Air-biased-coherent-detection Research Articles

Measurement of the Dispersion of χ(3)$\chi ^{(3)}$ of SiO2${\rm SiO}_2$ and SiN Across the THz and Far‐Infrared Frequency Bands

AbstractTerahertz (THz) radiation sources based on two‐color femtosecond plasmas in air are becoming a mature technology for coherent spectroscopy and strong‐field physics across the extended THz range to several tens of THz. The field‐resolved detection of such THz transients relies on the third‐order nonlinearity of the detection medium. Here, a comparative measurement is demonstrated with air‐biased coherent detection (ABCD) and solid‐state biased detection (SSBCD) as a novel method to measure the dispersion of the magnitude and phase of the relevant third‐order nonlinearity for fused silica () and silicon nitride (SiN). Based on the development of the ultrabroadband SSBCD device with a detection bandwidth exceeding 30 THz, measurements are obtained across the 1–28 THz frequency range, hence covering the THz and far‐infrared. It is shown that the vibrational modes in and SiN in the THz range lead to strong resonant enhancement and dispersion of the nonlinearity. The SSBCD devices operate down to nanojoule (nJ) probe energy, and their is demonstrated by measuring the dielectric function of the Lorentzian line profile of transverse‐optical (TO) phonon mode at 9 THz in single‐crystal gallium arsenide (GaAs) and observing the weak phonon combination bands near the TO phonon.

Terahertz unipolar polarimetry by second-harmonic generation in air

Femtosecond laser-based terahertz (THz) sources have gained attention for their potential in various applications. As for any electromagnetic radiation, the wave polarization is a critical parameter, which needs to be under control in a wide class of those applications. However, characterizing the polarization of broadband THz pulses remains challenging due to their limited efficient optics. THz air-biased coherent detection has emerged as a promising candidate. The technique employed is heterodyne detection, utilizing second-harmonic generation induced by THz radiation in laser-induced air plasmas. This approach provides exceptional spectral bandwidth and an unbounded power detection limit, rendering it highly suitable for ultra-broadband and high-power THz sources. It enables a very efficient polarization measurement too. However, recent findings have revealed that the laser-induced air plasma generated in this technique can exhibit birefringence, which in turn adds systematic errors to the polarization-state determination. In this Letter, we propose a simplified approach that utilizes a weak probe beam and avoids high-voltage DC bias-fields. Unlike the terahertz (THz) air-biased coherent detection scheme, our approach yields a unipolar, intensity-proportional signal for second-harmonic generation. The experimental results reported in this Letter show the absence of induced birefringence in air and, hence, demonstrate accurate measurements of the polarization state of ultra-broadband THz pulses. Therefore, our technique may provide valuable results in applications where the polarization state, and not the full electric field waveform, is required for analysis or characterization. Finally, we discuss a possible application of our method to the emergent field of THz singular optics.

Remote terahertz spectroscopy from extended two-color plasma filaments: The ALTESSE 2 project

Coherent time-domain spectroscopy (TDS) using terahertz radiation is valuable for fundamental science, security, and medical applications. This study investigates the performance of air-biased coherent detection terahertz spectroscopy (ABCD-THz) when an extended plasma filament is created in the air over long distances. We report on the latest results obtained within the follow-up of the ALTESSE project (Bergé L. et al., EPL, 126 (2019) 24001) whose objective is to measure a set of spectral signatures characterizing suspicious materials over meter-long distances. As one of the most critical steps towards routinely applying this technique, we verified the feasibility of a remote THz time-domain spectroscopy by loosely focusing two-color ultrashort laser pulses at more than 3 meters from the laser source. The absorption spectra of amino acids and explosives analyzed in such a filamentation geometry are compared with those obtained using a standard ABCD scheme where the plasma is generated at much shorter distances of .

Air-photonics based terahertz source and detection system

Two-color air plasma-based broadband terahertz (THz) generation and subsequent air-biased coherent detection (ABCD) of the THz field are presented. Both source and detection systems are characterized experimentally and numerically, yielding excellent agreement of measured and simulated signals. We reveal that it is crucial to model the whole optical setup and include the various pump distortions, like temporal and spatial walk-off as well as ellipticity of polarization, in order to interpret the experimental measurements correctly. Moreover, it turns out that geometrical effects in the ABCD scheme shape the recorded THz spectra and need to be taken into account. We confirm that THz electric fields with peak amplitude in the MV/cm range and large spectral bandwidth are produced, allowing us to demonstrate THz spectroscopy with molecular samples.

Air-photonics terahertz platform with versatile micro-controller based interface and data acquisition.

We present a terahertz (THz) platform employing air plasma produced by an ultrashort two-color laser pulse as a broadband THz source and air biased coherent detection (ABCD) of the THz field. In contrast to previous studies, a simple peak detector connected to a micro-controller board acquires the ABCD-signal coming from the avalanche photodiode. Numerical simulations of the whole setup yield temporal and spectral profiles of the terahertz electric field in both source and detection area. The latter ones are in excellent agreement with our measurements, confirming THz electric fields with peak amplitude in the MV/cm range. We further illustrate the capabilities of the platform by performing THz spectroscopy of water vapor and a polystyrene reference sample.

Gas-plasma-based generation of broadband terahertz radiation with 640 mW average power.

We present a high-power source of broadband terahertz (THz) radiation covering the whole THz spectral region (0.1-30 THz). The two-color gas plasma generation process is driven by a state-of-the-art ytterbium fiber chirped pulse amplification system based on coherent combination of 16 rod-type amplifiers. Prior to the THz generation, the pulses are spectrally broadened in a multipass cell and compressed to 37 fs with a pulse energy of 1.3 mJ at a repetition rate of 500 kHz. A gas-jet scheme has been employed for the THz generation, increasing the efficiency of the process to 0.1%. The air-biased coherent detection scheme is implemented to characterize the full bandwidth of the generated radiation. A THz average power of 640 mW is generated, which is the highest THz average power achieved to date. This makes this source suitable for a variety of applications, e.g., spectroscopy of strongly absorbing samples or driving nonlinear effects for the studies of material properties.

Investigation of aging characteristics in explosive using terahertz time-domain spectroscopy

The terahertz absorption spectrum of the five aging explosive samples (PETN, RDX, HMX, LLM-105 and TATB) was measured and calculated by Terahertz time-domain spectroscopy system (THz-TDS) and air-biased coherent detection system (ZAP-ABCD), respectively. In this paper, compared with the unaging explosive, each aging explosive sample’s terahertz time-domain spectra were obtained and the terahertz absorption spectra were calculated by using Fourier transform and Lambert’s law. The results show that there are several terahertz absorption peaks which were called “fingerprint spectra” for different aging explosive samples in the range of 0.3–6.0 THz spectrum. Meanwhile, the results also show that the locations of the characteristic absorption peaks are not the same. Moreover, the unaging and aging explosive samples have obviously different terahertz absorption spectra.

High dynamic range, hyper-terahertz detection with silicon photoconductors

The frequency response of ion implanted silicon photoconductive devices designed for coherent detection in time domain terahertz spectroscopy has been studied between 0.2 and 30 THz. Unlike devices using polar photoconductors or ones having polar substrates, which have a complicated response spectrum in the region of their reststrahlen bands, the response of silicon detectors fabricated on silicon substrates is relatively featureless. When used with amplified laser systems, the dynamic range of Si detectors is shown to be very similar to that of GaAs devices with the same geometry over a 20 THz range, superior to air-biased coherent detection (ABCD) at frequencies below ∼7 THz and comparable with both ABCD and electro-optic sampling in thin ZnTe crystals between 7 and 20 THz. Together with their ease of use and linear response in terahertz fields approaching 1 MV/cm, this suggests that Si photoconductors could be a competitive choice for sensitive detection in nonlinear hyper-terahertz spectroscopy.

Linearity of Air-Biased Coherent Detection for Terahertz Time-Domain Spectroscopy

The performance of air-biased coherent detection (ABCD) in a broadband two-color laser-induced air plasma system for terahertz time-domain spectroscopy (THz-TDS) has been investigated. Fundamental parameters of the ABCD detection, including signal-to-noise ratio (SNR), dynamic range (DR), and linearity of detection have been characterized. Moreover, the performance of a photomultiplier tube (PMT) and an avalanche photodiode (APD) as photodetector in the ABCD have been compared. We have observed nonlinear behavior of PMT detector, which leads to artificial gain factor in TDS spectroscopy. The APD turns out to have superior linearity and three times higher dynamic compared to the PMT.

Polarization-dependent study of THz air-biased coherent detection.

We present an investigation of the polarization dependence of THz air-biased coherent detection (ABCD) on the polarization directions of fundamental waves. The intensity, ellipticity, and polarization angle of the THz-field-induced second-harmonic are affected by the air plasma birefringence and can be predicted by cross-phase modulation theory. Due to the plasma birefringence, the polarization state of THz waves cannot be determined by the polarization state of the second harmonic with the traditional polarization measurement method. It would be inaccurate to measure arbitrary THz-wave polarization in a single scan with THz ABCD when the birefringence effect is significant.

Metamaterial composite bandpass filter with an ultra-broadband rejection bandwidth of up to 240 terahertz

We present a metamaterial, consisting of a cross structure and a metal mesh filter, that forms a composite with greater functional bandwidth than any terahertz (THz) metamaterial to date. Metamaterials traditionally have a narrow usable bandwidth that is much smaller than common THz sources, such as photoconductive antennas and difference frequency generation. The composite structure shown here expands the usable bandwidth to exceed that of current THz sources. To highlight the applicability of this combination, we demonstrate a series of bandpass filters with only a single pass band, with a central frequency (f0) that is scalable from 0.86–8.51 THz, that highly extinguishes other frequencies up to >240 THz. The performance of these filters is demonstrated in experiment, using both air biased coherent detection and a Fourier transform infrared spectrometer (FTIR), as well as in simulation. We present equations—and discuss their scaling laws—which detail the f0 and full width at half max (Δf) of the pass band, as well as the required geometric dimensions for their fabrication using standard UV photolithography and easily achievable fabrication linewidths. With these equations, the geometric parameters and Δf for a desired frequency can be quickly calculated. Using these bandpass filters as a proof of principle, we believe that this metamaterial composite provides the key for ultra-broadband metamaterial design.

Investigation of ultra-broadband terahertz time-domain spectroscopy with terahertz wave gas photonics

Recently, air plasma, produced by focusing an intense laser beam to ionize atoms or molecules, has been demonstrated to be a promising source of broadband terahertz waves. However, simultaneous broadband and coherent detection of such broadband terahertz waves is still challenging. Electro-optical sampling and photoconductive antennas are the typical approaches for terahertz wave detection. The bandwidth of these detection methods is limited by the phonon resonance or carrier’s lifetime. Unlike solid-state detectors, gaseous sensors have several unique features, such as no phonon resonance, less dispersion, no Fabry-Perot effect, and a continuous renewable nature. The aim of this article is to review the development of a broadband terahertz time-domain spectrometer, which has both a gaseous emitter and sensor mainly based on author’s recent investigation. This spectrometer features high efficiency, perceptive sensitivity, broad bandwidth, adequate signal-to-noise ratio, sufficient dynamic range, and controllable polarization. The detection of terahertz waves with ambient air has been realized through a third order nonlinear optical process: detecting the second harmonic photon that is produced by mixing one terahertz photon with two fundamental photons. In this review, a systematic investigation of the mechanism of broadband terahertz wave detection was presented first. The dependence of the detection efficiency on probe pulse energy, bias field strength, gas pressure and third order nonlinear susceptibility of gases were experimentally demonstrated with selected gases. Detailed discussions of phase matching and Gouy phase shift were presented by considering the focused condition of Gaussian beams. Furthermore, the bandwidth dependence on probe pulse duration was also demonstrated. Over 240 times enhancement of dynamic range had been accomplished with n-hexane vapor compared to conventional air sensor. Moreover, with sub-20 fs laser pulses delivered from a hollow fiber pulse compressor, an ultra-broad spectrum covering from 0.3 to 70 THz was also showed. In addition, a balanced detection scheme using a polarization dependent geometry was developed by author to improve signal-to-noise ratio and dynamic range of conventional terahertz air-biased-coherent-detection (ABCD) systems. Utilizing the tensor property of third order nonlinear susceptibility, second harmonic pulses with two orthogonal polarizations was detected by two separated photomultiplier tubes (PMTs). The differential signal from these two PMTs offers a realistic method to reduce correlated laser fluctuation, which circumvents signal-to-noise ratio and dynamic range of conventional terahertz ABCD systems. A factor of two improvement of signal-to-noise ratio was experimentally demonstrated. This paper also introduces a unique approach to directly produce a broadband elliptically polarized terahertz wave from laser-induced plasma with a pair of double helix electrodes. The theoretical and experimental results demonstrated that velocity mismatch between excitation laser pulses and generated terahertz waves plays a key role in the properties of the elliptically polarized terahertz waves and confirmed that the far-field terahertz emission pattern is associated with a coherent process. The results give insight into the important influence of propagation effects on terahertz wave polarization control and complete the mechanism of terahertz wave generation from laserinduced plasma. This review provides a critical understanding of broadband terahertz time-domain spectroscopy (THz-TDS) and introduces further guidance for scientific applications of terahertz wave gas photonics.

Ultrabroadband terahertz spectroscopy of a liquid crystal

Liquid crystals (LCs) are becoming increasingly important for applications in the terahertz frequency range. A detailed understanding of the spectroscopic parameters of these materials over a broad frequency range is crucial in order to design customized LC mixtures for improved performance. We present the frequency dependent index of refraction and the absorption coefficients of the nematic liquid crystal 5CB over a frequency range from 0.3 THz to 15 THz using a dispersion-free THz time-domain spectrometer system based on two-color plasma generation and air biased coherent detection (ABCD). We show that the spectra are dominated by multiple strong spectral features mainly at frequencies above 4 THz, originating from intramolecular vibrational modes of the weakly LC molecules.

Terahertz field enhancement to the MV/cm regime in a tapered parallel plate waveguide

We investigate field enhancement properties of a tapered parallel plate waveguide for ultrashort terahertz (THz) pulses. We use two independent methods, air biased coherent detection inside the waveguide and free-space electro-optic sampling, respectively, which enables a calibrated, quantitative measurement of the field strength at the output of the waveguide. Field enhancement factors greater than 20 are demonstrated and record-high field strengths of > 1.4 MV/cm are reached. We find an excellent agreement between the two independent methods of field measurement and a numerical 3D full-vectorial time-domain simulations.

Analysis of Gouy phase shift for optimizing terahertz air-biased-coherent-detection

Terahertz (THz) air-biased-coherent-detection (ABCD) uses a local oscillator to enhance THz-wave detection sensitivity by mixing an optical field, a THz field, and a biased electric field (local oscillator) in air. The width of the electrodes providing the local oscillator, the longitudinal distribution of the optical and THz waves, both play important roles in the overall detection sensitivity. By analyzing the effect of the Gouy phase shift on the electric field distribution at the mixing location, we determine the optimal electrode width and observe an enhancement of the detection efficiency by a factor of two relative to the traditional THz-ABCD system using thin-wire electrodes.

Study of broadband THz time-domain spectroscopy at different relative humidity levels

Two detection techniques of broadband terahertz (THz) time-domain spectroscopy-THz air-biased coherent detection (THz-ABCD; from 0.3 to 14 THz) and electro-optical (EO) detection (from 0.3 to 7 THz) - are both performed at several different relative humidity levels. The THz power exponentially decays with the increase in relative humidity. The dynamic range of the main pulse in the time domain linearly decreases as the relative humidity increases from 0% to 40%, and linear fittings show that the slopes are -0.017 and -0.019 for THz-ABCD and EO detection, respectively. Because of the multiple reflections caused by the crystal in the common EO detection, THz-ABCD has better spectral resolution (17 GHz) than that of EO detection (170 GHz). The spectrum of water vapor absorption measured by THz-ABCD is also compared with that measured by the Fourier transform infrared spectroscopy (FTIR).

Design and performance of reflective terahertz air-biased-coherent-detection for time-domain spectroscopy

When a sample being tested is optically opaque or has a high absorption coefficient, a reflective measurement is often more suitable than a transmission measurement. We report the design and evaluation of a reflective terahertz time-domain spectroscopy (R-THz-TDS), using air as THz wave emitter and sensor, together with air-biased-coherent-detection (ABCD) method for the first time. With an 85 fs pulse amplified laser, we demonstrate a usable bandwidth from 0.5 THz to 12 THz, together with a peak dynamic range (DR) better than 2000:1 and a peak THz electrical field greater than 30 kV/cm. With a 32 fs pulse amplified laser, the usable bandwidth is remarkably expanded to a continuous 35 THz. Several far-infrared optical properties in various samples are reported. Furthermore, the time-resolved optical pump-THz probe experiment is performed. Finally, the uniqueness and advantage of this spectrometer are comprehensively compared with traditional THz-TDS and Fourier transform infrared (FTIR) spectroscopy.

Broadband (0.3∼11THz) reflection spectroscopy using terahertz air photonics

AbstractPulsed THz wave spectroscopy using air as the THz wave emitter with the excitation of femtosecond laser provides intense (>100 kV/cm) and broadband THz waves (usable bandwidth from 0.3 to 11 THz). Using the air-biased-coherent-detection (ABCD) method, air can also coherently detect pulsed THz waves over a broadband spectrum. By utilizing these two technologies, we developed a prototype THz air photonics time-domain reflection spectrometer, and applied it on many materials in normal reflection geometry. Optical properties of CaCO3 crystals and several other samples in the THz range were studied. The system provided a signal-to-noise ratio (SNR) over 1000:1, with 0.1 cm−1 frequency resolution. The results acquired from both transmission and reflection measurements were then compared.