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Copper (Cu) oxide compounds (Cu

Gold nanoparticles play an important role in plasmonic arrays, including, but not limited to, photovoltaic, biomedical, sensing, optical, and catalytic applications. For plasmonic arrays, control o...

We present an alternative approach to dielectric meta-surfaces and demonstrate its scalability, mechanical durability and laser damage resilience. The process is based on laser raster-scan of a thin metal film on a glass, followed by dry-etching and removal of the metal nano-particles mask. We will present new approaches developed to “boost” the attainable optical response based on new underlying physics of the laser printed Au nanoparticle mask.

Generally, a high-temperature postannealing process is required to enhance the photoelectrochemical (PEC) performance of hematite nanorod (NR) photoanodes. However, the thermal annealing time is limited to a short duration as thermal annealing at high temperatures can result in some critical problems, such as conductivity degradation of the fluorine-doped tin oxide film and deformation of the glass substrate. In this study, selective laser processing is introduced for hematite-based PEC cells as an alternative annealing process. The developed laser-induced phase transformation (LIPT) process yields hematite NRs with enhanced optical, chemical, and electrical properties for application in hematite NR-based PEC cells. Owing to its improved properties, the LIPT-processed hematite NR PEC cell exhibits an enhanced water oxidation performance compared to that processed by the conventional annealing process. As the LIPT process is conducted under ambient conditions, it would be an excellent alternative annealing technique for heat-sensitive flexible substrates in the future.

Many optical applications that could potentially benefit from the design flexibility provided by the metasurface approach are being prohibited by the limited scalability of the fabrication and the robustness of the end-result structures when using a resonant meta-elements-based approach. An alternative demonstrated approach with superior scalability and robustness is substrate-engraved metasurfaces, based on medium mixing homogenization, yet it suffers from very limited optical response. Here we propose advancing this approach by coupling the metasurface with buried etalon layers, leading to enhancement in the optical response. A transfer matrix analysis is used to study the parameter space, predicting that the patterned reflectance values range of a beam shaper could be raised from only 4% to 30% when the metasurface is engraved in silica, and even up to 66% when engraved into higher-index oxides. Using the method proposed here, the phase difference range across the metasurface could be increased by 0.4 radians beyond the range achievable by a metasurface engraved in silica and could reach even higher values when embedded in higher-index materials. Full-wave numerical simulations are used to demonstrate a cylindrical metareflector and a metalens, further validating the analysis.

We present a method for producing spatially patterned glass engraved meta-surfaces, which is scalable, has high mechanical stability and high laser damage durability, and thus promising for ultra-thin optics implementation for high-power lasers. The process is based on laser raster-scan of a thin metal film on a glass, followed by dry-etching and removal of the metal mask. We present fabricated structures, characterization of their optical performance, mechanical stability and laser damage performance.

In pursuit of the elusive mechanism of high-TC superconductors (HTSC), spectroscopic imaging scanning tunneling microscopy (SI-STM) is an indispensable tool for surveying local properties of HTSC. ...

Here we demonstrate laser transmission welding of vertically aligned carbon nanotube (VACNT) arrays for joining polymer sheets. The unique characteristics of VACNTs make them suitable for use in laser welding. First, the excellent light absorption of the VACNTs induces selective heating at the contact plane with a polymer sheet, minimizing thermal damage to the polymer. Second, the porous and compliant structure of the VACNTs prevents the formation of air pockets inside the contact space. Successful welding is obtained when the laser irradiation power is at an optimal level, below which the adhesion is too weak and above which the excessive heat causes periodic damage along the scanning path. The optimized laser welding technique is expected to become a new method for implementing carbon nanotubes as mechanical linkers for various thermoplastic polymers.

Direct ink writing (DIW) three-dimensional (3D) printing provides a revolutionary approach to fabricating components with gradients in material properties. Herein, we report a method for generating colloidal germania feedstock and germania-silica inks for the production of optical quality germania-silica (GeO2-SiO2) glasses by DIW, making available a new material composition for the development of multimaterial and functionally graded optical quality glasses and ceramics by additive manufacturing. Colloidal germania and silica particles are prepared by a base-catalyzed sol-gel method and converted to printable shear-thinning suspensions with desired viscoelastic properties for DIW. The volatile solvents are then evaporated, and the green bodies are calcined and sintered to produce transparent, crack-free glasses. Chemical and structural evolution of GeO2-SiO2 glasses is confirmed by nuclear magnetic resonance, X-ray diffraction, and Raman spectroscopy. UV-vis transmission and optical homogeneity measurements reveal comparable performance of the 3D printed GeO2-SiO2 glasses to glasses produced using conventional approaches and improved performance over 3D printed TiO2-SiO2 inks. Moreover, because GeO2-SiO2 inks are compatible with DIW technology, they offer exciting options for forming new materials with patterned compositions such as gradients in the refractive index that cannot be achieved with conventional manufacturing approaches.

We present a simple and scalable method for the production of optics with incorporated metasurfaces, resulting in durable all-dielectric based meta-optics. The scalability and robustness of this method overcome limitations imposed by current technology when fabricating metasurfaces for high power laser applications, while the simplicity of the fabrication process makes it an exciting technique for metasurface generation. This talk will describe the method, show resultant fabricated metasurfaces and the sensitivity introduced by processing parameters – i.e. control over generated surfaces, and discuss the laser damage performance of these engineered large-scale metasurfaces.

Optical performance of anti-reflective random meta-surfaces are studied numerically for coherent beam propagation systems, such as lasers. A methodology for the modeling of such optics performance is developed and applied to study the reflectivity and laser beam quality degradation. These quantitative metrics and design considerations highlight that reducing the size of the meta-surface period much below the light wavelength is not necessarily required.

A key challenge for metasurface research is locally controlling at will the nanoscale geometric features on meter-scale apertures. Such a technology is expected to enable large aperture meta-optics and revolutionize fields such as long-range imaging, lasers, laser detection and ranging (LADAR), and optical communications. Furthermore, these applications are often more sensitive to light-induced and environmental degradation, which constrains the possible materials and fabrication process. Here, we present a relatively simple and scalable method to fabricate a substrate-engraved metasurface with locally printed index determined by induced illumination, which, therefore, addresses both the challenges of scalability and durability. In this process, a thin metal film is deposited onto a substrate and transformed into a mask via local laser-induced dewetting into nanoparticles. The substrate is then dry-etched through this mask, and selective mask removal finally reveals the metasurface. We show that masking by the local nanoparticle distribution, and, therefore, the local index, is dependent on the local light-induced dewetting temperature. We demonstrate printing of a free-form pattern engraved into a fused silica glass substrate using a laser raster scan. Large-scale spatially controlled engraving of metasurfaces has implications on other technological fields beyond optics, such as surface fluidics, acoustics, and thermomechanics.

Metasurfaces (MSs), or surfaces consisting of engineered spatially oriented sub-wavelength elements—also known as meta-atoms—are quickly becoming a burgeoning field of interest due to their seemingly unparalleled control over the propagation of light. This article will discuss the emergence of a MS technology that is based on dewetting thin metal films to form dry etching masks for MS fabrication. The novelty this process presents is the ability to spatially vary mask features—which translates into spatially varying index of the finished surface—in a way that, rather than writing subwavelength elements one-by-one, writes entire areas at once to provide a route to easily scale the process up to meter-sized optics. Glass-engraved MSs have shown to be laser damage resistant, with damage thresholds close to the parent substrate damage thresholds. Furthermore, these surfaces have proven to be mechanically durable and capable of handling normal loads two orders of magnitude higher than that of an average fingerprint pressure. This indicates that accidental handling contact is not detrimental to the MS optical performance. Also discussed are the foreseeable technological challenges, potential solutions for those obstacles, and some currently unexplored directions for future efforts.

This article summarizes recent research on laser-based processing of two-dimensional (2D) atomic layered materials, including graphene and transition-metal dichalcogenides (TMDCs). Ultrafast lasers offer unique processing routes that take advantage of distinct interaction mechanisms with 2D materials to enable extremely localized energy deposition. Experiments have shown that ablative direct patterning of graphene by ultrafast lasers can achieve resolutions of tens of nanometers, as well as single-step pattern transfer. Ultrafast lasers also induce non-thermal excitation mechanisms that are useful for the thinning of TMDCs to tune the 2D material bandgap. Laser-assisted site-specific doping was recently demonstrated and ultrafast laser radiation under ambient air environment could be used for the direct writing of high-quality graphene patterns on insulating substrates. This article concludes with an outlook on developing further advanced laser processing with scalability, in situ monitoring strategies, and potential applications.

Hollow cylindrical tubes grown directly from flat glass substrates as well as spherical glow-discharge-polymer substrates were made using two-photon polymerization. The tube diameters were as small...

A critical component for all high-power laser systems that is particularly susceptible to laser damage is the antireflective coating, which maximizes energy transmission and minimizes scattered and stray light. We demonstrate the ability to generate substrate-engraved nanostructured surfaces (NS) for scalable and designable antireflective (AR) coatings that are monolithic to the substrate and can handle peak power levels comparable to the bulk material. Experimentally measured reflectance from these fabricated structures has validated our effective index theory-based transmission matrix model, demonstrating the designability of the AR properties. Upon exposure to sufficiently high fluences, a new mode of damage, nanostructured surface damage, has been observed and is likely the result of thermally driven material reflow accompanied by plasma initiation on the nanostructured surface. At 1053 nm, nanostructured surface damage onsets at 39 J / c m 2 with sample cleaning and 74 J / c m 2 after laser conditioning—very close to the reference substrate at 81 J / c m 2 . At 351 nm we show damage onset of 30 J / c m 2 , with reference substrate material damage onset of 47 J / c m 2 . Therefore, damage is close to the bulk material and represents an improvement with respect to other methods. The nanostructured surfaces were found to be mechanically durable and able to withstand cleaning procedures with sonication. Under normal incidence mechanical testing with a 200 µm radius indenter tip, the AR performance of these nanostructured surfaces was minimally impacted at pressures orders of magnitude higher than an average fingerprint pressure—indicating that incidental handling contact will not affect NS structures. Mechanical damage is attributed to plastic compression, not fracturing of the NS features. We demonstrate for the first time, to the best of our knowledge, that NS AR coatings, despite being rich in etched surface features, can tolerate laser fluences comparable to unprocessed optical surfaces. Furthermore, laser-damage features of NS indicate a unique non-growing failure mode whereby following absorption the featureless damage site does not precipitate future damage growth, reducing considerably the burdens for managing optics processing in high-power laser systems.

Compared to tedious, multi-step treatments for electroless gold plating of traditional thermoplastics, this communication describes a simpler three-step procedure for 3D printed crosslinked polyacrylate substrates. This allows for the synthesis of ultralight gold foam microlattice materials with great potential for architecture-sensitive applications in future energy, catalysis, and sensing.

Wetting has been studied in various fields: chemical industry, automobile manufacturing, food companies, and even life sciences. In these studies, super-hydrophobic surfaces have been achieved through complex steps and processes. To realize super-hydrophobicity, however, we demonstrated a simple and single pass laser process for the fabrication of micro/nano hierarchical structures on the flexible polytetrafluoroethylene (PTFE, Teflon) surface. The fabricated hierarchical structures helped increase the hydrophobicity by augmenting the surface roughness and promoting air-trapping. In addition, we employed a low-cost and high-throughput replication process producing numerous polydimethylsiloxane (PDMS) replicas from the laser-processed PTFE film. Thanks to the anti-adhesive characteristics of PTFE and the elasticity of PDMS, the structure perfectly transferred to the replica without any mechanical failure. Moreover, our designed mesh patterns offered the possibility of large area applications through varying the process parameters (pitch, beam spot size, laser fluence, and scan speed). Even though mesh patterns had relatively large pitch (190 &mu, m), we were able to achieve high contact angle (&gt, 150&deg, ). Through pneumatically deformed structure, we clearly showed that the shape of the droplets on our laser-processed super-hydrophobic surface was spherical. Based on these outcomes, we can expect our single laser pulse exposure process can overcome many drawbacks and offer opportunities for advancing applications of the wetting phenomena.

This work is concerned with the kinetics of laser-induced reductive sintering of nonstoichiometric crystalline nickel oxide (NiO) nanoparticles (NPs) under ambient conditions. The mechanism of photophysical reductive sintering upon irradiation using a 514.5 nm continuous-wave (CW) laser on NiO NP thin films has been studied through modulating the laser power density and illumination time. Protons produced due to high-temperature decomposition of the solvent present in the NiO NP ink, oxygen vacancies in the NiO NPs, and electronic excitation in the NiO NPs by laser irradiation all affect the early stage of the reductive sintering process. Once NiO NPs are reduced by laser irradiation to Ni, they begin to coalesce, forming a conducting material. In situ optical and electrical measurements during the reductive sintering process take advantage of the distinct differences between the oxide and the metallic phases to monitor the transient evolution of the process. We observe four regimes: oxidation, reduction,...

We demonstrate the fabrication of flexible micro-supercapacitors based on laser carbonization of polyimide sheets. Localized pulsed laser irradiation rapidly converts the pristine polyimide surface into an electrically conductive porous carbon structure in ambient conditions. Thus, the polyimide sheet acts as both a precursor for the carbonization and a flexible substrate. Effects of various laser parameters are examined to enhance electrical properties and morphology of the carbonized structures. The interdigitated electrode patterns are produced directly on the polyimide sheets by programmed laser scanning. A solid-state polyvinyl alcohol–phosphoric acid gel electrolyte is introduced into the active electrode area to realize a flexible all solid-state microcapacitor assembly. Cyclic voltammetry measurements exhibit the expected electrical double layer behavior. The specific capacitance of the supercapacitors reaches ∼800 μF/cm2 at a voltage scan rate of 10 mV/s with good capacitance retention under mechanical bending. The proposed laser-based approach enables facile fabrication of flexible micro-supercapacitors without tedious photolithographic patterning of porous carbon and metal current collectors.

A robust, millimeter-sized low-density Cu foam with ∼90% (v/v) porosity, ∼30 nm thick walls, and ∼1 μm diameter spherical pores is prepared by the slip-casting of metal-coated polymer core-shell particles followed by a thermal removal of the polymer. In this paper, we report our key findings that enable the development of the low-density Cu foams. First, we need to synthesize polystyrene (PS) particles coated with a very thin Cu layer (in the range of tens of nanometers). A simple reduction in the amount of Cu deposited onto the PS was not sufficient to form such a low-density Cu foams due to issues related to foam collapse and densification upon the subsequent polymer removal step. Precise control over the morphology of the Cu coating on the particles is essential for the synthesis of a lower density of foams. Second, improving the dispersion of PS-Cu particles in a suspension used for the casting as well as careful optimization of a baking condition minimize the formation of irregular large voids, leading to Cu foams with a more uniform packing and a better connectivity of neighboring Cu hollow shells. Finally, we analyzed mechanical properties of the Cu foams with a depth-sensing indentation test. The uniform Cu foams show a significant improvement in mechanical properties (∼1.5× modulus and ∼3× hardness) compared to those of uncontrolled foam samples with a similar foam density but irregular large voids. Higher surface areas and a good electric conductivity of the Cu foams present a great potential to future applications.

The ablation of magnetron sputtered metal films on fused silica substrates by a 1053 nm, picosecond class laser was studied as part of a demonstration of its use for in-situ characterization of the laser spot under conditions commonly used at the sample plane for laser machining and damage studies. Film thicknesses were 60 and 120 nm. Depth profiles and SEM images of the ablation sites revealed several striking and unexpected features distinct from those typically observed for ablation of bulk metals. Very sharp thresholds were observed for both partial and complete ablation of the films. Partial film ablation was largely independent of laser fluence with a surface smoothness comparable to that of the unablated surface. Clear evidence of material displacement was seen at the boundary for complete film ablation. These features were common to a number of different metal films including Inconel on commercial neutral density filters, stainless steel, and aluminum. We will present data showing the morphology of the ablation sites on these films as well as a model of the possible physical mechanisms producing the unique features observed.

Transparent conducting films with superior laser damage performance have drawn intense interests toward optoelectronic applications under high energy density environment. In order to make optoelectronic applications with high laser damage performance, a fundamental understanding of damage mechanisms of conducting films is crucial. In this study, we performed laser damage experiments on tin-doped indium oxide films (ITO, Bandgap = 4.0 eV) using a nanosecond (ns) pulse laser (1064 nm) and investigated the underlying physical damage mechanisms. Single ns laser pulse irradiation on ITO films resulted in common thermal degradation features such as melting and evaporation although the laser photon energy (1.03 eV, 1064 nm) was smaller than the bandgap. Dominant laser energy absorption of the ITO film is attributed to free carriers due to degenerate doping. Upon multi-pulse irradiation on the film, damage initiation and growth were observed at lower laser influences, where no apparent damage was formed upon single pulse, suggesting a laser-induced incubation effect.

This study investigates the physical processes involved in picosecond pulse (20-28 ps FWHM) laser ablation of Al 6061, 316L stainless steel, and undoped crystalline Si (〈100〉) over a range of laser wavelength (355 nm and 1064 nm) and fluence (0.1-40 J/cm2). Experimental measurements of material ablation rate show enhanced removal at the 355 nm wavelength, primarily due to laser-plasma interaction (LPI) within the ablative plume that approaches an order of magnitude increase over the measured removal at 1064 nm. A transition in the ablation rate at 355 nm is identified around ∼10 J/cm2 above which the removal efficiency increases by a factor of two to three. Multi-physics radiation hydrodynamic simulations, considering LPI effects and utilizing a novel mixed-phase equation of state model, show that the transition in ablation efficiency is due to the onset of melt ejection through cavitation, where laser-driven shock heating sets the depth of melt penetration and the ensuing release wave from the ablation surface drives cavitation through the imposition of tensile strain within the melt. High-speed pump-probe imaging of the ejecta and ejecta collection studies, as well as scanning electron microscopy of the ablation craters, support the proposed cavitation mechanism in the higher fluence range. The ablation process is critically influenced by LPI effects and the thermophysical properties of the material.

An operando x-ray diffraction system is presented for elucidating optimal laser assisted chemical vapor deposition growth conditions. The technique is utilized to investigate deposition dynamics of boron-carbon materials using trimethyl borate precursor. Trimethyl borate exhibits vastly reduced toxicological and flammability hazards compared to existing precursors, but has previously not been applied to boron carbide growth. Crystalline boron-rich carbide material is produced in a narrow growth regime on addition of hydrogen during the growth phase at high temperature. The use of the operando x-ray diffraction system allows for the exploration of highly nonequilibrium conditions and rapid process control, which are not possible using ex situ diagnostics.

Micron-sized ablated surface structures with nano-sized 'bumpy' structures were produced by femtosecond (fs) laser ablation of polytetrafluoroethylene (PTFE) film under ambient conditions. Upon just a single step, the processed surface exhibited hierarchical micro/nano morphology. In addition, due to the tribological properties of PTFE, polydimethylsiloxane (PDMS) could be replicated from the laser-ablated PTFE surface without anti-adhesive surface treatment. By controlling the design of the ablated patterns, tunable wettability and superhydrophobicity were achieved on both PTFE and PDMS replica surfaces. Furthermore, using fs laser ablation direct writing, a flexible superhydrophobic PDMS cage formed by superhydrophobic patterns encompassing the unmodified region was demonstrated for aqueous droplet positioning and trapping. Through evaporation-driven colloidal self-assembly in this superhydrophobic cage, a colloidal droplet containing polystyrene (PS) particles dried into a self-assembled photonic crystal, whose optical band gap could be manipulated by the particle size.

We present two strategies to minimize laser damage in transparent conductive films. The first consists of improving heat dissipation by selection of substrates with high thermal diffusivity or by addition of capping layer heatsinks. The second is reduction of bulk energy absorption by lowering free carrier density and increasing mobility, while maintaining film conductance with thicker films. Multi-pulse laser damage tests were performed on tin-doped indium oxide (ITO) films configured to improve optical lifetime damage performance. Conditions where improvements were not observed are also described. When bulk heating is not the dominant damage process, discrete defect-induced damage limits damage behavior.

A laser damage test method based on damage size analysis (DSA) is described that simplifies the derivation of the lifetime optical damage threshold of film materials critical in the design of devices used in high-repetition-rate, high-power laser systems. The DSA method presented here is solely based on imaging to measure the damage site size produced from exposure to a known Gaussian-shaped beam with a fixed, systematically selected fluence well above the ablation threshold. The method locates the damage boundary produced from repeated exposures, using images with a high contrast, and maps it to the beam profile to extract a lifetime laser damage fluence threshold value. We validate the DSA approach using a few relevant transparent film material systems and by comparing it to the standard S/1 laser damage test method. The DSA method can be more efficient and accelerate materials development and validation necessary to support the design of high-power repetition-rated lasers and optoelectronic devices.

In this study, we investigated whether the optical and electrical properties of indium tin oxide (ITO) films are degraded under laser irradiation below their laser ablation threshold. While performing multi-pulse laser damage experiments on a single ITO film (4.7 ns, 1064 nm, 10 Hz), we examined the optical and electrical properties in situ. A decrease in reflectance was observed prior to laser damage initiation. However, under sub-damage threshold irradiation, conductivity and reflectance of the film were maintained without measurable degradation. This indicates that ITO films in optoelectronic devices may be operated below their lifetime laser damage threshold without noticeable performance degradation.

The optical damage performance of electrically conductive gallium nitride (GaN) and indium tin oxide (ITO) films is addressed using large area, high power laser beam exposures at 1064 nm sub-bandgap wavelength. Analysis of the laser damage process assumes that onset of damage (threshold) is determined by the absorption and heating of a nanoscale region of a characteristic size reaching a critical temperature. This model is used to rationalize semi-quantitatively the pulse width scaling of the damage threshold from picosecond to nanosecond timescales, along with the pulse width dependence of the damage threshold probability derived by fitting large beam damage density data. Multi-shot exposures were used to address lifetime performance degradation described by an empirical expression based on the single exposure damage model. A damage threshold degradation of at least 50% was observed for both materials. Overall, the GaN films tested had 5-10 × higher optical damage thresholds than the ITO films tested for comparable transmission and electrical conductivity. The route to optically robust, large aperture transparent electrodes and power optoelectronics may thus involve use of next generation widegap semiconductors such as GaN.

Laser damage mechanisms of two conductive wide-bandgap semiconductor films - indium tin oxide (ITO) and silicon doped GaN (Si:GaN) were studied via microscopy, spectroscopy, photoluminescence (PL), and elemental analysis. Nanosecond laser pulse exposures with a laser photon energy (1.03 eV, 1064 nm) smaller than the conductive films bandgaps were applied and radically different film damage morphologies were produced. The laser damaged ITO film exhibited deterministic features of thermal degradation. In contrast, laser damage in the Si:GaN film resulted in highly localized eruptions originating at interfaces. For ITO, thermally driven damage was related to free carrier absorption and, for GaN, carbon complexes were proposed as potential damage precursors or markers.

Irradiation of a thin film with a beam-shaped laser is proposed to achieve site-selectively controlled dewetting of the film into nanoscale structures. As a proof of concept, the laser-directed dewetting of an amorphous silicon thin film on a glass substrate is demonstrated using a donut-shaped laser beam. Upon irradiation of a single laser pulse, the silicon film melts and dewets on the substrate surface. The irradiation with the donut beam induces an unconventional lateral temperature profile in the film, leading to thermocapillary-induced transport of the molten silicon to the center of the beam spot. Upon solidification, the ultrathin amorphous silicon film is transformed to a crystalline silicon nanodome of increased height. This morphological change enables further dimensional reduction of the nanodome as well as removal of the surrounding film material by isotropic silicon etching. These results suggest that laser-based dewetting of thin films can be an effective way for scalable manufacturing of patterned nanostructures.