Enhanced XUV harmonics generated in mixed noble gases using three-color laser fields.

High repetition coherent extreme ultraviolet (XUV) harmonics offer a powerful tool for investigating electron dynamics and understanding the underlying physics in a wide range of systems. We demonstrate the utilization of combined three-color (ω+2ω+3ω) laser fields in the generation of coherent extreme ultraviolet radiation in mixed noble gases. The three-color field results from the combination of fundamental, second-, and third-order harmonics of the near-infrared laser pulses in the nonlinear crystals. Different noble gases were selected as gas targets based on their ionization potentials, which are important parameters for generating higher cut-offs and intensities for the XUV harmonics. Enhanced XUV harmonic intensities were observed in the mixture of He + Kr gases when using three-color laser fields, compared to harmonics generated in the He + Kr mixture under a single-color pump. On the other hand, suppression of XUV harmonic intensity was observed in the mixture of He + Xe under the three-color pump due to the highest ionization level for these two mixed gases at similar laser conditions. Strong harmonic yields in the range of 25 to 80 eV of photon energy were observed.

Outstanding nonlinear optical properties of all-inorganic perovskite CsPbX3 (X=Cl, Br, I) precursor solutions and polycrystalline films.

In this work, we systematically explore the third-order nonlinear optical properties of all-inorganic CsPbX3 (X = Cl, Br, I) perovskite precursor solutions and thin films using femtosecond and nanosecond laser pulses. We show that these samples possess strong two-photon absorption (TPA) and reverse saturable absorption (RSA), which depend on the excitation wavelength. The obtained nonlinear absorption and refraction coefficients for precursor solutions are followed by the relation CsPbCl3 > CsPbBr3 > CsPbI3 for the 800 and 1,064 nm excitation wavelengths, whereas this relation became reverse in the case of 355 and 400 nm laser pulses. It was shown that CsPbCl3 thin film possesses RSA at 400 nm, CsPbCI3 shows RSA+ saturable absorption (SA), and CsPbBr3 demonstrates SA + RSA. In addition, at 800 nm excitation, the CsPbBr3 thin films show SA + RSA at low peak intensity, and the absorption becomes reverse (TPA+SA) with a further increase in the input laser intensity. The suitability of nonlinear absorption depends on the band gap of the thin films with respect to the pumping photon energy. Our studies demonstrate that these perovskites can be used as the excellent materials for the all-optical signal processing.

High-order harmonics generation in Cd and Pd laser-induced plasmas.

We demonstrate the generation of high-order harmonics of laser pulses in palladium and cadmium plasmas. We adjusted the wavelength of driving pulses to investigate the resonance enhancement in different ranges of extreme ultraviolet region. The summation of incommensurate waves during the two-color pump of Pd and Cd plasmas allowed the generation of a broader range of harmonics. The theoretical aspects of the two-color pump of the laser-induced plasma are discussed.

Variation of Nonlinear Refraction and Three-Photon Absorption of Indium-Tin Oxide Quantum Dot Thin Films and Solutions in Near Infrared Range.

We characterize the nonlinear optical properties of indium-tin oxide (ITO) quantum dots (QDs) in the IR range using the Z-scan method. We present results of three-photon absorption (3PA), third harmonic generation (3HG), and Kerr-effect-induced nonlinear refraction in ITO QDs. Z-scan measurements were carried out for the QDs solution, while 3HG was demonstrated using QD thin films. The Kerr-induced nonlinear refractive index was analyzed along the 800-950 nm range showing an increase in this parameter from -6.7 × 10-18 to -1.5 × 10-17 m2 W-1. At longer wavelengths (1000-1100 nm), the higher-order effects started to contribute to a nonlinear refractive index. The 3PA coefficient at 950 nm was measured to be 1.42 × 10-25 m3/W2. We discuss the peculiarities in the wavelength-dependent variation of the coefficient of nonlinear absorption responsible for 3PA in the range of 800-1150 nm. Third harmonic generation was analyzed in the 1200-1550 nm spectral range. The absolute value of 3HG conversion efficiency in the 150 nm thick film at the wavelength of laser radiation (1350 nm) was estimated to be ~10-5.

High-order harmonics enhancement in laser-induced plasma.

The methods of enhancement of the strong high-order harmonics of femtosecond pulses in laser-induced plasma are demonstrated. It comprises the application of the four techniques allowing the enhancement of harmonics in different spectral ranges. Among them are the selection of targets for ablation to create the conditions for resonance enhancement of single harmonic, formation of the quasi-phase-matching of a spectrally tunable group of harmonics, application of the two-color pump of plasma, and the formation of nanoparticles-contained plasmas. The number of generated coherent XUV photons increased in the region of single resonantly enhanced harmonic (62 nm) and the shorter-wavelength region (30-50 nm). The above techniques of harmonics enhancement allowed a significant (up to 50 times) growth in a whole harmonic yield in the case of indium plasma. We discuss the reasons preventing the joint implementation of the four methods of harmonics enhancement in the same spectral region.

Quantum-Dot-Induced Modification of Surface Functionalization for Active Applications of Whispering Gallery Mode Resonators.

Quantum dots can modify the properties of the whispering gallery mode resonators (WGMRs) used in various potential applications. A deposition of a suitable nanomaterial for the surface functionalization of WGMRs allows for the achievement of high quality (Q) factors. Here, we show that the WGMR surface can be functionalized using quantum dots. We demonstrate that WGMRs covered with thin layers of HgS and PbS quantum dots are suitable for third-harmonic generation due to the high Q factor of the developed microresonators, thus significantly lowering the pumping power required for nonlinear optical interactions.

High-Order Harmonics Generation in MoS2 Transition Metal Dichalcogenides: Effect of Nickel and Carbon Nanotube Dopants.

The transition metal dichalcogenides have instigated a lot of interest as harmonic generators due to their exceptional nonlinear optical properties. Here, the molybdenum disulfide (MoS2) molecular structures with dopants being in a plasma state are used to demonstrate the generation of intense high-order harmonics. The MoS2 nanoflakes and nickel-doped MoS2 nanoflakes produced stronger harmonics with higher cut-offs compared with Mo bulk and MoS2 bulk. Conversely, the MoS2 with nickel nanoparticles and carbon nanotubes (MoS2-NiCNT) produced weaker coherent XUV emissions than other materials, which is attributed to the influence of phase mismatch. The influence of heating and driving pulse intensities on the harmonic yield and cut-off energies are investigated in MoS2 molecular structures. The enhanced coherent extreme ultraviolet emission at ~32 nm (38 eV) due to the 4p-4d resonant transitions is obtained from all aforementioned molecular structures, except for MoS2-NiCNT.

Quasi-phase-matching of resonance-enhanced high-order harmonics in laser plasmas.

The resonance-enhanced harmonics in laser-induced arsenic and selenium plasmas are studied at the quasi-phase-matching (QPM) conditions. We demonstrate that the enhancement of these harmonics was significantly smaller than the one of the neighboring harmonics. Though the enhancement factors of the harmonics in the vicinity of resonance-enhanced harmonics were in the range of 5× to 18×, the resonance-enhanced harmonics were almost unenhanced at QPM conditions. The most probable reason for such restriction in the enhancement of specific harmonics at the conditions of QPM was a stronger influence of free electrons on the phase-matching conditions of the resonance-enhanced single harmonic compared to the QPM-enhanced group of harmonics.

Harmonics Generation in the Laser-Induced Plasmas of Metal and Semiconductor Carbide Nanoparticles.

Carbon-containing plasma is an attractive medium for generation of harmonics of laser pulses in the extreme ultraviolet range. We ablate two metal carbide (B4C and Cr3C2) nanoparticles and silicon carbide (SiC) nanoparticles and generate harmonics after propagation of 35 fs pulses through the laser-induced plasmas. We analyze the spectra, spectral shifts, and splitting of harmonics from nanoparticles-contained plasmas, which demonstrate the chirp-related harmonic cut-off scaling. In addition, we present the simplified two-color pump model calculations of HHG based on the strong field approximation.

High-order harmonics generation in nanosecond-pulses-induced plasma containing Ni-doped CsPbBr3perovskite nanocrystals using chirp-free and chirped femtosecond pulses.

We demonstrate high-order harmonic generation in Ni-doped CsPbBr3perovskite nanocrystals ablated by nanosecond pulses using chirp-free 35 fs, and chirped 135 fs pulses in the case of single-color pump (800 nm) and a two-color pump (800 and 400 nm). We analyzed the spectral shift, cut-off, and intensity distribution of harmonics in the case of chirped drving pulses compared to chirp-free pulses. It is shown that the presence of Ni dopants and CsPbBr3plasma components improves the harmonics emission. Also, we measured the third-order nonlinear optical (NLO) properties of these nanocrystals using 800 nm, 60 fs, 1 kHz pulses. The variations of measured NLO parameters of CsPbBr3perovskite nanocrystals containing different concentrations of nickel correlate with variations of generated high-order harmonics from laser induced plasmas of studied nanocrystals in terms of harmonics intensity, cut-off, and spectral shift (in case of chirped driving pulses). The spectral shift of the harmonics generated from the Ni-doped CsPbBr3perovskite nanocrystals can be used to form tunable extreme ultraviolet sources.

Application of vector beams for enhanced high-order harmonics generation in laser-induced plasmas.

High-order harmonics driven by phase- and polarization-structured femtosecond pulses are unique sources of the extreme ultraviolet vortex and vector beams, which have various applications. Here, we report the generation of intense high-order harmonics during propagation of the polarization-structured vector beams (radially polarized beam, azimuthally polarized beam, and their superposition) through the laser-induced plasmas (In, C, CdS, Zns, Ag2S). Low-order harmonics became stronger with radially polarized and azimuthally polarized driving beams compared with the linearly polarized beams, which is explained on the basis of phase matching and specific properties of vector beams. Contrary to that, the resonance-enhanced harmonic generated in the indium plasma in the case of radially polarized and azimuthally polarized beams was twice weaker compared with the harmonic generated by the LP beam due to modification in the resonant transition selection rules leading to a decrease of the oscillator strength of ionic transitions. Harmonic cut-off and intensity in the case of superposition of the radially and azimuthally polarized beams were lesser compared with the cases of the individual (radially polarized and azimuthally polarized) beams.

Laser-Induced Molecular Plasma: A Medium for High-Order Harmonics Generation of Ultrashort Pulses.

I present a study of laser-induced plasmas (LIPs) produced on the surfaces of molecular targets to create optimal conditions for high-order harmonics generation during the propagation of femtosecond pulses through the LIP. The resonance enhancement of a harmonic, two-color pump of plasma, quasi-phase-matching and nanoparticle-induced growth of the harmonic yield are analyzed, which allows for the formation of sources of coherent extreme ultraviolet radiation based on molecular plasma formation.

High-order harmonics generation in the laser-induced lead-free perovskites-containing plasmas.

High-order harmonics generation in the laser-induced plasmas produced on the surfaces of lead-free perovskites is studied. We analyze the harmonics generation in (CH3NH3)2CuCl4 and (CH3NH3)2CuBr4 plasmas during their ablation by the femtosecond, picosecond, and nanosecond pulses. The modifications of the high-order harmonics spectra are studied using the -color pump scheme (800 nm and 400 nm, 40 fs pulses). The influence of the variations of laser chirp and pulse duration on the dynamics of high-order harmonics generation is examined. The spectral shift, chirp-related harmonic cutoff scaling, and the role of the pulse duration of converting and heating laser radiation are examined at different conditions of plasma formation and harmonic generation. The dependencies of the pulse duration and the fluence of heating pulses on the harmonic's blue shift are found. The effect of harmonics broadening and splitting on the two red- and blue-shifted components is demonstrated.

Nonlinear Reconstruction of Images from Patterns Generated by Deterministic or Random Optical Masks-Concepts and Review of Research.

Indirect-imaging methods involve at least two steps, namely optical recording and computational reconstruction. The optical-recording process uses an optical modulator that transforms the light from the object into a typical intensity distribution. This distribution is numerically processed to reconstruct the object's image corresponding to different spatial and spectral dimensions. There have been numerous optical-modulation functions and reconstruction methods developed in the past few years for different applications. In most cases, a compatible pair of the optical-modulation function and reconstruction method gives optimal performance. A new reconstruction method, termed nonlinear reconstruction (NLR), was developed in 2017 to reconstruct the object image in the case of optical-scattering modulators. Over the years, it has been revealed that the NLR can reconstruct an object's image modulated by an axicons, bifocal lenses and even exotic spiral diffractive elements, which generate deterministic optical fields. Apparently, NLR seems to be a universal reconstruction method for indirect imaging. In this review, the performance of NLR isinvestigated for many deterministic and stochastic optical fields. Simulation and experimental results for different cases are presented and discussed.

Investigation of Nonlinear Optical Processes in Mercury Sulfide Quantum Dots.

The authors report the third-harmonic generation, nonlinear refraction, and nonlinear absorption in HgS quantum dot (QD) suspensions and films using the nanosecond and femtosecond pulses. High conversion efficiency (7 × 10-4) towards the third harmonic (TH) of the 900-1700 nm, 150 fs laser in the thin (70 nm) films containing HgS QDs deposited on the glass substrates is obtained. The authors analyze spectral dependencies of the TH, nonlinear refractive indices, and nonlinear absorption coefficients of QDs in the 500-1700 nm range and discuss the relation between the TH process and the low-order nonlinear optical properties of these quantum dots.

Third-order optical nonlinearities of exfoliated Bi2Te3 nanoparticle films in UV, visible and near-infrared ranges measured by tunable femtosecond pulses.

We characterize the nonlinear optical properties of synthesized Bi2Te3 nanoparticle-contained thin films using the tunable femtosecond laser in the spectral range of 400-1000 nm. These nanoparticles possess a strong saturable absorption and positive nonlinear refraction (-6.8×10-5 cm W-1 in the case of 500 nm, 150 fs probe pulses, and 3×10-10 cm2 W-1 in the case of 400 nm, 150 fs probe pulses, respectively). The spectral, intensity, and temporal variation of saturable absorption and nonlinear refraction of the thin films containing exfoliated Bi2Te3 nanoparticles are discussed.

Nonlinear Absorption and Refraction of Picosecond and Femtosecond Pulses in HgTe Quantum Dot Films.

We report measurements of the saturated intensities, saturable absorption, and nonlinear refraction in 70-nm thick films containing 4 nm HgTe quantum dots. We demonstrate strong nonlinear refraction and saturable absorption in the thin films using tunable picosecond and femtosecond pulses. Studies were carried out using tunable laser pulses in the range of 400-1100 nm. A significant variation of the nonlinear refraction along this spectral range was demonstrated. The maximal values of the nonlinear absorption coefficients and nonlinear refractive indices determined within the studied wavelength range were -2.4 × 10-5 cm2 W-1 (in the case of 28 ps, 700 nm probe pulses) and -3 × 10-9 cm2 W-1 (in the case of 28 ps, 400 nm probe pulses), respectively. Our studies show that HgTe quantum dots can be used in different fields e.g., as efficient emitters of high-order harmonics of ultrashort laser pulses or as laser mode-lockers.

Analysis of laser plasma dynamics using the time resolved nonlinear optical response of ablated carbon nanocomposites mixed with epoxy resin.

Nonlinear optical properties of carbon nanostructures attract attention due to the unique response of these materials during interactions with ultrashort laser pulses. Here we probe the carbon nanocomposites mixed with epoxy resin in laser-induced plasmas using the high-order harmonics generation (HHG) method. We analyze the nanosecond pulses induced plasmas containing three carbon nanostructures (fullerenes, multiwalled carbon nanotubes and diamond nanoparticles) using 40 fs pulses propagating through these plasmas. HHG efficiencies in ablated graphite and nanocomposites are compared. We utilize two digitally synchronized (nanosecond and femtosecond) laser sources allowing for the HHG-based analysis of the evolution of different plasma plumes up to 10 µs delay from the beginning of ablation. The role of different carbon-containing nanocomposites is analyzed and the evidence for the presence of various nanomaterials in laser-induced plasma at the moment of propagation of the driving femtosecond pulses is demonstrated.

Nonlinear Optical Characterization of InP@ZnS Core-Shell Colloidal Quantum Dots Using 532 nm, 10 ns Pulses.

InP@ZnS core-shell colloidal quantum dots (CQDs) were synthesized and characterized using the z-scan technique. The nonlinear refraction and nonlinear absorption coefficients (γ = -2 × 10-12 cm2 W-1, ß = 4 × 10-8 cm W-1) of these CQDs were determined using 10 ns, 532 nm pulses. The saturable absorption (ß = -1.4 × 10-9 cm W-1, Isat = 3.7 × 108 W cm-2) in the 3.5 nm CQDs dominated at small intensities of the probe pulses (I ≤ 7 × 107 W cm-2) followed by reverse saturable absorption at higher laser intensities. We report the optical limiting studies using these CQDs showing the suppression of propagated nanosecond radiation in the intensity range of 8 × 107-2 × 109 W cm-2. The role of nonlinear scattering is considered using off-axis z-scan scheme, which demonstrated the insignificant role of this process along the whole range of used intensities of 532 nm pulses. We discuss the thermal nature of the negative nonlinear refraction in the studied species.

Synthesis and low-order optical nonlinearities of colloidal HgSe quantum dots in the visible and near infrared ranges.

We synthesize colloidal HgSe quantum dots and characterize their nonlinear refraction and nonlinear absorption using a Nd:YAG laser and its second harmonic. The 7.5 nm quantum dots were synthesized using the hot-injection method. The nonlinear absorption (ß = 9×10-7 cm W-1) and negative nonlinear refraction (γ = -5×10-12 cm2 W-1) coefficients of colloidal quantum dots were determined using the 10 ns, 532 nm laser radiation. The joint influence of above processes was realized at a higher intensity of probe pulses. In the case of 10 ns, 1064 nm radiation, only negative nonlinear refraction dominated during z-scans of these quantum dots. The studies of optical limiting using two laser sources demonstrated the effectiveness of this process at 532 nm. The role of nonlinear scattering is analyzed. We discuss the mechanisms responsible for the nonlinear refraction processes in colloidal HgSe quantum dots.