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We report on the crystal structure and ferroelectric properties of epitaxial ZrO$_2$ films ranging from 7 to 42 nm thickness grown on La$_{0.67}$Sr$_{0.33}$MnO$_3$-buffered (110)-oriented SrTiO$_3$ substrate. By employing X-ray diffraction, we confirm a tetragonal phase at all investigated thicknesses, with slight in-plane strain due to the substrate in the thinnest films. Further confirmation of the tetragonal phase was obtained through Infrared absorption spectroscopy with synchrotron light, performed on ZrO$_2$ membrane transferred onto a high resistive Silicon substrate. Up to a thickness of 31 nm, the ZrO$_2$ epitaxial films exhibit ferroelectric behavior, at variance with the antiferroelectric behavior reported previously for the tetragonal phase in polycrystalline films. However, the ferroelectricity is found here to diminish with increasing film thickness, with a polarization of about 13 $\mu$C.cm$^{-2}$ and down to 1 $\mu$C.cm$^{-2}$ for 7 nm and 31 nm-thick ZrO$_2$ films, respectively. This highlights the role of thickness reduction, substrate strain, and surface effects in promoting polarization in the tetragonal ZrO$_2$ thin films. These findings provide new insights into the ferroelectric properties and structure of ZrO$_2$ thin films, and open up new directions to investigate the origin of ferroelectricity in ZrO$_2$ and to optimize this material for future applications.

In metal-organic-framework (MOF) perovskites, both magnetic and ferroelectric orderings can be readily realized by compounding spin and charge degrees of freedom. The hydrogen bonds that bridge the magnetic framework and organic molecules have long been thought of as a key in generating multiferroic properties. However, the underlying physical mechanisms remain unclear. Here, we combine neutron diffraction, quasielastic and inelastic neutron scattering, and THz spectroscopy techniques to thoroughly investigate the dynamical properties of the multiferroic MOF candidate [CH$_3$NH$_3$][Co(HCOO)$_3$] through its multiple phase transitions. The wide range of energy resolutions reachable by these techniques enables us to scrutinize the coupling between the molecules and the framework throughout the phase transitions and interrogate a possible magnetoelectric coupling. Our results also reveal a structural change around 220 K which may be associated with the activation of a nodding donkey mode of the methylammonium molecule due to the ordering of the CH$_3$ groups. Upon the occurrence of the modulated phase transition around 130 K, the methylammonium molecules undergo a freezing of its reorientational motions which is concomitant with a change of the lattice parameters and anomalies of collective lattice vibrations. No significant change has been however observed in the lattice dynamics around the magnetic ordering, which therefore indicates the absence of a substantial magneto-electric coupling in zero-field.

We present a high-pressure investigation of the semiconductor-to-metal transition in MoS2 and WS2 carried out by synchrotron-based far-infrared spectroscopy, to reconcile the controversial estimates of the metallization pressure found in the literature and gain new insight into the mechanisms ruling this electronic transition. Two spectral descriptors are found indicative of the onset of metallicity and of the origin of the free carriers in the metallic state: the absorbance spectral weight, whose abrupt increase defines the metallization pressure threshold, and the asymmetric lineshape of the E1u peak, whose pressure evolution, interpreted within the Fano model, suggests the electrons in the metallic state originate from n-type doping levels. Combining our results with those reported in the literature, we hypothesize a two-step mechanism is at work in the metallization process, in which the pressure-induced hybridization between doping and conduction band states drives an early metallic behaviour, while the band-gap closes at higher pressures., Comment: 8 pages, 3 figures

While the spin liquid state in the frustrated pyrochlore Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ has been studied both experimentally and theoretically for more than two decades, no definite description of this unconventional state has been achieved. Using synchrotron based THz spectroscopy in combination with quantum numerical simulations, we highlight a significant link between two previously unrelated features: the existence of a quadrupolar order following an ice rule and the presence of strong magneto-elastic coupling in the form of hybridized Tb$^{3+}$ crystal-field and phonon modes. The magnitude of this so-called vibronic process, which involves quadrupolar degrees of freedom, is significantly dependent on small off-stoichiometry $x$ and favors all-in all-out like correlations between quadrupoles. This mechanism competes with the long range ordered quadrupolar ice, and for slightly different stoichiometry, is able to destabilize it., Comment: Main text: 7 pages, 3 figures ; Supplemental Material: 6 pages, 2 figures

The intensive search for alternative non-cuprate high-transition-temperature ($T_c$) superconductors has taken a positive turn recently with the discovery of superconductivity in infinite layer nickelates. This discovery is expected to be the basis for disentangling the puzzle behind the physics of high $T_c$ in oxides. In the unsolved quest for the physical conditions necessary for inducing superconductivity, we report an optical study of a Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ film measured using optical spectroscopy, at temperatures above and below the critical temperature $T_c\sim 13$ K. The normal-state electrodynamics of Nd$_{0.8}$Sr$_{0.2}$NiO$_2$, is described by the Drude model characterized by a scattering time just above $T_c$ ($\tau \sim 1.7\times 10^{-14}$ s) and a plasma frequency $\omega_p = 8500$ cm$^{-1}$ in combination with an absorption band in the Mid-Infrared (MIR) around $\omega_0 \sim 4000$ cm$^{-1}$. The MIR absorption indicates the presence of strong electronic correlation effect in the NiO$_2$ plane similarly to cuprates. Below $T_c$, a superconducting energy gap ($2\Delta$) of $\sim 3.2$ meV is extracted from the Terahertz reflectivity using the the Mattis-Bardeen model. From the Ferrel-Glover-Thinkam Rule applied to the real part of the optical conductivity, we also estimate a London penetration depth of about 490 nm, in agreement with a type-II superconductivity in Nd$_{0.8}$Sr$_{0.2}$NiO$_2$ Nickelate., Comment: there were some mistakes in previous arXiv

Electromagnetic resonators, which are based on optical cavities or electronic circuits, are key elements to enhance and control light-matter interaction. In the THz range, current optical cavities exhibit very high-quality factors with $(\lambda/2)^3$ mode volumes limited by diffraction, whereas resonant electronic circuits show low quality factor but provide strong subwavelength effective volume ($10^{-6} \lambda^3$). To overcome the limitations of each type of resonator, great efforts are being devoted to improving the performances of current methods or to the emergence of original approaches. Here, we report on an optical resonator based on Tamm modes newly applied to the THz range, comprising a metallic layer on a distributed Bragg reflector and demonstrating a high-quality factor of 230 at $\sim$1 THz. We further experimentally and theoretically show a fine-tuning of the Tamm mode frequency (over a 250 GHz range) and polarization sensitivity by subwavelength structuration of the metallic layer. Electromagnetic simulations also reveal that THz Tamm modes are confined over a $\lambda$/2 length within the distributed Bragg reflector and can be ideally coupled to both bulk materials and 2D materials. These THz Tamm cavities are therefore attractive as basic building blocks of lasers, for the development of advanced THz optoelectronic devices such as sensitive detectors, high-contrast modulators, narrow filters, and polarizers, as well as for THz cavity quantum electrodynamics in nanostructures., Comment: 8 pages, 4 figures

Single-shot recording of terahertz electric signals has recently become possible at high repetition rates, by using the photonic time-stretch electro-optic sampling (EOS) technique. However the moderate sensitivity of time-stretch EOS is still a strong limit for a range of applications. Here we present a variant enabling to increase the sensitivity of photonic time-stretch for free-propagating THz signals. A key point is to integrate the idea presented in Ref. [Ahmed et al., Rev. Sci. Instrum. 85, 013114 (2014)], for upgrading classical time-stretch systems. The method is tested using the high repetition rate terahertz coherent synchrotron radiation source (CSR) of the SOLEIL synchrotron radiation facility. The signal-to-noise ratio of our terahertz digitizer could thus be straightforwardly improved by a factor $\approx 6.5$, leading to a noise-equivalent input electric field below $1.25$~V/cm inside the electro-optic crystal, over the 0-300~GHz band (i.e, 2.3~$\mu$V/cm/$\sqrt{\text{Hz}}$). The sensitivity is scalable with respect to the available laser power, potentially enabling further sensitivity improvements when needed., Comment: 9 pages, 7 figures

The great potential of Dirac electrons for plasmonics and photonics has been readily recognized after their discovery in graphene, followed by applications to smart optical devices. Dirac carriers are also found in topological insulators (TI) --quantum systems having an insulating gap in the bulk and intrinsic Dirac metallic states at the surface--. Here, we investigate the plasmonic response of ring structures patterned in Bi$_2$Se$_3$ TI films, which we investigate through terahertz (THz) spectroscopy. The rings are observed to exhibit a bonding and an antibonding plasmon modes, which we tune in frequency by varying their diameter. We develop an analytical theory based on the THz conductivity of unpatterned films, which accurately describes the strong plasmon-phonon hybridization and Fano interference experimentally observed as the bonding plasmon is swiped across the promineng 2\,THz phonon exhibited by this material. This work opens the road for the investigation of plasmons in topological insulators and for their application in tunable THz devices., Comment: 9 pages, 2 figures. To be published in Advanced Optical Materials

Pb$_{0.77}$Sn$_{0.23}$Se is a novel alloy of two promising thermoelectric materials PbSe and SnSe that exhibits a temperature dependent band inversion below 300 K. Recent work has shown that this band inversion also coincides with a trivial to nontrivial topological phase transition. To understand how the properties critical to thermoelectric efficiency are affected by the band inversion, we measured the broadband optical response of Pb$_{0.77}$Sn$_{0.23}$Se as a function of temperature. We find clear optical evidence of the band inversion at $160\pm15$ K, and use the extended Drude model to accurately determine a $T^{3/2}$ dependence of the bulk carrier lifetime, associated with electron-acoustic phonon scattering. Due to the high bulk carrier doping level, no discriminating signatures of the topological surface states are found, although their presence cannot be excluded from our data., Comment: 11 pages, 6 figures

The low energy dynamical properties of the multiferroic hexagonal perovskite ErMnO3 have been studied by inelastic neutron scattering as well as terahertz and far infrared spectroscopies on synchrotron source. From these complementary techniques, we have determined the magnon and crystal field spectra and identified a zone center magnon only excitable by the electric field of an electromagnetic wave. Using comparison with the isostructural YMnO3 compound and crystal field calculations, we propose that this dynamical magnetoelectric process is due to the hybridization of a magnon with an electro-active crystal field transition., Comment: 6 pages

We have determined the terahertz spectrum of the chiral langasite Ba$_3$NbFe$_3$Si$_2$O$_{14}$ by means of synchrotron-radiation measurements. Two excitations are revealed that are shown to have a different nature. The first one, purely magnetic, is observed at low temperature in the magnetically ordered phase and is assigned to a magnon. The second one persits far into the paramagnetic phase and exhibits both an electric and a magnetic activity at slightly different energies. This magnetoelectric excitation is interpreted in terms of atomic rotations and requires a helical electric polarization.