Large Optical Tunability from Charge Density Waves in 1T-TaS2 under Incoherent Illumination.

Strongly correlated materials possess a complex energy landscape and host many interesting physical phenomena, including charge density waves (CDWs). CDWs have been observed and extensively studied in many materials since their first discovery in 1972. Yet they present ample opportunities for discovery. Here, we report a large tunability in the optical response of a quasi-2D CDW material, 1T-TaS2, upon incoherent light illumination at room temperature. We hypothesize that the observed tunability is a consequence of light-induced rearrangement of CDW stacking across the layers of 1T-TaS2. Our model, based on this hypothesis, agrees reasonably well with experiments suggesting that the interdomain CDW interaction is a vital potentially knob to control the phase of strongly correlated materials.

Non-Hermitian Selective Thermal Emitters using Metal-Semiconductor Hybrid Resonators.

All open systems that exchange energy with their environment are non-Hermitian. Thermal emitters are open systems that can benefit from the rich set of physical phenomena enabled by their non-Hermitian description. Using phase, symmetry, chirality, and topology, thermal radiation from hot surfaces can be unconventionally engineered to generate light with new states. Such thermal emitters are necessary for a wide variety of applications in sensing and energy conversion. Here, a non-Hermitian selective thermal emitter is experimentally demonstrated, which exhibits passive PT-symmetry in thermal emission at 700 °C. Furthermore, the effect of internal phase of the oscillator system on far-field thermal radiation is experimentally demonstrated. The ability to tune the oscillator phase provides new pathways for both engineering and controlling selective thermal emitters for applications in sensing and energy conversion.

Wavelength-Dependent Optical Force Imaging of Bimetallic Al-Au Heterodimers.

Many important applications of nanometer-scale metallic complexes arise from the light-induced, near-field interactions between their component structures. Here we examine the near-field interactions in bimetallic Al-Au plasmonic nanodisk heterodimers, where the coupling between the primitive plasmons of nanostructures composed of two different metals is studied. Understanding the correlations between nanoparticle morphology and near-field optical properties, particularly for nanostructures composed of two different metals, requires spectrally resolved near-field spatial information. An ideal tool for such investigations is the recently developed photoinduced force microscopy, where the electromagnetic forces between an optically excited plasmonic nanostructure and an adjacent scanning nanoscale tip are measured. Using this approach, we visualize the wavelength-dependent near-field interactions in these bimetallic heterodimers. This system provides a prime example of the diabatic, antenna-reactor picture of plasmon coupling where for a given wavelength the more resonant primitive "driving" plasmon induces a response, the "forced" plasmon, in the off-resonant component. We critically examine spectrally resolved tip-nanostructure forces, comparing experiment with theory, for tips and nanoscale structures of realistic dimensions relative to frequently used approximations for tip geometries. The contrasting effects of dielectric versus metallic tips on acquired spectral force profiles are also examined.

Chemically Responsive Elastomers Exhibiting Unity-Order Refractive Index Modulation.

Chameleons are masters of light, expertly changing their color, pattern, and reflectivity in response to their environment. Engineered materials that share this tunability can be transformative, enabling active camouflage, tunable holograms, and novel colorimetric medical sensors. While progress has been made in creating artificial chameleon skin, existing schemes often require external power, are not continuously tunable, and may prove too stiff or bulky for applications. Here, a chemically tunable, large-area metamaterial is demonstrated that accesses a wide range of colors and refractive indices. An ordered monolayer of nanoresonators is fabricated, then its optical response is dynamically tuned by infiltrating its polymer substrate with solvents. The material shows a strong magnetic response with a dependence on resonator spacing that leads to a highly tunable effective permittivity, permeability, and refractive index spanning negative and positive values. The unity-order index tuning exceeds that of traditional electro-optic and photochromic materials and is robust to cycling, providing a path toward programmable optical elements and responsive light routing.

Hot-Carrier-Mediated Photon Upconversion in Metal-Decorated Quantum Wells.

Manipulating the frequency of electromagnetic waves forms the core of many modern technologies, ranging from imaging and spectroscopy to radio and optical communication. The process of converting photons from higher to lower energy is easily accomplished and technologically widespread. However, upconversion, which is the process of converting lower-energy photons into higher-energy photons, is still a growing field of study with nascent applications and burgeoning interest. Here, we experimentally demonstrate a new photon upconversion technique mediated by hot carriers in plasmonic nanostructures. Hot holes and hot electrons generated via plasmon decay in illuminated metal nanoparticles are injected into an adjacent semiconductor quantum well where they radiatively recombine to emit higher-energy photons. Using GaN/InGaN quantum wells decorated with gold and silver nanoparticles, we show photon upconversion from 2.4 to 2.8 eV. The process scales linearly with illumination power and enables both geometry- and polarization-based tunability. The conversion of plasmonic losses into upconverted optical emission has the potential to impact bioimaging, on-chip wavelength conversion, and high-efficiency photovoltaics.

Refractory plasmonics with titanium nitride: broadband metamaterial absorber.

A high-temperature stable broadband plasmonic absorber is designed, fabricated, and optically characterized. A broadband absorber with an average high absorption of 95% and a total thickness of 240 nm is fabricated, using a refractory plasmonic material, titanium nitride. This absorber integrates both the plasmonic resonances and the dielectric-like loss. It opens a path for the interesting applications such as solar thermophotovoltaics and optical circuits.

Epitaxial superlattices with titanium nitride as a plasmonic component for optical hyperbolic metamaterials.

Titanium nitride (TiN) is a plasmonic material having optical properties resembling gold. Unlike gold, however, TiN is complementary metal oxide semiconductor-compatible, mechanically strong, and thermally stable at higher temperatures. Additionally, TiN exhibits low-index surfaces with surface energies that are lower than those of the noble metals which facilitates the growth of smooth, ultrathin crystalline films. Such films are crucial in constructing low-loss, high-performance plasmonic and metamaterial devices including hyperbolic metamaterials (HMMs). HMMs have been shown to exhibit exotic optical properties, including extremely high broadband photonic densities of states (PDOS), which are useful in quantum plasmonic applications. However, the extent to which the exotic properties of HMMs can be realized has been seriously limited by fabrication constraints and material properties. Here, we address these issues by realizing an epitaxial superlattice as an HMM. The superlattice consists of ultrasmooth layers as thin as 5 nm and exhibits sharp interfaces which are essential for high-quality HMM devices. Our study reveals that such a TiN-based superlattice HMM provides a higher PDOS enhancement than gold- or silver-based HMMs.

Optical absorption of hyperbolic metamaterial with stochastic surfaces.

We investigate the absorption properties of planar hyperbolic metamaterials (HMMs) consisting of metal-dielectric multilayers, which support propagating plane waves with anomalously large wavevectors and high photonic-density-of-states over a broad bandwidth. An interface formed by depositing indium-tin-oxide nanoparticles on an HMM surface scatters light into the high-k propagating modes of the metamaterial and reduces reflection. We compare the reflection and absorption from an HMM with the nanoparticle cover layer versus those of a metal film with the same thickness also covered with the nanoparticles. It is predicted that the super absorption properties of HMM show up when exceedingly large amounts of high-k modes are excited by strong plasmonic resonances. In the case that the coupling interface is formed by non-resonance scatterers, there is almost the same enhancement in the absorption of stochastically perturbed HMM compared to that of metal.

Towards CMOS-compatible nanophotonics: ultra-compact modulators using alternative plasmonic materials.

We propose several planar layouts of ultra-compact plasmonic modulators that utilize alternative plasmonic materials such as transparent conducting oxides and titanium nitride. The modulation is achieved by tuning the carrier concentration in a transparent conducting oxide layer into and out of the plasmon resonance with an applied electric field. The resonance significantly increases the absorption coefficient of the modulator, which enables larger modulation depth. We show that an extinction ratio of 46 dB/µm can be achieved, allowing for a 3-dB modulation depth in much less than one micron at the telecommunication wavelength. Our multilayer structures can be integrated with existing plasmonic and photonic waveguides as well as novel semiconductor-based hybrid photonic/electronic circuits.

Local heating with lithographically fabricated plasmonic titanium nitride nanoparticles.

Titanium nitride is considered a promising alternative plasmonic material and is known to exhibit localized surface plasmon resonances within the near-infrared biological transparency window. Here, local heating efficiencies of disk-shaped nanoparticles made of titanium nitride and gold are compared in the visible and near-infrared regions numerically and experimentally with samples fabricated using e-beam lithography. Results show that plasmonic titanium nitride nanodisks are efficient local heat sources and outperform gold nanodisks in the biological transparency window, dispensing the need for complex particle geometries.

Alternative plasmonic materials: beyond gold and silver.

Materials research plays a vital role in transforming breakthrough scientific ideas into next-generation technology. Similar to the way silicon revolutionized the microelectronics industry, the proper materials can greatly impact the field of plasmonics and metamaterials. Currently, research in plasmonics and metamaterials lacks good material building blocks in order to realize useful devices. Such devices suffer from many drawbacks arising from the undesirable properties of their material building blocks, especially metals. There are many materials, other than conventional metallic components such as gold and silver, that exhibit metallic properties and provide advantages in device performance, design flexibility, fabrication, integration, and tunability. This review explores different material classes for plasmonic and metamaterial applications, such as conventional semiconductors, transparent conducting oxides, perovskite oxides, metal nitrides, silicides, germanides, and 2D materials such as graphene. This review provides a summary of the recent developments in the search for better plasmonic materials and an outlook of further research directions.

Shape-dependent plasmonic response and directed self-assembly in a new semiconductor building block, indium-doped cadmium oxide (ICO).

The influence of particle shape on plasmonic response and local electric field strength is well-documented in metallic nanoparticles. Morphologies such as rods, plates, and octahedra are readily synthesized and exhibit drastically different extinction spectra than spherical particles. Despite this fact, the influence of composition and shape on the optical properties of plasmonic semiconductor nanocrystals, in which free electrons result from heavy doping, has not been well-studied. Here, we report the first observation of plasmonic resonance in indium-doped cadmium oxide (ICO) nanocrystals, which exhibit the highest quality factors reported for semiconductor nanocrystals. Furthermore, we are able to independently control the shape and free electron concentration in ICO nanocrystals, allowing for the influence of shape on the optical response of a plasmonic semiconductor to be conclusively demonstrated. The highly uniform particles may be self-assembled into ordered single component and binary nanocrystal superlattices, and in thin films, exhibit negative permittivity in the near infrared (NIR) region, validating their use as a new class of tunable low-loss plasmonic building blocks for 3-D optical metamaterials.

Demonstration of Al:ZnO as a plasmonic component for near-infrared metamaterials.

Noble metals such as gold and silver are conventionally used as the primary plasmonic building blocks of optical metamaterials. Making subwavelength-scale structural elements from these metals not only seriously limits the optical performance of a device due to high absorption, it also substantially complicates the manufacturing process of nearly all metamaterial devices in the optical wavelength range. As an alternative to noble metals, we propose to use heavily doped oxide semiconductors that offer both functional and fabrication advantages in the near-infrared wavelength range. In this letter, we replace a metal with aluminum-doped zinc oxide as a new plasmonic material and experimentally demonstrate negative refraction in an Al:ZnO/ZnO metamaterial in the near-infrared range.