Hamiltonian Optics of Hyperbolic Polaritons in Nanogranules

Semiclassical quantization rules and numerical calculations are applied to study polariton modes of materials whose permittivity tensor has principal values of opposite sign (so-called hyperbolic materials). The spectra of volume- and surface-confined polaritons are computed for spheroidal nanogranules of hexagonal boron nitride, a natural hyperbolic crystal. The field distribution created by polaritons excited by an external dipole source is predicted to exhibit raylike patterns due to classical periodic orbits. Near-field infrared imaging and Purcell-factor measurements are suggested to test these predictions

IR Near-Field Spectroscopy and Imaging of Single Li_<i>x</i>FePO₄ Microcrystals

This study demonstrates the unique capability of infrared near-field nanoscopy combined with Fourier transform infrared spectroscopy to map phase distributions in microcrystals of Li_<i>x</i>FePO₄, a positive electrode material for Li-ion batteries. Ex situ nanoscale IR imaging provides direct evidence for the coexistence of LiFePO₄ and FePO₄ phases in partially delithiated single-crystal microparticles. A quantitative three-dimensional tomographic reconstruction of the phase distribution within a single microcrystal provides new insights into the phase transformation and/or relaxation mechanism, revealing a FePO₄ shell surrounding a diamond-shaped LiFePO₄ inner core, gradually shrinking in size and vanishing upon delithiation of the crystal. The observed phase propagation pattern supports recent functional models of LiFePO₄ operation relating electrochemical performance to material design. This work demonstrates the remarkable potential of near-field optical techniques for the characterization of electrochemical materials and interfaces

Ultrafast Dynamics of Surface Plasmons in InAs by Time-Resolved Infrared Nanospectroscopy

We report on time-resolved mid-infrared (mid-IR) near-field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump–probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photomodulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions. The photoinduced change of the probe intensity due to plasmons in InAs is found to exceed that of other mid-IR or near-IR media by 1–2 orders of magnitude. Remarkably, the required control pulse fluence is as low as 60 μJ/cm², much smaller than fluences of ∼1–10 mJ/cm² previously utilized in ultrafast control of near-IR plasmonics. These low excitation densities are easily attained with a standard 1.56 μm fiber laser. Thus, InAsa common semiconductor with favorable plasmonic properties such as a low effective masshas the potential to become an important building block of optically controlled plasmonic devices operating at infrared frequencies

Imaging the Localized Plasmon Resonance Modes in Graphene Nanoribbons

We report a nanoinfrared (IR) imaging study of the localized plasmon resonance modes of graphene nanoribbons (GNRs) using a scattering-type scanning near-field optical microscope (s-SNOM). By comparing the imaging data of GNRs that are aligned parallel and perpendicular to the in-plane component of the excitation laser field, we observed symmetric and asymmetric plasmonic interference fringes, respectively. Theoretical analysis indicates that the asymmetric fringes are formed due to the interplay between the localized surface plasmon resonance (SPR) mode excited by the GNRs and the propagative surface plasmon polariton (SPP) mode launched by the s-SNOM tip. With rigorous simulations, we reproduce the observed fringe patterns and address quantitatively the role of the s-SNOM tip on both the SPR and SPP modes. Furthermore, we have seen real-space signatures of both the dipole and higher-order SPR modes by varying the ribbon width

Ultraconfined Plasmonic Hotspots Inside Graphene Nanobubbles

We report on a nanoinfrared (IR) imaging study of ultraconfined plasmonic hotspots inside graphene nanobubbles formed in graphene/hexagonal boron nitride (hBN) heterostructures. The volume of these plasmonic hotspots is more than one-million-times smaller than what could be achieved by free-space IR photons, and their real-space distributions are controlled by the sizes and shapes of the nanobubbles. Theoretical analysis indicates that the observed plasmonic hotspots are formed due to a significant increase of the local plasmon wavelength in the nanobubble regions. Such an increase is attributed to the high sensitivity of graphene plasmons to its dielectric environment. Our work presents a novel scheme for plasmonic hotspot formation and sheds light on future applications of graphene nanobubbles for plasmon-enhanced IR spectroscopy

Tuning and Persistent Switching of Graphene Plasmons on a Ferroelectric Substrate

We characterized plasmon propagation in graphene on thin films of the high-κ dielectric PbZr_0.3Ti_0.7O₃ (PZT). Significant modulation (up to ±75%) of the plasmon wavelength was achieved with application of ultrasmall voltages (< ±1 V) across PZT. Analysis of the observed plasmonic fringes at the graphene edge indicates that carriers in graphene on PZT behave as noninteracting Dirac Fermions approximated by a semiclassical Drude response, which may be attributed to strong dielectric screening at the graphene/PZT interface. Additionally, significant plasmon scattering occurs at the grain boundaries of PZT from topographic and/or polarization induced graphene conductivity variation in the interior of graphene, reducing the overall plasmon propagation length. Lastly, through application of 2 V across PZT, we demonstrate the capability to persistently modify the plasmonic response of graphene through transient voltage application

Graphene-Based Platform for Infrared Near-Field Nanospectroscopy of Water and Biological Materials in an Aqueous Environment

Scattering scanning near-field optical microscopy (s-SNOM) has emerged as a powerful nanoscale spectroscopic tool capable of characterizing individual biomacromolecules and molecular materials. However, applications of scattering-based near-field techniques in the infrared (IR) to native biosystems still await a solution of how to implement the required aqueous environment. In this work, we demonstrate an IR-compatible liquid cell architecture that enables near-field imaging and nanospectroscopy by taking advantage of the unique properties of graphene. Large-area graphene acts as an impermeable monolayer barrier that allows for nano-IR inspection of underlying molecular materials in liquid. Here, we use s-SNOM to investigate the tobacco mosaic virus (TMV) in water underneath graphene. We resolve individual virus particles and register the amide I and II bands of TMV at <i>ca</i>. 1520 and 1660 cm^–1, respectively, using nanoscale Fourier transform infrared spectroscopy (nano-FTIR). We verify the presence of water in the graphene liquid cell by identifying a spectral feature associated with water absorption at 1610 cm^–1

Faraday Rotation Due to Surface States in the Topological Insulator (Bi_1–<i>x</i>Sb_<i>x</i>)₂Te₃

Using magneto-infrared spectroscopy, we have explored the charge dynamics of (Bi,Sb)₂Te₃ thin films on InP substrates. From the magneto-transmission data we extracted three distinct cyclotron resonance (CR) energies that are all apparent in the broad band Faraday rotation (FR) spectra. This comprehensive FR-CR data set has allowed us to isolate the response of the bulk states from the intrinsic surface states associated with both the top and bottom surfaces of the film. The FR data uncovered that electron- and hole-type Dirac Fermions reside on opposite surfaces of our films, which paves the way for observing many exotic quantum phenomena in topological insulators

Active Optical Metasurfaces Based on Defect-Engineered Phase-Transition Materials

Active, widely tunable optical materials have enabled rapid advances in photonics and optoelectronics, especially in the emerging field of meta-devices. Here, we demonstrate that spatially selective defect engineering on the nanometer scale can transform phase-transition materials into optical metasurfaces. Using ion irradiation through nanometer-scale masks, we selectively defect-engineered the insulator-metal transition of vanadium dioxide, a prototypical correlated phase-transition material whose optical properties change dramatically depending on its state. Using this robust technique, we demonstrated several optical metasurfaces, including tunable absorbers with artificially induced phase coexistence and tunable polarizers based on thermally triggered dichroism. Spatially selective nanoscale defect engineering represents a new paradigm for active photonic structures and devices

Active Optical Metasurfaces Based on Defect-Engineered Phase-Transition Materials

Active, widely tunable optical materials have enabled rapid advances in photonics and optoelectronics, especially in the emerging field of meta-devices. Here, we demonstrate that spatially selective defect engineering on the nanometer scale can transform phase-transition materials into optical metasurfaces. Using ion irradiation through nanometer-scale masks, we selectively defect-engineered the insulator-metal transition of vanadium dioxide, a prototypical correlated phase-transition material whose optical properties change dramatically depending on its state. Using this robust technique, we demonstrated several optical metasurfaces, including tunable absorbers with artificially induced phase coexistence and tunable polarizers based on thermally triggered dichroism. Spatially selective nanoscale defect engineering represents a new paradigm for active photonic structures and devices