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. Here we visualize propagating magnetoexciton polaritons at their native length scales and report their magnetic-field-tunable dispersion in near-charge-neutral graphene. Imaging these collective modes and their associated nano-electro-optical responses allows us to identify polariton-modulated optical and photo-thermal electric effects at the sample edges, which are the most pronounced near charge neutrality. Our work is enabled by innovations in cryogenic near-field optical microscopy techniques that allow for the nano-imaging of the near-field responses of two-dimensional materials under magnetic fields up to 7 T. This nano-magneto-optics approach allows us to explore and manipulate magnetopolaritons in specimens with low carrier doping via harnessing high magnetic fields.

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. As a proof-of-concept demonstration, we investigate here the in-plane phonon responses of two prototypical samples, i.e. in (100) sapphire and x-cut lithium niobate (LiNbO3). In particular, the sapphire in-plane vibrations between 350 cm-1 to 800 cm-1 that correspond to LO phonon modes along the crystal b- and c-axis are determined with a spatial resolution of < λ/10, without needing any fitting parameters. In LiNbO3, we identify the in-plane orientation of its optical axis via the phonon modes, demonstrating that our method can be applied without prior knowledge of the crystal orientation. Our method can be elegantly adapted to retrieve the in-plane anisotropic response of a broad range of materials, i.e. subwavelength microcrystals, van-der-Waals materials, or topological insulators.

Infrared nano-spectroscopy of ferroelastic domain walls in hybrid improper ferroelectric Ca3Ti2O7.

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]. By locally mapping the Ti-O stretching and Ti-O-Ti bending modes, we reveal how structural order parameters rotate across a wall. Thus, we link observed near-field amplitude changes to underlying structural modulations and test ferroelectric switching models against real space measurements of local structure. This initiative opens the door to broadband infrared nano-imaging of heterogeneity in ferroics.

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, 0.15, and 0.23). The results of infrared measurements as a function of pressure indicate the closing and the reopening of the band gap as well as a maximum in the free carrier spectral weight. The enhanced density of states near the band gap in the topological phase gives rise to a steep interband absorption edge. The change of density of states also yields a maximum in the pressure dependence of the Fermi level. Thus, our conclusive results provide a consistent picture of pressure-induced topological phase transitions and highlight the bulk origin of the novel properties in topological insulators.

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 2.0-2.9 GPa, indicating an enhanced c-axis bonding through p(z) band crossing as expected during the transition. Over the same pressure range, the infrared spectra reveal a maximum in the optical spectral weight of the charge carriers, reflecting the closing and reopening of the semiconducting band gap. Both of these features are characteristics of a topological quantum phase transition and are consistent with a recent theoretical proposal.

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). Fourier-transform infrared (FT-IR) spectrometer is used for multi-wavelength data acquisition. The sample stage has temperature variation between 4.2 and 450 K, wide range of θ-2θ angular rotation, χ tilt angle adjustment, and X-Y-Z translation. A LabVIEW-based software controls the motors, sample temperature, and FT-IR spectrometer and also allows to run fully automated experiments with pre-programmed measurement schedules. Data analysis is based on Berreman's 4 × 4 propagation matrix formalism to calculate the Mueller matrix parameters of anisotropic samples with magnetic permeability µ ≠ 1. A nonlinear regression of the rotating analyzer ellipsometry and∕or Mueller matrix (MM) spectra, which are usually acquired at variable angles of incidence and sample crystallographic orientations, allows extraction of dielectric constant and magnetic permeability tensors for bulk and thin-film samples. Applications of this ellipsometer setup for multiferroic and ferrimagnetic materials with µ ≠ 1 are illustrated with experimental results and simulations for TbMnO3 and Dy3Fe5O12 single crystals. We demonstrate how magnetic and electric dipoles, such as magnons and phonons, can be distinguished from a single MM measurement without adducing any modeling arguments. The parameters of magnetoelectric components of electromagnon excitations are determined using MM spectra of TbMnO3.

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. Recently, progress been made toward efficiently coupling synchrotron IR beamlines to multipixel detectors, but they utilize expensive and highly customized optical schemes. Here we demonstrate the development and application of a simple optical configuration that can be implemented on most existing synchrotron IR beamlines to achieve full-field IR imaging with diffraction-limited spatial resolution. Specifically, the synchrotron radiation fan is extracted from the bending magnet and split into four beams that are combined on the sample, allowing it to fill a large section of the FPA. With this optical configuration, we are able to oversample an image by more than a factor of 2, even at the shortest wavelengths, making image restoration through deconvolution algorithms possible. High chemical sensitivity, rapid acquisition times, and superior signal-to-noise characteristics of the instrument are demonstrated. The unique characteristics of this setup enabled the real-time study of heterogeneous chemical dynamics with diffraction-limited spatial resolution for the first time.

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. These observations reflect the strong coupling between phonons and interband electronic transitions in these systems and the distinctive variation in the joint density of electronic states in samples of differing thickness and stacking order.

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 ∼0.26 to 2.6 THz with a bandwidth of ∼0.16 THz.

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. The resiliency of the soft organic ring is a major factor in the stability of this material. Interestingly, the collective character of the lattice vibrations masks direct information on the Cu-N and Cu-O linkages through the series of pressure-induced Jahn-Teller axis switching transitions, although Cu-F bond softening is clearly identified above 3 GPa. These findings illustrate the importance of combined bulk and local probe techniques for microscopic structure determination in complex materials.

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. The field was applied parallel to the film surface and the conductivity extracted from far-infrared transmission and reflection measurements. The real part shows the superconducting gap, which we observe to be suppressed by the applied magnetic field. We compare our results with the pair-breaking theory of Abrikosov and Gor'kov and confirm directly the theory's validity for the optical conductivity.

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. The observed THz-induced cross-phase modulation agrees well with a time-dependent phase-shift model.

Coherent THz synchrotron radiation from a storage ring with high-frequency RF system.

The generation of brilliant, stable, and broadband coherent synchrotron radiation (CSR) in electron storage rings depends strongly on ring rf system properties such as frequency and gap voltage. We have observed intense coherent radiation at frequencies approaching the THz regime produced by the MIT-Bates South Hall Ring, which employs a high-frequency S-band rf system. The measured CSR spectral intensity enhancement with 2 mA stored current was up to 10,000 times above background for wave numbers near 3 cm(-1). The measurements also uncovered strong beam instabilities that must be suppressed if such a very high rf frequency electron storage ring is to become a viable coherent THz source.

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. The ability for thesynchrotron source to perform microscopy ata frequency of 1 THz is demonstrated.

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. For clarity we compare thissource with one based on ultrafast lasertechniques.

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. In contrast to conventional THz radiation, however, the intensity is many orders of magnitude greater due to the relativistic enhancement.

High-power terahertz radiation from relativistic electrons.

Terahertz (THz) radiation, which lies in the far-infrared region, is at the interface of electronics and photonics. Narrow-band THz radiation can be produced by free-electron lasers and fast diodes. Broadband THz radiation can be produced by thermal sources and, more recently, by table-top laser-driven sources and by short electron bunches in accelerators, but so far only with low power. Here we report calculations and measurements that confirm the production of high-power broadband THz radiation from subpicosecond electron bunches in an accelerator. The average power is nearly 20 watts, several orders of magnitude higher than any existing source, which could enable various new applications. In particular, many materials have distinct absorptive and dispersive properties in this spectral range, so that THz imaging could reveal interesting features. For example, it would be possible to image the distribution of specific proteins or water in tissue, or buried metal layers in semiconductors; the present source would allow full-field, real-time capture of such images. High peak and average power THz sources are also critical in driving new nonlinear phenomena and for pump-probe studies of dynamical properties of materials.

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. This statement does not hold for the Afro-American hair analysed. For this, the FT-IR spectra do not change within the hair section and are insensitive to solvent extraction. The importance of the origin of hair on its physical and chemical properties has to be taken into account in future investigations.

Optical properties of c-axis oriented superconducting MgB2 films.

Temperature dependent optical conductivities and dc resistivity of c-axis oriented superconducting (T(c) = 39.6 K) MgB2 films (approximately 450 nm) have been measured. The normal state ab-plane optical conductivities can be described by the Drude model with a temperature independent Drude plasma frequency of omega(p,D) = 13 600+/-100 cm(-1) or 1.68+/-0.01 eV. The normal state resistivity is fitted by the Bloch-Grüneisen formula with an electron-phonon coupling constant lambda(tr) = 0.13+/-0.02. The optical conductivity spectra below T(c) of these films suggest that MgB2 is a multigap superconductor.