Terahertz Spin-Conductance Spectroscopy: Probing Coherent and Incoherent Ultrafast Spin Tunneling.

Thin-film stacks F|H consisting of a ferromagnetic-metal layer F and a heavy-metal layer H are spintronic model systems. Here, we present a method to measure the ultrabroadband spin conductance across a layer X between F and H at terahertz frequencies, which are the natural frequencies of spin-transport dynamics. We apply our approach to MgO tunneling barriers with thickness d = 0-6 Å. In the time domain, the spin conductance Gs has two components. An instantaneous feature arises from processes like coherent spin tunneling. Remarkably, a longer-lived component is a hallmark of incoherent resonant spin tunneling mediated by MgO defect states, because its relaxation time grows monotonically with d to as much as 270 fs at d = 6.0 Å. Our results are in full agreement with an analytical model. They indicate that terahertz spin-conductance spectroscopy will yield new and relevant insights into ultrafast spin transport in a wide range of spintronic nanostructures.

Accessing Ultrafast Spin-Transport Dynamics in Copper Using Broadband Terahertz Spectroscopy.

We study the spatiotemporal dynamics of ultrafast electron spin transport across nanometer-thick copper layers using ultrabroadband terahertz emission spectroscopy. Our analysis of temporal delays, broadening, and attenuation of the spin-current pulse reveals ballisticlike propagation of the pulse peak, approaching the Fermi velocity, and diffusive features including a significant velocity dispersion. A comparison to the frequency-dependent Fick's law identifies the diffusion-dominated transport regime for distances >2 nm. These findings lay the groundwork for designing future broadband spintronic devices.

All-Oxide Metasurfaces Formed by Synchronized Local Ionic Gating.

Ionic gating of oxide thin films has emerged as a novel way of manipulating the properties of thin films. Most studies are carried out on single devices with a three-terminal configuration, but, by exploring the electrokinetics during the ionic gating, such a configuration with initially insulating films leads to a highly non-uniform gating response of individual devices within large arrays of the devices. It is shown that such an issue can be circumvented by the formation of a uniform charge potential by the use of a thin conducting underlayer. This synchronized local ionic gating allows for the simultaneous manipulation of the electrical, magnetic, and/or optical properties of large arrays of devices. Designer metasurfaces formed in this way from SrCoO2.5 thin films display an anomalous optical reflection of light that relies on the uniform and coherent response of all the devices. Beyond oxides, almost any material whose properties can be controlled by the addition or removal of ions via gating can form novel metasurfaces using this technique. These findings provide insights into the electrokinetics of ionic gating and a wide range of applications using synchronized local ionic gating.

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.

Imaging and phase-locking of non-linear spin waves.

Non-linear processes are a key feature in the emerging field of spin-wave based information processing and allow to convert uniform spin-wave excitations into propagating modes at different frequencies. Recently, the existence of non-linear magnons at half-integer multiples of the driving frequency has been predicted for Ni80Fe20 at low bias fields. However, it is an open question under which conditions such non-linear spin waves emerge coherently and how they may be used in device structures. Usually non-linear processes are explored in the small modulation regime and result in the well known three and four magnon scattering processes. Here we demonstrate and image a class of spin waves oscillating at half-integer harmonics that have only recently been proposed for the strong modulation regime. The direct imaging of these parametrically generated magnons in Ni80Fe20 elements allows to visualize their wave vectors. In addition, we demonstrate the presence of two degenerate phase states that may be selected by external phase-locking. These results open new possibilities for applications such as spin-wave sources, amplifiers and phase-encoded information processing with magnons.

Water-soluble ruthenium complex-pyrene dyads with extended triplet lifetimes for efficient energy transfer applications.

Long triplet lifetimes of excited photosensitizers are essential for efficient energy transfer reactions in water, given that the concentrations of dissolved oxygen and suitable acceptors in aqueous media are typically much lower than in organic solvents. Herein, we report the design, synthesis and photochemical characterization of two structurally related water-soluble ruthenium complex-based dyads decorated with a covalently attached pyrene chromophore. The triplet energy of the latter is slightly below that of the metal complex enabling a so-called triplet reservoir and excited-state lifetime extensions of up to two orders of magnitude. The diimine co-ligands, which can be modified easily, have a major impact on both the ultrafast intramolecular energy transfer (iEnT) kinetics upon excitation with visible light and the lifetime of the resulting long-lived pyrene triplet. The phenanthroline-containing dyad shows fast triplet pyrene formation (25 ps) and an exceptionally long triplet lifetime beyond 50 microseconds in neat water. The iEnT process via the Dexter mechanism is slower by a factor of two when bipyridine co-ligands are employed, which is rationalized by a poor orbital overlap. Both dyads are very efficient sensitizers for the formation of singlet oxygen in air-saturated water as well as for the bimolecular generation of anthracene triplets that are key intermediates in upconversion mechanisms. This is demonstrated by the 5-hydroxymethylfurfural oxidation, which yields completely different main products depending on the pH value of the aqueous solution, as an initial application-related experiment and by time-resolved spectroscopy. Our findings are important in the greater contexts of photocatalysis and energy conversion in the "green" solvent water.

Atomic Scale Control of Spin Current Transmission at Interfaces.

Ferromagnet/heavy metal bilayers represent a central building block for spintronic devices where the magnetization of the ferromagnet can be controlled by spin currents generated in the heavy metal. The efficiency of spin current generation is paramount. Equally important is the efficient transfer of this spin current across the ferromagnet/heavy metal interface. Here, we show theoretically and experimentally that for Ta as heavy metal the interface only partially transmits the spin current while this effect is absent when Pt is used as heavy metal. This is due to magnetic moment reduction at the interface caused by 3d-5d hybridization effects. We show that this effect can be avoided by atomically thin interlayers. On the basis of our theoretical model we conclude that this is a general effect and occurs for all 5d metals with less than half-filled 5d shell.

Frequency multiplication by collective nanoscale spin-wave dynamics.

Frequency multiplication is a process in modern electronics in which harmonics of the input frequency are generated in nonlinear electronic circuits. Devices based on the propagation and interaction of spin waves are a promising alternative to conventional electronics. The characteristic frequency of these excitations is in the gigahertz (GHz) range and devices are not readily interfaced with conventional electronics. Here, we locally probe the magnetic excitations in a soft magnetic material by optical methods and show that megahertz-range excitation frequencies cause switching effects on the micrometer scale, leading to phase-locked spin-wave emission in the GHz range. Indeed, the frequency multiplication process inside the magnetic medium covers six octaves and opens exciting perspectives for spintronic applications, such as all-magnetic mixers or on-chip GHz sources.

Electric-Field Control of Propagating Spin Waves by Ferroelectric Domain-Wall Motion in a Multiferroic Heterostructure.

Magnetoelectric coupling in multiferroic heterostructures offers a promising platform for electric-field control of magnonic devices based on low-power spin-wave transport. Here, electric-field manipulation of the amplitude and phase of propagating spin waves in a ferromagnetic Fe film on top of a ferroelectric BaTiO3 substrate is demonstrated experimentally. Electric-field effects in this composite material system are mediated by strain coupling between alternating ferroelectric stripe domains with in-plane and perpendicular polarization and fully correlated magnetic anisotropy domains with differing spin-wave transport properties. The propagation of spin waves across the strain-induced magnetic anisotropy domains of the Fe film is directly imaged and it is shown how reversible electric-field-driven motion of ferroelectric domain walls and pinned anisotropy boundaries turns the spin-wave signal on and off. Furthermore, linear electric-field tuning of the spin-wave phase by altering the width of strain-coupled stripe domains is demonstrated. The results provide a new route toward energy-efficient reconfigurable magnonics.

Nanoscale magnonic Fabry-Pérot resonator for low-loss spin-wave manipulation.

Active control of propagating spin waves on the nanoscale is essential for beyond-CMOS magnonic computing. Here, we experimentally demonstrate reconfigurable spin-wave transport in a hybrid YIG-based material structure that operates as a Fabry-Pérot nanoresonator. The magnonic resonator is formed by a local frequency downshift of the spin-wave dispersion relation in a continuous YIG film caused by dynamic dipolar coupling to a ferromagnetic metal nanostripe. Drastic downscaling of the spin-wave wavelength within the bilayer region enables programmable control of propagating spin waves on a length scale that is only a fraction of their wavelength. Depending on the stripe width, the device structure offers full nonreciprocity, tunable spin-wave filtering, and nearly zero transmission loss at allowed frequencies. Our results provide a practical route for the implementation of low-loss YIG-based magnonic devices with controllable transport properties.

Frequency-Independent Terahertz Anomalous Hall Effect in DyCo5 , Co32 Fe68 , and Gd27 Fe73 Thin Films from DC to 40 THz.

The anomalous Hall effect (AHE) is a fundamental spintronic charge-to-charge-current conversion phenomenon and closely related to spin-to-charge-current conversion by the spin Hall effect. Future high-speed spintronic devices will crucially rely on such conversion phenomena at terahertz (THz) frequencies. Here, it is revealed that the AHE remains operative from DC up to 40 THz with a flat frequency response in thin films of three technologically relevant magnetic materials: DyCo5 , Co32 Fe68 , and Gd27 Fe73 . The frequency-dependent conductivity-tensor elements σxx and σyx  are measured, and good agreement with DC measurements is found. The experimental findings are fully consistent with ab initio calculations of σyx for CoFe and highlight the role of the large Drude scattering rate (≈100 THz) of metal thin films, which smears out any sharp spectral features of the THz AHE. Finally, it is found that the intrinsic contribution to the THz AHE dominates over the extrinsic mechanisms for the Co32 Fe68 sample. The results imply that the AHE and related effects such as the spin Hall effect are highly promising ingredients of future THz spintronic devices reliably operating from DC to 40 THz and beyond.

Terahertz Spin-to-Charge Conversion by Interfacial Skew Scattering in Metallic Bilayers.

The efficient conversion of spin to charge transport and vice versa is of major relevance for the detection and generation of spin currents in spin-based electronics. Interfaces of heterostructures are known to have a marked impact on this process. Here, terahertz (THz) emission spectroscopy is used to study ultrafast spin-to-charge-current conversion (S2C) in about 50 prototypical F|N bilayers consisting of a ferromagnetic layer F (e.g., Ni81 Fe19 , Co, or Fe) and a nonmagnetic layer N with strong (Pt) or weak (Cu and Al) spin-orbit coupling. Varying the structure of the F/N interface leads to a drastic change in the amplitude and even inversion of the polarity of the THz charge current. Remarkably, when N is a material with small spin Hall angle, a dominant interface contribution to the ultrafast charge current is found. Its magnitude amounts to as much as about 20% of that found in the F|Pt reference sample. Symmetry arguments and first-principles calculations strongly suggest that the interfacial S2C arises from skew scattering of spin-polarized electrons at interface imperfections. The results highlight the potential of skew scattering for interfacial S2C and propose a promising route to enhanced S2C by tailored interfaces at all frequencies from DC to terahertz.

Femtosecond formation dynamics of the spin Seebeck effect revealed by terahertz spectroscopy.

Understanding the transfer of spin angular momentum is essential in modern magnetism research. A model case is the generation of magnons in magnetic insulators by heating an adjacent metal film. Here, we reveal the initial steps of this spin Seebeck effect with <27 fs time resolution using terahertz spectroscopy on bilayers of ferrimagnetic yttrium iron garnet and platinum. Upon exciting the metal with an infrared laser pulse, a spin Seebeck current js arises on the same ~100 fs time scale on which the metal electrons thermalize. This observation highlights that efficient spin transfer critically relies on carrier multiplication and is driven by conduction electrons scattering off the metal-insulator interface. Analytical modeling shows that the electrons' dynamics are almost instantaneously imprinted onto js because their spins have a correlation time of only ~4 fs and deflect the ferrimagnetic moments without inertia. Applications in material characterization, interface probing, spin-noise spectroscopy and terahertz spin pumping emerge.

Observation of orbital two-channel Kondo effect in a ferromagnetic L10-MnGa film.

The experimental existence and stability of the fixed point of the two-channel Kondo (2CK) effect displaying exotic non-Fermi liquid physics have been buried in persistent confusion despite the intensive theoretical and experimental efforts in past three decades. Here we report an experimental realization of the two-level system resonant scattering-induced orbital 2CK effect in a ferromagnetic L10-MnGa film, which is signified by a magnetic field-independent resistivity upturn that has a logarithmic and a square-root temperature dependence beyond and below the Kondo temperature of ~14.5 K, respectively. Our results not only evidence the robust existence of orbital 2CK effect even in the presence of strong magnetic fields and long-range ferromagnetic ordering, but also extend the scope of 2CK host materials from nonmagnetic nanoscale point contacts to diffusive conductors of disordered alloys.

Three-dimensional Character of the Magnetization Dynamics in Magnetic Vortex Structures: Hybridization of Flexure Gyromodes with Spin Waves.

Three-dimensional linear spin-wave eigenmodes of a vortex-state Permalloy disk are studied by micromagnetic simulations based on the Landau-Lifshitz-Gilbert equation. The simulations confirm that the increase of the disk thickness leads to the appearance of additional exchange-dominated so-called gyrotropic flexure modes having nodes along the disk thickness, and eigenfrequencies that decrease when the thickness is increased. We observe the formation of a gap in the mode spectrum caused by the hybridization of the first flexure mode with one of the azimuthal spin-wave modes of the disk. A qualitative change of the transverse profile of this azimuthal mode is found, demonstrating that in a thick vortex-state disk the influence of the "transverse" and the "azimuthal" coordinates cannot be separated. The three-dimensional character of the eigenmodes is essential to explain the recently observed asymmetries in an experimentally obtained phase diagram of vortex-core reversal in relatively thick Permalloy disks.

Nonlinear spin-wave excitations at low magnetic bias fields.

Nonlinear magnetization dynamics is essential for the operation of numerous spintronic devices ranging from magnetic memory to spin torque microwave generators. Examples are microwave-assisted switching of magnetic structures and the generation of spin currents at low bias fields by high-amplitude ferromagnetic resonance. Here we use X-ray magnetic circular dichroism to determine the number density of excited magnons in magnetically soft Ni80Fe20 thin films. Our data show that the common model of nonlinear ferromagnetic resonance is not adequate for the description of the nonlinear behaviour in the low magnetic field limit. Here we derive a model of parametric spin-wave excitation, which correctly predicts nonlinear threshold amplitudes and decay rates at high and at low magnetic bias fields. In fact, a series of critical spin-wave modes with fast oscillations of the amplitude and phase is found, generalizing the theory of parametric spin-wave excitation to large modulation amplitudes.

Spin Hall voltages from a.c. and d.c. spin currents.

In spin electronics, the spin degree of freedom is used to transmit and store information. To this end the ability to create pure spin currents--that is, without net charge transfer--is essential. When the magnetization vector in a ferromagnet-normal metal junction is excited, the spin pumping effect leads to the injection of pure spin currents into the normal metal. The polarization of this spin current is time-dependent and contains a very small d.c. component. Here we show that the large a.c. component of the spin currents can be detected efficiently using the inverse spin Hall effect. The observed a.c.-inverse spin Hall voltages are one order of magnitude larger than the conventional d.c.-inverse spin Hall voltages measured on the same device. Our results demonstrate that ferromagnet-normal metal junctions are efficient sources of pure spin currents in the gigahertz frequency range.

Vortex core reversal due to spin wave interference.

In this Letter we address spin wave dynamics involved in fast and selective vortex core polarity reversal by rotating magnetic field bursts. In a first example we explain the origin of the delayed switching for excitations with short bursts of only one period duration as an interference effect between spin wave modes. Second, when the vortex core is initially no longer at rest but in gyrotropic motion, the magnetization dynamics become more complicated and the interaction of spin waves with the vortex core leads to a variety of nonlinear effects. Our analysis allows us to explain the experimentally observed switching diagram for simultaneous excitation of spin waves and gyrotropic mode.

Magnetic vortex core reversal by excitation of spin waves.

Micron-sized magnetic platelets in the flux-closed vortex state are characterized by an in-plane curling magnetization and a nanometer-sized perpendicularly magnetized vortex core. Having the simplest non-trivial configuration, these objects are of general interest to micromagnetics and may offer new routes for spintronics applications. Essential progress in the understanding of nonlinear vortex dynamics was achieved when low-field core toggling by excitation of the gyrotropic eigenmode at sub-GHz frequencies was established. At frequencies more than an order of magnitude higher vortex state structures possess spin wave eigenmodes arising from the magneto-static interaction. Here we demonstrate experimentally that the unidirectional vortex core reversal process also occurs when such azimuthal modes are excited. These results are confirmed by micromagnetic simulations, which clearly show the selection rules for this novel reversal mechanism. Our analysis reveals that for spin-wave excitation the concept of a critical velocity as the switching condition has to be modified.