Near-infrared two-photon excited photoluminescence from Yb3+-doped CsPbClxBr3-x perovskite nanocrystals embedded into amphiphilic silica microspheres.

Nonlinear absorption of metal-halide perovskite nanocrystals (NCs) makes them an ideal candidate for applications which require multiphoton-excited photoluminescence. By doping perovskite NCs with lanthanides, their emission can be extended into the near-infrared (NIR) spectral region. We demonstrate how the combination of Yb3+ doping and bandgap engineering of cesium lead halide perovskite NCs performed by anion exchange (from Cl- to Br-) leads to efficient and tunable emitters that operate under two-photon excitation in the NIR spectral region. By optimizing the anion composition, Yb3+-doped CsPbClxBr3-x NCs exhibited high values of two-photon absorption cross-section reaching 2.3 × 105 GM, and displayed dual-band emission located both in the visible (407-493 nm) and NIR (985 nm). With a view of practical applications of bio-visualisation in the NIR spectral range, these NCs were embedded into silica microspheres which were further wrapped with amphiphilic polymer shells to ensure their water-compatibility. The resulting microspheres with embedded NCs could be easily dispersed in both toluene and water, while still exhibiting a dual-band emission in visible and NIR under both one- and two-photon excitation conditions.

Elimination of signal amplitude disturbance in ghost imaging using an auxiliary laser channel.

Ghost imaging can be used to detect objects in a nonstationary environment or in the presence of variable ambient light, making it attractive when conventional imaging methods are ineffective. However, the conventional ghost imaging algorithm is susceptible to temporal fluctuations in the detected signal. In this work, we propose a polarization-multiplexed auxiliary laser channel propagating along the same optical path with the main one. The signal in the auxiliary channel is used as a reference and allows the elimination of signal disturbance. A quantitative analysis and comparison of the proposed method's performance to the high-pass filtering method are demonstrated. For an illumination pattern refresh rate of 10 Hz, effective suppression of bucket signal fluctuations has been experimentally demonstrated. For a disturbance frequency from 1 Hz to 10 Hz, the auxiliary channel method demonstrated a ghost image Pearson correlation coefficient (PCC) of not less than 0.70, while the high-pass filtering method showed a PCC sharp drop from 0.65 to 0.02.

Engineering the Optical Properties of CsPbBr3 Nanoplatelets through Cd2+ Doping.

Lead halide perovskite nanoplatelets (NPls) attract significant attention due to their exceptional and tunable optical properties. Doping is a versatile strategy for modifying and improving the optical properties of colloidal nanostructures. However, the protocols for B-site doping have been rarely reported for 2D perovskite NPls. In this work, we investigated the post-synthetic treatment of CsPbBr3 NPls with different Cd2+ sources. We show that the interplay between Cd2+ precursor, NPl concentrations, and ligands determines the kinetics of the doping process. Optimization of the treatment allows for the boosting of linear and nonlinear optical properties of CsPbBr3 NPls via doping or/and surface passivation. At a moderate doping level, both the photoluminescence quantum yield and two-photon absorption cross section increase dramatically. The developed protocols of post-synthetic treatment with Cd2+ facilitate further utilization of perovskite NPls in nonlinear optics, photonics, and lightning.

Radiation shift from triple to quadruple frequency caused by the interaction of terahertz pulses with a nonlinear Kerr medium.

High-intensity optical radiation propagation in a transparent dielectric medium causes the phenomena of pulse self-action and radiation generation at triple frequencies due to the cubic nonlinearity of the medium. However, quadratic nonlinear effects usually outshine the cubic ones in anisotropic nonlinear crystals. In this work, we demonstrate that for certain experimental parameters the nonlinear effect of the third order can be stronger than the second order one in the MgO:[Formula: see text] crystal for terahertz frequency range. We experimentally and theoretically show that this effect can lead to the significant modification of the classical phenomenon of radiation generation at triple frequencies in the case when the pulse represents only one complete oscillation of the optical field. The experiment demonstrated that the phenomenon of generation of radiation at triple frequencies with respect to the frequency of the maximum spectral density in a nonlinear medium of the pulse disappears, and it is replaced by the generation of radiation at quadruple frequencies. The analysis confirms that this effect is based on the asymmetry and large width of the initial spectrum of such extremely short pulses in terms of the number of oscillations.

Improved One- and Multiple-Photon Excited Photoluminescence from Cd2+-Doped CsPbBr3 Perovskite NCs.

Metal halide perovskite nanocrystals (NCs) attract much attention for light-emitting applications due to their exceptional optical properties. More recently, perovskite NCs have begun to be considered a promising material for nonlinear optical applications. Numerous strategies have recently been developed to improve the properties of metal halide perovskite NCs. Among them, B-site doping is one of the most promising ways to enhance their brightness and stability. However, there is a lack of study of the influence of B-site doping on the nonlinear optical properties of inorganic perovskite NCs. Here, we demonstrate that Cd2+ doping simultaneously improves both the linear (higher photoluminescence quantum yield, larger exciton binding energy, reduced trap states density, and faster radiative recombination) and nonlinear (higher two- and three-photon absorption cross-sections) optical properties of CsPbBr3 NCs. Cd2+ doping results in a two-photon absorption cross-section, reaching 2.6 × 106 Goeppert-Mayer (GM), which is among the highest reported for CsPbBr3 NCs.

Speckle patterns formed by broadband terahertz radiation and their applications for ghost imaging.

Speckle patterns can be very promising for many applications due to their unique properties. This paper presents the possibility of numerically and experimentally formation of speckle patterns using broadband THz radiation. Strong dependence of the statistical parameters of speckles, such as size and sharpness on the parameters of the diffuser are demonstrated: the correlation length and the mean square deviation of the phase surface inhomogeneity. As the surface correlation length is increasing, the speckle size also increases and its sharpness goes down. Alternatively, the magnification of the standard deviation of the surface height leads to the speckle size diminishing and growth of the speckle sharpness. The dimensions of the experimentally formed speckles correspond to the results of numerical simulation. The possibility of utilizing formed speckle patterns for the implementation of the ghost imaging technique has been demonstrated by methods of numerical modeling.

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.

Impact of laser-ionized liquid nonlinear characteristics on the efficiency of terahertz wave generation.

The generation of terahertz (THz) radiation during the propagation of subpicosecond pulses in liquid media is investigated using a theoretical model considering the relative contribution of Kerr and plasma nonlinearity. The dependences of the THz emission generation efficiency on the contribution of plasma nonlinearity with a fixed third-order nonlinearity value revealed the existence of weak and strong ionization modes. It is shown that the transition between these modes is determined by the ratio of plasma to Kerr nonlinearity coefficients and the pump energy. In the strong ionization mode and with the fixed contribution of plasma nonlinearity, the optical-to-THz conversion efficiency decreases with increasing Kerr nonlinearity due to the redistribution of the pump energy for the third-order effects. These results contribute to estimating the potential of liquid media as highly efficient THz sources.

Double-pump technique - one step closer towards efficient liquid-based THz sources.

By irradiating a water jet with double pulses, we demonstrate 4-fold higher THz wave generation than for a single pump pulse. The dependence of the enhanced THz signal on the temporal delay between two collinear pulses reveals the optimal time for launching signal pulse is near 2-4 ps, which corresponds to the time needed to create the complete pre-ionization state when sufficient electron density is already induced, and there is no plasma reflection of the pump pulse radiation. The increase in THz waves generation efficiency corresponds to the case of water jet excitation by the pulses with an optimal duration for a certain jet thickness, which is determined by the spatial pulse size. Using a theoretical model of the interaction of a high-intensity sub-picosecond pulse with an isotropic medium, we held a numerical simulation, which well describes the experimental results when using 3 ps value of population relaxation time. Thus, in this work, double pump method allows not only to increase the energy of the generated THz waves, but also to determine the characteristic excited state lifetime of liquid water. The optical-to-terahertz conversion efficiency in case of double pulse excitation of water column is of the order of 0.5⋅10 -3, which exceeds the typical values for THz waves generation during two-color filamentation in air and comparable with the achievable values due to the optical rectification in some crystals.

Transmission Properties of FeCl3-Intercalated Graphene and WS2 Thin Films for Terahertz Time-Domain Spectroscopy Applications.

Time-resolved terahertz spectroscopy has become a common method both for fundamental and applied studies focused on improving the quality of human life. However, the issue of finding materials applicable in these systems is still relevant. One of the appropriate solution is 2D materials. Here, we demonstrate the transmission properties of unique graphene-based structures with iron trichloride FeCl3 dopant on glass, sapphire and Kapton polyimide film substrates that previously were not investigated in the framework of the above-described problems in near infrared and THz ranges. We also show properties of a thin tungsten disulfide WS2 film fabricated from liquid crystal solutions transferred to a polyimide and polyethylene terephthalate substrates. The introduction of impurities, the selection of structural dimensions and the use of an appropriate substrate for modified 2D layered materials allow to control the transmission of samples for both the terahertz and infrared ranges, which can be used for creation of effective modulators and components for THz spectroscopy systems.

Flat liquid jet as a highly efficient source of terahertz radiation.

Polar liquids are strong absorbers of electromagnetic waves in the terahertz range, therefore, historically such liquids have not been considered as good candidates for terahertz sources. However, flowing liquid medium has explicit advantages, such as a higher damage threshold compared to solid-state sources and more efficient ionization process compared to gases. Here we report systematic study of efficient generation of terahertz radiation in flat liquid jets under sub-picosecond single-color optical excitation. We demonstrate how medium parameters such as molecular density, ionization energy and linear absorption contribute to the terahertz emission from the flat liquid jets. Our simulation and experimental measurements reveal that the terahertz energy has quasi-quadratic dependence on the optical excitation pulse energy. Moreover, the optimal pump pulse duration, which depends on the thickness of the jet is theoretically predicted and experimentally confirmed. The obtained optical-to-terahertz energy conversion efficiency is more than 0.05%. It is comparable to the commonly used optical rectification in most of electro-optical crystals and two-color air filamentation. These results, significantly advancing prior research, can be successfully applied to create a new alternative source of terahertz radiation.

Methodical inaccuracy of the Z-scan method for few-cycle terahertz pulses.

Modern sources of THz radiation generate high-intensity pulses allowing to observe nonlinear effects in this spectral range. To describe many nonlinear effects theoretically, it is necessary to know the nonlinear refractive index coefficient of optical materials. The work studies the applicability of the Z-scan method to determine the nonlinear refractive index coefficient in the THz frequency range for few-cycle pulses. We have discussed the correctness of the known Z-scan method for calculating the nonlinear refractive index coefficient for broadband THz radiation regarding number of cycles pulses have. We have demonstrated that the error in determining the nonlinear refractive index coefficient is always greater than 70% for true single-cycle pulses. With the increase in the number of oscillations to the measurement error shows strong dependence on the sample thickness and can vary from 2% to 90% regarding the parameters chosen. The fact that such radiation dispersion length is commensurate with the nonlinear length or even less than the latter results in the discrepancy mentioned. It is demonstrated that the decrease in the sample thickness leads to the reduction of the nonlinear refractive index coefficient determination error, and this error is <2% when the ratio between the sample thickness and the pulse longitudinal spatial size is ≤1. This can relate to the fact that the nonlinear effects in such a thin sample occur faster than the dispersion ones.

High Kerr nonlinearity of water in THz spectral range.

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.