Demonstration of a Plasmonic Nonlinear Pseudodiode.

We demonstrate a nonlinear plasmonic metasurface that exhibits strongly asymmetric second-harmonic generation: nonlinear scattering is efficient upon excitation in one direction, and it is substantially suppressed when the excitation direction is reversed, thus enabling a diode-like functionality. A significant (approximately 10 dB) extinction ratio of SHG upon opposite excitations is measured experimentally, and those findings are substantiated with full-wave simulations. This effect is achieved by employing a combination of two commonly used metals─aluminum and silver─producing a material composition asymmetry that results in a bianisotropic response of the system, as confirmed by performing homogenization analysis and extracting an effective susceptibility tensor. Finally, we discuss the implications of our results from the more fundamental perspectives of reciprocity and time-reversal asymmetry.

Ultimate Limit for Optical Losses in Gold, Revealed by Quantitative Near-Field Microscopy.

We report thorough measurements of surface plasmon polaritons (SPPs) running along nearly perfect air-gold interfaces formed by atomically flat surfaces of chemically synthesized gold monocrystals. By means of amplitude- and phase-resolved near-field microscopy, we obtain their propagation length and effective mode index at visible wavelengths (532, 594, 632.8, 729, and 800 nm). The measured values are compared with the values obtained from the dielectric functions of gold that are reported in literature. Importantly, a reported dielectric function of monocrystalline gold implies ∼1.5 times shorter propagation lengths than those observed in our experiments, whereas a dielectric function reported for properly fabricated polycrystalline gold leads to SPP propagation lengths matching our results. We argue that the SPP propagation lengths measured in our experiments signify the ultimate limit of optical losses in gold, encouraging further comprehensive characterization of optical material properties of pure gold as well as other plasmonic materials.

Near-field probing of image phonon-polaritons in hexagonal boron nitride on gold crystals.

Near-field mapping has been widely used to study hyperbolic phonon-polaritons in van der Waals crystals. However, an accurate measurement of the polaritonic loss remains challenging because of the inherent complexity of the near-field signal and the substrate-mediated loss. Here we demonstrate that large-area monocrystalline gold flakes, an atomically flat low-loss substrate for image polaritons, provide a platform for precise near-field measurement of the complex propagation constant of polaritons in van der Waals crystals. As a topical example, we measure propagation loss of the image phonon-polaritons in hexagonal boron nitride, revealing that their normalized propagation length exhibits a parabolic spectral dependency. Furthermore, we show that image phonon-polaritons exhibit up to a twice longer normalized propagation length, while being 2.4 times more compressed compared to the case of the dielectric substrate. We conclude that the monocrystalline gold flakes provide a unique nanophotonic platform for probing and exploitation of the image modes in low-dimensional materials.

Extremely confined gap plasmon modes: when nonlocality matters.

Historically, the field of plasmonics has been relying on the framework of classical electrodynamics, with the local-response approximation of material response being applied even when dealing with nanoscale metallic structures. However, when the confinement of electromagnetic radiation approaches atomic scales, mesoscopic effects are anticipated to become observable, e.g., those associated with the nonlocal electrodynamic surface response of the electron gas. Here, we investigate nonlocal effects in propagating gap surface plasmon modes in ultrathin metal-dielectric-metal planar waveguides, exploiting monocrystalline gold flakes separated by atomic-layer-deposited aluminum oxide. We use scanning near-field optical microscopy to directly access the near-field of such confined gap plasmon modes and measure their dispersion relation via their complex-valued propagation constants. We compare our experimental findings with the predictions of the generalized nonlocal optical response theory to unveil signatures of nonlocal damping, which becomes appreciable for few-nanometer-sized dielectric gaps.

Anisotropic second-harmonic generation from monocrystalline gold flakes.

Noble metals with well-defined crystallographic orientation constitute an appealing class of materials for controlling light-matter interactions on the nanoscale. Nonlinear optical processes, being particularly sensitive to anisotropy, are a natural and versatile probe of crystallinity in nano-optical devices. Here we study the nonlinear optical response of monocrystalline gold flakes, revealing a polarization dependence in second-harmonic generation from the {111} surface that is markedly absent in polycrystalline films. Our findings confirm that second-harmonic microscopy is a robust and non-destructive method for probing the crystallographic orientation of gold, and can serve as a guideline for enhancing nonlinear response in plasmonic systems.

Laser Writing of Bright Colors on Near-Percolation Plasmonic Reflector Arrays.

Coloration by surface nanostructuring has attracted a great deal of attention by the virtue of making use of environment-friendly recyclable materials and generating nonbleaching colors. Recently, it was found possible to delegate the task of color printing to laser postprocessing that modifies carefully designed and fabricated nanostructures. Here we take the next crucial step in the development of structural color printing by dispensing with preformed nanostructures and using instead near-percolation metal films atop dielectric-metal sandwiches, that is, near-percolation plasmonic reflector arrays. Scanning rapidly (∼20 µm/s) across 4 nm-thin island-like gold films supported by 30 nm-thin silica layers atop 100 nm-thick gold layers with a strongly focused Ti-sapphire laser beam, while adjusting the average laser power from 1 to 10 mW, we produce bright colors varying from green to red by laser-heating-induced merging and reshaping of gold islands. Selection of strongly heated islands and their reshaping, both originating from excitation of plasmonic resonances, are strongly influenced by the polarization direction of laser illumination, so that the colors produced are well pronounced only when viewed with the same polarization. Conversely, the laser color writing with circular polarizations results in bright polarization-independent color images. The fabrication procedure for near-percolation reflector arrays is exceedingly simple and scalable to mass production, while the laser-induced modification occurs inherently with the subwavelength resolution. This combination of features makes the approach developed for laser color writing readily amenable for practical implementation and use in diverse applications ranging from nanoscale patterning for security marking to large-scale color printing for decoration.