The success of metal-based plasmonics for manipulating light at the nanoscale has been empowered by imaginative designs and advanced nano-fabrication. However, the fundamental optical and electronic ...properties of elemental metals, the prevailing plasmonic media, are difficult to alter using external stimuli. This limitation is particularly restrictive in applications that require modification of the plasmonic response at sub-picosecond timescales. This handicap has prompted the search for alternative plasmonic media, with graphene emerging as one of the most capable candidates for infrared wavelengths. Here we visualize and elucidate the properties of non-equilibrium photo-induced plasmons in a high-mobility graphene monolayer. We activate plasmons with femtosecond optical pulses in a specimen of graphene that otherwise lacks infrared plasmonic response at equilibrium. In combination with static nano-imaging results on plasmon propagation, our infrared pump-probe nano-spectroscopy investigation reveals new aspects of carrier relaxation in heterostructures based on high-purity graphene.
Hexagonal boron nitride (h-BN) is a natural hyperbolic material, in which the dielectric constants are the same in the basal plane (ε(t) ≡ ε(x) = ε(y)) but have opposite signs (ε(t)ε(z) < 0) in the ...normal plane (ε(z)). Owing to this property, finite-thickness slabs of h-BN act as multimode waveguides for the propagation of hyperbolic phonon polaritons--collective modes that originate from the coupling between photons and electric dipoles in phonons. However, control of these hyperbolic phonon polaritons modes has remained challenging, mostly because their electrodynamic properties are dictated by the crystal lattice of h-BN. Here we show, by direct nano-infrared imaging, that these hyperbolic polaritons can be effectively modulated in a van der Waals heterostructure composed of monolayer graphene on h-BN. Tunability originates from the hybridization of surface plasmon polaritons in graphene with hyperbolic phonon polaritons in h-BN, so that the eigenmodes of the graphene/h-BN heterostructure are hyperbolic plasmon-phonon polaritons. The hyperbolic plasmon-phonon polaritons in graphene/h-BN suffer little from ohmic losses, making their propagation length 1.5-2.0 times greater than that of hyperbolic phonon polaritons in h-BN. The hyperbolic plasmon-phonon polaritons possess the combined virtues of surface plasmon polaritons in graphene and hyperbolic phonon polaritons in h-BN. Therefore, graphene/h-BN can be classified as an electromagnetic metamaterial as the resulting properties of these devices are not present in its constituent elements alone.
Uniaxial materials whose axial and tangential permittivities have opposite signs are referred to as indefinite or hyperbolic media. In such materials, light propagation is unusual leading to novel ...and often non-intuitive optical phenomena. Here we report infrared nano-imaging experiments demonstrating that crystals of hexagonal boron nitride, a natural mid-infrared hyperbolic material, can act as a 'hyper-focusing lens' and as a multi-mode waveguide. The lensing is manifested by subdiffractional focusing of phonon-polaritons launched by metallic disks underneath the hexagonal boron nitride crystal. The waveguiding is revealed through the modal analysis of the periodic patterns observed around such launchers and near the sample edges. Our work opens new opportunities for anisotropic layered insulators in infrared nanophotonics complementing and potentially surpassing concurrent artificial hyperbolic materials with lower losses and higher optical localization.
van der Waals heterostructures assembled from atomically thin crystalline layers of diverse two-dimensional solids are emerging as a new paradigm in the physics of materials. We used infrared ...nanoimaging to study the properties of surface phonon polaritons in a representative van der Waals crystal, hexagonal boron nitride. We launched, detected, and imaged the polaritonic waves in real space and altered their wavelength by varying the number of crystal layers in our specimens. The measured dispersion of polaritonic waves was shown to be governed by the crystal thickness according to a scaling law that persists down to a few atomic layers. Our results are likely to hold true in other polar van der Waals crystals and may lead to new functionalities.
We introduce ultraresolving terahertz (THz) near-field microscopy based on THz scattering at atomic force microscope tips. Nanoscale resolution is achieved by THz field confinement at the very tip ...apex to within 30 nm, which is in good agreement with full electro-dynamic calculations. Imaging semiconductor transistors, we provide first evidence of 40 nm (λ/3000) spatial resolution at 2.54 THz (wavelength λ = 118 μm) and demonstrate the simultaneous THz recognition of materials and mobile carriers in a single nanodevice. Fundamentally important, we find that the mobile carrier contrast can be directly related to near-field excitation of THz-plasmons in the doped semiconductor regions. This opens the door to quantitative studies of local carrier concentration and mobility at the nanometer scale. The THz near-field response is extraordinary sensitive, providing contrast from less than 100 mobile electrons in the probed volume. Future improvements could allow for THz characterization of even single electrons or biomolecules.
Graphene, a two-dimensional honeycomb lattice of carbon atoms of great interest in (opto)electronics and plasmonics, can be obtained by means of diverse fabrication techniques, among which chemical ...vapour deposition (CVD) is one of the most promising for technological applications. The electronic and mechanical properties of CVD-grown graphene depend in large part on the characteristics of the grain boundaries. However, the physical properties of these grain boundaries remain challenging to characterize directly and conveniently. Here we show that it is possible to visualize and investigate the grain boundaries in CVD-grown graphene using an infrared nano-imaging technique. We harness surface plasmons that are reflected and scattered by the graphene grain boundaries, thus causing plasmon interference. By recording and analysing the interference patterns, we can map grain boundaries for a large-area CVD graphene film and probe the electronic properties of individual grain boundaries. Quantitative analysis reveals that grain boundaries form electronic barriers that obstruct both electrical transport and plasmon propagation. The effective width of these barriers (∼10-20 nm) depends on the electronic screening and is on the order of the Fermi wavelength of graphene. These results uncover a microscopic mechanism that is responsible for the low electron mobility observed in CVD-grown graphene, and suggest the possibility of using electronic barriers to realize tunable plasmon reflectors and phase retarders in future graphene-based plasmonic circuits.
Optical near fields exist close to any illuminated object. They account for interesting effects such as enhanced pinhole transmission or enhanced Raman scattering enabling single-molecule ...spectroscopy. Also, they enable high-resolution (below 10 nm) optical microscopy. The plasmon-enhanced near-field coupling between metallic nanostructures opens new ways of designing optical properties and of controlling light on the nanometre scale. Here we study the strong enhancement of optical near-field coupling in the infrared by lattice vibrations (phonons) of polar dielectrics. We combine infrared spectroscopy with a near-field microscope that provides a confined field to probe the local interaction with a SiC sample. The phonon resonance occurs at 920 cm-1. Within 20 cm-1 of the resonance, the near-field signal increases 200-fold; on resonance, the signal exceeds by 20 times the value obtained with a gold sample. We find that phonon-enhanced near-field coupling is extremely sensitive to chemical and structural composition of polar samples, permitting nanometre-scale analysis of semiconductors and minerals. The excellent physical and chemical stability of SiC in particular may allow the design of nanometre-scale optical circuits for high-temperature and high-power operation.
Identification of chemical compounds by vibrational spectroscopy at infrared
wavelengths requires macroscopic samples: the spatial resolution is diffraction-limited
to a scale of about half the ...wavelength, or about five micrometres. The scanning
near-field optical microscope,, however, can
reveal sub-wavelength detail because it uses near-field probing rather than
beam focusing. Here we demonstrate the use of the aperture-less approach to
scanning near-field optical microscopy to obtain contrast
in vibrational absorption on a scale of about 100 nanometres, about one-hundredth
of a wavelength. We record infrared scattering from the tip of an atomic force
microscope scanned over a composite polymer film. At the boundary between
different polymers we observe contrast changes owing to changes in vibrational
absorption. The contrast is strongly enhanced in the near field of the probe
tip, which we interpret as evidence of surface-enhanced infrared absorption. When extended to multi-wavelength operation, this approach should
enable imaging of chemical composition at nanometre resolution.
Surface plasmons are collective oscillations of electrons in metals or semiconductors that enable confinement and control of electromagnetic energy at subwavelength scales. Rapid progress in ...plasmonics has largely relied on advances in device nano-fabrication, whereas less attention has been paid to the tunable properties of plasmonic media. One such medium--graphene--is amenable to convenient tuning of its electronic and optical properties by varying the applied voltage. Here, using infrared nano-imaging, we show that common graphene/SiO(2)/Si back-gated structures support propagating surface plasmons. The wavelength of graphene plasmons is of the order of 200 nanometres at technologically relevant infrared frequencies, and they can propagate several times this distance. We have succeeded in altering both the amplitude and the wavelength of these plasmons by varying the gate voltage. Using plasmon interferometry, we investigated losses in graphene by exploring real-space profiles of plasmon standing waves formed between the tip of our nano-probe and the edges of the samples. Plasmon dissipation quantified through this analysis is linked to the exotic electrodynamics of graphene. Standard plasmonic figures of merit of our tunable graphene devices surpass those of common metal-based structures.
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