Defect-Rich CuZn Nanoparticles for Model Catalysis Produced by Femtosecond Laser Ablation.

Femtosecond laser ablation of Cu0.70Zn0.30 targets in ethanol led to the formation of periodic surface nanostructures and crystalline CuZn alloy nanoparticles with defects, low-coordinated surface sites, and, controlled by the applied laser fluence, different sizes and elemental composition. The Cu/Zn ratio of the nanoparticles was determined by energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and selected area electron diffraction. The CuZn nanoparticles were about 2-3 nm in size, and Cu-rich, varying between 70 and 95%. Increasing the laser fluence from 1.6 to 3.2 J cm-2 yielded larger particles, more stacking fault defects, and repeated nanotwinning, as evident from high-resolution transmission electron microscopy, aided by (inverse) fast Fourier transform analysis. This is due to the higher plasma temperature, leading to increased random collisions/diffusion of primary nanoparticles and their incomplete ordering due to immediate solidification typical of ultrashort pulses. The femtosecond laser-synthesized often nanotwinned CuZn nanoparticles were supported on highly oriented pyrolytic graphite and applied for ethylene hydrogenation, demonstrating their promising potential as model catalysts. Nanoparticles produced at 3.2 J cm-2 exhibited lower catalytic activity than those made at 2.7 J cm-2. Presumably, agglomeration/aggregation of especially 2-3 nm sized nanoparticles, as observed by postreaction analysis, resulted in a decrease in the surface area to volume ratio and thus in the number of low-coordinated active sites.

Dumbbell-Shaped Ho-Doped Fiber Laser Mode-Locked by Polymer-Free Single-Walled Carbon Nanotubes Saturable Absorber.

We propose a simple dumbbell-shaped scheme of a Holmium-doped fiber laser incorporating a minimum number of optical elements. Mode-locking regimes were realized with the help of polymer-free single-walled carbon nanotubes (SWCNTs) synthesized using an aerosol (floating catalyst) CVD method. We show that such a laser scheme is structurally simple and more efficient than a conventional one using a ring cavity and a similar set of optical elements. In addition, we investigated the effect of SWCNT film transmittance, defined by the number of 40 nm SWCNT layers on the laser's performance: operating regimes, stability, and self-starting. We found that three SWCNT layers with an initial transmittance of about 40% allow stable self-starting soliton mode-locking at a wavelength of 2076 nm with a single pulse energy of 0.6 nJ and a signal-to-noise ratio of more than 60 dB to be achieved.

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.

Tesla-Range Femtosecond Pulses of Stationary Magnetic Field, Optically Generated at the Nanoscale in a Plasmonic Antenna.

The inverse Faraday effect allows the generation of stationary magnetic fields through optical excitation only. This light-matter interaction in metals results from creating drift currents via nonlinear forces that light applies to the conduction electrons. Here, we describe the theory underlying the generation of drift currents in metals, particularly its application to photonic nanostructures using numerical simulations. We demonstrate that a gold photonic nanoantenna, optimized by a genetic algorithm, allows, under high excitation power, to maximize the drift currents and generate a pulse of stationary magnetic fields in the tesla range. This intense magnetic field, confined at the nanoscale and for a few femtoseconds, results from annular optical confinement and not from the creation of a single optical hot spot. Moreover, by controlling the incident polarization state, we demonstrate the orientation control of the created magnetic field and its reversal on demand. Finally, the stationary magnetic field's temporal behavior and the drift currents associated with it reveal the subcycle nature of this light-matter interaction. The manipulation of drift currents by a plasmonic nanostructure for the generation of stationary magnetic field pulses finds applications in the ultrafast control of magnetic domains with applications not only in data storage technologies but also in research fields such as magnetic trapping, magnetic skyrmion, magnetic circular dichroism, to spin control, spin precession, spin currents, and spin-waves, among others.

Ultrafast Photon-Induced Tunneling Microscopy.

Unification of the techniques of ultrafast science and scanning tunneling microscopy (STM) has the potential of tracking electronic motion in molecules simultaneously in real space and real time. Laser pulses can couple to an STM junction either in the weak-field or in the strong-field interaction regime. The strong-field regime entails significant modification (dressing) of the tunneling barrier of the STM junction, whereas the weak-field or the photon-driven regime entails perturbative interaction. Here, we describe how photons carried in an ultrashort pulse interact with an STM junction, defining the basic fundamental framework of ultrafast photon-induced tunneling microscopy. Selective dipole coupling of electronic states by photons is shown to be controllable by adjusting the DC bias at the STM junction. An ultrafast tunneling microscopy involving photons is established. Consolidation of the technique calls for innovative approaches to detect photon-induced tunneling currents at the STM junction. We introduce and characterize here three techniques involving dispersion, polarization, and frequency modulation of the laser pulses to lock-in detect the laser-induced tunneling current. We show that photon-induced tunneling currents can simultaneously achieve angstrom scale spatial resolution and sub-femtosecond temporal resolution. Ultrafast photon-induced tunneling microscopy will be able to directly probe electron dynamics in complex molecular systems, without the need of reconstruction techniques.

Scattering of Ultrashort X-ray Pulses by Various Nanosystems.

Currently, the study of the scattering of ultrashort X-ray pulses (USPs) by various objects is an urgent task, in connection with the creation of powerful sources of USP generation. In this paper, the theory of the scattering of attosecond pulses by polyatomic structures is developed taking into account the magnetic component of USPs. It is shown that the scattering spectra depend not only on the structure of the target, but also on other characteristics of USPs. Results are presented of the calculation of the scattering spectra on various nanosystems, such as rings, groups of rings, carbon nanotubes (CNTs), and groups of co-directed CNTs (forest CNTs). The calculation results are presented in an analytical form, which allows a general analysis of the expressions. It was found that taking the magnetic component of the momentum into the scattering spectra into account leads to the generation of the second harmonic. In this case, the spectra have characteristic features and differ from the scattering spectra at the carrier frequency, which can complement ultra-high-resolution X-ray analysis. It is shown that the scattering spectra of some structures, for example, forest CNTs, have a strictly specified radiation direction and such material in the field of such USPs is non-reflective (completely black).

Laser-Induced Periodic Surface Structuring of Poly(trimethylene terephthalate) Films Containing Tungsten Disulfide Nanotubes.

We report the study of the formation of Laser Induced Periodic Surface Structures (LIPSS), with UV femtosecond laser pulses (λ = 265 nm), in free-standing films of both Poly(trimethylene terephthalate) (PTT) and the composite PTT/tungsten disulfide inorganic nanotubes (PTT-WS2). We characterized the range of fluences and number of pulses necessary to induce LIPSS formation and measured the topography of the samples by Atomic Force Microscopy, the change in surface energy and contact angle using the sessile drop technique, and the modification in both Young's modulus and adhesion force values with Peak Force-Quantitative Nanomechanical Mapping. LIPSS appeared parallel to the laser polarization with a period close to its wavelength in a narrow fluence and number of pulses regime, with PTT-WS2 needing slightly larger fluence than raw PTT due to its higher crystallinity and heat diffusion. Little change was found in the total surface energy of the samples, but there was a radical increase in the negative polar component (γ-). Besides, we measured small variations in the samples Young's modulus after LIPSS formation whereas adhesion is reduced by a factor of four. This reduction, as well as the increase in γ-, is a result of the modification of the surface chemistry, in particular a slight oxidation, during irradiation.

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.

Femtosecond Laser Micromachining of Soda-Lime Glass in Ambient Air and under Various Aqueous Solutions.

We have studied femtosecond ablation of soda-lime glass sample under thin water film, under KOH and NaCl aqueous solutions films and their influence and benefits compared with ablation in the air atmosphere. These have been studied in case of the groove ablation using the infrared (IR) femtosecond laser. KOH aqueous solution film above the glass sample improved the ablation efficiency and led to the formation of the grooves with a higher aspect ratio when multi-scan glass cutting conditions were applied.

A readily usable two-photon fluorescence lifetime microendoscope.

A two-photon fluorescence lifetime (2P-FLIM) microendoscope, capable of energetic metabolism imaging through the intracellular nicotinamide adenine dinucleotide (NADH) autofluorescence, at sub-cellular resolution, is demonstrated. It exhibits readily usable characteristics such as convenient endoscope probe diameter (≈2 mm), fiber length (>5 m) and data accumulation rate (16 frames per second (fps)), leading to a FLIM refreshing rate of ≈0.1 to 1 fps depending on the sample. The spiral scanning image formation does not influence the instrument response function (IRF) characteristics of the system. Near table-top microscope performances are achieved through a comprehensive system including a home-designed spectro-temporal pulse shaper and a custom air-silica double-clad photonic crystal fiber, which enables to reach up to 40 mW of ≈100 fs pulses @ 760 nm with a 80 MHz repetition rate. A GRadient INdex (GRIN) lens provides a lateral resolution of 0.67 µm at the focus of the fiber probe. Intracellular NADH fluorescence lifetime data are finally acquired on cultured cells at 16 fps.

Challenges of dosimetry of ultra-short pulsed very high energy electron beams.

Very high energy electrons (VHEE) in the range from 100 to 250MeV have the potential of becoming an alternative modality in radiotherapy because of their improved dosimetric properties compared with 6-20MV photons generated by clinical linear accelerators (LINACs). VHEE beams have characteristics unlike any other beams currently used for radiotherapy: femtosecond to picosecond duration electron bunches, which leads to very high dose per pulse, and energies that exceed that currently used in clinical applications. Dosimetry with conventional online detectors, such as ionization chambers or diodes, is a challenge due to non-negligible ion recombination effects taking place in the sensitive volumes of these detectors. FLUKA and Geant4 Monte Carlo (MC) codes have been employed to study the temporal and spectral evolution of ultrashort VHEE beams in a water phantom. These results are complemented by ion recombination measurements employing an IBA CC04 ionization chamber for a 165MeV VHEE beam. For comparison, ion recombination has also been measured using the same chamber with a conventional 20MeV electron beam. This work demonstrates that the IBA CC04 ionization chamber exhibits significant ion recombination and is therefore not suitable for dosimetry of ultrashort pulsed VHEE beams applying conventional correction factors. Further study is required to investigate the applicability of ion chambers in VHEE dosimetry.

Simple route toward efficient frequency conversion for generation of fully coherent supercontinua in the mid-IR and UV range.

Fiber supercontinua represent light sources of pivotal importance for a wide range of applications, ranging from optical communications to frequency metrology. Although spectra encompassing more than three octaves can be produced, the applicability of such spectra is strongly hampered due to coherence degradation during spectral broadening. Assuming pulse parameters at the cutting edge of currently available laser technology, we demonstrate the possibility of strongly coherent supercontinuum generation. In a fiber with two zero-dispersion wavelengths a higher-order soliton experiences a temporal breakdown, without any compression or splitting behavior, which leads to nearly complete conversion of input solitonic radiation into resonant nonsolitonic radiation in the dispersive wave regime. As the process is completely deterministic and shows little sensitivity to input noise, the resulting pulses appear to be compressible down to the sub-cycle level and may thus hold a new opportunity for direct generation of attosecond pulses in the visible to near ultraviolet wavelength range.