Nanoplasmonic aptasensor for sensitive, selective, and real-time detection of dopamine from unprocessed whole blood.

Neurotransmitters are crucial for the proper functioning of neural systems, with dopamine playing a pivotal role in cognition, emotions, and motor control. Dysregulated dopamine levels are linked to various disorders, underscoring the need for accurate detection in research and diagnostics. Single-stranded DNA (ssDNA) aptamers are promising bioreceptors for dopamine detection due to their selectivity, improved stability, and synthesis feasibility. However, discrepancies in dopamine specificity have presented challenges. Here, we surface-functionalized a nano-plasmonic biosensing platform with a dopamine-specific ssDNA aptamer for selective detection. The biosensor, featuring narrowband hybrid plasmonic resonances, achieves high specificity through functionalization with aptamers and passivation processes. Sensitivity and selectivity for dopamine detection are demonstrated across a wide range of concentrations, including in diverse biological samples like protein solutions, cerebrospinal fluid, and whole blood. These results highlight the potential of plasmonic "aptasensors" for developing rapid and accurate diagnostic tools for disease monitoring, medical diagnostics, and targeted therapies.

Multispectral Molecular Chiral Barcoding.

More than half of pharmaceutical drugs in use are chiral, necessitating accurate techniques for their characterization. Enantiomers, molecules with mirrored symmetry, often exhibit similar physical traits but possess distinct chemical and biological implications. This study harnesses the strong light-matter interaction induced by "superchiral" light to perform Surface-Enhanced Infrared Absorption (SEIRA) induced vibrational circular dichroism measurements in the mid-infrared spectral region. Utilizing a nanopatterned pixelated array of achiral plasmonic nanostructures, the system allows unique identification of enantiomers and biomolecules. Tunability of plasmon resonance facilitates spectral variation of the optical chirality over a wide infrared range, enabling development of a unique chiral "barcoding" scheme to distinguish chiral molecules based on their infrared fingerprint. This simple, yet robust sensor presents a low-cost solution for chiral mapping of drugs and biomolecules.

Self-Assembled Plasmonic Structural Color Colorimetric Sensor for Smartphone-Based Point-Of-Care Ammonia Detection in Water.

Monitoring chemical levels is crucial for safeguarding both the environment and public health. Elevated levels of ammonia, for instance, can harm both humans and aquatic ecosystems, often indicating contamination from agriculture, industry, or sewage. Developing portable, high-resolution, and affordable methods for in situ monitoring of ammonia is thus imperative. Plasmonic sensors offer a promising solution, detecting ammonia by correlating changes in their optical response to the target analyte's concentration. While they are highly sensitive and can be fabricated in a variety of portable and user-friendly formats, some still require reagents or expensive optical equipment, which hinder their widespread adoption. Here, we present a self-assembled nanoplasmonic colorimetric sensor capable of directly detecting ammonia concentrations in aqueous matrices. The proposed sensor exploits the plasmonic resonance of the nanostructures to transduce changes in the chemical environment into alterations in color, offering a label-free method for real-time analysis. The sensor is fabricated using a self-assembling technique compatible with low-cost mass production based on aluminum and aluminum oxide, ensuring affordability and avoiding the use of other toxic chemicals. We developed a model to predict ammonia concentrations based on visible color change of the sensor, achieving a detection limit of 8.5 ppm. Furthermore, to address the need for on-site detection, we integrated smartphone technology for real-time color change analysis, eliminating the need for expensive, bulky optical instruments. Indeed, our approach offers a cost-effective, portable, and user-friendly solution for ammonia detection in water without the need for chemical reagents or spectrometers, making it ideal for field applications. Interestingly, this platform extends its applicability beyond ammonia detection, enabling the monitoring of various chemicals using a smartphone, without the need for any additional costly equipment.

Roadmap for Optical Metasurfaces.

Metasurfaces have recently risen to prominence in optical research, providing unique functionalities that can be used for imaging, beam forming, holography, polarimetry, and many more, while keeping device dimensions small. Despite the fact that a vast range of basic metasurface designs has already been thoroughly studied in the literature, the number of metasurface-related papers is still growing at a rapid pace, as metasurface research is now spreading to adjacent fields, including computational imaging, augmented and virtual reality, automotive, display, biosensing, nonlinear, quantum and topological optics, optical computing, and more. At the same time, the ability of metasurfaces to perform optical functions in much more compact optical systems has triggered strong and constantly growing interest from various industries that greatly benefit from the availability of miniaturized, highly functional, and efficient optical components that can be integrated in optoelectronic systems at low cost. This creates a truly unique opportunity for the field of metasurfaces to make both a scientific and an industrial impact. The goal of this Roadmap is to mark this "golden age" of metasurface research and define future directions to encourage scientists and engineers to drive research and development in the field of metasurfaces toward both scientific excellence and broad industrial adoption.

Tunable plasmonic superchiral light for ultrasensitive detection of chiral molecules.

The accurate detection, classification, and separation of chiral molecules are pivotal for advancing pharmaceutical and biomolecular innovations. Engineered chiral light presents a promising avenue to enhance the interaction between light and matter, offering a noninvasive, high-resolution, and cost-effective method for distinguishing enantiomers. Here, we present a nanostructured platform for surface-enhanced infrared absorption-induced vibrational circular dichroism (VCD) based on an achiral plasmonic system. This platform enables precise measurement, differentiation, and quantification of enantiomeric mixtures, including concentration and enantiomeric excess determination. Our experimental results exhibit a 13 orders of magnitude higher detection sensitivity for chiral enantiomers compared to conventional VCD spectroscopic techniques, accounting for respective path lengths and concentrations. The tunable spectral characteristics of this achiral plasmonic system facilitate the detection of a diverse range of chiral compounds. The platform's simplicity, tunability, and exceptional sensitivity holds remarkable potential for enantiomer classification in drug design, pharmaceuticals, and biological applications.

Ultralight plasmonic structural color paint.

All present commercial colors are based on pigments. While such traditional pigment-based colorants offer a commercial platform for large-volume and angle insensitiveness, they are limited by their instability in atmosphere, color fading, and severe environmental toxicity. Commercial exploitation of artificial structural coloration has fallen short due to the lack of design ideas and impractical nanofabrication techniques. Here, we present a self-assembled subwavelength plasmonic cavity that overcomes these challenges while offering a tailorable platform for rendering angle and polarization-independent vivid structural colors. Fabricated through large-scale techniques, we produce stand-alone paints ready to be used on any substrate. The platform offers full coloration with a single layer of pigment, surface density of 0.4 g/m2, making it the lightest paint in the world.

DNA-Modified Plasmonic Sensor for the Direct Detection of Virus Biomarkers from the Blood.

The rapid spread of viral infections demands early detection strategies to minimize proliferation of the disease. Here, we demonstrate a plasmonic biosensor to detect Dengue virus, which was chosen as a model, via its nonstructural protein NS1 biomarker. The sensor is functionalized with a synthetic single-stranded DNA oligonucleotide and provides high affinity toward NS1 protein present in the virus genome. We demonstrate the detection of NS1 protein at a concentration of 0.1-10 µg/mL in bovine blood using an on-chip microfluidic plasma separator integrated with the plasmonic sensor which covers the clinical threshold of 0.6 µg/mL of high risk of developing Dengue hemorrhagic fever. The conceptual and practical demonstration shows the translation feasibility of these microfluidic optical biosensors for early detection of a wide range of viral infections, providing a rapid clinical diagnosis of infectious diseases directly from minimally processed biological samples at point of care locations.

Organic Non-Wettable Superhydrophobic Fullerite Films.

A long-standing quest in material science has been the development of non-wettable superhydrophobic films based on a single organic material, without the requirement of fluorination or silane treatment. Here, such films and coatings, which are developed using colloidal gels of fullerite C60 and C70 nanocrystals, are described. It is illustrated that despite the high surface energy of these van der Waals molecular crystals their gelation can create films having self-affine fractal surfaces with multiscale roughness. Water droplets on resulting surfaces of fullerite films bead like a pearl resting in a Fakir state with contact angle exceeding 150°. The films are extremely water repellent and non-wettable; when submerged in water they stay dry up to 3 h even at a water depth of two feet and exhibit the plastron effect. A series of experiments are presented to provide comprehensive inspection of water droplet dynamics on these films. These include rolling, bouncing, squeezing, freezing, melting, evaporating; along with acidic and alkaline tests. Non-wettable films of such materials are unique as fullerites get photosensitized instantaneously generating extremely high yields (≈100%) of singlet oxygen (1 O2 ) that can destroy viruses and bacteria; thereby enabling their use in rheology, water purification, and medicinal devices.

Scalable Van der Waals Two-Dimensional PtTe2 Layers Integrated onto Silicon for Efficient Near-to-Mid Infrared Photodetection.

In recent years, there has been increasing interest in leveraging two-dimensional (2D) van der Waals (vdW) crystals for infrared (IR) photodetection, exploiting their unusual optoelectrical properties. Some 2D vdW materials with small band gap energies such as graphene and black phosphorus have been explored as stand-alone IR responsive layers in photodetectors. However, the devices incorporating these IR-sensitive 2D layers often exhibited poor performances owing to their preparation issues such as limited scalability and air instability. Herein, we explored wafer-scale 2D platinum ditelluride (PtTe2) layers for near-to-mid IR photodetection by directly growing them onto silicon (Si) wafers. 2D PtTe2/Si heterojunctions exhibited wavelength- and intensity-dependent high photocurrents in a spectral range of ∼1-7 µm, significantly outperforming stand-alone 2D PtTe2 layers. The observed superiority is attributed to their excellent Schottky junction characteristics accompanying suppressed carrier recombination as well as optical absorbance competition between 2D PtTe2 layers and Si. The direct and scalable growth of 2D PtTe2 layers was further extended to demonstrate mechanically flexible IR photodetectors.

Self-assembled plasmonics for angle-independent structural color displays with actively addressed black states.

Nanostructured plasmonic materials can lead to the extremely compact pixels and color filters needed for next-generation displays by interacting with light at fundamentally small length scales. However, previous demonstrations suffer from severe angle sensitivity, lack of saturated color, and absence of black/gray states and/or are impractical to integrate with actively addressed electronics. Here, we report a vivid self-assembled nanostructured system which overcomes these challenges via the multidimensional hybridization of plasmonic resonances. By exploiting the thin-film growth mechanisms of aluminum during ultrahigh vacuum physical vapor deposition, dense arrays of particles are created in near-field proximity to a mirror. The sub-10-nm gaps between adjacent particles and mirror lead to strong multidimensional coupling of localized plasmonic modes, resulting in a singular resonance with negligible angular dispersion and ∼98% absorption of incident light at a desired wavelength. The process is compatible with arbitrarily structured substrates and can produce wafer-scale, diffusive, angle-independent, and flexible plasmonic materials. We then demonstrate the unique capabilities of the strongly coupled plasmonic system via integration with an actively addressed reflective liquid crystal display with control over black states. The hybrid display is readily programmed to display images and video.

Dirac plasmon-assisted asymmetric hot carrier generation for room-temperature infrared detection.

Due to the low photon energy, detection of infrared photons is challenging at room temperature. Thermoelectric effect offers an alternative mechanism bypassing material bandgap restriction. In this article, we demonstrate an asymmetric plasmon-induced hot-carrier Seebeck photodetection scheme at room temperature that exhibits a remarkable responsivity of 2900 VW-1, detectivity of 1.1 × 109 Jones along with a fast response of ~100 ns in the technologically relevant 8-12 µm band. This is achieved by engineering the asymmetric electronic environment of the generated hot carriers on chemical vapor deposition grown large area nanopatterned monolayer graphene, which leads to a temperature gradient of 4.7 K across the device terminals for an incident power of 155 nW, thereby enhancing the photo-thermoelectric voltage by manifold compared to previous reports. The results presented outline a strategy for uncooled, tunable, and multispectral infrared detection.

Buckling and twisting of advanced materials into morphable 3D mesostructures.

Recently developed methods in mechanically guided assembly provide deterministic access to wide-ranging classes of complex, 3D structures in high-performance functional materials, with characteristic length scales that can range from nanometers to centimeters. These processes exploit stress relaxation in prestretched elastomeric platforms to affect transformation of 2D precursors into 3D shapes by in- and out-of-plane translational displacements. This paper introduces a scheme for introducing local twisting deformations into this process, thereby providing access to 3D mesostructures that have strong, local levels of chirality and other previously inaccessible geometrical features. Here, elastomeric assembly platforms segmented into interconnected, rotatable units generate in-plane torques imposed through bonding sites at engineered locations across the 2D precursors during the process of stress relaxation. Nearly 2 dozen examples illustrate the ideas through a diverse variety of 3D structures, including those with designs inspired by the ancient arts of origami/kirigami and with layouts that can morph into different shapes. A mechanically tunable, multilayered chiral 3D metamaterial configured for operation in the terahertz regime serves as an application example guided by finite-element analysis and electromagnetic modeling.

Novel liquid crystal photonic devices enabled by two-photon polymerization [Invited].

In addition to displays, liquid crystals (LCs) have also found widespread applications in photonic devices, such as adaptive lens, adaptive optics, and sensors, because of their responses to electric field, temperature, and light. As the fabrication technique advances, more sophisticated devices can be designed and created. In this review, we report recent advances of two-photon polymerization-based direct-laser writing enabled LC devices. Firstly, we describe the basic working principle of two-photon polymerization. With this powerful fabrication technique, we can generate anchoring energy by surface morphology to align LC directors on different form factors. To prove this concept, we demonstrate LC alignment on planar, curvilinear surfaces as well as in three-dimensional volumes. Based on the results, we further propose a novel, ultra-broadband, twisted-nematic diffractive waveplate that can potentially be fulfilled by this technique. Next, we briefly discuss the current status of direct-laser writing on LC reactive mesogens and its potential applications. Finally, we present two design challenges: fabrication yield and polymer relaxation/deformation, remaining to be overcome.

Wireless, battery-free optoelectronic systems as subdermal implants for local tissue oximetry.

Monitoring regional tissue oxygenation in animal models and potentially in human subjects can yield insights into the underlying mechanisms of local O2-mediated physiological processes and provide diagnostic and therapeutic guidance for relevant disease states. Existing technologies for tissue oxygenation assessments involve some combination of disadvantages in requirements for physical tethers, anesthetics, and special apparatus, often with confounding effects on the natural behaviors of test subjects. This work introduces an entirely wireless and fully implantable platform incorporating (i) microscale optoelectronics for continuous sensing of local hemoglobin dynamics and (ii) advanced designs in continuous, wireless power delivery and data output for tether-free operation. These features support in vivo, highly localized tissue oximetry at sites of interest, including deep brain regions of mice, on untethered, awake animal models. The results create many opportunities for studying various O2-mediated processes in naturally behaving subjects, with implications in biomedical research and clinical practice.

Wide Angle Dynamically Tunable Enhanced Infrared Absorption on Large-Area Nanopatterned Graphene.

Enhancing light-matter interaction by exciting Dirac plasmons on nanopatterned monolayer graphene is an efficient route to achieve high infrared absorption. Here, we designed and fabricated hexagonal planar arrays of nanoholes and nanodisks with and without optical cavity to excite Dirac plasmons on patterned graphene and investigate the role of plasmon lifetime, extinction cross-section, incident light polarization, angle of incident light, and pattern dimensions on the light-absorption spectra. By incorporating a high-k Al2O3 layer as the gate dielectric for dynamic electrostatic tuning of the Fermi level, we demonstrate peak absorptions of 60% and 90% for the nanohole and nanodisk patterns, respectively, in the atmospheric transparent 8-12 µm infrared imaging band with high spectral tunability. Finally, we theoretically and experimentally demonstrate angular dependence of both s- and p-polarized light absorption in monolayer graphene. Our results showcase the practical usability of low carrier mobility CVD-grown graphene for wide angle infrared absorption, which is suitable for next-generation optoelectronic devices such as photodetectors, optical switches, modulators, etc.

Enzyme-Free Plasmonic Biosensor for Direct Detection of Neurotransmitter Dopamine from Whole Blood.

Complex biological fluids without pretreatment, separation, or purification impose stringent limitations on the practical deployment of label-free plasmonic biosensors for advanced assays needed in point of care applications. In this work, we present an enzyme-free plasmonic neurotransmitter dopamine biosensor integrated with a microfluidic plasma separator. This integrated device allows the in-line separation of plasma directly from the bloodstream and channels it to the active detection area, where inorganic cerium oxide nanoparticles function as local selective dopamine binding sites through strong surface redox reaction. A thorough understanding and engineering of the nanoparticles is carried out to maximize its dopamine sensitivity and selectivity. We obtain detection of dopamine at 100 fM concentration in simulated body fluid and 1 nM directly from blood without any prior sample preparation. The detection selectivity is found to be at least five-times higher compared to the common interfering species. This demonstration shows the feasibility of the practical implementation of the proposed plasmonic system in detection of variety of biomarkers directly from the complex biological fluids.

Cavity-induced hybrid plasmon excitation for perfect infrared absorption.

Photonic microcavity coupling of a subwavelength hole-disk array, a two-element metal/dielectric composite structure with enhanced extraordinary transmission, leads to 100% coupling of incident light to the cavity system and subsequent absorption. This light-funneling process arises from the temporal and spatial coupling of the broadband localized surface plasmon resonance on the coupled hole-disk array and the photonic modes of the optical cavity, which induces spectral narrowing of the perfect absorption of light. A simple nanoimprint lithography-based large-area fabrication process paves the path towards practical implementation of plasmonic cavity-based devices and sensors.

Covert infrared image encoding through imprinted plasmonic cavities.

Functional surfaces that can control light across the electromagnetic spectrum are highly desirable. Plasmonic nanostructures can assume this role by exhibiting dimension-tunable resonances that span multiple electromagnetic regimes. However, changing these structural parameters often impacts the higher-order resonances and spectral features in lower-wavelength domains. In this study, we discuss a cavity-coupled plasmonic system with resonances that are tunable across the 3-5 or 8-14 µm infrared bands while retaining near-invariant spectral properties in the visible domain. This result is accomplished by regime-dependent resonance mechanisms and their dependence on independent structural parameters. Through the identification and constraint of key parameters, we demonstrate multispectral data encoding, where images, viewable in the infrared spectral domain, appear as uniform areas of color in the visible domain-effectively hiding the information. Fabricated by large area nanoimprint lithography and compatible with flexible surfaces, the proposed system can produce multifunctional coatings for thermal management, camouflage, and anti-counterfeiting.

Switchable Pancharatnam-Berry microlens array with nano-imprinted liquid crystal alignment.

We report a rapid nano-imprinting technique to pattern the liquid crystal alignment of a Pancharatnam-Berry phase microlens array. Through implementing a single-side aligned cell, we demonstrate a switchable microlens array with fast response time and low operation voltage. Further investigation of focusing property as well as imaging capability ensure the good quality of the microlens array. Besides planar structures, this method is also promising for patterning liquid crystal alignment on curvilinear surfaces.

Adaptive liquid crystal microlens array enabled by two-photon polymerization.

A tunable-focus liquid crystal microlens array is demonstrated and characterized. Using two-photon polymerization based direct-laser writing, a polymerized microlens array is fabricated on one substrate. Such a microlens array creates inhomogeneous electric field distribution and homogeneous-like liquid-crystal alignment, simultaneously. The phase profile and thus the focal length can be tuned dynamically by the applied voltage. We also further investigate the focusing property and the imaging capability of the fabricated sample. Using the adaptive microlens array as an example, we demonstrate that directly forming a curvilinear surface with liquid-crystal alignment is feasible. In addition to adaptive lens, this direct-laser writing method is also a powerful tool for making other tunable photonic devices.