Probing equilibrium glass flow up to exapoise viscosities

Glasses are out-of-equilibrium systems aging under the crystallization threat. During ordinary glass formation, the atomic diffusion slows down rendering its experimental investigation impractically long, to the extent that a timescale divergence is taken for granted by many. We circumvent here these limitations, taking advantage of a wide family of glasses rapidly obtained by physical vapor deposition directly into the solid state, endowed with different "ages" rivaling those reached by standard cooling and waiting for millennia. Isothermally probing the mechanical response of each of these glasses, we infer a correspondence with viscosity along the equilibrium line, up to exapoise values. We find a dependence of the elastic modulus on the glass age, which, traced back to temperature steepness index of the viscosity, tears down one of the cornerstones of several glass transition theories: the dynamical divergence. Critically, our results suggest that the conventional wisdom picture of a glass ceasing to flow at finite temperature could be wrong.Comment: 4 figures and 1 supplementary figur

Tracking the connection between disorder and energy landscape in glasses using geologically hyperaged amber

Fossil amber offers the unique opportunity of investigating an amorphous material which has been exploring its energy landscape for more than 110 Myears of natural aging. By applying different x-ray scattering methods to amber before and after annealing the sample to erase its thermal history, we identify a link between the potential energy landscape and the structural and vibrational properties of glasses. We find that hyperaging induces a depletion of the vibrational density of states in the THz region, also ruling the sound dispersion and attenuation properties of the corresponding acoustic waves. Critically, this is accompanied by a densification with structural implications different in nature from that caused by hydrostatic compression. Our results, rationalized within the framework of fluctuating elasticity theory, reveal how upon approaching the bottom of the potential energy landscape (9% decrease in the fictive temperature $T_f$) the elastic matrix becomes increasingly less disordered (6%) and longer-range correlated (22%).Comment: 9 pages, 10 figure

Mapping propagation of collective modes in Bi2Se3 and Bi2Te2.2Se0.8 topological insulators by near-field terahertz nanoscopy

Near-field microscopy discloses a peculiar potential to explore novel quantum state of matter at the nanoscale, providing an intriguing playground to investigate, locally, carrier dynamics or propagation of photoexcited modes as plasmons, phonons, plasmon-polaritons or phonon-polaritons. Here, we exploit a combination of hyperspectral time domain spectroscopy nano-imaging and detectorless scattering near-field optical microscopy, at multiple terahertz frequencies, to explore the rich physics of layered topological insulators as Bi2Se3 and Bi2Te2.2Se0.8, hyperbolic materials with topologically protected surface states. By mapping the near-field scattering signal from a set of thin flakes of Bi2Se3 and Bi2Te2.2Se0.8 of various thicknesses, we shed light on the nature of the collective modes dominating their optical response in the 2-3 THz range. We capture snapshots of the activation of transverse and longitudinal optical phonons and reveal the propagation of sub-diffractional hyperbolic phonon-polariton modes influenced by the Dirac plasmons arising from the topological surface states and of bulk plasmons, prospecting new research directions in plasmonics, tailored nanophotonics, spintronics and quantum technologies

Acoustic-like dynamics of amorphous drugs in the THz regime

The high frequency dynamics of Indomethacin and Celecoxib glasses has been investigated by inelastic x-ray scattering, accessing a momentum-energy region still unexplored in amorphous pharmaceuticals. We find evidence of phonon-like acoustic dynamics, and determine the THz behavior of sound velocity and acoustic attenuation. Connections with ordinary sound propagation are discussed, along with the relation between fast and slow degrees of freedom as represented by non-ergodicity factor and kinetic fragility, respectively

Terahertz near-field nanoscopy based on detectorless laser feedback interferometry under different feedback regimes

Near-field imaging techniques, at terahertz frequencies (1-10 THz), conventionally rely on bulky laser sources and detectors. Here, we employ a semiconductor heterostructure laser as a THz source and, simultaneously, as a phase-sensitive detector, exploiting optical feedback interferometry combined with scattering near-field nanoscopy. We analyze the amplitude and phase sensitivity of the proposed technique as a function of the laser driving current and of the feedback attenuation, discussing the operational conditions ideal to optimize the nano-imaging contrast and the phase sensitivity. As a targeted nanomaterial, we exploit a thin (39 nm) flake of Bi2Te2.2Se0.8, a topological insulator having infrared active optical phonon modes. The self-mixing interference fringes are analyzed within the Lang-Kobayashi formalism to rationalize the observed variations as a function of Acket’s parameter C in the full range of weak feedback (C < 1)

Terahertz Near-field Nanoscopy Based on Self-mixing Interferometry with Quantum Cascade Resonators

Near-field imaging techniques at terahertz frequencies (0.5-10 THz), conventionally rely on bulky laser sources and detectors. Here, we devise a compact configuration for scattering near-field nanoscopy based on quantum cascade lasers (QCL) that can simultaneously act as powerful THz source and phase-sensitive detector, exploiting optical feedback interferometry [1] , (see Fig 1a ). Self-detection is based on the reinjection of the field scattered by the AFM tip into the laser cavity causing coherent interference. The near-field scattering is measured through the induced changes in the contact voltage of the QCL. By changing the path length with a movable mirror, self-mixing interference fringes are acquired and allow to retrieve both the amplitude and phase of the scattered field giving access to the complex-valued dielectric response of the sample [2]. Interestingly for imaging applications, this detection approach is fundamentally limited only by electron transport in the QCL allowing for fast image acquisition

Tunable, Grating-Gated, Graphene-On-Polyimide Terahertz Modulators

An electrically switchable graphene terahertz (THz) modulator with a tunable-by-design optical bandwidth is presented and it is exploited to compensate the cavity dispersion of a quantum cascade laser (QCL). Electrostatic gating is achieved by a metal grating used as a gate electrode, with an HfO2/AlOx gate dielectric on top. This is patterned on a polyimide layer, which acts as a quarter wave resonance cavity, coupled with an Au reflector underneath. The authors achieve 90% modulation depth of the intensity, combined with a 20 kHz electrical bandwidth in the 1.9–2.7 THz range. The modulator is then integrated with a multimode THz QCL. By adjusting the modulator operational bandwidth, the authors demonstrate that the graphene modulator can partially compensate the QCL cavity dispersion, resulting in an integrated laser behaving as a stable frequency comb over 35% of the operational range, with 98 equidistant optical modes and a spectral coverage ~1.2 THz. This paves the way for applications in the terahertz, such as tunable transformation-optics devices, active photonic components, adaptive and quantum optics, and metrological tools for spectroscopy at THz frequencies

Ultrafast optical control of nonlinear dielectric nanoantennas

Efficient ultrafast reconfiguration of the second-harmonic generation of AlGaAs nonlinear nanoantennas operating at 1550 nm telecom wavelength, is achieved by ultrafast interband photoexcitation with femtosecond visible pulses. The combination of broadband transient transmittivity, time-revolved second harmonic generation, and nonlinear optics nanoscale modeling, allows to track the ultrafast modulation of the second harmonic signal, into the nanoscale charge carrier dynamics at the base of a giant permittivity change at the semiconducting band edg