Enantioselective sensing by collective circular dichroism.

Quantitative determination and in situ monitoring of molecular chirality at extremely low concentrations is still challenging with simple optics because of the molecular-scale mismatch with the incident light wavelength. Advances in spectroscopy1-4 and nanophotonics have successfully lowered the detection limit in enantioselective sensing, as it can bring the microscopic chiral characteristics of molecules into the macroscopic scale5-7 or squeeze the chiral light into the subwavelength scale8-17. Conventional nanophotonic approaches depend mainly on the optical helicity density8,9 by localized resonances within an individual structure, such as localized surface plasmon resonances (LSPRs)10-16 or dielectric Mie resonances17. These approaches use the local chiral hotspots in the immediate vicinity of the structure, whereas the handedness of these hotspots varies spatially. As such, these localized resonance modes tend to be error-prone to the stochasticity of the target molecular orientations, vibrations and local concentrations18,19. Here we identified enantioselective characteristics of collective resonances (CRs)20 arising from assembled 2D crystals of isotropic, 432-symmetric chiral gold nanoparticles (helicoids)21,22. The CRs exhibit a strong and uniform chiral near field over a large volume above the 2D crystal plane, resulting from the collectively spinning, optically induced dipoles at each helicoid. Thus, energy redistribution by molecular back action on the chiral near field shifts the CRs in opposite directions, depending on the handedness of the analyte, maximizing the modulation of the collective circular dichroism (CD).

Tailoring Two-Dimensional Matter Using Strong Light-Matter Interactions.

The shaping of matter into desired nanometric structures with on-demand functionalities can enhance the miniaturization of devices in nanotechnology. Herein, strong light-matter interaction was used as an optical lithographic tool to tailor two-dimensional (2D) matter into nanoscale architectures. We transformed 2D black phosphorus (BP) into ultrafine, well-defined, beyond-diffraction-limit nanostructures of ten times smaller size and a hundred times smaller spacing than the incident, femtosecond-pulsed light wavelength. Consequently, nanoribbons and nanocubes/cuboids scaling tens of nanometers were formed by the structured ablation along the extremely confined periodic light fields originating from modulation instability, the tailoring process of which was visualized in real time via light-coupled in situ transmission electron microscopy. The current findings on the controllable nanoscale shaping of BP will enable exotic physical phenomena and further advance the optical lithographic techniques for 2D materials.

Topological Control of 2D Perovskite Emission in the Strong Coupling Regime.

Momentum space topology can be exploited to manipulate radiation in real space. Here we demonstrate topological control of 2D perovskite emission in the strong coupling regime via polaritonic bound states in the continuum (BICs). Topological polarization singularities (polarization vortices and circularly polarized eigenstates) are observed at room temperature by measuring the Stokes parameters of photoluminescence in momentum space. Particularly, in symmetry-broken structures, a very large degree of circular polarization (DCP) of ∼0.835 is achieved in the perovskite emission, which is the largest in perovskite materials to our knowledge. In the strong coupling regime, lower polariton modes shift to the low-loss spectral region, resulting in strong emission enhancement and large DCP. Our reciprocity analysis reveals that DCP is limited by material absorption at the emission wavelength. Polaritonic BICs based on 2D perovskite materials combine unique topological features with exceptional material properties and may become a promising platform for active nanophotonic devices.

Gyroelectric guided modes with transverse optical spin.

The transverse nature of light leads to longitudinal optical spin. Here, the unprecedented transverse optical spin of propagating waves and guided modes in a gyroelectric medium is clarified. We identify the propagation modes in a bulk gyroelectric medium and their polarization in terms of optical spin. The anisotropic permittivity of a gyroelectric medium results in two propagation modes, slow and fast, in which the optical spin varies according to the propagation direction. When the magnetization direction of the gyroelectric medium and the propagation direction of the light are not parallel, these modes possess both the longitudinal and transverse components of optical spin. We also confirm that a gyroelectric slab waveguide induces transverse optical spin in the guided light. We investigate the transport behavior of transverse optical spin in a gyroelectric slab using numerical calculations with a modified 3D finite difference time domain method. These new gyroelectric guided modes offer a novel approach to the manipulation of optical spin on a nanoscale.

Selective bright and dark mode excitation in coupled nanoantennas.

Coupled nanoantennas as metamaterial unit elements possess peculiar spectral and radiational behaviors. We show that nanoantennas made of two identical plasmonic slot resonators can greatly enhance the quality factors of resonance spectra and control radiation patterns through the selective excitation of bright and dark coupled modes. We confirm experimentally the enhanced quality factor of a bright mode in coupled nanoantennas. Adding phase modulators to the coupled microwave antennas, we demonstrate the "dark mode only" excitation of coupled microwave antennas with an incident plane wave. We also show that the bright-to-dark mode conversion and the related changes in radiation patterns can be controlled by the polarization of incident waves. In particular, we achieve leftward or rightward uni-directional radiation upon the injection of left or right circularly polarized waves.

Plasmon Enhanced Direct Bandgap Emissions in Cu7 S4 @Au2 S@Au Nanorings.

Nanostructured copper sulfides, promising earth-abundant p-type semiconductors, have found applications in a wide range of fields due to their versatility, tunable low bandgap, and environmental sustainability. The synthesis of hexagonal Cu7 S4 @Au2 S@Au nanorings exhibiting plasmon enhanced emissions at the direct bandgap is reported. The synthesized Cu7 S4 @Au2 S@Au nanorings show greatly enhanced absorption and emission by local plasmons compared to pure copper sulfide nanoparticles.

Exploring anti-reflection modes in disordered media.

Sensing and manipulating targets hidden under scattering media are universal problems that take place in applications ranging from deep-tissue optical imaging to laser surgery. A major issue in these applications is the shallow light penetration caused by multiple scattering that reflects most of incident light. Although advances have been made to eliminate image distortion by a scattering medium, dealing with the light reflection has remained unchallenged. Here we present a method to minimize reflected intensity by finding and coupling light into the anti-reflection modes of a scattering medium. In doing so, we achieved more than a factor of 3 increase in light penetration. Our method of controlling reflected waves makes it readily applicable to in vivo applications in which detector sensors can only be positioned at the same side of illumination and will therefore lay the foundation of advancing the working depth of many existing optical imaging and treatment technologies.

Chiral Light-Matter Interaction in Optical Resonators.

The Purcell effect explains the modification of the spontaneous decay rate of quantum emitters in a resonant cavity. For quantum emitters such as chiral molecules, however, the cavity modification of the spontaneous decay rate has been little known. Here we extend Purcell's work to the chiral light-matter interaction in optical resonators and find the differential spontaneous decay rate of chiral molecules coupled to left and right circularly polarized resonator modes. We determine the chiral Purcell factor, which characterizes the ability of optical resonators to enhance chiroptical signals, by the quality factor and the chiral mode volume of a resonator, representing, respectively, the temporal confinement of light and the spatial confinement of the helicity of light. We show that the chiral Purcell effect can be applied to chiroptical spectroscopy. Specifically, we propose a realistic scheme to achieve resonator enhanced chiroptical spectroscopy that uses the double fishnet structure as a nanoscale cuvette supporting the chiral Purcell effect.

Babinet-inverted optical Yagi-Uda antenna for unidirectional radiation to free space.

Nanophotonics capable of directing radiation or enhancing quantum-emitter transition rates rely on plasmonic nanoantennas. We present here a novel Babinet-inverted magnetic-dipole-fed multislot optical Yagi-Uda antenna that exhibits highly unidirectional radiation to free space, achieved by engineering the relative phase of the interacting surface plasmon polaritons between the slot elements. The unique features of this nanoantenna can be harnessed for realizing energy transfer from one waveguide to another by working as a future "optical via".

Maximal light-energy transfer through a dielectric/metal-layered electrode on a photoactive device.

We report the fabrication of an optimized low reflective dielectric/metal-layered electrode that provides significant electrical conductivity and light transparency in the near-infrared wavelength regime. By making the metal film thickness thick enough and choosing a proper dielectric layer with a certain thickness, we show that our suggested electrode significantly reduces the light reflection while preserving high electrical conductivity. We demonstrate our optimized electrodes present a highly conductive surface with a sheet resistance of 5.2 Ω/sq and a high light transmittance of near 85% in the near-infrared regime. We also apply our optimized electrode to thin-film organic photovoltaic devices and show the electrode helps in absorbing light energy inside an active layer. We believe that this simple but powerful layered electrode will pave the way for designing transparent electrodes on photoactive devices.

Localized plasmon resonances of bimetallic AgAuAg nanorods.

We investigated the localized surface plasmon resonances of individual AgAuAg nanorods (NRs) using the dark-field spectro-microscopy technique. We find that the scattering spectra of such hetero-NRs show longitudinal resonance wavelengths that are nearly insensitive to the relative composition of Ag and Au. Instead, the resonance is mostly governed by the overall length of the nanorod. This shows that the plasmons oscillate along the entire length of the NR without the significant perturbation at the Ag-Au interfaces. The results demonstrate that the overall geometry as well as the composition determine the tunability of the hetero-metallic nanostructures, and provide an important design rule for the composition-tunable bimetallic plasmon structures.

Rainbow radiating single-crystal Ag nanowire nanoantenna.

Optical antennas interface an object with optical radiation and boost the absorption and emission of light by the objects through the antenna modes. It has been much desired to enhance both excitation and emission processes of the quantum emitters as well as to interface multiwavelength channels for many nano-optical applications. Here we report the experimental implementation of an optical antenna operating in the full visible range via surface plasmon currents induced in a defect-free single-crystalline Ag nanowire (NW). With its atomically flat surface, the long Ag NW reliably establishes multiple plasmonic resonances and produces a unique rainbow antenna radiation in the Fresnel region. Detailed antenna radiation properties, such as radiating near-field patterns and polarization states, were experimentally examined and precisely analyzed by numerical simulations and antenna theory. The multiresonant Ag NW nanoantenna will find superb applications in nano-optical spectroscopy, high-resolution nanoimaging, photovoltaics, and nonlinear signal conversion.

Perfect transmission through Anderson localized systems mediated by a cluster of localized modes.

In a strongly scattering medium where Anderson localization takes place, constructive interference of local non-propagating waves dominate over the incoherent addition of propagating waves. This results in the disappearance of propagating waves within the medium, which significantly attenuates energy transmission. In this numerical study performed in the optical regime, we systematically found resonance modes, called eigenchannels, of a 2-D Anderson localized system that allow for the near-perfect energy transmission. We observed that the internal field distribution of these eigenchannels exhibit dense clustering of localized modes. This strongly suggests that the clustered resonance modes facilitate long-range energy flow of local waves. Our study explicitly elucidates the interplay between wave localization and transmission enhancement in the Anderson localization regime.

Slot antenna as a bound charge oscillator.

We study the scattering properties of an optical slot antenna formed from a narrow rectangular hole in a metal film. We show that slot antennas can be modeled as bound charge oscillators mediating resonant light scattering. A simple closed-form expression for the scattering spectrum of a slot antenna is obtained that reveals the nature of a bound charge oscillator and also the effect of a substrate. We find that the spectral width of scattering resonance is dominated by a radiative damping caused by the Abraham-Lorentz force acting on a bound charge. The bound charge oscillator model provides not only an intuitive physical picture for the scattering of an optical slot antenna but also reasonable numerical agreements with rigorous calculations using the finite-difference time-domain method.

Terahertz pinch harmonics enabled by single nano rods.

A pinch harmonic (or guitar harmonic) is a musical note produced by lightly pressing the thumb of the picking hand upon the string immediately after it is picked [J. Chem. Educ. 84, 1287 (2007)]. This technique turns off the fundamental and all overtones except those with a node at that location. Here we present a terahertz analogue of pinch harmonics, whereby a metallic nano rod placed at a harmonic node on a terahertz nanoresonator suppresses the fundamental mode, making the higher harmonics dominant. Strikingly, a skin depth-wide nano rod placed at the mid-point turns off all resonances. Our work demonstrates that terahertz electromagnetic waves can be tailored by nanoparticles strategically positioned, paving important path towards terahertz switching and detection applications.

Active terahertz nanoantennas based on VO2 phase transition.

Unusual performances of metamaterials such as negative index of refraction, memory effect, and cloaking originate from the resonance features of the metallic composite atom(1-6). Indeed, control of metamaterial properties by changing dielectric environments of thin films below the metallic resonators has been demonstrated(7-11). However, the dynamic control ranges are still limited to less than a factor of 10,(7-11) with the applicable bandwidth defined by the sharp resonance features. Here, we present ultra-broad-band metamaterial thin film with colossal dynamic control range, fulfilling present day research demands. Hybridized with thin VO(2) (vanadium dioxide) (12-18) films, nanoresonator supercell arrays designed for one decade of spectral width in terahertz frequency region show an unprecedented extinction ratio of over 10000 when the underlying thin film experiences a phase transition. Our nanoresonator approach realizes the full potential of the thin film technology for long wavelength applications.

Nanoscale Terahertz Monitoring on Multiphase Dynamic Assembly of Nanoparticles under Aqueous Environment.

Probing the kinetic evolution of nanoparticle (NP) growth in liquids is essential for understanding complex nano-phases and their corresponding functions. Terahertz (THz) sensing, an emerging technology for next-generation laser photonics, has been developed with unique photonic features, including label-free, non-destructive, and molecular-specific spectral characteristics. Recently, metasurface-based sensing platforms have helped trace biomolecules by overcoming low THz absorption cross-sectional limits. However, the direct probing of THz signals in aqueous environments remains difficult. Here, the authors report that vertically aligned nanogap-hybridized metasurfaces can efficiently trap traveling NPs in the sensing region, thus enabling us to monitor the real-time kinetic evolution of NP assemblies in liquids. The THz photonics approach, together with an electric tweezing technique via spatially matching optical hotspots to particle trapping sites with a nanoscale spatial resolution, is highly promising for underwater THz analysis, forging a route toward unraveling the physicochemical events of nature within an ultra-broadband wavelength regime.

Circularly Polarized Emission from Organic-Inorganic Hybrid Perovskites via Chiral Fano Resonances.

Organic-inorganic hybrid perovskites hold great potential for various optoelectronic devices with exceptional properties. Although the direct generation of circularly polarized emission from perovskites would enable various compact devices, achieving a large degree of circular polarization (DCP) at room temperature still remains challenging. Herein, we demonstrate that DCP can be strongly enhanced at the narrow mode position of chiral Fano resonances. In our design, a perovskite film is spin-coated on a symmetry-broken structure with a relatively large feature size. A large DCP of more than 0.5 is achieved at room temperature without the direct patterning of the perovskite layer. Reciprocity calculation reveals that chiral field enhancement enables the emission of opposite helicity to couple into counter-propagating slab modes and leads to a large DCP. Our design is very general and scalable. Our work may lead to circularly polarized light sources based on various perovskite materials.

Near-field transmission matrix microscopy for mapping high-order eigenmodes of subwavelength nanostructures.

As nanoscale photonic devices are densely integrated, multiple near-field optical eigenmodes take part in their functionalization. Inevitably, these eigenmodes are highly multiplexed in their spectra and superposed in their spatial distributions, making it extremely difficult for conventional near-field scanning optical microscopy (NSOM) to address individual eigenmodes. Here, we develop a near-field transmission matrix microscopy for mapping the high-order eigenmodes of nanostructures, which are invisible with conventional NSOM. At an excitation wavelength where multiple modes are superposed, we measure the near-field amplitude and phase maps for various far-field illumination angles, from which we construct a fully phase-referenced far- to near-field transmission matrix. By performing the singular value decomposition, we extract orthogonal near-field eigenmodes such as anti-symmetric mode and quadruple mode of multiple nano-slits whose gap size (50 nm) is smaller than the probe aperture (150 nm). Analytic model and numerical mode analysis validated the experimentally observed modes.

Polyhedral Au nanocrystals exclusively bound by {110} facets: the rhombic dodecahedron.

The rhombic dodecahedral Au nanocrystals enclosed by 12 {110} facets could be readily prepared without the use of any seeds, surfactants, or foreign metal ions but only with N,N-dimethylformamide as both reductant and solvent.