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.

Chiral electroluminescence from thin-film perovskite metacavities.

Chiral light sources realized in ultracompact device platforms are highly desirable for various applications. Among active media used for thin-film emission devices, lead-halide perovskites have been extensively studied for photoluminescence due to their exceptional properties. However, up to date, there have been no demonstrations of chiral electroluminescence with a substantial degree of circular polarization (DCP) based on perovskite materials, being critical for the development of practical devices. Here, we propose a concept of chiral light sources based on a thin-film perovskite metacavity and experimentally demonstrate chiral electroluminescence with a peak DCP approaching 0.38. We design a metacavity created by a metal and a dielectric metasurface supporting photonic eigenstates with a close-to-maximum chiral response. Chiral cavity modes facilitate asymmetric electroluminescence of pairs of left and right circularly polarized waves propagating in the opposite oblique directions. The proposed ultracompact light sources are especially advantageous for many applications requiring chiral light beams of both helicities.

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.

Planar chiral metasurfaces with maximal and tunable chiroptical response driven by bound states in the continuum.

Optical metasurfaces with high quality factors (Q-factors) of chiral resonances can boost substantially light-matter interaction for various applications of chiral response in ultrathin, active, and nonlinear metadevices. However, current approaches lack the flexibility to enhance and tune the chirality and Q-factor simultaneously. Here, we suggest a design of chiral metasurface supporting bound state in the continuum (BIC) and demonstrate experimentally chiroptical responses with ultra-high Q-factors and near-perfect circular dichroism (CD = 0.93) at optical frequencies. We employ the symmetry-reduced meta-atoms with high birefringence supporting winding elliptical eigenstate polarizations with opposite helicity. It provides a convenient way for achieving the maximal planar chirality tuned by either breaking in-plane structure symmetry or changing illumination angle. Beyond linear CD, we also achieved strong near-field enhancement CD and near-unitary nonlinear CD in the same planar chiral metasurface design with circular eigen-polarization. Sharply resonant chirality realized in planar metasurfaces promises various practical applications including chiral lasers and chiral nonlinear filters.

Asymmetric topological pumping in nonparaxial photonics.

Topological photonics was initially inspired by the quantum-optical analogy between the Schrödinger equation for an electron wavefunction and the paraxial equation for a light beam. Here, we reveal an unexpected phenomenon in topological pumping observed in arrays of nonparaxial optical waveguides where the quantum-optical analogy becomes invalid. We predict theoretically and demonstrate experimentally an asymmetric topological pumping when the injected field transfers from one side of the waveguide array to the other side whereas the reverse process is unexpectedly forbidden. Our finding could open an avenue for exploring topological photonics that enables nontrivial topological phenomena and designs in photonics driven by nonparaxiality.

Inverse-Designed Metaphotonics for Hypersensitive Detection.

Controlling the flow of broadband electromagnetic energy at the nanoscale remains a critical challenge in optoelectronics. Surface plasmon polaritons (or plasmons) provide subwavelength localization of light but are affected by significant losses. On the contrary, dielectrics lack a sufficiently robust response in the visible to trap photons similar to metallic structures. Overcoming these limitations appears elusive. Here we demonstrate that addressing this problem is possible if we employ a novel approach based on suitably deformed reflective metaphotonic structures. The complex geometrical shape engineered in these reflectors emulates nondispersive index responses, which can be inverse-designed following arbitrary form factors. We discuss the realization of essential components such as resonators with an ultrahigh refractive index of n = 100 in diverse profiles. These structures support the localization of light in the form of bound states in the continuum (BIC), fully localized in air, in a platform in which all refractive index regions are physically accessible. We discuss our approach to sensing applications, designing a class of sensors where the analyte directly contacts areas of ultrahigh refractive index. Leveraging this feature, we report an optical sensor with sensitivity two times higher than the closest competitor with a similar micrometer footprint. Inversely designed reflective metaphotonics offers a flexible technology for controlling broadband light, supporting optoelectronics' integration with large bandwidths in circuitry with miniaturized footprints.

Wafer-Scale Functional Metasurfaces for Mid-Infrared Photonics and Biosensing.

Metasurfaces have emerged as a breakthrough platform for manipulating light at the nanoscale and enabling on-demand optical functionalities for next-generation biosensing, imaging, and light-generating photonic devices. However, translating this technology to practical applications requires low-cost and high-throughput fabrication methods. Due to the limited choice of materials with suitable optical properties, it is particularly challenging to produce metasurfaces for the technologically relevant mid-infrared spectral range. These constraints are overcome by realizing functional metasurfaces on almost completely transparent free-standing metal-oxide membranes. A versatile nanofabrication process is developed and implemented for highly efficient dielectric and plasmonic mid-infrared metasurfaces with wafer-scale and complementary metal-oxide-semiconductor (CMOS)-compatible manufacturing techniques. The advantages of this method are revealed by demonstrating highly uniform and functional metasurfaces, including high-Q structures enabling fine spectral selectivity, large-area metalenses with diffraction-limited focusing capabilities, and birefringent metasurfaces providing polarization control at record-high conversion efficiencies.  Aluminum plasmonic devices and their integration into microfluidics for real-time and label-free mid-infrared biosensing of proteins and lipid vesicles are further demonstrated. The versatility of this approach and its compatibility with mass-production processes bring infrared metasurfaces markedly closer to commercial applications, such as thermal imaging, spectroscopy, and biosensing.

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.

All-Dielectric Active Terahertz Photonics Driven by Bound States in the Continuum.

The remarkable emergence of all-dielectric meta-photonics governed by the physics of high-index dielectric materials offers a low-loss platform for efficient manipulation and subwavelength control of electromagnetic waves from microwaves to visible frequencies. Dielectric metasurfaces can focus electromagnetic waves, generate structured beams and vortices, enhance local fields for advanced sensing, and provide novel functionalities for classical and quantum technologies. Recent advances in meta-photonics are associated with the exploration of exotic electromagnetic modes called the bound states in the continuum (BICs), which offer a simple interference mechanism to achieve large quality factors (Q) through excitation of supercavity modes in dielectric nanostructures and resonant metasurfaces. Here, a BIC-driven terahertz metasurface with dynamic control of high-Q silicon supercavities that are reconfigurable at a nanosecond timescale is experimentally demonstrated. It is revealed that such supercavities enable low-power, optically induced terahertz switching and modulation of sharp resonances for potential applications in lasing, mode multiplexing, and biosensing.

Angle-multiplexed all-dielectric metasurfaces for broadband molecular fingerprint retrieval.

Infrared spectroscopy resolves the structure of molecules by detecting their characteristic vibrational fingerprints. Subwavelength light confinement and nanophotonic enhancement have extended the scope of this technique for monolayer studies. However, current approaches still require complex spectroscopic equipment or tunable light sources. Here, we introduce a novel metasurface-based method for detecting molecular absorption fingerprints over a broad spectrum, which combines the device-level simplicity of state-of-the-art angle-scanning refractometric sensors with the chemical specificity of infrared spectroscopy. Specifically, we develop germanium-based high-Q metasurfaces capable of delivering a multitude of spectrally selective and surface-sensitive resonances between 1100 and 1800 cm-1. We use this approach to detect distinct absorption signatures of different interacting analytes including proteins, aptamers, and polylysine. In combination with broadband incoherent illumination and detection, our method correlates the total reflectance signal at each incidence angle with the strength of the molecular absorption, enabling spectrometer-less operation in a compact angle-scanning configuration ideally suited for field-deployable applications.

Single-Mode Lasing from Imprinted Halide-Perovskite Microdisks.

Halide-perovskite microlasers have demonstrated fascinating performance owing to their low-threshold lasing at room temperature and low-cost fabrication. However, being synthesized chemically, controllable fabrication of such microlasers remains challenging, and it requires template-assisted growth or complicated nanolithography. Here, we suggest and implement an approach for the fabrication of microlasers by direct laser ablation of a thin film on glass with donut-shaped femtosecond laser beams. The fabricated microlasers represent MAPbBr xI y microdisks with 760 nm thickness and diameters ranging from 2 to 9 µm that are controlled by a topological charge of the vortex beam. As a result, this method allows one to fabricate single-mode perovskite microlasers operating at room temperature in a broad spectral range (550-800 nm) with Q-factors up to 5500. High-speed fabrication and reproducibility of microdisk parameters, as well as a precise control of their location on a surface, make it possible to fabricate centimeter-sized arrays of such microlasers. Our finding is important for direct writing of fully integrated coherent light sources for advanced photonic and optoelectronic circuitry.

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.

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.

Quantum metasurface for multiphoton interference and state reconstruction.

Metasurfaces based on resonant nanophotonic structures have enabled innovative types of flat-optics devices that often outperform the capabilities of bulk components, yet these advances remain largely unexplored for quantum applications. We show that nonclassical multiphoton interferences can be achieved at the subwavelength scale in all-dielectric metasurfaces. We simultaneously image multiple projections of quantum states with a single metasurface, enabling a robust reconstruction of amplitude, phase, coherence, and entanglement of multiphoton polarization-encoded states. One- and two-photon states are reconstructed through nonlocal photon correlation measurements with polarization-insensitive click detectors positioned after the metasurface, and the scalability to higher photon numbers is established theoretically. Our work illustrates the feasibility of ultrathin quantum metadevices for the manipulation and measurement of multiphoton quantum states, with applications in free-space quantum imaging and communications.

Disorder-free weak dynamic localization in deformable lattices.

We study the electron transport in a deformable lattice modeled in the semiclassical approximation as a discrete nonlinear elastic chain where acoustic phonons are in thermal equilibrium at temperature T. We reveal that an effective dynamic disorder induced in the system due to thermalized phonons is not strong enough to produce Anderson localization. However, for weak nonlinearity we observe a transition between ballistic (low T) and diffusive (high T) regimes, while for strong nonlinearity the transition occurs between the localized soliton (low T) and diffusive (high T) regimes. Thus, the electron-phonon interaction results in weak temperature-dependent dynamic localization.