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At the selected frequencies from 0.3 to 10 THz we measured the two-dimensional (2D) distributions of fluence and polarization of terahertz (THz) emission from a single-color femtosecond filament. At the majority of frequencies studied, the THz beam has a donut-like shape with azimuthal modulations and radial polarization. At the maximal modulation, THz beam takes the form of the two lobes and polarization of the THz field degenerates into orthogonal to the laser pulse polarization direction. Violation of the radially polarized donut beam shape is due to destructive interference of THz waves driven by light pressure directed along the laser beam propagation axis and ponderomotive force parallel to the laser polarization.

The terahertz (THz) radiation emitted by an air-based femtosecond filament biased by a static electric field is known to have on-axis shape and relatively low frequency spectrum in contrast to the unbiased single-color and two-color schemes. Here, we measure the THz emission of a 15-kV/cm-biased filament in air produced by a 740-nm, 1.8-mJ, 90-fs pulse and demonstrate that a flat-top on-axis THz angular distribution of the emission at 0.5-1 THz transforms into a contrast ring-shaped one at 10 THz.

Based on our experimental study of spectral characteristics of an improved compact CO laser system, the prospects of using such a laser system for solving urgent problems of atmospheric sounding were demonstrated. An increase in the number of laser lines due to intracavity generation of the second harmonic and sum-frequencies in a nonlinear zinc germanium phosphide (ZnGeP 2 ) crystal enriches capabilities of the laser. It was shown that such a CO laser system with frequency conversion in ZnGeP 2 crystal can be used for detection and measuring concentration of at least 14 minor natural and pollution gases components of the atmosphere. The advantages and disadvantages of various laser operation modes, and the prospects for using its radiation for atmospheric remote sensing in various spectral ranges are discussed.

We study the angular distribution of different spectral components of the terahertz emission from a single-color laser filament plasma. The opening angle of a terahertz cone is experimentally demonstrated to be proportional to the inverse square root of both plasma channel length and terahertz frequency in the non-linear focusing mode, whereas in the case of linear focusing this dependence breaks down. We also experimentally show that any conclusions of terahertz radiation spectral composition require the angle range from which it is collected to be specified.

High-intensity (∼1 TW/cm2 and higher) region formed in the propagation of ∼60 GW, 90 fs Ti:Sapphire laser pulse on a ∼100 m path in air spans for several tens of meters and includes a plasma filament and a postfilament light channel. The intensity in this extended region is high enough to generate an infrared supercontinuum wing and to initiate laser-induced discharge in the gap between the electrodes. In the experiment and simulations, we delay the high-intensity region along the propagation direction by inserting metal-wire meshes with square cells at the laser system output. We identify the presence of a high-intensity region from the clean-spatial-mode distributions, appearance of the infrared supercontinuum wing, and occurrence of the laser-induced discharge. In the case of free propagation (without any meshes), the onset of the high-intensity zone is at 40-52 m from the laser system output with ∼30 m extension. Insertion of the mesh with 3 mm cells delays the beginning of the high-intensity region to 49-68 m with the same ∼30 m extension. A decrease in the cell size to 1 mm leads to both delay and shrinking of the high-intensity zone to 71-73 m and 6 m, respectively. Three-dimensional simulations in space confirm the mesh-induced delay of the high-intensity zone as the cell size decreases., Competing Interests: The authors declare no conflicts of interest.

Microscale filamentation of 0.25 NA-focused, linearly and circularly polarized 1030 nm and 515 nm ultrashort laser pulses of variable pulse widths in fused silica, fluorite, and natural and synthetic diamonds demonstrates the Raman-Kerr effect in the form of critical pulse power magnitudes, proportional to squared wavelength and inversely proportional to laser pulse width of 0.3-10 ps. The first trend represents the common spectral relationship between the quantities, while the second indicates its time-integrated inertial contribution of Raman-active lattice polarization, appearing in transmission spectra via ultrafast optical-phonon Raman scattering. The optical-phonon contribution to the nonlinear polarization could come from laser field-induced spontaneous/stimulated Raman scattering and coherent optical phonons generated by electron-hole plasma with its clamped density in the nonlinear focus. Almost constant product value of the (sub)picosecond laser pulse widths and corresponding critical pulse powers for self-focusing and filamentation in the dielectrics ("critical pulse energy") apparently implies constant magnitude of the nonlinear polarization and other "clamped" filamentation parameters at the given wavelength.

Results concerning the controllable ablation of nano-layered thin films (NLTF) by femtosecond laser pulses are presented. Investigated samples were titanium-aluminum bilayers, deposited on a silicon substrate, with the top titanium or aluminum layer of variable thickness on the surface. Irradiation was done in ambient air with single femtosecond laser pulses under standard laboratory conditions. The samples were analyzed by complementary methods of optical and scanning electron microscopy and optical profilometry, exhibiting laser-fluence-dependent ablative removal either of the top layer or the entire bilayer or even partial ablation of the underlying silicon substrate. The removal (spallation) threshold fluences for the topmost layer are scalable versus its thickness almost irrespectively of its material, being rather selective for the Ti-coated samples and much less selective for the Al-coated samples. The removal of the entire bilayers was found to be strongly influenced by electronic properties of the underlying metallic layer, dictating the NLTF-Si adhesion, heat conduction, and capacity in the NLTFs toward the NLTF-Si interface and beyond, as well as by their thermophysical characteristics, e.g., almost twice higher melting temperature and enthalpy for Ti. As a result, precise fs-laser machining of the entire NLTFs is pronounced and selective for the samples with the fusible Al at the low-adhesion Al-Si interfaces, compared with the incomplete NLTF removal from the high-adhesion and refractory Ti-Si interfaces.

In the experiment, the laser pulse (744 nm, 0.5 mJ, 90 fs) focused into the air gap between the plane electrodes biased by a 10 kV/cm field (DC-biased filament) produced terahertz (THz) radiation. At the selected frequencies of ν =0.3, 0.5, 1 THz, a wide flat-top angular distribution was measured by a bolometer rotating in the plane of the electrodes. The simulations based on the unidirectional pulse propagation equation with fine 0.01 THz resolution and 3 PHz frequency domain showed the transition of the THz directional diagram from the flat-top at ν ≲1 T H z to the conical one at ν >8 T H z due to the destructive interference of THz waves from the ionization front propagating with the superluminal velocity. Refraction on the plasma is not the major factor in ring formation.

Broadband frequency downconversion of a 90 fs 744 nm Ti:sapphire laser pulse into the mid-infrared (IR) was demonstrated via its filamentation-induced self-frequency shift in air and subsequent intra-pulse difference frequency generation in a L i G a S 2 crystal. The filamentation of the laser pulse in air provided its continuous spectral broadening to the Stokes wing with spectral humps separated by ∼1000 c m -1 that was appropriate for the laser pulse difference frequency conversion into the mid-IR. The difference frequency emission spectrum spanned from 8.5 to 13.5 µm at the e -2 level. The transform limited pulse duration of the mid-IR pulse was 47 fs, which corresponded to a 1.3-cycle laser pulse. Energy conversion efficiency was up to 10 -4 and 5⋅10 -4 without and with chirp compensation, respectively.

The influence of plasma channel length on an angular terahertz (THz) radiation distribution is experimentally studied for the channel formed under filamentation of an ultrashort laser pulse. It is shown that the angular distribution of the THz emission depends only on laser intensity in the filament and plasma density of the plasma channel and does not depend on the plasma channel length. A qualitative explanation of the THz emission screening by the filament plasma channel is proposed.

Transient stimulated Raman scattering (SRS) of 0.3 ps 515 nm laser pulses in ${\rm BaWO_4}$BaWO 4 crystal was experimentally demonstrated with efficiency up to ${\sim}{20}\% $∼20% for the Stokes component with a wavenumber of ${\sim}{925}\;{{\rm cm}^{ - 1}}$∼925cm -1 in a simple single-pass geometry. This anomalous high efficiency was obtained due to the laser pulse self-phase modulation resulting in spectral broadening and seeding the SRS. The applicability of seed pulse production for a high-pressure sub-picosecond ${{\rm CO}_2}$CO 2 laser amplifier via difference frequency generation in ${{\rm LiGaS}_2}$LiGaS 2 crystal was numerically verified.

Single microscale filaments were produced in monocrystalline Ia-type diamond by 1030 nm, 300 fs laser pulses tightly focused at NA = 0.3 and different peak powers, visualized by transverse imaging and spectrally characterized by longitudinal micro-spectroscopy, using intrinsic UV A-band photoluminescence (PL) with its peak at about 430 nm. Power-dependent scaling relationships for the local PL yield and diameters of the accompanying luminous micro-channels of recombining electron-hole plasma indicate a transition from three-photon absorption to free-carrier plasma absorption, as the consequent energy deposition mechanisms at increasing peak laser power. Power-dependent elongation of the luminous micro-channels versus peak laser power fitted by a Marburger formula yields, on average a diffraction-based estimate of 0.6 MW critical power for self-focusing within the diamond at the pump laser wavelength of 1030 nm.

Surface-enhanced IR absorption (SEIRA) microscopy was used to reveal main chemical and physical interactions between Staphylococcus aureus bacteria and different laser-nanostructured bactericidal Si surfaces via simultaneous chemical enhancement of the corresponding IR-absorption in the intact functional chemical groups. A cleaner, less passivated surface of Si nanoripples, laser-patterned in water, exhibits much stronger enhancement of SEIRA signals compared to the bare Si wafer, the surface coating of oxidized Si nanoparticles and oxidized/carbonized Si (nano) ripples, laser-patterned in air and water. Additional very strong bands emerge in the SEIRA spectra on the clean Si nanoripples, indicating the potential chemical modifications in the bacterial membrane and nucleic acids during the bactericidal effect.

Difference frequency generation under mixing of repetitively-pulsed CO- and CO 2 -laser radiation in AgGaSe 2 , BaGa 2 GeSe 6 and PbIn 6 Te 10 nonlinear crystals was studied. Efficiency and refractive indices were examined for this frequency conversion into the long-wave domain of ∼12-20 µm in the mid-IR. The highest frequency conversion efficiency of 10 -4 was obtained for a relatively new PbIn 6 Te 10 crystal, which is an order of magnitude higher than previous results.

At first glance, the amount of water molecules naturally contained in humid air is negligibly small to affect filamentation of ultrashort laser pulses. However, here we show, both experimentally and numerically, that for ultraviolet laser pulses with 248 nm wavelength this is not true. We demonstrate that with increase of air humidity the plasma channels generated by the ultraviolet laser pulses in air become longer and wider, while the corresponding electron density in humid air can be up to one order of magnitude higher compared to dry air.

The examination and verification of a simple integral figure of merit for nonlinear crystals, taking into account different crystal properties, was studied. The examination was carried out on the basis of experimental data on the broadband sum frequency generation of CO laser radiation in ZnGeP 2 , Ba Ga 2 Ge Se 6 , AgGaSe 2 , GaSe, and Pb In 6 Te 10 mid-IR nonlinear crystals. Taking into account spectral and angular phase-matching bandwidths, the figure of merit provides the best agreement with the experiment and can be applied for qualitative, and even quantitative, comparison of the nonlinear crystals.

Low- and ultralow-energy tightly focused 200 fs, 515 nm donut-shaped laser pulses at 0.25 and 0.65 NA focusing were used for single-shot ablative pulse-energy scalable nanopatterning of 50 nm thick gold film and the following plasmonic excitation of dye monolayer photoluminescence (PL) in the fabricated nanostructures, respectively. The same pulses at much lower, non-ablative nanojoule energies, and the same focusing and linear, azimuthal, or radial polarizations provided efficient spectrally and symmetry-matched excitation of both localized and delocalized surface electromagnetic modes in the separate, ring-like through holes and their arrays in the film envisioned by our modeling, thus resulting in a polarization-sensitive yield of rhodamine 6G dye PL. The demonstrated consistency between the symmetries of the donut-shaped low-energy photo-exciting laser beam, its polarization state, and the donut-shaped gold nanostructures, produced by the same beam at high, ablative pulse energies, paves the way to smart, self-consistent nanofabrication and plasmonic sensing, when the structured light interacts with the consistently structured matter.

A comprehensive picture of the nanosecond-laser generation of colloidal nanoparticles in liquids is nowadays the demand of their high-throughput industrial fabrication for diverse perspective biomedical, material science, and optoelectronic applications. In this study, using silicon as an example, we present a self-consistent experimental visualization and theoretical description of key transient stages during nanosecond-laser generation of colloidal nanoparticles in liquids: plasma-mediated injection of ablated mass into the liquid and driving the vapor bubble, finalized by the colloid appearance in the liquid. The explored fundamental transient stages envision the basic temporal and spatial scales, as well as laser parameter windows, for the demanded high-throughput nanosecond-laser generation of colloidal nanoparticles in liquids.

Barriers were produced in porous glass through its local bulk density modification by direct femtosecond writing accompanied by СО 2 -laser surface thermal densification, to make functional microfluidic elements separated by such physical barriers with different controlled permeability. The separation of multi-component solutions into individual components with different molecule sizes (molecular separation) was performed in this first integrated microfluidic device fabricated in porous glass. Its application in the environmental gas-phase analysis was demonstrated.

A compact repetitively pulsed broadband carbon monoxide (CO) laser system with intracavity frequency conversion, for which a nonlinear crystal was also used as an output coupler, was launched for the first time, to the best of our knowledge. The laser system simultaneously operated in two spectral ranges: CO laser fundamental band (4.9-6.0 μm) and its sum frequencies band (2.45-2.95 μm). Different designs of the laser cavity were considered. Peak powers of the fundamental and sum frequencies laser pulses were up to 2 kW and 10 W, respectively.

Broadband three-stage frequency conversion of multiline sub-microsecond CO laser radiation in a single sample of ZnGeP 2 crystal was experimentally and numerically studied for the first time, to the best of our knowledge. As a result, the hybrid laser system emitted more than 200 narrow spectral lines within the 2.4-6.2 μm spectral range. The measured conversion efficiencies of the first, second, and third stages were about 4.8%, 0.4%, and 0.05%, respectively. Our numerical simulation demonstrated that the third stage of this frequency conversion can extend the laser system spectrum toward the shorter wavelength of 2.2 μm.

A technique is presented to create uninterrupted long ultraviolet filaments in air using appropriately structured transmission mesh. The mesh with different cell sizes was inserted into 10-cm parallel beam of 0.2-J, 248-nm, and 870-fs pulse propagating along ~100-m corridor. Transverse positions of multiple filaments formed by the optimum size cells were reproducible within at least 15 m along the propagation path. 3D+time simulations confirmed uninterrupted plasma channels with fixed positions in the transverse space similar to the experiment. Unoptimized cell size resulted in filaments shifting towards the cell center and destruction of uninterrupted filaments.

Multi-sector broadband diffractive optical elements (DOEs) were designed and fabricated from fused silica for high-efficiency multiplexing of femtosecond and nanosecond Gaussian laser beams into multiple (up to one 100) optically tunable microbeams with increased high-numerical aperture (NA) focal depths. Various DOE-related issues, such as high-NA laser focusing, laser pulsewidth, and DOE symmetry-dependent heat conduction effects, as well as the corresponding spatial resolution, were discussed in the context of high-throughput laser patterning. The increased focal depths provided by such DOEs, their high multiplexing efficiency and damage threshold, as well as easy-to-implement optical shaping of output microbeams provide advanced opportunities for direct, mask-free, and vacuum-free high-throughput subtractive (ablative) and displacive pulsed-laser patterning of various nanoplasmonic films for surface-enhanced spectroscopy, sensing, and light control.

A carbon monoxide laser emitting on the highest ever observed vibrational transition with a wavelength of 8.7 μm was for the first time launched. An influence of gas mixture content on the CO laser spectrum and factors limiting the longest CO laser wavelength are discussed.

PbIn 6 Te 10 is a new mid-infrared (IR) nonlinear crystal with a very wide transparency range from 1.7 up to 31 μm. Calculated phase-matching angles show possibility of frequency conversion throughout the transparency range. Sum frequency generation of multiline carbon monoxide (CO) laser and difference frequency generation when mixing CO and carbon dioxide laser radiation were experimentally studied. Laser-induced damage threshold and frequency conversion efficiency under multiline CO laser pumping were measured.

For the first time, to the best of our knowledge, a broadband two-stage frequency conversion of multiline CO laser radiation was theoretically and experimentally demonstrated in a single AgGaSe 2 crystal. The first stage is sum frequency generation of CO laser radiation. The second stage is concurrent difference frequency generation within 4.3-4.9 μm spectral range when mixing sum frequency radiation with the pump radiation in the same AgGaSe 2 crystal. Internal sum frequency generation efficiency of multiline CO laser was up to 1%, while internal difference frequency generation efficiency was up to 0.065%.

Both normal and abnormal sub-100-nanometer ripples (wavenumber ∼10  μm(-1)) were separately observed on Ti surfaces excited by linearly polarized IR femtosecond laser pulses at lower and higher fluences. Numerical modeling of dispersion curves for surface plasmon-polaritons on the photoexcited Ti surfaces demonstrates its surface plasmon resonance with the peak wavenumber ∼8  μm(-1) spectrally tuned by prompt surface optical response, prompt surface charging, and pre-oxidation, with normal/abnormal nanoripples appearing at its red/blue shoulders, respectively.

Frequency conversion of CO laser radiation was experimentally studied in ZnGeP(2) and GaSe nonlinear crystals. To enhance conversion efficiency, we applied a CO laser system "master oscillator power amplifier" with concurrent mode locking and Q switching. The laser system emitted ∼1-μs train of ns pulses. Internal efficiency of frequency doubling reached 37% in ZnGeP(2) crystal and 5% in GaSe crystal. Two-stage frequency conversion (including second-harmonic and difference-frequency generation) in ZnGeP(2) crystal under optical pumping by a selective two-spectral line CO laser was studied.

In this work, we demonstrate an all-laser method of fabrication of optical nanoantennas (ONAs) with an additional coupling/focusing diffractive element. This method is based on double-shot femtosecond laser nanoablation of a thin supported metallic film, inducing a sequence of electrodynamic (surface plasmon-polariton [SPP] excitation and interference), thermal (melting, ablation and ultrafast cooling), and hydrodynamic processes. In particular, the thermal and hydrodynamic processes are important for ONA formation after the first laser shot, while second spatially shifted laser shot via an induced SPP wave results in a radial surface grating near the nanoantenna. Such gratings provide efficient coupling between incident laser radiation and SPP waves, thus significantly improving the ONA efficiency.

In this work the formation of laser-induced periodic surface structures (LIPSS) on a titanium surface upon irradiation by linearly polarized femtosecond (fs) laser pulses with a repetition rate of 1 kHz in air environment was studied experimentally. In particular, the dependence of high-spatial-frequency-LIPSS (HSFL) characteristics on various laser parameters: fluence, pulse number, wavelength (800 nm and 400 nm), pulse duration (10 fs - 550 fs), and polarization was studied in detail. In comparison with low-spatial-frequency-LIPSS (LSFL), the HSFL emerge at a much lower fluence with orientation perpendicular to the ridges of the LSFL. It was observed that these two types of LIPSS demonstrate different fluence, shot number and wavelength dependencies, which suggest their origin is different. Therefore, the HSFL formation mechanism cannot be described by the widely accepted interference model developed for describing LSFL formation.

Experiments have been performed at hybrid Ti:sapphire/KrF laser facility GARPUN-MTW to develop a novel technique to create a hollow-core sliding-mode plasma-filament waveguide for directed transfer of microwave radiation. Efficient multiphoton air ionization was produced by a train of picosecond 1-TW UV pulses at 248 nm wavelength, or by amplitude-modulated 100 ns pulse combining a short-pulse train with a free-running 1-GW pulse, which detached electrons off O2- ions. Multiple filamentation of UV laser radiation in air was observed, and filamentation theory based on resonance-enhanced ionization was developed to explain the experimental results.

A type of laser-induced surface relief nanostructure-the nanocrown-on thin metallic films was studied both experimentally and theoretically. The nanocrowns, representing a thin corrugated rim of resolidified melt and resembling well-known impact-induced water-crown splashes, were produced by single diffraction-limited nanosecond laser pulses on thin gold films of variable thickness on low-melting copper and high-melting tungsten substrates, providing different transient melting and adhesion conditions for these films. The proposed model of the nanocrown formation, based on a hydrodynamical (thermocapillary Marangoni) surface instability and described by a Kuramoto-Sivashinsky equation, envisions key steps of the nanocrown appearance and gives qualitative predictions of the acquired nanocrown parameters.

Femtosecond laser treatment of a glass surface was used to fabricate a multimodal roughness having regular surface ripples with a period of a few micrometers decorated by aggregates of nearly spherical nanoparticles. UV-ozone treatment followed by chemisorption of the appropriate functional fluorosilanes onto the textured surface makes it possible to fabricate a superhydrophobic coating with a specific surface resistance on the order of petaohms on a glass surface. The main advantage of the fabricated coating under severe operating conditions with abrasion loads is the significant durability of its electro-insulating properties. The longevity of the high surface resistivity, even on long-term contact with a water vapor-saturated atmosphere, is directly related to the peculiarities of the surface texture and ripple structure.

Separate nanoholes with the minimum size down to 35 nm (~λ/15) and nanohole arrays with the hole size about 100 nm (~λ/5) were fabricated in a 50 nm optically "thick" Au/Pd film, using single 532 nm pump nanosecond laser pulses focused to diffraction-limited spots by a specially designed apertureless dielectric fiber probe. Nanohole fabrication in the metallic film was found to result from lateral heat diffusion and center-symmetrical lateral expulsion of the melt by its vapor recoil pressure. The optimized apertureless dielectric microprobe was demonstrated to enable laser fabrication of deep through nanoholes.

Collinear cascaded mid-IR frequency conversion in a single nonlinear optical crystal was accomplished. Concurrent collinear generation of the sum frequency of multiline fundamental band carbon monoxide laser radiation as a first frequency conversion cascade resulted in collinear difference frequency generation within the 4.3 to 4.9 μm spectral range when mixing this sum frequency radiation with the fundamental one as the second cascade in the same ZnGeP(2) nonlinear optical crystal.

Removal rate, air shock, and ablative recoil pressure parameters were measured as a function of laser intensity I(peak) during nanosecond laser ablation of graphite. Surface vaporization of molten graphite at low intensities I(peak)<0.15 GW/cm(2) was observed to transform into its near-critical phase explosion (intense homogeneous boiling) at the threshold intensity I(PE)≈0.15 GW/cm(2) in the form of a drastic, correlated rise of removal rate, air shock, and ablative recoil pressure magnitudes. Just above this threshold (I(peak)≥0.25 GW/cm(2)), the explosive mass removal ended up with saturation of the removal rate, much slower increase of the air and recoil pressure magnitudes, and appearance of a visible surface plasma spark. In this regime, the measured far-field air shock pressure amplitude exhibits a sublinear dependence on laser intensity (∝I(peak)(4/9)), while the source plasma shock pressure demonstrates a sublinear trend (∝I(peak)(3/4)), both indicating the subcritical character of the plasma. Against expectations, in this regime the plasma recoil pressure increases versus I(peak) superlinearly (∝I(peak)(1.1)), rather than sublinearly (∝I(peak)(3/4)), with the mentioned difference related to the intensity-dependent initial spatial plasma dimensions within the laser waist on the graphite surface and to the plasma formation time during the heating laser pulse (overall, the pressure source effect). The strict coincidence of the phase explosion, providing high (kbar) hydrodynamic pressures of ablation products, and the ignition of ablative laser plasma in the carbon plume may indicate the ablative pressure-dependent character of the underlying optical breakdown at the high plume pressures, initiating the plasma formation. The experimental data evidence that the spatiotemporal extension of the plasma in the laser plume and ambient air during the heating laser pulse is supported by fast lateral electron and radiative heat conduction (laser-supported combustion wave regime), rather than by propagation of a strong shock wave (laser-supported detonation wave regime).