Tuning Multipolar Mie Scattering of Particles on a Dielectric-Covered Mirror.

Optically resonant particles are key building blocks of many nanophotonic devices such as optical antennas and metasurfaces. Because the functionalities of such devices are largely determined by the optical properties of individual resonators, extending the attainable responses from a given particle is highly desirable. Practically, this is usually achieved by introducing an asymmetric dielectric environment. However, commonly used simple substrates have limited influences on the optical properties of the particles atop. Here, we show that the multipolar scattering of silicon microspheres can be effectively modified by placing the particles on a dielectric-covered mirror, which tunes the coupling between the Mie resonances of microspheres and the standing waves and waveguide modes in the dielectric spacer. This tunability allows selective excitation, enhancement, suppression, and even elimination of the multipolar resonances and enables scattering at extended wavelengths, providing transformative opportunities in controlling light-matter interactions for various applications. We further demonstrate with experiments the detection of molecular fingerprints by single-particle mid-infrared spectroscopy and with simulations strong optical repulsive forces that could elevate the particles from a substrate.

Three-Dimensional Optothermal Manipulation of Light-Absorbing Particles in Phase-Change Gel Media.

Rational manipulation and assembly of discrete colloidal particles into architected superstructures have enabled several applications in materials science and nanotechnology. Optical manipulation techniques, typically operated in fluid media, facilitate the precise arrangement of colloidal particles into superstructures by using focused laser beams. However, as the optical energy is turned off, the inherent Brownian motion of the particles in fluid media impedes the retention and reconfiguration of such superstructures. Overcoming this fundamental limitation, we present on-demand, three-dimensional (3D) optical manipulation of colloidal particles in a phase-change solid medium made of surfactant bilayers. Unlike liquid crystal media, the lack of fluid flow within the bilayer media enables the assembly and retention of colloids for diverse spatial configurations. By utilizing the optically controlled temperature-dependent interactions between the particles and their surrounding media, we experimentally exhibit the holonomic microscale control of diverse particles for repeatable, reconfigurable, and controlled colloidal arrangements in 3D. Finally, we demonstrate tunable light-matter interactions between the particles and 2D materials by successfully manipulating and retaining these particles at fixed distances from the 2D material layers. Our experimental results demonstrate that the particles can be retained for over 120 days without any change in their relative positions or degradation in the bilayers. With the capability of arranging particles in 3D configurations with long-term stability, our platform pushes the frontiers of optical manipulation for distinct applications such as metamaterial fabrication, information storage, and security.

Observation of Room-Temperature Exciton-Polariton Emission from Wide-Ranging 2D Semiconductors Coupled with a Broadband Mie Resonator.

Two-dimensional exciton-polaritons in monolayer transition metal dichalcogenides (TMDs) exhibit practical advantages in valley coherence, optical nonlinearities, and even bosonic condensation owing to their light-emission capability. To achieve robust exciton-polariton emission, strong photon-exciton couplings are required at the TMD monolayer, which is challenging due to its atomic thickness. High-quality (Q) factor optical cavities with narrowband resonances are an effective approach but typically limited to a specific excitonic state of a certain TMD material. Herein, we achieve on-demand exciton-polariton emission from a wide range of TMDs at room temperature by hybridizing excitons with broadband Mie resonances spanning the whole visible spectrum. By confining broadband light at the TMD monolayer, our one type of Mie resonator on different TMDs enables enhanced light-matter interactions with multiple excitonic states simultaneously. We demonstrate multi-Rabi splittings and robust polaritonic photoluminescence in monolayer WSe2, WS2, and MoS2. The hybrid system also shows the potential to approach the ultrastrong coupling regime.

Room-Temperature Observation of Near-Intrinsic Exciton Linewidth in Monolayer WS2.

The homogeneous exciton linewidth, which captures the coherent quantum dynamics of an excitonic state, is a vital parameter in exploring light-matter interactions in 2D transition metal dichalcogenides (TMDs). An efficient control of the exciton linewidth is of great significance, and in particular of its intrinsic linewidth, which determines the minimum timescale for the coherent manipulation of excitons. However, such a control is rarely achieved in TMDs at room temperature (RT). While the intrinsic A exciton linewidth is down to 7 meV in monolayer WS2 , the reported RT linewidth is typically a few tens of meV due to inevitable homogeneous and inhomogeneous broadening effects. Here, it is shown that a 7.18 meV near-intrinsic linewidth can be observed at RT when monolayer WS2 is coupled with a moderate-refractive-index hydrogenated silicon nanosphere in water. By boosting the dynamic competition between exciton and trion decay channels in WS2 through the nanosphere-supported Mie resonances, the coherent linewidth can be tuned from 35 down to 7.18 meV. Such modulation of exciton linewidth and its associated mechanism are robust even in presence of defects, easing the sample quality requirement and providing new opportunities for TMD-based nanophotonics and optoelectronics.

Directional Modulation of Exciton Emission Using Single Dielectric Nanospheres.

Coupling emitters with nanoresonators is an effective strategy to control light emission at the subwavelength scale with high efficiency. Low-loss dielectric nanoantennas hold particular promise for this purpose, owing to their strong Mie resonances. Herein, a highly miniaturized platform is explored for the control of emission based on individual subwavelength Si nanospheres (SiNSs) to modulate the directional excitation and exciton emission of 2D transition metal dichalcogenides (2D TMDs). A modified Mie theory for dipole-sphere hybrid systems is derived to instruct the optimal design for desirable modulation performance. Controllable forward-to-backward intensity ratios are experimentally validated in 532 nm laser excitation and 635 nm exciton emission from a monolayer WS2 . Versatile light emission control is achieved for different emitters and excitation wavelengths, benefiting from the facile size control and isotropic shape of SiNSs. Simultaneous modulation of excitation and emission via a single SiNS at visible wavelengths significantly improves the efficiency and directionality of TMD exciton emission and leads to the potential of multifunctional integrated photonics. Overall, the work opens promising opportunities for nanophotonics and polaritonic systems, enabling efficient manipulation, enhancement, and reconfigurability of light-matter interactions.

Tunable Chiral Optics in All-Solid-Phase Reconfigurable Dielectric Nanostructures.

Subwavelength nanostructures with tunable compositions and geometries show favorable optical functionalities for the implementation of nanophotonic systems. Precise and versatile control of structural configurations on solid substrates is essential for their applications in on-chip devices. Here, we report all-solid-phase reconfigurable chiral nanostructures with silicon nanoparticles and nanowires as the building blocks in which the configuration and chiroptical response can be tailored on-demand by dynamic manipulation of the silicon nanoparticle. We reveal that the optical chirality originates from the handedness-dependent coupling between optical resonances of the silicon nanoparticle and the silicon nanowire via numerical simulations and coupled-mode theory analysis. Furthermore, the coexisting electric and magnetic resonances support strong enhancement of optical near-field chirality, which enables label-free enantiodiscrimination of biomolecules in single nanostructures. Our results not only provide insight into the design of functional high-index materials but also bring new strategies to develop adaptive devices for photonic and electronic applications.

Broadband Forward Light Scattering by Architectural Design of Core-Shell Silicon Particles.

A goal in the field of nanoscale optics is the fabrication of nanostructures with strong directional light scattering at visible frequencies. Here, the synthesis of Mie-resonant core-shell particles with overlapping electric and magnetic dipole resonances in the visible spectrum is demonstrated. The core consists of silicon surrounded by a lower index silicon oxynitride (SiOxNy) shell of an adjustable thickness. Optical spectroscopies coupled to Mie theory calculations give the first experimental evidence that the relative position and intensity of the magnetic and electric dipole resonances are tuned by changing the core-shell architecture. Specifically, coating a high-index particle with a low-index shell coalesces the dipoles, while maintaining a high scattering efficiency, thus generating broadband forward scattering. This synthetic strategy opens a route toward metamaterial fabrication with unprecedented control over visible light manipulation.

Suppressing material loss in the visible and near-infrared range for functional nanophotonics using bandgap engineering.

All-dielectric nanostructures have recently opened exciting opportunities for functional nanophotonics, owing to their strong optical resonances along with low material loss in the near-infrared range. Pushing these concepts to the visible range is hindered by their larger absorption coefficient, thus encouraging the search for alternative dielectrics for nanophotonics. Here, we employ bandgap engineering to synthesize hydrogenated amorphous Si nanoparticles (a-Si:H NPs) offering ideal features for functional nanophotonics. We observe significant material loss suppression in a-Si:H NPs in the visible range caused by hydrogenation-induced bandgap renormalization, producing strong higher-order resonant modes in single NPs with Q factors up to ~100 in the visible and near-IR range. We also realize highly tunable all-dielectric meta-atoms by coupling a-Si:H NPs to photochromic spiropyran molecules. ~70% reversible all-optical tuning of light scattering at the higher-order resonant mode under a low incident light intensity is demonstrated. Our results promote the development of high-efficiency visible nanophotonic devices.

Opto-thermoelectric pulling of light-absorbing particles.

Optomechanics arises from the photon momentum and its exchange with low-dimensional objects. It is well known that optical radiation exerts pressure on objects, pushing them along the light path. However, optical pulling of an object against the light path is still a counter-intuitive phenomenon. Herein, we present a general concept of optical pulling-opto-thermoelectric pulling (OTEP)-where the optical heating of a light-absorbing particle using a simple plane wave can pull the particle itself against the light path. This irradiation orientation-directed pulling force imparts self-restoring behaviour to the particles, and three-dimensional (3D) trapping of single particles is achieved at an extremely low optical intensity of 10-2 mW µm-2. Moreover, the OTEP force can overcome the short trapping range of conventional optical tweezers and optically drive the particle flow up to a macroscopic distance. The concept of self-induced opto-thermomechanical coupling is paving the way towards freeform optofluidic technology and lab-on-a-chip devices.

Enhanced Coloration Efficiency of Electrochromic Tungsten Oxide Nanorods by Site Selective Occupation of Sodium Ions.

Coloration efficiency is an important figure of merit in electrochromic windows. Though it is thought to be an intrinsic material property, we tune optical modulation by effective utilization of ion intercalation sites. Specifically, we enhance the coloration efficiency of m-WO2.72 nanocrystal films by selectively intercalating sodium ions into optically active hexagonal sites. To accurately measure coloration efficiencies, significant degradation during cycling is mitigated by introducing atomic-layer-deposited Al2O3 layers. Galvanostatic spectroscopic measurement shows that the site-selective intercalation of sodium ions in hexagonal tunnels enhances the coloration efficiency compared to a nonselective lithium ion-based electrolyte. Electrochemical rate analysis shows insertion of sodium ions to be capacitive-like, another indication of occupying hexagonal sites. Our results emphasize the importance of different site occupation on spectroelectrochemical properties, which can be used for designing materials and selecting electrolytes for enhanced electrochromic performance. In this context, we suggest sodium ion-based electrolytes hold unrealized potential for tungsten oxide electrochromic applications.

Optical nanomanipulation on solid substrates via optothermally-gated photon nudging.

Constructing colloidal particles into functional nanostructures, materials, and devices is a promising yet challenging direction. Many optical techniques have been developed to trap, manipulate, assemble, and print colloidal particles from aqueous solutions into desired configurations on solid substrates. However, these techniques operated in liquid environments generally suffer from pattern collapses, Brownian motion, and challenges that come with reconfigurable assembly. Here, we develop an all-optical technique, termed optothermally-gated photon nudging (OPN), for the versatile manipulation and dynamic patterning of a variety of colloidal particles on a solid substrate at nanoscale accuracy. OPN takes advantage of a thin surfactant layer to optothermally modulate the particle-substrate interaction, which enables the manipulation of colloidal particles on solid substrates with optical scattering force. Along with in situ optical spectroscopy, our non-invasive and contactless nanomanipulation technique will find various applications in nanofabrication, nanophotonics, nanoelectronics, and colloidal sciences.

All-optical reconfigurable chiral meta-molecules.

Chirality is a ubiquitous phenomenon in the natural world. Many biomolecules without inversion symmetry such as amino acids and sugars are chiral molecules. Measuring and controlling molecular chirality at a high precision down to the atomic scale are highly desired in physics, chemistry, biology, and medicine, however, have remained challenging. Herein, we achieve all-optical reconfigurable chiral meta-molecules experimentally using metallic and dielectric colloidal particles as artificial atoms or building blocks to serve at least two purposes. One is that the on-demand meta-molecules with strongly enhanced optical chirality are well-suited as substrates for surface-enhanced chiroptical spectroscopy of chiral molecules and as active components in optofluidic and nanophotonic devices. The other is that the bottom-up-assembled colloidal meta-molecules provide microscopic models to better understand the origin of chirality in the actual atomic and molecular systems.

Tunable Resonance Coupling in Single Si Nanoparticle-Monolayer WS2 Structures.

Two-dimensional semiconducting transition metal dichalcogenides (TMDCs) are extremely attractive materials for optoelectronic applications in the visible and near-infrared range. Coupling these materials to optical nanocavities enables advanced quantum optics and nanophotonic devices. Here, we address the issue of resonance coupling in hybrid exciton-polariton structures based on single Si nanoparticles (NPs) coupled to monolayer (1L)-WS2. We predict a strong coupling regime with a Rabi splitting energy exceeding 110 meV for a Si NP covered by 1L-WS2 at the magnetic optical Mie resonance because of the symmetry of the mode. Further, we achieve a large enhancement in the Rabi splitting energy up to 208 meV by changing the surrounding dielectric material from air to water. The prediction is based on the experimental estimation of TMDC dipole moment variation obtained from the measured photoluminescence spectra of 1L-WS2 in different solvents. An ability of such a system to tune the resonance coupling is realized experimentally for optically resonant spherical Si NPs placed on 1L-WS2. The Rabi splitting energy obtained for this scenario increases from 49.6 to 86.6 meV after replacing air by water. Our findings pave the way to develop high-efficiency optoelectronic, nanophotonic, and quantum optical devices.