Noble-Metal Nanoparticle-Embedded Silicon Nanogratings via Single-Step Laser-Induced Periodic Surface Structuring.

Here, we show that direct femtosecond laser nanostructuring of monocrystalline Si wafers in aqueous solutions containing noble-metal precursors (such as palladium dichloride, potassium hexachloroplatinate, and silver nitrate) allows for the creation of nanogratings decorated with mono- (Pd, Pt, and Ag) and bimetallic (Pd-Pt) nanoparticles (NPs). Multi-pulse femtosecond-laser exposure was found to drive periodically modulated ablation of the Si surface, while simultaneous thermal-induced reduction of the metal-containing acids and salts causes local surface morphology decoration with functional noble metal NPs. The orientation of the formed Si nanogratings with their nano-trenches decorated with noble-metal NPs can be controlled by the polarization direction of the incident laser beam, which was justified, for both linearly polarized Gaussian and radially (azimuthally) polarized vector beams. The produced hybrid NP-decorated Si nanogratings with a radially varying nano-trench orientation demonstrated anisotropic antireflection performance, as well as photocatalytic activity, probed by SERS tracing of the paraaminothiophenol-to-dimercaptoazobenzene transformation. The developed single-step maskless procedure of liquid-phase Si surface nanostructuring that proceeds simultaneously with the localized reduction of noble-metal precursors allows for the formation of hybrid Si nanogratings with controllable amounts of mono- and bimetallic NPs, paving the way toward applications in heterogeneous catalysis, optical detection, light harvesting, and sensing.

Investigation of Laser-Induced Periodic Surface Structures Using Synthetic Optical Holography.

In this paper, the investigation of laser-induced periodic surface structures (LIPSSs) on a polycrystalline diamond substrate using synthetic optical holography (SOH) is demonstrated. While many techniques for LIPSS detection operate with sample contact and/or require preparation or processing of the sample, this novel technique operates entirely non-invasively without any processing of or contact with the LIPSS sample at all. The setup provides holographic amplitude and phase images of the investigated sample with confocally enhanced and diffraction-limited lateral resolution, as well as three-dimensional surface topography images of the periodic structures via phase reconstruction with one single-layer scan only.

Deep Subwavelength Laser-Induced Periodic Surface Structures on Silicon as a Novel Multifunctional Biosensing Platform.

Strong light localization inside the nanoscale gaps provides remarkable opportunities for creation of various medical and biosensing platforms stimulating an active search for inexpensive and easily scalable fabrication at a sub-100 nm resolution. In this paper, self-organized laser-induced periodic surface structures (LIPSSs) with the shortest ever reported periodicity of 70 ± 10 nm were directly imprinted on the crystalline Si wafer upon its direct femtosecond-laser ablation in isopropanol. Appearance of such a nanoscale morphology was explained by the formation of a periodic topography on the surface of photoexcited Si driven by interference phenomena as well as subsequent down-scaling of the imprinted grating period via Rayleigh-Taylor hydrodynamic instability. The produced deep subwavelength LIPSSs demonstrate strong anisotropic anti-reflection performance, ensuring efficient delivery of the incident far-field radiation to the electromagnetic "hot spots" localized in the Si nanogaps. This allows realization of various optical biosensing platforms operating via strong interactions of quantum emitters with nanoscale light fields. The demonstrated 80-fold enhancement of spontaneous emission from the attached nanolayer of organic dye molecules and in situ optical tracing of catalytic molecular transformations substantiate bare and metal-capped deep subwavelength Si LIPSSs as a promising inexpensive multifunctional biosensing platform.

Laser Printing of Plasmonic Nanosponges.

Three-dimensional porous nanostructures made of noble metals represent novel class of nanomaterials promising for nonlinear nanooptics and sensors. Such nanostructures are typically fabricated using either reproducible yet time-consuming and costly multi-step lithography protocols or less reproducible chemical synthesis that involve liquid processing with toxic compounds. Here, we combined scalable nanosecond-laser ablation with advanced engineering of the chemical composition of thin substrate-supported Au films to produce nanobumps containing multiple nanopores inside. Most of the nanopores hidden beneath the nanobump surface can be further uncapped using gentle etching of the nanobumps by an Ar-ion beam to form functional 3D plasmonic nanosponges. The nanopores 10-150 nm in diameter were found to appear via laser-induced explosive evaporation/boiling and coalescence of the randomly arranged nucleation sites formed by nitrogen-rich areas of the Au films. Density of the nanopores can be controlled by the amount of the nitrogen in the Au films regulated in the process of their magnetron sputtering assisted with nitrogen-containing discharge gas.

Three-Step Description of Single-Pulse Formation of Laser-Induced Periodic Surface Structures on Metals.

Two different scenarios are usually invoked in the formation of femtosecond Laser-Induced Periodic Surface Structures (LIPSS), either "self-organization" mechanisms or a purely "plasmonic" approach. In this paper, a three-step model of formation of single-laser-shot LIPSS is summarized. It is based on the periodic perturbation of the electronic temperature followed by an amplification, for given spatial periods, of the modulation in the lattice temperature and a final possible relocation by hydrodynamic instabilities. An analytical theory of the evolution of the temperature inhomogeneities is reported and supported by numerical calculations on the examples of three different metals: Al, Au, and Mo. The criteria of the possibility of hydrodynamic instabilities are also discussed.

Two-photon polymerization with diode lasers emitting ultrashort pulses with high repetition rate.

In this Letter, we investigate the resolution of two-photon polymerization (2PP) with an amplified mode-locked external cavity diode laser with adjustable pulse length and a high repetition rate. The experimental results are analyzed with a newly developed 2PP model. Even with low pulse peak intensity, the produced structural dimensions are comparable to those generated by traditional 2PP laser sources. Thus, we show that a compact monolithic picosecond laser diode without amplification and with a repetition rate in the GHz regime can also be applied for 2PP. These results show the high application potential of compact mode-locked diode lasers for low-cost and compact 2PP systems.

Influence of defects on structural colours generated by laser-induced ripples.

The colourisation of metallic surface which appears due to periodic surface patterns induced by ultrashort laser pulses is studied. Ripples due to the sub-micrometer size of their period act as a diffraction grating, generating structural colours. Carefully chosen strategy of the laser spot scanning allows us to mimic the nanostructures responsible for structural colours of some flowers on the metal substrate. We investigate the correlation between the colourising effects and the artificially-induced defects in the ripples structure and show that these defects can make the colours observable in a larger range of viewing angles. Further we address the influence of the processing parameters on the spectral profile of the reflected light.

Generation of bioinspired structural colors via two-photon polymerization.

Colors of crystals, pigments, metals, salt solutions and bioluminescence occur in nature due to the optical properties of electrons in atoms and molecules. However, colors can also result from interference effects on nanostructures. In contrast to artificial coloration, which are caused by well-defined regular structures, the structural colors of living organisms are often more intense and almost angle-independent. In this paper, we report the successful manufacturing of a lamellar nanostructure that mimics the ridge shape of the Morpho butterfly using a 3d-direct laser writing technique. The viewing angle dependency of the color was analyzed via a spectrometer and the structure was visualized using a scanning electron microscope. The generated nano- and micro-structures and their optical properties were comparable to those observed in the Morpho butterfly.

Synthesis of Magnetic Nanoparticles by Ultrashort Pulsed Laser Ablation of Iron in Different Liquids.

Magnetic nanoparticles were generated by ultrashort pulsed laser ablation of an iron target in water, methanol, ethanol, acetone and toluene. The relationship between ablation rate, liquid properties and the physical and chemical properties of the nanoparticles was studied. Composition, morphology and magnetic properties were investigated by TEM, XPS and vibrating-sample (VSM) and SQUID magnetometry. The properties of the generated nanoparticle ensembles reflected the influence of the liquid environment on the particle formation process. For example, the composition was strongly dependent on the carbon to oxygen ratio within the molecules of the liquid. In contrast to short pulsed laser ablation in liquids, the nanoparticles generated by ultrashort pulses had a higher level of polycrystallinity.

The production of free-standing large aspect ratio metal nanofilms by femtosecond laser separation.

We demonstrate a new method for the production of free-standing metal films of thickness down to several tens of nanometres. Films of different metals as well as multilayer structures have been produced by means of femtosecond laser-induced separation of evaporated layers from a plane glass surface. This technology enables the production of large-area films with different properties for optical or nanotechnological applications. We study the properties of the film and demonstrate the possibility of high-pass filtering of electrons with an energy of several keV by means of the free-standing films. The physical mechanisms leading to the film separation under femtosecond laser radiation are discussed.

Dewetting of liquid filaments in wedge-shaped grooves.

The dewetting of liquid filaments in linear grooves of a triangular cross section is studied experimentally and theoretically. Homogeneous filaments of glassy polystyrene (PS) are prepared in triangular grooves in a nonequilibrium state. At elevated temperatures, the molten PS restores its material contact angle with the substrate. Liquid filaments with a convex liquid-vapor interface decay into isolated droplets with a characteristic spacing depending on the wedge geometry, wettability, and filament width. This instability is driven by the interplay of local filament width and Laplace pressure and constitutes a wide class of 1D instabilities that also include the Rayleigh-Plateau instability as a special case. Our results show an accurately exponential buildup of the instability, suggesting that fluctuations have a minor influence in our system.