Laser-assisted direct roller imprinting of large-area microstructured optical surfaces.

In this study, a high-throughput fabrication method called laser-assisted direct roller imprinting (LADRI) was developed to lower the cost of nanoimprinting large-area polymer films and to address problems associated with nanoimprinting, namely, microstructural damage and precision in flatness of entire film. With LADRI, the laser directly heats the microstructured surface of the roller mold, which heats and melts the surface of a polymethyl methacrylate (PMMA) film to replicate the microstructures on the mold rapidly. In this study, the effects of laser power density, scanning speed, size of the microstructures, and contact pressure on the replication speed were investigated experimentally. The replication speed increased as the power and scanning speed increased. However, because the film required heating until it filled the entire depth of the microstructure, an appropriate replication speed was necessary. This result was supported by simulation of the temperature distribution inside the mold and the PMMA using transient heat conduction analyses. To demonstrate the applications of LADRI, two different optical surfaces were replicated: an antireflection (AR) structure with conical structures sized several hundred nanometers and a light-extraction structure with a microlens array (MLA) comprising 10 µm lenses, for display and illumination, respectively. The replication degree of the MLA was governed by the contact pressure. Polymer flow simulation indicated that the heat conduction and flow speeds of the melted PMMA surface were comparable within several tens of micrometers. In addition, the reflectivity of the AR structure decreased from 4 to 0.5%, and the light intensity of the light-extraction structure increased by a factor of 1.47.

Mechanism and performance evaluation of transient and selective laser processing of glass based on optical monitoring.

Femtosecond laser processing has been widely applied in glass processing owing to its ability to fabricate microscale components. To improve processing efficiency, a transient and selective laser (TSL) processing technique was previously developed, in which electron excitation was induced inside a transparent medium by a single pulse of femtosecond (fs) laser, and a single pulse of microsecond (µs) laser can be selectively absorbed in this excited region to heat and remove the material. However, because of its high speed removal process, the unclear mechanism and inefficient evaluation of its processing performance limit its further application. This study analyzes the transient spatiotemporal evolution of the induced plasma and the related material removal mechanism of the TSL processing using a side high-speed monitoring method. To achieve a rapid performance evaluation, a quantitative analysis of the optical plasma signals (on a microsecond timescale) generated in TSL processing was performed by employing a developed coaxial high-speed monitoring method using a photodetector. The variations in the shapes, intensity distribution, and dimensions of the plasma were quantitatively investigated. In addition, the relation between the plasma signal and drilling performance under different laser parameters, including hole depth, hole types, and cracks, was explored and quantitatively analyzed. The revealed mechanism is expected to contribute to the broadening of the application of TSL processing in microfabrication. Furthermore, the developed high-speed and precision monitoring technology can be utilized for high-speed evaluation and precision control of machining quality in real time during ultrahigh-speed laser machining, without time-consuming camera observations.

Quantitative Description of Bubble Formation in Response to Electrolyte Engineering.

The green hydrogen economy is expected to play a crucial role in carbon neutrality, but industrial-scale water electrolysis requires improvements in efficiency, operation costs, and capital costs before broad deployment. Electrolysis operates at a high current density and involves the substantial formation of gaseous products from the electrode surfaces to the electrolyte, which may lead to additional resistance and a resulting loss of efficiency. A detailed clarification of the bubble departure phenomena against the electrode surface and the surrounding electrolytes is needed to further control bubbles in a water electrolyzer. This study clarifies how electrolyte properties affect the measured bubble detachment sizes from the comparisons with analytical expressions and dynamic simulations. Bubble behavior in various electrolyte solutions and operating conditions was described using various physical parameters. A quantitative relationship was then established to connect electrolyte properties and bubble departure diameters, which can help regulate the bubble management through electrolyte engineering.

High-speed microgroove processing of glass by expanding the high-temperature region formed by transient and selective laser absorption.

Microgroove processing of glass is important in many fields, however, it is difficult to achieve the processing with a high speed. In this study, we developed a novel method for the high-speed microgroove processing of glass using two types of lasers, namely a femtosecond laser and a near-infrared continuous-wave (CW) laser. A single femtosecond laser pulse was initially focused on the surface of the material, enabling the area to absorb the CW laser, which is otherwise not absorbed by the glass. The CW laser was then scanned along the material surface, expanding the machined hole to form a groove. The resulting grooves, with a width of approximately 10 µm and depths of up to 350 µm, can be machined with a scanning speed of up to 200 mm/s, 25 times faster than conventional methods. This method exhibits the potential to improve the industrial application of fast laser microprocessing of glass.

Sample-efficient parameter exploration of the powder film drying process using experiment-based Bayesian optimization.

Parameter optimization is a long-standing challenge in various production processes. Particularly, powder film forming processes entail multiscale and multiphysical phenomena, each of which is usually controlled by a combination of several parameters. Therefore, it is difficult to optimize the parameters either by numerical-model-based analysis or by "brute force" experiment-based exploration. In this study, we focus on a Bayesian optimization method that has led to breakthroughs in materials informatics. Specifically, we apply this method to exploration of production-process-parameter for the powder film forming process. To this end, a slurry containing a powder, polymer, and solvent was dropped, the drying temperature and time were controlled as parameters to be explored, and the uniformity of the fabricated film was evaluated. Using this experiment-based Bayesian optimization system, we searched for the optimal parameters among 32,768 (85) parameter sets to minimize defects. This optimization converged at 40 experiments, which is a substantially smaller number than that observed in brute-force exploration and traditional design-of-experiments methods. Furthermore, we inferred the mechanism corresponding to the unknown drying conditions discovered in the parameter exploration that resulted in uniform film formation. This demonstrates that a data-driven approach leads to high-throughput exploration and the discovery of novel parameters, which inspire further research.

Ultrafast internal modification of glass by selective absorption of a continuous-wave laser into excited electrons.

The internal modification of glass using ultrashort pulse lasers has been attracting attention in a wide range of applications. However, the remarkably low processing speed has impeded its use in the industry. In this study, we achieved ultrafast internal modification of glass by coaxially focusing a single-pulse femtosecond laser and continuous-wave (CW) laser with the wavelength that is transparent to the glass. Compared with the conventional method, the processing speed increased by a factor of 500. The observation of high-speed phenomena revealed that the CW laser was absorbed by the seed electrons that were generated by the femtosecond laser pulse. This technique may help expand the applications of femtosecond lasers in the industry.

Simulation of ultrashort pulse laser drilling of glass considering heat accumulation.

In accordance with the increasing demand for high-speed processing, the repetition rate of ultrashort pulse lasers has continued to increase. With the development of these lasers, there is a growing demand for the prediction of shapes processed at high repetition rates. However, the prediction of these shapes is a major challenge, because of the difficulty associated with the estimation of heat accumulation. In this study, we developed a simulation of ultrashort laser drilling in glass including heat accumulation calculation between pulses. In this simulation model, temperature is considered as an additional criterion of material removal, thus, the dependency of the repetition rate can be estimated. Two model parameters of laser absorption at high temperatures are investigated and determined by experiments under high environmental temperatures. Using the simulation model, high shape-prediction accuracy at high repetition rates was achieved and validated by comparison with experiments. This study may contribute to broadening the applications of high-repetition-rate ultrashort pulse lasers.

Dynamics of pressure waves during femtosecond laser processing of glass.

Although femtosecond lasers enable microfabrication of transparent materials, precise processing is difficult owing to the inevitable damage caused to the surroundings of the processed region. In the present work, we combine pump-probe imaging with a high-speed camera to capture the dynamics of pressure waves varying from pulse to pulse, before a desired shape is created by hundreds of pulses. The results demonstrate that the pressure waves change their forms and locations as the number of pulses increases. The numerical analyses explain that a tensile stress, much greater than the tensile strength, is distributed around the processed region during the travel of the pressure wave, and that repetitive pressure waves result in cracks. The identified mechanism of the damage generation will contribute to developing strategies to prevent damage and expand the range of applications of femtosecond laser processing.

Laser-Assisted Thermal Imprinting of Microlens Arrays-Effects of Pressing Pressure and Pattern Size.

Polymer films with nano- or microstructured surfaces have been widely applied to optical devices, bioplates, and printed electronics. Laser-assisted thermal imprinting (LATI), in which a laser directly heats the surfaces of a mold and a thermoplastic polymer, is one of the high-throughput methods of replicating nano- or microstructures on polymer films. Only the surfaces of the mold and polymer film are heated and cooled rapidly, therefore it is possible to replicate nano- or microstructures on polymer films more rapidly than by using conventional thermal nanoimprinting. In this study, microlens arrays (MLAs) were replicated on polymethylmethacrylate (PMMA) films using LATI, and the effects of the pressing pressure (10-50 MPa) and the pattern size (33- and 5-µm pitch) of the MLA on the filling ratio were investigated by analyzing a microlens replicated using different laser-irradiation times (0.1-2 ms). The filling ratio increased with increasing pressing pressure and laser-irradiation time in the replication of MLAs with varying sizes, while the flow of the PMMA varied with the pressing pressure and laser-irradiation time. It was found that during filling, the shape of the polymer cross-sectional surface demonstrated a double and single peak in the 33- and 5-µm-pitch patterns, respectively. This was because the depth of the heated area in the 33-µm-pitch pattern was smaller than the pattern size, whereas that of the 5-µm-pitch pattern was comparable to (or larger) than the pattern size.

Fabrication of highly ordered Ta2O5 and Ta3N5 nanorod arrays by nanoimprinting and through-mask anodization.

Using highly ordered porous anodic alumina membrane fabricated with the aid of nanoimprinting as a mask, Ta2O5 nanorod array with uniform diameter, length, and distribution is grown in situ on a Ta substrate by through-mask anodization. The Ta2O5 nanorod array is further transformed into Ta3N5 nanorod array without damaging the nanorod structure by nitridation. Solar-driven photoelectrochemical water splitting with a maximum solar energy conversion efficiency of 0.36% is demonstrated with the Ta3N5 nanorod array after modifying the surface with cobalt-phosphate as a co-catalyst. The Ta2O5 and Ta3N5 nanorod arrays have potential applications in catalysis, photonics, UV photodetection and solar energy conversion.