Terahertz Emission Spectroscopy Research Articles

Enhanced terahertz spin transmittance in the NiO/Pt structure through interface engineering

Since antiferromagnets (AFMs) have the potential to drive spintronic devices to higher speed and stability, generation, and transportation of terahertz (THz) spin currents in AFM/heavy metal (HM) structures have been extensively studied. However, effective methods to optimize the efficiency of THz spin current transmission at the interface are still lacking. Here, we demonstrated a significant enhancement of THz spin current in NiO/Pt structures by using THz emission spectroscopy. The spin transmittance is increased by up to a factor of 3.7 after heating the samples at a temperature of 350 °C for 0.5 h. This enhancement can be attributed to the optimization of the NiO/Pt interface resulting from the heating process. In contrast, the control samples NiO/Cu/Pt and NiO did not exhibit a similar enhancement, indicating that the improvement in spin current transmission is specific to the NiO/Pt interface. The scanning transmission electron microscopy is used to observe the optimized interface and confirmed the reason for THz signal enhancement. Our work paves a way for the modulation of AFM/HM interfaces and the optimization of ultrafast spintronic devices based on AFMs.

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

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

Comprehensive study of the ultrafast photoexcited carrier dynamics in Sb2Te3–GeTe superlattices

Abstract Chalcogenide superlattices Sb2Te3-GeTe is a candidate for interfacial phase-change memory (iPCM) data storage devices. By employing terahertz emission spectroscopy and the transient reflectance spectroscopy together, we investigate the ultrafast photoexcited carrier dynamics and current transients in Sb2Te3-GeTe superlattices. Sample orientation and excitation polarization dependences of the THz emission confirm that ultrafast thermo-electric, shift and injection currents contribute to the THz generation in Sb2Te3-GeTe superlattices. By decreasing the thickness and increasing the number of GeTe and Sb2Te3 layer, the interlayer coupling can be enhanced, which significantly reduces the contribution from circular photo-galvanic effect (CPGE). A photo-induced bleaching in the transient reflectance spectroscopy probed in the range of ~1100 nm to ~1400 nm further demonstrates a gapped state resulting from the interlayer coupling. These demonstrates play an important role in the development of iPCM-based high-speed optoelectronic devices.

Temperature-Dependent Spin-to-Charge Conversion and Efficient Manipulation of Elliptical THz Waves in Bi2Te3/TbFeCo Heterostructures.

Topological insulators (TIs) with spin-momentum-locked surface states and considerable spin-to-charge conversion (SCC) efficiency are ideal substitutes for the nonmagnetic layer in the traditional ferromagnetic/nonmagnetic (FM/NM) spintronic terahertz (THz) emitters. Here, the TI/ferrimagnetic structure as an effective polarization tunable THz source is verified by terahertz emission spectroscopy. The emitted THz electric field can be separated into two THz components utilizing their opposite symmetry on pump polarization and the magnetic field. TI not only emits a THz electric field via the linear photogalvanic effect (LPGE) but also serves as the medium of SCC via the inverse Edelstein effect (IEE) in the heterostructure. In addition, the amplitude and polarity of the SCC component can be efficiently manipulated by temperature in our ferrimagnetic TbFeCo layer compared with Co or Fe. Once these two THz components are delicately set orthogonally, an elliptical THz wave is generated by the intrinsic phase difference at the THz frequency range. The feasible control of its polarization and chirality is demonstrated by three means: pump polarization, magnetic field, and temperature. These appealing observations may pave the way for the development of elliptical THz wave emitters and polarization-sensitive THz spectroscopy.

Ultrafast Shift Current in SnS2 Single Crystals: Structure Considerations, Modeling, and THz Emission Spectroscopy

AbstractAbove‐band gap optical excitation of non‐centrosymmetric semiconductors can lead to the spatial shift of the center of electron charge in a process known as shift current. Shift current is investigated in single‐crystal SnS2, a layered semiconductor with the band gap of ≈2.3 eV, by THz emission spectroscopy and first principles density functional theory (DFT). It is observed that normal incidence excitation with above gap (400 nm; 3.1 eV) pulses results in THz emission from 2H SnS2 () polytype, where such emission is nominally forbidden by symmetry. It is argued that the underlying symmetry breaking arises due to the presence of stacking faults that are known to be ubiquitous in SnS2 single crystals and construct a possible structural model of a stacking fault with symmetry properties consistent with the experimental observations. In addition to shift current, it is observed THz emission by optical rectification excited by below band gap (800 nm; 1.55 eV) pulses but it requires excitation fluence more than two orders of magnitude higher to produce same signal amplitude. These results suggest that ultrafast shift current in which can be excited with visible light in blue–green portion of the spectrum makes SnS2 a promising source material for THz photonics.

Sensitive Characterization of the Graphene Transferred onto Varied Si Wafer Surfaces via Terahertz Emission Spectroscopy and Microscopy (TES/LTEM).

Graphene shows great potential in developing the next generation of electronic devices. However, the real implementation of graphene-based electronic devices needs to be compatible with existing silicon-based nanofabrication processes. Characterizing the properties of the graphene/silicon interface rapidly and non-invasively is crucial for this endeavor. In this study, we employ terahertz emission spectroscopy and microscopy (TES/LTEM) to evaluate large-scale chemical vapor deposition (CVD) monolayer graphene transferred onto silicon wafers, aiming to assess the dynamic electronic properties of graphene and perform large-scale graphene mapping. By comparing THz emission properties from monolayer graphene on different types of silicon substrates, including those treated with buffered oxide etches, we discern the influence of native oxide layers and surface dipoles on graphene. Finally, the mechanism of THz emission from the graphene/silicon heterojunction is discussed, and the large-scale mapping of monolayer graphene on silicon is achieved successfully. These results demonstrate the efficacy of TES/LTEM for graphene characterization in the modern graphene-based semiconductor industry.

Unveiling of Terahertz Emission from Ultrafast Demagnetization and the Anomalous Hall Effect in a Single Ferromagnetic Film

Using THz emission spectroscopy, we investigate the elementary spin dynamics in ferromagnetic single-layer Fe on a sub-picosecond timescale. We demonstrate that THz radiation changes its polarity with reversal of the magnetization applied by the external magnetic field. In addition, it is found that the sign of THz polarity excited from different sides is defined by the thickness of the Fe layer and Fe/dielectric interface. Based on the thickness and symmetry dependences of THz emission, we experimentally distinguish between the two major contributions: ultrafast demagnetization and the anomalous Hall effect. Our experimental results not only enrich understanding of THz electromagnetic generation induced by femtosecond laser pulses but also provide a practical way to access laser-induced ultrafast spin dynamics in magnetic structures.

Giant Photon‐Drag‐Induced Ultrafast Photocurrent in Diamond for Nonlinear Photonics

AbstractDiamond is emerging as an attractive third‐generation wide‐bandgap semiconductor for future on‐chip nonlinear photonics and quantum optics due to its unique thermal, optical, and mechanical properties. However, the light‐driven current under below‐band gap excitation from the second‐order nonlinear optical effect in diamond is still challenging. Herein, a giant second‐order nonlinear photocurrent is observed in the chemical vapor deposition (CVD) diamond by utilizing terahertz (THz) emission spectroscopy. This ultrafast photocurrent originates from the photon drag effect (PDE), during which the momentum transfer from the incident photons to the charge carriers at the rich grain boundaries of the CVD diamond after the exclusive subgap π–π* transition upon femtosecond laser excitation. Especially, the interplay between circular and linear PDE to the THz generation is clarified and distinguished under elliptically polarized light excitation. Furthermore, the picosecond ultrafast dynamics of these charge carriers are also verified by infrared spectroscopy. Owing to the giant photon‐drag‐induced ultrafast photocurrent, the CVD diamond presents the highest THz emission efficiency compared with the reported carbon allotropes, which expands the new functionality of diamond nonlinear photonics into on‐chip THz devices.

Enhanced luminescence efficiency in Eu-doped GaN superlattice structures revealed by terahertz emission spectroscopy

Eu-doped Gallium nitride (GaN) is a promising candidate for GaN-based red light-emitting diodes, which are needed for future micro-display technologies. Introducing a superlattice structure comprised of alternating undoped and Eu-doped GaN layers has been observed to lead to an order-of-magnitude increase in output power; however, the underlying mechanism remains unknown. Here, we explore the optical and electrical properties of these superlattice structures utilizing terahertz emission spectroscopy. We find that ~0.1% Eu doping reduces the bandgap of GaN by ~40 meV and increases the index of refraction by ~20%, which would result in potential barriers and carrier confinement within a superlattice structure. To confirm the presence of these potential barriers, we explored the temperature dependence of the terahertz emission, which was used to estimate the barrier potentials. The result revealed that even a dilutely doped superlattice structure induces significant confinement for carriers, enhancing carrier recombination within the Eu-doped regions. Such an enhancement would improve the external quantum efficiency in the Eu-doped devices. We argue that the benefits of the superlattice structure are not limited to Eu-doped GaN, which provides a roadmap for enhanced optoelectronic functionalities in all rare-earth-doped semiconductor systems.

Terahertz radiation from shockwave front irradiated with femtosecond optical pulses

AbstractFemtosecond double optical pulse experiments with nanosecond time delay were conducted in air. Terahertz pulses were generated from laser plasmas produced by the irradiation with the main pulses on shockwave excited by the pre‐pulse illumination. Intensity of the terahertz pulses depends on the time difference Δt and relative position Δy between the pre‐ and main pulses. We found a characteristic dependence of the intensity of the terahertz pulses on Δy at a longer time delay, Δt = 14.7 ns, which has two maxima while only one maximum was observed when delay times were at and shorter than 9.7 ns. The results are discussed taking into account air density distribution of the shockwave. The terahertz emission spectroscopy shown here can be a useful technique for investigating density structure and its time variation of shockwave with high temporal resolution.

Ultrafast terahertz spin and orbital transport in magnetic/nonmagnetic multilayer heterostructures and a perspective

Ultrafast optically excited ferromagnetic (FM)/nonmagnetic (NM) multilayer heterostructures have been demonstrated recently as efficient, high-power, and broadband sources of terahertz (THz) electromagnetic radiation. Since these spintronic THz emitters exploit the conversion from ultrafast spin to charge current, either in bulk or at the interface, the THz pulses inhere all the characteristics of the involved mechanisms and dynamics associated with spin-charge interconversion processes. Deconvolving the same requires meticulous and careful experimentation and analysis. In this article, we review the current state-of-the-art in this field and provide a perspective on the emerging phenomena, which are prospering as new research avenues and demonstrate application potential for futuristic THz technologies. In the process of developing efficient spintronic THz emitters by optimizing various conditions including those with material parameters and excitation light, it turns out that THz emission spectroscopy itself can be a unique experimental tool for probing microscopic dynamical magnetic and spintronic effects, induced by femtosecond laser pulse excitation, in a noncontact and noninvasive manner. Several breakthroughs can be listed from the literature in this regard from the last decade. Just recently, ultrafast orbitronics is another dimension that is taking shape and will impact the field immensely. A fair account to this topic is also presented in the article.

Giant room-temperature nonlinearities in a monolayer Janus topological semiconductor

Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and certain topological properties, such as the Berry curvature and the quantum metric tensor, have attracted considerable interest. Here, we report giant room-temperature nonlinearities in non-centrosymmetric two-dimensional topological materials—the Janus transition metal dichalcogenides in the 1 T’ phase, synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently show orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities in 1 T’ MoSSe (e.g., > 50 times higher than 2H MoS2 for 18th order harmonic generation; > 20 times higher than 2H MoS2 for terahertz emission). We link this giant nonlinear optical response to topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and heralds the applications of topological materials in optoelectronics down to the monolayer limit.

Terahertz Emission Spectroscopy of Exchange-Biased Spintronic Heterostructures: Single- and Double-Pump Techniques

We show that terahertz (THz) emission spectroscopy is a method to probe the in-plane magnetic state in spintronic heterostructures with exchange bias between the constituent antiferromagnetic and ferromagnetic layers. We demonstrate that the intense laser excitation can switch and reversibly reset the direction of the pinning axis arising from the exchange bias in technologically relevant tunnel magnetoresistance elements. By applying the double-pump THz emission spectroscopy, we reveal that this switching exhibits a threshold character in the pump intensity.

Generalized framework for the step response of semiconducting materials to optically switched electrical bias input in terahertz emission spectroscopy

In this paper, a generalized framework for the step response of semiconducting materials to optically switched electrical bias input in terahertz emission spectroscopy was developed, introducing a complex response function into the frequency domain. A comprehensive formula was obtained for calculating the transient current from the poles of the response function under bias field. This formula was found to give transient currents of an exponentially saturated, overshooting, or oscillating nature for three different regimes of charge transport in an isolated energy band. Furthermore, it was clarified how the transient terahertz emission is linked to the response function and its retarded contribution. When either true current or polarization current is linear with respect to bias field and dominates the transient current, the retarded contribution is identified as the small-signal ac complex conductivity. Two different spectral examples of the retarded contribution were given for actual terahertz Bloch oscillations in biased semiconductor superlattices, describing the small-signal response of polarization current under the Wannier–Stark localization and the large-signal response of true current under interminiband mixing.

Exceptional Spin‐to‐Charge Conversion in Selective Band Topology of Bi/Bi1‐xSbx with Spintronic Singularity

AbstractIn this study, spin‐to‐charge conversion (SCC) of various topological materials with ferromagnet is investigated using spintronic terahertz (THz) emission spectroscopy. Compared with other topological materials, significantly large THz emission is observed for topologically nontrivial phases of Bi1‐xSbx (x > 0.2) that predominantly originates from the topological surface state. When Bi is superposed above a certain stoichiometry of Bi1‐xSbx, it plays a crucial role in generating a highly spin‐split state and enhancing the spin‐mixing conductance, resulting in colossal THz emission. This proves that improving the SCC efficiency through interface engineering is a useful strategy to design a powerful spintronic device. Collectively, this study proposes a methodology for systematically analyzing SCC efficiency or spin Hall angle using THz emission spectroscopy and offers an efficient structure for future spintronic devices.

Spin-Momentum Locking and Ultrafast Spin-Charge Conversion in Ultrathin Epitaxial Bi1 - x Sbx Topological Insulator.

The helicity of three-dimensional (3D) topological insulator surface states has drawn significant attention in spintronics owing to spin-momentum locking where the carriers' spin is oriented perpendicular to their momentum. This property can provide an efficient method to convert charge currents into spin currents, and vice-versa, through the Rashba-Edelstein effect. However, experimental signatures of these surface states to the spin-charge conversion are extremely difficult to disentangle from bulk state contributions. Here, spin- and angle-resolved photo-emission spectroscopy, and time-resolved THz emission spectroscopy are combined to categorically demonstrate that spin-charge conversion arises mainly from the surface state in Bi1 - x Sbx ultrathin films, down to few nanometers where confinement effects emerge. This large conversion efficiency is correlated, typically at the level of the bulk spin Hall effect from heavy metals, to the complex Fermi surface obtained from theoretical calculations of the inverse Rashba-Edelstein response. Both surface state robustness and sizeable conversion efficiency in epitaxial Bi1 - x Sbx thin films bring new perspectives for ultra-low power magnetic random-access memories and broadband THzgeneration.

Terahertz emission from transient currents and coherent phonons in layered MoSe2 and WSe2

Terahertz (THz) time-domain emission spectroscopy was performed on layered 2H-MoSe 2 and 2H-WSe 2. The THz emission shows an initial cycle attributed to surge currents and is followed by oscillations attributed to coherent interlayer phonon modes. To obtain the frequencies of the interlayer vibrations, an analysis of the THz emission waveforms was performed, separating the two contributions to the total waveform. Results of the fitting show several vibrational modes in the range of 5.87–32.75 cm − 1 for the samples, attributed to infrared-active interlayer shear and breathing modes. This study demonstrates that THz emission spectroscopy provides a means of observing these low-frequency vibrational modes in layered materials.

Near-field terahertz nonlinear optics with blue light

The coupling of terahertz optical techniques to scattering-type scanning near-field microscopy (s-SNOM) has recently emerged as a valuable new paradigm for probing the properties of semiconductors and other materials on the nanoscale. Researchers have demonstrated a family of related techniques, including terahertz nanoscopy (elastic scattering, based on linear optics), time-resolved methods, and nanoscale terahertz emission spectroscopy. However, as with nearly all examples of s-SNOM since the technique’s inception in the mid-1990s, the wavelength of the optical source coupled to the near-field tip is long, usually at energies of 2.5 eV or less. Challenges in coupling of shorter wavelengths (i.e., blue light) to the nanotip has greatly inhibited the study of nanoscale phenomena in wide bandgap materials such as Si and GaN. Here, we describe the first experimental demonstration of s-SNOM using blue light. With femtosecond pulses at 410 nm, we generate terahertz pulses directly from bulk silicon, spatially resolved with nanoscale resolution, and show that these signals provide spectroscopic information that cannot be obtained using near-infrared excitation. We develop a new theoretical framework to account for this nonlinear interaction, which enables accurate extraction of material parameters. This work establishes a new realm of possibilities for the study of technologically relevant wide-bandgap materials using s-SNOM methods.

Ultrafast light-driven magneto-optical nonlinearity in ferromagnetic heterostructures.

The dynamic control of magnetization by short laser pulses has recently attracted interest. The transient magnetization at the metallic magnetic interface has been investigated through second-harmonic generation and the time-resolved magneto-optical effect. However, the ultrafast light-driven magneto-optical nonlinearity in ferromagnetic heterostructures for terahertz (THz) radiation remains unclear. Here, we present THz generation from a metallic heterostructure, Pt/CoFeB/Ta, which is ascribed to an ∼6-8% contribution from the magnetization-induced optical rectification and an ∼94-92% contribution from both spin-to-charge current conversion and ultrafast demagnetization. Our results show that THz-emission spectroscopy is a powerful tool to study the picosecond-time-scale nonlinear magneto-optical effect in ferromagnetic heterostructures.

Intervalley energy separation in the conduction band of InAs1−x Bi x determined by terahertz emission spectroscopy

InAsBi layers with different bismuth content were grown on InAs substrates by solid source MBE. The amount of bismuth incorporated in the layers was estimated using X-ray diffraction measurements. The relaxation degree of the grown crystalline layers was evaluated using reciprocal space map analysis. The intervalley energy separation in the conduction band of InAsBi was studied by Terahertz Excitation Spectroscopy. It has been found that this separation slightly decreases with increasing Bi content. In the studied samples with Bi content varying from 2.7% to 4.5% the Γ-L separation shifts down to about 0.9 eV.