Wandering principal optical axes in van der Waals triclinic materials.

Nature is abundant in material platforms with anisotropic permittivities arising from symmetry reduction that feature a variety of extraordinary optical effects. Principal optical axes are essential characteristics for these effects that define light-matter interaction. Their orientation - an orthogonal Cartesian basis that diagonalizes the permittivity tensor, is often assumed stationary. Here, we show that the low-symmetry triclinic crystalline structure of van der Waals rhenium disulfide and rhenium diselenide is characterized by wandering principal optical axes in the space-wavelength domain with above π/2 degree of rotation for in-plane components. In turn, this leads to wavelength-switchable propagation directions of their waveguide modes. The physical origin of wandering principal optical axes is explained using a multi-exciton phenomenological model and ab initio calculations. We envision that the wandering principal optical axes of the investigated low-symmetry triclinic van der Waals crystals offer a platform for unexplored anisotropic phenomena and nanophotonic applications.

Planar hyperbolic polaritons in 2D van der Waals materials.

Anisotropic planar polaritons - hybrid electromagnetic modes mediated by phonons, plasmons, or excitons - in biaxial two-dimensional (2D) van der Waals crystals have attracted significant attention due to their fundamental physics and potential nanophotonic applications. In this Perspective, we review the properties of planar hyperbolic polaritons and the variety of methods that can be used to experimentally tune them. We argue that such natural, planar hyperbolic media should be fairly common in biaxial and uniaxial 2D and 1D van der Waals crystals, and identify the untapped opportunities they could enable for functional (i.e. ferromagnetic, ferroelectric, and piezoelectric) polaritons. Lastly, we provide our perspectives on the technological applications of such planar hyperbolic polaritons.

van der Waals Materials for Overcoming Fundamental Limitations in Photonic Integrated Circuitry.

With the advance of on-chip nanophotonics, there is a high demand for high-refractive-index and low-loss materials. Currently, this technology is dominated by silicon, but van der Waals (vdW) materials with a high refractive index can offer a very advanced alternative. Still, up to now, it was not clear if the optical anisotropy perpendicular to the layers might be a hindering factor for the development of vdW nanophotonics. Here, we studied WS2-based waveguides in terms of their optical properties and, particularly, in terms of possible crosstalk distance. Surprisingly, we discovered that the low refractive index in the direction perpendicular to the atomic layers improves the characteristics of such devices, mainly due to expanding the range of parameters at which single-mode propagation can be achieved. Thus, using anisotropic materials offers new opportunities and novel control knobs when designing nanophotonic devices.

Origin of Zenneck-like waves excited by optical nanoantennas in non-plasmonic transition metals.

The scattering properties of metallic optical antennas are typically examined through the lens of their plasmonic resonances. However, non-plasmonic transition metals also sustain surface waves in the visible. We experimentally investigate in this work the far-field diffraction properties of apertured optical antennas milled on non-plasmonic W films and compare the results with plasmonic references in Ag and Au. The polarization-dependent diffraction patterns and the leakage signal emerging from apertured antennas in both kinds of metals are recorded and analyzed. This thorough comparison with surface plasmon waves reveals that surface waves are launched on W and that they have the common abilities to confine the visible light at metal-dielectric interfaces offering the possibility to tailor the far-field emission. The results have been analyzed through theoretical models accounting for the propagation of a long range surface mode launched by subwavelength apertures, that is scattered in free space by the antenna. This surface mode on W can be qualitatively described as an analogy in the visible of the Zenneck wave in the radio regime. The nature of the new surface waves have been elucidated from a careful analysis of the asymptotic expansion of the electromagnetic propagators, which provides a convenient representation for explaining the Zenneck-like character of the excited waves and opens new ways to fundamental studies of surface waves at the nanoscale beyond plasmonics.

Twisted Two-Dimensional Material Stacks for Polarization Optics.

The ability to control the light polarization state is critically important for diverse applications in information processing, telecommunications, and spectroscopy. Here, we propose that a stack of anisotropic van der Waals materials can facilitate the building of optical elements with Jones matrices of unitary, Hermitian, non-normal, singular, degenerate, and defective classes. We show that the twisted stack with electrostatic control can function as arbitrary-birefringent wave-plate or arbitrary polarizer with tunable degree of non-normality, which in turn give access to plethora of polarization transformers including rotators, pseudorotators, symmetric and ambidextrous polarizers. Moreover, we discuss an electrostatic-reconfigurable stack which can be tuned to operate as four different polarizers and be used for Stokes polarimetry.

Neural network assisted design of plasmonic nanostructures on superconducting transition-edge-sensors for single photon detectors.

Transition edge sensors (TESs) are extremely sensitive thermometers made of superconducting materials operating at their transition temperature, where small variations in temperature give rise to a measurable increase in electrical resistance. Coupled to suitable absorbers, they are used as radiation detectors with very good energy resolution in several experiments. Particularly interesting are the applications that TESs may bring to single photon detection in the visible and infrared regimes. In this work, we propose a method to enhance absorption efficiency at these wavelengths. The operation principle exploits the generation of highly absorbing plasmons on the metallic surface. Following this approach, we report nanostructures featuring theoretical values of absorption reaching 98%, at the telecom design frequency (λ = 1550 nm). The optimization process takes into account the TES requirements in terms of heat capacity, critical temperature and energy resolution leading to a promising design for an operating device. Neural networks were first trained and then used as solvers of the optical properties of the nanostructures. The neural network topology takes the geometrical parameters, the properties of materials and the wavelength of light as input, predicting the absorption spectrum at single wavelength as output. The incorporation of the material properties and the dependence with frequency was crucial to reduce the number of required spectra for training. The results are almost indistinguishable from those calculated with a commonly used numerical method in computational electromagnetism, the finite-difference time-domain algorithm, but up to 106 times faster than the numerical simulation.

Plasmonic Split-Trench Resonator for Trapping and Sensing.

On-chip integration of plasmonics and electronics can benefit a broad range of applications in biosensing, signal processing, and optoelectronics. A key requirement is a chip-scale manufacturing method. Here, we demonstrate a split-trench resonator platform that combines a high-quality-factor resonant plasmonic biosensor with radio frequency (RF) nanogap tweezers. The split-trench resonator can simultaneously serve as a dielectrophoretic trap and a nanoplasmonic sensor. Trapping is accomplished by applying an RF electrical bias across a 10 nm gap, thereby either attracting or repelling analytes. Trapped analytes are detected in a label-free manner using refractive-index sensing, enabled by interference between surface-plasmon standing waves in the trench and light transmitted through the gap. This active sample concentration mechanism enables detection of nanoparticles and proteins at a concentration as low as 10 pM. We can manufacture centimeter-long split-trench cavity resonators with high throughput via photolithography and atomic layer deposition, toward practical applications in biosensing, spectroscopy, and optoelectronics.

Plasmonic antenna coupling to hyperbolic phonon-polaritons for sensitive and fast mid-infrared photodetection with graphene.

Integrating and manipulating the nano-optoelectronic properties of Van der Waals heterostructures can enable unprecedented platforms for photodetection and sensing. The main challenge of infrared photodetectors is to funnel the light into a small nanoscale active area and efficiently convert it into an electrical signal. Here, we overcome all of those challenges in one device, by efficient coupling of a plasmonic antenna to hyperbolic phonon-polaritons in hexagonal-BN to highly concentrate mid-infrared light into a graphene pn-junction. We balance the interplay of the absorption, electrical and thermal conductivity of graphene via the device geometry. This approach yields remarkable device performance featuring room temperature high sensitivity (NEP of 82 pW[Formula: see text]) and fast rise time of 17 nanoseconds (setup-limited), among others, hence achieving a combination currently not present in the state-of-the-art graphene and commercial mid-infrared detectors. We also develop a multiphysics model that shows very good quantitative agreement with our experimental results and reveals the different contributions to our photoresponse, thus paving the way for further improvement of these types of photodetectors even beyond mid-infrared range.

Terahertz and infrared nonlocality and field saturation in extreme-scale nanoslits.

With advances in nanofabrication techniques, extreme-scale nanophotonic devices with critical gap dimensions of just 1-2 nm have been realized. The plasmonic response in these extreme-scale gaps is significantly affected by nonlocal electrodynamics, quenching field enhancement and blue-shifting the resonance with respect to a purely local behavior. The extreme mismatch in lengthscales, ranging from millimeter-long wavelengths to atomic-scale charge distributions, poses a daunting computational challenge. In this paper, we perform computations of a single nanoslit using the hybridizable discontinuous Galerkin method to solve Maxwell's equations augmented with the hydrodynamic model for the conduction-band electrons in noble metals. This method enables the efficient simulation of the slit while accounting for the nonlocal interactions between electrons and the incident light. We study the impact of gap width, film thickness and electron motion model on the plasmon resonances of the slit for two different frequency regimes: (1) terahertz frequencies, which lead to 1000-fold field amplitude enhancements that saturate as the gap shrinks; and (2) the near- and mid-infrared regime, where we show that narrow gaps and thick films cluster Fabry-Pérot (FP) resonances towards lower frequencies, derive a dispersion relation for the first FP resonance, in addition to observing that nonlocality boosts transmittance and reduces enhancement.

High-Contrast Infrared Absorption Spectroscopy via Mass-Produced Coaxial Zero-Mode Resonators with Sub-10 nm Gaps.

We present a wafer-scale array of resonant coaxial nanoapertures as a practical platform for surface-enhanced infrared absorption spectroscopy (SEIRA). Coaxial nanoapertures with sub-10 nm gaps are fabricated via photolithography, atomic layer deposition of a sacrificial Al2O3 layer to define the nanogaps, and planarization via glancing-angle ion milling. At the zeroth-order Fabry-Pérot resonance condition, our coaxial apertures act as a "zero-mode resonator (ZMR)", efficiently funneling as much as 34% of incident infrared (IR) light along 10 nm annular gaps. After removing Al2O3 in the gaps and inserting silk protein, we can couple the intense optical fields of the annular nanogap into the vibrational modes of protein molecules. From 7 nm gap ZMR devices coated with a 5 nm thick silk protein film, we observe high-contrast IR absorbance signals drastically suppressing 58% of the transmitted light and infer a strong IR absorption enhancement factor of 104∼105. These single nanometer gap ZMR devices can be mass-produced via batch processing and offer promising routes for broad applications of SEIRA.

Electrically controlled terahertz magneto-optical phenomena in continuous and patterned graphene.

The magnetic circular dichroism and the Faraday rotation are the fundamental phenomena of great practical importance arising from the breaking of the time reversal symmetry by a magnetic field. In most materials, the strength and the sign of these effects can be only controlled by the field value and its orientation. Furthermore, the terahertz range is lacking materials having the ability to affect the polarization state of the light in a non-reciprocal manner. Here we demonstrate, using broadband terahertz magneto-electro-optical spectroscopy, that in graphene both the magnetic circular dichroism and the Faraday rotation can be modulated in intensity, tuned in frequency and, importantly, inverted using only electrostatic doping at a fixed magnetic field. In addition, we observe strong magneto-plasmonic resonances in a patterned array of graphene antidots, which potentially allows exploiting these magneto-optical phenomena in a broad THz range.

Polaritons in layered two-dimensional materials.

In recent years, enhanced light-matter interactions through a plethora of dipole-type polaritonic excitations have been observed in two-dimensional (2D) layered materials. In graphene, electrically tunable and highly confined plasmon-polaritons were predicted and observed, opening up opportunities for optoelectronics, bio-sensing and other mid-infrared applications. In hexagonal boron nitride, low-loss infrared-active phonon-polaritons exhibit hyperbolic behaviour for some frequencies, allowing for ray-like propagation exhibiting high quality factors and hyperlensing effects. In transition metal dichalcogenides, reduced screening in the 2D limit leads to optically prominent excitons with large binding energy, with these polaritonic modes having been recently observed with scanning near-field optical microscopy. Here, we review recent progress in state-of-the-art experiments, and survey the vast library of polaritonic modes in 2D materials, their optical spectral properties, figures of merit and application space. Taken together, the emerging field of 2D material polaritonics and their hybrids provide enticing avenues for manipulating light-matter interactions across the visible, infrared to terahertz spectral ranges, with new optical control beyond what can be achieved using traditional bulk materials.

Waveguide and Plasmonic Absorption-Induced Transparency.

Absorption-induced transparency (AIT) is one of the family of induced transparencies that has emerged in recent decades in the fields of plasmonics and metamaterials. It is a seemingly paradoxical phenomenon in which transmission through nanoholes in gold and silver is dramatically enhanced at wavelengths where a physisorbed dye layer absorbs strongly. The origin of AIT remains controversial, with both experimental and theoretical work pointing to either surface (plasmonic) or in-hole (waveguide) mechanisms. Here, we resolve this controversy by carefully filling nanoholes in a silver film with dielectric material before depositing dye on the surface. Our experiments and modeling show that not only do plasmonic and waveguide contributions to AIT both exist, but they are spectrally identical, operating in concert when the dye is both in the holes and on the surface.

High-Throughput Fabrication of Resonant Metamaterials with Ultrasmall Coaxial Apertures via Atomic Layer Lithography.

We combine atomic layer lithography and glancing-angle ion polishing to create wafer-scale metamaterials composed of dense arrays of ultrasmall coaxial nanocavities in gold films. This new fabrication scheme makes it possible to shrink the diameter and increase the packing density of 2 nm-gap coaxial resonators, an extreme subwavelength structure first manufactured via atomic layer lithography, both by a factor of 100 with respect to previous studies. We demonstrate that the nonpropagating zeroth-order Fabry-Pérot mode, which possesses slow light-like properties at the cutoff resonance, traps infrared light inside 2 nm gaps (gap volume ∼ λ(3)/10(6)). Notably, the annular gaps cover only 3% or less of the metal surface, while open-area normalized transmission is as high as 1700% at the epsilon-near-zero (ENZ) condition. The resulting energy accumulation alongside extraordinary optical transmission can benefit applications in nonlinear optics, optical trapping, and surface-enhanced spectroscopies. Furthermore, because the resonance wavelength is independent of the cavity length and dramatically red shifts as the gap size is reduced, large-area arrays can be constructed with λresonance ≫ period, making this fabrication method ideal for manufacturing resonant metamaterials.

Absorption-induced transparency metamaterials in the terahertz regime.

Contrary to what might be expected, when an organic dye is sputtered onto an opaque holey metal film, transmission bands can be observed at the absorption energies of the molecules. This phenomenon, known as absorption-induced transparency, is aided by a strong modification of the propagation properties of light inside the holes when filled by the molecules. Despite having been initially observed in metallic structures in the optical regime, new routes for investigation and applications at different spectral regimes can be devised. Here, to illustrate the potential use of absorption-induced transparency at terahertz, a method for molecular detection is presented and supported by a theoretical analysis.

Ultraefficient Coupling of a Quantum Emitter to the Tunable Guided Plasmons of a Carbon Nanotube.

We show that a single quantum emitter can efficiently couple to the tunable plasmons of a highly doped single-wall carbon nanotube (SWCNT). Plasmons in these quasi-one-dimensional carbon structures exhibit deep subwavelength confinement that pushes the coupling efficiency close to 100% over a very broad spectral range. This phenomenon takes place for distances and tube diameters comprising the nanometer and micrometer scales. In particular, we find a ß factor ≈1 for QEs placed 1-100 nm away from SWCNTs that are just a few nanometers in diameter, while the corresponding Purcell factor exceeds 10(6).

Stacking Structures of Few-Layer Graphene Revealed by Phase-Sensitive Infrared Nanoscopy.

The stacking orders in few-layer graphene (FLG) strongly influences the electronic properties of the material. To explore the stacking-specific properties of FLG in detail, one needs powerful microscopy techniques that visualize stacking domains with sufficient spatial resolution. We demonstrate that infrared (IR) scattering scanning near-field optical microscopy (sSNOM) directly maps out the stacking domains of FLG with a nanometric resolution, based on the stacking-specific IR conductivities of FLG. The intensity and phase contrasts of sSNOM are compared with the sSNOM contrast model, which is based on the dipolar tip-sample coupling and the theoretical conductivity spectra of FLG, allowing a clear assignment of each FLG domain as Bernal, rhombohedral, or intermediate stacks for tri-, tetra-, and pentalayer graphene. The method offers 10-100 times better spatial resolution than the far-field Raman and infrared spectroscopic methods, yet it allows far more experimental flexibility than the scanning tunneling microscopy and electron microscopy.

Nonlinear quantum optics in the (ultra)strong light-matter coupling.

The propagation of N photons in one dimensional waveguides coupled to M qubits is discussed, both in the strong and ultrastrong qubit-waveguide coupling. Special emphasis is placed on the characterisation of the nonlinear response and its linear limit for the scattered photons as a function of N, M, qubit inter distance and light-matter coupling. The quantum evolution is numerically solved via the matrix product states technique. The time evolutions for both the field and qubits are computed. The nonlinear character (as a function of N/M) depends on the computed observable. While perfect reflection is obtained for N/M≅1, photon-photon correlations are still resolved for ratios N/M=non-zero. Inter-qubit distance enhances the nonlinear response. Moving to the ultrastrong coupling regime, we observe that inelastic processes are robust against the number of qubits and that the qubit-qubit interaction mediated by the photons is qualitatively modified. The theory developed in this work models experiments in circuit QED, photonic crystals and dielectric waveguides.

Substrate-sensitive mid-infrared photoresponse in graphene.

We report mid-infrared photocurrent spectra of graphene nanoribbon arrays on SiO2 dielectrics showing dual signatures of the substrate interaction. First, hybrid polaritonic modes of graphene plasmons and dielectric surface polar phonons produce a thermal photocurrent in graphene with spectral features that are tunable by gate voltage, nanoribbon width, and light polarization. Second, phonon polaritons associated with the substrate are excited, which indirectly heat up the graphene, leading to a graphene photocurrent with fixed spectral features. Models for other commonly used substrates show that the responsivity of graphene infrared photodetectors can be tailored to specific mid-IR frequency bands by the choice of the substrate.