Observation of intrinsic chiral bound states in the continuum.

Photons with spin angular momentum possess intrinsic chirality, which underpins many phenomena including nonlinear optics1, quantum optics2, topological photonics3 and chiroptics4. Intrinsic chirality is weak in natural materials, and recent theoretical proposals5-7 aimed to enlarge circular dichroism by resonant metasurfaces supporting bound states in the continuum that enhance substantially chiral light-matter interactions. Those insightful works resort to three-dimensional sophisticated geometries, which are too challenging to be realized for optical frequencies8. Therefore, most of the experimental attempts9-11 showing strong circular dichroism rely on false/extrinsic chirality by using either oblique incidence9,10 or structural anisotropy11. Here we report on the experimental realization of true/intrinsic chiral response with resonant metasurfaces in which the engineered slant geometry breaks both in-plane and out-of-plane symmetries. Our result marks, to our knowledge, the first observation of intrinsic chiral bound states in the continuum with near-unity circular dichroism of 0.93 and a high quality factor exceeding 2,663 for visible frequencies. Our chiral metasurfaces may lead to a plethora of applications in chiral light sources and detectors, chiral sensing, valleytronics and asymmetric photocatalysis.

Stabilization of hydrogen-bonded molecular chains by carbon nanotubes.

We study numerically nonlinear dynamics of several types of molecular systems composed of hydrogen-bonded chains placed inside carbon nanotubes with open edges. We demonstrate that carbon nanotubes provide a stabilization mechanism for quasi-one-dimensional molecular chains via the formation of their secondary structures. In particular, a polypeptide chain (Gly)N placed inside a carbon nanotube can form a stable helical chain (310-, α-, π-, and ß-helix) with parallel chains of hydrogen-bonded peptide groups. A chain of hydrogen fluoride molecules ⋯FH⋯FH⋯FH can form a hydrogen-bonded zigzag chain. Remarkably, we demonstrate that for molecular complexes (Gly)N∈CNT and (FH)N∈CNT, the hydrogen-bonded chains will remain stable even at T=500 K. Thus, our results suggest that the use of carbon nanotubes with encapsulated hydrogen fluoride molecules may be important for the realization of high proton conductivity at high temperatures.

Chiral organic molecular structures supported by planar surfaces.

We employ the molecular dynamics simulations to study the dynamics of acetanilide (ACN) molecules placed on a flat surface of planar multilayer hexagonal boron nitride. We demonstrate that the ACN molecules, known to be achiral in the three-dimensional space, become chiral after being placed on the substrate. Homochirality of the ACN molecules leads to stable secondary structures stabilized by hydrogen bonds between peptide groups of the molecules. By employing molecular dynamics simulations, we reveal that the structure of the resulting hydrogen-bond chains depends on the isomeric composition of the molecules. If all molecules are homochiral (i.e., with only one isomer being present), they form secondary structures (chains of hydrogen bonds in the shapes of arcs, circles, and spirals). If the molecules at the substrate form a racemic mixture, then no regular secondary structures appear, and only curvilinear chains of hydrogen bonds of random shapes emerge. A hydrogen-bond chain can form a zigzag array only if it has an alternation of isomers. Such chains can create two-dimensional (2D) regular lattices or 2D crystals. The melting scenarios of such 2D crystals depend on density of its coverage of the substrate. At 25% coverage, melting occurs continuously in the temperature interval 295-365 K. For a complete coverage, melting occurs at 415-470 K due to a shift of 11% of all molecules into the second layer of the substrate.

All-Dielectric Nanostructures with a Thermoresponsible Dynamic Polymer Shell.

We suggest a new strategy for creating stimuli-responsive bio-integrated optical nanostructures based on Mie-resonant silicon nanoparticles covered by an ensemble of similarity negatively charged polyelectrolytes (heparin and sodium polystyrene sulfonate). The dynamic tuning of the nanostructures' optical response is due to light-induced heating of the nanoparticles and swelling of the polyelectrolyte shell. The resulting hydrophilic/hydrophobic transitions significantly change the shell thickness and reversible shift of the scattering spectra for individual nanoparticles up to 60 nm. Our findings bring novel opportunities for the application of smart nanomaterials in nanomedicine and bio-integrated nanophotonics.

Metasurfaces with Maximum Chirality Empowered by Bound States in the Continuum.

We demonstrate that rotationally symmetric chiral metasurfaces can support sharp resonances with the maximum optical chirality determined by precise shaping of bound states in the continuum (BICs). Being uncoupled from one circular polarization of light and resonantly coupled to its counterpart, a metasurface hosting the chiral BIC resonance exhibits a narrow peak in the circular dichroism spectrum with the quality factor limited by weak dissipation losses. We propose a realization of such chiral BIC metasurfaces based on pairs of dielectric bars and validate the concept of maximum chirality by numerical simulations.

Photon-Mediated Localization in Two-Level Qubit Arrays.

We predict the existence of a novel interaction-induced spatial localization in a periodic array of qubits coupled to a waveguide. This localization can be described as a quantum analogue of a self-induced optical lattice between two indistinguishable photons, where one photon creates a standing wave that traps the other photon. The localization is caused by the interplay between on-site repulsion due to the photon blockade and the waveguide-mediated long-range coupling between the qubits.

Manipulation of Magnetic Dipole Emission from Eu3+ with Mie-Resonant Dielectric Metasurfaces.

Mie-resonant high-index dielectric nanoparticles and metasurfaces have been suggested as a viable platform for enhancing both electric and magnetic dipole transitions of fluorescent emitters. While the enhancement of the electric dipole transitions by such dielectric nanoparticles has been demonstrated experimentally, the case of magnetic-dipole transitions remains largely unexplored. Here, we study the enhancement of spontaneous emission of Eu3+ ions, featuring both electric and magnetic-dominated dipole transitions, by dielectric metasurfaces composed of Mie-resonant silicon nanocylinders. By coating the metasurfaces with a layer of an Eu3+ doped polymer, we observe an enhancement of the Eu3+ emission associated with the electric (at 610 nm) and magnetic-dominated (at 590 nm) dipole transitions. The enhancement factor depends systematically on the spectral proximity of the atomic transitions to the Mie resonances as well as their multipolar order, both controlled by the nanocylinder size. Importantly, the branching ratio of emission via the electric or magnetic transition channel can be modified by carefully designing the metasurface, where the magnetic dipole transition is enhanced more than the electric transition for cylinders with radii of about 130 nm. We confirm our observations by numerical simulations based on the reciprocity principle. Our results open new opportunities for bright nanoscale light sources based on magnetic transitions.

Inelastic Scattering of Photon Pairs in Qubit Arrays with Subradiant States.

We develop a rigorous theoretical approach for analyzing inelastic scattering of photon pairs in arrays of two-level qubits embedded into a waveguide. Our analysis reveals a strong enhancement of the scattering when the energy of incoming photons resonates with the double-excited subradiant states. We identify the role of different double-excited states in the scattering, such as superradiant, subradiant, and twilight states, as a product of single-excitation bright and subradiant states. Importantly, the N-excitation subradiant states can be engineered only if the number of qubits exceeds 2N. Both the subradiant and twilight states can generate long-lived photon-photon correlations, paving the way to storage and processing of quantum information.

Light-Emitting Halide Perovskite Nanoantennas.

Nanoantennas made of high-index dielectrics with low losses in visible and infrared frequency ranges have emerged as a novel platform for advanced nanophotonic devices. On the other hand, halide perovskites are known to possess high refractive index, and they support excitons at room temperature with high binding energies and quantum yield of luminescence that makes them very attractive for all-dielectric resonant nanophotonics. Here we employ halide perovskites to create light-emitting nanoantennas with enhanced photoluminescence due to the coupling of their excitons to dipolar and multipolar Mie resonances. We demonstrate that the halide perovskite nanoantennas can emit light in the range of 530-770 nm depending on their composition. We employ a simple technique based on laser ablation of thin films prepared by wet-chemistry methods as a novel cost-effective approach for the fabrication of resonant perovskite nanostructures.

Tunable Hybrid Fano Resonances in Halide Perovskite Nanoparticles.

Halide perovskites are known to support excitons at room temperatures with high quantum yield of luminescence that make them attractive for all-dielectric resonant nanophotonics and meta-optics. Here we report the observation of broadly tunable Fano resonances in halide perovskite nanoparticles originating from the coupling of excitons to the Mie resonances excited in the nanoparticles. Signatures of the photon-exciton (" hybrid") Fano resonances are observed in dark-field spectra of isolated nanoparticles, and also in the extinction spectra of aperiodic lattices of such nanoparticles. In the latter case, chemical tunability of the exciton resonance allows reversible tuning of the Fano resonance across the 100 nm bandwidth in the visible frequency range, providing a novel approach to control optical properties of perovskite nanostructures. The proposed method of chemical tuning paves the way to an efficient control of emission properties of on-chip-integrated light-emitting nanoantennas.

Active Tuning of Spontaneous Emission by Mie-Resonant Dielectric Metasurfaces.

Mie-resonant dielectric metasurfaces offer comprehensive opportunities for the manipulation of light fields with high efficiency. Additionally, various strategies for the dynamic tuning of the optical response of such metasurfaces were demonstrated, making them important candidates for reconfigurable optical devices. However, dynamic control of the light-emission properties of active Mie-resonant dielectric metasurfaces by an external control parameter has not been demonstrated so far. Here, we experimentally demonstrate the dynamic tuning of spontaneous emission from a Mie-resonant dielectric metasurface that is situated on a fluorescent substrate and embedded into a liquid crystal cell. By switching the liquid crystal from the nematic state to the isotropic state via control of the cell temperature, we induce a shift of the spectral position of the metasurface resonances. This results in a change of the local photonic density of states, which, in turn, governs the enhancement of spontaneous emission from the substrate. Specifically, we observe spectral tuning of both the electric and magnetic dipole resonances, resulting in a 2-fold increase of the emission intensity at λ ≈ 900 nm. Our results demonstrate a viable strategy to realize flat tunable light sources based on dielectric metasurfaces.

Noninterleaved Metasurface for (26-1) Spin- and Wavelength-Encoded Holograms.

Nanostructured metasurfaces demonstrate extraordinary capabilities to control light at the subwavelength scale, emerging as key optical components to physical realization of multitasked devices. Progress in multitasked metasurfaces has been witnessed in making a single metasurface multitasked by mainly resorting to extra spatial freedom, for example, interleaved subarrays, different angles. However, it imposes a challenge of suppressing the cross-talk among multiwavelength without the help of extra spatial freedom. Here, we introduce an entirely novel strategy of multitasked metasurfaces with noninterleaved single-size Si nanobrick arrays and minimalist spatial freedom demonstrating massive information on 6-bit encoded color holograms. The interference between electric dipole and magnetic dipole in individual Si nanobricks with in-plane orientation enables manipulating six bases of incident photons simultaneously to reconstructed 6-bit wavelength- and spin-dependent multicolor images. Those massively reconstructed images can be distinguished by pattern recognition. It opens an alternative route for integrated optics, data encoding, security encryption, and information engineering.

Generalized Kerker effects in nanophotonics and meta-optics [Invited].

The original Kerker effect was introduced for a hypothetical magnetic sphere, and initially it did not attract much attention due to a lack of magnetic materials required. Rejuvenated by the recent explosive development of the field of metamaterials and especially its core concept of optically-induced artificial magnetism, the Kerker effect has gained an unprecedented impetus and rapidly pervaded different branches of nanophotonics. At the same time, the concept behind the effect itself has also been significantly expanded and generalized. Here we review the physics and various manifestations of the generalized Kerker effects, including the progress in the emerging field of meta-optics that focuses on interferences of electromagnetic multipoles of different orders and origins. We discuss not only the scattering by individual particles and particle clusters, but also the manipulation of reflection, transmission, diffraction, and absorption for metalattices and metasurfaces, revealing how various optical phenomena observed recently are all ubiquitously related to the Kerker's concept.

Engineering scattering patterns with asymmetric dielectric nanorods.

By controlling interference of Mie resonance modes of various nanostructures, we can achieve a large number of nontrivial effects in nanophotonics. In this work, we propose a cylindrical structure in which the spectral overlap of the Mie-type modes can be controlled by drilling a hole parallel to the axis, thus changing unidirectional scattering. We further demonstrate that the scattering patterns can be tailored by rotating the structure to achieve almost arbitrary scattered wave direction.

Nonlinear Optical Magnetism Revealed by Second-Harmonic Generation in Nanoantennas.

Nonlinear effects at the nanoscale are usually associated with the enhancement of electric fields in plasmonic structures. Recently emerged new platform for nanophotonics based on high-index dielectric nanoparticles utilizes optically induced magnetic response via multipolar Mie resonances and provides novel opportunities for nanoscale nonlinear optics. Here, we observe strong second-harmonic generation from AlGaAs nanoantennas driven by both electric and magnetic resonances. We distinguish experimentally the contribution of electric and magnetic nonlinear response by analyzing the structure of polarization states of vector beams in the second-harmonic radiation. We control continuously the transition between electric and magnetic nonlinearities by tuning polarization of the optical pump. Our results provide a direct observation of nonlinear optical magnetism through selective excitation of multipolar nonlinear modes in nanoantennas.

Efficient Second-Harmonic Generation in Nanocrystalline Silicon Nanoparticles.

Recent trends to employ high-index dielectric particles in nanophotonics are motivated by their reduced dissipative losses and large resonant enhancement of nonlinear effects at the nanoscale. Because silicon is a centrosymmetric material, the studies of nonlinear optical properties of silicon nanoparticles have been targeting primarily the third-harmonic generation effects. Here we demonstrate, both experimentally and theoretically, that resonantly excited nanocrystalline silicon nanoparticles fabricated by an optimized laser printing technique can exhibit strong second-harmonic generation (SHG) effects. We attribute an unexpectedly high yield of the nonlinear conversion to a nanocrystalline structure of nanoparticles supporting the Mie resonances. The demonstrated efficient SHG at green light from a single silicon nanoparticle is 2 orders of magnitude higher than that from unstructured silicon films. This efficiency is significantly higher than that of many plasmonic nanostructures and small silicon nanoparticles in the visible range, and it can be useful for a design of nonlinear nanoantennas and silicon-based integrated light sources.

High-Q Supercavity Modes in Subwavelength Dielectric Resonators.

Recent progress in nanoscale optical physics is associated with the development of a new branch of nanophotonics exploring strong Mie resonances in dielectric nanoparticles with a high refractive index. The high-index resonant dielectric nanostructures form building blocks for novel photonic metadevices with low losses and advanced functionalities. However, unlike extensively studied cavities in photonic crystals, such dielectric resonators demonstrate low quality factors (Q factors). Here, we uncover a novel mechanism for achieving giant Q factors of subwavelength nanoscale resonators by realizing the regime of bound states in the continuum. In contrast to the previously suggested multilayer structures with zero permittivity, we reveal strong mode coupling and Fano resonances in homogeneous high-index dielectric finite-length nanorods resulting in high-Q factors at the nanoscale. Thus, high-index dielectric resonators represent the simplest example of nanophotonic supercavities, expanding substantially the range of applications of all-dielectric resonant nanophotonics and meta-optics.

Multifold Enhancement of Third-Harmonic Generation in Dielectric Nanoparticles Driven by Magnetic Fano Resonances.

Strong Mie-type magnetic dipole resonances in all-dielectric nanostructures provide novel opportunities for enhancing nonlinear effects at the nanoscale due to the intense electric and magnetic fields trapped within the individual nanoparticles. Here we study third-harmonic generation from quadrumers of silicon nanodisks supporting high-quality collective modes associated with the magnetic Fano resonance. We observe nontrivial wavelength and angular dependencies of the generated harmonic signal featuring a multifold enhancement of the nonlinear response in oligomeric systems.

Nonlinear Generation of Vector Beams From AlGaAs Nanoantennas.

The quest for nanoscale light sources with designer radiation patterns and polarization has motivated the development of nanoantennas that interact strongly with the incoming light and are able to transform its frequency, radiation, and polarization patterns. Here, we demonstrate dielectric AlGaAs nanoantennas for efficient second harmonic generation, enabling the control of both directionality and polarization of nonlinear emission. This is enabled by specialized III-V semiconductor nanofabrication of high-quality AlGaAs nanostructures embedded in optically transparent low-index material, thus allowing for simultaneous forward and backward nonlinear emission. We show that the nanodisk AlGaAs antennas can emit second harmonic in preferential direction with a backward-to-forward ratio of up to five and can also generate complex vector polarization beams, including beams with radial polarization.