Charge Transfer Plasmonics in Bespoke Graphene/α-RuCl Cavities.

Surface plasmon polaritons (SPPs) provide a window into the nano-optical, electrodynamic response of their host material and its dielectric environment. Graphene/α-RuCl serves as an ideal model system for imaging SPPs since the large work function difference between these two layers facilitates charge transfer that hole dopes graphene with ∼ 10 cm free carriers. In this work, we study the emergent THz response of graphene/α-RuCl heterostructures using our home-built cryogenic scanning near-field optical microscope.

Tunable Phonon Polariton Hybridization in a Van der Waals Hetero-Bicrystal.

Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero-bicrystals composed of molybdenum oxide (MoO) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, the polariton eigenmodes in MoO-hBN hetero-bicrystals self-assembled on ultrasmooth gold are systematically studied using synchrotron infrared nanospectroscopy.

Ultrabroadband Terahertz Near-Field Nanospectroscopy with a HgCdTe Detector.

While near-field infrared nanospectroscopy provides a powerful tool for nanoscale material characterization, broadband nanospectroscopy of elementary material excitations in the single-digit terahertz (THz) range remains relatively unexplored. Here, we study liquid-Helium-cooled photoconductive HgCdTe (MCT) for use as a fast detector in near-field nanospectroscopy. Compared to the common = 77 K operation, liquid-Helium cooling reduces the MCT detection threshold to ∼22 meV, improves the noise performance, and yields a response bandwidth exceeding 10 MHz.

Infrared nano-imaging of Dirac magnetoexcitons in graphene.

Magnetic fields can have profound effects on the motion of electrons in quantum materials. Two-dimensional electron systems subject to strong magnetic fields are expected to exhibit quantized Hall conductivity, chiral edge currents and distinctive collective modes referred to as magnetoplasmons and magnetoexcitons. Generating these propagating collective modes in charge-neutral samples and imaging them at their native nanometre length scales have thus far been experimentally elusive.

Probing subwavelength in-plane anisotropy with antenna-assisted infrared nano-spectroscopy.

Infrared nano-spectroscopy based on scattering-type scanning near-field optical microscopy (s-SNOM) is commonly employed to probe the vibrational fingerprints of materials at the nanometer length scale. However, due to the elongated and axisymmetric tip shank, s-SNOM is less sensitive to the in-plane sample anisotropy in general. In this article, we report an easy-to-implement method to probe the in-plane dielectric responses of materials with the assistance of a metallic disk micro-antenna.

Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric CaTiO.

Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low power memory and logic devices as well as novel computing architectures. In this work, we employ synchrotron-based near-field infrared nano-spectroscopy to reveal the vibrational properties of ferroelastic (90[Formula: see text] ferroelectric) domain walls in the hybrid improper ferroelectric Ca[Formula: see text]Ti[Formula: see text]O[Formula: see text].

Bulk signatures of pressure-induced band inversion and topological phase transitions in Pb(1-x)Sn(x)Se.

The characteristics of topological insulators are manifested in both their surface and bulk properties, but the latter remain to be explored. Here we report bulk signatures of pressure-induced band inversion and topological phase transitions in Pb(1-x)Sn(x)Se (x=0.00, 0.

Signatures of a pressure-induced topological quantum phase transition in BiTeI.

We report the observation of two signatures of a pressure-induced topological quantum phase transition in the polar semiconductor BiTeI using x-ray powder diffraction and infrared spectroscopy. The x-ray data confirm that BiTeI remains in its ambient-pressure structure up to 8 GPa. The lattice parameter ratio c/a shows a minimum between 2.

Synchrotron radiation-based far-infrared spectroscopic ellipsometer with full Mueller-matrix capability.

We developed far-IR spectroscopic ellipsometer at the U4IR beamline of the National Synchrotron Light Source in Brookhaven National Laboratory. This ellipsometer is able to measure both, rotating analyzer and full-Mueller matrix spectra using rotating retarders, and wire-grid linear polarizers. We utilize exceptional brightness of synchrotron radiation in the broad spectral range between about 20 and 4000 cm(-1).

Dynamic full-field infrared imaging with multiple synchrotron beams.

Microspectroscopic imaging in the infrared (IR) spectral region allows for the examination of spatially resolved chemical composition on the microscale. More than a decade ago, it was demonstrated that diffraction-limited spatial resolution can be achieved when an apertured, single-pixel IR microscope is coupled to the high brightness of a synchrotron light source. Nowadays, many IR microscopes are equipped with multipixel Focal Plane Array (FPA) detectors, which dramatically improve data acquisition times for imaging large areas.

Structure-dependent Fano resonances in the infrared spectra of phonons in few-layer graphene.

The in-plane optical phonons around 200 meV in few-layer graphene are investigated utilizing infrared absorption spectroscopy. The phonon spectra exhibit unusual asymmetric features characteristic of Fano resonances, which depend critically on the layer thickness and stacking order of the sample. The phonon intensities in samples with rhombohedral (ABC) stacking are significantly higher than those with Bernal (AB) stacking.

Imaging the material properties of bone specimens using reflection-based infrared microspectroscopy.

Fourier transform infrared microspectroscopy (FTIRM) is a widely used method for mapping the material properties of bone and other mineralized tissues, including mineralization, crystallinity, carbonate substitution, and collagen cross-linking. This technique is traditionally performed in a transmission-based geometry, which requires the preparation of plastic-embedded thin sections, limiting its functionality. Here, we theoretically and empirically demonstrate the development of reflection-based FTIRM as an alternative to the widely adopted transmission-based FTIRM, which reduces specimen preparation time and broadens the range of specimens that can be imaged.

Tunable few-cycle and multicycle coherent terahertz radiation from relativistic electrons.

We report the generation of tunable, narrow-band, few-cycle and multicycle coherent terahertz (THz) pulses from a temporally modulated relativistic electron beam. We demonstrate that the frequency of the THz radiation and the number of the oscillation cycles of the THz electric field can be tuned by changing the modulation period of the electron beam through a temporally shaped photocathode drive laser. The central frequency of the THz spectrum is tunable from ∼0.

Pressure-induced local structure distortions in Cu(pyz)F2(H2O)2.

We employed infrared spectroscopy along with complementary lattice dynamics and spin density calculations to investigate pressure-driven local structure distortions in the copper coordination polymer Cu(pyz)F(2)(H(2)O)(2). Here, pyz is pyrazine. Our study reveals rich and fully reversible local lattice distortions that buckle the pyrazine ring, disrupt the bc-plane O-H···F hydrogen-bonding network, and reinforce magnetic property switching.

Far-infrared conductivity measurements of pair breaking in superconducting Nb 0.5 Ti 0.5 N thin films induced by an external magnetic field.

We report the complex optical conductivity of a superconducting thin film of Nb 0.5 Ti 0.5 N in an external magnetic field.

Organic reagent interaction with hair spatially characterized by infrared microspectroscopy using synchrotron radiation.

The penetration of chemical reagents through human hair after bleaching has been spatially characterized using infrared microspectroscopy (IMS) with a synchrotron source. Chemical imaging of hair cross sections before and after bleaching was achieved with high contrast, using the peptide and lipid mid-infrared vibrational bands which are characteristic of hair. The ability to make images using functional groups as a contrast mechanism can be applied to studies of other chemical groups, if present, in the structure of the hair.

Profiling lipids across Caucasian and Afro-American hair transverse cuts, using synchrotron infrared microspectrometry.

Synchrotron-based infrared microscopic measurements have been performed on various hair transverse sections, sampled either from the heads of Caucasian or Afro-American subjects. Lipid content of various virgin hair transverse sections was established, with an unprecedented resolution. The variations in shape and intensity of the CH(2), CH(3), amide I and amide II bands, before and after lipid removal by solvent extraction, were profiled, showing clearly that Caucasian hair often contains lipids localized inside the medulla and to a lesser extent inside the cuticle.

Silicon beam splitter for far-infrared and terahertz spectroscopy.

Silicon beam splitters several millimeters thick offer numerous advantages over thin freestanding dielectric beam splitters. For routine spectroscopy for which resolutions of better than 1 cm(-1) are not required, a silicon beam splitter can replace several Mylar beam splitters to span the entire far-infrared region. In addition to superior long-wavelength performance that extends well into the terahertz region, the silicon beam splitter has the additional advantage that its efficiency displays little polarization dependence.

Nonlinear cross-phase modulation with intense single-cycle terahertz pulses.

We have demonstrated nonlinear cross-phase modulation in electro-optic crystals using intense, single-cycle terahertz (THz) radiation. Individual THz pulses, generated by coherent transition radiation emitted by subpicosecond electron bunches, have peak energies of up to 100 microJ per pulse. The time-dependent electric field of the intense THz pulses induces cross-phase modulation in electro-optic crystals through the Pockels effect, leading to spectral shifting, broadening, and modulation of copropagating laser pulses.

Very High Power THz Radiation Sources.

We report the production of high power (20watts average, ∼ 1 Megawatt peak) broadbandTHz light based on coherent emission fromrelativistic electrons. Such sources areideal for imaging, for high power damagestudies and for studies of non-linearphenomena in this spectral range. Wedescribe the source, presenting theoreticalcalculations and their experimentalverification.

Synchrotron-based Biological Microspectroscopy: From the Mid-Infrared through the Far-Infrared Regimes.

Infrared radiation from synchrotron storagerings serves as a high-brightness source fordiffraction-limited microspectroscopy inboth the mid- and far-infrared spectralranges. Mid-infrared absorption, due to localvibrational modes within complex molecules,is shown to be sensitive to small chemicalchanges associated with certain diseases.Farinfrared modes are believed to result from thefolding or twisting of larger, morecomplex molecules.

Very high power THz radiation at Jefferson Lab.

We report the production of high power (20 W average, approximately 1 MW peak) broadband THz light based on coherent emission from relativistic electrons. We describe the source, presenting theoretical calculations and their experimental verification. For clarity we compare this source with that based on ultrafast laser techniques, and in fact the radiation has qualities closely analogous to those produced by such sources, namely that it is spatially coherent, and comprises short duration pulses with transform-limited spectral content.