Time-Dependent Ultrafast Quadratic Nonlinearity in an Epsilon-Near-Zero Platform.

Ultrafast nonlinearity, which results in modulation of the linear optical response, is a basis for the development of time-varying media, in particular those operating in the epsilon-near-zero (ENZ) regime. Here, we demonstrate that the intraband excitation of hot electrons in the ENZ film results in a second-harmonic resonance shift of ∼10 THz (40 nm) and second-harmonic generation (SHG) intensity changes of >100% with only minor (<1%) changes in linear transmission. The modulation is 10-fold enhanced by a plasmonic metasurface coupled to a film, allowing for ultrafast modulation of circularly polarized SHG. The effect is described by the plasma frequency renormalization in the ENZ material and the modification of the electron damping, with a possible influence of the hot-electron dynamics on the quadratic susceptibility. The results elucidate the nature of the second-order nonlinearity in ENZ materials and pave the way to the rational engineering of active nonlinear metamaterials and metasurfaces for time-varying applications.

Entangled dark state mediated by a dielectric cavity within epsilon-near-zero materials.

Two emitters can be entangled by manipulating them through optical fields within a photonic cavity. However, maintaining entanglement for a long time is challenging due to the decoherence of the entangled qubits, primarily caused by cavity loss and atomic decay. Here, we found the entangled dark state between two emitters mediated by a dielectric cavity within epsilon-near-zero (ENZ) materials, ensuring entanglement maintenance over an extended period. To obtain the entangled dark state, we derived an effective model with degenerate mode modulation. In the dielectric cavities within ENZ materials, the decay rate of emitters can be regarded as 0, which is the key to achieving the entangled dark state. Meanwhile, the dark state immune to cavity loss exists when two emitters are in symmetric positions in the dielectric cavity. Additionally, by adjusting the emitters to specific asymmetric positions, it is possible to achieve transient entanglement with higher concurrence. By overcoming the decoherence of the entangled qubits, this study demonstrates stable, long-term entanglement with ENZ materials, holding significant importance for applications such as nanodevice design for quantum communication and quantum information processing.

Giant Enhancement of Second-Order Nonlinearity of Epsilon-near- Zero Medium by a Plasmonic Metasurface.

Nonlinear frequency conversion at the nanoscale is important for many applications in free space and integrated photonics. In epsilon-near-zero (ENZ) materials, second-harmonic generation (SHG) is significantly enhanced but the oblique incidence is required to address nonlinearity. To circumvent this constraint, we design a hybrid metasurface consisting of plasmonic nanostructures on an ENZ nanofilm generating strongly enhanced SHG at normal incidence in transmission. We show that the Au meta-atoms on an indium-tin-oxide (ITO) layer provide an approximately 104-fold experimentally measured SHG enhancement at normal incidence at the fundamental wavelength near the ENZ condition of ITO. This giant enhancement stems from reshaping the vectorial properties of the incident light near the Au nanostructures and its increased coupling to the ENZ film. The proposed hybrid ENZ metasurface offers a promising platform for developing ultracompact and efficient nonlinear optical sources at the nanoscale.

An Electrically Tunable Dual-Wavelength Refractive Index Sensor Based on a Metagrating Structure Integrating Epsilon-Near-Zero Materials.

In this paper, a reconfigurable sensing platform based on an asymmetrical metal-insulator-metal stacked structure integrating an indium tin oxide (ITO) ultrathin film is proposed and investigated numerically. The epsilon-near-zero (ENZ) mode and antisymmetric mode can be resonantly excited, generating near-perfect absorption of over 99.7% at 1144 and 1404 nm, respectively. The absorptivity for the ENZ mode can be modulated from 90.2% to 98.0% by varying the ENZ wavelength of ITO by applying different voltages. To obtain a highly sensitive biosensor, we show that the proposed structure has a full-width at half-maximum (FWHM) of 8.65 nm and a figure-of-merit (FOM) of 24.7 with a sensitivity of 213.3 nm/RI (refractive index) for the glucose solution. Our proposed device has potential for developing tunable biosensors for real-time health monitoring.

Dual-Gated Active Metasurface at 1550 nm with Wide (>300°) Phase Tunability.

Active metasurfaces composed of electrically reconfigurable nanoscale subwavelength antenna arrays can enable real-time control of scattered light amplitude and phase. Achievement of widely tunable phase and amplitude in chip-based active metasurfaces operating at or near 1550 nm wavelength has considerable potential for active beam steering, dynamic hologram rendition, and realization of flat optics with reconfigurable focal lengths. Previously, electrically tunable conducting oxide-based reflectarray metasurfaces have demonstrated dynamic phase control of reflected light with a maximum phase shift of 184° ( Nano Lett. 2016 , 16 , 5319 ). Here, we introduce a dual-gated reflectarray metasurface architecture that enables much wider (>300°) phase tunability. We explore light-matter interactions with dual-gated metasurface elements that incorporate two independent voltage-controlled MOS field effect channels connected in series to form a single metasurface element that enables wider phase tunability. Using indium tin oxide (ITO) as the active metasurface material and a composite hafnia/alumina gate dielectric, we demonstrate a prototype dual-gated metasurface with a continuous phase shift from 0 to 303° and a relative reflectance modulation of 89% under applied voltage bias of 6.5 V.

Gate-Tunable Conducting Oxide Metasurfaces.

Metasurfaces composed of planar arrays of subwavelength artificial structures show promise for extraordinary light manipulation. They have yielded novel ultrathin optical components such as flat lenses, wave plates, holographic surfaces, and orbital angular momentum manipulation and detection over a broad range of the electromagnetic spectrum. However, the optical properties of metasurfaces developed to date do not allow for versatile tunability of reflected or transmitted wave amplitude and phase after their fabrication, thus limiting their use in a wide range of applications. Here, we experimentally demonstrate a gate-tunable metasurface that enables dynamic electrical control of the phase and amplitude of the plane wave reflected from the metasurface. Tunability arises from field-effect modulation of the complex refractive index of conducting oxide layers incorporated into metasurface antenna elements which are configured in reflectarray geometry. We measure a phase shift of 180° and ∼30% change in the reflectance by applying 2.5 V gate bias. Additionally, we demonstrate modulation at frequencies exceeding 10 MHz and electrical switching of ±1 order diffracted beams by electrical control over subgroups of metasurface elements, a basic requirement for electrically tunable beam-steering phased array metasurfaces. In principle, electrically gated phase and amplitude control allows for electrical addressability of individual metasurface elements and opens the path to applications in ultrathin optical components for imaging and sensing technologies, such as reconfigurable beam steering devices, dynamic holograms, tunable ultrathin lenses, nanoprojectors, and nanoscale spatial light modulators.

Tailoring the Thickness-Dependent Optical Properties of Conducting Nitrides and Oxides for Epsilon-Near-Zero-Enhanced Photonic Applications.

The unique properties of the emerging photonic materials, conducting nitrides and oxides, especially their tailorability, large damage thresholds, and, importantly, the so-called epsilon-near-zero (ENZ) behavior, have enabled novel photonic phenomena spanning optical circuitry, tunable metasurfaces, and nonlinear optical devices. This work explores direct control of the optical properties of polycrystalline titanium nitride (TiN) and aluminum-doped zinc oxide (AZO) by tailoring the film thickness, and their potential for ENZ-enhanced photonic applications. This study demonstrates that TiN-AZO bilayers support Ferrell-Berreman modes using the thickness-dependent ENZ resonances in the AZO films operating in the telecom wavelengths spanning from 1470 to 1750 nm. The bilayer stacks also act as strong light absorbers in the ultraviolet regime using the radiative ENZ modes and the Fabry-Perot modes in the constituent TiN films. The studied Berreman resonators exhibit optically induced reflectance modulation of 15% with picosecond response time. Together with the optical response tailorability of conducting oxides and nitrides, using the field enhancement near the tunable ENZ regime can enable a wide range of nonlinear optical phenomena, including all-optical switching, time refraction, and high-harmonic generation.

Broadband Epsilon-near-Zero Reflectors Enhance the Quantum Efficiency of Thin Solar Cells at Visible and Infrared Wavelengths.

The engineering of broadband absorbers to harvest white light in thin-film semiconductors is a major challenge in developing renewable materials for energy harvesting. Many solution-processed materials with high manufacturability and low cost, such as semiconductor quantum dots, require the use of film structures with thicknesses on the order of 1 µm to absorb incoming photons completely. The electron transport lengths in these media, however, are 1 order of magnitude smaller than this length, hampering further progress with this platform. Herein, we show that, by engineering suitably disordered nanoplasmonic structures, we have created a new class of dispersionless epsilon-near-zero composite materials that efficiently harness white light. Our nanostructures localize light in the dielectric region outside the epsilon-near-zero material with characteristic lengths of 10-100 nm, resulting in an efficient system for harvesting broadband light when a thin absorptive film is deposited on top of the structure. By using a combination of theory and experiments, we demonstrate that ultrathin layers down to 50 nm of colloidal quantum dots deposited atop the epsilon-near-zero material show an increase in broadband absorption ranging from 200% to 500% compared to a planar structure of the same colloidal quantum-dot-absorber average thickness. When the epsilon-near-zero nanostructures were used in an energy-harvesting module, we observed a spectrally averaged 170% broadband increase in the external quantum efficiency of the device, measured at wavelengths between 400 and 1200 nm. Atomic force microscopy and photoluminescence excitation measurements demonstrate that the properties of these epsilon-near-zero structures apply to general metals and could be used to enhance the near-field absorption of semiconductor structures more widely. We have developed an inexpensive electrochemical deposition process that enables scaled-up production of this nanomaterial for large-scale energy-harvesting applications.

Nonradiating and radiating modes excited by quantum emitters in open epsilon-near-zero cavities.

Controlling the emission and interaction properties of quantum emitters (QEs) embedded within an optical cavity is a key technique in engineering light-matter interactions at the nanoscale, as well as in the development of quantum information processing. State-of-the-art optical cavities are based on high quality factor photonic crystals and dielectric resonators. However, wealthier responses might be attainable with cavities carved in more exotic materials. We theoretically investigate the emission and interaction properties of QEs embedded in open epsilon-near-zero (ENZ) cavities. Using analytical methods and numerical simulations, we demonstrate that open ENZ cavities present the unique property of supporting nonradiating modes independently of the geometry of the external boundary of the cavity (shape, size, topology, etc.). Moreover, the possibility of switching between radiating and nonradiating modes enables a dynamic control of the emission by, and the interaction between, QEs. These phenomena provide unprecedented degrees of freedom in controlling and trapping fields within optical cavities, as well as in the design of cavity opto- and acoustomechanical systems.