suppressed under pressure and can be extrapolated to 0 K at approximately 2.47 GPa, thereby showing a similar pressure dependence of T N as shown by undoped CeIn3. The kink-like feature in resistivity at T N of CeIn3 changed to an obvious jump in the doped compound for pressures higher than 1.64 GPa, indicating depletion in the carrier density due to a gap opening. AC calorimetry measurements under applied pressure show that the size of the specific heat jump at T N decreases with increasing pressure, but any signatures associated with the gap opening are not obvious, suggesting that the pressure-induced kink-to-jump change at T N in the resistivity is not a phase transition, but rather a gradual crossover. The low-temperature specific heat divided by temperature, C/T, does not strongly diverge with decreasing temperature, but is almost saturated near the projected quantum critical point, which can be attributed to a weak enhancement in the effective mass up to 2.6 GPa.

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.