Ultrashort Terahertz Research Articles

Observation of terahertz nonlinear absorption activity in Al2O3

We investigate the terahertz (THz) nonlinear absorption characteristics in a thin Al2O3 crystal using nonlinear THz spectroscopy. A THz saturable absorption performance with a high modulation depth (27.5%) and a relatively low saturable intensity (6.99 µJ/cm2) of Al2O3 is revealed, covering the THz spectrum from 0.1 to 8 THz. The inevitable presence of oxygen vacancies and impurities in Al2O3 single crystal results in the existence of free electrons within the conduction band. The transmission enhancement can be described by the change of the mobility of electrons due to intervalley scattering induced by THz pulses, based on first-principles calculations. Therefore, Al2O3 crystals have promising application potential in mode-locked devices for directly delivering broadband ultrashort THz pulses.

Quantum theory of the spin dynamics excited by ultrashort THz laser pulses in rare earth antiferromagnets. DyFeO3

A quantum theory of spin dynamics in the rare-earth orthoferrites excited by terahertz laser pulses is developed. The study demonstrates that dynamic magnetic configurations, triggered by a light pulse, exhibit stability even after the excitation source is ceased. The magnitude of post-excitation oscillations is linked to the ratio between the frequency of rare-earth ion excitations and the frequency of the external source. According to the analysis presented, dynamic response is significantly amplified when the system is exposed to ultrashort terahertz pulses. The physical characteristics of the oscillations emerging after the pulse are determined, and the factors governing their amplitude and phase are identified. The response signal is found to be dependent on the initial part of the pulse, specifically the half-period of the ultrashort light wave, while the subsequent part of the pulse contributes minimally to post-pulse magnetization dynamics. The findings highlight that in DyFeO3, terahertz dynamics primarily result from the influence of the magnetic field of the light, leading to excitations of electrons from the ground state to low-lying electronic levels of Dy3+ions. Additionally, the dynamic magnetoelectric effect excited by the electric field of the pulse is explored, revealing the emergence of odd magnetic modes.

Mechanisms Underlying a Quantum Superposition Microscope Based on THz-Driven Coherent Oscillations in a Two-Level Molecular Sensor.

We report pump-probe measurements of a hydrogen molecule (H_{2}) in the tunnel junction of a scanning tunneling microscope coupled to ultrashort terahertz (THz) pulses. The coherent oscillation of the THz-induced dc tunneling current at a frequency of ∼0.5 THz fingerprints the absorption by H_{2} as a two-level system (TLS). Two components of the oscillatory signal are observed and point to both photon and field aspects of the THz pulses. A few loosely bound states with similar energies for the upper state of the TLS are evidenced by the coherent revival of oscillatory signal. Furthermore, the comparison of spectroscopic features of H_{2} with different tips provides an understanding of the TLS for H_{2}.

Linear and phase controllable terahertz frequency conversion via ultrafast breaking the bond of a meta-molecule

The metasurface platform with time-varying characteristics has emerged as a promising avenue for exploring exotic physics associated with Floquet materials and for designing photonic devices like linear frequency converters. However, the limited availability of materials with ultrafast responses hinders their applications in the terahertz range. Here we present a time-varying metasurface comprising an array of superconductor-metal hybrid meta-molecules. Each meta-molecule consists of two meta-atoms that are “bonded” together by double superconducting microbridges. Through experimental investigations, we demonstrate high-efficiency linear terahertz frequency conversion by rapidly breaking the bond using a coherent ultrashort terahertz pump pulse. The frequency and relative phase of the converted wave exhibit strong dependence on the pump-probe delay, indicating phase controllable wave conversion. The dynamics of the meta-molecules during the frequency conversion process are comprehensively understood using a time-varying coupled mode model. This research not only opens up new possibilities for developing innovative terahertz sources but also provides opportunities for exploring topological dynamics and Floquet physics within metasurfaces.

Magnetization dynamics induced by ultrashort terahertz radiation: Toward designing spin-based terahertz sensors

Magnetization dynamics induced by ultrashort terahertz radiation: Toward designing spin-based terahertz sensors

A novel scheme for ultrashort terahertz pulse generation over a gapless wide spectral range: Raman-resonance-enhanced four-wave mixing

Ultrashort energetic terahertz (THz) pulses have created an exciting new area of research on light interactions with matter. For material studies in small laboratories, widely tunable femtosecond THz pulses with peak field strength close to MV cm−1 are desired. Currently, they can be largely acquired by optical rectification and difference frequency generation in crystals without inversion symmetry. We describe in this paper a novel scheme of THz pulse generation with no frequency tuning gap based on Raman-resonance-enhanced four-wave mixing in centrosymmetric media, particularly diamond. We show that we could generate highly stable, few-cycle pulses with near-Gaussian spatial and temporal profiles and carrier frequency tunable from 5 to >20 THz. They had a stable and controllable carrier-envelop phase and carried ~15 nJ energy per pulse at 10 THz (with a peak field strength of ~1 MV cm−1 at focus) from a 0.5-mm-thick diamond. The measured THz pulse characteristics agreed well with theoretical predictions. Other merits of the scheme are discussed, including the possibility of improving the THz output energy to a much higher level.

Single-Cycle Terahertz Pulse Generation via Superimposed Diffraction With Cherenkov Effect

The ultrashort terahertz (THz) pulse with a broad frequency spectrum has important applications in THz spectroscopy and imaging. Previous THz-pulse generating methods are restricted by either low power or high cost. Here, we propose a novel scheme for generating ultrashort THz pulses, which uses a low-energy sheet electron beam to drive an inclined array of size-graded grooves. The diffraction radiation (DR) from each groove is successively generated and coherently superimposed at a specified direction via the Cherenkov effect. A single-cycle THz pulse with a spectrum band covering the region from 0.1 to 1 THz can be realized. In addition, using several arrays of grooves, a train of ultrashort THz pulses can be further obtained. The radiation power, which depends on the beam current, reaches as high as several kilowatts by using available electron beams. It affords an effective way of generating ultrashort THz pulses with broad application prospects.

Broadband one-dimensional range profiles characteristic of rough surface in terahertz band

<sec>The one-dimensional (1D) range profile is an important back scattering characteristic of objective, which reveals the longitudinal distribution of radar cross section (RCS) along the detection beam. Since the shape and posture can be reflected by the 1D range profile, it is of great significance in military to determine the target orientation, velocity and whether it is armed. In this paper, broadband terahertz 1D-range-profile measurement system is built based on the time-domain spectroscopy (TDS) system. It is in bistatic configuration (bistatic angle of 9°) and the signal-to-noise ratio (SNR) is 34.5 dB, with a gold mirror used as a reflector. Benefiting from the ultrashort terahertz pulse width (full pulse width of 0.52 ps), the bandwidth covers the frequency range from 0.1 THz to 2.5 THz (peaked at 0.9 THz), corresponding to the range resolution on a submillimeter scale.</sec><sec>Firstly, the 1D range profiles of several objects in different shapes are measured, including the step, cylinder, step cone and their combination, which indicates that the geometric profile of the target in the detection direction is adequate to identify the shape feature of the target and proves the reliability of the 1D range profile measuring system based on TDS. Secondly, aluminum plates with different surface roughness in a range of 0–25 μm are also characterized. The Kirchhoff approximation theory and small perturbation method (SPM) are introduced to illustrate the characteristics of broadband terahertz 1D range profile related to the surface roughness of target. It is found that the scattering characteristic of metal object in the terahertz range is sensitive to surface roughness. If the surface roughness of the object is larger, the peak intensity of the 1D range profile will be weaker and the echo signal pulse width becomes wider. The rule is also applicable for the cases with different incident angles. Furthermore, it is revealed that the time delay of the 1D range profile in the bistatic system is related to the rotation direction of the target, which is useful in estimating the posture of the target. In summary, the characteristics of 1D range profile for metal objects relating to shape, surface roughness and posture are studied. The conclusions have certain guiding significance for the target detection and recognition of terahertz radar.</sec>

Ultrafast Buildup Dynamics of Terahertz Pulse Generation in Mode-Locked Quantum Cascade Lasers

Ultrashort terahertz pulse generation is essential for a range of proven terahertz applications, from time-resolved spectroscopy of fundamental excitations to nondestructive testing and imaging. Recently, it has been shown that semiconductor-based terahertz quantum cascade lasers (QCLs) can be used to generate pulses as short as a few picoseconds through active mode locking. However, further progress for subpicosecond and high peak power pulse generation is hampered by poor knowledge on how the electric field actually forms in these lasers. Here, we theoretically and experimentally show the amplitude- and phase-resolved buildup of pulse generation through active mode locking, from initiation of pulse generation to the nanosecond steady state. The experimental results, using an ultrafast coherent seeding technique to probe the laser from femtosecond to nanosecond time scales, are in full agreement with the theoretical calculations based on a theoretical model using multimode reduced rate equations. In particular, we show that the electric field buildup to achieve short pulse operation is extremely fast, requiring only a few photon round trips, owing to the ultrafast gain dynamics of the lasers. Further, this shows a gain recovery time of the order of a few picoseconds, an order of magnitude smaller than the photon round-trip time, highlighting that terahertz QCLs are categorically class-A lasers. This demonstration marks an important formulism for future progress towards exploring the ultrafast pulse generation buildup dynamics of these complex semiconductor lasers.

Propagation of an Ultrashort Terahertz Pulse with a High Electric Field Amplitude in a Silicon Sample

Propagation of an Ultrashort Terahertz Pulse with a High Electric Field Amplitude in a Silicon Sample

A non-collinear autocorrelator for single-shot characterization of ultrabroadband terahertz pulses.

Conventional terahertz (THz) waveform or spectral diagnostics mainly employ the electro-optic-based techniques or the multi-shot Michelson interferometer. Simultaneously, single-shot, ultrabroadband THz spectral measurements remain challenging. In this paper, a novel probe-free scheme based on the non-collinear autocorrelation technique is proposed to characterize the ultrabroadband THz spectrum at a single-shot mode. The non-collinear autocorrelator is a modified beam-division interferometer, in which the two beams are recombined non-collinearly onto a camera. The temporal or spectral resolution and range depend on the noncollinear configuration and camera parameters. This simple approach has been applied experimentally to characterize the ultrashort THz pulse generated from ultraintense laser-solid interactions, demonstrating the capability of single-shot ultrabroadband measurements without an auxiliary ultrafast laser probe. The proposed non-collinear autocorrelator here would be much useful for characterization and applications of low-repetition-rate intense THz sources and could also be extended to other frequency bands.

Molecular orientation echoes via concerted terahertz and near-IR excitations.

A new and efficient method for orientation echo spectroscopy is presented and realized experimentally. The excitation scheme utilizes concerted rotational excitations by both ultrashort terahertz and near-IR pulses and its all-optical detection is enabled by the molecular orientation-induced second harmonic method [J. Phys. Chem. A126, 3732 (2022)10.1021/acs.jpca.2c03237]. This method provides practical means for orientation echo spectroscopy of gas phase molecules and highlights the intriguing underlying physics of coherent rotational dynamics induced by judiciously-orchestrated interactions with both resonant (terahertz) and nonresonant (NIR) fields.

Dynamical characteristics of ultrashort terahertz pulse in metamaterials

We develop a time-dependent theoretical approach to study the interaction between the ultrashort terahertz pulse and the metamaterials beyond the steady-state approximation. By using photoconductive silicon, we show that the system dispersion is changed from abnormal to normal via the classical interference effect. As a result, the terahertz pulse propagates through the material with subluminal/superluminal group velocity. We show that it is not accurate to predict the propagation characteristics of the terahertz pulses by using the steady-state solution of coupled wave equations, and the high-order dispersion terms take a significant role which attributes to the pulse shape deformation and the position-dependent group velocity modification. The theoretical approach presented here is essential of describing the propagation properties of the terahertz pulse in metamaterials and is helpful to understand the nature of quantum interference in electromagnetically induced transparency metamaterial.

Giant effective magnetic fields from optically driven chiral phonons in 4f paramagnets

We present a mechanism by which optically driven chiral phonon modes in rare-earth trihalides generate giant effective magnetic fields acting on the paramagnetic $4f$ spins. With cerium trichloride (CeCl$_3$) as our example system, we calculate the coherent phonon dynamics in response to the excitation by an ultrashort terahertz pulse using a combination of phenomenological modeling and first-principles calculations. We find that effective magnetic fields of over 100 tesla can possibly be generated that polarize the spins for experimentally accessible pulse energies. The direction of induced magnetization can be reversed by changing the handedness of circular polarization of the laser pulse. The underlying process is a phonon analog of the inverse Faraday effect in optics that has been described recently, and which enables novel ways of achieving control over and switching of magnetic order at terahertz frequencies.

Generation dynamics of free carriers in silicon induced by ultrashort intense terahertz pulses

Generation dynamics of free carriers in silicon induced by ultrashort intense terahertz pulses

Self-consistent three-dimensional model of ultrashort terahertz pulse amplification in a laser-induced nonequilibrium plasma channel in xenon

The propagation and amplification of ultrashort terahertz pulses in a nonequilibrium photoionization plasma channel formed in xenon by a powerful femtosecond UV laser pulse is studied in three-dimensional geometry. The study is based on the self-consistent numerical integration of the second-order wave equation in cylindrical geometry and the Boltzmann kinetic equation in the two-term expansion to describe the electron velocity distribution function in the spatially inhomogeneous nonequilibrium plasma of the channel. Keywords: nonlinear optics, terahertz radiation, nonequilibrium plasma channel, numerical simulation.

Самосогласованная трехмерная модель усиления ультракороткого терагерцового импульса в лазерноиндуцированном неравновесном плазменном канале в ксеноне

The propagation and amplification of ultrashort terahertz pulses in a nonequilibrium photoionization plasma channel formed in xenon by a powerful femtosecond UV laser pulse is studied in In three-dimensional geometry. The study is based on the self-consistent numerical integration of the second-order wave equation in cylindrical geometry and the Boltzmann kinetic equation in the two-term eхpansion to describe the electron velocity distribution function in the spatially inhomogeneous nonequilibrium plasma of the channel.

Design of broadband terahertz vector and vortex beams: I. Review of materials and components

In this paper, we review the existing approaches for vortex and vector beam shaping and generation in the terahertz frequency range. The particular focus of this review is on the possibility of homogeneous topological charge formation in the ultra-wide spectral interval inherent to ultrashort terahertz pulses. We review the available materials and components, analyse proposed and potentially possible solutions for broadband terahertz vortex and vector beam shaping, compare all developed approaches, and put forward a unified concept for constructing passive shapers of such beams from the existing component base.

Tuning electron bunch with a longitudinally shaped laser to generate half-cycle terahertz radiation pulse

We present a new scheme for the realization of ultrashort terahertz (THz) radiation pulses by electron beam with a frequency-chirped microbunching structure travelling in a tapered undulator. In this proposal, a longitudinally modulated laser pulse with a chirp rate in the instantaneous modulation frequency is obtained through the optical beating of dual-chirp pulses; then the chirped micro-structure is converted to a chirped density modulation on electron beams by the laser-electron interaction and dispersion effect; finally by sending this electron beam into a designed undulator, ultrashort pulse and broad-band THz radiation can be produced. Considering the fact that the density modulation of the electron beam is directly inherited from the shaped laser, the central frequency and chirp rate can be easily tuned by the optical elements. Numerical simulations confirm that radiation pulses with ultrashort duration can be generated from such a microbunched electron beam. This technique may open new research avenues for strong-field few-cycle THz photonics.

Free-carrier generation dynamics induced by ultrashort intense terahertz pulses in silicon.

We report the results of experimental studies and numerical simulation of the dynamics of the electron-hole pairs formation in silicon under the action of a two-period terahertz pulse with a maximum electric field strength of up to 23 MV/cm. It is shown that an inhomogeneous distribution of the charge carrier concentration over the depth of the silicon sample is formed, which persists for several microseconds. This inhomogeneity is formed due to a sharp increase in the rate of filling the conduction band with free carriers in the subsurface input layer of the silicon wafer, which occurs at a field strength above 15 MV/cm.