Manipulating the chirality at nanoscale has drawn great attention among scientists, considering its pivotal role in various applications of current interest, including nano-optics, biomedicine, and photocatalysis. In this work, we delve into this arena by fabricating chiral Swiss roll nanoarray (SRNA) continuous films employing colloidal lithography. The technique permits the dimension of Swiss roll metamaterials to reduce to nanoscale, thus achieving chiroptical response (circular dichroism (CD)) in the visible region. The interplay between the CD signals and plasmon resonance modes is revealed through theoretical simulations, enabling a deep understanding of chiral plasmonic metamaterials. The polarization-sensitive photocatalytic activity of chiral SRNAs is investigated, noting a marked increase in the reaction rate when the chirality of SRNAs matches with the handedness of circularly polarized light (CPL). Notably, the SRNA continuous films based on substrate possess integration and reusability without complex recycling process, enhancing their practicality in applications like sensing and plasmonic nanochemistry, particularly toward polarization-dependent photocatalysis.

Implantable devices for brain-machine interfaces and managing neurological disorders have experienced rapid growth in recent years. Although functional implants offer significant benefits, issues related to transient trauma and long-term biocompatibility and safety are of significant concern. Acute inflammatory reaction in the brain tissue caused by microimplants is known to be an issue but remains poorly studied. This study presents the use of titanium oxynitride (TiNO) nanofilm with defined surface plasmon resonance (SPR) properties for point-of-care characterizing of acute inflammatory responses during robot-controlled micro-neuro-implantation. By leveraging surface-enriched oxynitride, TiNO nanofilms can be biomolecular-functionalized through silanization. This label-free TiNO-SPR biosensor exhibits a high sensitivity toward the inflammatory cytokine interleukin-6 with a detection limit down to 6.3 fg ml-1 and a short assay time of 25 min. Additionally, intraoperative monitoring of acute inflammatory responses during microelectrode implantation in the mice brain has been accomplished using the TiNO-SPR biosensors. Through intraoperative cerebrospinal fluid sampling and point-of-care plasmonic biosensing, the rhythm of acute inflammatory responses induced by the robot-controlled brain microelectrodes implantation has been successfully depicted, offering insights into intraoperative safety assessment of invasive brain-machine interfaces.

Optical microcavities, particularly whispering gallery mode (WGM) microcavities enhanced by plasmonic nanorods, are emerging as powerful platforms for single-molecule sensing. However, the impact of optical forces from the plasmonic near field on analyte molecules is inadequately understood. Using a standard optoplasmonic WGM single-molecule sensor to monitor two enzymes, both of which undergo an open-to-closed-to-open conformational transition, the work done on an enzyme by the WGM sensor as atoms of the enzyme move through the electric field gradient of the plasmonic hotspot during conformational change has been quantified. As the work done by the sensor on analyte enzymes can be modulated by varying WGM intensity, the WGM microcavity system can be used to apply free energy penalties to regulate enzyme activity at the single-molecule level. The findings advance the understanding of optical forces in WGM single-molecule sensing, potentially leading to the capability to precisely manipulate enzyme activity at the single-molecule level through tailored optical modulation.

Plasmonic metal nanostructures can simultaneously scatter and absorb light, with resonance wavelength and strength depending on their morphology and composition. This work demonstrates that unique dichroic effects and high-contrast colour-switching can be achieved by leveraging the resonant scattering and absorption of light by plasmonic nanostructures and the specular reflection of the resulting transmitted light. Using core/shell nanostructures comprising a metal core and a dielectric shell, we show that their spray coating on reflective substrates produces dichroic films that can display colour switching at different viewing angles. The high-contrast colour switching, high flexibility in designing multicolour patterns, and convenience for large-scale production promise their wide range of applications, including anticounterfeiting, mechanochromic sensing, colour display, and printing.

Superchiral fields, supported by chiral plasmonic structures, have shown outstanding performance for chiral molecule sensing via enhanced chiral light-matter interaction. However, this sensing capability cannot fully reveal the chiral origin of the molecules as the chiroptic response of the molecules is intertwined with the chiroptic response of the chiral plasmonic nanostructures, which can potentially be excluded by using a plasmonic racemic mixture. Such a plasmonic racemic mixture is not easily attainable, as it normally requires complex fabrication and expensive instrumentation, whose structural fineness is limited by the fabrication precision. Here, we demonstrate trace-amount chiral molecule detection with plasmonic racemic arrays fabricated by direct laser writing with vector beams, which is facile, cost-effective, and highly controllable. The racemic arrays present no inherent circular differential scattering but a large local superchiral field, which reflects the intrinsic chiral features of the chiral molecules. They are further applied to discriminate enantiomers of phenylalanine with a limit of detection (LOD) of 10.0 ± 2.8 μM, which is an order of magnitude smaller than the LOD of conventional circular dichroism spectroscopy. The strong local superchiral field provided by the plasmonic racemic arrays enlightens the design of a superior sensing platform, which holds promising applications for biomedical detection and enantioselective drug development.

Optical chirality, which plays important roles in liquid crystal display and biological and chemical detection, has been attracting scientists\' attention due to its potential applications in optical information processing. Usually, the chiral optical response of natural molecules is very weak. However, the emergence of metasurfaces offers a promising solution to solve this issue. By judiciously designing the geometry of meta-atoms, we have realized strong optical circular dichroism (CD) in both linear and nonlinear optical regimes. However, tuning of the CD with a metasurface remains challenging. Here, we propose the twist-angle-controlled nonlinear CD effect by using the second-harmonic generation process on a gold-crystal hybrid metasurface. The CD effect of the second-harmonic waves can be tuned well by controlling the twist angle between the two constituent materials. The proposed hybrid metasurface may open new avenues for developing ultracompact and multifunctional nonlinear optical devices.

The emergence of interlayer excitons (IX) in atomically thin heterostructures of transition metal dichalcogenides (TMDCs) has drawn great attention due to their unique and exotic optical and optoelectronic properties. Because of the spatially indirect nature of IX, its oscillator strength is 2 orders of magnitude smaller than that of the intralayer excitons, resulting in a relatively low photoluminescence (PL) efficiency. Here, we achieve the PL enhancement of IX by more than 2 orders of magnitude across the entire heterostructure area with a plasmonic lattice on mirror (PLoM) structure. The significant PL enhancement mainly arises from resonant coupling between the amplified electric field strength within the PLoM gap and the out-of-plane dipole moment of IX excitons, increasing the emission efficiency by a factor of around 47.5 through the Purcell effect. This mechanism is further verified by detuning the PLoM resonance frequency with respect to the IX emission energy, which is consistent with our theoretical model. Moreover, our simulation results reveal that the PLoM structure greatly alters the far-field radiation of the IX excitons preferentially to the surface normal direction, which increases the collection efficiency by a factor of around 10. Our work provides a reliable and universal method to enhance and manipulate the emission properties of the out-of-plane excitons in a deterministic way and holds great promise for boosting the development of photoelectronic devices based on the IX excitons.

Developing innovative surface-enhanced Raman scattering (SERS) nanotags continues to attract significant attention due to their unparalleled sensitivity and specificity for in vitro diagnostic and in vivo tumor imaging applications. Here, we report a new class of bright and stable SERS nanotags using alkylmercaptan-PEG (AMP) polymers. Due to its amphiphilic structure and a thiol anchoring group, these polymers strongly absorb onto gold nanoparticles, leading to an inner hydrophobic layer and an outer hydrophilic PEG layer. The inner hydrophobic layer serves to \"lock in\" the Raman reporter molecules adsorbed on the particle surface via favorable hydrophobic interactions that also allow denser PEG coatings, which \"lock out\" other molecules from competitive binding or adsorbing to the gold surface, thereby providing superior colloidal and signal stability. The higher grafting densities of AMP polymers compared to conventional thiolated PEG also led to dramatic increases in cellular target selectivity, with specific-to-nonspecific binding ratios reaching beyond an order of magnitude difference. Experimental evaluations and theoretical considerations of dielectric polarization and light scattering indicate that the hydrophobic layer provides a more favorable dielectric environment with less plasmon dampening, greater particle scattering efficiency, and increased Raman reporter polarizability. Accordingly, SERS nanotags with AMP polymer coatings are observed to be considerably brighter (∼10-fold). Furthermore, the AMP-coated SERS nanotag\'s increased intensity and avidity can boost cellular detection sensitivity by nearly two orders of magnitude.

Semitransparent organic photovoltaics (ST-OPVs) offer promising prospects for application in building-integrated photovoltaic systems and greenhouses, but further improvement of their performance faces a delicate trade-off between the two competing indexes of power conversion efficiency (PCE) and average visible transmittance (AVT). Herein, the authors take advantage of coupling plasmonics with the optical design of ST-OPVs to enhance near-infrared absorption and hence simultaneously improve efficiency and visible transparency to the maximum extent. By integrating core-bishell PdCu@Au@SiO2 nanotripods that act as optically isotropic Lambertian sources with near-infrared-customized localized surface plasmon resonance in an optimal ternary PM6:BTP-eC9:L8-BO-based ST-OPV, it is shown that their interplay with a multilayer optical coupling layer, consisting of ZnS(130 nm)/Na3AlF6(60 nm)/WO3(100 nm)/LaF3(50 nm) identified from high-throughput optical screening, leads to a record-high PCE of 16.14% (certified as 15.90%) along with an excellent AVT of 33.02%. The strong enhancement of the light utilization efficiency by ≈50% as compared to the counterpart device without optical engineering provides an encouraging and universal pathway for promoting breakthroughs in ST-OPVs from meticulous optical design.

Due to their broken symmetry, chiral plasmonic nanostructures have unique optical properties and numerous applications. However, there is still a lack of comprehension regarding how chirality transfer occurs between circularly polarized light (CPL) and these structures. Here, we thoroughly investigate the plasmon-assisted growth of chiral nanoparticles from achiral Au nanocubes (AuNCs) via CPL without the involvement of any chiral molecule stimulators. We identify the structural chirality of our synthesized chiral plasmonic nanostructures using circular differential scattering (CDS) spectroscopy, which is correlated with scanning electron microscopy imaging at both the single-particle and ensemble levels. Theoretical simulations, including hot-electron surface maps, reveal that the plasmon-induced chirality transfer is mediated by the asymmetric distribution of hot electrons on achiral AuNCs under CPL excitation. Furthermore, we shed light on how this plasmon-induced chirality transfer can also be utilized for chiral growth in bimetallic systems, such as Ag or Pd on AuNCs. The results presented here uncover fundamental aspects of chiral light-matter interaction and have implications for the future design and optimization of chiral sensors and chiral catalysis, among others.