Supplementary document for Nano-compositional imaging of the lanthanum silicide system at THz wavelengths - 6651359.pdf

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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

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

Terahertz Nanoimaging of Graphene

Accessing the nonradiative near-field electromagnetic interactions with high in-plane momentum (<i>q</i>) is the key to achieve super resolution imaging far beyond the diffraction limit. At far-infrared and terahertz (THz) wavelengths (e.g., 300 μm = 1 terahertz = 4 meV), the study of high <i>q</i> response and nanoscale near-field imaging is still a nascent research field. In this work, we report on THz nanoimaging of exfoliated single and multilayer graphene flakes by using a state-of-the-art scattering-type near-field optical microscope (s-SNOM). We experimentally demonstrated that the single layer graphene is close to a perfect near-field reflector at ambient environment, comparable to that of the noble metal films at the same frequency range. Further modeling and analysis considering the nonlocal graphene conductivity indicate that the high near-field reflectivity of graphene is a rather universal behavior: graphene operates as a perfect high-<i>q</i> reflector at room temperature. Our work uncovers the unique high-<i>q</i> THz response of graphene, which is essential for future applications of graphene in nano-optics or tip-enhanced technologies

Efficiency of Launching Highly Confined Polaritons by Infrared Light Incident on a Hyperbolic Material

We investigated phonon–polaritons in hexagonal boron nitridea naturally hyperbolic van der Waals materialby means of the scattering-type scanning near-field optical microscopy. Real-space nanoimages we have obtained detail how the polaritons are launched when the light incident on a thin hexagonal boron nitride slab is scattered by various intrinsic and extrinsic inhomogeneities, including sample edges, metallic nanodisks deposited on its top surface, random defects, and surface impurities. The scanned tip of the near-field microscope is itself a polariton launcher whose efficiency proves to be superior to all the other types of polariton launchers we studied. Our work may inform future development of polaritonic nanodevices as well as fundamental studies of collective modes in van der Waals materials

Ultrafast and Nanoscale Plasmonic Phenomena in Exfoliated Graphene Revealed by Infrared Pump–Probe Nanoscopy

Pump–probe spectroscopy is central for exploring ultrafast dynamics of fundamental excitations, collective modes, and energy transfer processes. Typically carried out using conventional diffraction-limited optics, pump–probe experiments inherently average over local chemical, compositional, and electronic inhomogeneities. Here, we circumvent this deficiency and introduce pump–probe infrared spectroscopy with ∼20 nm spatial resolution, far below the diffraction limit, which is accomplished using a scattering scanning near-field optical microscope (s-SNOM). This technique allows us to investigate exfoliated graphene single-layers on SiO₂ at technologically significant mid-infrared (MIR) frequencies where the local optical conductivity becomes experimentally accessible through the excitation of surface plasmons via the s-SNOM tip. Optical pumping at near-infrared (NIR) frequencies prompts distinct changes in the plasmonic behavior on 200 fs time scales. The origin of the pump-induced, enhanced plasmonic response is identified as an increase in the effective electron temperature up to several thousand Kelvin, as deduced directly from the Drude weight associated with the plasmonic resonances