Strain Engineering of Epitaxial Pt/Fe Spintronic Terahertz Emitter
Rahul Gupta, Ebrahim Bagherikorani, Venkatesh Mottamchetty, Martin Pavelka, Kasturie Jatkar, Dragos Dancila, Karim Mohammadpour-Aghdam, Anders Rydberg, Rimantas… 展开作者
Rahul Gupta, Ebrahim Bagherikorani, Venkatesh Mottamchetty, Martin Pavelka, Kasturie Jatkar, Dragos Dancila, Karim Mohammadpour-Aghdam, Anders Rydberg, Rimantas Brucas, Hermann A. Dürr, Peter Svedlindh
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 spin source layer. On the one hand, the THz electric field amplitude is found to be larger when Pt/Fe is grown on MgO even though the crystalline quality of the Fe film is superior when grown on MAO. This is because of the larger defect density, smaller electron relaxation time, and lower electrical conductivity in the THz regime when Fe is grown on MgO. On the other hand, the bandwidth is found to be larger for Pt/Fe grown on MAO and is explained by the uncoupled/coupled Lorentz oscillator models. This study provides an insightful pathway to further engineer metallic spintronic THz emitters in terms of the proper choice of substrate and microscopic properties of the emitter layers.
Spintronic terahertz emitters are novel, broadband and efficient sources of terahertz radiation, which emerged at the intersection of ultrafast spintronics and terahertz photonics. They are based on efficient spin-current generation, spin-to-charge-current and current-to-field conversion at terahertz rates. In this review, we address the recent developments and applications, the current understanding of the physical processes as well as the future challenges and perspectives of broadband spintronic terahertz emitters.
The ultrafast relaxation and recombination dynamics of photogenerated electrons and holes in epitaxial graphene are studied using optical-pump Terahertz-probe spectroscopy. The conductivity in graphene at Terahertz frequencies depends on the carrier concentration as well as the carrier distribution in energy. Time-resolved studies of the conductivity can therefore be used to probe the dynamics associated with carrier intraband relaxation and interband recombination. We report the electron-hole recombination times in epitaxial graphene for the first time. Our results show that carrier cooling o…
We present experimental results on the optical absorption spectra of epitaxial graphene from the visible to the terahertz (THz) frequency range. In the THz range, the absorption is dominated by intraband processes with a frequency dependence similar to the Drude model. In the near IR range, the absorption is due to interband processes and the measured optical conductivity is close to the theoretical value of $e^{2}/4\hbar$. We extract values for the carrier densities, the number of carbon atom layers, and the intraband scattering times from the measurements.
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…
We experimentally observe the fast relaxation and relatively slow recombination dynamics of photogenerated electrons/holes in an epitaxial graphene-on-Si heterostructure under pumping with a 1550-nm, 80-fs pulsed fiber laser beam and probing with the corresponding terahertz (THz) beam generated by and synchronized with the pumping laser. The time-resolved electric-field intensity originating from the coherent terahertz photon emission is electro-optically sampled in total-reflection geometry. The Fourier spectrum from 1.8 to 5.2 THz agrees well the pumping photon spectrum. This result is attri…
To explore the capabilities of metallic spintronic thin-film stacks as a source of intense and broadband terahertz electromagnetic fields, we excite a W/CoFeB/Pt trilayer on a large-area glass substrate (diameter of 7.5 cm) by a femtosecond laser pulse (energy 5.5 mJ, duration 40 fs, wavelength 800 nm). After focusing, the emitted terahertz pulse is measured to have a duration of 230 fs, a peak field of 300 kV cm$^{-1}$ and an energy of 5 nJ. In particular, the waveform exhibits a gapless spectrum extending from 1 to 10 THz at 10% of amplitude maximum, thereby facilitating nonlinear control ov…
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 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…
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 …
Materials in which charge and spin degrees of freedom interact strongly offer applications known as spintronics. Following a remarkable success of metallic spintronics based on the giant-magnetoresistive effect, tremendous efforts have been invested into the less developed semiconductor spintronics, in particular, with the aim to produce three-terminal spintronic devices, e.g. spin transistors. One of the most important prerequisites for such a technology is an effective injection of spin-polarized carriers from a ferromagnetic semiconductor into a nonmagnetic semiconductor, preferably one of …
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…
We report on the growth of epitaxial bilayers of the La2/3Sr1/3MnO3 (LSMO) half-metallic ferromagnet and the BiFeO3 (BFO) multiferroic, on SrTiO3(001) by pulsed laser deposition. The growth mode of both layers is two-dimensional, which results in unit-cell smooth surfaces. We show that both materials keep their properties inside the heterostructures, i.e. the LSMO layer (11 nm thick) is ferromagnetic with a Curie temperature of ~330K, while the BFO films shows ferroelectricity down to very low thicknesses (5 nm). Conductive-tip atomic force microscope mappings of BFO/LSMO bilayers for differen…
We study the broadband optical conductivity and ultrafast carrier dynamics of epitaxial graphene in the few-layer limit. Equilibrium spectra of nominally buffer, monolayer, and multilayer graphene exhibit significant terahertz and near-infrared absorption, consistent with a model of intra- and interband transitions in a dense Dirac electron plasma. Non-equilibrium terahertz transmission changes after photoexcitation are shown to be dominated by excess hole carriers, with a 1.2-ps mono-exponential decay that reflects the minority-carrier recombination time.
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…
The rapid discovery of two-dimensional (2D) van der Waals (vdW) quantum materials has led to heterostructures that integrate diverse quantum functionalities such as topological phases, magnetism, and superconductivity. In this context, the epitaxial synthesis of vdW heterostructures with well-controlled interfaces is an attractive route towards wafer-scale platforms for systematically exploring fundamental properties and fashioning proof-of-concept devices. Here, we use molecular beam epitaxy to synthesize a vdW heterostructure that interfaces two material systems of contemporary interest: a 2…
Future spintronics requires the realization of thin film of half-metallic ferromagnets having high Curie temperature and 100\% spin polarization at the Fermi level for potential spintronics applications. In this paper, we report the epitaxial thin films growth of half-metallic CoFeMnGe Heusler alloy on MgO (001) substrate using pulsed laser deposition system, along with the study of structural, magnetic and transport properties. The magnetic property measurements of the thin film suggest a soft ferromagnetic state at room temperature with an in-plane magnetic anisotropy and a Curie temperature…
The possibility of performing spintronics at the molecular level may be realized in devices that combine fully spin polarized oxides such as manganites with carbon nanotubes. However, it is not clear whether electrical transport between such different material systems is viable. Here we show that the room temperature conductance of manganite-nanotube-manganite devices is only half the value recorded in similar palladium-nanotube-palladium devices. Interestingly, the former shows a pseudogap in the conductivity below the relatively high temperature of 200 K. Our results suggest the possibility …
Spin information processing is a possible new paradigm for post-CMOS (complementary metal-oxide semiconductor) electronics and efficient spin propagation over long distances is fundamental to this vision. However, despite several decades of intense research, a suitable platform is still wanting. We report here on highly efficient spin transport in two-terminal polarizer/analyser devices based on high-mobility epitaxial graphene grown on silicon carbide. Taking advantage of high-impedance injecting/detecting tunnel junctions, we show spin transport efficiencies up to 75%, spin signals in the me…
We report on terahertz emission from a single layer ferromagnet which involves the generation of backflow nonthermal charge current from the ferromagnet/dielectric interface by femtosecond laser excitation and subsequent conversion of the charge current to a transverse transient charge current via the anomalous Hall effect, thereby generating the THz radiation. The THz emission can be either enhanced or suppressed, or even the polarity can be reversed, by introducing a magnetization gradient in the thickness direction of the ferromagnet. Unlike spintronic THz emitters reported previously, it d…
Two-dimensional (2D) ferromagnetic materials have been exhibiting promising potential in applications, such as spintronics devices. To grow epitaxial magnetic films on silicon substrate, in the single-layer limit, is practically important but challenging. In this study, we realized the epitaxial growth of MnSn monolayer on Si(111) substrate, with an atomically thin Sn/Si(111)-$2\sqrt{3}\times2\sqrt{3}$- buffer layer, and controlled the MnSn thickness with atomic-layer precision. We discovered the ferromagnetism in MnSn monolayer with the Curie temperature (Tc) of ~54 K. As the MnSn film is gro…
Graphene is attractive for spintronics due to its long spin life time and high mobility. So far only thick and polycrystalline slabs have been used as ferromagnetic electrodes. We report the growth of flat, epitaxial ultrathin Co films on graphene. These display perpendicular magnetic anisotropy in the thickness range 0.5-1nm, which is confirmed by theory. PMA, epitaxy and ultrathin thickness bring new perspectives for graphene-based spintronic devices such as the zero-field control of an arbitrary magnetization direction, band matching between electrodes and graphene, and interface effects su…
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 $σ_{xx}$ …
Magnon-polarons are coherently mixed quasiparticles that originate from the strong magnetoelastic coupling of lattice vibrations and spin waves in magnetic-ordered materials. Recently, magnon-polarons have attracted a lot of attention since they provide a powerful tool to manipulate magnons, which is essential for magnon-based spintronic devices. In this work, we report the experimental observation of facet-dependent magnon-polarons in epitaxial ferrimagnetic Fe3O4 thin films via spin Seebeck effect measurement. The critical magnetic fields for the magnon-polarons in the (110)- and (100)-orien…
Nanoscale Fe3O4 epitaxial thin film has been synthesized on MgO/GaAs(100) spintronic heterostructure, and studied with X-ray magnetic circular dichroism (XMCD). We have observed a total magnetic moment of (3.32 +- 0.1) uB/f.u., retaining 83% of the bulk value. Unquenched orbital moment of (0.47 +- 0.05) uB/f.u. has been confirmed by carefully applying the sum rule. The results offer direct experimental evidence of the bulk-like total magnetic moment and a large orbital moment in the nanoscale fully epitaxial Fe3O4/MgO/GaAs(100) heterostructure, which is significant for spintronics applications…
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…
The ferrimagnetic spinel oxide Zn(x)Fe(3-x)O(4) combines high Curie temperature and spin polarization with tunable electrical and magnetic properties, making it a promising functional material for spintronic devices. We have grown epitaxial thin films with 0<=x<=0.9 on MgO(001) substrates with excellent structural properties both in pure Ar atmosphere and an Ar/O2 mixture by laser molecular beam epitaxy. We find that the electrical conductivity and the saturation magnetization can be tuned over a wide range during growth. Our extensive characterization of the films provides a clear picture of …
We show that in graphene epitaxially grown on SiC the Drude absorption is transformed into a strong terahertz plasmonic peak due to natural nanoscale inhomogeneities, such as substrate terraces and wrinkles. The excitation of the plasmon modifies dramatically the magneto-optical response and in particular the Faraday rotation. This makes graphene a unique playground for plasmon-controlled magneto-optical phenomena thanks to a cyclotron mass 2 orders of magnitude smaller than in conventional plasmonic materials such as noble metals.
Ferrimagnets, which contain the advantages of both ferromagnets (detectable moments) and antiferromagnets (ultrafast spin dynamics), have recently attracted great attention. Here we report the optimization of epitaxial growth of a tetragonal perpendicularly magnetized ferrimagnet Mn2Ga on MgO. Electrical transport, magnetic properties and the anomalous Hall effect (AHE) were systematically studied. Furthermore, we successfully integrated high-quality epitaxial ferrimagnetic Mn2Ga thin films onto ferroelectric PMN-PT single crystals with a MgO buffer layer. It was found that the AHE of such a f…
Antiferromagnetic materials are of great interest for spintronics. Here we present a comprehensive study of the growth, structural characterization, and resulting magnetic properties of thin films of the non-collinear antiferromagnet Mn$_{3}$Ir. Using epitaxial engineering on MgO (001) and Al$_{2}$O$_{3}$ (0001) single crystal substrates, we control the growth of cubic $γ$-Mn$_{3}$Ir in both (001) and (111) crystal orientations, and discuss the optimization of growth conditions to achieve high-quality crystal structures with low surface roughness. Exchange bias is studied in bilayers, with exc…
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…
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…
We report about the anomalous Hall effect in 4f 3d metallic alloys measured using terahertz time-domain spectroscopy. The strength of the observed terahertz spin-dependent transport phenomenon is in good agreement with expectations based on electronic transport measurements. Employing this effect, we succeeded to reveal ultrafast dynamics of the anomalous Hall effect which accompanies the sub-100 picosecond optically induced magnetization reversal in a GdFeCo alloy. The experiments demonstrate the ability to control currents at terahertz frequencies in spintronic devices magnetically and ultra…
The ability to manipulate antiferromagnetic (AF) moments is a key requirement for the emerging field of antiferromagnetic spintronics. Electrical switching of bi-state AF moments has been demonstrated in metallic AFs, CuMnAs and Mn$_2$Au. Recently, current-induced "saw-tooth" shaped Hall resistance was reported in Pt/NiO bilayers, while its mechanism is under debate. Here, we report the first demonstration of convincing, non-decaying, step-like electrical switching of tri-state Néel order in Pt/$α$-Fe$_2$O$_3$ bilayers. Our experimental data, together with Monte-Carlo simulations, reveal the c…
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…
A major challenge for the next generation of spintronics devices is the implementation of ferromagnetic-semiconductor thin films as spin injectors and detectors. Spin-polarised carrier injection cannot be accomplished efficiently from metals, and coupled with the rarity of intrinsic ferromagnetic semiconductors this has driven intensive study of diluted magnetic semiconductors. Chief among these is the doped III-V compound (Ga,Mn)As. These materials suffer from a number of drawbacks; they (i) require magnetic-ion doping well above the solubility limit, and (ii) must be hole doped to above 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…
Development of future sensor, memory, and computing nanodevices based on novel physical concepts is one of the significant research endeavors in solid-state research. The field of spintronics is one such promising area of nanoelectronics which utilizes both the charge and spin of an electron for device operations. The advantage offered by spin systems is in their non-volatility and low-power functionality. This paper reviews emerging spintronic phenomena and the research advancements in diverse spin based applications. Spin devices and systems for logic, memories, emerging computing schemes, f…
Recent studies have demonstrated the potential of antiferromagnets as the active component in spintronic devices. This is in contrast to their current passive role as pinning layers in hard disk read heads and magnetic memories. Here we report the epitaxial growth of a new high-temperature antiferromagnetic material, tetragonal CuMnAs, which exhibits excellent crystal quality, chemical order and compatibility with existing semiconductor technologies. We demonstrate its growth on the III-V semiconductors GaAs and GaP, and show that the structure is also lattice matched to Si. Neutron diffractio…
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…
