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.

Comparing Water Transport Properties of Janus Membranes Fabricated from Copper Mesh and Foam Using a Femtosecond Laser.

One of the important aspects of manipulating and controlling liquid transport is the design of membrane surfaces. Janus membranes with opposite wettability characteristics can be manufactured for efficient directional water transfer. In this work, two types of materials were used to fabricate membranes with an asymmetric wettability behavior: copper foam and copper mesh. One side of the membranes was treated by scanning with a femtosecond laser beam, as a result of which it was converted to a superhydrophilic state, while the untreated side remained hydrophobic. Both membranes demonstrated excellent properties of a water diode through which water droplets could easily pass from the hydrophobic side to the hydrophilic side, but not vice versa. This behavior was achieved by finding the optimal laser scanning speed. This type of Janus membrane has found applications in collecting water droplets from fog; therefore, the samples obtained were also tested in terms of harvesting micro-droplets. The Janus mesh-based structure has demonstrated a higher water collection efficiency (3.9 g/cm2 h) compared to the foam-based membrane (2.5 g/cm2 h). Since the fog-water conversion efficiency decreased over time (to 0.5 g/cm2 h in 2 weeks) due to the absorbance of organic pollutants, a coating of titanium oxide was applied to the laser-treated side of the Janus membranes. As a result, the effective function of the systems became distinctly long-lasting and was well maintained for at least 60 days. Moreover, the fabricated systems were protected from further degradation by simply placing them under sunlight for several hours. Our results prove to be useful in developing asymmetric hydrophobic-superhydrophilic membranes, which have potential applications in high-precision drop control and in harvesting water from arid environments.

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.

Visualization of bond rearrangements in acetylene using near single-cycle laser pulses.

The migration of hydrogen atoms resulting in the isomerization of hydrocarbons is an important process which can occur on ultrafast timescales. Here, we visualize the light-induced hydrogen migration of acetylene to vinylidene in an ionic state using two synchronized 4 fs intense laser pulses. The first pulse induces hydrogen migration, and the second is used for monitoring transient structural changes via Coulomb explosion imaging. Varying the time delay between the pulses reveals the migration dynamics with a time constant of 54 ± 4 fs as observed in the H+ + H+ + CC+ channel. Due to the high temporal resolution, vibrational wave-packet motions along the CC- and CH-bonds are observed. Even though a maximum in isomerization yield for kinetic energy releases above 16 eV is measured, we find no indication for a backwards isomerization - in contrast to previous measurements. Here, we propose an alternative explanation for the maximum in isomerization yield, namely the surpassing of the transition state to the vinylidene configuration within the excited dication state.

Determining the Role of Oxygen in Obtaining Long-Term Stable Superhydrophilic Surfaces on Metals Treated with a Femtosecond Laser.

Laser processing is a simple way to obtain hydrophobic or even superhydrophobic properties of metal surfaces. However, preparation of superhydrophilic surfaces by this method, the properties of which do not change under the influence of various factors, remains a difficult task. In this work, we show that with increasing laser power, the degree of oxidation of the treated metal surface also increases. As a result, highly oxidized samples showed highly stable superhydrophilic properties. A Janus membrane fabricated from a stainless steel mesh with asymmetric hydrophilic-hydrophobic wettability demonstrated stable water diode properties. In addition, it was found that during the examination of sample surfaces by Raman spectroscopy, organic compounds adsorbed on the hydrophobic surface were decomposed by the laser of the spectrometer, which imposes limitations on the laser power when using this method in characterizing hydrophobic surfaces of metals fabricated by laser processing.

Study on the Origin and Evolution of Femtosecond Laser-Induced Surface Structures: LIPSS, Quasi-Periodic Grooves, and Aperiodic Micro-Ridges.

We investigate the evolution mechanisms of the laser-induced periodic surface structures (LIPSS) and quasi-periodic grooves that are formed on the surface of monocrystalline silicon (mono-Si) when exposed to femtosecond laser radiation of different pulse duration, state of polarization, and fluence. The conditions required for producing LIPSS-free complex micro-ridge patterns are elaborated. The LIPSS evolution mechanism is explained in terms of scattering/interference-based phenomena. To establish the basis for our interpretation, single femtosecond pulses of different pulse durations are irradiated on mono-Si. The absence/appearance of LIPSS rudiments is explained in the context of spectral bandwidth and the associated effects on the intensity of the central wavelength. Shorter fs pulses of a wider bandwidth are employed to induce LIPSS-free micro-ridge patterns. It is demonstrated that the resultant micro-ridge patterns depend on the laser fluence distribution and can be manipulated through laser polarization. The curved morphology of LIPSS rudiments and the evolution mechanism of low- and high-spatial frequency LIPSS, i.e., LSFL and HSFL, are discussed. Finally, it is demonstrated that the consolidated quasi-periodic grooves result from HSFL welding together groups of LSFL. Although our findings are based on fs laser interaction with mono-Si, the results can also be applied to many other materials.

Enhancing Anticorrosion Resistance of Aluminum Alloys Using Femtosecond Laser-Based Surface Structuring and Coating.

We report a robust two-step method for developing adherent and anticorrosive molybdenum (Mo)-based coatings over an aluminum (Al) 6061 alloy substrate using a femtosecond (fs) laser. The fs laser nanostructuring of Al 6061 alloy in air gives rise to regular arrays of microgrooves exhibiting superhydrophilic surface properties. The microstructured surface is further coated with an Mo layer using the fs-pulsed laser deposition (fs-PLD) technique. The combination of the two femtosecond laser surface treatments (microstructuring followed by coating) enabled the development of a highly corrosion-resistant surface, with a corrosion current of magnitude less than that of the pristine, the only structured, and the annealed alloy samples. The underlying mechanism is attributed to the laser-assisted formation of highly rough hierarchical oxide structures on the Al 6061 surface along with post heat treatment, which passivates the surface and provide the necessary platform for firm adhesion for Mo coating. Our results reveal that the corrosive nature of the Al-based alloys can be controlled and improved using a combined approach of femtosecond laser-based surface structuring and coating.

A Two-Step Femtosecond Laser-Based Deposition of Robust Corrosion-Resistant Molybdenum Oxide Coating.

A two-step femtosecond-pulsed laser deposition (fs-PLD) process is reported for the rapid development of uniform, poreless, crack-free, and well-adhering amorphous coatings of source materials with a high melting point. The first step comprises a high-rate raw deposition of the source material via fs-PLD, followed by a second step of scanning the raw sample with fs laser pulses of optimized fluence and scan parameters. The technique is applied to develop substoichiometric molybdenum oxide (MoOx, x < 3) coatings on mild steel. The thickness of the layer was ~4.25 µm with roughness around 0.27 µm. Comprehensive surface characterization reveals highly uniform and relatively moderate roughness coatings, implying the potential of these films as robust corrosion-resistant coats. Corrosion measurements in an aqueous NaCl environment revealed that the coated mild steel samples possess an average corrosion inhibition efficiency of around 95% relative to polished mild steel.

Enhancing Gas Solubility in Water via Femtosecond Laser-Induced Plasma.

The generation of laser-induced plasma at the gas-liquid interface provides many fundamental and interesting scientific phenomena such as ionization, sharp explosion, shock wave radiation, bubble creation, and water splitting. However, despite the extensive research in this area, there is no reference on the effect of the surrounding environment on the chemical processes that occur during the laser-induced plasma-water interaction. In this work, we investigate the effect of the surrounding gas environment on femtosecond laser-induced plasma when generated at the pure water-gas interface. Ultrashort laser pulses were applied to water in the presence of air and N2 and Ar gas environments. Formation of a significant number of nitrate-based species in water was observed after exposure to femtosecond laser-induced plasma in air and N2 environments. The detected NO3 ions formed in the laser-treated water led to the appearance of an absorption peak in the UV range, a significant decrease in the water pH value, and a significant increase in water's electrical conductivity. All induced properties of water were stable for 3 months of monitoring after laser treatment. Our work shows that the generation of laser-induced plasma in water propagating into a gaseous medium facilitates the interaction between the two media, as a result of which the compositions of substances present in the gaseous medium can be dissolved in water without increasing the gas pressure. The presented approach may find applications in areas such as water purification, material synthesis, and environmental stewardship.

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.

Pulsed Laser Deposited Zeolite Coatings on Femtosecond Laser-Nanostructured Steel Meshes for Durable Superhydrophilic/Oleophobic Functionalities.

Ultrafast laser structuring has proven to alter the wettability performance of surfaces drastically due to controlled modification of the surface roughness and energy. Surface alteration can be achieved also by coating the surfaces with functional materials with enhanced durability. On this line, robust and tunable surface wettability performance can be achieved by the synergic effects of ultrafast laser structuring and coating. In this work, femtosecond laser-structured stainless steel (SS-100) meshes were used to host the growth of NaAlSi2O6-H2O zeolite films. Contact angle measurements were carried on pristine SS-100 meshes, zeolite-coated SS-100 meshes, laser-structured SS-100 meshes, and zeolite-coated laser-structured SS-100 meshes. Enhanced hydrophilic behavior was observed in the zeolite-coated SS-100 meshes (contact angle 72°) and in laser-structured SS-100 meshes (contact angle 41°). On the other hand, superior durable hydrophilic behavior was observed for the zeolite-coated laser-structured SS-100 meshes (contact angle 14°) over an extended period and reusability. In addition, the zeolite-coated laser-structured SS-100 meshes were subjected to oil-water separation tests and revealed augmented effectuation for oil-water separation.

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.

Anomalous formation of trihydrogen cations from water on nanoparticles.

Regarded as the most important ion in interstellar chemistry, the trihydrogen cation, [Formula: see text], plays a vital role in the formation of water and many complex organic molecules believed to be responsible for life in our universe. Apart from traditional plasma discharges, recent laboratory studies have focused on forming the trihydrogen cation from large organic molecules during their interactions with intense radiation and charged particles. In contrast, we present results on forming [Formula: see text] from bimolecular reactions that involve only an inorganic molecule, namely water, without the presence of any organic molecules to facilitate its formation. This generation of [Formula: see text] is enabled by "engineering" a suitable reaction environment comprising water-covered silica nanoparticles exposed to intense, femtosecond laser pulses. Similar, naturally-occurring, environments might exist in astrophysical settings where hydrated nanometer-sized dust particles are impacted by cosmic rays of charged particles or solar wind ions. Our results are a clear manifestation of how aerosolized nanoparticles in intense femtosecond laser fields can serve as a catalysts that enable exotic molecular entities to be produced via non-traditional routes.

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.

Few-cycle laser driven reaction nanoscopy on aerosolized silica nanoparticles.

Nanoparticles offer unique properties as photocatalysts with large surface areas. Under irradiation with light, the associated near-fields can induce, enhance, and control molecular adsorbate reactions on the nanoscale. So far, however, there is no simple method available to spatially resolve the near-field induced reaction yield on the surface of nanoparticles. Here we close this gap by introducing reaction nanoscopy based on three-dimensional momentum-resolved photoionization. The technique is demonstrated for the spatially selective proton generation in few-cycle laser-induced dissociative ionization of ethanol and water on SiO2 nanoparticles, resolving a pronounced variation across the particle surface. The results are modeled and reproduced qualitatively by electrostatic and quasi-classical mean-field Mie Monte-Carlo (M3C) calculations. Reaction nanoscopy is suited for a wide range of isolated nanosystems and can provide spatially resolved ultrafast reaction dynamics on nanoparticles, clusters, and droplets.