Enhancing the stability of polymer nanostructures via ultrathin oxide coatings for nano-optical device applications.

Polymer nanostructures have drawn tremendous attention due to their wide applications in nanotechnology. However, the morphology of the polymer nanostructures is fragile under harsh conditions such as high-power irradiation and organic-solution environments during the fabrication or the measurement processes, significantly limiting their potential applications. In this work, we propose and demonstrate a simple approach to improve the stability of polymer nanostructures by coating a conformal ultrathin oxide film via atomic-layer deposition. Due to the refractory and dense coating of the oxide layer, the stability of polymer structures is enhanced by the prohibition of deformation occurrences from thermally induced reflow and organic solution. As a proof of concept, poly(methyl methacrylate) (PMMA) nanostructures coated with a sub-10-nm TiO2layer are demonstrated, and the structures exhibit high temperature stability at 180 °C and good resistance to soluble damage from organic solutions. Subsequently, the mechanism of the improved thermal stability is analyzed via mechanical simulations. Such an effective approach is proposed to significantly broaden the application of polymer nanostructures as functional elements for optical structures/devices that require excellent thermal and chemical stability.

Periodic planar Fabry-Perot nanocavities with tunable interference colors based on filling density effects.

Structural colors of high performance and economically feasible fabrication are desired in various applications. Herein, we demonstrate that reflective full-color filters based on the interference effect can be realized in periodic Fabry-Perot (F-P) nanocavity arrays of the same thickness. Enabled by simply adjusting the nanocavity size and array period, the resonant wavelengths can be successively tuned in the whole visible light range, which is mainly attributed to the varied effective refractive index introduced by the different filling density of the F-P nanocavity. Compared to the plasmonic colors utilizing the similar nanostructures, the proposed interference colors offer unique advantages of higher color contrast, wider gamut, and lower fabrication requirements. Besides, these color filters do not involve modulating the vertical dimensions of the F-P nanocavities, which is conducive to the monolithic integration of multicolor optical cavities and their large-area applications in consumable products combined with replica patterning techniques, such as nanoimprinting and soft lithography.

Recent advances in focused ion beam nanofabrication for nanostructures and devices: fundamentals and applications.

The past few decades have witnessed growing research interest in developing powerful nanofabrication technologies for three-dimensional (3D) structures and devices to achieve nano-scale and nano-precision manufacturing. Among the various fabrication techniques, focused ion beam (FIB) nanofabrication has been established as a well-suited and promising technique in nearly all fields of nanotechnology for the fabrication of 3D nanostructures and devices because of increasing demands from industry and research. In this article, a series of FIB nanofabrication factors related to the fabrication of 3D nanostructures and devices, including mechanisms, instruments, processes, and typical applications of FIB nanofabrication, are systematically summarized and analyzed in detail. Additionally, current challenges and future development trends of FIB nanofabrication in this field are also given. This work intends to provide guidance for practitioners, researchers, or engineers who wish to learn more about the FIB nanofabrication technology that is driving the revolution in 3D nanostructures and devices.

Strongly coupled evenly divided disks: a new compact and tunable platform for plasmonic Fano resonances.

Plasmonic artificial molecules are promising platforms for linear and nonlinear optical modulation at various regimes including the visible, infrared and terahertz bands. Fano resonances in plasmonic artificial structures are widely used for controlling spectral lineshapes and tailoring of near-field and far-field optical response. Generation of a strong Fano resonance usually relies on strong plasmon coupling in densely packed plasmonic structures. Challenges in reproducible fabrication using conventional lithography significantly hinders the exploration of novel plasmonic nanostructures for strong Fano resonance. In this work, we propose a new class of plasmonic molecules with symmetric structure for Fano resonances, named evenly divided disk, which shows a strong Fano resonance due to the interference between a subradiant anti-bonding mode and a superradiant bonding mode. We successfully fabricated evenly divided disk structures with high reproducibility and with sub-20 nm gaps, using our recently developed sketch and peel lithography technique. The experimental spectra agree well with the calculated response, indicating the robustness of the Fano resonance for the evenly divided disk geometry. Control experiments reveal that the strength of the Fano resonance gradually increases when increasing the number of split parts on the disk from three to eight individual segments. The Fano-resonant plasmonic molecules that can also be reliably defined by our unique fabrication approach open up new avenues for application and provide insight into the design of artificial molecules for controlling light-matter interactions.

Huge field enhancement and high transmittance enabled by terahertz bow-tie aperture arrays: a simulation study.

Sub-wavelength aperture arrays featuring small gaps have an extraordinary significance in enhancing the interactions of terahertz (THz) waves with matters. But it is difficult to obtain large light-substance interaction enhancement and high optical response signal detection capabilities at the same time. Here, we propose a simple terahertz bow-tie aperture arrays structure with a large electric field enhancement factor and high transmittance at the same time. The field enhancement factor can reach a high value of 1.9×104 and the transmission coefficient of around 0.8 (the corresponding normalized-to-area transmittance is about 14.3) at 0.04 µm feature gap simultaneously. The systematic simulation results show that the designed structure can enhance the intensity of electromagnetic hotspot by continuously reducing the feature gap size without affecting the intensity of the transmittance. We also visually displayed the significant advantages of extremely strong electromagnetic hot spots in local terahertz refractive index detection, which provides a potential platform and simple strategy for enhanced THz spectral detection.

Kirigami-inspired multiscale patterning of metallic structures via predefined nanotrench templates.

Reliable fabrication of multiscale metallic patterns with precise geometry and size at both the nanoscale and macroscale is of importance for various applications in electronic and optical devices. The existing fabrication processes, which usually involve film deposition in combination with electron-beam patterning, are either time-consuming or offer limited precision. Inspired by the kirigami, an ancient handicraft art of paper cutting, this work demonstrates an electron-beam patterning process for multiscale metallic structures with significantly enhanced efficiency and precision. Similar to the kirigami, in which the final pattern is defined by cutting its contour in a paper and then removing the unwanted parts, we define the target multiscale structures by first creating nanotrench contours in a metallic film via an electron-beam-based process and then selectively peeling the separated film outside the contours. Compared with the conventional approach, which requires the exposure of the whole pattern, much less exposure area is needed for nanotrench contours, thus enabling reduced exposure time and enhanced geometric precision due to the mitigated proximity effect. A theoretical model based on interface mechanics allows a clear understanding of the nanotrench-assisted selective debonding behaviour in the peeling process. By using this fabrication process, multiscale metallic structures with sub-10-nm up to submillimetre features can be reliably achieved, having potential applications for anti-counterfeiting and gap-plasmon-enhanced spectroscopy.

3D-Integrated metasurfaces for full-colour holography.

Metasurfaces enable the design of optical elements by engineering the wavefront of light at the subwavelength scale. Due to their ultrathin and compact characteristics, metasurfaces possess great potential to integrate multiple functions in optoelectronic systems for optical device miniaturisation. However, current research based on multiplexing in the 2D plane has not fully utilised the capabilities of metasurfaces for multi-tasking applications. Here, we demonstrate a 3D-integrated metasurface device by stacking a hologram metasurface on a monolithic Fabry-Pérot cavity-based colour filter microarray to simultaneously achieve low-crosstalk, polarisation-independent, high-efficiency, full-colour holography, and microprint. The dual functions of the device outline a novel scheme for data recording, security encryption, colour displays, and information processing. Our 3D integration concept can be extended to achieve multi-tasking flat optical systems by including a variety of functional metasurface layers, such as polarizers, metalenses, and others.

Notched terahertz Bowtie metamaterials with strongly enhanced near-field and narrowed resonance linewidth.

Enhanced near-field and quality factor of resonance are key issues in plasmonic structures. Here, we demonstrate a kind of notched bowtie metamaterials in the terahertz (THz) regime with narrow linewidth and extremely enhanced near field. The notched bowtie is a variation of common bowtie structure created by introducing symmetric notches on the two sides of the triangular metallic structure. Benefiting from the introduction of notches, the modulation depth of transmittance spectra and near-field enhancement of the notched bowtie arrays were strongly enhanced due to the increase of the structure-derived equivalent inductance. The results demonstrated that near-field enhancement can be increased to above 4000. In addition, the designed structure possesses a narrowed resonance linewidth, and thus an improved quality factor, which could be a promising platform for THz sensing and other potential applications of THz metamaterials.

Transmissive structural color filters using vertically coupled aluminum nanohole/nanodisk array with a triangular-lattice.

We demonstrate a configuration to generate transmissive structural colors through triangular-lattice square nanohole arrays in aluminum (Al) film with Al nanodisks on the bottom of the nanoholes. By using a simple nanofabrication process, colors covering the entire visible light with different brightness and saturation are achieved by tuning both the period of arrays and the size of nanoholes. The optical behaviors of the structures are systematically investigated by both experimental and theoretical methods. The results indicate that the localized surface plasmon resonance of nanohole arrays plays the key role in the extraordinary transmission and meanwhile the coupling of disks and holes is also of importance for the enhanced transmission. With the wide color gamut, these kinds of vertically coupled Al nanohole/nanodisk arrays show the capabilities for high-resolution full-color printing. Compared to existing transmissive plasmonic color filters, the configuration in this work has the advantages of a simple fabrication process and using cheap aluminum materials.

Stepwise-Nanocavity-Assisted Transmissive Color Filter Array Microprints.

Visible-light color filters using patterned nanostructures have attracted much interest due to their various advantages such as compactness, enhanced stability, and environmental friendliness compared with traditional pigment or dye-based optical filters. While most existing studies are based on planar nanostructures with lateral variation in size, shape, and arrangement, the vertical dimension of structures is a long-ignored degree of freedom for the structural colors. Herein, we demonstrate a synthetic platform for transmissive color filter array by coordinated manipulations between height-varying nanocavities and their lateral filling fractions. The thickness variation of those nanocavities has been fully deployed as an alternative degree of freedom, yielding vivid colors with wide gamut and excellent saturation. Experimental results show that the color-rendering capability of the pixelated nanocavities can be still retained as pixels are miniaturized to 500 nm. Crosstalk between closely spaced pixels of a Bayer color filter arrangement was calculated, showing minimal crosstalk for 1 µm2 square subpixels. Our work provides an approach to designing and fabricating ultracompact color filter arrays for various potential applications including stained-glass microprints, microspectrometers, and high-resolution image sensing systems.

Release of an HtrA-Like Protease from the Cell Surface of Thermophilic Brevibacillus sp. WF146 via Substrate-Induced Autoprocessing of the N-terminal Membrane Anchor.

High-temperature requirement A (HtrA)-like proteases participate in protein quality control in prokaryotes and eukaryotes by degrading damaged proteins; however, little is known about HtrAs produced by thermophiles. HtrAw is an HtrA-like protease of thermophilic Brevibacillus sp. WF146. The intact form of HtrAw (iHtrAw) consisting of a transmembrane segment-containing N-terminal domain, a trypsin-like protease domain, and a C-terminal PDZ domain was produced in Escherichia coli. Purified iHtrAw itself is unable to cleave the N-terminal domain, but requires protein substrates to autoprocess the N-terminal domain intermolecularly, yielding a short form (sHtrAw). Mutation at the substrate-binding site in the PDZ domain affects the conversion of iHtrAw to sHtrAw. Deletion analysis revealed that the N-terminal domain is not necessary for enzyme folding, activity, and thermostability. Compared with other known HtrAs, HtrAw contains an additional Ca2+-binding Dx[DN]xDG motif important for enzyme stability and/or activity. When produced in an htrA/htrB double deletion mutant of Bacillus subtilis, iHtrAw localized predominantly to the cell pellet, and the amount of sHtrAw in the culture supernatant increased at elevated temperatures. Moreover, HtrAw increased the heat resistance of the B. subtilis mutant. In strain WF146, HtrAw exists in both a cell-associated intact form and a cell-free short form; an increase in growth temperature enhanced HtrAw production and the amount of cell-free short form. Release of the short form of HtrAw from the membrane may have the advantage of allowing the enzyme to freely access and degrade damaged proteins surrounding the bacterium living at high temperatures.

Low-voltage-exposure-enabled hydrogen silsesquioxane bilayer-like process for three-dimensional nanofabrication.

We report a bilayer-like electron-beam lithographic process to obtain three-dimensional (3D) nanostructures by using only a single hydrogen silsesquioxane (HSQ) resist layer. The process utilizes the short penetration depth of low-energy (1.5 keV) electron irradiation to first obtain a partially cross-linked HSQ top layer and then uses a high-voltage electron beam (30 keV) to obtain self-aligned undercut (e.g. mushroom-shaped) and freestanding HSQ nanostructures. Based on the well-defined 3D resist patterns, 3D metallic nanostructures were directly fabricated with high fidelity by just depositing a metallic layer. As an example, Ag-coated mushroom-shaped nanostructures were fabricated, which showed lower plasmon resonance damping compared to their planar counterparts. In addition, the undercut 3D nanostructures also enable more reliable lift-off in comparison with the planar nanostructures, with which high-quality silver nanohole arrays were fabricated which show distinct and extraordinary optical transmission in the visible range.

"Sketch and Peel" Lithography for High-Resolution Multiscale Patterning.

We report a unique lithographic process, termed "Sketch and Peel" lithography (SPL), for fast, clean, and reliable patterning of metallic structures from tens of nanometers to submillimeter scale using direct writing technology. The key idea of SPL process is to define structures using their presketched outlines as the templates for subsequent selective peeling of evaporated metallic layer. With reduced exposure area, SPL process enables significantly improved patterning efficiency up to hundreds of times higher and greatly mitigated proximity effect compared to current direct writing strategy. We demonstrate that multiscale hierarchical metallic structures with arbitrary shapes and minimal feature size of ∼15 nm could be defined with high fidelity using SPL process for potential nanoelectronic and nano-optical applications.

Reliable fabrication of plasmonic nanostructures without an adhesion layer using dry lift-off.

Lift-off is the most commonly used pattern-transfer method to define lithographic plasmonic metal nanostructures. A typical lift-off process is realized by dissolving patterned resists in solutions, which has the limits of low yield when not using adhesion layers and incompatibility with the fabrication of some specific structures and devices. In this work, we report an alternative 'dry' lift-off process to obtain metallic nanostructures via mechanical stripping by using the advantage of poor adhesion between resists and noble metal films. We show that this dry stripping lift-off method is effective for both positive- and negative-tone resists to fabricate sparse and densely-packed plasmonic nanostructures, respectively. In particular, this method is achieved without using an adhesion layer, which enables the mitigation of plasmon damping to obtain larger field enhancement. Dark-field scattering, one-photon luminescence and surface-enhanced Raman scattering measurements were performed to demonstrate the improved quality factor of the plasmonic nanostructures fabricated by this dry lift-off process.

Improving the Thermostability and Activity of a Thermophilic Subtilase by Incorporating Structural Elements of Its Psychrophilic Counterpart.

The incorporation of the structural elements of thermostable enzymes into their less stable counterparts is generally used to improve enzyme thermostability. However, the process of engineering enzymes with both high thermostability and high activity remains an important challenge. Here, we report that the thermostability and activity of a thermophilic subtilase were simultaneously improved by incorporating structural elements of a psychrophilic subtilase. There were 64 variable regions/residues (VRs) in the alignment of the thermophilic WF146 protease, mesophilic sphericase, and psychrophilic S41. The WF146 protease was subjected to systematic mutagenesis, in which each of its VRs was replaced with those from S41 and sphericase. After successive rounds of combination and screening, we constructed the variant PBL5X with eight amino acid residues from S41. The half-life of PBL5X at 85°C (57.1 min) was approximately 9-fold longer than that of the wild-type (WT) WF146 protease (6.3 min). The substitutions also led to an increase in the apparent thermal denaturation midpoint temperature (Tm) of the enzyme by 5.5°C, as determined by differential scanning calorimetry. Compared to the WT, PBL5X exhibited high caseinolytic activity (25 to 95°C) and high values of Km and kcat (25 to 80°C). Our study may provide a rational basis for developing highly stable and active enzymes, which are highly desired in industrial applications.