Terahertz time-domain spectroscopy (THz TDS) is a well-known tool for material analysis in the terahertz frequency band. One crucial system component in every time-domain spectrometer is the delay line which is necessary to accomplish the sampling of the electric field over time. Despite the fact that most of the uncertainty sources in TDS have been discussed, the delay line uncertainty has not been considered in detail. We model the impact of delay line uncertainty on the acquired THz TDS data. Interferometric measurements of the delay line precision and THz time-domain data are used to validate the theoretical model.
We introduce THz Stark spectroscopy by using intense single-cycle terahertz pulses as the electric field source and monitoring the induced spectral response of an isotropic molecular ensemble with a coincident femtosecond supercontinuum pulse. THz Stark spectroscopy offers several advantages over conventional Stark spectroscopy and opens previously inaccessible perspectives. Most importantly, THz pulses oscillate faster than typical molecular rotations and consequently eliminate the requirement to freeze the samples to prevent poling effects. Hence, THz Stark spectroscopy allows for time-resol…
Frequency combs have revolutionized time and frequency metrology and in recent years, new frequency comb lasers that are highly compact or even on-chip have been demonstrated in the mid-infrared and THz regions of the electromagnetic spectrum. The emerging technologies include electrically pumped quantum and interband cascade semiconductor devices, as well as high-quality factor microresonators. In this guest editorial, the authors summarize recent advances in the field, the potential for rapid broadband spectroscopy, as well as the challenges and prospects for use in molecular gas sensing.
Dual terahertz (THz) comb spectroscopy is a promising methods for high accuracy, high resolution, and broadband THz spectroscopy because the mode-resolved THz comb spectrum possesses both characteristics of broadband THz radiation and narrow-linewidth continuous-wave THz radiation and all frequency mode of THz comb can be phase-locked to a microwave frequency standard. However, requirement of stabilized dual femtosecond lasers has often hindered wide use of this method. In this article, we demonstrated the adaptive sampling, dual THz comb spectroscopy, enabling use of free-running dual femtose…
Broadband THz spectroscopy system beyond 25 THz using BNA crystals and a tunable single-ring-fiber compressor
University of Ottawa（渥太华大学）；Max Planck Institute for the Science of Light（马克斯·普朗克光科学研究所）；University of Erlangen-Nürnberg（埃尔朗根-纽伦堡大学）；National Research Council Canada（加拿大国家研究委员会）
THz extinction spectroscopy extends UV-Vis and NIR-spectroscopy to characterize particles from fine powders and dust to sand, grains and granulated materials. We extract particle sizes from the spectral position of the first peak of the interference structure and size distributions from the visibility of the fine ripple structure in the measured extinction spectra. As such, we can demonstrate a route for a quick determination of these parameters from single measurements.
We demonstrated combination of gapless terahertz (THz) comb with dual-comb spectroscopy, namely gapless dual-THz-comb spectroscopy, to achieve the spectral resolution equal to width of the THz comb tooth. The gapless THz comb was realized by interpolating frequency gaps between the comb teeth with sweeping of a laser mode-locked frequency. The demonstration of low-pressure gas spectroscopy with gapless dual-THz-comb spectroscopy clearly indicated that the spectral resolution was decreased down to 2.5-MHz width of the comb tooth and the spectral accuracy was enhanced to 10-6 within the spectral…
We present an integrated THz spectroscopy and sensing platform featuring low loss, vacuum-like dispersion, and strong field confinement in the fundamental mode. Its performance was characterized experimentally for frequencies between 0.1 THz and 1.5 THz. While linear THz spectroscopy and sensing gain mostly from low loss and an extended interaction length, nonlinear THz spectroscopy would also profit from the field enhancement associated to strong mode confinement. Moreover, the vacuum-like dispersion allows for a reshaping-free propagation of broadband single- to few-cycle pulses in gas-phase…
THz time-domain spectroscopy in transmission mode was applied to study dry and wet drawing inks. In specific, cochineal-, indigo- and iron-gall based inks have been investigated; some prepared following ancient recipes and others by using synthetic materials. The THz investigations have been realized on both pellet samples, made by dried inks blended with polyethylene powder, and layered inks, made by liquid deposition on polyethylene pellicles. We implemented an improved THz spectroscopic technique that enabled the measurement of the material optical parameters and thicknesses of the layered …
We investigated femtosecond laser ablation dynamics using THz time-domain spectroscopy. To clarify the breakdown dynamics of materials, we focused on the motion of charged particles and measured the terahertz waves emitted during laser ablation. We revealed that the Coulomb force dominated the ablation process. Furthermore, comparisons of the experimental results with theoretical models showed that material breakdown occurs within a few hundred femtoseconds. Our experimental results indicate that electrostatic ablation is the most likely ablation mechanism for metals.
Dual THz comb spectroscopy has the potential to be used as universal THz spectroscopy with high spectral resolution, high spectral accuracy, and broad spectral coverage; however, the requirement for dual stabilized femtosecond lasers hampers its versatility due to the bulky size, high complexity, and high cost. We here report the first demonstration of dual THz comb spectroscopy using a single free-running fibre laser. By tuning the cavity-loss-dependent gain profile with an intracavity Lyot filter together with precise management of the cavity length and dispersion, dual-wavelength pulsed lig…
High resolution (900 Hz full-width at half maximum) frequency domain spectroscopy near 0.2Terahertz is achieved using an exact frequency spacing comb-source in the optical communications band, filtering and photo-mixing in a custom Uni-Travelling-Carrier Photodiode (UTC-PD) for THz signal generation and coherent down-conversion for detection. Via time domain modulation of one of the comb lines, a fully controllable spectrometer can be defined in software, and this principle is demonstrated for magnetic field-free readout of the electronuclear spectrum for the Ho ions in \lihof, a material ofte…
We present a rapid-scan, time-domain terahertz spectrometer employing femtosecond Er:fiber technology and an acousto-optic delay with attosecond precision, enabling scanning of terahertz transients over a 12.4 ps time window at a waveform refresh rate of 36 kHz, and a signal-to-noise ratio of $1.7 \times 10^5/\sqrt{\rm Hz}$. Our approach enables real-time monitoring of dynamic THz processes at unprecedented speeds, which we demonstrate through rapid 2D thickness mapping of a spinning teflon disc at a precision of $10\,\rm nm/\sqrt{\rm Hz}$. The compact, all-optical design ensures alignment-fre…
Terahertz (THz) emission spectroscopy is a powerful method that allows one to measure the ultrafast dynamics of polarization, current, or magnetization in a material based on THz emission from the material. However, the practical implementation of this method can be challenging, and can result in significant errors in the reconstruction of the quantity of interest. Here, we experimentally and theoretically demonstrate a rigorous method of signal reconstruction in THz emission spectroscopy, and describe the main experimental and theoretical sources of reconstruction error. We identify the linea…
An electro-optic dual comb system based on chirped-pulse waveforms is used to simultaneously acquire temporally magnified rapid passage signals and normal spectral line shapes from the back-transformation to the time domain. Multi-heterodyne THz wave generation and detection is performed with the difference frequency mixing of two free-running lasers. The method is used to obtain THz spectra of formic acid in the 10 cm-1 to 20 cm-1 (300 GHz to 600 GHz) region over a range of pressures. The method is widely applicable across other spectral regions for investigations of the transient dynamics an…
Dry and wet drawing materials were investigated by THz time-domain spectroscopy in transmission mode. Carbon-based and iron-gall inks have been studied, some prepared following ancient recipes and others using current synthetic materials; a commercial ink was studied as well. We measured the THz signals on thin film of liquid inks deposited on polyethylene pellicles, comparing the results with the thick pellets of dried inks blended with polyethylene powder. This study required the implementation of a new experimental method and data analysis procedure able to provide a reliable extraction of …
In THz reflection spectroscopy the complex permittivity of an opaque medium is determined on the basis of the amplitude and of the phase of the reflected wave. There is usually a problem of phase error due to misplacement of the reference sample. Such experimental error brings inconsistency between phase and amplitude invoked by the causality principle. We propose a rigorous method to solve this relevant experimental problem by using an optimization method based upon singly subtractive Kramers-Kronig relations. The applicability of the method is demonstrated for measured data on an n-type undo…
Strong-field mid-infrared pump--terahertz (THz) probe spectroscopy has been proven as a powerful tool for light control of different orders in strongly correlated materials. We report the construction of an ultrafast broadband infrared pump--THz probe system in reflection geometry. A two-output optical parametric amplifier is used for generating mid-infrared pulses with GaSe as the nonlinear crystal. The setup is capable of pumping bulk materials at wavelengths ranging from 1.2 $μ$m to 15 $μ$m and beyond, and detecting the subtle, transient photoinduced changes in the reflected electric field …
Broadband terahertz comb with sub-Hz comb linewidth
Jinan Institute of Quantum Technology（济南量子技术研究院）；Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences（中国科学院上海微系统与信息研究所）
The achievable instrument sensitivity is a critical parameter for the continued development of THz applications. Techniques such as Cavity-Enhanced Techniques and Cavity Ring Down Spectroscopy have not yet been employed at THz frequency due to the difficulties to construct a high finesse Fabry-Pérot cavity. Here, we describe such a THz resonator based on a low-loss oversized corrugated waveguide with highly reflective photonic mirrors obtaining a finesse above 3000 around 620 GHz. These components enable a Fabry-Perot THz Absorption Spectrometer with an equivalent interaction length of one kil…
We demonstrate terahertz (THz) imaging and spectroscopy of a 15x15-mm^2 single-layer graphene film on Si using broadband THz pulses. The THz images clearly map out the THz carrier dynamics of the graphene-on-Si sample, allowing us to measure sheet conductivity with sub-mm resolution without fabricating electrodes. The THz carrier dynamics are dominated by intraband transitions and the THz-induced electron motion is characterized by a flat spectral response. A theoretical analysis based on the Fresnel coefficients for a metallic thin film shows that the local sheet conductivity varies across th…
Max Planck Institute for the Structure and Dynamics of Matter（马克斯·普朗克物质与结构动态研究所）；Center for Free-Electron Laser Science (CFEL)（自由电子激光科学中心）；Max Planck Institute for the Physics of Complex Systems（马克斯·普朗克复杂系统物理研究所）；Department of Physics, Columbia University（哥伦比亚大学物理系）
We report the first measurements of the $c$-axis Josephson Plasma Resonance (JPR) in Tl$_2$Ba$_2$CaCu$_2$O$_8$ as a function of temperature with and without a $c$-axis magnetic field using terahertz time-domain spectroscopy in transmission. The JPR is sensitive to the alignment of pancake vortices along the $c$-axis, and is observed to decrease when applying a magnetic field as expected.
We report on the group delay observed in continuous-wave terahertz spectroscopy based on photomixing with phase-sensitive homodyne detection. We discuss the different contributions of the experimental setup to the phase difference Δϕ(ν) between transmitter arm and receiver arm. A simple model based on three contributions yields a quantitative description of the overall behavior of Δϕ(ν). Firstly, the optical path-length difference gives rise to a term linear in frequency. Secondly, the ultra-wideband log-spiral antennae effectively radiate and receive in a frequency-dependent active region, wh…
Free space delay lines provide pulses of variable time spacing for optical experiments such as pump-probe spectroscopy and coherent quantum control, including spin and photon echo techniques. However, in the terahertz (THz) region of the spectrum, beam divergence due to diffraction limits the useful length of traditional free space delay lines. We present a novel double-folded variable delay line for light in the frequency range 0.24-1.2 THz, which incorporates a symmetric arrangement of lenses whose spacing can be adjusted to compensate for diffraction at each delay. Scalable for use in other…
The effect of terahertz (THz) pulse generation has revolutionized broadband coherent spectroscopy and imaging at THz frequencies. However, THz pulses typically lack spatial structure, whereas structured beams are becoming essential for advanced spectroscopy applications. Non-linear optical metasurfaces with nanoscale THz emitters can provide a solution by defining the beam structure at the generation stage. We develop a non-linear InAs metasurface consisting of nanoscale optical resonators for simultaneous generation and structuring of THz beams. We find that THz pulse generation in the resona…
Mode-resolved dual-comb spectroscopy (DCS) is an emerging spectroscopic tool with the potential to simultaneously achieve a broad spectral coverage and ultrahigh spectral resolution in terahertz (THz) spectroscopy. However, the need for two independently stabilized ultrafast lasers significantly hampers the potential application of DCS techniques. In this article, we demonstrate mode-resolved DCS in the THz region based on a free-running single-cavity dual-comb fiber laser with adaptive sampling. Low-pressure spectroscopy of acetonitrile gas with absorption features approaching the Doppler lim…
Intersubband (ISB) transitions in semiconductor multi-quantum well (MQW) structures are promising candidates for the development of saturable absorbers at terahertz (THz) frequencies. Here, we exploit amplitude and phase-resolved two-dimensional (2D) THz spectroscopy on the sub-cycle time scale to observe directly the saturation dynamics and coherent control of ISB transitions in a metal-insulator MQW structure. Clear signatures of incoherent pump-probe and coherent four-wave mixing signals are recorded as a function of the peak electric field of the single-cycle THz pulses. All nonlinear sign…
We present a modified $8f$ geometry for time domain terahertz (THz) spectroscopy (TDTS) experiments. We show, through simulations and data, that a simple rearranging of the off-axis parabolic mirrors, which are typically used to focus and direct THz radiation in TDTS experiments, results in a nearly 40% reduction in the THz focal spot diameter. This effect stems from significant reduction of the principle optical aberrations which are enhanced in the conventional $8f$ geometry but partially compensated in the modified $8f$ experimental setup. We compare data from our home-built TDTS spectromet…
Subwavelength metallic resonators provide a route to achieving strong light-matter coupling by means of tight confinement of resonant electromagnetic fields. Investigation of such resonators however often presents experimental difficulties, particularly at terahertz (THz) frequencies. A single subwavelength resonator weakly interacts with THz beams, making it difficult to probe it using far-field methods; whereas arrays of resonators exhibit inter-resonator coupling, which affects the resonator spectral signature and field confinement. Here, traditional far-field THz spectroscopy is systematic…
Phase-stable electromagnetic pulses in the THz frequency range offer several unique capabilities in time-resolved spectroscopy. However, the diversity of their application is limited by the covered spectral bandwidth. In particular, the upper frequency limit of photoconductive emitters - the most widespread technique in THz spectroscopy - reaches only up to 7 THz in regular transmission mode due to the absorption by infrared-active optical phonons. Here, we present ultra-broadband (extending up to 70 THz) THz emission from Au implanted Ge emitter which is compatible with a fibre laser operatin…
Backscattering Raman spectroscopic investigations were performed on an yttrium-iron garnet single crystal using linearly and circularly polarized light. A terahertz (THz) magnon of the Kaplan-Kittel (KK) exchange resonance was discovered, which had been regarded as unobservable via optical methods. The KK exchange resonance had a 7.8-THz frequency at 80 K, and the polarization selection rule led to an antisymmetric Raman tensor of the $A_{2}$ mode. Moreover, the assignment of all the Raman-active phonon modes, $3A_{1g}$, $8E_{g}$, and $14T_{2g}$, was proposed. This study will stimulate further…
By using two mutually phase-locked optical frequency combs with slightly different repetition rates, we demonstrate asynchronous optical-sampling terahertz time-domain spectroscopy (ASOPS THz-TDS) without using any trigger signals or optical delay lines. Due to a tight stabilization of the repetition frequencies, it was possible to accumulate the data over 48 minutes in a triggerless manner without signal degradation. The fractional frequency stability of the measured terahertz signal is evaluated to be $\sim$8.0$\times$10$^{- 17}$ after 730 s. The frequency accuracy of the obtained terahertz …
We report on the first experimental observation of a very strong nonlinear response in crystalline quartz in the terahertz (THz) frequency region through THz time-domain spectroscopy (THz-TDS). Theoretical modelling is presented and predicts a Kerr coefficient n2 equal to 5.17*10^-14 m^2 W^-1. The time-domain analysis of the measured data shows that with increasing of the THz peak amplitude, the pulse experiences a larger time delay in the sample. As the THz amplitude increases to values higher than 110 kV cm^-1, the growth rate of the delay decreases, indicating a saturation process. The valu…
A new difference-frequency method based on electro-optic phase modulators and two free-running lasers is reported to perform THz dual-comb spectroscopy.
Terahertz (THz) Time domain spectroscopy (THz-TDS) is a broadband spectroscopic technique spreading its uses in multiple fields: in science from material science to biology, in industry where it measures the thickness of a paint layer during the painting operation. Using such practical commercial apparatus with broad spectrum for gas spectroscopy could be a major asset for air quality monitoring and tracking of atmospheric composition. However, gas spectroscopy needs high resolution and the usual approach in THz-TDS, where the recorded time trace is Fourier transform, suffers from resolution l…
In this paper, we report on an approach for shaping the spectra of THz pulse generation in photoconductive antennas (PCAs) by frequency-dependent impedance modulation. We introduce a theoretical model describing the THz pulse generation in PCAs and accounting for impedances of the photoconductor and of the antenna. In order to showcase an impact of frequency-dependent impedance modulation on the spectra of THz pulse generation, we applied this model to simulating broadband PCAs with log-spiral topology. Finally, we fabricated two different log-spiral PCAs and characterized them experimentally …
Coherent continuous wave (CW) terahertz spectroscopy is an extremely valuable technique that allows for the interrogation of systems that exhibit narrow resonances in the terahertz (THz) frequency range, such as high-quality (high-Q) THz whispering-gallery mode resonators. Unfortunately, common implementations are dramatically impaired by deficiencies in the used data analysis schemes. Here, we show that the physics of the problem presents an elegant solution whose full potential has remained overlooked until now. We argue that, thanks to the causality of physical systems, Hilbert transformati…
We report on the nonlinear spectroscopy of water vapor at THz frequencies. Atmospheric water vapor has a rich spectrum with several strong resonances at frequencies below 3 THz, falling within the range of operation of most existing THz sources. We observe an extremely large nonlinear response to THz radiation at the positions of these resonances. Using the optical Kerr model for the nonlinear response, we estimate a minimum nonlinear refractive index of the order of 10^2 m^2/W. Our results provide insight into the energy levels of the water molecule and give a more accurate picture of its res…
Phase-locked ultrashort pulses in the rich terahertz (THz) spectral range have provided key insights into phenomena as diverse as quantum confinement, first-order phase transitions, high-temperature superconductivity, and carrier transport in nanomaterials. Ultrabroadband electro-optic sampling of few-cycle field transients can even reveal novel dynamics that occur faster than a single oscillation cycle of light. However, conventional THz spectroscopy is intrinsically restricted to ensemble measurements by the diffraction limit. As a result, it measures dielectric functions averaged over the s…
Recent years have seen an explosive research and development of nanoplasmonics in the visible and near-infrared (near-ir) frequency regions. One of the most fundamental effects in nanoplasmonics is nano-concentration of optical energy. Plasmonic nanofocusing has been predicted and experimentally achieved. It will be very beneficial for the fundamental science, engineering, environmental, and defense applications to be able to nano-concentrate terahertz radiation (frequency 1 - 10 THz or vacuum wavelength 300 - 30 microns). This will allow for the nanoscale spatial resolution for THz imaging an…
We use the terahertz (THz) emission spectroscopy to study femtosecond photocurrent dynamics in the prototypical 2D semiconductor, transition metal dichalcogenide MoSe$_2$. We identify several distinct mechanisms producing THz radiation in response to an ultrashort ($30\,$fs) optical excitation in a bilayer (BL) and a multilayer (ML) sample. In the ML, the THz radiation is generated at a picosecond timescale by out-of-plane currents due to the drift of photoexcited charge carriers in the surface electric field. The BL emission is generated by an in-plane shift current. Finally, we observe oscil…
