Objective-Free Ultrasensitive Biosensing on Large-Area Metamaterial Surfaces in the Near-IR.

Plasmonic metamaterials have opened new avenues in medical diagnostics. However, the transfer of the technology to the markets has been delayed due to multiple challenges. The need of bulky optics for signal reading from nanostructures patterned on submillimeter area limits the miniaturization of the devices. The use of objective-free optics can solve this problem, which necessitates large area patterning of the nanostructures. In this work, we utilize laser interference lithography (LIL) to pattern nanodisc-shaped metamaterial absorber nanoantennas over a large area (4 cm2) within minutes. The introduction of a sacrificial layer during the fabrication process enables an inverted hole profile and a well-controlled liftoff, which ensures perfectly defined uniform nanopatterning almost with no defects. Furthermore, we use a macroscopic reflection probe for optical characterization in the near-IR, including the detection of the binding kinematics of immunologically relevant proteins. We show that the photonic quality of the plasmonic nanoantennas commensurates with electron-beam-lithography-fabricated ones over the whole area. The refractive index sensitivity of the LIL-fabricated metasurface is determined as 685 nm per refractive index unit, which demonstrates ultrasensitive detection. Moreover, the fabricated surfaces can be used multiple times for biosensing without losing their optical quality. The combination of rapid and large area nanofabrication with a simple optical reading not only simplifies the detection process but also makes the biosensors more environmentally friendly and cost-effective. Therefore, the improvements provided in this work will empower researchers and industries for accurate and real-time analysis of biological systems.

Hollow Microcavity Electrode for Enhancing Light Extraction.

Luminous efficiency is a pivotal factor for assessing the performance of optoelectronic devices, wherein light loss caused by diverse factors is harvested and converted into the radiative mode. In this study, we demonstrate a nanoscale vacuum photonic crystal layer (nVPCL) for light extraction enhancement. A corrugated semi-transparent electrode incorporating a periodic hollow-structure array was designed through a simulation that utilizes finite-difference time-domain computational analysis. The corrugated profile, stemming from the periodic hollow structure, was fabricated using laser interference lithography, which allows the precise engineering of various geometrical parameters by controlling the process conditions. The semi-transparent electrode consisted of a 15 nm thick Ag film, which acted as the exit mirror and induced microcavity resonance. When applied to a conventional green organic light-emitting diode (OLED) structure, the optimized nVPCL-integrated device demonstrated a 21.5% enhancement in external quantum efficiency compared to the reference device. Further, the full width at half maximum exhibited a 27.5% reduction compared to that of the reference device, demonstrating improved color purity. This study presents a novel approach by applying a hybrid thin film electrode design to optoelectronic devices to enhance optical efficiency and color purity.

Real-Time Imaging of Plasmonic Concentric Circular Gratings Fabricated by Lens-Axicon Laser Interference Lithography.

Concentric circular gratings are diffractive optical elements useful for polarization-independent applications in photonics and plasmonics. They are usually fabricated using a low-throughput and expensive electron beam lithography technique. In this paper, concentric circular gratings with selectable pitch values were successfully manufactured on thin films of azobenzene molecular glass using a novel laser interference lithography technique utilizing Bessel beams generated by a combined lens-axicon configuration. This innovative approach offers enhanced scalability and a simplified manufacturing process on larger surface areas compared to the previously reported techniques. Furthermore, the plasmonic characteristics of these concentric circular gratings were investigated using conventional spectrometric techniques after transferring the nanostructured patterns from azobenzene to transparent gold/epoxy thin films. In addition, the real-time imaging of surface plasmon resonance colors transmitted from the concentric circular gratings was obtained using a 45-megapixel digital camera. The results demonstrated a strong correlation between the real-time photographic technique and the spectroscopy measurements, validating the efficacy and accuracy of this approach for the colorimetric studying of surface plasmon resonance responses in thin film photonics.

Performance of Grating Couplers Used in the Optical Switch Configuration.

Surface plasmon resonance is an effect widely used for biosensing. Biosensors based on this effect operate in different configurations, including the use of diffraction gratings as couplers. Gratings are highly tunable and are easy to integrate into a fluidic system due to their planar configuration. We discuss the optimization of plasmonic grating couplers for use in a specific sensor configuration based on the optical switch. These gratings present a sinusoidal profile with a high depth/period ratio. Their interaction with a p-polarized light beam results in two significant diffracted orders (the 0th and the -1st), which enable differential measurements cancelling noise due to common fluctuations. The gratings are fabricated by combining laser interference lithography with nanoimprinting in a process that is aligned with the challenges of low-cost mass production. The effects of different grating parameters such as the period, depth and profile are theoretically and experimentally investigated.

Crater-like nanoelectrode arrays for electrochemical detection of dopamine release from neuronal cells.

Stem cell therapy has shown great potential in treating various incurable diseases using conventional chemotherapy. Parkinson's disease (PD)-a neurodegenerative disease-has been reported to be caused by quantitative loss or abnormal functionality of dopaminergic neurons (DAnergic neurons). To date, stem cell therapies have shown some potential in treating PD throughex vivoengraftment of stem-cell-derived neurons. However, accurately identifying the differentiation and non-invasively evaluating the functionality and maturity of DAnergic neurons are formidable challenges in stem cell therapies. These strategies are important in enhancing the efficacy of stem cell therapies. In this study, we report a novel cell cultivation platform, that is, a nanocrater-like electrochemical nanoelectrode array (NCENA) for monitoring dopamine (DA) release from neurons to detect exocytotic DA release from DAnergic neurons. In particular, the developed NCENA has a nanostructure in which three-dimensional porous gold nanopillars are uniformly arranged on conductive electrodes. The developed NCENA exhibited great DA sensing capabilities with a linear range of 0.39-150µM and a limit of detection of 1.16µM. Furthermore, the nanotopographical cues provided by the NCENA are suitable for cell cultivation with enhanced cellular adhesion. Finally, we successfully analysed the functionality and maturity of differentiated neurons on the NCENA through its excellent sensing ability for exocytotic DA.

Laser Interference Lithography-A Method for the Fabrication of Controlled Periodic Structures.

A microstructure determines macro functionality. A controlled periodic structure gives the surface specific functions such as controlled structural color, wettability, anti-icing/frosting, friction reduction, and hardness enhancement. Currently, there are a variety of controllable periodic structures that can be produced. Laser interference lithography (LIL) is a technique that allows for the simple, flexible, and rapid fabrication of high-resolution periodic structures over large areas without the use of masks. Different interference conditions can produce a wide range of light fields. When an LIL system is used to expose the substrate, a variety of periodic textured structures, such as periodic nanoparticles, dot arrays, hole arrays, and stripes, can be produced. The LIL technique can be used not only on flat substrates, but also on curved or partially curved substrates, taking advantage of the large depth of focus. This paper reviews the principles of LIL and discusses how the parameters, such as spatial angle, angle of incidence, wavelength, and polarization state, affect the interference light field. Applications of LIL for functional surface fabrication, such as anti-reflection, controlled structural color, surface-enhanced Raman scattering (SERS), friction reduction, superhydrophobicity, and biocellular modulation, are also presented. Finally, we present some of the challenges and problems in LIL and its applications.

Exploring SERS from complex patterns fabricated by multi-exposure laser interference lithography.

Designing uniform plasmonic surfaces in a large area is highly recommended for surface-enhanced Raman scattering (SERS). As periodic morphologies exhibit uniform SERS and optical tunability, diverse fabrication methods of periodic nanostructures have been reported for SERS applications. Laser interference lithography (LIL) is one of the most versatile tools since it can rapidly fabricate periodic patterns without the usage of photomasks. Here, we explore complex interference patterns for spatially uniform SERS sensors and its cost-effective fabrication method termed multi-exposure laser interference lithography (MELIL). MELIL can produce nearly periodic profiles along every direction confirmed by mathematical background, and in virtue of periodicity, we show that highly uniform Raman scattering (relative standard deviation <6%) can also be achievable in complex geometries as the conventional hole patterns. We quantitatively characterize the Raman enhancement of the MELIL complex patterns after two different metal deposition processes, Au e-beam evaporation and Ag electroplating, which results in 0.387 × 105and 1.451 × 105in enhancement factor respectively. This alternative, vacuum-free electroplating method realizes an even more cost-effective process with enhanced performance. We further conduct the optical simulation for MELIL complex patterns which exhibits the broadened and shifted absorption peaks. This result supports the potential of the expanded optical tunability of the suggested process.

Structural Color Surface on Transparent PDMS Fabricated by Carbon-Assisted Laser Interference Lithography for Real-Time Quantification of Soft Actuators Motion.

Dynamic and real-time monitoring of the motion state of soft actuators is of great significance for optimizing their performance. However, present noncontact measurement approaches based on diffractive groove arrays fabricated by imprinting have some limitation, e.g., the grooves should be processed before the solidification of soft materials or the depth and period of grooves cannot be flexibly adjusted. Here, a flexible and high-efficiency fabrication approach carbon-assisted laser interference lithography (CLIL) for periodical groove structures with structural color is proposed. This technique is to irradiate the interference laser on the PDMS surface coated by a carbon layer, which is used for enhanced laser absorption. The processing parameters are systematically studied and optimized to achieve a bright structural color. Benefiting from the advantages of CLIL, the structural color can be processed on a solidified transparent surface with controllable characteristics such as groove period and depth. Lastly, the motion of an electric-driven actuator can be real-time quantified by calibrating the relationship between the observation angle and the observed structural color.

Enhancing Neurogenesis of Neural Stem Cells Using Homogeneous Nanohole Pattern-Modified Conductive Platform.

Biocompatible platforms, wherein cells attach and grow, are important for controlling cytoskeletal dynamics and steering stem cell functions, including differentiation. Among various components, membrane integrins play a key role in focal adhesion of cells (18-20 nm in size) and are, thus, highly sensitive to the nanotopographical features of underlying substrates. Hence, it is necessary to develop a platform/technique that can provide high flexibility in controlling nanostructure sizes. We report a platform modified with homogeneous nanohole patterns, effective in guiding neurogenesis of mouse neural stem cells (mNSCs). Sizes of nanoholes were easily generated and varied using laser interference lithography (LIL), by changing the incident angles of light interference on substrates. Among three different nanohole patterns fabricated on conductive transparent electrodes, 500 nm-sized nanoholes showed the best performance for cell adhesion and spreading, based on F-actin and lamellipodia/filopodia expression. Enhanced biocompatibility and cell adhesion of these nanohole patterns ultimately resulted in the enhanced neurogenesis of mNSCs, based on the mRNAs expression level of the mNSCs marker and several neuronal markers. Therefore, platforms modified with homogeneous nanohole patterns fabricated by LIL are promising for the precise tuning of nanostructures in tissue culture platforms and useful for controlling various differentiation lineages of stem cells.

Sensitive and Reproducible Gold SERS Sensor Based on Interference Lithography and Electrophoretic Deposition.

Surface-enhanced Raman spectroscopy (SERS) is a promising analytical tool due to its label-free detection ability and superior sensitivity, which enable the detection of single molecules. Since its sensitivity is highly dependent on localized surface plasmon resonance, various methods have been applied for electric field-enhanced metal nanostructures. Despite the intensive research on practical applications of SERS, fabricating a sensitive and reproducible SERS sensor using a simple and low-cost process remains a challenge. Here, we report a simple strategy to produce a large-scale gold nanoparticle array based on laser interference lithography and the electrophoretic deposition of gold nanoparticles, generated through a pulsed laser ablation in liquid process. The fabricated gold nanoparticle array produced a sensitive, reproducible SERS signal, which allowed Rhodamine 6G to be detected at a concentration as low as 10-8 M, with an enhancement factor of 1.25 × 105. This advantageous fabrication strategy is expected to enable practical SERS applications.

Patent Review on Laser Interference Lithography Technique for Producing Periodic Nanostructure.

BACKGROUND: Because line width has been close to atom size, for semiconductor industry, except for achieving the target of line width, the cost will be more important. The mask-less laser interference lithography (LIL) technique lowers the cost makes it standing out in the market of lithographic equipment of the excessive cost in the semiconductor industry. METHOD: The Keywords of patent retrieval with the theme of LIL are based on the technical features of both the conditions of producing interference lithography and different types of experimental configuration of LIL. Method of patent retrieval include Boolean logic operators are used to express the relationship between sets. Furthermore, it's necessary to find whether common patent classification codes exist in the highly correlated patents and confirm the definition of that. RESULTS: The patent review in this research show the patents of LIL technique are classified according to optical method and lithographic equipment. The patents related to optical method of LIL technique take beam splitter based configuration as the main stream; in the technique of lithographic equipment, the patents of system planning technique are the most. CONCLUSION: The findings of this review confirm the importance of improving the precision of LIL technique for avoiding the defocus of high-density line width. Besides, it's particularly suitable for the micro nanofluid device in the emerging bionanotechnology to observe fluid behavior at the minimum scale. It doesn't need mask and can produce periodic pattern with nanoscale make it devote to the field of periodicity.

Introduction of Laser Interference Lithography to Make Nanopatterned Surfaces for Fundamental Studies on Stem Cell Response.

The extracellular matrix (ECM) is a nanostructured environment that provides chemical, mechanical, and topographical stimuli for various cellular functions. Here, we introduce the application of laser interference lithography (LIL) to generate hexagonally arranged gold nanostructures of three different dimensions on silicon to study the effect of feature dimensions on human adipose-derived stem cells (hADSC) in terms of adhesion, growth, and differentiation. Self-assembled monolayers (SAM) were used to passivate the background silicon surface with a long-chain polyethylene glycol (PEG), whereas the gold nanostructures were activated with mercaptoundecanoic acid (MUDA) to direct protein adsorption and cell adhesive structures to them, only. It was possible to show that the size and distance of the nanostructures affected the spreading of hADSC with a decrease of cell size with the increase of feature dimensions, which corresponded also to the expression of focal adhesions and presence of the small GTPase RhoA. Effects of these early events, related to outside-in signal transduction, were visible by an enhanced cell growth on smaller feature dimensions and distinct effects on cell differentiation. Because of the precise control of chemical and topographical cues, the presented system offers great potential to study effects of material topography on stem cell behavior, which may pave the way for applications in tailoring surfaces of implants and tissue engineering scaffolds.

Realizing Large-Area Arrays of Semiconducting Fullerene Nanostructures with Direct Laser Interference Patterning.

We present a laser interference patterning method for the facile fabrication of large-area and high-contrast arrays of semiconducting fullerene nanostructures, which does not rely on a tedious application of sacrificial photoresists or photomasks. A solution-deposited phenyl-C61-butyric acid methyl ester (PCBM) fullerene thin film is exposed to a spatially modulated illumination intensity, as realized by a two-beam laser interference. The PCBM molecules exposed to strong intensity are photochemically transformed into a low-solubility dimeric state, so that the nontransformed PCBM molecules can be selectively removed in a subsequent solution-based development step. Following brief exposure to green laser light (λ = 532 nm, t = 5 s, p = 0.17 W cm-2) in the designed two-beam interference setup, and a 1 min development in a tuned acetone-chloroform solution, we realize well-defined and ordered PCBM nanostripe patterns with a fwhm line width of ∼200 nm and a repetition rate of ∼2.900 lines mm-1 over a large area of 1 cm2. We demonstrate that a desired high contrast is effectuated because the initial PCBM-dimer transformation rate is dependent on the square of the illumination intensity. The semiconducting functionality of the patterned fullerene is verified in a field-effect transistor experiment, where a typical PCBM nanostripe featured an electron mobility of 5.3 × 10-3 cm2 V-1 s-1 and an on/off ratio of 3 × 103.

Using Laser Interference Lithography in the Fabrication of a Simplified Micro- and Nanofluidic Device for Label-free Detection.

Recently, we developed a label-free detection method based on optical diffraction, and implemented it in on our fabricated micro- and nanofluidic device. This detection method is simple and useful for detecting biomolecules, but the device fabrication consists of complicated processes. In this paper, we propose a simple method for fabricating the micro- and nanofluidic device; the fabrication combines laser interference lithography with conventional photolithography. The performance of a device fabricated by the proposed method is comparable to the performance of the device in our previous study.

Determination of aqueous antibiotic solutions using SERS nanogratings.

The emergence of antibiotics and their active metabolites in aquatic ecosystem has motivated the development of sensitive and reliable sensors to monitor traces of antibiotics and metabolites in drinking water sources (i.e. surface water). The surface enhanced Raman scattering (SERS) technique, which is widely recognized as a high sensitivity method for molecular vibrational detection, is potentially a powerful tool for trace environmental contamination analysis. The main goal of this work is to demonstrate pharmaceutical and metabolite multiplexing detection using the SERS approach. Periodic metallic nanostructures were fabricated using laser interference lithography (LIL) and used as SERS substrates (platform that supports the SERS effect). The LIL method allowed excellent substrate-to-substrate geometric parameters variations; for instance, the variations in periodicity were determined to be less than 1%. A common fluoroquinolone (FQ) parent-and-metabolite pair, enrofloxacin (ENRO) and ciprofloxacin (CIPRO), was targeted for multiplexing detection on the relative uniform substrates fabricated by LIL. The quantifications of the analytes mixtures were achieved by chemometric analysis (i.e. non-negative matrix factorization with alternating least square algorithm (NMF-ALS)). The limit of the quantification (LOQ) of the present method is in the ppm-level with less than 10% spatial variation in the SERS signal.

Experimental research on laser interference micro/nano fabrication of hydrophobic modification of stent surface.

Coronary artery disease (CAD) has become one of the important causes of human death, and coronary stent implantation is one of the most effective methods for the treatment of CAD. But the current clinical treatment has a high long-term restenosis rate and is easy to form late stent thrombosis. In order to solve these problems, coronary artery stent surface was directly modified by laser interference lithography and the highly ordered concave structures were fabricated. The morphology and contact angle (CA) of the microstructure were measured with scanning electron microscopy (SEM) and CA system. The water repellent property of the stent was also evaluated by the method of contacting the water drop with the stent and then separating. The result showed that the close-packed concave structure with the period of about 12.194 µm can be fabricated on the stent surface under special parameters (laser energy density of 3.5 J/cm-2, incident angles of 3°, exposure time of 80 s) by the three-beam laser interference of 1064 nm and the form structure has good water repellency with contact angle of 120°.

Plasmonic Periodic Nanodot Arrays via Laser Interference Lithography for Organic Photovoltaic Cells with >10% Efficiency.

In this study, we demonstrate a viable and promising optical engineering technique enabling the development of high-performance plasmonic organic photovoltaic devices. Laser interference lithography was explored to fabricate metal nanodot (MND) arrays with elaborately controlled dot size as well as periodicity, allowing spectral overlap between the absorption range of the active layers and the surface plasmon band of MND arrays. MND arrays with ∼91 nm dot size and ∼202 nm periodicity embedded in a poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) hole transport layer remarkably enhanced the average power conversion efficiency (PCE) from 7.52% up to 10.11%, representing one of the highest PCE and degree of enhancement (∼34.4%) levels compared to the pristine device among plasmonic organic photovoltaics reported to date. The plasmonic enhancement mechanism was investigated by both optical and electrical analyses using finite difference time domain simulation and conductive atomic force microscopy studies.

Color Rendering Plasmonic Aluminum Substrates with Angular Symmetry Breaking.

We fabricate and characterize large-area plasmonic substrates that feature asymmetric periodic nanostructures made of aluminum. Strong coupling between localized and propagating plasmon resonances leads to characteristic Fano line shapes with tunable spectral positions and widths. Distinctive colors spanning the entire visible spectrum are generated by tuning the system parameters, such as the period and the length of the aluminum structures. Moreover, the asymmetry of the aluminum structures gives rise to a strong symmetry broken color rendering effect, for which colors are observed only from one side of the surface normal. Using a combination of immersed laser interference lithography and nanoimprint lithography, our color rendering structures can be fabricated on areas many inches in size. We foresee applications in anticounterfeiting, photovoltaics, sensing, displays, and optical security.

Three-dimensional ordered ZnO/Cu2O nanoheterojunctions for efficient metal-oxide solar cells.

Interface modulation for broad-band light trapping and efficient carrier collection has always been the research focus in solar cells, which provides the most effective way to achieve performance enhancement. In this work, solution-processed 3D ordered ZnO/Cu2O nanoheterojunctions, consisting of patterned n-ZnO nanorod arrays (NRAs) and p-Cu2O films, are elaborately designed and fabricated for the first time. By taking advantage of nanoheterojunctions with square patterned ZnO NRAs, solar cells demonstrate the maximum current density and efficiency of 9.89 mA cm(-2) and 1.52%, which are improved by 201% and 127%, respectively, compared to that of cells without pattern. Experimental analysis and theoretical simulation confirm that this exciting result originates from a more efficient broad-band light trapping and carrier collection of the 3D ordered ZnO/Cu2O nanoheterojunctions. Such 3D ordered nanostructures will have a great potential application for low-cost and all oxide solar energy conversion. Furthermore, the methodology applied in this work can be also generalized to rational design of other efficient nanodevices and nanosystems.