Intrinsic supercurrent non-reciprocity coupled to the crystal structure of a van der Waals Josephson barrier.

Non-reciprocal electronic transport in a spatially homogeneous system arises from the simultaneous breaking of inversion and time-reversal symmetries. Superconducting and Josephson diodes, a key ingredient for future non-dissipative quantum devices, have recently been realized. Only a few examples of a vertical superconducting diode effect have been reported and its mechanism, especially whether intrinsic or extrinsic, remains elusive. Here we demonstrate a substantial supercurrent non-reciprocity in a van der Waals vertical Josephson junction formed with a Td-WTe2 barrier and NbSe2 electrodes that clearly reflects the intrinsic crystal structure of Td-WTe2. The Josephson diode efficiency increases with the Td-WTe2 thickness up to critical thickness, and all junctions, irrespective of the barrier thickness, reveal magneto-chiral characteristics with respect to a mirror plane of Td-WTe2. Our results, together with the twist-angle-tuned magneto-chirality of a Td-WTe2 double-barrier junction, show that two-dimensional materials promise vertical Josephson diodes with high efficiency and tunability.

Chiral antiferromagnetic Josephson junctions as spin-triplet supercurrent spin valves and d.c. SQUIDs.

Spin-triplet supercurrent spin valves are of practical importance for the realization of superconducting spintronic logic circuits. In ferromagnetic Josephson junctions, the magnetic-field-controlled non-collinearity between the spin-mixer and spin-rotator magnetizations switches the spin-polarized triplet supercurrents on and off. Here we report an antiferromagnetic equivalent of such spin-triplet supercurrent spin valves in chiral antiferromagnetic Josephson junctions as well as a direct-current superconducting quantum interference device. We employ the topological chiral antiferromagnet Mn3Ge, in which the Berry curvature of the band structure produces fictitious magnetic fields, and the non-collinear atomic-scale spin arrangement accommodates triplet Cooper pairing over long distances (>150 nm). We theoretically verify the observed supercurrent spin-valve behaviours under a small magnetic field of <2 mT for current-biased junctions and the direct-current superconducting quantum interference device functionality. Our calculations reproduce the observed hysteretic field interference of the Josephson critical current and link these to the magnetic-field-modulated antiferromagnetic texture that alters the Berry curvature. Our work employs band topology to control the pairing amplitude of spin-triplet Cooper pairs in a single chiral antiferromagnet.

Zero-field polarity-reversible Josephson supercurrent diodes enabled by a proximity-magnetized Pt barrier.

Simultaneous breaking of inversion and time-reversal symmetries in a conductor yields a non-reciprocal electronic transport1-3, known as the diode or rectification effect, that is, low (ideally zero) conductance in one direction and high (ideally infinite) conductance in the other. So far, most of the diode effects observed in non-centrosymmetric polar/superconducting conductors4-7 and Josephson junctions8-10 require external magnetic fields to break the time-reversal symmetry. Here we report zero-field polarity-switchable Josephson supercurrent diodes, in which a proximity-magnetized Pt layer by ferrimagnetic insulating Y3Fe5O12 serves as the Rashba(-type) Josephson barrier. The zero-field diode efficiency of our proximity-engineered device reaches up to ±35% at 2 K, with a clear square-root dependence on temperature. Measuring in-plane field-strength/angle dependences and comparing with Cu-inserted control junctions, we demonstrate that exchange spin-splitting11-13 and Rashba(-type) spin-orbit coupling13-15 at the Pt/Y3Fe5O12 interface are key for the zero-field giant rectification efficiency. Our achievement advances the development of field-free absolute Josephson diodes.

Control of Oxygen Vacancy Ordering in Brownmillerite Thin Films via Ionic Liquid Gating.

Oxygen defects and their atomic arrangements play a significant role in the physical properties of many transition metal oxides. The exemplary perovskite SrCoO3-δ (P-SCO) is metallic and ferromagnetic. However, its daughter phase, the brownmillerite SrCoO2.5 (BM-SCO), is insulating and an antiferromagnet. Moreover, BM-SCO exhibits oxygen vacancy channels (OVCs) that in thin films can be oriented either horizontally (H-SCO) or vertically (V-SCO) to the film's surface. To date, the orientation of these OVCs has been manipulated by control of the thin film deposition parameters or by using a substrate-induced strain. Here, we present a method to electrically control the OVC ordering in thin layers via ionic liquid gating (ILG). We show that H-SCO (antiferromagnetic insulator, AFI) can be converted to P-SCO (ferromagnetic metal, FM) and subsequently to V-SCO (AFI) by the insertion and subtraction of oxygen throughout thick films via ILG. Moreover, these processes are independent of substrate-induced strain which favors formation of H-SCO in the as-deposited film. The electric-field control of the OVC channels is a path toward the creation of oxitronic devices.

Role of Two-Dimensional Ising Superconductivity in the Nonequilibrium Quasiparticle Spin-to-Charge Conversion Efficiency.

Nonequilibrium studies of two-dimensional (2D) superconductors (SCs) with Ising spin-orbit coupling are prerequisite for their successful application to equilibrium spin-triplet Cooper pairs and, potentially, Majorana Fermions. By taking advantage of the recent discoveries of 2D SCs and their compatibility with any other materials, we fabricate here nonlocal magnon devices to examine how such 2D Ising superconductivity affects the conversion efficiency of magnon spin to quasiparticle charge in superconducting flakes of 2H-NbSe2 transferred onto ferrimagnetic insulating Y3Fe5O12. Comparison with a reference device based on a conventionally paired superconductor shows that the Y3Fe5O12-induced in-plane (IP) exchange spin-splitting in the NbSe2 flake is hindered by its inherent out-of-plane (OOP) spin-orbit field, which, in turn, limits the transition-state enhancement of the spin-to-charge conversion efficiency. Our out-of-equilibrium study highlights the significance of symmetry matching between underlying Cooper pairs and exchange-induced spin-splitting for the giant transition-state spin-to-charge conversion and may have implications toward proximity-engineered spin-polarized triplet pairing via tuning the relative strength of IP exchange and OOP spin-orbit fields in ferromagnetic insulator/2D Ising SC bilayers.

Long-range supercurrents through a chiral non-collinear antiferromagnet in lateral Josephson junctions.

The proximity-coupling of a chiral non-collinear antiferromagnet (AFM)1-5 with a singlet superconductor allows spin-unpolarized singlet Cooper pairs to be converted into spin-polarized triplet pairs6-8, thereby enabling non-dissipative, long-range spin correlations9-14. The mechanism of this conversion derives from fictitious magnetic fields that are created by a non-zero Berry phase15 in AFMs with non-collinear atomic-scale spin arrangements1-5. Here we report long-ranged lateral Josephson supercurrents through an epitaxial thin film of the triangular chiral AFM Mn3Ge (refs. 3-5). The Josephson supercurrents in this chiral AFM decay by approximately one to two orders of magnitude slower than would be expected for singlet pair correlations9-14 and their response to an external magnetic field reflects a clear spatial quantum interference. Given the long-range supercurrents present in both single- and mixed-phase Mn3Ge, but absent in a collinear AFM IrMn16, our results pave a way for the topological generation of spin-polarized triplet pairs6-8 via Berry phase engineering15 of the chiral AFMs.

Giant Transition-State Quasiparticle Spin-Hall Effect in an Exchange-Spin-Split Superconductor Detected by Nonlocal Magnon Spin Transport.

Although recent experiments and theories have shown a variety of exotic transport properties of nonequilibrium quasiparticles (QPs) in superconductor (SC)-based devices with either Zeeman or exchange spin-splitting, how a QP interplays with magnon spin currents remains elusive. Here, using nonlocal magnon spin-transport devices where a singlet SC (Nb) on top of a ferrimagnetic insulator (Y3Fe5O12) serves as a magnon spin detector, we demonstrate that the conversion efficiency of magnon spin to QP charge via inverse spin-Hall effect (iSHE) in such an exchange-spin-split SC can be greatly enhanced by up to 3 orders of magnitude compared with that in the normal state, particularly when its interface superconducting gap matches the magnon spin accumulation. Through systematic measurements by varying the current density and SC thickness, we identify that superconducting coherence peaks and exchange spin-splitting of the QP density-of-states, yielding a larger spin excitation while retaining a modest QP charge-imbalance relaxation, are responsible for the giant QP iSHE. The latter exchange-field-modified QP relaxation is experimentally proved by spatially resolved measurements with varying the separation of electrical contacts on the spin-split Nb.

Enhanced spin pumping into superconductors provides evidence for superconducting pure spin currents.

Unlike conventional spin-singlet Cooper pairs, spin-triplet pairs can carry spin1,2. Triplet supercurrents were discovered in Josephson junctions with metallic ferromagnet spacers, where spin transport can occur only within the ferromagnet and in conjunction with a charge current. Ferromagnetic resonance injects a pure spin current from a precessing ferromagnet into adjacent non-magnetic materials3,4. For spin-singlet pairing, the ferromagnetic resonance spin pumping efficiency decreases below the critical temperature (Tc) of a coupled superconductor5,6. Here we present ferromagnetic resonance experiments in which spin sink layers with strong spin-orbit coupling are added to the superconductor. Our results show that the induced spin currents, rather than being suppressed, are substantially larger in the superconducting state compared with the normal state; although further work is required to establish the details of the spin transport process, we show that this cannot be mediated by quasiparticles and is most likely a triplet pure spin supercurrent.

Voltage tuning of thermal spin current in ferromagnetic tunnel contacts to semiconductors.

Spin currents are paramount to manipulate the magnetization of ferromagnetic elements in spin-based memory, logic and microwave devices, and to induce spin polarization in non-magnetic materials. A unique approach to create spin currents employs thermal gradients and heat flow. Here we demonstrate that a thermal spin current can be tuned conveniently by a voltage. In magnetic tunnel contacts to semiconductors (silicon and germanium), it is shown that a modest voltage (~200 mV) changes the thermal spin current induced by Seebeck spin tunnelling by a factor of five, because it modifies the relevant tunnelling states and thereby the spin-dependent thermoelectric parameters. The magnitude and direction of the spin current is also modulated by combining electrical and thermal spin currents with equal or opposite sign. The results demonstrate that spin-dependent thermoelectric properties away from the Fermi energy are accessible, and open the way towards tailoring thermal spin currents and torques by voltage, rather than material design.

Thermal spin injection and accumulation in CoFe/MgO/n-type Ge contacts.

Understanding the interplay between spin and heat is a fundamental and intriguing subject. Here we report thermal spin injection and accumulation in CoFe/MgO/n-type Ge contacts with an asymmetry of tunnel spin polarization. Using local heating of electrodes by laser beam or electrical current, the thermally-induced spin accumulation is observed for both polarities of the temperature gradient across the tunnel contact. We observe that the magnitude of thermally injected spin signal scales linearly with the power of local heating of electrodes, and its sign is reversed as we invert the temperature gradient. A large Hanle magnetothermopower (HMTP) of about 7.0% and the Seebeck spin tunneling coefficient of larger than 0.74 meV K(-1) are obtained at room temperature.