Terahertz beam with radial or orthogonal to laser polarization from a single-color femtosecond filament.

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.

Observation of conical emission from DC-biased filament at 10 THz.

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.

Pulse-width-dependent critical power for self-focusing of ultrashort laser pulses in bulk dielectrics.

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.

Broadband (8.5-13.5 µm) intra-pulse difference frequency generation in a LiGaS2 crystal of a 90 fs 744 nm laser pulse after its continuous redshift in air.

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 LiGaS2 crystal. The filamentation of the laser pulse in air provided its continuous spectral broadening to the Stokes wing with spectral humps separated by ∼1000cm-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.

Flat-top THz directional diagram of a DC-biased filament.

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≲1THz to the conical one at ν>8THz 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.

Controllable ablative machining of Al/Ti and Ti/Al nano-layers on a Si substrate by single-pulse femtosecond laser irradiation.

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.

IR femtosecond laser micro-filaments in diamond visualized by inter-band UV photoluminescence.

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.

Highly efficient stimulated Raman scattering of sub-picosecond laser pulses in BaWO4 for 10.6 µm difference frequency generation.

Transient stimulated Raman scattering (SRS) of 0.3 ps 515 nm laser pulses in ${\rm BaWO_4}$BaWO4 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 ${{\rm CO}_2}$CO2 laser amplifier via difference frequency generation in ${{\rm LiGaS}_2}$LiGaS2 crystal was numerically verified.

Frequency conversion of mid-IR lasers into the long-wavelength domain of 12-20 µm with AgGaSe2, BaGa2GeSe6 and PbIn6Te10 nonlinear crystals.

Difference frequency generation under mixing of repetitively-pulsed CO- and CO2-laser radiation in AgGaSe2, BaGa2GeSe6 and PbIn6Te10 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 PbIn6Te10 crystal, which is an order of magnitude higher than previous results.

Symmetry-wise nanopatterning and plasmonic excitation of ring-like gold nanoholes by structured femtosecond laser pulses with different polarizations.

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.

Verification of an integral figure of merit for mid-IR nonlinear crystals.

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 ZnGeP2, BaGa2GeSe6, AgGaSe2, GaSe, and PbIn6Te10 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.

Three-stage frequency conversion of sub-microsecond multiline CO laser pulse in a single ZnGeP2 crystal.

Broadband three-stage frequency conversion of multiline sub-microsecond CO laser radiation in a single sample of ZnGeP2 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.

Sum frequency generation of multi-line slab radio frequency discharge carbon monoxide laser system with intracavity nonlinear BaGa2GeSe6 crystal.

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.

Fifteen meter long uninterrupted filaments from sub-terawatt ultraviolet pulse in air.

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.

Frequency tunable CO laser operating on the highest vibrational transition with wavelength of 8.7 µm.

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.

Multi-beam pulsed-laser patterning of plasmonic films using broadband diffractive optical elements.

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.

Frequency conversion of molecular gas lasers in PbIn6Te10 crystal within mid-IR range.

PbIn6Te10 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.

Broadband two-stage frequency conversion of CO laser in AgGaSe(2) crystal.

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 AgGaSe2 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 AgGaSe2 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%.

Dynamic polarization flip in nanoripples on photoexcited Ti surface near its surface plasmon resonance.

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 mode-locked and Q-switched CO laser radiation with efficiency up to 37%.

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.