Ultrafast terahertz Stark spectroscopy reveals the excited-state dipole moments of retinal in bacteriorhodopsin.

The photoinduced all-trans to 13-cis isomerization of the retinal Schiff base represents the ultrafast first step in the reaction cycle of bacteriorhodopsin (BR). Extensive experimental and theoretical work has addressed excited-state dynamics and isomerization via a conical intersection with the ground state. In conflicting molecular pictures, the excited state potential energy surface has been modeled as a pure S[Formula: see text] state that intersects with the ground state, or in a 3-state picture involving the S[Formula: see text] and S[Formula: see text] states. Here, the photoexcited system passes two crossing regions to return to the ground state. The electric dipole moment of the Schiff base in the S[Formula: see text] and S[Formula: see text] state differs strongly and, thus, its measurement allows for assessing the character of the excited-state potential. We apply the method of ultrafast terahertz (THz) Stark spectroscopy to measure electric dipole changes of wild-type BR and a BR D85T mutant upon electronic excitation. A fully reversible transient broadening and spectral shift of electronic absorption is induced by a picosecond THz field of several megavolts/cm and mapped by a 120-fs optical probe pulse. For both BR variants, we derive a moderate electric dipole change of 5 [Formula: see text] 1 Debye, which is markedly smaller than predicted for a neat S[Formula: see text]-character of the excited state. In contrast, S[Formula: see text]-admixture and temporal averaging of excited-state dynamics over the probe pulse duration gives a dipole change in line with experiment. Our results support a picture of electronic and nuclear dynamics governed by the interaction of S[Formula: see text] and S[Formula: see text] states in a 3-state model.

Photovoltaic effect by soft phonon excitation.

SignificanceThe quantum-mechanical geometric phase of electrons provides various phenomena such as the dissipationless photocurrent generation through the shift current mechanism. So far, the photocurrent generations are limited to above or near the band-gap photon energy, which contradicts the increasing demand of the low-energy photonic functionality. We demonstrate the photocurrent through the optical phonon excitations in ferroelectric BaTiO3 by using the terahertz light with photon energy far below the band gap. This photocurrent without electron-hole pair generation is never explained by the semiclassical treatment of electrons and only arises from the quantum-mechanical geometric phase. The observed photon-to-current conversion efficiency is as large as that for electronic excitation, which can be well accounted for by newly developed theoretical formulation of shift current.

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.

Calibration-free, high-precision, and robust terahertz ultrafast metasurfaces for monitoring gastric cancers.

Optical sensors, with great potential to convert invisible bioanalytical response into readable information, have been envisioned as a powerful platform for biological analysis and early diagnosis of diseases. However, the current extraction of sensing data is basically processed via a series of complicated and time-consuming calibrations between samples and reference, which inevitably introduce extra measurement errors and potentially annihilate small intrinsic responses. Here, we have proposed and experimentally demonstrated a calibration-free sensor for achieving high-precision biosensing detection, based on an optically controlled terahertz (THz) ultrafast metasurface. Photoexcitation of the silicon bridge enables the resonant frequency shifting from 1.385 to 0.825 THz and reaches the maximal phase variation up to 50° at 1.11 THz. The typical environmental measurement errors are completely eliminated in theory by normalizing the Fourier-transformed transmission spectra between ultrashort time delays of 37 ps, resulting in an extremely robust sensing device for monitoring the cancerous process of gastric cells. We believe that our calibration-free sensors with high precision and robust advantages can extend their implementation to study ultrafast biological dynamics and may inspire considerable innovations in the field of medical devices with nondestructive detection.

Generation and Propagation of Ultrafast Terahertz Magnons in Atomically Architectured Nanomagnets.

Utilizing ultrafast terahertz (THz) magnons, the quanta of collective magnetic excitations, as carriers may provide a promising alternative to overcome the problems associated with electrical losses in nanoelectronic devices and circuits. However, efficient excitation of propagating coherent THz magnons in magnonic nanowaveguides is an essential requirement for the development of such devices. Here, by growing ultrathin ferromagnetic nanostructures on a reconstructed surface, we create well-ordered periodic magnetic nanostripes. We demonstrate that such atomically architectured nanowaveguides not only provide a versatile platform for an efficient generation of THz magnons but also allow for their fast propagation. Our results reveal the complex nature of the spin dynamics within such designed nanowaveguides and pave the way for designing ultrafast magnon-based logic devices with THz operation frequencies.

Terahertz Spin-Conductance Spectroscopy: Probing Coherent and Incoherent Ultrafast Spin Tunneling.

Thin-film stacks F|H consisting of a ferromagnetic-metal layer F and a heavy-metal layer H are spintronic model systems. Here, we present a method to measure the ultrabroadband spin conductance across a layer X between F and H at terahertz frequencies, which are the natural frequencies of spin-transport dynamics. We apply our approach to MgO tunneling barriers with thickness d = 0-6 Å. In the time domain, the spin conductance Gs has two components. An instantaneous feature arises from processes like coherent spin tunneling. Remarkably, a longer-lived component is a hallmark of incoherent resonant spin tunneling mediated by MgO defect states, because its relaxation time grows monotonically with d to as much as 270 fs at d = 6.0 Å. Our results are in full agreement with an analytical model. They indicate that terahertz spin-conductance spectroscopy will yield new and relevant insights into ultrafast spin transport in a wide range of spintronic nanostructures.

Magneto-optical Effects of an Artificially Layered Ferromagnetic Topological Insulator with a TC of 160 K.

Magnetic topological insulators are a fertile platform for studying the interplay between magnetism and topology. The unique electronic band structure can induce exotic transport and optical properties. However, a comprehensive optical study at both near-infrared and terahertz frequencies has been lacking. Here, we report magneto-optical effects from a heterostructure of a Cr-incorporated topological insulator, CBST. By measuring the magneto-optical Kerr effect, we observe a high temperature ferromagnetic transition (160 K) in the CBST film. We also use time-domain terahertz polarimetry to reveal a terahertz Faraday rotation of 1.5 mrad and a terahertz Kerr rotation of 3.6 mrad at 2 K. The calculated terahertz Hall conductance is 0.42 e2/h. Our work shows the optical responses of an artificially layered magnetic topological insulator, paving the way toward a high-temperature quantum anomalous Hall effect via heterostructure engineering.

Room-Temperature Plasmon-Assisted Resonant THz Detection in Single-Layer Graphene Transistors.

Frequency-selective or even frequency-tunable terahertz (THz) photodevices are critical components for many technological applications that require nanoscale manipulation, control, and confinement of light. Within this context, gate-tunable phototransistors based on plasmonic resonances are often regarded as the most promising devices for the frequency-selective detection of THz radiation. The exploitation of constructive interference of plasma waves in such detectors promises not only frequency selectivity but also a pronounced sensitivity enhancement at target frequencies. However, clear signatures of plasmon-assisted resonances in THz detectors have been revealed only at cryogenic temperatures so far and remain unobserved at application-relevant room-temperature conditions. In this work, we demonstrate the sought-after room-temperature resonant detection of THz radiation in short-channel gated photodetectors made from high-quality single-layer graphene. The survival of this intriguing resonant regime at room temperature ultimately relies on the weak intrinsic electron-phonon scattering in monolayer graphene, which avoids the damping of the plasma oscillations present in the device channel.

Optical Tweezing Terahertz Probing for a Single Metal Nanoparticle.

Recently, extensive research has been reported on the detection of metal nanoparticles using terahertz waves, due to their potential for efficient and nondestructive detection of chemical and biological samples without labeling. Resonant terahertz nanoantennas can be used to detect a small amount of molecules whose vibrational modes are in the terahertz frequency range with high sensitivity. However, the positioning of target molecules is critical to obtaining a reasonable signal because the field distribution is inhomogeneous over the antenna structure. Here, we combine an optical tweezing technique and terahertz spectroscopy based on nanoplasmonics, resulting in extensive controllable tweezing and sensitive detection at the same time. We observed optical tweezing of a gold nanoparticle and detected it with terahertz waves by using a single bowtie nanoantenna. Furthermore, the calculations confirm that molecular fingerprinting is possible by using our technique. This study will be a prestep of biomolecular detection using gold nanoparticles in terahertz spectroscopy.

Giant Terahertz Birefringence in an Ultrathin Anisotropic Semimetal.

Manipulating the polarization of light at the nanoscale is key to the development of next-generation optoelectronic devices. This is typically done via waveplates using optically anisotropic crystals, with thicknesses on the order of the wavelength. Here, using a novel ultrafast electron-beam-based technique sensitive to transient near fields at THz frequencies, we observe a giant anisotropy in the linear optical response in the semimetal WTe2 and demonstrate that one can tune the THz polarization using a 50 nm thick film, acting as a broadband wave plate with thickness 3 orders of magnitude smaller than the wavelength. The observed circular deflections of the electron beam are consistent with simulations tracking the trajectory of the electron beam in the near field of the THz pulse. This finding offers a promising approach to enable atomically thin THz polarization control using anisotropic semimetals and defines new approaches for characterizing THz near-field optical response at far-subwavelength length scales.

Anomalous Hall Transport by Optically Injected Isospin Degree of Freedom in Dirac Semimetal Thin Film.

Chirality of massless fermions emerging in condensed matter is a key to understand their characteristic behavior as well as to exploit their functionality. However, the chiral nature of massless fermions in Dirac semimetals has remained elusive, due to equivalent occupation of carriers with the opposite chirality in thermal equilibrium. Here, we show that the isospin degree of freedom, which labels the chirality of massless carriers from a crystallographic point of view, can be injected by circularly polarized light. Terahertz Faraday rotation spectroscopy successfully detects the anomalous Hall conductivity by a light-induced isospin polarization in a three-dimensional Dirac semimetal, Cd3As2. Spectral analysis of the Hall conductivity reveals a long scattering time and a long decay time, which are characteristic of the isospin. The long-lived, robust, and reversible character of the isospin promises a potential application of Dirac semimetals in future information technology.

Tunable Surface Wettability via Terahertz Electrowave Controlled Vicinal Subnanoscale Water Layer.

Achieving timely, reversible, and long-range remote tunability over surface wettability is highly demanded across diverse fields, including nanofluidic systems, drug delivery, and heterogeneous catalysis. Herein, using molecular dynamic simulations, we show, for the first time, a theoretical design of electrowetting to achieve remotely controllable surface wettability via using a terahertz wave. The key idea driving the design is the unique terahertz collective vibration identified in the vicinal subnanoscale water layer, which is absent in bulk water, enabling efficient energy transfer from the terahertz wave to the rotational motion of the vicinal subnanoscale water layer. Consequently, a frequency-specific alternating terahertz electric field near the critical strength can significantly affect the local hydrogen-bonding network of the contact water layer on the solid surface, thereby achieving tunable surface wettability.

Molecular Junctions for Terahertz Switches and Detectors.

Molecular electronics targets tiny devices exploiting the electronic properties of the molecular orbitals, which can be tailored and controlled by the chemical structure and configuration of the molecules. Many functional devices have been experimentally demonstrated; however, these devices were operated in the low-frequency domain (mainly dc to MHz). This represents a serious limitation for electronic applications, although molecular devices working in the THz regime have been theoretically predicted. Here, we experimentally demonstrate molecular THz switches at room temperature. The devices consist of self-assembled monolayers of molecules bearing two conjugated moieties coupled through a nonconjugated linker. These devices exhibit clear negative differential conductance behaviors (peaks in the current-voltage curves), as confirmed by ab initio simulations, which were reversibly suppressed under illumination with a 30 THz wave. We analyze how the THz switching behavior depends on the THz wave properties (power and frequency), and we benchmark that these molecular devices would outperform actual THz detectors.

Fundamental Limits of Few-Layer NbSe2 Microbolometers at Terahertz Frequencies.

The rapid development of infrared spectroscopy, observational astronomy, and scanning near-field microscopy has been enabled by the emergence of sensitive mid- and far-infrared photodetectors. Superconducting hot-electron bolometers (HEBs), known for their exceptional signal-to-noise ratio and fast photoresponse, play a crucial role in these applications. While superconducting HEBs are traditionally crafted from sputtered thin films such as NbN, the potential of layered van der Waals (vdW) superconductors is untapped at THz frequencies. Here, we introduce superconducting HEBs made from few-layer NbSe2 microwires. By improving the interface between NbSe2 and metal leads, we overcome impedance mismatch with RF readout, enabling large responsivity THz detection (0.13 to 2.5 THz) with a minimal noise equivalent power of 7 pW/ Hz and nanosecond-range response time. Our work highlights NbSe2 as a promising platform for HEB technology and presents a reliable vdW assembly protocol for custom bolometer production.

Capturing Coherent Magnons by Tip-Assisted Terahertz Spectroscopy.

Our study highlights the versatility of tip-assisted terahertz spectroscopy in probing coherent magnons, the elementary quanta of spin waves in magnetic materials. We identify two distinct coherent magnon types in canted antiferromagnet YFeO3. The remarkable consistency with far-field terahertz spectroscopy in crucial magnon parameters, such as coherence time and resonance frequency, firmly establishes the credibility of tip-assisted terahertz spectroscopy. Notably, we capture more coherent ferromagnetic magnons near the sample surface, underscoring the strength of the technique. This approach paves the way for local, free-standing, and real-space investigations of spin waves in solid magnets.

Ultrafast Exciton Dynamics in the Atomically Thin van der Waals Magnet CrSBr.

Among atomically thin semiconductors, CrSBr stands out as both its bulk and monolayer forms host tightly bound, quasi-one-dimensional excitons in a magnetic environment. Despite its pivotal importance for solid-state research, the exciton lifetime has remained unknown. While terahertz polarization probing can directly trace all excitons, independently of interband selection rules, the corresponding large far-field foci substantially exceed the lateral sample dimensions. Here, we combine terahertz polarization spectroscopy with near-field microscopy to reveal a femtosecond decay of paramagnetic excitons in a monolayer of CrSBr, which is 30 times shorter than the bulk lifetime. We unveil low-energy fingerprints of bound and unbound electron-hole pairs in bulk CrSBr and extract the nonequilibrium dielectric function of the monolayer in a model-free manner. Our results demonstrate the first direct access to the ultrafast dielectric response of quasi-one-dimensional excitons in CrSBr, potentially advancing the development of quantum devices based on ultrathin van der Waals magnets.

Emerging potentials of Fe-based nanomaterials for chiral sensing and imaging.

Fe-based nanostructures have possessed promising properties that make it suitable for chiral sensing and imaging applications owing to their ultra-small size, non-toxicity, biocompatibility, excellent photostability, tunable fluorescence, and water solubility. This review summarizes the recent research progress in the field of Fe-based nanostructures and places special emphases on their applications in chiral sensing and imaging. The synthetic strategies to prepare the targeted Fe-based structures were also introduced. The chiral sensing and imaging applications of the nanostructures are discussed in details.

All-Dielectric Integrated Meta-Antenna Operating in 6G Terahertz Communication Window.

Efficient transceivers and antennas at terahertz frequencies are leading the development of 6G terahertz communication systems. The antenna design for high-resolution terahertz spatial sensing and communication remains challenging, while emergent metallic metasurface antennas can address this issue but often suffer from low efficiency and complex manufacturing. Here, an all-dielectric integrated meta-antenna operating in 6G terahertz communication window for high-efficiency beam focusing in the sub-wavelength scale is reported. With the antenna surface functionalized by metagrating arrays with asymmetric scattering patterns, the design and optimization methods are demonstrated with a physical size constraint. The highest manipulation and diffraction efficiencies achieve 84.1% and 48.1%. The commercially accessible fabrication method with low cost and easy to implement has been demonstrated for the meta-antenna by photocuring 3D printing. A filamentous focal spot is measured as 0.86λ with a long depth of focus of 25.3λ. Its application for integrated imaging and communication has been demonstrated. The proposed technical roadmap provides a general pathway for creating high-efficiency integrated meta-antennas with great potential in high-resolution 6G terahertz spatial sensing and communication applications.

Graphene Terahertz Devices for Sensing and Communication.

Graphene-based terahertz (THz) devices have emerged as promising platforms for a variety of applications, leveraging graphene's unique optoelectronic properties. This review explores recent advancements in utilizing graphene in THz technology, focusing on two main aspects: THz molecular sensing and THz wave modulation. In molecular sensing, the environment-sensitive THz transmission and emission properties of graphene are utilized for enabling molecular adsorption detection and biomolecular sensing. This capability holds significant potential, from the detection of pesticides to DNA at high sensitivity and selectivity. In THz wave modulation, crucial for next-generation wireless communication systems, graphene demonstrates remarkable potential in absorption modulation when gated. Novel device structures, spectroscopic systems, and metasurface architectures have enabled enhanced absorption and wave modulation. Furthermore, techniques such as spatial phase modulation and polarization manipulation have been explored. From sensing to communication, graphene-based THz devices present a wide array of opportunities for future research and development. Finally, advancements in sensing techniques not only enhance biomolecular analysis but also contribute to optimizing graphene's properties for communication by enabling efficient modulation of electromagnetic waves. Conversely, developments in communication strategies inform and enhance sensing capabilities, establishing a mutually beneficial relationship.

Recent Progress of 2D Materials-Based Photodetectors from UV to THz Waves: Principles, Materials, and Applications.

Photodetectors are one of the most critical components for future optoelectronic systems and it undergoes significant advancements to meet the growing demands of diverse applications spanning the spectrum from ultraviolet (UV) to terahertz (THz). 2D materials are very attractive for photodetector applications because of their distinct optical and electrical properties. The atomic-thin structure, high carrier mobility, low van der Waals (vdWs) interaction between layers, relatively narrower bandgap engineered through engineering, and significant absorption coefficient significantly benefit the chip-scale production and integration of 2D materials-based photodetectors. The extremely sensitive detection at ambient temperature with ultra-fast capabilities is made possible with the adaptability of 2D materials. Here, the recent progress of photodetectors based on 2D materials, covering the spectrum from UV to THz is reported. In this report, the interaction of light with 2D materials is first deliberated on in terms of optical physics. Then, various mechanisms on which detectors work, important performance parameters, important and fruitful fabrication methods, fundamental optical properties of 2D materials, various types of 2D materials-based detectors, different strategies to improve performance, and important applications of photodetectors are discussed.