Laser manufacturing of spatial resolution approaching quantum limit.

Atomic and close-to-atom scale manufacturing is a promising avenue toward single-photon emitters, single-electron transistors, single-atom memory, and quantum-bit devices for future communication, computation, and sensing applications. Laser manufacturing is outstanding to this end for ease of beam manipulation, batch production, and no requirement for photomasks. It is, however, suffering from optical diffraction limits. Herein, we report a spatial resolution improved to the quantum limit by exploiting a threshold tracing and lock-in method, whereby the two-order gap between atomic point defect complexes and optical diffraction limit is surpassed, and a feature size of <5 nm is realized. The underlying physics is that the uncertainty of local atom thermal motion dominates electron excitation, rather than the power density slope of the incident laser. We show that the colour centre yield in hexagonal boron nitride is transformed from stochastic to deterministic, and the emission from individual sites becomes polychromatic to monochromatic. As a result, single colour centres in the regular array are deterministically created with a unity yield and high positional accuracy, serving as a step forward for integrated quantum technological applications.

Optical near fields for ablation of periodic structures.

The formation mechanism of laser-induced periodic surface structures (LIPSS) has been a key to high-resolution sub-diffraction lithography or high-efficiency large-area nanotexturing. We show the evolution of LIPSS formation from a nanohole seed structure to high-spatial-frequency LIPSS by using a tightly focused and rectangular-shaped laser beam with different shape-polarization orientations. Formation of LIPSS based on light intensity distribution without invoking any long-range electromagnetic modes achieved quantitative match between modeling and experiment. Our results clearly show the entire step-like and deterministic process of LIPSS evolution based on experimental data and numerical simulations, revealing the dominant structural near-field enhancement on the ripple formation. A rectangular-shaped beam with an aspect ratio of 7:3 was used to break the symmetry of a circularly shaped focus. By azimuthally rotating the orientation of the focal spot and the polarization, it is possible to visualize the far-field effect for the initial seed structure formation and the competition between the far and near fields in the subsequent structure evolution.

Nanoscale control of non-reciprocal ripple writing.

Femtosecond laser-induced deep-subwavelength structures have attracted much attention as a nanoscale surface texturization technique. A better understanding of the formation conditions and period control is required. Herein, we report a method of non-reciprocal writing via a tailored optical far-field exposure, where the period of ripples varies along different scanning directions, and achieve a continuous manipulation of the period from 47 to 112 nm (±4 nm) for a 100-nm-thick indium tin oxide (ITO) on glass. A full electromagnetic model was developed to demonstrate the redistributed localized near-field at different stages of ablation with nanoscale precision. It explains the formation of ripples and the asymmetry of the focal spot determines the non-reciprocity of ripple writing. Combined with beam shaping techniques, we achieved non-reciprocal writing (regarding scanning direction) using an aperture-shaped beam. The non-reciprocal writing is expected to open new paths for precise and controllable nanoscale surface texturing.

Nanoscale Printing of Indium-Tin-Oxide by Femtosecond Laser Pulses.

For constructing optical and electrical micro-devices, the deposition/printing of materials with sub-1 µm precision and size (cross-section) is required. Crystalline c-ITO (indium tin oxide) nanostructures were patterned on glass with sufficient precision to form 20-50 nm gaps between individual disks or lines of ∼250 nm diameter or width. The absorbed energy density [J/cm3] followed a second-order dependence on pulse energy. This facilitated high-resolution and precise nanoscale laser-writing at a laser wavelength of 515 nm. Patterns for optical elements such as circular gratings and micro-disks were laser-printed using ITO as a resist. Unexposed amorphous a-ITO was chemically removed in aqueous 1% vol. HF solution. This use of a-ITO as a solid resist holds promise for metamaterial and micro-optical applications.

Miniature optoelectronic compound eye camera.

Inspired by insect compound eyes (CEs) that feature unique optical schemes for imaging, there has recently been growing interest in developing optoelectronic CE cameras with comparable size and functions. However, considering the mismatch between the complex 3D configuration of CEs and the planar nature of available imaging sensors, it is currently challenging to reach this end. Here, we report a paradigm in miniature optoelectronic integrated CE camera by manufacturing polymer CEs with 19~160 logarithmic profile ommatidia via femtosecond laser two-photon polymerization. In contrast to µ-CEs with spherical ommatidia that suffer from defocusing problems, the as-obtained µ-CEs with logarithmic ommatidia permit direct integration with a commercial CMOS detector, because the depth-of-field and focus range of all the logarithmic ommatidia are significantly increased. The optoelectronic integrated µ-CE camera enables large field-of-view imaging (90°), spatial position identification and sensitive trajectory monitoring of moving targets. Moreover, the miniature µ-CE camera can be integrated with a microfluidic chip and serves as an on-chip camera for real-time microorganisms monitoring. The insect-scale optoelectronic µ-CE camera provides a practical route for integrating well-developed planar imaging sensors with complex micro-optics elements, holding great promise for cutting-edge applications in endoscopy and robot vision.

Ultrafast laser-inscribed nanogratings in sapphire for geometric phase elements.

We systematically studied femtosecond laser-inscribed self-organized nanogratings and geometric phase elements such as a polarization diffraction focusing lens and Q-plate in sapphire crystal. Besides the void structures observed in the focus, nanogratings with periods of 150~300 nm were observed, depending on a nanoslit that took the role of a seeding effect by localized light field enhancement. The non-polarized refractive index change and birefringence were measured with values around 1∼2×10-3 and 6×10-4, respectively. Based on the laser-inscribed form birefringence, a geometric phase lens and Q-plate were successfully demonstrated in sapphire with high imaging and a focusing effect. We expect that our findings may promote the understanding of laser-induced nanogratings in bulk and potential applications in geometric phase elements.

High-Efficiency Fabrication of Geometric Phase Elements by Femtosecond-Laser Direct Writing.

The nanoresolution of geometric phase elements for visible wavelengths calls for a flexible technology with high throughout and free from vacuum. In this article, we propose a high-efficiency and simple manufacturing method for the fabrication of geometric phase elements with femtosecond-laser direct writing (FsLDW) and thermal annealing by combining the advantages of high-efficiency processing and thermal smoothing effect. By using a femtosecond laser at a wavelength of 343 nm and a circular polarization, free-form nanogratings with a period of 300 nm and 170-nm-wide grooves were obtained in 50 s by laser direct ablation at a speed of 5 mm/s in a non-vacuum environment. After fine-tuning through a hot-annealing process, the surface morphology of the geometric phase element was clearly improved. With this technology, we fabricated blazed gratings, metasurface lens, vortex Q-plates and "M" holograms and confirmed the design performance by analyzing their phases at the wavelength of 808 nm. The efficiency and capabilities of our proposed method can pave the possible way to fabricate geometric phase elements with essentially low loss, high-temperature resistance, high phase gradients and novel polarization functionality for potentially wide applications.

O-FIB: far-field-induced near-field breakdown for direct nanowriting in an atmospheric environment.

Nanoscale surface texturing, drilling, cutting, and spatial sculpturing, which are essential for applications, including thin-film solar cells, photonic chips, antireflection, wettability, and friction drag reduction, require not only high accuracy in material processing, but also the capability of manufacturing in an atmospheric environment. Widely used focused ion beam (FIB) technology offers nanoscale precision, but is limited by the vacuum-working conditions; therefore, it is not applicable to industrial-scale samples such as ship hulls or biomaterials, e.g., cells and tissues. Here, we report an optical far-field-induced near-field breakdown (O-FIB) approach as an optical version of the conventional FIB technique, which allows direct nanowriting in air. The writing is initiated from nanoholes created by femtosecond-laser-induced multiphoton absorption, and its cutting "knife edge" is sharpened by the far-field-regulated enhancement of the optical near field. A spatial resolution of less than 20 nm (λ/40, with λ being the light wavelength) is readily achieved. O-FIB is empowered by the utilization of simple polarization control of the incident light to steer the nanogroove writing along the designed pattern. The universality of near-field enhancement and localization makes O-FIB applicable to various materials, and enables a large-area printing mode that is superior to conventional FIB processing.

Control of diameter and numerical aperture of microlens by a single ultra-short laser pulse.

We demonstrate a versatile method for fast and flexible fabrication of either one or an array of microlenses. Multi-foci axial intensity distribution generated by a phase pattern displayed on a spatial light modulator irradiates silica, causing ablation and its internal modification. The following wet etching step defines the diameter r, while the radius of curvature R (hence, the focal length f) is maintained the same. As a result, the numerical aperture NA=r/f changes from 0.2 to 0.4 for the same pulse energy (but different number of multi-foci) during ablation. An isotropic wet etching of silica becomes highly anisotropic for the initial stages of etching following the irradiated pattern. Subsequent evolution of the shape is governed by an isotropic silica etch and forms a spherical lens. This method can be extended to other materials and geometries of micro-optical elements.

Laser-Inscribed Stress-Induced Birefringence of Sapphire.

Birefringence of 3 × 10 - 3 is demonstrated inside cross-sectional regions of 100 µ m, inscribed by axially stretched Bessel-beam-like fs-laser pulses along the c-axis inside sapphire. A high birefringence and retardance of λ / 4 at mid-visible spectral range (green) can be achieved using stretched beams with axial extension of 30-40 µ m. Chosen conditions of laser-writing ensure that there are no formations of self-organized nano-gratings. This method can be adopted for creation of polarization optical elements and fabrication of spatially varying birefringent patterns for optical vortex generation.

Effect of drying-wetting cycles on leaching behavior of cement solidified lead-contaminated soil.

Lead contaminated soil was treated by different concentration of ordinary Portland cement (OPC). Solidified cylindrical samples were dried at 40°C in oven for 48 h subsequent to 24h of immersing in different solution for one drying-wetting. 10 cycles were conducted on specimens. The changes in mass loss of specimens, as well as leaching concentration and pH of filtered leachates were studied after each cycle. Results indicated that drying-wetting cycles could accelerate the leaching and deterioration of solidified specimens. The cumulative leached lead with acetic acid (pH=2.88) in this study was 109, 83 and 71 mg respectively for solidified specimens of cement-to-dry soil (C/Sd) ratios 0.2, 0.3 and 0.4, compared to 37, 30, and 25mg for a semi-dynamic leaching test. With the increase of cycle times, the cumulative mass loss of specimens increased linearly, but pH of filtered leachates decreased. The leachability and deterioration of solidified specimens increased with acidity of solution. Increases of C/Sd clearly reduced the leachability and deterioration behavior.

The Tension and Puncture Properties of HDPE Geomembrane under the Corrosion of Leachate.

To investigate the gradual failure of high-density polyethylene (HDPE) geomembrane as a result of long-term corrosion, four dynamic corrosion tests were conducted at different temperatures and durations. By combining tension and puncture tests, we systematically studied the variation law of tension and puncture properties of the HDPE geomembrane under different corrosion conditions. Results showed that tension and puncture failure of the HDPE geomembrane was progressive, and tensile strength in the longitudinal grain direction was evidently better than that in the transverse direction. Punctures appeared shortly after puncture force reached the puncture strength. The tensile strength of geomembrane was in inversely proportional to the corrosion time, and the impact of corrosion was more obvious in the longitudinal direction than transverse direction. As corrosion time increased, puncture strength decreased and corresponding deformation increased. As with corrosion time, the increase of corrosion temperature induced the decrease of geomembrane tensile strength. Tensile and puncture strength were extremely sensitive to temperature. Overall, residual strength had a negative correlation with corrosion time or temperature. Elongation variation increased initially and then decreased with the increase in temperature. However, it did not show significant law with corrosion time. The reduction in puncture strength and the increase in puncture deformation had positive correlations with corrosion time or temperature. The geomembrane softened under corrosion condition. The conclusion may be applicable to the proper designing of the HDPE geomembrane in landfill barrier system.