Conventional optical components are limited to size scales much larger than the wavelength of light, as changes to the amplitude, phase and polarization of the electromagnetic fields are accrued ...gradually along an optical path. However, advances in nanophotonics have produced ultrathin, so-called 'flat' optical components that beget abrupt changes in these properties over distances significantly shorter than the free-space wavelength. Although high optical losses still plague many approaches, phonon polariton (PhP) materials have demonstrated long lifetimes for sub-diffractional modes in comparison to plasmon-polariton-based nanophotonics. We experimentally observe a threefold improvement in polariton lifetime through isotopic enrichment of hexagonal boron nitride (hBN). Commensurate increases in the polariton propagation length are demonstrated via direct imaging of polaritonic standing waves by means of infrared nano-optics. Our results provide the foundation for a materials-growth-directed approach aimed at realizing the loss control necessary for the development of PhP-based nanophotonic devices.
Strongly anisotropic media, where the principal components of the dielectric tensor have opposite signs, are called hyperbolic. Such materials exhibit unique nanophotonic properties enabled by the ...highly directional propagation of slow-light modes localized at deeply sub-diffractional length scales. While artificial hyperbolic metamaterials have been demonstrated, they suffer from high plasmonic losses and require complex nanofabrication, which in turn induces size-dependent limitations on optical confinement. The low-loss, mid-infrared, natural hyperbolic material hexagonal boron nitride is an attractive alternative. Here we report on three-dimensionally confined 'hyperbolic polaritons' in boron nitride nanocones that support four series (up to the seventh order) modes in two spectral bands. The resonant modes obey the predicted aspect ratio dependence and exhibit high-quality factors (Q up to 283) in the strong confinement regime (up to λ/86). These observations assert hexagonal boron nitride as a promising platform for studying novel regimes of light-matter interactions and nanophotonic device engineering.
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.
Plasmonics provides great promise for nanophotonic applications. However, the high optical losses inherent in metal-based plasmonic systems have limited progress. Thus, it is critical to identify ...alternative low-loss materials. One alternative is polar dielectrics that support surface phonon polariton (SPhP) modes, where the confinement of infrared light is aided by optical phonons. Using fabricated 6H-silicon carbide nanopillar antenna arrays, we report on the observation of subdiffraction, localized SPhP resonances. They exhibit a dipolar resonance transverse to the nanopillar axis and a monopolar resonance associated with the longitudinal axis dependent upon the SiC substrate. Both exhibit exceptionally narrow linewidths (7–24 cm–1), with quality factors of 40–135, which exceed the theoretical limit of plasmonic systems, with extreme subwavelength confinement of (λres 3/V eff)1/3 = 50–200. Under certain conditions, the modes are Raman-active, enabling their study in the visible spectral range. These observations promise to reinvigorate research in SPhP phenomena and their use for nanophotonic applications.
We use scanning near-field optical microscopy to study the response of hexagonal boron nitride nanocones at infrared frequencies, where this material behaves as a hyperbolic medium. The obtained ...images are dominated by a series of “hot” rings that occur on the sloped sidewalls of the nanocones. The ring positions depend on the incident laser frequency and the nanocone shape. Both dependences are consistent with directional propagation of hyperbolic phonon-polariton rays that are launched at the edges and zigzag through the interior of the nanocones, sustaining multiple internal reflections off the sidewalls. Additionally, we observe a strong overall enhancement of the near-field signal at discrete resonance frequencies. These resonances attest to low dielectric losses that permit coherent standing waves of the subdiffractional polaritons to form. We comment on potential applications of such shape-dependent resonances and the field concentration at the hot rings.
Phonon polaritons, hybrid light-matter quasiparticles resulting from strong coupling of the electromagnetic field with the lattice vibrations of polar crystals are a promising platform for ...mid-infrared photonics but for the moment there has been no proposal allowing for their electrical pumping. Electrical currents in fact mainly generate longitudinal optical phonons, while only transverse ones participate in the creation of phonon polaritons. We demonstrate how to exploit long-cell polytypes of silicon carbide to achieve strong coupling between transverse phonon polaritons and zone-folded longitudinal optical phonons. We develop a microscopic theory predicting the existence of the resulting hybrid longitudinal-transverse excitations. We then provide an experimental observation by tuning the resonance of a nanopillar array through the folded longitudinal optical mode, obtaining a clear spectral anti-crossing. The hybridisation of phonon polaritons with longitudinal phonons could represent an important step toward the development of phonon polariton-based electrically pumped mid-infrared emitters.
The field of nanophotonics focuses on the ability to confine light to nanoscale dimensions, typically much smaller than the wavelength of light. The goal is to develop light-based technologies that ...are impossible with traditional optics. Subdiffractional confinement can be achieved using either surface plasmon polaritons (SPPs) or surface phonon polaritons (SPhPs). SPPs can provide a gate-tunable, broad-bandwidth response, but suffer from high optical losses; whereas SPhPs offer a relatively low-loss, crystal-dependent optical response, but only over a narrow spectral range, with limited opportunities for active tunability. Here, motivated by the recent results from monolayer graphene and multilayer hexagonal boron nitride heterostructures, we discuss the potential of electromagnetic hybrids--materials incorporating mixtures of SPPs and SPhPs--for overcoming the limitations of the individual polaritons. Furthermore, we also propose a new type of atomic-scale hybrid--the crystalline hybrid--where mixtures of two or more atomic-scale (∼3 nm or less) polar dielectric materials lead to the creation of a new material resulting from hybridized optic phonon behaviour of the constituents, potentially allowing direct control over the dielectric function. These atomic-scale hybrids expand the toolkit of materials for mid-infrared to terahertz nanophotonics and could enable the creation of novel actively tunable, yet low-loss optics at the nanoscale.
The creation of a single electron–hole pair (i.e., exciton) per incident photon is a fundamental limitation for current optoelectronic devices including photodetectors and photovoltaic cells. The ...prospect of multiple exciton generation per incident photon is of great interest to fundamental science and the improvement of solar cell technology. Multiple exciton generation is known to occur in semiconductor nanostructures with increased efficiency and reduced threshold energy compared to their bulk counterparts. Here we report a significant enhancement of multiple exciton generation in PbSe quasi-one-dimensional semiconductors (nanorods) over zero-dimensional nanostructures (nanocrystals), characterized by a 2-fold increase in efficiency and reduction of the threshold energy to (2.23 ± 0.03)E g, which approaches the theoretical limit of 2Eg. Photovoltaic cells based on PbSe nanorods are capable of improved power conversion efficiencies, in particular when operated in conjunction with solar concentrators.
Accessing mid-infrared radiation is of great importance for a range of applications, including thermal imaging, sensing, and radiative cooling. Here, we study light interaction with hexagonal boron ...nitride (hBN) nanocavities and reveal strong and tunable resonances across its hyperbolic transition. In addition to conventional phonon-polariton excitations, we demonstrate that the high refractive index of hexagonal boron nitride outside the Reststrahlen band allows enhanced light–matter interactions in deep subwavelength (<λ/15) nanostructures across a broad 7–8 μm range. Emergence and interplay of Fabry–Perot and Mie-like resonances are examined experimentally and theoretically. Near-unity absorption and high quality (Q ≥ 80) resonance interaction in the vicinity of the hBN transverse optical phonon is further observed. Our study provides avenues to design highly efficient and ultracompact structures for controlling mid-infrared radiation and accessing strong light–matter interactions with hBN.
We present X-ray photoelectron spectroscopy, van der Pauw Hall mobilities, low-temperature far-infrared magneto transmission (FIR-MT), and atomic force microscopy (AFM) results from graphene films ...produced by radiative heating in an ultrahigh vacuum (UHV) chamber or produced by radio frequency (RF) furnace annealing in a high vacuum chemical vapor deposition system on Si- and C-face 4H SiC substrates at 1200−1600 °C. Although the vacuum level and heating methods are different, graphene films produced by the two methods are chemically similar with the RF furnace annealing typically producing thicker graphene films than UHV. We observe, however, that the formation of graphene on the two faces is different with the thicker graphene films on the C-face RF samples having higher mobility. The FIR-MT showed a 0(−1) → 1(0) Landau level transition with a √B dependence and a line width consistent with a Dirac fermion with a mobility >250 000 cm2·V−1·s−1 at 4.2 K in a C-face RF sample having a Hall-effect carrier mobility of 425 cm2·V−1·s−1 at 300 K. AFM shows that graphene grows continuously over the varying morphology of both Si and C-face substrates.
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