Spintronic THz emitters based on transition metals and semi-metals/Pt multilayers
J. Hawecker, E. Rongione, A. Markou, S. Krishnia, F. Godel, S. Collin, R. Lebrun, J. Tignon, J. Mangeney, T. Boulier, J. -M. George, C. Felser, H. Jaffrès, S. Dhillon
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 their application to trilayer structures, the use of spin-sinks to simultaneously enhance the THz emitted fields and reduce the use of thick Pt layers to reduce optical absorption, and the use of semi-metals to increase the spin polarization and thus the THz emission. Through these approaches, significant enhancements of the THz field can be achieved. Importantly, taking into account the optical absorption permits to elucidate novel phenomena such as the relation between the spin diffusion length and the spin-sink using THz spectroscopy, as well as possibly distinguishing between self and interface spin-to-charge conversion in semi-metals.
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$…
Significant progress has been made in answering fundamental questions about how and, more importantly, on what time scales interactions between electrons, spins, and phonons occur in solid state materials. These complex interactions are leading to the first real applications of terahertz (THz) spintronics: THz emitters that can compete with traditional THz sources and provide additional functionalities enabled by the spin degree of freedom. This tutorial article is intended to provide the background necessary to understand, use, and improve THz spintronic emitters. A particular focus is the in…
THz pulses are generated from femtosecond pulse-excited ferromagnetic/nonmagnetic spintronic heterostructures via inverse spin Hall effect. The contribution from ultrafast demagnetization/remagnetization is extremely weak, in the comparison. The highest possible THz signal strength from spintronic THz emitters is limited by the optical damage threshold of the corresponding heterostructures. The THz generation efficiency does not saturate with the excitation fluence even up till the damage threshold. Bilayer (Fe, CoFeB)/(Pt, Ta) based FM/NM spintronic heterostructures have been studied for an o…
We present cmtj - a comprehensive simulation package that allows large-scale macrospin simulations for a variety of multilayer spintronics devices. Apart from conventional static simulations, such as magnetoresistance and magnetisation hysteresis loops, cmtj implements a mathematical model of dynamic experimental techniques commonly used for spintronics devices characterisation, for instance: spin diode ferromagnetic resonance, pulse-induced microwave magnetometry, or harmonic Hall voltage measurements. We demonstrate the accuracy of the macrospin simulations on a variety of examples, accompan…
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 $σ_{xx}$ …
Most experimental studies to date of multilayer epitaxial graphene on C-face SiC have indicated that the electronic states of different layers are decoupled as a consequence of rotational stacking. We have measured the third order nonlinear tensor in epitaxial graphene as a novel approach to probe interlayer electronic coupling, by studying THz emission from coherently controlled photocurrents as a function of the optical pump and THz beam polarizations. We find that the polarization dependence of the coherently controlled THz emission expected from perfectly uncoupled layers, i.e. a single gr…
We suggest a new class of hyperbolic metamaterials for THz frequencies based on multilayer graphene structures. We calculate the dielectric permittivity tensor of the effective nonlocal medium with a periodic stack of graphene layers and demonstrate that tuning from elliptic to hyperbolic dispersion can be achieved with an external gate voltage. We reveal that such graphene structures can demonstrate a giant Purcell effect that can be used for boosting the THz emission in semiconductor devices. Tunability of these structures can be enhanced further with an external magnetic field which leads t…
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…
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 …
THz polarization control upon generation is a crucially missing functionality. THz spintronic emitters based on the inverse spin Hall effect allow for this by the strict implicit orthogonality between their magnetization state and the emitted polarization. This control was up till now only demonstrated using cumbersome external magnetic field biasing to impose a polarization direction. We present here for the first time an efficient voltage control of the polarization state of terahertz spintronic emitters. Using a ferromagnetic spin pumping multilayer exhibiting simultaneously strong uniaxial…
In this paper we analyze in details the electronic properties of (Co/Ni) multilayers, a model system for spintronics devices. We use magneto-optical Kerr (MOKE), spin-polarized photoemission spectroscopy (SRPES), x-ray magnetic circular dichroism (XMCD) and anomalous surface diffraction experiments to investigate the electronic properties and perpendicular magnetic anisotropy (PMA) in [Co(x)/Ni(y)] single-crystalline stacks grown by molecular beam epitaxy.
Thermal switching provides an effective way for active heat flow control, which has recently attracted increasing attention in terms of nanoscale thermal management technologies. In magnetic and spintronic materials, the thermal conductivity depends on the magnetization configuration: this is the magneto-thermal resistance effect. Here we show that an epitaxial Cu/Co$_{50}$Fe$_{50}$ multilayer film exhibits giant magnetic-field-induced modulation of the cross-plane thermal conductivity. The magneto-thermal resistance ratio for the Cu/Co$_{50}$Fe$_{50}$ multilayer reaches 150% at room temperatu…
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…
Femtosecond laser-induced photoexcitation of ferromagnet (FM)/heavy metal (HM) heterostructures have attracted attention by emitting broadband terahertz frequencies. The phenomenon relies on the formation of ultrafast spin current, which is largely attributed to the direct photoexcitation of the FM layer. However, we reveal that during the process, the FM layer also experiences a secondary excitation led by the hot electrons from the HM layer that travel across the FM/HM interface and transfer additional energy in the FM. Thus, the generated secondary spins enhance the total spin current forma…
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…
Exchange-coupled nonmagnetic (NM) and ferromagnetic (FM) conducting multilayers are crucial for microwave spintronic devices of the future. We demonstrate, experimentally and theoretically, that in broadband measurements of ferromagnetic resonance (FMR) 10-70 nm-thick permalloy (Py) layers are shielded from the dynamic magnetic field of the microstrip line by eddy currents circulating in the NM capping layers, which strongly diminishes the amplitude of magnetisation precession in the FM material. Our findings have direct implications for designing broadband FMR and measurements of spin current…
Magnetic skyrmions are localized, topologically protected spin-structures that have been proposed for storing or processing information due to their intriguing dynamical and transport properties. Important in terms of applications is the recent discovery of interface stabilized skyrmions as evidenced in ultra-thin transition-metal films. However, so far only skyrmions at interfaces with a single atomic layer of a magnetic material were reported, which greatly limits their potential for application in devices. Here, we predict the emergence of skyrmions in [4d/Fe_2/5d]_n multilayers, i.e. struc…
Multifunctional materials composed of ultrathin magnetic films with perpendicular magnetic anisotropy combined with ferroelectric substrates represent a new approach toward low power, fast, high density spintronics. Here we demonstrate Co/Ni multilayered films with tunable saturation magnetization and perpendicular anisotropy grown directly on ferroelectric PZT [Pb(Zr_xTi_1-x)O_3] substrate plates. Electric fields up to +/- 2 MV/m expand the PZT by 0.1% and generate at least 0.02% in-plane compression in the Co/Ni multilayered film. Modifying the strain with a voltage can reduce the coercive f…
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…
Advancement of molecular devices will critically depend on the approach to establish electrical connections to the functional molecule(s). We produced a molecular device strategy which is based on chemically attaching of molecules between the two magnetic/nonmagnetic metallic electrodes along the multilayer edge(s) of a prefabricated tunnel junction. Here, we present the fabrication methodology for producing these multilayer edge molecular electronics/spintronics devices (MEMEDs/MEMSDs) and details of the associated challenges and their solutions. The key highlight of our MEMED/MEMSD approach …
Hexagonal boron nitride (h-BN) is a promising material for implementation in spintronics due to a large band gap, low spin-orbit coupling, and a small lattice mismatch to graphene and to close-packed surfaces of fcc-Ni(111) and hcp-Co(0001). Epitaxial deposition of h-BN on ferromagnetic metals is aimed at small interface scattering of charge and spin carriers. We report on the controlled growth of h-BN/Ni(111) by means of molecular beam epitaxy (MBE). Structural and electronic properties of this system are investigated using cross-section transmission electron microscopy (TEM) and electron spe…
To address thermal stability issues for spintronic devices with a reduced size, we investigate spin-orbit torque in Co/Pt multilayers with strong perpendicular magnetic anisotropy. Note that the spin-orbit torque arises from the global imbalance of the spin currents from the top and bottom interfaces for each Co layer. By inserting Ta or Cu layers to strengthen the top-down asymmetry, the spin-orbit torque efficiency can be greatly modified without compromised perpendicular magnetic anisotropy. Above all, the efficiency builds up as the number of layers increases, realizing robust thermal stab…
A mechanical equivalent system is introduced to mimic the behavior of multilayer structures with diffusive spin transport. The analogy allows one to use existing mechanical intuition to predict the influence of various parameters on spin torques and spin-dependent magnetoresistance. In particular, it provides an understanding of the sign-changing behavior of spin torque in asymmetric F/N/F spin valves. It further helps to uncover the physical reason behind the singular behavior of spin magnetoresistance in devices with ultra-thin N-layers.
Spin-to-charge conversion (SCC) involving topological surface states (TSS) is one of the most promising routes for highly efficient spintronic devices for terahertz (THz) emission. Here, the THz generation generally occurs mainly via SCC consisting in efficient dynamical spin injection into spin-locked TSS. In this work, we demonstrate sizable THz emission from a nanometric thick topological insultator (TI)/ferromagnetic junction - SnBi$_2$Te$_4$/Co - specifically designed to avoid bulk band crossing with the TSS at the Fermi level, unlike its parent material Bi$_2$Te$_3$. THz emission time do…
The ultimate limitations on carrier mobilities in metal dichalcogenides, and the dynamics associated with carrier relaxation, are unclear. We present measurements of the frequency-dependent conductivity of multilayer dichalcogenide MoS2 by optical-pump terahertz-probe spectroscopy. We find mobilities in this material approaching 4200 cm2/Vs at low temperatures. The temperature dependence of scattering indicates that the mobility, an order of magnitude larger than previously reported for MoS2, is intrinsically limited by acoustic phonon scattering at THz frequencies. Our measurements of carrier…
Ultrafast THz radiation generation from ferromagnetic/nonmagnetic bilayer heterostructure-based spintronic emitters generally exploits the conversion from spin- to charge-current within the nonmagnetic layer and its interface with the ferromagnetic layer. Various possible sub-contributions to the underlying mechanism of inverse spin Hall effect for the THz emission from such structures, need to be exploited for not only investigating the intricacies at the fundamental level in the material properties themselves but also for improving their performance for broadband and high-power THz emission.…
Antiferromagnetic spin motion at terahertz (THz) frequencies attracts growing interests for fast spintronics, however their smaller responses to external field inhibit device application. Recently the noncollinear antiferromagnet Mn$_3$Sn, a Weyl semimetal candidate, was reported to show large anomalous Hall effect (AHE) at room temperature comparable to ferromagnets. Dynamical aspect of such large responses is an important issue to be clarified for future THz data processing. Here the THz anomalous Hall conductivity in Mn$_3$Sn thin films is investigated by polarization-resolved spectroscopy.…
Molybdenum disulfide has recently emerged as a promising two-dimensional semiconducting material for nano-electronic, opto-electronic and spintronic applications. However, demonstrating spin-transport through a semiconducting MoS2 channel is challenging. Here we demonstrate the electrical spin injection and detection in a multilayer MoS2 semiconducting channel. A magnetoresistance (MR) around 1% has been observed at low temperature through a 450nm long, 6 monolayer thick channel with a Co/MgO spin injector and detector. From a systematic study of the bias voltage, temperature and back-gate vol…
Terahertz (THz) spin-to-charge conversion has become an increasingly important process for THz pulse generation and as a tool to probe ultrafast spin interactions at magnetic interfaces. However, its relation to traditional, steady state, ferromagnetic resonance techniques is poorly understood. Here we investigate nanometric trilayers of Co/X/Pt (X=Ti, Au or Au0:85W0:15) as a function of the 'X' layer thickness, where THz emission generated by the inverse spin Hall effect is compared to the Gilbert damping of the ferromagnetic resonance. Through the insertion of the 'X' layer we show that the …
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…
Spin-orbit torque (SOT) magnetization switching of ferromagnets with large perpendicular magnetic anisotropy has a great potential for the next-generation non-volatile magnetoresistive random-access memory (MRAM). It requires a high-performance pure spin current source with a large spin Hall angle and high electrical conductivity, which can be fabricated by a mass production technique. In this work, we demonstrate ultrahigh efficient and robust SOT magnetization switching in all-sputtered BiSb topological insulator - perpendicularly magnetized Co/Pt multilayers. Despite fabricated by the indus…
We report a THz emitter with excellent performances based on nonmagnetic (NM) and ferromagnetic (FM) heterostructures. The spin currents are first excited by the femtosecond laser beam in the NM/FM bilayer, and then transient charge currents are generated by inverse spin Hall effect, leading to THz emission out of the structure. The broadband THz waves emitted from our film stacks have a peak intensity exceeding 500 um thick ZnTe crystals (standard THz emitters). Our device is insensitive to the polarization of an incident laser beam which indicates the noise resistive feature. In contrast, th…
In this work, we report our study on the THz emission in Fe/Pt magnetic heterostructures. We have carried out a comprehensive investigation of THz emission from Fe/Pt magnetic heterostructures, employing time-domain THz spectroscopy. We reveal that by properly tuning the thickness of Fe or Pt layer, THz emission can be greatly improved in this type of heterostructure. We further demonstrate that the THz field strength emitted from a newly designed multilayer (Pt/Fe/MgO)$_n$ with n=3 can reach a value of ~1.6 kV/cm, which is comparable to the values from the conventional GaAs antenna with a bia…
