Highly Efficient Ultraviolet Third-Harmonic Generation in an Isolated Thin Si Meta-Structure.

Nonlinear nanophotonic devices have shown great potential for on-chip information processing, quantum source, 3D microfabrication, greatly promoting the developments of integrated optics, quantum science, nanoscience and technologies, etc. To promote the applications of nonlinear nanodevices, improving the nonlinear efficiency, expanding the spectra region of nonlinear response and reducing device thickness are three key issues. Herein, this study focuses on the nonlinear effect of third-harmonic generation (THG), and present a thin Si meta-sructure to improve the THG efficiency in the ultraviolet (UV) region. The measured THG efficiency is up to 10-5 at an emission wavelength of 309 nm. Also, the THG nanosystem is only 100 nm in thickness, which is two-five times thinner than previous all-dielectric nanosystems applied in THG studies. These findings not only present a powerful thin meta-structure with highly efficient THG emission in UV region, but also provide a constructive avenue for further understanding the light-matter interactions at subwavelength scales, guiding the design and fabricating of advanced photonic devices in future.

Strong Coupling of Resonant Metasurfaces with Epsilon-Near-Zero Guided Modes.

We study, both theoretically and experimentally, strong interaction between a quasi-bound state in the continuum (QBIC) supported by a resonant metasurface with an epsilon-near-zero (ENZ) guided mode excited in an ultrathin ITO layer. We observe and quantify the strong coupling regime of the QBIC-ENZ interaction in the hybrid metasurface manifested through the mode splitting over 200 meV. We also measure experimentally the resonant nonlinear response enhanced near the ENZ frequency and observe the effective nonlinear refractive index up to ∼4 × 10-13 m2/W in the ITO-integrated dielectric nanoresonators, which provides a promising platform for low-power nonlinear photonic devices.

Multiplexed manipulation of orbital angular momentum and wavelength in metasurfaces based on arbitrary complex-amplitude control.

Due to its unbounded and orthogonal modes, the orbital angular momentum (OAM) is regarded as a key optical degree of freedom (DoF) for future information processing with ultra-high capacity and speed. Although the manipulation of OAM based on metasurfaces has brought about great achievements in various fields, such manipulation currently remains at single-DoF level, which means the multiplexed manipulation of OAM with other optical DoFs is still lacking, greatly hampering the application of OAM beams and advancement of metasurfaces. In order to overcome this challenge, we propose the idea of multiplexed coherent pixel (MCP) for metasurfaces. This approach enables the manipulation of arbitrary complex-amplitude under incident lights of both plane and OAM waves, on the basis of which we have realized the multiplexed DoF control of OAM and wavelength. As a result, the MCP method expands the types of incident lights which can be simultaneously responded by metasurfaces, enriches the information processing capability of metasurfaces, and creates applications of information encryption and OAM demultiplexer. Our findings not only provide means for the design of high-security and high-capacity metasurfaces, but also raise the control and application level of OAM, offering great potential for multifunctional nanophotonic devices in the future.

High-Resolution Metalens Imaging Polarimetry.

Imaging polarimeters find many critical applications in applications ranging from remote sensing to biological detection. Metasurfaces have been proposed as a compact approach for imaging polarimeters, but prior strategies suffer from low imaging resolution. Here, we propose an interleaved metalens configuration for polarization imaging where three-row metasurface units within a group individually interact with three pairs of orthogonal polarization channels. The optical paths between the object and adjacent three-row metasurfaces are nearly equal, allowing the construction of a metalens polarimeter with an unlimited numerical aperture (NA), which is beneficial for high-resolution polarization imaging. The metalens polarimeter fabricated by crystalline silicon nanostructures has a NA of 0.51 at 632.8 nm and achieves an imaging resolution of up to a 1.2-fold wavelength. Polarimetric microscopy experiments demonstrate that metalens polarimeters can realize high-resolution polarization imaging for various microscopic samples. This study offers a promising solution for high-resolution metasurface polarization imaging, with the potential for widespread applications.

Enhancing chiroptical responses in the nanoparticle system by manipulating the far-field and near-field couplings.

Employing nanostructure to generate large chiroptical response has been cultivated as an emerging field, for its great potentials in integrated optics, biochemistry detections, etc. However, the lack of intuitive approaches for analytically describing the chiroptical nanoparticles has discouraged researchers from effectively designing advanced chiroptical structures. In this work, we take the twisted nanorod dimer system as a basic example to provide an analytical approach from the perspective of mode coupling, including far-field coupling and near-field coupling of nanoparticles. Using this approach, we can calculate the expression of circular dichroism (CD) in the twisted nanorod dimer system, which can establish the analytical relationship between the chiroptical response and the basic parameters of this system. Our results show that the CD response can be engineered by modulating the structure parameters, and a high CD response of ∼ 0.78 under the guidance of this approach has been achieved.

Color-selective three-dimensional polarization structures.

Polarization as an important degree of freedom for light plays a key role in optics. Structured beams with controlled polarization profiles have diverse applications, such as information encoding, display, medical and biological imaging, and manipulation of microparticles. However, conventional polarization optics can only realize two-dimensional polarization structures in a transverse plane. The emergent ultrathin optical devices consisting of planar nanostructures, so-called metasurfaces, have shown much promise for polarization manipulation. Here we propose and experimentally demonstrate color-selective three-dimensional (3D) polarization structures with a single metasurface. The geometric metasurfaces are designed based on color and phase multiplexing and polarization rotation, creating various 3D polarization knots. Remarkably, different 3D polarization knots in the same observation region can be achieved by controlling the incident wavelengths, providing unprecedented polarization control with color information in 3D space. Our research findings may be of interest to many practical applications such as vector beam generation, virtual reality, volumetric displays, security, and anti-counterfeiting.

Au@Ag Nanorods-PDMS Wearable Mouthguard as a Visualized Detection Platform for Screening Dental Caries and Periodontal Diseases.

The development of easy-to-use, low-cost, and visualized detection platforms for screening human dental caries and periodontal diseases is in urgent demand. In this work, a Au@Ag nanorods-poly(dimethylsiloxane) (Au@Ag NRs-PDMS) wearable mouthguard, which can visualize the tooth lesion sites through the color change of it at the corresponding locations, is presented. The Au@Ag NRs-PDMS composite exhibits a distinct color response to hydrogen sulfide (H2 S) gas generated by bacterial decay at the lesion sites. Moreover, the Au@Ag NRs-PDMS mouthguard is demonstrated to own desired mechanical properties, excellent chemical stability, as well as good biocompatibility, and can accurately locate the lesion sites in human oral cavity. These findings suggest that the mouthguard has the potential to be utilized on a large scale to help people self-monitor their oral health in daily life, and treat oral diseases locally.

Steering Room-Temperature Plexcitonic Strong Coupling: A Diexcitonic Perspective.

Plexcitonic strong coupling between a plasmon-polariton and a quantum emitter empowers ultrafast quantum manipulations in the nanoscale under ambient conditions. The main body of previous studies deals with homogeneous quantum emitters. To enable multiqubit states for future quantum computing and network, the strong coupling involving two excitons of the same material but different resonant energies has been investigated and observed primarily at very low temperature. Here, we report a room-temperature diexcitonic strong coupling (DiSC) nanosystem in which the excitons of a transition metal dichalcogenide monolayer and dye molecules are both strongly coupled to a single Au nanocube. Coherent information exchange in this DiSC nanosystem could be observed even when exciton energy detuning is about five times larger than the respective line widths. The strong coupling behaviors in such a DiSC nanosystem can be manipulated by tuning the plasmon resonant energies and the coupling strengths, opening up a paradigm of controlling plasmon-assisted coherent energy transfer.

Metaoptronic Multiplexed Interface for Probing Bioentity Behaviors.

Biointerface sensors have brought about remarkable advances in modern biomedicine. To accurately monitor bioentity's behaviors, biointerface sensors need to capture three main types of information, which are the electric, spectroscopic, and morphologic signals. Simultaneously obtaining these three types of information is of critical importance in the development of future biosensor, which is still not possible in the existing biosensors. Herein, by synergizing metamaterials, optical, and electronic sensing designs, we proposed the metaoptronic multiplexed interface (MMI) and built a MMI biosensor which can collectively record electric, spectroscopic, and morphologic information on bioentities. The MMI biosensor enables the real-time triple-monitoring of cellular dynamics and opens up the possibility for powerlessly monitoring ocular dryness. Our findings not only demonstrate an advanced multiplexed biointerface sensor with integrated capacities but also help to identify a uniquely significant arena for the nanomaterials, meta-optics, and nanotechnologies to play their roles in a complementary manner.

On-demand spin-state manipulation of single-photon emission from quantum dot integrated with metasurface.

The semiconductor quantum dot (QD) has been successfully demonstrated as a potentially scalable and on-chip integration technology to generate the triggered photon streams that have many important applications in quantum information science. However, the randomicity of these photon streams emitted from the QD seriously compromises its use and especially hinders the on-demand manipulation of the spin states. Here, by accurately integrating a QD and its mirror image onto the two foci of a bifocal metalens, we demonstrate the on-demand generation and separation of the spin states of the emitted single photons. The photon streams with different spin states emitted from the QD can be flexibly manipulated to propagate along arbitrarily designed directions with high collimation of the smallest measured beaming divergence angle of 3.17°. Our work presents an effectively integrated quantum method for the simultaneously on-demand manipulation of the polarization, propagation, and collimation of the emitted photon streams.

Reconfigurable Photon Sources Based on Quantum Plexcitonic Systems.

A single photon in a strongly nonlinear cavity is able to block the transmission of a second photon, thereby converting incident coherent light into antibunched light, which is known as the photon blockade effect. Photon antipairing, where only the entry of two photons is blocked and the emission of bunches of three or more photons is allowed, is based on an unconventional photon blockade mechanism due to destructive interference of two distinct excitation pathways. We propose quantum plexcitonic systems with moderate nonlinearity to generate both antibunched and antipaired photons. The proposed plexcitonic systems benefit from subwavelength field localizations that make quantum emitters spatially distinguishable, thus enabling a reconfigurable photon source between antibunched and antipaired states via tailoring the energy bands. For a realistic nanoprism plexcitonic system, chemical and optical schemes of reconfiguration are demonstrated. These results pave the way to realize reconfigurable nonclassical photon sources in a simple quantum plexcitonic platform.

Perturbative countersurveillance metaoptics with compound nanosieves.

The progress of metaoptics relies on identifying photonic materials and geometries, the combination of which represents a promising approach to complex and desired optical functionalities. Material candidate options are primarily limited by natural availability. Thus, the search for meta-atom geometries, by either forward or inverse means, plays a pivotal role in achieving more sophisticated phenomena. Past efforts mainly focused on building the geometric library of individual meta-atoms and synthesizing various ones into a design. However, those efforts neglected the powerfulness of perturbative metaoptics due to the perception that perturbations are usually regarded as adverse and in need of being suppressed. Here, we report a perturbation-induced countersurveillance strategy using compound nanosieves mediated by structural and thermal perturbations. Private information can be almost perfectly concealed and camouflaged by the induced thermal-spectral drifts, enabling information storage and exchange in a covert way. This perturbative metaoptics can self-indicate whether the hidden information has been attacked during delivery. Our results establish a perturbative paradigm of securing a safer world of information and internet of things.

Full-colour nanoprint-hologram synchronous metasurface with arbitrary hue-saturation-brightness control.

The colour gamut, a two-dimensional (2D) colour space primarily comprising hue and saturation (HS), lays the most important foundation for the colour display and printing industries. Recently, the metasurface has been considered a promising paradigm for nanoprinting and holographic imaging, demonstrating a subwavelength image resolution, a flat profile, high durability, and multi-functionalities. Much effort has been devoted to broaden the 2D HS plane, also known as the CIE map. However, the brightness (B), as the carrier of chiaroscuro information, has long been neglected in metasurface-based nanoprinting or holograms due to the challenge in realising arbitrary and simultaneous control of full-colour HSB tuning in a passive device. Here, we report a dielectric metasurface made of crystal silicon nanoblocks, which achieves not only tailorable coverage of the primary colours red, green and blue (RGB) but also intensity control of the individual colours. The colour gamut is hence extruded from the 2D CIE to a complete 3D HSB space. Moreover, thanks to the independent control of the RGB intensity and phase, we further show that a single-layer silicon metasurface could simultaneously exhibit arbitrary HSB colour nanoprinting and a full-colour hologram image. Our findings open up possibilities for high-resolution and high-fidelity optical security devices as well as advanced cryptographic approaches.

Compounding Plasmon⁻Exciton Strong Coupling System with Gold Nanofilm to Boost Rabi Splitting.

Various plasmonic nanocavities possessing an extremely small mode volume have been developed and applied successfully in the study of strong light-matter coupling. Driven by the desire of constructing quantum networks and other functional quantum devices, a growing trend of strong coupling research is to explore the possibility of fabricating simple strong coupling nanosystems as the building blocks to construct complex systems or devices. Herein, we investigate such a nanocube-exciton building block (i.e. AuNC@J-agg), which is fabricated by coating Au nanocubes with excitonic J-aggregate molecules. The extinction spectra of AuNC@J-agg assembly, as well as the dark field scattering spectra of the individual nanocube-exciton, exhibit Rabi splitting of 100⁻140 meV, which signifies strong plasmon⁻exciton coupling. We further demonstrate the feasibility of constructing a more complex system of AuNC@J-agg on Au film, which achieves a much stronger coupling, with Rabi splitting of 377 meV. This work provides a practical pathway of building complex systems from building blocks, which are simple strong coupling systems, which lays the foundation for exploring further fundamental studies or inventing novel quantum devices.

A Low-Cost Metal-Free Photocatalyst Based on Black Phosphorus.

An efficient metal-free photocatalyst composed of black phosphorus (BP) and graphitic carbon nitride (CN) is prepared on a large scale by ball milling. Using economical urea and red phosphorus (RP) as the raw materials, the estimated materials cost of BP/CN is 0.235 Euro per gram. The BP/CN heterostructure shows efficient charge separation and possesses abundant active sites, giving rise to excellent photocatalytic H2 evolution and rhodamine B (RhB) degradation efficiency. Without using a co-catalyst, the metal-free BP/CN emits H2 consistently at a rate as large as 786 µmol h-1 g-1 and RhB is decomposed in merely 25 min during visible-light irradiation. The corresponding electron/hole transfer and catalytic mechanisms are analyzed and described. The efficient metal-free catalyst is promising in visible-light photocatalysis and the simple ball-milling synthetic method can be readily scaled up.

Black Phosphorus/Platinum Heterostructure: A Highly Efficient Photocatalyst for Solar-Driven Chemical Reactions.

A 2D black phosphorus/platinum heterostructure (Pt/BP) is developed as a highly efficient photocatalyst for solar-driven chemical reactions. The heterostructure, synthesized by depositing BP nanosheets with ultrasmall (≈1.1 nm) Pt nanoparticles, shows strong Pt-P interactions and excellent stability. The Pt/BP heterostructure exhibits obvious P-type semiconducting characteristics and efficient absorption of solar energy extending into the infrared region. Furthermore, during light illumination, accelerated charge separation is observed from Pt/BP as manifested by the ultrafast electron migration (0.11 ps) detected by a femtosecond pump-probe microscopic optical system as well as efficient electron accumulation on Pt revealed by in situ X-ray photoelectron spectroscopy. These unique properties result in remarkable performance of Pt/BP in typical hydrogenation and oxidation reactions under simulated solar light illumination, and its efficiency is much higher than that of other common Pt catalysts and even much superior to that of conventional thermal catalysis. The 2D Pt/BP heterostructure has enormous potential in photochemical reactions involving solar light and the results of this study provide insights into the design of next-generation high-efficiency photocatalysts.

Continuous wave pumped single-mode nanolasers in inorganic perovskites with robust stability and high quantum yield.

Perovskite lasers have aroused great interest in recent years due to their ultra-low lasing threshold, high quantum yields, easily tuned emission colors and great potential for electrically pumped nanolasing, which opens up new possibilities in obtaining highly coherent light sources at the nanoscale. Compared with the widely studied organic-inorganic hybrid perovskites, the inorganic (CsPbX3) have gradually become an emerging research focus because of their relatively better stability. However, some problems still hinder their actual applications, such as the seldom explored lasing quantum yield and the difficulties of further improving stability. Herein, a simple method is proposed to synthesize CsPbX3 nanowires in ambient conditions, and these CsPbX3 nanowires exhibit perfect crystallization and outstanding stability (over 1 year). Perovskite lasing with single mode and a low threshold of 12.33 µJ cm-2 as well as a high lasing quantum yield up to ∼58% are obtained. More interestingly, a high quality single-mode laser with ultra-narrow linewidth of 0.09 nm can be obtained when the CsPbX3 NWs are excited by continuous wave in low-temperature condition. Our results not only enrich the study of inorganic perovskite materials with a new synthetic method, but also uncover new lasing properties of CsPbX3 NWs, suggesting a broad application of the inorganic perovskite materials.

Combining gold nanoparticle antennas with single-molecule fluorescence resonance energy transfer (smFRET) to study DNA hairpin dynamics.

The association of a plasmonic nano-antenna with single-molecule FRET technique presents new prospects to investigate the dynamics of biological molecules. However, the presence of a plasmonic nano-antenna significantly modifies the FRET rate and efficiency; this makes its applicability to the prevalent single-molecule FRET experiments unclear. Herein, using gold nanoparticle antennas of different sizes and DNA hairpins labelled with FRET pairs (Cy3 and Cy5) as the model system, we performed experiments to study the folding dynamics of single DNA hairpins at various salt concentrations. Our results indicate that gold nanoparticle antennas can enhance single-molecule fluorescence of Cy3 and Cy5 up to 3-5 folds, substantially reduce the FRET efficiency, and alter the obtained FRET efficiency histograms. However, the folding dynamics of DNA hairpins remains unaffected, and the correct kinetic and dynamic information can still be extracted from the seriously modified FRET efficiencies. Therefore, our experiments demonstrate the feasibility and compatibility for applying plasmonic nano-antennas to the mostly used single-molecule FRET assays, which provide a broad range of possibilities for the future applications of these nano-antennas in studying various essential biological processes.

Precise characterization of self-catalyzed III-V nanowire heterostructures via optical second harmonic generation.

We demonstrate the utility of optical second harmonic generation (SHG) polarimetry to perform structural characterization of self-assembled zinc-blende/wurtzite III-V nanowire heterostructures. By analyzing four anisotropic SHG polarimetric patterns, we distinguish between wurtzite (WZ), zinc-blende (ZB) and ZB/WZ mixing III-V semiconducting crystal structures in nanowire systems. By neglecting the surface contributions and treating the bulk crystal within the quasi-static approximation, we can well explain the optical SHG polarimetry from the NWs with diameter from 200-600 nm. We show that the optical in-coupling and out-coupling coefficients arising from depolarization field can determine the polarization of the SHG. We also demonstrate micro-photoluminescence of GaAs quantum dots in related ZB and ZB/WZ mixing sections of core-shell NW structure, in agreement with the SHG polarimetry results. The ability to perform in situ SHG-based crystallographic study of semiconducting single and multi-crystalline nanowire heterostructures will be useful in displaying structure-property relationships of nanodevices.

Strong Light-Matter Interactions in Single Open Plasmonic Nanocavities at the Quantum Optics Limit.

Reaching the quantum optics limit of strong light-matter interactions between a single exciton and a plasmon mode is highly desirable, because it opens up possibilities to explore room-temperature quantum devices operating at the single-photon level. However, two challenges severely hinder the realization of this limit: the integration of single-exciton emitters with plasmonic nanostructures and making the coupling strength at the single-exciton level overcome the large damping of the plasmon mode. Here, we demonstrate that these two hindrances can be overcome by attaching individual J aggregates to single cuboid Au@Ag nanorods. In such hybrid nanosystems, both the ultrasmall mode volume of ∼71 nm^{3} and the ultrashort interaction distance of less than 0.9 nm make the coupling coefficient between a single J-aggregate exciton and the cuboid nanorod as high as ∼41.6 meV, enabling strong light-matter interactions to be achieved at the quantum optics limit in single open plasmonic nanocavities.