THz Pulses Research Articles

Terahertz Time-Domain Spectroscopy of Low-Concentration N2O Using Long-Range Multipass Gas Cell

We developed a long-range multipass gas cell that extends the beam path to 18.61 m, for which a THz beam shows multiple reflections within a diameter of only 32 cm and a height of 54 cm. Due to the very long propagation THz beam path in the multipass gas cell, the absorbance and absorption coefficients of nitrous oxide can be measured very sensitively from 0.2 to 1.2 THz bandwidth. The gas concentration can be determined from the measured THz pulses for the absorption. As the gas concentration increased sequentially from 1.0% to 8.3% at atmospheric pressure, the absorbance lines also increased sequentially. The resulting absorptions and frequencies of transitions showed good agreement between experiment and calculations performed with the HITRAN database.

Highly scalable multicycle THz production with a homemade periodically poled macrocrystal

The THz regime is widely appealing across many disciplines including solid-state physics, life sciences, and increasingly in particle acceleration. Multicycle THz pulses are typically formed via optical rectification in periodically poled crystals. However the manufacturing procedures of these crystals limit their apertures to below ~1 cm, which from damage limitations of the crystal, limits the total pump power which can be employed, and ultimately, the total THz power which can be produced. Here we report on the simple in-house fabrication of a periodically poled crystal using ~300 μm thick wafers. Each wafer is consecutively rotated by 180∘ to support quasi-phase matching. We validate the concept with a Joule-class laser system operating at 10 Hz and measure up to 1.3 mJ of energy at 160 GHz, corresponding to an average peak power of approximately 35 MW and a conversion efficiency of 0.14%. In addition, a redshifting of the pump spectrum of ~50 nm is measured. Our results indicate that high-power THz radiation can be produced with existing and future high-power lasers in a scalable way, setting a course toward multi-gigawatt multicycle THz pulses.

Excitation of molecular rotational levels by unipolar subcycle pulses

We study theoretically the action of subcycle unipolar pulses on the rotational dynamics of polar molecules. We show that efficient excitation of molecular rotational resonances by subcycle pump pulses with respect to bipolar single-cycle one is achieved, provided that duration of excitation pulses is much smaller than the rotational period of the molecule. The excitation probability for different rotational levels is analysed in dependence on the parameters of molecules and pump pulses. Remarkably, our analysis revealed the possibility of the almost single level excitation and the formation of the population inversion in the rotational levels excited by unipolar pulses, in spite of the nonresonant interaction and ultrabroad spectrum of subcycle pulses. This approach is entirely different from the traditional resonant excitation techniques with long quasi-monochromatic pulses tuned to the molecular transition. And from the other methods, when multi-color laser pulses or single-cycle THz pulses are used for control of the molecular properties. This opens new avenues in applications related to control of molecular systems and lasing creation, since it allows efficient ultrafast control over different rotational levels.

Injection-Seeded Terahertz Parametric Oscillator with a Ring-Cavity Configuration

This paper reports the characteristics of an injection-seeded terahertz parametric oscillator (TPO) with a ring-cavity configuration based on the MgO:LiNbO3 crystal. The ring cavity is constituted of three mirrors and the THz wave output surface where the pump and Stokes beams are totally reflected. The THz pulse energies and the Stokes pulse energies as functions of the pump pulse energy for different seed powers of 47.5 mW, 150.7 mW, and 312.8 mW were investigated. The experimental results showed that the injection-seeded ring cavity TPO exhibited the benefits of lower pump thresholds and higher output energies for the Stokes and THz waves. The smaller the pump pulse energy, the more obvious the effect of the seed injection. The reasons for the laser performance improvement were analyzed.

Sub-nanosecond terahertz radiation obtained with an aperiodically poled lithium niobate and organic HMQ-TMS.

We report a compact, simple source of terahertz radiation that can be tuned to well-defined frequencies spanning ∼1.4 to 10 THz, based on difference-frequency generation in an HMQ-TMS crystal. The pair of pump pulses required for this process is obtained by optical parametric generation in an aperiodically-poled lithium niobate crystal; the center wavelength of this pair of pulses is around 1.45 µm. We obtained 40 nJ THz pulses using 38 µJ, 0.85 ns pump pulses.

Broadband terahertz wave emission from liquid metal

Metals have been studied as terahertz sources for decades. Recent research has shown the potential of metals in generating extremely high THz pulse energy excited by intense laser pulses. To avoid the metal surface debris caused by laser pulses, here, we report the results of the broadband terahertz wave emission from a flowing liquid metal line excited by subpicosecond laser pulses. The THz signal emitted from the liquid gallium line shows the stronger field with the broader bandwidth compared to the signal from water under the identical optical excitation conditions. Our preliminary study suggests that the liquid metals have the potential to serve as efficient and powerful THz sources for the intense lasers with a high repetition rate.

Pulsed THz imaging for thickness characterization of plastic sheets

The thickness of 2, 4, 6, 8, 10, and 12 mm thick polycarbonate (PC) and poly-methyl methacrylate (PMMA) sheets were characterized nondestructively by terahertz time-of-flight tomography in reflection. Due to terahertz attenuation and dispersion in the material, first characterized in transmission, features in the reflected signal associated with structure deep in the sample (i.e., the back interface) may be difficult to identify, and therefore signal processing is employed, namely frequency-wavelet domain deconvolution and a cross-correlation approach in which we account for dispersion. The refractive indices are found to be n(ν)=1.67−0.0096vfor PC and n(ν)=1.61−0.0085vfor PMMA, while the absorption coefficients, which follow the form of the universal dielectric response, are αν=0.564+9.075v1.669 for PC and αν=0.0406+13.66v1.776 for PMMA, where ν is measured in THz and the absorption coefficient is in units of cm−1. We show that straightforward analysis techniques that neglect dispersion are limited to measuring layer thicknesses in these materials of less than ~17 mm, while accounting for dispersion results in a factor-of-two improvement, allowing us to measure samples as thick as ~36 mm.

Feasibility study for a THz acceleration experiment on the PHIL accelerator at LAL

We present a feasibility study for an experiment aiming to post-accelerate an electron bunch, coming from the PHIL (Photo-Injecteur au LAL) photoinjector at LAL (Laboratoire de l’Accélérateur Linéaire), in a circular partially dielectric-loaded waveguide (DLW) driven by a multicycle THz pulse generated by the infrared laser coming from the LASERIX (Installation laser XUV/IR de l’Université Paris Sud) facility. We first discuss the considerations taken into account to fix the DLW design and the THz pulse properties, especially the choice of a 160 GHz THz pulse frequency, and then provide a set of values for their main parameters. We then perform start-to-end simulations of the acceleration experiment, taking into account the current achievable range of parameters at PHIL and the THz pulse properties already achieved with LASERIX with some margins for the coupling losses. They demonstrate the possibility to obtain a 1.2 MeV energy gain for a 10 pC bunch, without charge losses, with a clear shift of the energy spectrum, which would represent a significant improvement compared to the current state-of-the-art of THz acceleration. An overview of the upcoming steps towards the realization of the experiment is finally given.

THz Radiation of Photoconductive Antennas based on {LT-GaAa/GaAa:Si} Superlattice Structures

A material in the form of a multilayer structure based on low-temperature LT-GaAs grown on (111)A-oriented substrates is proposed for fabrication of THz photoconductive antennas. These structures contain active LT-GaAs layers and doping acceptor GaAs:Si-based layers. At the optical pump power of 19 mW and the bias voltage of 30 V, a photoconductive antenna based on the optimized {LT-GaAs/GaAs:Si} (111)A structure emits THz pulses with the average power of 2.3 μW at the pulse repetition frequency of 80 MHz; the conversion efficiency is 1.2 × 10–4. It is shown that the dependence of the integral power of THz pulses of the antenna based on the {LT-GaAs/GaAs:Si} (111)A structure on the applied voltage is superlinear; the dependence of this parameter on the optical pump power is plotted as a curve with saturation. It is shown that the designed antennas have a practical application in THz spectroscopy of biological solutions.

Electromagnetic and Beam Dynamics Studies for High Gradient Accelerators at Terahertz Frequencies

THz radiation is one of the most appealing portion of the electromagnetic spectrum in terms of multi-disciplinary use in basic science and technology. Beyond the numerous applications, a great interest is its potential for future, compact linear accelerators.Conventional radio-frequency accelerating structures operating at the S and C band can reach gradients up to 30 - 50MV/m, respectively; higher accelerating gradients, of the order of 100MV/m, have been obtained with X-band cavities. THz-based accelerating structures enable operation at even higher gradient, potentially up to the GV/m scale, holding great potential for their application to free-electron lasers and linear colliders, for instance.Here we present electromagnetic and beam dynamics studies about the use of a dielectric loaded waveguide to accelerate electron bunches by mean of a narrow-band multi-cycle THz pulse. The excitation of the accelerating structure by the THz pulse and the bunch acceleration in the excited field are investigated through CST Microwave Studio and GPT simulations.

Long-Lasting Molecular Orientation Induced by a Single Terahertz Pulse.

We present a novel, previously unreported phenomenon appearing in a thermal gas of nonlinear polar molecules excited by a single THz pulse. We find that the induced orientation lasts long after the excitation pulse is over. In the case of symmetric-top molecules, the time-averaged orientation remains indefinitely constant, whereas in the case of asymmetric-top molecules the orientation persists for a long time after the end of the pulse. We discuss the underlying mechanism, study its nonmonotonous temperature and amplitude dependencies, and show that there exist optimal parameters for maximal residual orientation. The persistent orientation implies a long-lasting macroscopic dipole moment, which may be probed by even harmonic generation and may enable deflection by inhomogeneous electrostatic fields.

Generation of sub cycle terahertz pulses via coherent control of nonlinear medium by femtosecond pulses

In this paper, we revise our recent advances in study of high-efficient methods of sub cycle THz pulse generation and control of their wave shape. These methods are based on coherent control of low frequency oscillations in nonlinear medium excited by infrared femtosecond pulses. Our results showed the possibility of sub – and few-cycle pulse formation of controllable wave shapes: half-cycle, rectangular and triangular and single-cycle ones in THz, XUV and optical ranges.

A high-power, high-repetition-rate THz source for pump-probe experiments at Linac Coherent Light Source II.

Experiments using a THz pump and an X-ray probe at an X-ray free-electron laser (XFEL) facility like the Linac Coherent Light Source II (LCLS II) require frequency-tunable (3 to 20 THz), narrow bandwidth (∼10%), carrier-envelope-phase-stable THz pulses that produce high fields (>1 MV cm-1) at the repetition rate of the X-rays and are well synchronized with them. In this paper, a two-bunch scheme to generate THz radiation at LCLS II is studied: the first bunch produces THz radiation in an electromagnet wiggler immediately following the LCLS II undulator that produces X-rays from the second bunch. The initial time delay between the two bunches is optimized to compensate for the path difference in THz transport. The two-bunch beam dynamics, the THz wiggler and radiation are described, as well as the transport system bringing the THz pulses from the wiggler to the experimental hall.

Formation of gigahertz pulse train by chirped terahertz pulses interference

The state-of-art broadband THz sources can contribute to the development of short-range 6G communications. This paper has demonstrated the feasibility of forming the controllable sequence of THz subpulses in the temporal domain and the corresponding quasidiscrete spectrum by the interference of two THz pulses with an exponential chirp. Moreover, due to small time delay between these pulses the temporal and spectral structures are similar to each other (so-called “linkage relation”). This will benefit information encoding in the THz range. The calculated metrics for the prototype communication channel based on the proposed method are competitive with existing short-range THz CW channels.

Spectral filtering with diffractive reflection gratings for fast superconducting detectors in the THz frequency range

In this work we describe the design process of a grating spectrometer with fast superconducting THz detectors based on Niobiumnitride. The main application is the use as a diagnostic tool for accelerator-based sources of THz radiation like synchrotrons, where interactions of the electron bunches in storage ring lead to fluctuations in spectrum and intensity of the emitted radiation.Guidelines for the design of the two main parts, grating and detector design, are given. Here, a blazed reflection grating for a frequency range of 1 THz to 5 THz has been developed and successfully fabricated in a high-precision milling process out of brass. Also three different planar antenna designs (double-slot, annular slot and log-per spiral) in combination with quasioptical bandpass filters for the THz range have been simulated and evaluated for best spectral resolution and power coupling.Finally, we have verified grating performance for pulsed THz radiation of 1 THz in an experiment conducted at the synchrotron light source of the KIT. Excellent agreement of the grating performance to the simulations has been found.

Sub-Wavelength THz Imaging of the Domains in Periodically Poled Crystals Through Optical Rectification

By focusing a femtosecond laser beam onto the lateral face of a periodically poled KTP crystal, we generate a THz pulse through optical rectification of the laser pulse. The THz signal is recorded by means of a common THz time-domain technique, which allows us to obtain both the magnitude and sign of the THz waveform, and then the magnitude and phase of its spectral components thanks to a numerical Fourier-transform. By moving the laser beam along the crystal, we record a THz signal that renders for the alternative orientation of the crystal domains, with a lateral resolution as good as 10 μm, whatever the THz wavelength. This demonstrates the potential of the Optical Rectification TeraHertz Imaging (ORTI) technique to produce sub-wavelength THz images.

Temperature dependent inverse spin Hall effect in Co/Pt spintronic emitters

In bilayers of ferromagnets and heavy metals, which form the so-called spintronic emitters, the phenomena of ultrafast demagnetization and the inverse spin Hall effect (ISHE) conspire to yield remarkably efficient emission of electric pulses in the THz band. Light-induced demagnetization of the ferromagnet launches a pulse of spin current into the heavy metal, wherein it bifurcates into a radiative charge transient due to the ISHE. The influence of temperature on this combined effect should depend on both the magnetic phase diagram and the microscopic origin of spin Hall conductivity, but its exact dependence remains to be clarified. Here, we experimentally study the temperature dependence of an archetypal spintronic emitter, the Co/Pt bilayer, using electro-optic sampling of the emitted THz pulses in the time domain. The emission amplitude is attenuated with decreasing temperature, consistent with an inverse spin Hall effect in platinum of predominantly intrinsic origin.

Strong Anisotropy in Liquid Water upon Librational Excitation Using Terahertz Laser Fields.

Tracking the excitation of water molecules in the homogeneous liquid is challenging due to the ultrafast dissipation of rotational excitation energy through the hydrogen-bonded network. Here we demonstrate strong transient anisotropy of liquid water through librational excitation using single-color pump-probe experiments at 12.3 THz. We deduce a third-order response of χ3 exceeding previously reported values in the optical range by 3 orders of magnitude. Using a theory that replaces the nonlinear response with a material property amenable to molecular dynamics simulation, we show that the rotationally damped motion of water molecules in the librational band is resonantly driven at this frequency, which could explain the enhancement of the anisotropy in the liquid by the external terahertz field. By addition of salt (MgSO4), the hydration water is instead dominated by the local electric field of the ions, resulting in reduction of water molecules that can be dynamically perturbed by THz pulses.

Guiding and emission of milijoule single-cycle THz pulse from laser-driven wire-like targets.

The miscellaneous applications of terahertz have called for an urgent demand of a super intense terahertz source. Here, we demonstrate the capability of femtosecond laser-driven wires as an efficient ultra-intense terahertz source using 700 mJ laser pulses. When focused onto a wire target, coherent THz generation took place in the miniaturized gyrotron-like undulator where emitted electrons move in the radial electric field spontaneously created on wire surface. The single-cycle terahertz pulse generated from the target is measured to be radially polarized with a pulse energy of a few milijoule. By further applying this scheme to a wire-tip target, we show the near field of the 500 nm radius apex could reach up to 90 GV/m. This efficient THz energy generation and intense THz electric field mark a substantial improvement toward ultra-intense terahertz sources.

High-intensity THz pulse generation by TW laser radiation in ionized gas and nonlinear crystals

Intense electromagnetic fields can be obtained now in THz frequency range. THz pulses with electric field intensity above 1 MV/cm are now requested for strong-field applications like particle acceleration, short electron bunches measurements, controlling the state of the matter. The advantage of a THz pulse in comparison with the visible frequency range is the almost non-oscillating field that interacts with charged particles more efficiently. The advantage over a direct field is the ability to remotely focus this radiation in space and in time. Except for the huge free-electron lasers facilities, the only way to get THz pulses of MV/cm intensity is the conversion of high-power femtosecond laser pulses. We compare two ways of generating intense THz pulses using the radiation of TW and GW laser systems operating at 800 nm. They are two-color filamentation in gas and optical rectification in nonlinear crystals. The prospects for scaling of THz generation methods for a petawatt laser are discussed.