The fundamental properties of water molecules, such as their molecular polarizability, have not yet been clarified. The hydrogen bond network is generally considered to play an important role in the thermodynamic properties of water. The terahertz (THz) Kerr effect technique, as a novel tool, is expected to be useful in exploring the low-frequency molecular dynamics of liquid water. Here, we use an intense and ultrabroadband THz pulse (peak electric field strength of 14.9 MV/cm, centre frequency of 3.9 THz, and bandwidth of 1–10 THz) to resonantly excite intermolecular modes of liquid water. Bipolar THz field-induced transient birefringence signals are observed in a free-flowing water film. We propose a hydrogen bond harmonic oscillator model associated with the dielectric susceptibility and combine it with the Lorentz dynamic equation to investigate the intermolecular structure and dynamics of liquid water. We mainly decompose the bipolar signals into a positive signal caused by hydrogen bond stretching vibration and a negative signal caused by hydrogen bond bending vibration, indicating that the polarizability perturbation of water presents competing contributions under bending and stretching conditions. A Kerr coefficient equation related to the intermolecular modes of water is established. The ultrafast intermolecular hydrogen bond dynamics of water revealed by an ultrabroadband THz pump pulse can provide further insights into the transient structure of liquid water corresponding to the pertinent modes.
We present a polarization sensitive terahertz detection method which is able to measure both orthogonal components of the terahertz electric field. It allows for the study of polarization dependent properties of materials. Azimuthal angle dependent transmittance in 0.2–2.6 THz frequency region for crystalline quartz is measured. Polarized terahertz transmission spectroscopy shows that birefringence can result in transmission minima. This work suggests that polarization sensitive detection is effective for removing fake absorption features caused by material birefringence.
We present terahertz reference-free phase imaging for identification of three explosive materials (HMX, RDX, and DNT. We propose a feature extraction technique to locate the spectral position of an unknown material’s absorption lines without using the reference signal. The samples are identified by their absorption peaks extracted from the negative first-order derivative of the sample signal phase divided by the frequency at each pixel. This technique will greatly benefit the future development of standoff distance, large size focal-plane terahertz imaging system.
Both solids and gases have been demonstrated as the materials for terahertz (THz) coherent detection. The gas-based coherent detection methods require a high-energy probe laser beam and the detection bandwidth is limited in the solid-based methods. Whether liquids can be used for THz detection and relax these problems has not yet been reported, which becomes a timely and interesting topic due to the recent observation of efficient THz wave generation in liquids. Here, we propose a THz coherent detection scheme based on liquid water. When a THz pulse and a fundamental laser beam are mixed on a free-flowing water film, a second harmonic (SH) beam is generated as the plasma is formed. Combining this THz-induced SH beam with a control SH beam, we successfully achieve the time-resolved waveform of the THz field with the frequency range of 0.1–18 THz. The required probe laser energy is as low as a few microjoules. The sensitivity of our scheme is 1 order of magnitude higher than that of the air-based method under comparable detection conditions. The scheme is sensitive to the THz polarization and the phase difference between the fundamental and control SH beams, which brings direct routes for optimization and polarization sensitive detection. Energy scaling and polarization properties of the THz-induced beam indicate that its generation can be attributed to a four-wave mixing process. This generation mechanism makes simple relationships among the probe laser, THz-induced SH, and THz field, favorable for robustness and flexibility of the detection device.
We report on terahertz (THz) generation from organic crystal N-benzyl-2-methyl-4-nitroaniline using a 1.15–1.55 μm near infrared pump. We observed a very large emission spectrum extending up to 7 THz, compared to 2.5 THz from a Ti:Sa pump in previous reports. The maximum optical-to-THz conversion efficiency in our experiment was 0.8% at a repetition rate of 1 kHz and without saturation, leading to a peak electric field of 1 GV/m. Our results show pronounced phase matching privilege for intense terahertz generation using a pump in the 1.15–1.25 μm range where high energy near infrared pump sources operate.
Coherent detection measures both the amplitude and phase of pulsed terahertz (THz) waves simultaneously, forming the foundation for THz time-domain spectroscopy (THz-TDS). This technique has become increasingly prominent in the fields of physics and materials science, allowing researchers to investigate the dynamic properties of various dielectric materials within the 0.1 to 10 THz frequency range, which is previously a challenging spectrum to access. This paper reviews recent advancements and the challenges faced by commonly used coherent detectors in THz-TDS. Our discussion emphasizes the potential for new discoveries in THz photonics and highlights the crucial role of coherent detection in the study of laser-matter interactions.