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This paper presents a study of the structure dynamics in BaFe$_2$Se$_3$. We combined first-principle calculations, infrared measurements and a thorough symmetry analysis. Our study confirms that $Pnma$ cannot be the space group of BaFe$_2$Se$_3$, even at room temperature. The phonons assignment requires $Pm$ to be the BaFe$_2$Se$_3$ space group, not only in the magnetic phase, but also in the paramagnetic phase at room temperature. This is due to a strong coupling between a short range spin-order along the ladders, and the lattice degrees of freedom associated with the Fe-Fe bond length. This coupling induces a change in the bond-length pattern from an alternated trapezoidal one (as in $Pnma$) to an alternated small/large rectangular one. Out of the two patterns, only the latter is fully compatible with the observed block-type magnetic structure. Finally, we propose a complete symmetry analysis of the BaFe$_2$Se$_3$ phase diagram in the 0-600\,K range., Comment: 15 page, 5 fig

Magnetic and crystallographic transitions in the Cairo pentagonal magnet Bi2Fe4O9 are investigated by means of infrared synchrotron-based spectroscopy as a function of temperature (20 - 300 K) and pressure (0 - 15.5 GPa). One of the phonon modes is shown to exhibit an anomalous softening as a function of temperature in the antiferromagnetic phase below 240 K, highlighting spin-lattice coupling. Moreover, under applied pressure at 40 K, an even larger softening is observed through the pressure induced structural transition. Lattice dynamical calculations reveal that this mode is indeed very peculiar as it involves a minimal bending of the strongest superexchange path in the pentagonal planes, as well as a decrease of the distances between second neighbor irons. The latter confirms the hypothesis made by Friedrich et al.,1 about an increase in the oxygen coordination of irons being at the origin of the pressure-induced structural transition. As a consequence, one expects a new magnetic superexchange path that may alter the magnetic structure under pressure., Comment: 11 pages, 8 figures, 5 tables

The low energy lattice dynamics of the quasi-periodic spin-ladder cuprate Sr$_{14-x}$Ca$_x$Cu$_{24}$O$_{41}$ are investigated using terahertz frequency synchrotron radiation. A high density of low-lying optical excitations are present in the 1-3 THz energy range, while at least two highly absorbing excitations stemming from rigid acoustic oscillations of the incommensurate chain and ladder sublattices, are observed at sub-terahertz frequencies. The effects of Ca substitution on the sub-terahertz quasi-acoustic sliding mode gaps is investigated using coherent synchrotron radiation. Analysis of the results suggest increasing substitution of Sr for Ca is accompanied by a transfer of spectral weight between sliding modes associated with different chain-ladder dynamics. The observation is consistent with a transfer of hole charges from the chains to the ladders and modification of the sublattice dimensions following Ca substitution. The results are discussed in context to the significance of low-lying vibrational dynamics and electron-phonon coupling in the superconducting state of certain quasi-periodic systems.

In the multiferroic hexagonal manganite HoMnO3, inelastic neutron scattering and synchrotron based THz spectroscopy have been used to investigate the spin waves associated to the Mn order together with Ho crystal field excitations. While the Mn order sets in first below 80 K, a spin reorientation occurs below 37 K, a rare feature in the rare earth manganites. We show that severalHo crystal field excitations are present in the same energy range as the magnons, and that they are all affected by the spin reorientation. Moreover, several anomalous features are observed in the excitations at low temperature. Our analysis and calculations for the Mn spin waves and Ho crystal field excitations support Mn-Ho coupling mechanisms as well as coupling to the lattice affecting the dynamics.

Spontaneous formation of spatial structures (patterns) occurs in various contexts, ranging from sand dunes and rogue wave formation, to traffic jams. These last decades, very practical reasons also led to studies of pattern formation in relativistic electron bunches used in synchrotron radiation light sources. As the main motivation, the patterns which spontaneously appear during an instability increase the terahertz radiation power by factors exceeding 10000. However the irregularity of these patterns largely prevented applications of this powerful source. Here we show how to make the spatio-temporal patterns regular (and thus the emitted THz power) using a point of view borrowed from chaos control theory. Mathematically, regular unstable solutions are expected to coexist with the undesired irregular solutions, and may thus be controllable using feedback control. We demonstrate the stabilization of such regular solutions in the Synchrotron SOLEIL storage ring. Operation of these "controlled unstable solutions" enables new designs of high charge and stable synchrotron radiation sources., Comment: 7 pages, 4 figures

We have used grazing-angle infrared spectroscopy to detect the Berreman effect (BE) in the quasi-two-dimensional electron system (q-2DES) which forms spontaneously at the interface between SrTiO$_{3}$ (STO) and a thin film of LaAlO$_3$ (LAO). From the BE, which allows one to study longitudinal optical excitations in ultrathin films like the q-2DES, we have extracted at different temperatures its thickness, the charge density and mobility of the carriers under crystalline LAO (sample A), and the charge density under amorphous LAO (sample B). This quantity turns out to be higher than in sample A, but a comparison with Hall measurements shows that under amorphous LAO the charges are partly localized at low $T$ with a low activation energy (about 190 K in $k_B$ units), and are thermally activated according to a model for large polarons. The thickness of the q-2DES extracted from our spectra turns out to be 4 $\pm 1$ nm for crystalline LAO, 7 $\pm 2$ nm for amorphous LAO., Comment: 21 pages, 7 figures

To model the cold dust emission observed in the diffuse interstellar medium, in dense molecular clouds or in cold clumps that could eventually form new stars, it is mandatory to know the physical and spectroscopic properties of this dust and to understand its emission. This work is a continuation of previous studies aiming at providing astronomers with spectroscopic data of realistic cosmic dust analogues for the interpretation of observations. Ferromagnesium amorphous silicate dust analogues were produced with a mean composition close to $\mathrm{Mg_{1-x}Fe_{x}SiO_3}$ with x = 0.1, 0.2, 0.3, 0.4. Part of each sample was annealed at 500$^{\circ}$C for two hours in a reducing atmosphere to modify the oxidation state of iron. We have measured the mass absorption coefficient (MAC) of these ferromagnesium amorphous silicate dust analogues in the spectral domain 30 - 1000 $\mu$m for grain temperature in the range 10 - 300 K and at room temperature in the 5 - 40 $\mu$m range. The MAC of ferromagnesium samples behaves in the same way as the MAC of pure Mg-rich amorphous silicate samples. In the 30 - 300 K range, the MAC increases with increasing grain temperature whereas in the range 10 - 30 K, we do not see any change of the MAC. The MAC cannot be described by a single power law in ${\lambda}^{-\beta}$. The MAC of all the samples is much higher than the MAC calculated by dust models. The complex behavior of the MAC of amorphous silicates with wavelength and temperature is observed whatever the exact silicate composition (Mg vs. Fe amount). It is a universal characteristic of amorphous materials, and therefore of amorphous cosmic silicates, that should be taken into account in astronomical modeling. The enhanced MAC of the measured samples compared to the MAC calculated for cosmic dust model implies that dust masses are overestimated by the models.

A wealth of data from the Herschel and Planck satellites and now from ALMA, revealing cold dust thermal emission, is available for astronomical environments ranging from interstellar clouds, cold clumps, circumstellar envelops, and protoplanetary disks. The interpretation of these observations relies on the understanding and modeling of cold dust emission and on the knowledge of the dust optical properties. The aim of this work is to provide astronomers with a set of spectroscopic data of realistic interstellar dust analogues that can be used to interpret the observations. Glassy silicates of mean composition (1-x)MgO - xSiO2 with x = 0.35, 0.40 and 0.50 were synthesized. The mass absorption coefficient (MAC) of the samples was measured in the spectral domain 30 - 1000 $\mu$m for grain temperature in the range 300 K - 10 K and at room temperature in the 5 - 40 $\mu$m domain. We find that the MAC of all samples varies with the grains temperature. In the FIR/submm, and above 30K, the MAC value at a given wavelength increases with the temperature as thermally activated absorption processes appear. The studied materials exhibit different and complex behaviors at long wavelengths (lambda $\geq$ 200 to 700 $\mu$m depending on the samples) and the MAC cannot be approximated by a single power law in ${\lambda}^{-\beta}$. These behaviors are attributed to the amorphous nature of dust and to the amount and nature of the defects within this amorphous structure. Above 20 $\mu$m, the measured MAC are much higher than the MAC calculated from interstellar silicate dust models indicating that the analogues measured in this study are more emissive than the silicates in cosmic dust models. This has important astrophysical implications because masses are overestimated by the models. Moreover, constraints on elemental abundance of heavy elements in cosmic dust models are relaxed

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 information

The origin of quantum fluctuations responsible for the spin liquid state in Tb$_2$Ti$_2$O$_7$ has remained a long standing problem. By synchrotron-based terahertz measurements, we show evidence of strong coupling between the magnetic and lattice degrees of freedom that provides a path to the quantum melting process. As revealed by hybrid crystal electric field-phonon excitations that appear at 0.67 THz below 200 K, and around 0.42 THz below 50 K, the double vibronic process is unique for Tb$^{3+}$ in the titanate family due to adequate energy matching and strong quadrupolar moments. The results suggest that lattice motion can indeed be the driving force behind spin flips within the hybridized ground and first excited states, promoting quantum terms in the effective Hamiltonian that describes Tb$_2$Ti$_2$O$_7$.

In recent synchrotron radiation facilities, the use of short (picosecond) electron bunches is a powerful method for producing giant pulses of Terahertz Coherent Synchrotron Radiation (THz CSR). Here we report on the first direct observation of these pulse shapes with a few picoseconds resolution, and of their dynamics over a long time. We 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 (a broadband Terahertz comb) stemming from the shortness of the electron bunches. Above this threshold, a large part of the emission is dominated by drifting structures, which appear through spontaneous self-organization. These challenging single-shot THz recordings are made possible by using a recently developed photonic time stretch detector with a high sensitivity. The experiment has been realized at the SOLEIL storage ring.

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.

Emission of light by a single electron moving on a curved trajectory (synchrotron radiation) is one of the most well-known fundamental radiation phenomena. However experimental situations are more complex as they involve many electrons, each being exposed to the radiation of its neighbors. This interaction has dramatic consequences, one of the most spectacular being the spontaneous formation of spatial structures inside electrons bunches. This fundamental effect is actively studied as it represents one of the most fundamental limitations in electron accelerators, and at the same time a source of intense terahertz radiation (Coherent Synchrotron Radiation, or CSR). Here we demonstrate the possibility to directly observe the electron bunch microstructures with subpicosecond resolution, in a storage ring accelerator. The principle is to monitor the terahertz pulses emitted by the structures, using a strategy from photonics, time-stretch, consisting in slowing-down the phenomena before recording. This opens the way to unpreceeded possibilities for analyzing and mastering new generation high power coherent synchrotron sources., Comment: 7 pages, 6 figures

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.

We perform a comparative experimental and theoretical study of the temperature dependence up to 700 K of the frequency and linewidths of the graphite E1u and E2g optical phonons (~1590 and 1580 cm-1) by infra-red (IR) and Raman spectroscopy. Despite their similar character, the temperature dependence of the two modes is quite different, being, e.g., the frequency shift of the IR-active E1u mode is almost twice as big as that of the Raman active E2g mode. Ab initio calculations of the anharmonic properties are in remarkable agreement with measurements and explain the observed behavior., Comment: 5 pages, 4 figures

Cold dust grains emission in the FIR/submm is usually expressed as a modified black body law in which the dust mass absorption coefficient (MAC), is described with a temperature- and wavelength-independent emissivity spectral index, beta. However, numerous data from space and balloon-born missions and recently from Herschel and Planck show that dust emission is not well understood, as revealed by the observed anti-correlation of beta with the grain temperature. In order to give astronomers the necessary data to interpret FIR/submm observations, we synthesised analogues of interstellar amorphous and crystalline silicate grains, rich in Mg and Ca, and having stiochiometry of olivine and pyroxene and measured their MAC, in the 100-1000/1500 \mum range for grain temperatures varying from 300 to 10 K. We find that the grain MAC decreases when the grain temperature decreases and that the local spectral index, beta, defined as the slope of the MAC curve, is anti-correlated with the grain temperature. These variations, which are not observed in the crystallised samples, are related to the amorphous nature of the samples. In addition, the spectral shape of the MAC is complex: at short wavelengths (lambda < 500/700 \mum), beta is in the range 1.6 - 2.1 for all grain temperature and grain composition whereas at longer wavelengths (lambda > 500/700 \mum), beta < 2 for samples with a pyroxene stoichiometry and beta > 2 for samples with an olivine stoichiometry. Hence, the simplifying asymptotic expression based on a single temperature- and wavelength-independent spectral index used by astronomers is not appropriate to describe the dust MAC and thus the dust emission, and may induce significant errors on the derived parameters such as the dust mass and the dust physical and chemical properties. Instead, dust emission models should use the dust MAC as a function of wavelength and temperature.