Spectroscopy of H3_3S: evidence of a new energy scale for superconductivity

The discovery of a superconducting phase in sulfur hydride under high pressure with a critical temperature above 200 K has provided a new impetus to the search for even higher $T_c$. Theory predicted and experiment confirmed that the phase involved is H$_3$S with Im-3m crystal structure. The observation of a sharp drop in resistance to zero at $T_c$, its downward shift with magnetic field and a Meissner effect confirm superconductivity but the mechanism involved remains to be determined. Here, we provide a first optical spectroscopy study of this new superconductor. Experimental results for the optical reflectivity of H$_3$S, under high pressure of 150 GPa, for several temperatures and over the range 60 to 600 meV of photon energies, are compared with theoretical calculations based on Eliashberg theory using DFT results for the electron-phonon spectral density $\alpha^2$F($\Omega$). Two significant features stand out: some remarkably strong infrared active phonons at $\approx$ 160 meV and a band with a depressed reflectance in the superconducting state in the region from 450 meV to 600 meV. In this energy range, as predicted by theory, H$_3$S is found to become a better reflector with increasing temperature. This temperature evolution is traced to superconductivity originating from the electron-phonon interaction. The shape, magnitude, and energy dependence of this band at 150 K agrees with our calculations. This provides strong evidence of a conventional mechanism. However, the unusually strong optical phonon suggests a contribution of electronic degrees of freedom.Comment: 10 pages, 8 figures. Main manuscript and supplementary informatio

Molecular assembling in mixtures of hydrophilic 1-butyl-1-methylpyrrolidinium dicyanamide ionic liquid and water

The infrared absorbance spectrum of the ionic liquid 1-butyl-1-methylpyrrolidinium dicyanamide, mixed with water at two different concentrations, was measured between 160 and 300 K in the mid infrared range. Both mixtures do not crystallize on cooling; however, remarkably, the one with an ionic liquid (IL):water composition of 1:3 displays a cold crystallization process on heating in a restricted temperature range between 240 and 250 K. A portion of the water participates to the cold crystallization. On the contrary, with an IL:water composition of 1:6.6 no crystallization takes place. Upon water addition the vibration frequencies of the anion and of some lines of the cation are blue shifted, while the absorption lines of water are red shifted. These facts are interpreted as the evidence of the occurrence of the hydrogen bonding of water, as the hydrogen bonding acceptor with respect to the anion (anion···O-H bonds develop) and as hydrogen donor for the cation (C-H···O bonds can form). Microscopic inhomogeneities in the samples and their evolution with temperature are discussed

Phonons in the multiferroic langasite Ba_3\_3NbFe_3\_3Si_2\_2O_14\_{14} : evidences for symmetry breaking

The chiral langasite Ba$\_3$NbFe$\_3$Si$\_2$O$\_{14}$ is a multiferroic compound. While its magnetic order below T$\_N$=27 K is now well characterised, its polar order is still controversial. We thus looked at the phonon spectrum and its temperature dependence to unravel possible crystal symmetry breaking. We combined optical measurements (both infrared and Raman spectroscopy) with ab initio calculations and show that signatures of a polar state are clearly present in the phonon spectrum even at room temperature. An additional symmetry lowering occurs below 120~K as seen from emergence of softer phonon modes in the THz range. These results confirm the multiferroic nature of this langasite and open new routes to understand the origin of the polar state

Lattice and spin excitations in multiferroic h-YMnO3

We used Raman and terahertz spectroscopies to investigate lattice and magnetic excitations and their cross-coupling in the hexagonal YMnO3 multiferroic. Two phonon modes are strongly affected by the magnetic order. Magnon excitations have been identified thanks to comparison with neutron measurements and spin wave calculations but no electromagnon has been observed. In addition, we evidenced two additional Raman active peaks. We have compared this observation with the anti-crossing between magnon and acoustic phonon branches measured by neutron. These optical measurements underly the unusual strong spin-phonon coupling

Grazing-angle reflectivity setup for the low-temperature infrared spectroscopy of two-dimensional systems

A new optical setup is described that allows the reflectivity at grazing incidence to be measured, including ultrathin films and two-dimensional electron systems (2DES) down to liquid-helium temperatures, by exploiting the Berreman effect and the high brilliance of infrared synchrotron radiation. This apparatus is well adapted to detect the absorption of a 2DES of nanometric thickness, namely that which forms spontaneously at the interface between a thin film of LaAlO3 and its SrTiO3 substrate, and to determine its Drude parameters

A NEW SCHEME FOR ELECTRO-OPTIC SAMPLING AT RECORD REPETITION RATES: PRINCIPLE AND APPLICATION TO THE FIRST (TURN-BY-TURN) RECORDINGS OF THz CSR BURSTS AT SOLEIL

Abstract The microbunching instability is an ubiquitous problem in storage rings at high current density. However, the involved fast time-scales hampered the possibility to make direct real-time recordings of theses structures. When the structures occur at a cm scale, recent works at UVSOR [1], revealed that direct recording of the coherent synchrotron radiation (CSR) electric field with ultra-high speed electronics (17 ps) provides extremely precious informations on the microbunching dynamics. However, when CSR occurs at THz frequencies (and is thus out of reach of electronics), the problem remained largely open. Here we present a new opto-electronic strategy that enabled to record series of successive electric field pulses shapes with picosecond resolution (including carrier and envelope), every 12 ns, over a total duration of several milliseconds. We also present the first experimental results obtained with this method at Synchrotron SOLEIL, above the microbunching instability threshold. The method can be applied to the detection of ps electric fields in other situations where high repetition rate is also an issue

High repetition-rate electro-optic sampling: Recent studies using photonic time-stretch

Single-shot electro-optic sampling (EOS) is a powerful characterization tool for monitoring the shape of electron bunches, and coherent synchrotron radiation pulses. For reaching high acquisition rates, an efficient possibility consists to associate classic EOS systems with the so-called photonic time-stretch technique [1]. We present recent results obtained at SOLEIL and ANKA using this strategy. In particular, we show how a high sensitivity variant of photonic time stretch [2] EOS enabled to monitor the CSR pulses emitted by short electron bunches at SOLEIL [3]. We could thus confirm in a very direct way the theories predicting an interplay between two physical processes. Below a critical bunch charge, we observe a train of identical THz pulses stemming from the shortness of the electron bunches. Above this threshold, CSR emission is dominated by drifting structures appearing through spontaneous self-organization. We also consider the association of time-stretch and EOS for recording electron bunch near fields at high repetition rate. We present preliminary results obtained at ANKA, aiming at recording the electron bunch shape evolution during the microbunching instability

Ab initio molecular dynamics of liquid water using embedded-fragment second-order many-body perturbation theory towards its accurate property prediction

A direct, simultaneous calculation of properties of a liquid using an ab initio electron-correlated theory has long been unthinkable. Here we present structural, dynamical, and response properties of liquid water calculated by ab initio molecular dynamics using the embedded-fragment spin-component-scaled second-order many-body perturbation method with the aug-cc-pVDZ basis set. This level of theory is chosen as it accurately and inexpensively reproduces the water dimer potential energy surface from the coupled-cluster singles, doubles, and noniterative triples with the augcc-pVQZ basis set, which is nearly exact. The calculated radial distribution function, self-diffusion coefficient, coordinate number, and dipole moment, as well as the infrared and Raman spectra are in excellent agreement with experimental results. The shapes and widths of the OH stretching bands in the infrared and Raman spectra and their isotropic-anisotropic Raman noncoincidence, which reflect the diverse local hydrogen-bond environment, are also reproduced computationally. The simulation also reveals intriguing dynamic features of the environment, which are difficult to probe experimentally, such as a surprisingly large fluctuation in the coordination number and the detailed mechanism by which the hydrogen donating water molecules move across the first and second shells, thereby causing this fluctuationopen