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HighlightsUltrafast laser-induced nano-topography modifications: generation of highly concentrated 20 nm diameter nanowells on the surface with expected applications for storage of chemical and biological active species and for blocking crack propagation.Ultrafast laser-induced structural modifications: turning of a metallic glass to a composite material of monoclinic zirconia crystallites embedded inside amorphous metallic glass.A flexible one-step laser irradiation process without direct mechanical contact for thin film metallic glasses surface functionalization.We present an effective approach for fabricating nanowell arrays in a one-step laser process with promising applications for the storage and detection of chemical or biological elements. Biocompatible thin films of metallic glasses are manufactured with a selected composition of Zr65Cu35, known to exhibit remarkable mechanical properties and glass forming ability. Dense nanowell arrays spontaneously form in the ultrafast laser irradiation spot with dimensions down to 20 nm. The flared shape observed by transmission electron microscopy is ideal to ensure chemical or biological material immobilization into the nanowells. This also indicates that the localization of the cavitation-induced nanopores can be tuned by the density and size of the initial nanometric interstice from the columnar structure of films deposited by magnetron sputtering. In addition to the topographic functionalization, the laser-irradiated amorphous material exhibits structural changes analyzed by spectroscopic techniques at the nanoscale such as energy-dispersive X-ray spectroscopy and electron energy loss spectroscopy. Results reveal structural changes consisting of nanocrystals of monoclinic zirconia that grow within the amorphous matrix. The mechanism is driven by local oxidation process catalyzed by extreme temperature and pressure conditions estimated by an atomistic simulation of the laser-induced nanowell formation.

Using coupled electromagnetic and hydrodynamic calculations, we elucidate theoretically the topographic transition from a random metallic surface to a periodic sub-wavelength grating by ultrashort laser ablation. The origin of this transition lies in the successive selection of hybrid surface waves scattered by random nanoholes. Contrary to the common belief that surface plasmon polaritons play the dominant role in the process and define the grating periodicity, we show that both quasi-cylindrical and surface plasmon waves are involved, whereas the diversity in the resulting spacings /2– ( is the laser wavelength) is the manifestation of a broad frequency overlap of these waves, controlled by their relative phase shifts with respect to the plasmonic counterparts. The topography evolution imposes the dominant contribution to the surface sub-wavelength pattern by selecting the appropriate wave character from plasmonic modes to evanescent cylindrical waves. With the radiation dose, the grating periodicity exhibits a pronounced blue shift due to reinforced dipole–dipole coupling between the nanoholes and surface curvatures in the laser-processed area. This allows the creation of regular patterns with tunable periodicity.

A laser-irradiated surface is the paradigm of a self-organizing system, as coherent, aligned, chaotic, and complex patterns emerge at the microscale and even the nanoscale. A spectacular manifestation of dissipative structures consists of different types of randomly and periodically distributed nanostructures that arise from a homogeneous metal surface. The noninstantaneous response of the material reorganizes local surface topography down to tens of nanometers scale modifying long-range surface morphology on the impact scale. Under ultrafast laser irradiation with a regulated energy dose, the formation of nanopeaks, nanobumps, nanohumps and nanocavities patterns with 20–80 nm transverse size unit and up to 100 nm height are reported. We show that the use of crossed-polarized double laser pulse adds an extra dimension to the nanostructuring process as laser energy dose and multi-pulse feedback tune the energy gradient distribution, crossing critical values for surface self-organization regimes. The tiny dimensions of complex patterns are defined by the competition between the evolution of transient liquid structures generated in a cavitation process and the rapid resolidification of the surface region. Strongly influencing the light coupling, we reveal that initial surface roughness and type of roughness both play a crucial role in controlling the transient emergence of nanostructures during laser irradiation.

The capacity to synthesize and design highly intricated nanoscale objects of different sizes, surfaces, and shapes dramatically conditions the development of multifunctional nanomaterials. Ultrafast laser technology holds great promise as a contactless process able to rationally and rapidly manufacture complex nanostructures bringing innovative surface functions. The most critical challenge in controlling the growth of laser‐induced structures below the light diffraction limit is the absence of external order associated to the inherent local interaction due to the self‐organizing nature of the phenomenon. Here high aspect‐ratio nanopatterns driven by near‐field surface coupling and architectured by timely‐controlled polarization pulse shaping are reported. Electromagnetic coupled with hydrodynamic simulations reveal why this unique optical manipulation allows peaks generation by inhomogeneous local absorption sustained by nanoscale convection. The obtained high aspect‐ratio surface nanotopography is expected to prevent bacterial proliferation, and have great potential for catalysis, vacuum to deep UV photonics and sensing. A uniform formation of unconventional self‐organized patterns on the 100 nm scale has been generated by focused ultrafast light. Irradiated surface turns to a forest of self‐organized nanopeaks with a remarkable aspect ratio at the nanoscale. Laser beam polarization is timely controlled to prevent anisotropic energy absorption and to synchronize the laser energy delivery rate with the material dynamic response.

The presence of surface oxides on the formation of laser-induced periodic surface structures (LIPSS) is regularly advocated to favor or even trigger the formation of high-spatial-frequency LIPSS (HSFL) during ultrafast laser-induced nano-structuring. This paper reports the effect of the laser texturing environment on the resulting surface oxides and its consequence for HSFLs formation. Nanoripples are produced on tungsten samples using a Ti:sapphire femtosecond laser under atmospheres with varying oxygen contents. Specifically, ambient, 10 mbar pressure of air, nitrogen and argon, and 10−7 mbar vacuum pressure are used. In addition, removal of any native oxide layer is achieved using plasma sputtering prior to laser irradiation. The resulting HSFLs have a sub-100 nm periodicity and sub 20 nm amplitude. The experiments reveal the negligible role of oxygen during the HSFL formation and clarifies the significant role of ambient pressure in the resulting HSFLs period.

Surface nanostructuring by femtosecond laser is an efficient way to manipulate surface topography, creating advanced functionalities of irradiated materials. Thin-film metallic glasses obtained by physical vapor deposition exhibit microstructures free from grain boundaries, crystallites and dislocations but also characterized by a nanometric surface roughness. These singular properties make them more resilient to other metals to form laser-induced nanopatterns. Here we investigate the morphological response of Zr65Cu35 alloys under ultrafast irradiation with multipulse feedback. We experimentally demonstrate that the initial columnar microstructure affects the surface topography evolution and conditions the required energy dose to reach desired structures in the nanoscale domain. Double pulses femtosecond laser irradiation is also shown to be an efficient strategy to force materials to form uniform nanostructures even when their thermomechanical properties have a poor predisposition to generate them.

A self-organization hydrodynamic process has recently been proposed to partially explain the formation of femtosecond laser-induced nanopatterns on Nickel, which have important applications in optics, microbiology, medicine, etc. Exploring laser pattern space is difficult, however, which simultaneously (i) motivates using machine learning (ML) to search for novel patterns and (ii) hinders it, because of the few data available from costly and time-consuming experiments. In this paper, we use ML to predict novel patterns by integrating partial physical knowledge in the form of the Swift-Hohenberg (SH) partial differential equation (PDE). To do so, we propose a framework to learn with few data, in the absence of initial conditions, by benefiting from background knowledge in the form of a PDE solver. We show that in the case of a self-organization process, a feature mapping exists in which initial conditions can safely be ignored and patterns can be described in terms of PDE parameters alone, which drastically simplifies the problem. In order to apply this framework, we develop a second-order pseudospectral solver of the SH equation which offers a good compromise between accuracy and speed. Our method allows us to predict new nanopatterns in good agreement with experimental data. Moreover, we show that pattern features are related, which imposes constraints on novel pattern design, and suggest an efficient procedure of acquiring experimental data iteratively to improve the generalization of the learned model. It also allows us to identify the limitations of the SH equation as a partial model and suggests an improvement to the physical model itself.

Vanadium dioxide (VO2) with an insulator-to-metal (IMT) transition (∼68 °C) is considered a very attractive thermochromic material for smart window applications. Indeed, tailoring and understanding the thermochromic and surface properties at lower temperatures can enable room-temperature applications. The effect of W doping on the thermochromic, surface, and nanostructure properties of VO2 thin film was investigated in the present proof. W-doped VO2 thin films with different W contents were deposited by pulsed laser deposition (PLD) using V/W (+O2) and V2O5/W multilayers. Rapid thermal annealing at 400–450 °C under oxygen flow was performed to crystallize the as-deposited films. The thermochromic, surface chemistry, structural, and morphological properties of the thin films obtained were investigated. The results showed that the V5+ was more surface sensitive and W distribution was homogeneous in all samples. Moreover, the V2O5 acted as a W diffusion barrier during the annealing stage, whereas the V+O2 environment favored W surface diffusion. The phase transition temperature gradually decreased with increasing W content with a high efficiency of −26 °C per at. % W. For the highest doping concentration of 1.7 at. %, VO2 showed room-temperature transition (26 °C) with high luminous transmittance (62%), indicating great potential for optical applications.

New synthesis routes to tailor graphene properties by controlling the concentration and chemical configuration of dopants show great promise. Herein we report the direct reproducible synthesis of 2-3% nitrogen-doped ‘few-layer’ graphene from a solid state nitrogen carbide a-C:N source synthesized by femtosecond pulsed laser ablation. Analytical investigations, including synchrotron facilities, made it possible to identify the configuration and chemistry of the nitrogen-doped graphene films. Auger mapping successfully quantified the 2D distribution of the number of graphene layers over the surface, and hence offers a new original way to probe the architecture of graphene sheets. The films mainly consist in a Bernal ABA stacking three-layer architecture, with a layer number distribution ranging from 2 to 6. Nitrogen doping affects the charge carrier distribution but has no significant effects on the number of lattice defects or disorders, compared to undoped graphene synthetized in similar conditions. Pyridinic, quaternary and pyrrolic nitrogen are the dominant chemical configurations, pyridinic N being preponderant at the scale of the film architecture. This work opens highly promising perspectives for the development of self-organized nitrogen-doped graphene materials, as synthetized from solid carbon nitride, with various functionalities, and for the characterization of 2D materials using a significant new methodology.

Vanadium dioxide (VO ) with an insulator-to-metal (IMT) transition (∼68 °C) is considered a very attractive thermochromic material for smart window applications. Indeed, tailoring and understanding the thermochromic and surface properties at lower temperatures can enable room-temperature applications. The effect of W doping on the thermochromic, surface, and nanostructure properties of VO thin film was investigated in the present proof. W-doped VO thin films with different W contents were deposited by pulsed laser deposition (PLD) using V/W (+O ) and V O /W multilayers. Rapid thermal annealing at 400-450 °C under oxygen flow was performed to crystallize the as-deposited films. The thermochromic, surface chemistry, structural, and morphological properties of the thin films obtained were investigated. The results showed that the V was more surface sensitive and W distribution was homogeneous in all samples. Moreover, the V O acted as a W diffusion barrier during the annealing stage, whereas the V+O environment favored W surface diffusion. The phase transition temperature gradually decreased with increasing W content with a high efficiency of -26 °C per at. % W. For the highest doping concentration of 1.7 at. %, VO showed room-temperature transition (26 °C) with high luminous transmittance (62%), indicating great potential for optical applications.