Spontaneous generation and active manipulation of real-space optical vortices.

Optical vortices are beams of light that carry orbital angular momentum1, which represents an extra degree of freedom that can be generated and manipulated for photonic applications2-8. Unlike vortices in other physical entities, the generation of optical vortices requires structural singularities9-12, but this affects their quasiparticle nature and hampers the possibility of altering their dynamics or making them interacting13-17. Here we report a platform that allows the spontaneous generation and active manipulation of an optical vortex-antivortex pair using an external field. An aluminium/silicon dioxide/nickel/silicon dioxide multilayer structure realizes a gradient-thickness optical cavity, where the magneto-optic effects of the nickel layer affect the transition between a trivial and a non-trivial topological phase. Rather than a structural singularity, the vortex-antivortex pairs present in the light reflected by our device are generated through mathematical singularities in the generalized parameter space of the top and bottom silicon dioxide layers, which can be mapped onto real space and exhibit polarization-dependent and topology-dependent dynamics driven by external magnetic fields. We expect that the field-induced engineering of optical vortices that we report will facilitate the study of topological photonic interactions and inspire further efforts to bestow quasiparticle-like properties to various topological photonic textures such as toroidal vortices, polarization and vortex knots, and optical skyrmions.

Customizing Radiative Decay Dynamics of Two-Dimensional Excitons via Position- and Polarization-Dependent Vacuum-Field Interference.

Embodying bosonic and interactive characteristics in two-dimensional space, excitons in transition metal dichalcogenides (TMDCs) have garnered considerable attention. The utilization of the strong-correlation effects, long-range transport, and valley-dependent properties requires customizing exciton decay dynamics. Vacuum-field manipulation allows radiative decay engineering without disturbing intrinsic material properties. However, conventional flat mirrors cannot customize the radiative decay landscape in TMDC's plane or support vacuum-field interference with desired spectrum and polarization properties. Here, we present a meta-mirror platform resolving the issues with more optical degrees of freedom. For neutral excitons of the monolayer MoSe2, the optical layout formed by meta-mirrors manipulated the radiative decay rate in space by 2 orders of magnitude and revealed the statistical correlation between emission intensity and spectral line width. Moreover, the anisotropic meta-mirror demonstrated polarization-dependent radiative decay control. Our platform would be promising to tailor two-dimensional distributions of lifetime, density, diffusion, and polarization of TMDC excitons in advanced opto-excitonic applications.

Ultrawide meta-film replication process for the mass production of a flexible microwave absorbing meta-surface.

The manufacturing process for an ultrawide flexible microwave absorbing meta-surface was developed and optimized experimentally. The developed replication process consists of four main steps to demonstrate double-square loop array meta-structures: (1) mechanical machining of a master mold, (2) soft mold replication and patterned film imprinting, (3) conductive ink blade filling, (4) lamination of a base flexible film to meta sheet. Based on experimental optimization of the individual steps, the manufacturing process for a large-area flexible meta-film was established successfully. The feasibility of a developed process has been demonstrated with a 200 mm × 500 mm fabricated meta-film with a focus on microwave absorbing uniformity in the X-band region.

Directional radiation for optimal radiative cooling.

The omnidirectional radiation scheme has been widely applied to thermal emitters for radiative cooling. We quantitatively illustrate that significant net radiative absorption at high zenith angles limits the performance of such isotropic emitters, and demonstrate that simply cutting off components corresponding to high angles can substantially improve the cooling performance of commonly used isotropic emitter designs. We also present an expression for the ideal directional spectral emissivity at conditions below ambient temperature. As our approach can be applied to coolers with arbitrary surfaces, our results may serve as a basic guideline for designing practical systems with various surfaces, such as rooftops or façades of modern buildings with complicated geometries.

Spectrally sharp metasurfaces for wide-angle high extinction of green lasers.

In optical nanostructures used as artificial resonance-based color filters, there is unfortunate universal trade-off between spectral sharpness and angular tolerance as well as maximum extinction. We rigorously derive the maximum performance bounds of wavelength-rejection filters realized by single-layer plasmonic metasurfaces with a dominant resonance and weak near-field coupling, and propose a multi-layer approach to overcome these single-layer limits and trade-offs. We also present a realistic example that has a narrow full-width-at-half-maximum bandwidth of 24 nm with 10 dB extinction at 532 nm with good angular tolerance up to 60°. The performance of the proposed metasurface is close to the general theoretical bound.

Direct Chemical Synthesis of Plasmonic Black Colloidal Gold Superparticles with Broadband Absorption Properties.

Self-assembly of plasmonic metal nanoparticles can provide an opportunity of creating colloidal superparticles with fascinating optical properties arising from interparticle plasmonic coupling, but typically requires multiple steps involving solvent and/or ligand exchange. We developed a direct, one-step chemical synthesis of plasmonic black colloidal Au superparticles with broadband absorption in visible and near-infrared regions. During the synthesis, the Au superparticles were formed through self-assembly of in-situ-formed Au nanoparticles driven by solvophobic interactions between nanoparticles and solvent. These superparticles could be solution-processed to fabricate a thin film, which exhibited near-perfect absorption over a broad range from 400 nm to 2.5 µm as well as the excellent antireflective property. Thanks to their broadband absorption property, the Au superparticles showed good performances for near-infrared surface-enhanced Raman spectroscopy and light-to-heat conversion.

Effects of dorsiflexor functional electrical stimulation compared to an ankle/foot orthosis on stroke-related genu recurvatum gait.

[Purpose] We evaluated the effects of functional electrical stimulation (FES) and an ankle/foot orthosis (AFO) in hemiplegic patients exhibiting excessive plantar flexion during the stance phase, associated with genu recurvatum. [Participants and Methods] In total, 12 stroke patients were recruited. We measured changes in knee and ankle joint angles, gait speed, and step and stride length during the gait cycle during barefoot walking, walking while wearing an AFO, and walking after FES application; we used a three dimensional gait analysis system. [Results] In terms of kinematic variables, FES walking was associated with significant increases in peak ankle dorsiflexion during swing, dorsiflexion angle at initial contact, peak ankle dorsiflexion during stance, knee angle at initial contact, and peak knee flexion in the loading response compared to AFO and barefoot walking. AFO walking was associated with a significant difference in peak ankle dorsiflexion during swing compared to barefoot walking. [Conclusion] FES afforded kinematic advantages to the ankle and knee joints compared to AFO in hemiplegic patients with a genu recurvatum gait.

Bright and vivid plasmonic color filters having dual resonance modes with proper orthogonality.

The mode orthogonality fundamentally influences the scattering spectra of multi-resonance systems, such as plasmonic color filters. We show that planar arrays of silver nanostructures with dual localized surface plasmon resonances and the right mode orthogonality can function as transmissive RGB color filters with peak transmittances higher than 70%, and color gamut areas larger than 90% of the sRGB space. These are the brightest and most saturated of all designs proposed thus far. We present the Pareto frontier from designs with more than 80% peak transmittance, to designs that achieve a color gamut larger than 120% of the sRGB space.

Self-aligned deterministic coupling of single quantum emitter to nanofocused plasmonic modes.

The quantum plasmonics field has emerged and been growing increasingly, including study of single emitter-light coupling using plasmonic system and scalable quantum plasmonic circuit. This offers opportunity for the quantum control of light with compact device footprint. However, coupling of a single emitter to highly localized plasmonic mode with nanoscale precision remains an important challenge. Today, the spatial overlap between metallic structure and single emitter mostly relies either on chance or on advanced nanopositioning control. Here, we demonstrate deterministic coupling between three-dimensionally nanofocused plasmonic modes and single quantum dots (QDs) without any positioning for single QDs. By depositing a thin silver layer on a site-controlled pyramid QD wafer, three-dimensional plasmonic nanofocusing on each QD at the pyramid apex is geometrically achieved through the silver-coated pyramid facets. Enhancement of the QD spontaneous emission rate as high as 22 ± 16 is measured for all processed QDs emitting over ∼150-meV spectral range. This approach could apply to high fabrication yield on-chip devices for wide application fields, e.g., high-efficiency light-emitting devices and quantum information processing.

A terahertz metamaterial with unnaturally high refractive index.

Controlling the electromagnetic properties of materials, going beyond the limit that is attainable with naturally existing substances, has become a reality with the advent of metamaterials. The range of various structured artificial 'atoms' has promised a vast variety of otherwise unexpected physical phenomena, among which the experimental realization of a negative refractive index has been one of the main foci thus far. Expanding the refractive index into a high positive regime will complete the spectrum of achievable refractive index and provide more design flexibility for transformation optics. Naturally existing transparent materials possess small positive indices of refraction, except for a few semiconductors and insulators, such as lead sulphide or strontium titanate, that exhibit a rather high peak refractive index at mid- and far-infrared frequencies. Previous approaches using metamaterials were not successful in realizing broadband high refractive indices. A broadband high-refractive-index metamaterial structure was theoretically investigated only recently, but the proposed structure does not lend itself to easy implementation. Here we demonstrate that a broadband, extremely high index of refraction can be realized from large-area, free-standing, flexible terahertz metamaterials composed of strongly coupled unit cells. By drastically increasing the effective permittivity through strong capacitive coupling and decreasing the diamagnetic response with a thin metallic structure in the unit cell, a peak refractive index of 38.6 along with a low-frequency quasi-static value of over 20 were experimentally realized for a single-layer terahertz metamaterial, while maintaining low losses. As a natural extension of these single-layer metamaterials, we fabricated quasi-three-dimensional high-refractive-index metamaterials, and obtained a maximum bulk refractive index of 33.2 along with a value of around 8 at the quasi-static limit.

Anomalous rapid defect annihilation in self-assembled nanopatterns by defect melting.

Molecular self-assembly commonly suffers from dense structural defect formation. Spontaneous defect annihilation in block copolymer (BCP) self-assembly is particularly retarded due to significant energy barrier for polymer chain diffusion and structural reorganization. Here we present localized defect melting induced by blending short neutral random copolymer chain as an unusual method to promote the defect annihilation in BCP self-assembled nanopatterns. Chemically neutral short random copolymer chains blended with BCPs are specifically localized and induce local disordered states at structural defect sites in the self-assembled nanopatterns. Such localized "defect melting" relieves the energy penalty for polymer diffusion and morphology reorganization such that spontaneous defect annihilation by mutual coupling is anomalously accelerated upon thermal annealing. Interestingly, neutral random copolymer chain blending also causes morphology-healing self-assembly behavior that can generate large-area highly ordered 10 nm scale nanopattern even upon poorly defined defective prepatterns. Underlying mechanisms of the unusual experimental findings are thoroughly investigated by three-dimensional self-consistent field theory calculation.

One-way optical modal transition based on causality in momentum space.

The concept of parity-time (PT) symmetry has been used to identify a route toward unidirectional dynamics in optical k-space: imposing asymmetry on the flow of light. Although PT-symmetric potentials have been implemented under the requirement of V(x) = V*(-x), this precondition has only been interpreted within the mathematical framework for the symmetry of Hamiltonians and has not been directly linked to unidirectionality induced by PT symmetry. In this paper, within the context of light-matter interactions, we develop an alternative route toward unidirectionality in k-space by employing the concept of causality. We demonstrate that potentials with real and causal momentum spectra produce unidirectional transitions of optical modes inside the k-continuum, which corresponds to an exceptional point on the degree of PT symmetry. Our analysis reveals a critical link between non-Hermitian problems and spectral theory and also enables multi-dimensional designer manipulation of optical modes, in contrast to the one-dimensional approach that used a Schrödinger-like equation in previous PT-symmetric optics.

Negative-tone block copolymer lithography by in situ surface chemical modification.

Negative-tone block copolymer (BCP) lithography based on in situ surface chemical modification is introduced as a highly efficient, versatile self-assembled nanopatterning. BCP blends films consisting of end-functionalized low molecular weight poly(styrene-ran-methyl methacrylate) and polystyrene-block-Poly(methyl methacylate) can produce surface vertical BCP nanodomains on various substrates without prior surface chemical treatment. Simple oxygen plasma treatment is employed to activate surface functional group formation at various substrates, where the end-functionalized polymers can be covalently bonded during the thermal annealing of BCP thin films. The covalently bonded brush layer mediates neutral interfacial condition for vertical BCP nanodomain alignment. This straightforward approach for high aspect ratio, vertical self-assembled nanodomain formation facilitates single step, site-specific BCP nanopatterning widely useful for various substrates. Moreover, this approach is compatible with directed self-assembly approaches to produce device oriented laterally ordered nanopatterns.

Nanodomain swelling block copolymer lithography for morphology tunable metal nanopatterning.

Ordered metal nanopatterns are crucial requirements for electronics, magnetics, catalysts, photonics, and so on. Despite considerable progress in the synthetic route to metal nanostructures, highly ordered metal nanopatterning over a large-area is still challenging. Nanodomain swelling block copolymer lithography is presented as a general route to the systematic morphology tuning of metal nanopatterns from amphiphilic diblock copolymer self-assembly. Selective swelling of hydrophilic nanocylinder domains in amphiphilic block copolymer films during metal precursor loading and subsequent oxygen based etching generates diverse shapes of metal nanopatterns, including hexagonal nanoring array and hexagonal nanomesh and double line array in addition to common nanodot and nanowire arrays. Solvent annealing condition of block copolymer templates, selective swelling of hydrophilic cylinder nanodomains, block copolymer template thickness, and oxygen based etching methods are the decisive parameters for systematic morphology evolution. The plasmonic properties of ordered Au nanopatterns are characterized and analyzed with finite differential time domain calculation. This approach offers unprecedented opportunity for diverse metal nanopatterns from commonly used diblock copolymer self-assembly.

Optical vortex arrays from smectic liquid crystals.

We demonstrate large-area, closely-packed optical vortex arrays using self-assembled defects in smectic liquid crystals. Self-assembled smectic liquid crystals in a three-dimensional torus structure are called focal conic domains. Each FCD, having a micro-scale feature size, produces an optical vortex with consistent topological charge of 2. The spiral profile in the interferometry confirms the formation of an optical vortex, which is predicted by Jones matrix calculations.

Full-field subwavelength imaging using a scattering superlens.

Light-matter interaction gives optical microscopes tremendous versatility compared with other imaging methods such as electron microscopes, scanning probe microscopes, or x-ray scattering where there are various limitations on sample preparation and where the methods are inapplicable to bioimaging with live cells. However, this comes at the expense of a limited resolution due to the diffraction limit. Here, we demonstrate a novel method utilizing elastic scattering from disordered nanoparticles to achieve subdiffraction limited imaging. The measured far-field speckle fields can be used to reconstruct the subwavelength details of the target by time reversal, which allows full-field dynamic super-resolution imaging. The fabrication of the scattering superlens is extremely simple and the method has no restrictions on the wavelength of light that is used.

Photolithographic realization of target nanostructures in 3D space by inverse design of phase modulation.

The mass production of precise three-dimensional (3D) nanopatterns has long been the ultimate goal of fabrication technology. While interference lithography and proximity-field nanopatterning (PnP) may provide partial solutions, their setup complexity and limited range of realizable structures, respectively, remain the main problems. Here, we tackle these challenges by applying an inverse design to the PnP process. Our inverse design platform based on the adjoint method can efficiently find optimal phase masks for diverse target lattices and motifs. We fabricate a 2D rectangular array of nanochannels, which has not been reported for conventional PnP with normally incident light, as a proof of concept. With further demonstration of material conversion, our work provides versatile platforms for nanomaterial fabrication.

Universal Metasurfaces for Complete Linear Control of Coherent Light Transmission.

Recent advances in metasurfaces and optical nanostructures have enabled complex control of incident light with optically thin devices. However, it has thus far been unclear whether it is possible to achieve complete linear control of coherent light transmission, that is, independent control of polarization, amplitude, and phase for both input polarization states, with just a single, thin nanostructure array. Here, it is proved possible, and a universal metasurface is proposed, a bilayer array of high-index elliptic cylinders that possesses a complete degree of optical freedom with fully designable chirality and anisotropy. The completeness of achievable light control is mathematically shown with corresponding Jones matrices, new types of 3D holographic schemes that were formerly impossible are experimentally demonstrated, and a systematic way of realizing any input-state-sensitive vector linear optical device is presented. The results unlock previously inaccessible degrees of freedom in light transmission control.

Optical recoil of asymmetric nano-optical antenna.

We propose nano-optical antennas with asymmetric radiation patterns as light-driven mechanical recoil force generators. Directional antennas are found to generate recoil force efficiently when driven in the spectral proximity of their resonances. It is also shown that the recoil force is equivalent to the Poynting vector integrated over a closed sphere containing the antenna structures.

Directional photofluidization lithography for nanoarchitectures with controlled shapes and sizes.

Highly ordered metallic nanostructures have attracted an increasing interest in nanoscale electronics, photonics, and spectroscopic imaging. However, methods typically used for fabricating metallic nanostructures, such as direct writing and template-based nanolithography, have low throughput and are, moreover, limited to specific fabricated shapes such as holes, lines, and prisms, respectively. Herein, we demonstrate directional photofluidization lithography (DPL) as a new method to address the aforementioned problems of current nanolithography. The key idea of DPL is the use of photoreconfigurable polymer arrays to be molded in metallic nanostructures instead of conventional colloids or cross-linked polymer arrays. The photoreconfiguration of polymers by directional photofluidization allows unprecedented control over the sizes and shapes of metallic nanostructures. Besides the capability for precise control of structural features, DPL ensures scalable, parallel, and cost-effective processing, highly compatible with high-throughput fabrication. Therefore, DPL can expand not only the potential for specific metallic nanostructure applications but also large-scale innovative nanolithography.