Microscopic origins of charge currents and electromagnetic (EM) radiation generated by them in spintronic THz emitters -- such as, femtosecond laser pulse-driven single magnetic layer or its heterostructures with a nonmagnetic layer hosting strong spin-orbit coupling (SOC) -- remain poorly understood despite nearly three decades since the discovery of ultrafast demagnetization. We introduce a first-principles method to compute these quantities, where the dynamics of charge and current densities is obtained from real-time time-dependent density functional theory (TDDFT), which are then fed into the Jefimenko equations for properly retarded electric and magnetic field solutions of the Maxwell equations. By Fourier transforming different time-dependent terms in the Jefimenko equations, we unravel that in 0.1--30 THz range the electric field of far-field EM radiation by Ni layer, chosen as an example, is {\em dominated by charge current pumped by demagnetization}, while often invoked magnetic dipole radiation from time-dependent magnetization of a single magnetic layer is a negligible effect. Such overlooked case of charge current pumping by time-dependent quantum system, whose magnetization is shrinking while its vector does not rotate, does not require any spin-to-charge conversion via SOC effects. In Ni/Pt bilayer, EM radiation remains dominated by charge current within Ni layer, whose magnitude is larger than in the case of single Ni layer due to faster demagnetization, while often invoked spin-to-charge conversion within Pt layer provides additional but smaller contribution. By using Poynting vector and its flux, we also quantify efficiency of conversion of light into emitted EM radiation, as well as the angular distribution of the latter.
Identifying materials with an efficient spin-to-charge conversion is crucial for future spintronic applications. The spin Hall effect is a central mechanism as it allows for the interconversion of spin and charge currents. Spintronic material research aims at maximizing its efficiency, quantified by the spin Hall angle $Θ_{\textrm{SH}}$ and the spin-current relaxation length $λ_{\textrm{rel}}$. We develop an all-optical method with large sample throughput that allows us to extract $Θ_{\textrm{SH}}$ and $λ_{\textrm{rel}}$. Employing terahertz spectroscopy, we characterize magnetic metallic hete…
Terahertz electromagnetic radiation is extremely useful for numerous applications such as imaging and spectroscopy. Therefore, it is highly desirable to have an efficient table-top emitter covering the 1-to-30-THz window whilst being driven by a low-cost, low-power femtosecond laser oscillator. So far, all solid-state emitters solely exploit physics related to the electron charge and deliver emission spectra with substantial gaps. Here, we take advantage of the electron spin to realize a conceptually new terahertz source which relies on tailored fundamental spintronic and photonic phenomena in…
Spintronic ferromagnetic/non-magnetic heterostructures are novel sources for the generation of THz radiation based on spin-to-charge conversion in the layers. The key technological and scientific challenge of THz spintronic emitters is to increase their intensity and frequency bandwidth. Our work reveals the factors to engineer spintronic Terahertz generation by introducing the scattering lifetime and the interface transmission for spin polarized, non-equilibrium electrons. We clarify the influence of the electron-defect scattering lifetime on the spectral shape and the interface transmission …
Spintronic terahertz (THz) emitter provides the advantages such as apparently broader spectrum, significantly lower cost, and more flexibility in compared with the commercial THz emitters, and thus attracts great interests recently. In past few years, efforts have been made in optimizing the material composition and structure geometry, and the conversion efficiency has been improved close to that of ZnTe crystal. One of the drawbacks of the current designs is the rather limited laser absorption - more than 50% energy is wasted and the conversion efficiency is thus limited. Here, we theoretical…
Deciphering the origin of spin current in spintronic terahertz emitters and its imprint on their electromagnetic radiation via time-dependent density functional theory
Recent studies in spintronics have highlighted ultrathin magnetic metallic multilayers as a novel and very promising class of broadband terahertz radiation sources. Such spintronic multilayers consist of ferromagnetic (FM) and non-magnetic (NM) thin films. When triggered by ultrafast laser pulses, they generate pulsed THz radiation due to the inverse spin-Hall effect, a mechanism that converts optically driven spin currents from the magnetized FM layer into transient transverse charge currents in the NM layer, resulting in THz emission. As THz emitters, FM/NM multilayers have been intensively …
We report on generation of pulsed broadband terahertz radiation utilizing the inverse spin Hall effect in Fe/Pt bilayers on MgO and sapphire substrates. The emitter was optimized with respect to layer thickness, growth parameters, substrates and geometrical arrangement. The experimentally determined optimum layer thicknesses were in qualitative agreement with simulations of the spin current induced in the ferromagnetic layer. Our model takes into account generation of spin polarization, spin diffusion and accumulation in Fe and Pt and electrical as well as optical properties of the bilayer sam…
Narrowband terahertz (THz) radiation is crucial for high-resolution spectral identification, but a narrowband THz source driven by femtosecond (fs) laser has remained scarce. Here, it is computationally predicted that a metal/dielectric/magnetoelastic heterostructure enables converting a fs laser pulse into a multi-cycle THz pulse with a narrow linewidth down to ~1.5 GHz, which is in contrast with the single-cycle, broadband THz pulse from the existing fs-laser-excited emitters. It is shown that such narrowband THz pulse originates from the excitation and long-distance transport of THz spin wa…
Quantum-classical approach to spin and charge pumping and the ensuing radiation in THz spintronics: Example of ultrafast-light-driven Weyl antiferromagnet Mn$_3$Sn
Spin-based terahertz (THz) emitters, utilizing the inverse spin Hall effect, are ultra-modern sources for the generation of THz electromagnetic radiation. To make a powerful emitter having large THz amplitude and bandwidth, fundamental understanding in terms of microscopic models is essential. This study reveals important factors to engineer the THz emission amplitude and bandwidth in epitaxial Pt/Fe emitters grown on MgO and MgAl$_2$O$_4$ (MAO) substrates, where the choice of the substrate plays an important role. The THz amplitude and bandwidth are affected by the induced strain in the Fe sp…
To achieve a large terahertz (THz) amplitude from a spintronic THz emitter (STE), materials with 100\% spin polarisation such as Co-based Heusler compounds as the ferromagnetic layer are required. However, these compounds are known to loose their half-metallicity in the ultrathin film regime, as it is difficult to achieve L2$_1$ ordering, which has become a bottleneck for the film growth. Here, the successful deposition using room temperature DC sputtering of the L2$_1$ and B2 ordered phases of the Co$_2$FeAl full Heusler compound is reported. Co$_2$FeAl is used as ferromagnetic layer together…
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 effects at terahertz (THz) frequencies. Here, we reveal 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: DyCo$_{5}$, Co$_{32}$Fe$_{68}$ and Gd$_{27}$Fe$_{73}$. We measure the frequency-dependent conductivity-tensor elements $σ_{xx}$ …
Terahertz (THz) sciences and technologies have contributed to a rapid development of a wide range of applications and expanded the frontiers in fundamental science. Spintronic terahertz emitters offer conceptual advantages since the spin orientation in the magnetic layer can be easily controlled either by the externally applied magnetic field or by the internal magnetic field distribution determined by the specific shape of the magnetic elements. Here, we report a switchable terahertz source based on micropatterned magnetic heterostructures driven by femtosecond laser pulses. We show that the …
Employing electron spin instead of charge to develop spintronic devices holds the merits of low-power consumption in information technologies. Meanwhile, the demand for increasing speed in spintronics beyond current CMOS technology has further triggered intensive researches for ultrafast control of spins even up to unprecedent terahertz regime. The femtosecond laser has been emerging as a potential technique to generate an ultrafast spin-current burst for magnetization manipulation. However, there is a great challenge to establish all-optical control and monitor of the femtosecond transient sp…
Terahertz spintronics offers the prospect of devices which are both faster and more energy-efficient. A promising route to achieve this goal is to exploit current-induced spin-orbit torques. However, the high-frequency properties of these quantities remain unexplored both experimentally and theoretically, within a realistic material-specific approach. Here we investigate the dynamical transverse components of the torques and uncover contributions longitudinal to the magnetic moment capable of changing its magnitude. We show that, while the torques can be drastically altered in the dynamical re…
Spintronic emitters are a unique class of terahertz (THz) sources due to their quasi-two-dimensional geometry and thereby their capability to couple to resonator near fields. Global excitation of the emitters often obstructs the intricate details of the coupling mechanisms between local THz dipoles and the individual modes of resonator structures. Here, we demonstrate the spatial mapping of the coupling strength between a local terahertz source on a spintronic emitter and far-field light mediated by a structured metallic environment. For a bow-tie geometry, experimental results are reproduced …
The idea to utilize not only the charge but also the spin of electrons in the operation of electronic devices has led to the development of spintronics, causing a revolution in how information is stored and processed. A novel advancement would be to develop ultrafast spintronics using femtosecond laser pulses. Employing terahertz (10$^{12}$ Hz) emission spectroscopy, we demonstrate optical generation of spin-polarized electric currents at the interfaces of metallic ferromagnetic heterostructures at the femtosecond timescale. The direction of the photocurrent is controlled by the helicity of th…
Recent interest in developing fast spintronic devices and laser-controllable magnetic solids has sparked tremendous experimental and theoretical efforts to understand and manipulate ultrafast dynamics in materials. Studies of spin dynamics in the terahertz (THz) frequency range are particularly important for elucidating microscopic pathways toward novel device functionalities. Here, we review THz phenomena related to spin dynamics in rare-earth orthoferrites, a class of materials promising for antiferromagnetic spintronics. We expand this topic into a description of four key elements. (1) We s…
Spin pumping converting sub-terahertz electromagnetic waves to DC spin currents has recently been demonstrated in antiferromagnets (AFMs) with easy-axis magnetic anisotropy. However, easy-plane AFMs such as NiO, which are easier to prepare experimentally, are considered to be bad candidates for spin pumping because the Néel vector oscillation is linearly polarized, placing a major restriction on the material choice for practical applications. Through a case study of NiO, we show that an applied magnetic field below the spin-flop transition can substantially modify the polarization of the reson…
Laser-induced terahertz spin transport (TST) and ultrafast demagnetization (UDM) are central but so far disconnected phenomena in femtomagnetism and terahertz spintronics. Here, we use broadband terahertz emission spectroscopy to reliably measure both processes in one setup. We find that the rate of UDM of a single ferromagnetic metal film F has the same time evolution as the flux of TST from F into an adjacent normal-metal layer N. This remarkable agreement shows that UDM and TST are driven by the same force, which is fully determined by the state of the ferromagnet. An analytical model consi…
Terahertz (THz) signals, mainly generated by photonic or electronic approaches, are being sought for various applications, whereas the development of magnetic source might be a necessary step to harness the magnetic nature of electromagnetic radiation. We show that the relativistic effect on the current-driven domain-wall motion induces THz spin-wave emission in ferrimagnets. The required current density increases dramatically in materials with strong exchange interaction and rapidly exceeds 1012 A m-2, leading to the device breakdown and thus the lack of experimental evidence. By translating …
Magnetic Weyl semimetals are an emerging material class that combines magnetic order and a topologically non-trivial band structure. Here, we study ultrafast optically driven spin injection from thin films of the magnetic Weyl semimetals Co$_2$MnGa and Co$_2$MnAl into an adjacent Pt layer by means of terahertz emission spectroscopy. We find that (i) Co$_2$MnGa and Co$_2$MnAl are efficient terahertz spin-current generators reaching efficiencies of typical 3d-transition-metal ferromagnets such as Fe. (ii) The relaxation of the spin current provides an estimate of the electron-spin relaxation tim…
Recent developments in nanomagnetism and spintronics have enabled the use of ultrafast spin physics for terahertz (THz) emission. Spintronic THz emitters, consisting of ferromagnetic FM / non-magnetic (NM) thin film heterostructures, have demonstrated impressive properties for the use in THz spectroscopy and have great potential in scientific and industrial applications. In this work, we focus on the impact of the FM/NM interface on the THz emission by investigating Fe/Pt bilayers with engineered interfaces. In particular, we intentionally modify the Fe/Pt interface by inserting an ordered L1$…
Mn$_{3}$Sn is a non-collinear antiferromagnet which displays a large anomalous Hall effect at room temperature. It is believed that the principal contribution to its anomalous Hall conductivity comes from Berry curvature. Moreover, dc transport and photoemission experiments have confirmed that Mn$_{3}$Sn may be an example of a time-reversal symmetry breaking Weyl semimetal. Due to a small, but finite moment in the room temperature inverse triangular spin structure, which allows control of the Hall current with external field, this material has garnered much interest for next generation memory …
Terahertz emission spectroscopy of ultrathin multilayers of magnetic and heavy metals has recently attracted much interest. This method not only provides fundamental insights into photoinduced spin transport and spin-orbit interaction at highest frequencies but has also paved the way to applications such as efficient and ultrabroadband emitters of terahertz electromagnetic radiation. So far, predominantly standard ferromagnetic materials have been exploited. Here, by introducing a suitable figure of merit, we systematically compare the strength of terahertz emission from X/Pt bilayers with X b…
Spintronic structures are extensively investigated for their spin orbit torque properties, required for magnetic commutation functionalities. Current progress in these materials is dependent on the interface engineering for the optimization of spin transmission. Here, we advance the analysis of ultrafast spin-charge conversion phenomena at ferromagnetic-transition metal interfaces due to their inverse spin-Hall effect properties. In particular the intrinsic inverse spin Hall effect of Pt-based systems and extrinsic inverse spin-Hall effect of Au:W and Au:Ta in NiFe/Au:(W,Ta) bilayers are inves…
Columbia University（哥伦比亚大学）；Max Planck Institute for the Structure and Dynamics of Matter（马普物质结构与动力学研究所）；National Institute for Materials Science（国立材料研究所）
Although the development of spintronic devices has advanced significantly over the past decade with the use of ferromagnetic materials, the extensive implementation of such devices has been limited by the notable drawbacks of these materials. Antiferromagnets claim to resolve many of these shortcomings leading to faster, smaller, more energy-efficient, and more robust electronics. Antiferromagnets exhibit many desirable properties including zero net magnetization, imperviousness to external magnetic fields, intrinsic high-frequency dynamics with a characteristic precession frequency on the ord…
Spin transport is crucial for future spintronic devices operating at bandwidths up to the terahertz (THz) range. In F|N thin-film stacks made of a ferro/ferrimagnetic layer F and a normal-metal layer N, spin transport is mediated by (1) spin-polarized conduction electrons and/or (2) torque between electron spins. To identify a cross-over from (1) to (2), we study laser-driven spin currents in F|Pt stacks where F consists of model materials with different degrees of electrical conductivity. For the magnetic insulators YIG, GIG and maghemite, identical dynamics is observed. It arises from the TH…
Spintronic terahertz (THz) emitters (STE) based on the inverse spin Hall effect in ferromagnetic/heavy metal (FM/HM) heterostructures have become important sources for THz pulse generation. The design, materials and control of these interfaces at the nanometer level has become vital to engineer their THz emission properties.In this work, we present studies of the optimization of such structures through a multi-pronged approach, taking advantage of material and interface engineering to enhance the THz spintronic emission. This includes: the application of multi-stacks of HM/FM junctions and the…
Electric control of magnetic vortex dynamics in a reproducible way and on an ultrafast time scale is key element in the quest for efficient spintronic devices with low-energy consumption. To be useful the control scheme should ideally be swift, scalable, non-invasive, and resulting in reliable magnetic switching. Such requirements and in particular the reproducibility of altering the vortex chirality and/or polarity are not yet met by magnetic vortex switching via external magnetic fields, spin-polarized currents, spin waves, or laser pulses. Here we demonstrate a novel packaged-skyrmion media…
Bloch-Bloembergen-Slonczewski equation is adopted to simulate magnetization dynamics in spin-valve based spin-transfer torque oscillator with synthetic antiferromagnet acting as a free magnetic layer. High frequency up to the terahertz scale is predicted in synthetic antiferromagnet spin-transfer torque oscillator with no external magnetic field if the following requirements are fulfilled: antiferromagnetic coupling between synthetic antiferromagnetic layers is sufficiently strong, and the thickness of top (bottom) layer of synthetic antiferromagnet is sufficiently thick (thin) to achieve a wi…
Skyrmionic textures are being extensively investigated due to the occurrence of novel topological magnetic phenomena and their promising applications in a new generation of spintronic devices that take advantage of the robust topological stability of their spin structures. The development of practical devices relies on a detailed understanding of how skyrmionic structures can be formed, transferred, detected and annihilated. In this work, our considerations go beyond static skyrmions and theoretically show that the formation/annihilation of both skyrmions and antiskyrmions is enabled by the tr…
Control over spin transport in antiferromagnetic systems is essential for future spintronic applications with operational speeds extending to ultrafast time scales. Here, we study the transition from the gigahertz (GHz) to terahertz (THz) regime of spin transport and spin-to-charge current conversion (S2C) in the prototypical antiferromagnet IrMn by employing spin pumping and THz spectroscopy techniques. We reveal a factor of 4 shorter characteristic propagation lengths of the spin current at THz frequencies (~ 0.5 nm) as compared to the GHz regime (~ 2 nm) which may be attributed to the balli…
Two-dimensional (2D) magnetism has been long sought-after and only very recently realized in atomic crystals of magnetic van der Waals materials. So far, a comprehensive understanding of the magnetic excitations in such 2D magnets remains missing. Here we report polarized micro-Raman spectroscopy studies on a 2D honeycomb ferromagnet CrI3. We show the definitive evidence of two sets of zero-momentum spin waves at frequencies of 2.28 terahertz (THz) and 3.75 THz, respectively, that are three orders of magnitude higher than those of conventional ferromagnets. By tracking the thickness dependence…
In spin-based electronics, information is encoded by the spin state of electron bunches. Processing this information requires the controlled transport of spin angular momentum through a solid, preferably at frequencies reaching the so far unexplored terahertz (THz) regime. Here, we demonstrate, by experiment and theory, that the temporal shape of femtosecond spin-current bursts can be manipulated by using specifically designed magnetic heterostructures. A laser pulse is employed to drive spins from a ferromagnetic Fe thin film into a nonmagnetic cap layer that has either low (Ru) or high (Au) …
Observation of Ultrafast Coherent and Incoherent Spin Torques via Terahertz Spin-Hall Magnetoresistance
Charles University（查理大学）；University of Konstanz（康斯坦茨大学）；Freie Universität Berlin（柏林自由大学）；Czech Academy of Sciences（捷克科学院）；Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy（马克斯·玻恩非线性光学和短脉冲光谱研究所）；Johannes Gutenberg-Universität Mainz（美因茨约翰内斯·古腾堡大学）；Fudan University（复旦大学）；Shanghai Research Center for Quantum Sciences（上海量子科学研究中心）；Martin-Luther-Universität, Halle（哈雷马丁·路德大学）
The spin Hall effect in heavy-metal thin films is routinely employed to convert charge currents into transverse spin currents and can be used to exert torque on adjacent ferromagnets. Conversely, the inverse spin Hall effect is frequently used to detect spin currents by charge currents in spintronic devices up to the terahertz frequency range. Numerous techniques to measure the spin Hall effect or its inverse were introduced, most of which require extensive sample preparation by multi-step lithography. To enable rapid screening of materials in terms of charge-to-spin conversion, suitable high-…
Molecular spin crossover switches are the objects of intense theoretical and experimental studies in recent years. This interest is due to the fact that these systems allow one to control their spin state by applying an external photo-, thermo-, piezo-, or magnetic stimuli. The greatest amount of research is currently devoted to the study the effect of the photoexcitation on the bi-stable states of spin crossover single molecular magnets (SMMs). The main limitation of photo-induced bi-stable states is their short lifetime. In this paper we present the results of a study of the spin dynamics of…
