Spin-Orbit Torques and Magnetization Switching in (Bi,Sb)2Te3/Fe3GeTe2 Heterostructures Grown by Molecular Beam Epitaxy.

Topological insulators (TIs) hold promise for manipulating the magnetization of a ferromagnet (FM) through the spin-orbit torque (SOT) mechanism. However, integrating TIs with conventional FMs often leads to significant device-to-device variations and a broad distribution of SOT magnitudes. In this work, we present a scalable approach to grow a full van der Waals FM/TI heterostructure by molecular beam epitaxy, combining the charge-compensated TI (Bi,Sb)2Te3 with 2D FM Fe3GeTe2 (FGT). Harmonic magnetotransport measurements reveal that the SOT efficiency exhibits a non-monotonic temperature dependence and experiences a substantial enhancement with a reduction of the FGT thickness to 2 monolayers. Our study further demonstrates that the magnetization of ultrathin FGT films can be switched with a current density of Jc ∼ 1010 A/m2, with minimal device-to-device variations compared to previous investigations involving traditional FMs.

Experimental Demonstration of a Magnetically Induced Warping Transition in a Topological Insulator Mediated by Rare-Earth Surface Dopants.

Magnetic topological insulators constitute a novel class of materials whose topological surface states (TSSs) coexist with long-range ferromagnetic order, eventually breaking time-reversal symmetry. The subsequent bandgap opening is predicted to co-occur with a distortion of the TSS warped shape from hexagonal to trigonal. We demonstrate such a transition by means of angle-resolved photoemission spectroscopy on the magnetically rare-earth (Er and Dy) surface-doped topological insulator Bi2Se2Te. Signatures of the gap opening are also observed. Moreover, increasing the dopant coverage results in a tunable p-type doping of the TSS, thereby allowing for a gradual tuning of the Fermi level toward the magnetically induced bandgap. A theoretical model where a magnetic Zeeman out-of-plane term is introduced in the Hamiltonian governing the TSS rationalizes these experimental results. Our findings offer new strategies to control magnetic interactions with TSSs and open up viable routes for the realization of the quantum anomalous Hall effect.

Large-Area Synthesis of Ferromagnetic Fe5- x GeTe2 /Graphene van der Waals Heterostructures with Curie Temperature above Room Temperature.

Van der Waals (vdW) heterostructures combining layered ferromagnets and other 2D crystals are promising building blocks for the realization of ultracompact devices with integrated magnetic, electronic, and optical functionalities. Their implementation in various technologies depends strongly on the development of a bottom-up scalable synthesis approach allowing for realizing highly uniform heterostructures with well-defined interfaces between different 2D-layered materials. It is also required that each material component of the heterostructure remains functional, which ideally includes ferromagnetic order above room temperature for 2D ferromagnets. Here, it is demonstrated that the large-area growth of Fe5- x GeTe2 /graphene heterostructures is achieved by vdW epitaxy of Fe5- x GeTe2 on epitaxial graphene. Structural characterization confirms the realization of a continuous vdW heterostructure film with a sharp interface between Fe5- x GeTe2 and graphene. Magnetic and transport studies reveal that the ferromagnetic order persists well above 300 K with a perpendicular magnetic anisotropy. In addition, epitaxial graphene on SiC(0001) continues to exhibit a high electronic quality. These results represent an important advance beyond nonscalable flake exfoliation and stacking methods, thus marking a crucial step toward the implementation of ferromagnetic 2D materials in practical applications.

Milliwatt terahertz harmonic generation from topological insulator metamaterials.

Achieving efficient, high-power harmonic generation in the terahertz spectral domain has technological applications, for example, in sixth generation (6G) communication networks. Massless Dirac fermions possess extremely large terahertz nonlinear susceptibilities and harmonic conversion efficiencies. However, the observed maximum generated harmonic power is limited, because of saturation effects at increasing incident powers, as shown recently for graphene. Here, we demonstrate room-temperature terahertz harmonic generation in a Bi2Se3 topological insulator and topological-insulator-grating metamaterial structures with surface-selective terahertz field enhancement. We obtain a third-harmonic power approaching the milliwatt range for an incident power of 75 mW-an improvement by two orders of magnitude compared to a benchmarked graphene sample. We establish a framework in which this exceptional performance is the result of thermodynamic harmonic generation by the massless topological surface states, benefiting from ultrafast dissipation of electronic heat via surface-bulk Coulomb interactions. These results are an important step towards on-chip terahertz (opto)electronic applications.

Two-dimensional materials prospects for non-volatile spintronic memories.

Non-volatile magnetic random-access memories (MRAMs), such as spin-transfer torque MRAM and next-generation spin-orbit torque MRAM, are emerging as key to enabling low-power technologies, which are expected to spread over large markets from embedded memories to the Internet of Things. Concurrently, the development and performances of devices based on two-dimensional van der Waals heterostructures bring ultracompact multilayer compounds with unprecedented material-engineering capabilities. Here we provide an overview of the current developments and challenges in regard to MRAM, and then outline the opportunities that can arise by incorporating two-dimensional material technologies. We highlight the fundamental properties of atomically smooth interfaces, the reduced material intermixing, the crystal symmetries and the proximity effects as the key drivers for possible disruptive improvements for MRAM at advanced technology nodes.

Unraveling Heat Transport and Dissipation in Suspended MoSe2 from Bulk to Monolayer.

Understanding heat flow in layered transition metal dichalcogenide (TMD) crystals is crucial for applications exploiting these materials. Despite significant efforts, several basic thermal transport properties of TMDs are currently not well understood, in particular how transport is affected by material thickness and the material's environment. This combined experimental-theoretical study establishes a unifying physical picture of the intrinsic lattice thermal conductivity of the representative TMD MoSe2 . Thermal conductivity measurements using Raman thermometry on a large set of clean, crystalline, suspended crystals with systematically varied thickness are combined with ab initio simulations with phonons at finite temperature. The results show that phonon dispersions and lifetimes change strongly with thickness, yet the thinnest TMD films exhibit an in-plane thermal conductivity that is only marginally smaller than that of bulk crystals. This is the result of compensating phonon contributions, in particular heat-carrying modes around ≈0.1 THz in (sub)nanometer thin films, with a surprisingly long mean free path of several micrometers. This behavior arises directly from the layered nature of the material. Furthermore, out-of-plane heat dissipation to air molecules is remarkably efficient, in particular for the thinnest crystals, increasing the apparent thermal conductivity of monolayer MoSe2 by an order of magnitude. These results are crucial for the design of (flexible) TMD-based (opto-)electronic applications.

Van der Waals heterostructures for spintronics and opto-spintronics.

The large variety of 2D materials and their co-integration in van der Waals heterostructures enable innovative device engineering. In addition, their atomically thin nature promotes the design of artificial materials by proximity effects that originate from short-range interactions. Such a designer approach is particularly compelling for spintronics, which typically harnesses functionalities from thin layers of magnetic and non-magnetic materials and the interfaces between them. Here we provide an overview of recent progress in 2D spintronics and opto-spintronics using van der Waals heterostructures. After an introduction to the forefront of spin transport research, we highlight the unique spin-related phenomena arising from spin-orbit and magnetic proximity effects. We further describe the ability to create multifunctional hybrid heterostructures based on van der Waals materials, combining spin, valley and excitonic degrees of freedom. We end with an outlook on perspectives and challenges for the design and production of ultracompact all-2D spin devices and their potential applications in conventional and quantum technologies.

Control of Spin-Orbit Torques by Interface Engineering in Topological Insulator Heterostructures.

(Bi1-xSbx)2Te3 topological insulators (TIs) are gathering increasing attention owing to their large charge-to-spin conversion efficiency and the ensuing spin-orbit torques (SOTs) that can be used to manipulate the magnetization of a ferromagnet (FM). The origin of the torques, however, remains elusive, while the implications of hybridized states and the strong material intermixing at the TI/FM interface are essentially unexplored. By combining interface chemical analysis and spin-transfer ferromagnetic resonance (ST-FMR) measurements, we demonstrate that intermixing plays a critical role in the generation of SOTs. By inserting a suitable normal metal spacer, material intermixing is reduced and the TI properties at the interface are largely improved, resulting in strong variations in the nature of the SOTs. A dramatic enhancement of a field-like torque, opposing and surpassing the Oersted-field torque, is observed, which can be attributed to the non-equilibrium spin density in Rashba-split surface bands and to the suppression of spin memory loss. These phenomena can play a relevant role at other interfaces, such as those comprising transition metal dichalcogenides.

Molecular Approach for Engineering Interfacial Interactions in Magnetic/Topological Insulator Heterostructures.

Controlling interfacial interactions in magnetic/topological insulator heterostructures is a major challenge for the emergence of novel spin-dependent electronic phenomena. As for any rational design of heterostructures that rely on proximity effects, one should ideally retain the overall properties of each component while tuning interactions at the interface. However, in most inorganic interfaces, interactions are too strong, consequently perturbing, and even quenching, both the magnetic moment and the topological surface states at each side of the interface. Here, we show that these properties can be preserved using ligand chemistry to tune the interaction of magnetic ions with the surface states. By depositing Co-based porphyrin and phthalocyanine monolayers on the surface of Bi2Te3 thin films, robust interfaces are formed that preserve undoped topological surface states as well as the pristine magnetic moment of the divalent Co ions. The selected ligands allow us to tune the interfacial hybridization within this weak interaction regime. These results, which are in stark contrast with the observed suppression of the surface state at the first quintuple layer of Bi2Se3 induced by the interaction with Co phthalocyanines, demonstrate the capability of planar metal-organic molecules to span interactions from the strong to the weak limit.

Tunable room-temperature spin galvanic and spin Hall effects in van der Waals heterostructures.

Spin-orbit coupling stands as a powerful tool to interconvert charge and spin currents and to manipulate the magnetization of magnetic materials through spin-torque phenomena. However, despite the diversity of existing bulk materials and the recent advent of interfacial and low-dimensional effects, control of this interconversion at room temperature remains elusive. Here, we demonstrate strongly enhanced room-temperature spin-to-charge interconversion in graphene driven by the proximity of WS2. By performing spin precession experiments in appropriately designed Hall bars, we separate the contributions of the spin Hall and the spin galvanic effects. Remarkably, their corresponding conversion efficiencies can be tailored by electrostatic gating in magnitude and sign, peaking near the charge neutrality point with an equivalent magnitude that is comparable to the largest efficiencies reported to date. Such electric-field tunability provides a building block for spin generation free from magnetic materials and for ultra-compact magnetic memory technologies.

Bottom-up synthesis of multifunctional nanoporous graphene.

Nanosize pores can turn semimetallic graphene into a semiconductor and, from being impermeable, into the most efficient molecular-sieve membrane. However, scaling the pores down to the nanometer, while fulfilling the tight structural constraints imposed by applications, represents an enormous challenge for present top-down strategies. Here we report a bottom-up method to synthesize nanoporous graphene comprising an ordered array of pores separated by ribbons, which can be tuned down to the 1-nanometer range. The size, density, morphology, and chemical composition of the pores are defined with atomic precision by the design of the molecular precursors. Our electronic characterization further reveals a highly anisotropic electronic structure, where orthogonal one-dimensional electronic bands with an energy gap of ∼1 electron volt coexist with confined pore states, making the nanoporous graphene a highly versatile semiconductor for simultaneous sieving and electrical sensing of molecular species.

Impact of the in situ rise in hydrogen partial pressure on graphene shape evolution during CVD growth of graphene.

Exposing graphene to a hydrogen post-etching process yields dendritic graphene shapes. Here, we demonstrate that similar dendritic structures can be achieved at long growth times without adding hydrogen externally. These shapes are not a result of a surface diffusion controlled growth but of the competing backward reaction (etching), which dominates the growth dynamics at long times due to an in situ rise in the hydrogen partial pressure. We have performed a systematic study on the growth of graphene as a function of time to identify the onset and gradual evolution of graphene shapes caused by etching and then demonstrated that the etching can be stopped by reducing the flow of hydrogen from the feed. In addition, we have found that the etching rate due to the in situ rise in hydrogen is strongly dependent on the confinement (geometrical confinement) of copper foil. Highly etched graphene with dendritic shapes was observed in unconfined copper foil regions while no etching was found in graphene grown in a confined reaction region. This highlights the effect of the dynamic reactant distribution in activating the in situ etching process during growth, which needs to be counteracted or controlled for large scale growth.

Thermoelectric spin voltage in graphene.

In recent years, new spin-dependent thermal effects have been discovered in ferromagnets, stimulating a growing interest in spin caloritronics, a field that exploits the interaction between spin and heat currents 1,2 . Amongst the most intriguing phenomena is the spin Seebeck effect 3-5 , in which a thermal gradient gives rise to spin currents that are detected through the inverse spin Hall effect 6-8 . Non-magnetic materials such as graphene are also relevant for spin caloritronics, thanks to efficient spin transport 9-11 , energy-dependent carrier mobility and unique density of states 12,13 . Here, we propose and demonstrate that a carrier thermal gradient in a graphene lateral spin valve can lead to a large increase of the spin voltage near to the graphene charge neutrality point. Such an increase results from a thermoelectric spin voltage, which is analogous to the voltage in a thermocouple and that can be enhanced by the presence of hot carriers generated by an applied current 14-17 . These results could prove crucial to drive graphene spintronic devices and, in particular, to sustain pure spin signals with thermal gradients and to tune the remote spin accumulation by varying the spin-injection bias.

Determination of the spin-lifetime anisotropy in graphene using oblique spin precession.

We determine the spin-lifetime anisotropy of spin-polarized carriers in graphene. In contrast to prior approaches, our method does not require large out-of-plane magnetic fields and thus it is reliable for both low- and high-carrier densities. We first determine the in-plane spin lifetime by conventional spin precession measurements with magnetic fields perpendicular to the graphene plane. Then, to evaluate the out-of-plane spin lifetime, we implement spin precession measurements under oblique magnetic fields that generate an out-of-plane spin population. We find that the spin-lifetime anisotropy of graphene on silicon oxide is independent of carrier density and temperature down to 150 K, and much weaker than previously reported. Indeed, within the experimental uncertainty, the spin relaxation is isotropic. Altogether with the gate dependence of the spin lifetime, this indicates that the spin relaxation is driven by magnetic impurities or random spin-orbit or gauge fields.

Hot-Carrier Seebeck Effect: Diffusion and Remote Detection of Hot Carriers in Graphene.

We investigate hot carrier propagation across graphene using an electrical nonlocal injection/detection method. The device consists of a monolayer graphene flake contacted by multiple metal leads. Using two remote leads for electrical heating, we generate a carrier temperature gradient that results in a measurable thermoelectric voltage V(NL) across the remaining (detector) leads. Due to the nonlocal character of the measurement, V(NL) is exclusively due to the Seebeck effect. Remarkably, a departure from the ordinary relationship between Joule power P and V(NL), V(NL) ∼ P, becomes readily apparent at low temperatures, representing a fingerprint of hot-carrier dominated thermoelectricity. By studying V(NL) as a function of bias, we directly determine the carrier temperature and the characteristic cooling length for hot-carrier propagation, which are key parameters for a variety of new applications that rely on hot-carrier transport.

Electrical detection of spin precession in freely suspended graphene spin valves on cross-linked poly(methyl methacrylate).

Spin injection and detection is achieved in freely suspended graphene using cobalt electrodes and a nonlocal spin-valve geometry. The devices are fabricated with a single electron-beam-resist poly(methyl methacrylate) process that minimizes both the fabrication steps and the number of (aggressive) chemicals used, greatly reducing contamination and increasing the yield of high-quality, mechanically stable devices. As-grown devices can present mobilities exceeding 10(4) cm(2) V(-1) s(-1) at room temperature and, because the contacts deposited on graphene are only exposed to acetone and isopropanol, the method is compatible with almost any contacting material. Spin accumulation and spin precession are studied in these nonlocal spin valves. Fitting of Hanle spin precession data in bilayer and multilayer graphene yields a spin relaxation time of ∼125-250 ps and a spin diffusion length of 1.7-1.9 µm at room temperature.

Magnon-drag thermopile.

Thermoelectric effects in spintronics are gathering increasing attention as a means of managing heat in nanoscale structures and of controlling spin information by using heat flow. Thermal magnons (spin-wave quanta) are expected to play a major role; however, little is known about the underlying physical mechanisms involved. The reason is the lack of information about magnon interactions and of reliable methods to obtain it, in particular for electrical conductors because of the intricate influence of electrons. Here, we demonstrate a conceptually new device that enables us to gather information on magnon-electron scattering and magnon-drag effects. The device resembles a thermopile formed by a large number of pairs of ferromagnetic wires placed between a hot and a cold source and connected thermally in parallel and electrically in series. By controlling the relative orientation of the magnetization in pairs of wires, the magnon drag can be studied independently of the electron and phonon-drag thermoelectric effects. Measurements as a function of temperature reveal the effect on magnon drag following a variation of magnon and phonon populations. This information is crucial to understand the physics of electron-magnon interactions, magnon dynamics and thermal spin transport.

Experimental spin ratchet.

Spintronics relies on the ability to transport and use the spin properties of an electron rather than its charge. We describe a spin ratchet at the single-electron level that produces spin currents with no net bias or charge transport. Our device is based on the ground-state energetics of a single-electron transistor comprising a superconducting island connected to normal leads via tunnel barriers with different resistances that break spatial symmetry. We demonstrate spin transport and quantify the spin ratchet efficiency by using ferromagnetic leads with known spin polarization. Our results are modeled theoretically and provide a robust route to the generation and manipulation of pure spin currents.

Amplitude spectroscopy of a solid-state artificial atom.

The energy-level structure of a quantum system, which has a fundamental role in its behaviour, can be observed as discrete lines and features in absorption and emission spectra. Conventionally, spectra are measured using frequency spectroscopy, whereby the frequency of a harmonic electromagnetic driving field is tuned into resonance with a particular separation between energy levels. Although this technique has been successfully employed in a variety of physical systems, including natural and artificial atoms and molecules, its application is not universally straightforward and becomes extremely challenging for frequencies in the range of tens to hundreds of gigahertz. Here we introduce a complementary approach, amplitude spectroscopy, whereby a harmonic driving field sweeps an artificial atom through the avoided crossings between energy levels at a fixed frequency. Spectroscopic information is obtained from the amplitude dependence of the system's response, thereby overcoming many of the limitations of a broadband-frequency-based approach. The resulting 'spectroscopy diamonds', the regions in parameter space where transitions between specific pairs of levels can occur, exhibit interference patterns and population inversion that serve to distinguish the atom's spectrum. Amplitude spectroscopy provides a means of manipulating and characterizing systems over an extremely broad bandwidth, using only a single driving frequency that may be orders of magnitude smaller than the energy scales being probed.