Real-space observation of ultraconfined in-plane anisotropic acoustic terahertz plasmon polaritons.

Thin layers of in-plane anisotropic materials can support ultraconfined polaritons, whose wavelengths depend on the propagation direction. Such polaritons hold potential for the exploration of fundamental material properties and the development of novel nanophotonic devices. However, the real-space observation of ultraconfined in-plane anisotropic plasmon polaritons (PPs)-which exist in much broader spectral ranges than phonon polaritons-has been elusive. Here we apply terahertz nanoscopy to image in-plane anisotropic low-energy PPs in monoclinic Ag2Te platelets. The hybridization of the PPs with their mirror image-by placing the platelets above a Au layer-increases the direction-dependent relative polariton propagation length and the directional polariton confinement. This allows for verifying a linear dispersion and elliptical isofrequency contour in momentum space, revealing in-plane anisotropic acoustic terahertz PPs. Our work shows high-symmetry (elliptical) polaritons on low-symmetry (monoclinic) crystals and demonstrates the use of terahertz PPs for local measurements of anisotropic charge carrier masses and damping.

Hyperspectral Nanoimaging of van der Waals Polaritonic Crystals.

Phonon polaritons (PhPs) in van der Waals (vdW) crystal slabs enable nanoscale infrared light manipulation. Specifically, periodically structured vdW slabs behave as polaritonic crystals (vdW-PCs), where the polaritons form Bloch modes. Because the polariton wavelengths are smaller than that of light, conventional far-field spectroscopy does not allow for a complete characterization of vdW-PCs or for revealing their band structure. Here, we perform hyperspectral infrared nanoimaging and analysis of PhPs in a vdW-PC slab made of h-BN. We demonstrate that infrared spectra recorded at individual spatial positions within the unit cell of the vdW-PC can be associated with its band structure and local density of photonic states (LDOS). We thus introduce hyperspectral infrared nanoimaging as a tool for the comprehensive analysis of polaritonic crystals, which could find applications in the reconstruction of complex polaritonic dispersion surfaces in momentum-frequency space or for exploring exotic electromagnetic modes in topological photonic structures.

Planar refraction and lensing of highly confined polaritons in anisotropic media.

Refraction between isotropic media is characterized by light bending towards the normal to the boundary when passing from a low- to a high-refractive-index medium. However, refraction between anisotropic media is a more exotic phenomenon which remains barely investigated, particularly at the nanoscale. Here, we visualize and comprehensively study the general case of refraction of electromagnetic waves between two strongly anisotropic (hyperbolic) media, and we do it with the use of nanoscale-confined polaritons in a natural medium: α-MoO3. The refracted polaritons exhibit non-intuitive directions of propagation as they traverse planar nanoprisms, enabling to unveil an exotic optical effect: bending-free refraction. Furthermore, we develop an in-plane refractive hyperlens, yielding foci as small as λp/6, being λp the polariton wavelength (λ0/50 compared to the wavelength of free-space light). Our results set the grounds for planar nano-optics in strongly anisotropic media, with potential for effective control of the flow of energy at the nanoscale.

Substrate Matters: Surface-Polariton Enhanced Infrared Nanospectroscopy of Molecular Vibrations.

Infrared nanospectroscopy based on Fourier transform infrared near-field spectroscopy (nano-FTIR) is an emerging nanoanalytical tool with large application potential for label-free mapping and identification of organic and inorganic materials with nanoscale spatial resolution. However, the detection of thin molecular layers and nanostructures on standard substrates is still challenged by weak signals. Here, we demonstrate a significant enhancement of nano-FTIR signals of a thin organic layer by exploiting polariton-resonant tip-substrate coupling and surface polariton illumination of the probing tip. When the molecular vibration matches the tip-substrate resonance, we achieve up to nearly one order of magnitude signal enhancement on a phonon-polaritonic quartz (c-SiO2) substrate, as compared to nano-FTIR spectra obtained on metal (Au) substrates, and up to two orders of magnitude when compared to the standard infrared spectroscopy substrate CaF2. Our results will be of critical importance for boosting nano-FTIR spectroscopy toward the routine detection of monolayers and single molecules.

Launching of hyperbolic phonon-polaritons in h-BN slabs by resonant metal plasmonic antennas.

Launching and manipulation of polaritons in van der Waals materials offers novel opportunities for field-enhanced molecular spectroscopy and photodetection, among other applications. Particularly, the highly confined hyperbolic phonon polaritons (HPhPs) in h-BN slabs attract growing interest for their capability of guiding light at the nanoscale. An efficient coupling between free space photons and HPhPs is, however, hampered by their large momentum mismatch. Here, we show -by far-field infrared spectroscopy, infrared nanoimaging and numerical simulations- that resonant metallic antennas can efficiently launch HPhPs in thin h-BN slabs. Despite the strong hybridization of HPhPs in the h-BN slab and Fabry-Pérot plasmonic resonances in the metal antenna, the efficiency of launching propagating HPhPs in h-BN by resonant antennas exceeds significantly that of the non-resonant ones. Our results provide fundamental insights into the launching of HPhPs in thin polar slabs by resonant plasmonic antennas, which will be crucial for phonon-polariton based nanophotonic devices.

Deeply subwavelength phonon-polaritonic crystal made of a van der Waals material.

Photonic crystals (PCs) are periodically patterned dielectrics providing opportunities to shape and slow down the light for processing of optical signals, lasing and spontaneous emission control. Unit cells of conventional PCs are comparable to the wavelength of light and are not suitable for subwavelength scale applications. We engineer a nanoscale hole array in a van der Waals material (h-BN) supporting ultra-confined phonon polaritons (PhPs)-atomic lattice vibrations coupled to electromagnetic fields. Such a hole array represents a polaritonic crystal for mid-infrared frequencies having a unit cell volume of [Formula: see text] (with λ0 being the free-space wavelength), where PhPs form ultra-confined Bloch modes with a remarkably flat dispersion band. The latter leads to both angle- and polarization-independent sharp Bragg resonances, as verified by far-field spectroscopy and near-field optical microscopy. Our findings could lead to novel miniaturized angle- and polarization-independent infrared narrow-band couplers, absorbers and thermal emitters based on van der Waals materials and other thin polar materials.

Nanoimaging of resonating hyperbolic polaritons in linear boron nitride antennas.

Polaritons in layered materials-including van der Waals materials-exhibit hyperbolic dispersion and strong field confinement, which makes them highly attractive for applications including optical nanofocusing, sensing and control of spontaneous emission. Here we report a near-field study of polaritonic Fabry-Perot resonances in linear antennas made of a hyperbolic material. Specifically, we study hyperbolic phonon-polaritons in rectangular waveguide antennas made of hexagonal boron nitride (h-BN, a prototypical van der Waals crystal). Infrared nanospectroscopy and nanoimaging experiments reveal sharp resonances with large quality factors around 100, exhibiting atypical modal near-field patterns that have no analogue in conventional linear antennas. By performing a detailed mode analysis, we can assign the antenna resonances to a single waveguide mode originating from the hybridization of hyperbolic surface phonon-polaritons (Dyakonov polaritons) that propagate along the edges of the h-BN waveguide. Our work establishes the basis for the understanding and design of linear waveguides, resonators, sensors and metasurface elements based on hyperbolic materials and metamaterials.

Optical Nanoimaging of Hyperbolic Surface Polaritons at the Edges of van der Waals Materials.

Hyperbolic polaritons in van der Waals (vdW) materials recently attract a lot of attention, owing to their strong electromagnetic field confinement, ultraslow group velocities, and long lifetimes. Typically, volume-confined hyperbolic polaritons (HPs) are studied. Here we show the first near-field optical images of hyperbolic surface polaritons (HSPs), which are confined and guided at the edges of thin flakes of a vdW material. To that end, we applied scattering-type scanning near-field optical microscopy (s-SNOM) for launching and real-space nanoimaging of hyperbolic surface phonon polariton modes on a hexagonal boron nitride (h-BN) flake. Our imaging data reveal that the fundamental HSP mode exhibits a stronger field confinement (shorter wavelength), smaller group velocities, and nearly identical lifetimes, as compared to the fundamental HP mode of the same h-BN flake. Our experimental data, corroborated by theory, establish a solid basis for future studies and applications of HPs and HSPs in vdW materials.

Experimental demonstration of the microscopic origin of circular dichroism in two-dimensional metamaterials.

Optical activity and circular dichroism are fascinating physical phenomena originating from the interaction of light with chiral molecules or other nano objects lacking mirror symmetries in three-dimensional (3D) space. While chiral optical properties are weak in most of naturally occurring materials, they can be engineered and significantly enhanced in synthetic optical media known as chiral metamaterials, where the spatial symmetry of their building blocks is broken on a nanoscale. Although originally discovered in 3D structures, circular dichroism can also emerge in a two-dimensional (2D) metasurface. The origin of the resulting circular dichroism is rather subtle, and is related to non-radiative (Ohmic) dissipation of the constituent metamolecules. Because such dissipation occurs on a nanoscale, this effect has never been experimentally probed and visualized. Using a suite of recently developed nanoscale-measurement tools, we establish that the circular dichroism in a nanostructured metasurface occurs due to handedness-dependent Ohmic heating.

Real-Space Mapping of the Chiral Near-Field Distributions in Spiral Antennas and Planar Metasurfaces.

Chiral antennas and metasurfaces can be designed to react differently to left- and right-handed circularly polarized light, which enables novel optical properties such as giant optical activity and negative refraction. Here, we demonstrate that the underlying chiral near-field distributions can be directly mapped with scattering-type scanning near-field optical microscopy employing circularly polarized illumination. We apply our technique to visualize, for the first time, the circular-polarization selective nanofocusing of infrared light in Archimedean spiral antennas, and explain this chiral optical effect by directional launching of traveling waves in analogy to antenna theory. Moreover, we near-field image single-layer rosette and asymmetric dipole-monopole metasurfaces and find negligible and strong chiral optical near-field contrast, respectively. Our technique paves the way for near-field characterization of optical chirality in metal nanostructures, which will be essential for the future development of chiral antennas and metasurfaces and their applications.

Quantitative confocal phase imaging by synthetic optical holography.

We demonstrate quantitative phase mapping in confocal optical microscopy by applying synthetic optical holography (SOH), a recently introduced method for technically simple and fast phase imaging in scanning optical microscopy. SOH is implemented in a confocal microscope by simply adding a linearly moving reference mirror to the microscope setup, which generates a synthetic reference wave analogous to the plane reference wave of wide-field off-axis holography. We demonstrate that SOH confocal microscopy allows for non-contact surface profiling with sub-nanometer depth resolution. As an application for biological imaging, we apply SOH confocal microscopy to map the surface profile of an onion cell, revealing nanoscale-height features on the cell surface.

Controlling graphene plasmons with resonant metal antennas and spatial conductivity patterns.

Graphene plasmons promise unique possibilities for controlling light in nanoscale devices and for merging optics with electronics. We developed a versatile platform technology based on resonant optical antennas and conductivity patterns for launching and control of propagating graphene plasmons, an essential step for the development of graphene plasmonic circuits. We launched and focused infrared graphene plasmons with geometrically tailored antennas and observed how they refracted when passing through a two-dimensional conductivity pattern, here a prism-shaped bilayer. To that end, we directly mapped the graphene plasmon wavefronts by means of an imaging method that will be useful in testing future design concepts for nanoscale graphene plasmonic circuits and devices.

Efficient coupling of light to graphene plasmons by compressing surface polaritons with tapered bulk materials.

Graphene plasmons promise exciting nanophotonic and optoelectronic applications. Owing to their extremely short wavelengths, however, the efficient coupling of photons to propagating graphene plasmons-critical for the development of future devices-can be challenging. Here, we propose and numerically demonstrate coupling between infrared photons and graphene plasmons by the compression of surface polaritons on tapered bulk slabs of both polar and doped semiconductor materials. Propagation of surface phonon polaritons (in SiC) and surface plasmon polaritons (in n-GaAs) along the tapered slabs compresses the polariton wavelengths from several micrometers to around 200 nm, which perfectly matches the wavelengths of graphene plasmons. The proposed coupling device allows for a 25% conversion of the incident energy into graphene plasmons and, therefore, could become an efficient route toward graphene plasmon circuitry.

Synthetic optical holography for rapid nanoimaging.

Holography has paved the way for phase imaging in a variety of wide-field techniques, including electron, X-ray and optical microscopy. In scanning optical microscopy, however, the serial fashion of image acquisition seems to challenge a direct implementation of traditional holography. Here we introduce synthetic optical holography (SOH) for quantitative phase-resolved imaging in scanning optical microscopy. It uniquely combines fast phase imaging, technical simplicity and simultaneous operation at visible and infrared frequencies with a single reference arm. We demonstrate SOH with a scattering-type scanning near-field optical microscope (s-SNOM) where it enables reliable quantitative phase-resolved near-field imaging with unprecedented speed. We apply these capabilities to nanoscale, non-invasive and rapid screening of grain boundaries in CVD-grown graphene, by recording 65 kilopixel near-field images in 26 s and 2.3 megapixel images in 13 min. Beyond s-SNOM, the SOH concept could boost the implementation of holography in other scanning imaging applications such as confocal microscopy.

Electronic and plasmonic phenomena at graphene grain boundaries.

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.

Experimental verification of the spectral shift between near- and far-field peak intensities of plasmonic infrared nanoantennas.

Theory predicts a distinct spectral shift between the near- and far-field optical response of plasmonic antennas. Here we combine near-field optical microscopy and far-field spectroscopy of individual infrared-resonant nanoantennas to verify experimentally this spectral shift. Numerical calculations corroborate our experimental results. We furthermore discuss the implications of this effect in surface-enhanced infrared spectroscopy.

Correlative infrared-electron nanoscopy reveals the local structure-conductivity relationship in zinc oxide nanowires.

High-resolution characterization methods play a key role in the development, analysis and optimization of nanoscale materials and devices. Because of the various material properties, only a combination of different characterization techniques provides a comprehensive understanding of complex functional materials. Here we introduce correlative infrared-electron nanoscopy, a novel method yielding transmission electron microscope and infrared near-field images of one and the same nanostructure. While transmission electron microscopy provides structural information up to the atomic level, infrared near-field imaging yields nanoscale maps of chemical composition and conductivity. We demonstrate the method's potential by studying the relation between conductivity and crystal structure in ZnO nanowire cross-sections. The combination of infrared conductivity maps and the local crystal structure reveals a radial free-carrier gradient, which inversely correlates to the density of extended crystalline defects. Our method opens new avenues for studying the local interplay between structure, conductivity and chemical composition in widely different material systems.

Resolving the electromagnetic mechanism of surface-enhanced light scattering at single hot spots.

Light scattering at nanoparticles and molecules can be dramatically enhanced in the 'hot spots' of optical antennas, where the incident light is highly concentrated. Although this effect is widely applied in surface-enhanced optical sensing, spectroscopy and microscopy, the underlying electromagnetic mechanism of the signal enhancement is challenging to trace experimentally. Here we study elastically scattered light from an individual object located in the well-defined hot spot of single antennas, as a new approach to resolve the role of the antenna in the scattering process. We provide experimental evidence that the intensity elastically scattered off the object scales with the fourth power of the local field enhancement provided by the antenna, and that the underlying electromagnetic mechanism is identical to the one commonly accepted in surface-enhanced Raman scattering. We also measure the phase shift of the scattered light, which provides a novel and unambiguous fingerprint of surface-enhanced light scattering.

Infrared-spectroscopic nanoimaging with a thermal source.

Fourier-transform infrared (FTIR) spectroscopy is a widely used analytical tool for chemical identification of inorganic, organic and biomedical materials, as well as for exploring conduction phenomena. Because of the diffraction limit, however, conventional FTIR cannot be applied for nanoscale imaging. Here we demonstrate a novel FTIR system that allows for infrared-spectroscopic nanoimaging of dielectric properties (nano-FTIR). Based on superfocusing of thermal radiation with an infrared antenna, detection of the scattered light, and strong signal enhancement employing an asymmetric FTIR spectrometer, we improve the spatial resolution of conventional infrared spectroscopy by more than two orders of magnitude. By mapping a semiconductor device, we demonstrate spectroscopic identification of silicon oxides and quantification of the free-carrier concentration in doped Si regions with a spatial resolution better than 100 nm. We envisage nano-FTIR becoming a powerful tool for chemical identification of nanomaterials, as well as for quantitative and contact-free measurement of the local free-carrier concentration and mobility in doped nanostructures.

Phase-resolved mapping of the near-field vector and polarization state in nanoscale antenna gaps.

We demonstrate that the local near-field vector and polarization state on planar antenna structures and in nanoscale antenna gaps can be determined by scattering-type near-field optical microscopy (s-SNOM). The near-field vector is reconstructed from the amplitude and phase images of the in- and out-of-plane near-field components obtained by polarization-resolved interferometric detection. Experiments with a mid-infrared inverse bowtie antenna yield a vectorial near-field distribution with unprecedented resolution of about 10 nm and in excellent agreement with numerical simulations. Furthermore, we provide first direct experimental evidence that the nanoscale confined and strongly enhanced fields at the antenna gap are linearly polarized. s-SNOM vector-field mapping paves the way to a full near-field characterization of nanophotonic structures in the broad spectral range between visible and terahertz frequencies, which is essential for future development and quality control of metamaterials, optical sensors, and waveguides.