The values of the nonlinear refractive index coefficient for various materials in the terahertz frequency range exceed the ones in both visible and NIR ranges by several orders of magnitude. This allows to create nonlinear switches, modulators, systems requiring lower control energies in the terahertz frequency range. We report the direct measurement of the nonlinear refractive index coefficient of liquid water by using the Z-scan method with broadband pulsed THz beam. Our experimental result shows that nonlinear refractive index coefficient in water is positive and can be as large as 7×10⁻¹⁰ cm²/W in the THz frequency range, which exceeds the values for the visible and NIR ranges by 6 orders of magnitude. To estimate n₂, we use the theoretical model that takes into account ionic vibrational contribution to the third-order susceptibility. We show that the origins of the nonlinearity observed are the anharmonicity of molecular vibrations.

Black phosphorus (BP) in its monolayer form called phosphorene is thought of as a successor of graphene and is of great interest for (opto)electronic applications. A quantitative and scalable method for the synthesis of (mono-)few-layer phosphorene has been an outstanding challenge due to the process irreproducibility and environmental degradation capability of the BP. Here, we report a facile controlled electrochemical exfoliation method for the preparation of a few-layer phosphorene (FP) with nearly 100% yield. Our approach relies on the low-potential influence in anhydrous and oxygen-free low-boiling acetonitrile (AN) and N,N-dimethylformamide (DMF) using alkylammonium ions. Herein, intercalation of positive ions into BP interlayers occurred with a minimum potential of −2.95 V in DMF and −2.85 V in AN and the non-damaging and highly accurate electrochemical exfoliation lasted at −3.8 V. A variety of analytical methods have revealed that in particular DMF-based exfoliation results in high-quality phosphorene of 1–5 layers with good crystallinity and lateral sizes up to tens of micrometers. Moreover, assurance of the oxygen- and water-free environment allowed us to minimize the surface oxidation of BP and, consequently, exfoliated phosphorene. We pioneer an effective and reproducible printing transfer of electrochemically exfoliated phosphorene films onto various flexible and rigid substrates. The surfactant-free process of exfoliation allowed assembly and transfer of thin films based on FP. The phosphorene-based films characterized as direct gap semiconductors have a layer-number-dependent bandgap with a tuning range larger than that of other 2D materials. We show that on varying the films’ thickness, it is possible to modify their optical properties, which is a significant advantage for compact and switchable optoelectronic components.

The nonlinear response of liquids in the terahertz regime has recently attracted significant interest, even though very few measurements have been reported. Here, we report on our measurements based on a $z$-scan technique of the nonlinear refractive-index coefficient $n_2$ at terahertz frequencies for several liquids with noncentrosymmetric molecules, specifically, water, ethanol, and $\alpha$-pinene. We describe how the value of $n_2$ depends on the physical parameters of these molecules. The measured values of $n_2$ of the liquids in the terahertz region are as much as 6 orders of magnitude larger than their corresponding values in the visible or near-IR. Through a simple theoretical model, we confirm that the predominant source of this large third-order nonlinearity is the second-order perturbative component of the vibrational response of these molecules, which have resonances in the mid-IR.

Energy, pulse duration, and frequency of the spectral maximum are important characteristics of pulsed terahertz radiation. The unipolarity of radiation is another characteristic that is paid less attention to. This paper demonstrates possible ways how to determine the presence of unipolarity in the radiation of pulsed terahertz sources. The first approach is based on integrating the time dependence of the field strength in the far zone obtained experimentally. The second approach uses radio-technical equipment by means of recording low-frequency components of pulses, which exist in the unipolar terahertz radiation. The results of experiments are presented with recording the unipolar component of THz pulses by both methods. The existence of unipolarity is shown for pulses from some types of terahertz radiation sources. Estimations are made for the electric area and the degree of unipolarity of the pulsed radiation for the first time.

Our recent theoretical studies of generation of ultrashort pulses based on collective spontaneous emission from a thin resonant medium layer excited by a pair of high-frequency (compared to the transition frequency of the medium) pulses are reviewed. The source of generated radiation is a resonant polarization pulse in the medium (“stopped polarization pulse”), which is excited and switched off by a pair of light pump pulses. This method allows obtaining attosecond pulses in the optical and ultraviolet ranges, as well as femtosecond terahertz pulses. The effect of the superradiance in generation is discussed. The use of coherent and collective processes makes it possible to achieve a high efficiency of the generation of terahertz radiation. The proposed method is an alternative method of obtaining ultrashort pulses compared to the currently well-developed methods such as the high-harmonic generation method.

The first observation of liquid crystalline dispersions of liquid phase-exfoliated tungsten disulfide flakes is reported in a range of organic solvents. The liquid crystals demonstrate significant birefringence as observed in the linear and circular dichroism measurements respectively. In particular, linear dichroism is observed throughout the visible range while broad-band circular dichroism can be observed in the range from 500–800 nm. Under an applied magnetic field of ±1.5 T the circular dichroism can be switched ON/OFF, while the wavelength range for switching can be tuned from large to narrow range by the proper selection of the host solvent. In combination with photoluminescence capabilities of WS₂, this opens a pathway to a wide variety of applications, such as deposition of highly uniform films over large areas for photovoltaic and terahertz devices.