Compensated Ferrimagnets with Colossal Spin Splitting in Organic Compounds.

The study of the magnetic order has recently been invigorated by the discovery of exotic collinear antiferromagnets with time-reversal symmetry breaking. Examples include altermagnets and compensated ferrimagnets, which show spin splittings of the electronic band structures even at zero net magnetization, leading to several unique transport phenomena, notably spin-current generation. Altermagnets demonstrate anisotropic spin splitting, such as d-wave, in momentum space, whereas compensated ferrimagnets exhibit isotropic spin splitting. However, methods to realize compensated ferrimagnets are limited. Here, we demonstrate a method to realize a fully compensated ferrimagnet with isotropic spin splitting utilizing the dimer structures inherent in organic compounds. Moreover, based on ab initio calculations, we find that this compensated ferrimagnet can be realized in the recently discovered organic compound (EDO-TTF-I)_{2}ClO_{4}. Our findings provide an unprecedented strategy for using the dimer degrees of freedom in organic compounds to realize fully compensated ferrimagnets with colossal spin splitting.

Comprehensive Ab Initio Investigation of the Phase Diagram of Quasi-One-Dimensional Molecular Solids.

An ab initio investigation of the family of molecular compounds TM_{2}X is conducted, where TM is either TMTSF or TMTTF and X takes centrosymmetric monovalent anions. By deriving the extended Hubbard-type Hamiltonians from first-principles band calculations and evaluating not only the intermolecular transfer integrals but also the Coulomb parameters, we discuss their material dependence in the unified phase diagram. Furthermore, we apply the many-variable variational Monte Carlo method to accurately determine the symmetry-breaking phase transitions, and show the development of the charge and spin orderings. We show that the material-dependent parameter can be taken as the correlation effect, represented by the value of the screened on-site Coulomb interaction U relative to the intrachain transfer integrals, for the comprehensive understanding of the spin and charge ordering in this system.

Room-temperature magnetoresistance in Ni78Fe22/C8-BTBT/Ni78Fe22 nanojunctions fabricated from magnetic thin-film edges using a novel technique.

Molecular spintronic devices are gaining popularity because the organic semiconductors with long spin relaxation times are expected to have long spin diffusion lengths. A typical molecular spintronic device consists of organic molecules sandwiched between two magnetic layers, which exhibits magnetoresistance (MR) effect. Nanosized devices are also expected to have a high spin polarization, leading to a large MR effect owing to effective orbital hybridization. However, most studies on nanosized molecular spintronic devices have investigated the MR effect at low temperatures because of the difficulty in observing the MR effect at room temperature. Here we focus on high-mobility molecules expected to show long spin diffusion lengths, which lead to the observation of the MR effect in nanoscale junctions at room temperature. In this study, we fabricate magnetic nanojunctions consisting of high-mobility molecules, 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT), sandwiched between two Ni78Fe22 thin films with crossed edges. Transmission electron microscopy (TEM) images reveal that C8-BTBT molecular layers with smooth and clear interfaces can be deposited on the Ni78Fe22 thin-film edges. Consequently, we observe a clear positive MR effect, that is, R P < R AP, where R P and R AP are the resistances in the parallel (P) and antiparallel (AP) configurations, respectively, of two magnetic electrodes in the Ni78Fe22/C8-BTBT/Ni78Fe22 nanojunctions at room temperature. The obtained results indicate that the spin signal through the C8-BTBT molecules can be successfully observed. The study presented herein provides a novel nanofabrication technique and opens up new opportunities for research in high-mobility molecular nano-spintronics.

Semi-quantized Spin Pumping and Spin-Orbit Torques in Topological Dirac Semimetals.

We study the time-development processes of spin and charge transport phenomena in a topological Dirac semimetal attached to a ferromagnetic insulator with a precessing magnetization. Compared to conventional normal metals, topological Dirac semimetals manifest a large inverse spin Hall effect when a spin current is pumped from the attached ferromagnetic insulator. It is shown that the induced charge current is semi-quantized, i.e., it depends only on the distance between the two Dirac points in momentum space and hardly depends on the disorder strength when the system remains in the topological Dirac semimetal phase. As an inverse effect, we show that the electric field applied to the topological Dirac semimetal exerts a spin torque on the local magnetization in the ferromagnetic insulator via the exchange interaction and the semi-quantized spin Hall effect. Our study demonstrates that the topological Dirac semimetal offers a less-dissipative platform for spin-charge conversion and spin switching.

Robustness of Voltage-induced Magnetocapacitance.

One of the most important achievements in the field of spintronics is the development of magnetic tunnel junctions (MTJs). MTJs exhibit a large tunneling magnetoresistance (TMR). However, TMR is strongly dependent on biasing voltage, generally, decreasing with applying bias. The rapid decay of TMR was a major deficiency of MTJs. Here we report a new phenomenon at room temperature, in which the tunneling magnetocapacitance (TMC) increases with biasing voltage in an MTJ system based on Co40Fe40B20/MgO/Co40Fe40B20. We have observed a maximum TMC value of 102% under appropriate biasing, which is the largest voltage-induced TMC effect ever reported for MTJs. We have found excellent agreement between theory and experiment for the bipolar biasing regions using Debye-Fröhlich model combined with quartic barrier approximation and spin-dependent drift-diffusion model. Based on our calculation, we predict that the voltage-induced TMC ratio could reach 1100% in MTJs with a corresponding TMR value of 604%. Our work has provided a new understanding on the voltage-induced AC spin-dependent transport in MTJs. The results reported here may open a novel pathway for spintronics applications, e.g., non-volatile memories and spin logic circuits.

"Visible" 5d Orbital States in a Pleochroic Oxychloride.

Transition metal compounds sometimes exhibit attractive colors. Here, we report a new oxychloride, Ca3ReO5Cl2, that shows unusually distinct pleochroism; that is, the material exhibits different colors depending on the viewing direction. This pleochroism is a consequence of the coincidental complex crystal field splitting of the 5d orbitals of the Re6+ ion in a square-pyramidal coordination of low symmetry in the energy range of the visible spectrum. Since the relevant d-d transitions show characteristic polarization dependence according to the optical selection rule, the orbital states are "visible" in Ca3ReO5Cl2.

Inverse Tunnel Magnetocapacitance in Fe/Al-oxide/Fe3O4.

Magnetocapacitance (MC) effect, observed in a wide range of materials and devices, such as multiferroic materials and spintronic devices, has received considerable attention due to its interesting physical properties and practical applications. A normal MC effect exhibits a higher capacitance when spins in the electrodes are parallel to each other and a lower capacitance when spins are antiparallel. Here we report an inverse tunnel magnetocapacitance (TMC) effect for the first time in Fe/AlOx/Fe3O4 magnetic tunnel junctions (MTJs). The inverse TMC reaches up to 11.4% at room temperature and the robustness of spin polarization is revealed in the bias dependence of the inverse TMC. Excellent agreement between theory and experiment is achieved for the entire applied frequency range and the wide bipolar bias regions using Debye-Fröhlich model (combined with the Zhang formula and parabolic barrier approximation) and spin-dependent drift-diffusion model. Furthermore, our theoretical calculations predict that the inverse TMC effect could potentially reach 150% in MTJs with a positive and negative spin polarization of 65% and -42%, respectively. These theoretical and experimental findings provide a new insight into both static and dynamic spin-dependent transports. They will open up broader opportunities for device applications, such as magnetic logic circuits and multi-valued memory devices.

Self-optimized superconductivity attainable by interlayer phase separation at cuprate interfaces.

Stabilizing superconductivity at high temperatures and elucidating its mechanism have long been major challenges of materials research in condensed matter physics. Meanwhile, recent progress in nanostructuring offers unprecedented possibilities for designing novel functionalities. Above all, thin films of cuprate and iron-based high-temperature superconductors exhibit remarkably better superconducting characteristics (for example, higher critical temperatures) than in the bulk, but the underlying mechanism is still not understood. Solving microscopic models suitable for cuprates, we demonstrate that, at an interface between a Mott insulator and an overdoped nonsuperconducting metal, the superconducting amplitude is always pinned at the optimum achieved in the bulk, independently of the carrier concentration in the metal. This is in contrast to the dome-like dependence in bulk superconductors but consistent with the astonishing independence of the critical temperature from the carrier density x observed at the interfaces of La2CuO4 and La2-x Sr x CuO4. Furthermore, we identify a self-organization mechanism as responsible for the pinning at the optimum amplitude: An emergent electronic structure induced by interlayer phase separation eludes bulk phase separation and inhomogeneities that would kill superconductivity in the bulk. Thus, interfaces provide an ideal tool to enhance and stabilize superconductivity. This interfacial example opens up further ways of shaping superconductivity by suppressing competing instabilities, with direct perspectives for designing devices.

Superconductivity and its mechanism in an ab initio model for electron-doped LaFeAsO.

Two families of high-temperature superconductors whose critical temperatures are higher than 50 K are known. One are the copper oxides and the other are the iron-based superconductors. Comparisons of mechanisms between these two in terms of common ground as well as distinctions will greatly help in searching for higher T(c) superconductors. However, studies on mechanisms for the iron family based on first principles calculations are few. Here we first show that superconductivity emerges in the state-of-the-art numerical calculations for an ab initio multi-orbital model of an electron-doped iron-based superconductor LaFeAsO, in accordance with experimental observations. Then the mechanism of the superconductivity is identified as enhanced uniform density fluctuations by one-to-one correspondence with the instability towards inhomogeneity driven by first-order antiferromagnetic and nematic transitions. Despite many differences, certain common features with the copper oxides are also discovered in terms of the underlying orbital-selective Mottness found in the iron family.

Charge order in a two-dimensional Kondo lattice model.

The possibility of charge order is theoretically examined for the Kondo lattice model in two dimensions, which does not include bare repulsive interactions. Using two complementary numerical methods, we find that charge order appears at quarter filling in an intermediate Kondo coupling region. The charge ordered ground state is an insulator exhibiting an antiferromagnetic order at charge-poor sites, while the paramagnetic charge-ordered state at finite temperatures is metallic with pseudogap behavior. We confirm that the stability of charge order is closely related with the local Kondo-singlet formation at charge-rich sites. Our results settle the controversy on charge order in the Kondo lattice model in realistic spatial dimensions.

Ab initio evidence for strong correlation associated with Mott proximity in iron-based superconductors.

We predict that iron-based superconductors discovered near d(6) configuration (5 Fe 3d orbitals filled by 6 electrons) is located on the foot of an unexpectedly large dome of correlated electron matter centered at the Mott insulator at d(5) (namely, half filling). This is based on the many-variable variational Monte Carlo results for ab initio low-energy models derived by the downfolding. The d(5) Mott proximity extends to subsequent emergence of incoherent metals, orbital differentiations due to the Mott physics, and Hund's rule coupling, followed by antiferromagnetic quantum criticality, in quantitative accordance with available experiments.

Unconventional quantum criticality emerging as a new common language of transition-metal compounds, heavy-fermion systems, and organic conductors.

We analyze and overview some of the different types of unconventional quantum criticalities by focusing on two origins. One origin of the unconventionality is the proximity to first-order transitions. The border between the first-order and continuous transitions is described by a quantum tricritical point (QTCP) for symmetry breaking transitions. One of the characteristic features of the quantum tricriticality is the concomitant divergence of an order parameter and uniform fluctuations, in contrast to the conventional quantum critical point (QCP). The interplay of these two fluctuations generates unconventionality. Several puzzling non-Fermi-liquid properties in experiments are taken to be accounted for by the resultant universality, as in the cases of Y bRh(2)Si(2), CeRu(2)Si(2) and ß-Y bAlB(4). Another more dramatic unconventionality appears again at the border of the first-order and continuous transitions, but in this case for topological transitions such as metal-insulator and Lifshitz transitions. This border, the marginal quantum critical point (MQCP), belongs to an unprecedented universality class with diverging uniform fluctuations at zero temperature. The Ising universality at the critical end point of the first-order transition at nonzero temperatures transforms to the marginal quantum criticality when the critical temperature is suppressed to zero. The MQCP has a unique feature with a combined character of symmetry breaking and topological transitions. In the metal-insulator transitions, the theoretical results are supported by experimental indications for V(2 - x)Cr(x)O(3) and an organic conductor κ-(ET)(2)Cu[N(CN)(2)]Cl. Identifying topological transitions also reveals how non-Fermi liquid appears as a phase in metals. The theory also accounts for the criticality of a metamagnetic transition in ZrZn(2), by interpreting it as an interplay of Lifshitz transition and correlation effects. We discuss the common underlying physics in these examples.