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 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.

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.

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.

Giant Third-Order Nonlinear Response of Mixed Perovskite Nanocrystals.

Mixed (FAPbI3)0.92(MAPbBr3)0.08 perovskite thin films exhibit strong nonlinear optical responses, rendering them promising candidates for applications in photonics and optical communications. In this work, we present a systematic study on the ultrafast third-order nonlinear optical processes in mixed perovskite nanocrystals (NCs) by exploring the generation of third harmonic radiation and giant two-photon absorption-based photoluminescence (PL) when excited by femtosecond laser pulses of a 1030 nm central wavelength. A comparative analysis of the coherent third harmonic generation in the thin-film-containing perovskite nanocrystals has shown a 40× enhancement of the third harmonic signal compared to the signal generated in the pure quartz substrate. The cubic dependence of the third-nonlinear optical response of the (FAPbI3)0.92(MAPbBr3)0.08 perovskites on the intensity of the driving radiation was identified using broadband 38 femtosecond driving pulses. The positive nonlinear refractive index (γ = +1.4 × 10-12 cm2·W-1) is found to play an important role in improving the phase-matching conditions of the interacting pulses by generating a strong third order harmonic. The giant two-photon absorption (TPA)-assisted PL peak was monitored and a blue shift of the PL was obtained in the higher intensity range of the laser pulses, with the absorption coefficient ß estimated to be~+7.0 cm·MW-1 at a 1030 nm laser wavelength.

Enhanced XUV harmonics generation from diatomic gases using two orthogonally polarized laser fields.

Enhanced high repetition rate coherent extreme ultraviolet (XUV) harmonics represent efficient probe of electron dynamics in atoms, molecules and solids. In this work, we used orthogonally-polarized two-color laser field to generate strong even and odd high order harmonics from molecular gas targets. The dynamics of odd and even harmonics from O2, and N2 gases were investigated by employing single- and two-color laser fields using the fundamental radiation and second harmonic of 1030 nm, 37 fs, 50 kHz pulses. The relative efficiencies of harmonics were analyzed as a function of the thickness of the barium borate crystal used for second harmonic generation. Defocusing-assisted phase matching conditions were achieved in N2 gas for different groups of XUV harmonics.

Expedited Transition in the Wettability Response of Metal Meshes Structured by Femtosecond Laser Pulses for Oil-Water Separation.

Oil-water separation using super-wetting and the selective permeability of membranes for oil or water has great ecological and economic significance. We report on the transition of wettability response, from superhydrophilic underwater-superoleophobic to superhydrophobic-superoleophilic state, by nanostructuring stainless steel and copper meshes using ultrashort femtosecond laser pulses. Our approach is environment-friendly, chemical free, and efficient as it exploits the benefit of aging the processed samples in a high vacuum environment. We optimized the laser scanning parameters, mesh pore size, and aging conditions to produce membranes exhibiting an extraordinary separation efficiency of 98% for the oil-water mixture. A variation in the water and oil contact angles for different meshes is presented as a function of the laser scanning speed. Stainless steel meshes with 150 µm pore size and copper meshes with 100 µm pore size have demonstrated an excellent wettability response for oil and water phases. Vacuum aging causes rapid chemisorption of hydrocarbons on laser-structured surfaces in the absence of water molecules, rapidly transforming the wetting state from superhydrophilic to superhydrophobic.

High-order harmonics generation in the plasmas produced on different rotating targets during ablation using 1 kHz and 100 kHz lasers.

We analyze the high-order harmonics generation using 1 kHz and 100 kHz lasers by ablating different rotating targets. We demonstrate the high average flux of short-wavelength radiation using the latter laser, while comparing the plasma formation conditions at different pulse repetition rates. The analysis of harmonic stability in the case of the 100 kHz experiments showed the two-fold decay of the 27th harmonic generating in silver plasma after 3.5×106 shots. The advantages of shorter pulse-induced ablation for the improvement of harmonic generation stability are demonstrated. Two-color pump of plasma, resonance enhancement of single harmonic, and quasi-phase matching studies are presented for 1 kHz laser applications. The formation of modulated multi-jet plasma on the plane and curved surfaces during ablation by 100 kHz pulses is demonstrated. In the case of the 25th harmonic of 1030 nm radiation (E=30 eV) generated during experiments in carbon plasma, at 100 kHz and 40 W average power of driving pulses, 0.4 mW of average power for single harmonic in the 40 nm spectral range was achieved.

High-Order Harmonic Generation in Au Nanoparticle-Contained Plasmas.

Gold nanoparticles (NPs) have a wide range of applications in various fields. Here, we present high-order nonlinear optical studies of the plasmas produced from ablation of Au bulk targets and Au NP films deposited on paper and glass substrates. Experimentally, we analyze high-order harmonic generation (HHG) from gold NPs-containing plasmas. The HHG is produced by 35-fs pulses at 800 and 400 nm, while the plasmas are produced by femtosecond (35 fs, 800 nm), picosecond (200 ps, 800 nm), and nanosecond (5 ns, 1064 nm) pulses, respectively. High-order harmonics produced from ablated Au NPs on paper were 40 times stronger than the HHG from that ablated from the Au bulk targets. Through molecular dynamic simulations, we investigate the formation of gold NPs during laser ablation of a metal surface under different conditions.

Nonlinear optical characterization of copper oxide nanoellipsoids.

Recently, nonspherical nanoparticles took attention due to advanced properties of these structures. We report the study of the nonlinear optical properties of copper oxide nanoellipsoids using 800 nm and 400 nm, 60 fs pulses. The optical limiting effect of copper oxide nanoellipsoids is analyzed. The influence of band gap of copper nanoparticles and copper oxide nanoellipsoids on their nonlinear optical response was studied. For the first time, the low- and high-order nonlinear optical responses of copper nanoellipsoids were studied. The magnitudes of nonlinear optical parameters of the suspension of copper oxide nanoellipsoids were measured to be γ = 1.23 × 10-15 cm2 W-1, and ß = 1.0 × 10-11 cm W-1 respectively. We observed the four-fold enhancement of the nonlinear optical refraction of copper oxide nanoellipsoids at the wavelength of 400 nm, 60 fs probe pulses compared to 800 nm radiation. We also analyzed the high-order nonlinear response of CuO nanoellipsoids through generation of high-order harmonics of 800 nm, 60 fs pulses in the plasmas produced during laser ablation of the nanoellipsoid-contained targets. We demonstrated the harmonics up to the 35th order (E = 50 eV) in case of single-color pump and 24th (30 eV) in case of two-color pump.

Pulse Duration and Wavelength Effects of Laser Ablation on the Oxidation, Hydrolysis, and Aging of Aluminum Nanoparticles in Water.

We analyzed the formation of the aluminum (Al) nanoparticles (NPs) with triangular shape obtained by ablating Al bulk in liquid using pulses with different durations (5 ns, 200 ps, and 30 fs) and wavelengths (355 nm, 800 nm, and 1064 nm). We report three stages of synthesis and aging of Al NPs: Formation, transformation, and stable stage. The NPs prepared by different pulses are almost identical at the initial stage. The effects of duration and wavelength of the ablation pulses on the aging of NPs are revealed. Pulse duration is determined to be essential for morphological transformation of NPs, while pulse wavelength strongly influences particle sizes. NPs produced by ultra-short pulses have smaller sizes and narrow size distribution. We demonstrate that oxidation and hydrolysis of Al in water are the results of ablation for all pulse durations and wavelengths, which also strongly modify the preferable reaction path of NPs in water, thus affecting the composition and morphology of triangle NPs. The results of modeling of the NPs generation in water due to a 50 ps laser pulse interacting with a thick Al target are presented. Water-based effects in the formation of NPs, their evolution, and solidification are considered from the mechanical and thermophysical points of view. The detailed analysis of the modeling results allowed for determination of the main mechanism responsible for the ablation process followed by the NPs formation.

Effects of Laser Plasma Formation on Quasi-Phase Matching of High-Order Harmonics from Nanoparticles and Atoms.

The application of nanoparticles (NPs) and quasi-phase matching (QPM) each play an important role in the enhancement of high-order harmonics (HHG) of ultrashort laser pulses. We analyze various regimes of nanoparticle plasma formation for the creation conditions for maximal QPM-induced enhancement of the groups of harmonics in the extreme ultraviolet (XUV). Laser plasmas were formed on the surfaces of NPs- and microparticle (MPs)-contained targets using ablation by nanosecond, picosecond, and femtosecond pulses. Different conditions of laser plasma formation (extended and perforated plasma) and variable concentrations of free electrons in these three cases of laser ablation led to modifications of QPM conditions. We demonstrate novel approaches in the optimization of QPM at the conditions of laser ablation of NPs and MPs by pulses of different durations. The formation of QPM conditions using femtosecond and picosecond heating pulses during HHG in such plasmas allowed the growth of conversion efficiency of the groups of harmonics, with the enhancement factors exceeding 25× in different ranges of XUV, contrary to less efficient QPM in the case of nanosecond pulse-induced ablation.

Nonlinear Optical Studies of Gold Nanoparticle Films.

Gold films are widely used for different applications. We present the results of third- and high-order nonlinear optical studies of the thin films fabricated from Au nanoparticle solutions by spin-coating methods. These nanoparticles were synthesized by laser ablation of bulk gold in pure water using 200 ps, 800 nm pulses. The highest values of the nonlinear absorption coefficient (9 × 10-6 cm W-1), nonlinear refractive index (3 × 10-11 cm² W-1), and saturation intensity (1.3 × 1010 W cm-2) were achieved using 35 fs, 400 nm pulses. We also determined the relaxation time constants for transient absorption (220 fs and 1.6 ps) at 400 nm. The high-order harmonic generation was studied during propagation of 35 fs, 800 nm pulses through the plasma during the ablation of gold nanoparticle film and bulk gold. The highest harmonic cutoff (29th order) was observed in the plasma containing gold nanoparticles.

Effective high-order harmonic generation from metal sulfide quantum dots.

In the past, common media for high-order harmonic generation (HHG) has been atoms and molecules. More recently, clusters, and nanoparticles have been introduced as HHG emitting media. Multi-particle media can enhance HHG yields but have more stringent requirements in determining the optimal parameters. Here, we demonstrate, for the first time, the effective application of 1-3 nm metal sulfide quantum dots (QDs) for harmonic generation in the 20 - 115 nm extreme ultraviolet range. We report on the syntheses, ablation of Ag2S, CdS, and ZnS QDs, and HHG from laser-produced plasmas by using single- and two-color pumps. We compare HHG efficiency from the ablated QDs to that of bulk metal sulfides and show a seven-fold increase in harmonic yields. Further, the study also allows us to understand the effects of QD-contained plasma spreading dynamics on HHG yield.