Alexander J. Giles

Role of epsilon-near-zero substrates in the optical response of plasmonic antennas

Radiation patterns and the resonance wavelength of a plasmonic antenna are significantly influenced by its local environment, particularly its substrate. Here, we experimentally explore the role of dispersive substrates, such as aluminum- or gallium-doped zinc oxide in the near infrared and 4H-silicon carbide in the mid-infrared, upon Au plasmonic antennas, extending from dielectric to metal-like regimes, crossing through epsilon-near-zero (ENZ) conditions. We demonstrate that the vanishing index of refraction within this transition induces a “slowing down” of the rate of spectral shift for the antenna resonance frequency, resulting in an eventual “pinning” of the resonance near the ENZ frequency. This condition corresponds to a strong backward emission with near-constant phase. By comparing heavily doped semiconductors and undoped, polar dielectric substrates with ENZ conditions in the near- and mid-infrared, respectively, we also demonstrate the generality of the phenomenon using both surface plasmon and phonon polaritons, respectively. Furthermore, we also show that the redirected antenna radiation induces a Fano-like interference and an apparent stimulation of optic phonons within SiC.

Resonant Enhancement of Second-Harmonic Generation in the Mid-Infrared Using Localized Surface Phonon Polaritons in Subdiffractional Nanostructures

We report on the strong enhancement of mid-infrared second-harmonic generation (SHG) from SiC nanopillars due to the resonant excitation of localized surface phonon polaritons within the Reststrahlen band. A strong dependence of the SHG enhancement upon the optical mode distribution was observed. One such mode, the monopole, exhibits an enhancement that is beyond what is anticipated from field localization and dispersion of the linear and nonlinear SiC optical properties. Comparing the results for the identical nanostructures made of 4H and 6H SiC polytypes, we demonstrate the interplay of localized surface phonon polaritons with zone-folded weak phonon modes of the anisotropic crystal. Tuning the monopole mode in and out of the region where the zone-folded phonon is excited in 6H-SiC, we observe a further prominent increase of the already enhanced SHG output when the two modes are coupled. Envisioning this interplay as one of the showcase features of mid-infrared nonlinear nanophononics, we discuss its prospects for the effective engineering of nonlinear-optical materials with desired properties in the infrared spectral range.

Nanoscale Mapping and Spectroscopy of Nonradiative Hyperbolic Modes in Hexagonal Boron Nitride Nanostructures

The inherent crystal anisotropy of hexagonal boron nitride (hBN) provides the ability to support hyperbolic phonon polaritons, that is, polaritons that can propagate with very large wave vectors within the material volume, thereby enabling optical confinement to exceedingly small dimensions. Indeed, previous research has shown that nanometer-scale truncated nanocone hBN cavities, with deep subdiffractional dimensions, support three-dimensionally confined optical modes in the mid-infrared. Because of optical selection rules, only a few of the many theoretically predicted modes have been observed experimentally via far-field reflection and scattering-type scanning near-field optical microscopy (s-SNOM). The photothermal induced resonance (PTIR) technique probes optical and vibrational resonances overcoming weak far-field emission by leveraging an atomic force microscope (AFM) probe to transduce local sample expansion caused by light absorption. Here we show that PTIR enables the direct observation of previously unobserved, dark hyperbolic modes of hBN nanostructures. Leveraging these optical modes and their wide range of angular and radial momenta could provide a new degree of control over the electromagnetic near-field concentration, polarization in nanophotonic applications.

Experimental demonstration of the optical lattice resonance in arrays of Si nanoresonators

Optical resonances of crystalline Si nanopillar arrays on a Si substrate are studied using optical reflectivity and Raman spectroscopy. When the nanopillars are arranged in a two-dimensional lattice, a collective resonance is observed in the reflection spectra which is absent for randomly distributed nanopillars. The resonance is due to coherent oscillations in nanopillars, can be tuned spectrally by the nanopillar diameter and lattice period, and strongly suppresses reflection from the Si surface. Raman scattering demonstrates that the reduced reflectivity is accompanied by increased electromagnetic field confined in Si, thus suggesting potential application of the lattice resonance in surface enhanced spectroscopy and thin film solar cells.

Experimental evidence for mobile luminescence center mobility on partial dislocations in 4H-SiC using hyperspectral electroluminescence imaging

We report on the formation, motion, and concentration of localized green emission centers along partial dislocations (PDs) bounding recombination-induced stacking faults (RISFs) in 4H-SiC pin diodes. Electroluminescence imaging depicted the motion of these green emitting point defects during forward bias operation along carbon-core PDs that bound the RISFs. Following high temperature annealing, these green emitting point defects did not contract with the PDs, but remained in the final location during the expansion. This implies that the motion of these green emitting point dislocations is enabled through a recombination-enhanced motion, similar to the process for RISF expansion and contraction within SiC.

Active tuning of surface phonon polariton resonances via carrier photoinjection

Surface phonon polaritons (SPhPs) are attractive alternatives to infrared plasmonics for subdiffractional confinement of infrared light. Localized SPhP resonances in semiconductor nanoresonators are narrow, but that linewidth and the limited extent of the Reststrahlen band limit spectral coverage. To address this limitation, we report active tuning of SPhP resonances in InP and 4H-SiC by photoinjecting free carriers into nanoresonators, taking advantage of the coupling between the carrier plasma and optic phonons to blueshift SPhP resonances. We demonstrate state-of-the-art tuning figures of merit upon continuous-wave excitation (in InP) or pulsed excitation (in 4H-SiC). Lifetime effects cause the tuning to saturate in InP, and carrier redistribution leads to rapid (<50 ps) recovery of the resonance in 4H-SiC. This work demonstrates the potential for this method and opens a path towards actively tuned nanophotonic devices, such as modulators and beacons, in the infrared, and identifies important implications of coupling between electronic and phononic excitations.Infrared surface phonon polariton tuning is achieved by photoinjecting free carriers into resonators.

Aspect-ratio driven evolution of high-order resonant modes and near-field distributions in localized surface phonon polariton nanostructures

Polar dielectrics have garnered much attention as an alternative to plasmonic metals in the mid- to long-wave infrared spectral regime due to their low optical losses. As such, nanoscale resonators composed of these materials demonstrate figures of merit beyond those achievable in plasmonic equivalents. However, until now, only low-order, phonon-mediated, localized polariton resonances, known as surface phonon polaritons (SPhPs), have been observed in polar dielectric optical resonators. In the present work, we investigate the excitation of 16 distinct high-order, multipolar, localized surface phonon polariton resonances that are optically excited in rectangular pillars etched into a semi-insulating silicon carbide substrate. By elongating a single pillar axis we are able to significantly modify the far- and near-field properties of localized SPhP resonances, opening the door to realizing narrow-band infrared sources with tailored radiation patterns. Such control of the near-field behavior of resonances can also impact surface enhanced infrared optical sensing, which is mediated by polarization selection rules, as well as the morphology and strength of resonator hot spots. Furthermore, through the careful choice of polar dielectric material, these results can also serve as the guiding principles for the generalized design of optical devices that operate from the mid- to far-infrared.

Fabrication of phonon-based metamaterial structures using focused ion beam patterning

The focused ion beam (FIB) is a powerful tool for rapid prototyping and machining of functional nanodevices. It is employed regularly to fabricate test metamaterial structures but, to date, has been unsuccessful in fabricating metamaterial structures with features at the nanoscale that rely on surface phonons as opposed to surface plasmons because of the crystalline damage that occurs with the collision cascade associated with ion sputtering. In this study, we employ a simple technique of protecting the crystalline substrate in single-crystal 4H-SiC to design surface phonon polariton-based optical resonance structures. By coating the material surface with a thin film of chromium, we have placed a material of high sputter resistance on the surface, which essentially absorbs the energy in the beam tails. When the beam ultimately punches through the Cr film, the hard walls in the film have the effect of channeling the beam to create smooth sidewalls. This demonstration opens the possibility of further rapid-...

Processing of Cavities in SiC Material for Quantum Technologies

Quantum technology is a field of significant interest that will benefit many applications including communications and sensing. SiC is a promising material for quantum applications such as quantum memories, due to point defects, specifically VSi, in the material, which result in long spin coherence times. We have found that no VSi are present in our epitaxially grown unintentionally and nitrogen-doped 4H-SiC with electron concentrations ranging from 1014 to 1018 cm-3. We create these vacancies using electron irradiation, in concentrations from single defects to ensembles. To utilize the defect luminescence for realistic applications, we have fabricated the SiC into photonic crystal arrays. We present the processing steps required to create photonic crystal cavities in SiC and subsequent challenges.

Strong Coupling Effects Between IR-Inactive Zone Folded LO Phonon and Localized Surface Phonon Polariton Modes in SiC Nanopillars

While plasmonics have a broad range of technological applications including infrared photovoltaics and photodetectors, plasmonic metals are subject to high optical losses in the long-wave infrared spectral regime. In order to reduce optical losses in the infrared, alternatives to plasmonic metals are being explored. One promising alternative employs polar dielectric materials, which exhibit a highly-reflective, optically-metallic spectral band (Reststrahlen band), bounded by the LO and TO optical phonons, and are capable of supporting plasmonic-like resonance in the infrared. In polar dielectrics, plasmonic-like resonances, known as surface phonon polariton (SPhP) resonances, arise from a coupling between incident light and collective oscillations of bound lattice charges, which are mediated by the optical phonons. In this study, we have examined the SPhP resonances of SiC nanopillars with constant height of 950 nm and width in the range of 200–400 nm, as a function of their aspect ratio (AR=Length/Width=0.5–16). As the nanopillar width is decreased, we have found that localized SPhP resonances redshift towards the zone folded LO (ZFLO) phonon that is normally not infrared active. However, as localized SPhP resonances are spectrally tuned through the ZFLO mode, we have found that the latter mode becomes infrared active. Furthermore, reflectance measurements have revealed strong coupling between the ZFLO and both the monopolar and dipolar localized SPhP resonances.