10-million-elements-per-second printing of infrared-resonant plasmonic arrays by multiplexed laser pulses.

We report on high-quality infrared (IR)-resonant plasmonic nanoantenna arrays fabricated on a thin gold film by tightly focused femtosecond (fs) laser pulses coming at submegahertz repetition rates at a printing rate of 10 million elements per second. To achieve this, the laser pulses were spatially multiplexed by fused silica diffractive optical elements into 51 identical submicrometer-sized laser spots arranged into a linear array at periodicity down to 1 µm. The demonstrated high-throughput nanopatterning modality indicates fs laser maskless microablation as an emerging robust, flexible, and competitive lithographic tool for advanced fabrication of IR-range plasmonic sensors for environmental sensing, chemosensing, and biosensing.

Ultrafast laser printing of self-organized bimetallic nanotextures for multi-wavelength biosensing.

Surface-enhanced spectroscopy (SES) techniques, including surface-enhanced photoluminescence (SEPL), Raman scattering (SERS) and infrared absorption (SEIRA), represent powerful biosensing modalities, allowing non-invasive label-free identification of various molecules and quantum emitters in the vicinity of nanotextured surfaces. Enhancement of multi-wavelength (vis-IR) excitation of analyte molecules of interest atop a single textured substrate could pave the way toward ultimate chemosensing performance and further widespread implementation of the SES-based approaches in various crucial areas, such as point-ofcare diagnostics. In this paper, an easy-to-implement ultrafast direct laser printing via partial spallation of thermally-thick silver films and subsequent large-scale magnetron deposition of nanometer-thick Au layers of variable thickness was implemented to produce bimetallic textured surfaces with the cascaded nanotopography. The produced bimetallic textures demonstrate the strong broadband plasmonic response over the entire visible spectral range. Such plasmonic performance was confirmed by convenient spectroscopy-free Red-Green-Blue (RGB) color analysis of the dark-field (DF) scattering images supported by numerical calculations of the electromagnetic (EM) "near-fields", as well as comprehensive DF spectroscopic characterization. Bimetallic laser-printed nanotextures, which can be easily printed at ultrafast (square millimeters per second) rate, using galvanometric scanning, exhibited strong enhancement of the SEPL (up to 75-fold) and SERS (up to 106 times) yields for the organic dye molecules excited at various wavelengths. Additionally, comprehensive optical and sensing characterization of the laser-printed bimetallic surface structures allows substantiating the convenient spectroscopy-free RGB color analysis as a valuable tool for predictive assessment of the plasmonic properties of the various irregularly and quasi-periodically nanotextured surfaces.

Mapping the refractive index with single plasmonic nanoantenna.

As the size of the state-of-the-art optical devices shrinks to nanoscale, the need for tools allowing mapping the local optical properties at deep sub-diffraction resolution increases. Here we demonstrate successful mapping the variations of the refractive index of a smooth dielectric surface by detecting spectral response of a single spherical-shape Ag nanoparticle optically aligned with a supporting optical fiber axicon microlens. We propose and examine various excitation schemes of the plasmonic nanoantenna to provide efficient interaction of its dipolar and quadrupolar modes with the underlying sample surface and to optimize the mapping resolution and sensitivity. Moreover, we demonstrate an lithography-free approach for fabrication of the scanning probe combining the high-quality fiber microaxicon with the Ag spherical nanoparticle atop. Supporting finite-difference time-domain calculations are undertaken to tailor the interaction of the plasmonic nanoantenna and the underlying dielectric substrate upon various excitation conditions demonstrating good agreement with our experimental findings and explaining the obtained results.

Zero-orbital-angular-momentum laser printing of chiral nanoneedles.

Laser irradiation of various materials including metals, polymers, and semiconductors with vortex beams was previously shown to "twist" transiently molten matter providing the direct easy-to-implement way to obtain chiral surface relief. Specifically for metals, this effect was attributed to transfer of an orbital angular momentum (OAM) carried by a vortex beam. In this Letter, we report the formation of twisted metallic nanoneedles on surfaces of silver and gold films under their irradiation by a zero-OAM laser beam with a spiral-shaped intensity distribution. Our comparative experiments clearly demonstrate, for the first time to the best of our knowledge, that the formation of the chiral nanoneedles on the noble-metal films is mainly governed by the temperature-gradient-induced chiral thermocapillary mass transfer, rather than by OAM-driven rotation of the molten matter.

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.

Direct laser printing of chiral plasmonic nanojets by vortex beams.

Donut-shaped laser radiation, carrying orbital angular momentum, namely optical vortex, was recently shown to provide vectorial mass transfer, twisting transiently molten material and producing chiral micro-scale structures on surfaces of different bulk materials upon their resolidification. In this paper, we show that at high-NA focusing nanosecond laser vortices can produce chiral nanoneedles (nanojets) of variable size on thin films of such plasmonic materials, as silver and gold films, covering thermally insulating substrates. Main geometric parameters of the produced chiral nanojets, such as height and aspect ratio, were shown to be tunable in a wide range by varying metal film thickness, supporting substrates, and the optical size of the vortex beam. Donut-shaped vortex nanosecond laser pulses, carrying two vortices with opposite handedness, were demonstrated to produce two chiral nanojets twisted in opposite directions. These results suggest optical interference of the incident and reflected laser beams as a source of complex surface intensity distributions in metal films, possessing spiral components and driving both center-symmetric and spiral thermocapillary melt flows to yield in frozen nanoneedles with their pre-determined spiral nanocarving.

Laser printing of resonant plasmonic nanovoids.

Hollow reduced-symmetry resonant plasmonic nanostructures possess pronounced tunable optical resonances in the UV-vis-IR range, being a promising platform for advanced nanophotonic devices. However, the present fabrication approaches require several consecutive technological steps to produce such nanostructures, making their large-scale fabrication rather time-consuming and expensive. Here, we report on direct single-step fabrication of large-scale arrays of hollow parabolic- and cone-shaped nanovoids in silver and gold thin films, using single-pulse femtosecond nanoablation at high repetition rates. The lateral and vertical size of such nanovoids was found to be laser energy-tunable. Resonant light scattering from individual nanovoids was observed in the visible spectral range, using dark-field confocal microspectroscopy, with the size-dependent resonant peak positions. These colored geometric resonances in far-field scattering were related to excitation and interference of transverse surface plasmon modes in nanovoid shells. Plasmon-mediated electromagnetic field enhancement near the nanovoids was evaluated via finite-difference time-domain calculations for their model shapes simulated by three-dimensional molecular dynamics, and experimentally verified by means of photoluminescence microscopy and Raman spectroscopy.

Modeling of surface plasmon resonance in metalized optical waveguides with low V number by eigenmode expansion method.

The paper reports on the numerical study of surface plasmon resonance excitation in a bent metal-coated single mode optical fiber with a low V-number. It was shown that by choosing a proper combination of normalized frequency, bend radius, and metal film thickness one can achieve strong coupling between the fundamental mode guided by the fiber core, and symmetric surface plasmon mode supported by the metal layer applied to the fiber cladding. The effect is demonstrated to allow precision refractive index measurement, with spectral sensitivity and resolution estimated at 70 µm/refractive index unit and 3⋅10(-7), respectively.

Flash-imprinting of intense femtosecond surface plasmons for advanced nanoantenna fabrication.

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.

Analysis of surface plasmon resonance in bent single-mode waveguides with metal-coated cladding by eigenmode expansion method.

A numerical study is presented of surface plasmon waves excitation in a metal film applied to the cladding of a standard bent single-mode optical fiber. It was shown that by adjusting the bend radius and metal film thickness one can achieve effective coupling between the fiber fundamental mode and symmetric surface plasmon mode through the intermediary of whispering gallery modes supported by the cladding of the bent fiber. This effect is demonstrated to allow for refractometric measurement both in the wavelength and intensity-modulated regimes with a resolution of up to 10⁻8 RIU. Usage of standard noise reduction techniques for intensity-modulated optical signals promises further increase in accuracy.

Formation of crownlike and related nanostructures on thin supported gold films irradiated by single diffraction-limited nanosecond laser pulses.

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.

High-quality fiber microaxicons fabricated by a modified chemical etching method for laser focusing and generation of Bessel-like beams.

The fabrication method of the high-quality fiber microaxicons (FMAs) on the endface of the optical fiber was developed. Using several types of the commercially available optical fibers we experimentally demonstrated the fabrication of a high-quality FMA focusing a laser beam into a tiny spot with a FWHM≈0.6λ and Bessel-like field distribution. It was also demonstrated that choosing the appropriate chemical composition of the etching solution makes it possible to change the shape of the FMA tip from conical to hemispherical. This allows one to change the spatial distribution of the output laser beam, which can represent both the Bessel-like beam with a depth of focus of up to 49λ and a very tiny focal spot close to the diffraction limit size. Experimentally measured focusing characteristics of the fabricated FMAs obtained using a homemade collection-mode scanning near-field optical microscope setup demonstrate good agreement with numerical simulations based on the 3D finite-difference time-domain simulations.

Through nanohole formation in thin metallic film by single nanosecond laser pulses using optical dielectric apertureless probe.

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.

Cavity-based Fabry-Perot probe with protruding subwavelength aperture.

We investigate numerically and experimentally the possibility of development of a cavity-based probe for near-field optical microscopy systems based on a fiber Fabry-Perot interferometer with a subwavelength protruding aperture. It was shown that the probe provides a spatial resolution of no worse than λ/37 for λ=1550 nm.