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.

Atomic-Layer Controlled Transition from Inverse Rashba-Edelstein Effect to Inverse Spin Hall Effect in 2D PtSe2 Probed by THz Spintronic Emission.

2D materials, such as transition metal dichalcogenides, are ideal platforms for spin-to-charge conversion (SCC) as they possess strong spin-orbit coupling (SOC), reduced dimensionality and crystal symmetries as well as tuneable band structure, compared to metallic structures. Moreover, SCC can be tuned with the number of layers, electric field, or strain. Here, SCC in epitaxially grown 2D PtSe2 by THz spintronic emission is studied since its 1T crystal symmetry and strong SOC favor SCC. High quality of as-grown PtSe2 layers is demonstrated, followed by in situ ferromagnet deposition by sputtering that leaves the PtSe2 unaffected, resulting in well-defined clean interfaces as evidenced with extensive characterization. Through this atomic growth control and using THz spintronic emission, the unique thickness-dependent electronic structure of PtSe2 allows the control of SCC. Indeed, the transition from the inverse Rashba-Edelstein effect (IREE) in 1-3 monolayers (ML) to the inverse spin Hall effect (ISHE) in multilayers (>3 ML) of PtSe2 enabling the extraction of the perpendicular spin diffusion length and relative strength of IREE and ISHE is demonstrated. This band structure flexibility makes PtSe2 an ideal candidate to explore the underlying mechanisms and engineering of the SCC as well as for the development of tuneable THz spintronic emitters.

High Efficiency and Flexible Modulation of Spintronic Terahertz Emitters in Synthetic Antiferromagnets.

Spintronic terahertz (THz) emitters based on synthetic antiferromagnets (SAFs) of FM1/Ru/FM2 (FM: ferromagnet) have shown great potential for achieving coherent superposition and significant THz power enhancement due to antiparallel magnetization alignment. However, key issues regarding the effects of interlayer exchange coupling and net magnetization on THz emissions remain unclear, which will inevitably hinder the performance improvement and practical application of THz devices. In this work, we have investigated the femtosecond laser-induced THz emission in Pt (3)/CoFe (3)/Ru (tRu = 0-3.5)/CoFe (tCoFe = 1.5-10)/Pt (3) (in units of nm) films with compensated and uncompensated magnetic moments. Antiferromagnetic (AF) coupling occurs in the Ru thickness ranges of 0.2-1.1 and 1.9-2.3 nm, with the first peak (tRu = 0.4 nm) of the AF coupling field (Hex) significantly higher than that of the second peak (2.0 nm). Rather high THz amplitude is found for the samples with strong AF coupling. Nevertheless, despite the same remanence ratio of zero, the THz amplitude for the symmetric SAF films declines significantly as the tRu decreases from 0.8 to 0.4 nm, which is mainly ascribed to the noncolinear magnetization vectors due to the increased biquadratic coupling term. Specifically, we demonstrate that an asymmetric SAF structure with a dominant FM layer is more favored than the completely compensated one, which could generate significantly enhanced THz electric field with well-controlled polarity and intensity. In addition, as the temperature decreases, the THz emission intensity increases for the SAF samples of tRu = 0.9 nm with negligible biquadratic coupling, which is contrary to the decreasing trend of the tRu = 0.4 nm sample and has been attributed to the greatly enhanced Hex.

An innovative detection technique for capillary electrophoresis: Localized terahertz emission-time domain spectroscopy.

Terahertz (THz) time-domain spectroscopy (TDS) is a recently emerging analysis method which can provide unique information on molecular vibration and rotation induced by inter/intra-molecular interactions. Although the application of THz-TDS to high-performance microscale separation methods like capillary electrophoresis (CE) has been anticipated, it has been hindered due to the diffraction limit of THz wave (typically, hundreds µm). In order to realize CE-THz-TDS, in this study, we placed a narrow open-tubular capillary on the surface of a GaAs semiconductor substrate as a "localized" THz-emitter. By focusing femtosecond pulsed laser beams at the surface of a gallium arsenide (GaAs) substrate closest to the capillary, THz waves were locally generated to pass through the capillary, so that THz absorbance spectra were obtained from the capillary which has narrower inner diameter than the diffraction limit. As a typical result from acetic acid analysis in the CE-THz-TDS platform, information on the refractive index and extinction coefficient was obtained, which showed non-linear and linear concentration dependence, respectively, similar to conventional THz-TDS using large liquid cells. Finally, CE-THz-TDS analysis of several carboxylic acids was demonstrated. Two acids were successfully separated and detected with THz-TDS, where their electrophoretic mobility values were estimated as close to those obtained with conventional contactless conductivity detection. Our proposed CE-THz-TDS showed the potential for the systematic analysis of inter/intra-molecular weak interactions like hydrogen bonds, which are unable to obtain with conventional detectors.

Enhancement of Terahertz Emission by Silver Nanoparticles in a Liquid Medium.

Due to higher molecular density, lower ionization potential, and a better self-healing property compared with gases, liquid targets have been used for laser-induced terahertz generation for many years. In this work, a liquid target used for terahertz radiation is embedded with silver nanoparticles (Ag NPs), which makes the material have both the fluidity of liquids and conductivity of metals. Meanwhile, the experimental setup is easier to implement than that of liquid metals. Polyvinyl alcohol (PVA) is used as a stabilizing agent to avoid precipitation formation. It is observed that the power of 0.5 THz radiation from the Ag NP suspension is five times stronger than that from liquid water in identical experimental conditions. In addition, the reusability of the material is investigated using multiple excitations. UV-visible spectroscopy and TEM imaging are carried out to analyze the target material after each excitation. As a result, quasispherical Ag NP suspensions show good reusability for several excitations and only a decrease in particle concentration is observed. By contrast, the chain-like Ag NP suspension shows poor stability due to PVA damage caused by intense laser pulses, so it cannot be used in a recyclable manner.

Anomalous Nernst Effect Induced Terahertz Emission in a Single Ferromagnetic Film.

Despite its important role in understanding ultrafast spin dynamics and revealing novel spin/orbit effects, the mechanism of the terahertz (THz) emission from a single ferromagnetic nanofilm upon a femtosecond laser pump still remains elusive. Recent experiments have shown exotic symmetry, which is not expected from the routinely adopted mechanism of ultrafast demagnetization. Here, by developing a bidirectional pump-THz emission spectroscopy and associated symmetry analysis method, we set a benchmark for the experimental distinction of the THz emission induced by various mechanisms. Our results unambiguously unveil a new mechanism─anomalous Nernst effect (ANE) induced THz emission due to the ultrafast temperature gradient created by a femtosecond laser. Quantitative analysis shows that the THz emission exhibits interesting thickness dependence where different mechanisms dominate at different thickness ranges. Our work not only clarifies the origin of the ferromagnetic-based THz emission but also offers a fertile platform for investigating the ultrafast optomagnetism and THz spintronics.

Generation of Tunable Terahertz Waves from Tailored Versatile Spintronic Meta-Antenna Arrays.

Broadband spintronic terahertz (THz) radiation can be efficiently generated by spin-to-charge current conversion in a ferromagnetic/nonmagnetic heterostructure. There had been many studies on realizing the enhancement or the modulation of spintronic terahertz waves. However, reported devices so far focus on implementing certain specific modulation methods, either related to the spintronic stacks or related to the metamaterial structures. In this study, a set of femtosecond laser-driven versatile spintronic terahertz devices are proposed by integrating meta-antenna structures with W/CoFeB/Pt nanolayer stacks. These monolithic integrated devices exhibit spintronic terahertz wave emission, spectral modulation, and polarization manipulation simultaneously. The terahertz pulses are generated within the ferromagnetic heterostructure interfaces and transmitted along the metallic structures, leading to the modulation of the spintronic terahertz waves. Results have shown that the center-frequency shift is up to 140 GHz and the value of ellipticity can reach 0.6, demonstrating a set of integrated and efficient spintronic terahertz devices to modulate the emitted wave. In addition, compared with the slotline antenna, the maximum peak value of the bandpass band is enhanced up to 1.63 times by carefully designing the metamaterial structure. The spintronic meta-antenna array proposed here paves an integrated way for the manipulation of spintronic terahertz optoelectronic devices.

Transition from Diffusive to Superdiffusive Transport in Carbon Nanotube Networks via Nematic Order Control.

The one-dimensional confinement of quasiparticles in individual carbon nanotubes (CNTs) leads to extremely anisotropic electronic and optical properties. In a macroscopic ensemble of randomly oriented CNTs, this anisotropy disappears together with other properties that make them attractive for certain device applications. The question however remains if not only anisotropy but also other types of behaviors are suppressed by disorder. Here, we compare the dynamics of quasiparticles under strong electric fields in aligned and random CNT networks using a combination of terahertz emission and photocurrent experiments and out-of-equilibrium numerical simulations. We find that the degree of alignment strongly influences the excited quasiparticles' dynamics, rerouting the thermalization pathways. This is, in particular, evidenced in the high-energy, high-momentum electronic population (probed through the formation of low energy excitons via exciton impact ionization) and the transport regime evolving from diffusive to superdiffusive.

Ultrafast Electron Microscopy of Nanoscale Charge Dynamics in Semiconductors.

The ultrafast dynamics of charge carriers in solids plays a pivotal role in emerging optoelectronics, photonics, energy harvesting, and quantum technology applications. However, the investigation and direct visualization of such nonequilibrium phenomena remains as a long-standing challenge, owing to the nanometer-femtosecond spatiotemporal scales at which the charge carriers evolve. Here, we propose and demonstrate an interaction mechanism enabling nanoscale imaging of the femtosecond dynamics of charge carriers in solids. This imaging modality, which we name charge dynamics electron microscopy (CDEM), exploits the strong interaction of free-electron pulses with terahertz (THz) near fields produced by the moving charges in an ultrafast scanning transmission electron microscope. The measured free-electron energy at different spatiotemporal coordinates allows us to directly retrieve the THz near-field amplitude and phase, from which we reconstruct movies of the generated charges by comparison to microscopic theory. The CDEM technique thus allows us to investigate previously inaccessible spatiotemporal regimes of charge dynamics in solids, providing insight into the photo-Dember effect and showing oscillations of photogenerated electron-hole distributions inside a semiconductor. Our work facilitates the exploration of a wide range of previously inaccessible charge-transport phenomena in condensed matter using ultrafast electron microscopy.

Noncollinear antiferromagnetic textures driven high-harmonic generation from magnetic dynamics in the absence of spin-orbit coupling.

We demonstrate the generation of high order harmonics in carrier pumping from precessing ferromagnetic or antiferromagnetic orders, excited via magnetic resonance, in the presence of topological antiferromagnetic textures. This results in an enhancement of the carrier dynamics by orders of magnitude, enabling for an emission deep in the THz frequency range. Interestingly, the generation process occurs in an intrinsic manner, and is solely governed by the interplay between the s-d exchange coupling underlying the noncollinear antiferromagnetic order and the dynamical s-d exchange constant of the magnetic drive. Therefore, the relativistic spin-orbit interaction is not required for the emergence of high harmonics in the pumped currents. Accordingly, the noncollinear topological antiferromagnetic order is presented as an alternative to spin-orbit interaction for the purpose of harnessing high harmonic emission in carrier pumping. Furthermore, we demonstrate the emergence of high harmonics from random magnetic impurities. This suggests the universality of the magnetically induced high harmonic emission in the presence of real and/or momentum space noncollinear textures. Our proposal initiates a tantalizing prospect for the utilization of topological textures in the context of the highly active domains of ultrafast spintronics and THz emission.

Coherent emission from surface Josephson plasmons in striped cuprates.

The interplay between charge order and superconductivity remains one of the central themes of research in quantum materials. In the case of cuprates, the coupling between striped charge fluctuations and local electromagnetic fields is especially important, as it affects transport properties, coherence, and dimensionality of superconducting correlations. Here, we study the emission of coherent terahertz radiation in single-layer cuprates of the La2-xBaxCuO4 family, for which this effect is expected to be forbidden by symmetry. We find that emission vanishes for compounds in which the stripes are quasi-static but is activated when c-axis inversion symmetry is broken by incommensurate or fluctuating charge stripes, such as in La1.905Ba0.095CuO4 and in La1.845Ba0.155CuO4. In this case, terahertz radiation is emitted by surface Josephson plasmons, which are generally dark modes, but couple to free space electromagnetic radiation because of the stripe modulation.

Flexible Control of Broadband Polarization in a Spintronic Terahertz Emitter Integrated with Liquid Crystal and Metasurface.

Flexible polarization control of the terahertz wave in the wide bandwidth is crucial for numerous applications, such as terahertz communication, material characterization, imaging, and biosensing diagnosis. However, this promise is impeded by the operating bandwidth of circular polarization states, control modes, and the efficiency of the regulation. Here, we report a spintronic terahertz emitter integrated with phase complementary elements, consisting of a liquid crystal and metasurface, to achieve broadband polarization control with high flexibility. This strategy allows the broadband conversion between linear, elliptical, and circular polarization by changing the rotation angle to modulate the space-variant Pancharatnam-Berry phase. The device is characterized with a terahertz time-domain spectroscopy system, demonstrating that the ellipticity of the circular polarization state could keep greater than 0.9 in 0.60-0.99 THz. In the case of an external electro-magnetic field, further polarization modulation experiments are carried out to provide multiple conversion approaches for multi-azimuth. We first propose a method of full broadband polarization state control of the terahertz emitter based on Pancharatnam-Berry phase modulation and an external electro-magnetic field. We believe that such integrated devices with broadband working bandwidth and multiple control modes will make valuable contributions to the development and multi-scene applications of ultrafast terahertz technologies.

Light-Driven Spintronic Heterostructures for Coded Terahertz Emission.

The extraordinary proliferation of digital coding metasurfaces turns the real-time manipulation of electromagnetic (EM) waves into reality and promotes the programmable operation of multifunctional equipment. However, current studies are mainly involved in the modulation of the transmission process, and little attention has been given to the control of EM wave generation, especially in the terahertz (THz) band. Here, we conceptually propose and experimentally demonstrate coded terahertz emission, which integrates the efficient generation and control of THz waves across a wide frequency band. For validation, two types of stripe-patterned ferromagnetic heterostructures with opposite spin Hall angles were utilized as coding units. The two distinct states in each coding unit (with two polarization or phase states of 0° and 180°) can be characterized as "0" and "1" digits, which can be switched by manipulating the optical field distribution of the pump beam. Such an ability to realize simultaneous terahertz coding and terahertz emission is essential for meeting the increasingly demanding requirements of integration and miniaturization. Our work endows ferromagnetic heterostructures with controllable spatial characteristics and benefits their applications in wireless communications and holographic imaging.

Large In-Plane Anisotropic Terahertz Emission Induced by Asymmetric Polarization in Low-Symmetric PdSe2.

Palladium diselenide (PdSe2) exhibits air stability, low symmetry, and high carrier mobility, resulting in unique in-plane anisotropy for polarized optoelectronic devices. However, the relationship of the symmetry and the terahertz (THz) radiation remains elusive yet significant for both the THz source in technology and nonlinear optical physics in science. Herein, we observed large in-plane anisotropic THz radiation from multilayer PdSe2 under femtosecond laser excitation. The THz emission demonstrates 2α dependence on the optical polarization angle from the resonant optical rectification combined with a background from the photocarrier acceleration under the surface depletion field. Interestingly, the in-plane THz emission along and perpendicular to the puckered direction demonstrates large anisotropy. Furthermore, the THz time-domain signals exhibit reversed polarities along the positive and negative puckered directions. This asymmetric polarization could relate to the bonding of Pd-Se, resulting in the unidirectional photon-induced current. Our results bridge the gap between the low-symmetry two-dimensional materials and the THz technology, which could promote the development of THz-polarized devices based on low-symmetry layered materials.

Ultraefficient Terahertz Emission Mediated by Shift-Current Photovoltaic Effect in Layered Gallium Telluride.

Generating terahertz waves using thin-layered materials holds great potential for the realization of integrated terahertz devices. However, previous studies have been limited by restricted radiation intensity and finite efficiency. Exploiting materials with higher efficiency for terahertz emission has attracted increasing interest worldwide. Herein, with visible-light excitation, a thin-layered GaTe film is demonstrated to be a promising emitter of terahertz radiation induced by the shift-current photovoltaic effect. Through theoretical calculations, a transient charge-transfer process resulting from the asymmetric structure of GaTe is shown to be the origin of an ultrafast shift current. Furthermore, it was found that the amplitude of the resulting terahertz signals can be manipulated by both the fluence of the pump laser and the orientation of the sample. Such high emission efficiency from the shift current indicates that the layered material (GaTe) is an excellent candidate for photovoltaics and terahertz emitters.

Terahertz Photoconductivity Spectra of Electrodeposited Thin Bi Films.

Electron dynamics in the polycrystalline bismuth films were investigated by measuring emitted terahertz (THz) radiation pulses after their photoexcitation by tunable wavelength femtosecond duration optical pulses. Bi films were grown on metallic Au, Pt, and Ag substrates by the electrodeposition method with the Triton X-100 electrolyte additive, which allowed us to obtain more uniform films with consistent grain sizes on any substrate. It was shown that THz pulses are generated due to the spatial separation of photoexcited electrons and holes diffusing from the illuminated surface at different rates. The THz photoconductivity spectra analysis has led to a conclusion that the thermalization of more mobile carriers (electrons) is dominated by the carrier-carrier scattering rather than by their interaction with the lattice.

Roadmap of Terahertz Imaging 2021.

In this roadmap article, we have focused on the most recent advances in terahertz (THz) imaging with particular attention paid to the optimization and miniaturization of the THz imaging systems. Such systems entail enhanced functionality, reduced power consumption, and increased convenience, thus being geared toward the implementation of THz imaging systems in real operational conditions. The article will touch upon the advanced solid-state-based THz imaging systems, including room temperature THz sensors and arrays, as well as their on-chip integration with diffractive THz optical components. We will cover the current-state of compact room temperature THz emission sources, both optolectronic and electrically driven; particular emphasis is attributed to the beam-forming role in THz imaging, THz holography and spatial filtering, THz nano-imaging, and computational imaging. A number of advanced THz techniques, such as light-field THz imaging, homodyne spectroscopy, and phase sensitive spectrometry, THz modulated continuous wave imaging, room temperature THz frequency combs, and passive THz imaging, as well as the use of artificial intelligence in THz data processing and optics development, will be reviewed. This roadmap presents a structured snapshot of current advances in THz imaging as of 2021 and provides an opinion on contemporary scientific and technological challenges in this field, as well as extrapolations of possible further evolution in THz imaging.

Noninvasive, label-free, and quantitative monitoring of lipase kinetics using terahertz emission technology.

Enzymes catalyze chemical transformations of great importance in many fields, and analysis of the rate of these transformations is equally important. The latter are typically monitored using surrogate substrates that produce quantifiable optical signals, owing to limitations associated with "label-free" techniques that could be used to monitor the transformation of original substrate molecules. In this study, terahertz (THz) emission technology is used as a noninvasive and label-free technique to monitor the kinetics of lipase-induced hydrolysis of several substrate molecules (including the complex substrate whole cow's milk) and horseradish peroxidase-catalyzed oxidation of o-phenylenediamine in the presence of H2 O2 . This technique was found to be quantitative, and kinetic parameters are compared to those obtained by proton NMR spectroscopy or UV/Vis spectroscopy. This study sets the stage for investigating THz emission technology as a tool for research and development involving enzymes, and for monitoring industrial processes in the food, cosmetic, detergent, pharmaceutical, and biodiesel sectors.

Enhanced Spin-to-Charge Conversion Efficiency in Ultrathin Bi2Se3 Observed by Spintronic Terahertz Spectroscopy.

Owing to their remarkable spin-charge conversion (SCC) efficiency, topological insulators (TIs) are the most attractive candidates for spin-orbit torque generators. The simple method of enhancing SCC efficiency is to reduce the thickness of TI films to minimize the trivial bulk contribution. However, when the thickness reaches the ultrathin regime, the SCC efficiency decreases owing to intersurface hybridization. To overcome these contrary effects, we induced dehybridization of the ultrathin TI film by breaking the inversion symmetry between surfaces. For the TI film grown on an oxygen-deficient transition-metal oxide, the unbonded transition-metal d-orbitals affected only the bottom surface, resulting in asymmetric surface band structures. Spintronic terahertz emission spectroscopy, an emerging tool for investigating the SCC characteristics, revealed that the resulting SCC efficiency in symmetry-broken ultrathin Bi2Se3 was enhanced by up to ∼2.4 times.

Hybrid Perovskite Terahertz Photoconductive Antenna.

Hybrid organic-inorganic perovskites, while well examined for photovoltaic applications, remain almost completely unexplored in the terahertz (THz) range. These low-cost hybrid materials are extremely attractive for THz applications because their optoelectronic properties can be chemically engineered with relative ease. Here, we experimentally demonstrate the first attempt to apply solution-processed polycrystalline films of hybrid perovskites for the development of photoconductive terahertz emitters. By using the widely studied methylammonium-based perovskites MAPbI3 and MAPbBr3, we fabricate and characterize large-aperture photoconductive antennas. The work presented here examines polycrystalline perovskite films excited both above and below the bandgap, as well as the scaling of THz emission with the applied bias field and the optical excitation fluence. The combination of ultrafast time-resolved spectroscopy and terahertz emission experiments allows us to determine the still-debated room temperature carrier lifetime and mobility of charge carriers in halide perovskites using an alternative noninvasive method. Our results demonstrate the applicability of hybrid perovskites for the development of scalable THz photoconductive devices, making these materials competitive with conventional semiconductors for THz emission.