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Using angle resolved photoemission spectroscopy (ARPES) we report the first band dispersions and distinct features of the bulk Fermi surface (FS) in the paramagnetic metallic phase of the prototypical metal-insulator transition material V$_2$O$_3$. Along the $c$-axis we observe both an electron pocket and a triangular hole-like FS topology, showing that both V 3$d$ $a_{1g}$ and $e_g^{\pi}$ states contribute to the FS. These results challenge the existing correlation-enhanced crystal field splitting theoretical explanation for the transition mechanism and pave the way for the solution of this mystery., Comment: 5 pages, 4 figures plus supplement 12 pages, 3 figures, 1 table

LiOsO$_3$ has been recently identified as the first unambiguous "ferroelectric metal", experimentally realizing a prediction from 1965 by Anderson and Blount. In this work, we investigate the metallic state in LiOsO$_3$ by means of infrared spectroscopy supplemented by Density Functional Theory and Dynamical Mean Field Theory calculations. Our measurements and theoretical calculations clearly show that LiOsO$_3$ is a very bad metal with a small quasiparticle weight, close to a Mott-Hubbard localization transition. The agreement between experiments and theory allows us to ascribe all the relevant features in the optical conductivity to strong electron-electron correlations within the $t_{2g}$ manifold of the osmium atoms., Comment: 5 pages, 3 figures

We present an experimental and theoretical study exploring surface effects on the evolution of the metal-insulator transition in the model Mott-Hubbard compound Cr-doped V$_2$O$_3$. We find a microscopic domain formation that is clearly affected by the surface crystallographic orientation. Using scanning photoelectron microscopy and X-ray diffraction, we find that surface defects act as nucleation centers for the formation of domains at the temperature-induced isostructural transition and favor the formation of microscopic metallic regions. A density functional theory plus dynamical mean field theory study of different surface terminations shows that the surface reconstruction with excess vanadyl cations leads to doped, and hence more metallic surface states, explaining our experimental observations., Comment: 5 pages, 4 figures

The control of non-equilibrium phenomena in complex solids is an important research frontier, encompassing new effects like light induced superconductivity. Here, we show that coherent optical excitation of molecular vibrations in the organic conductor K3C60 can induce a non-equilibrium state with the optical properties of a superconductor. A transient gap in the real part of the optical conductivity and a low-frequency divergence of the imaginary part are measured for base temperatures far above equilibrium Tc=20 K. These findings underscore the role of coherent light fields in inducing emergent order., Comment: 40 pages, 23 figures

Vanadium sesquioxide V2O3 is considered a textbook example of Mott-Hubbard physics. In this paper we present an extended optical study of its whole temperature/doping phase diagram as obtained by doping the pure material with M=Cr or Ti atoms (V1-xMx)2O3. We reveal that its thermodynamically stable metallic and insulating phases, although macroscopically equivalent, show very different low-energy electrodynamics. The Cr and Ti doping drastically change both the antiferromagnetic gap and the paramagnetic metallic properties. A slight chromium content induces a mesoscopic electronic phase separation, while the pure compound is characterized by short-lived quasiparticles at high temperature. This study thus provides a new comprehensive scenario of the Mott-Hubbard physics in the prototype compound V2O3.

We have studied the optical properties of four (LaNiO$_3$)$_n$/(LaMnO$_3$)$_2$ superlattices (SL) ($n$=2, 3, 4, 5) on SrTiO$_3$ substrates. We have measured the reflectivity at temperatures from 20 K to 400 K, and extracted the optical conductivity through a fitting procedure based on a Kramers-Kronig consistent Lorentz-Drude model. With increasing LaNiO$_3$ thickness, the SLs undergo an insulator-to-metal transition (IMT) that is accompanied by the transfer of spectral weight from high to low frequency. The presence of a broad mid-infrared band, however, shows that the optical conductivity of the (LaNiO$_3$)$_n$/(LaMnO$_3$)$_2$ SLs is not a linear combination of the LaMnO$_3$ and LaNiO$_3$ conductivities. Our observations suggest that interfacial charge transfer leads to an IMT due to a change in valence at the Mn and Ni sites., Comment: Accepted for publication in Phys. Rev. Lett. 5 pages, 5 figures

One of the pivotal questions in the physics of high-temperature superconductors is whether the low-energy dynamics of the charge carriers is mediated by bosons with a characteristic timescale. This issue has remained elusive since electronic correlations are expected to dramatically speed up the electron-boson scattering processes, confining them to the very femtosecond timescale that is hard to access even with state-of-the-art ultrafast techniques. Here we simultaneously push the time resolution and the frequency range of transient reflectivity measurements up to an unprecedented level that enables us to directly observe the 16 fs build-up of the effective electron-boson interaction in hole-doped copper oxides. This extremely fast timescale is in agreement with numerical calculations based on the t-J model and the repulsive Hubbard model, in which the relaxation of the photo-excited charges is achieved via inelastic scattering with short-range antiferromagnetic excitations., Comment: to appear in Nature Physics

The optical properties of a V4O7 single crystal have been investigated from the high temperature metallic phase down to the low temperature antiferromagnetic insulating one. The temperature dependent behavior of the optical conductivity across the metal-insulator transition (MIT) can be explained in a polaronic scenario. Charge carriers form strongly localized polarons in the insulating phase as suggested by a far-infrared charge gap abruptly opening at T_MIT = 237 K. In the metallic phase instead the presence of a Drude term is indicative of fairly delocalized charges with a moderately renormalized mass m* = 5m_e. The electronic spectral weight is almost recovered on an energy scale of 1 eV, which is much narrower compared to VO2 and V2O3 cases. Those findings suggest that electron-lattice interaction rather than electronic correlation is the driving force for V4O7 metal-insulator transition., Comment: 5 pages, 3 figures

La1.8-xEu0.2SrxCuO4 (LESCO) is the member of the 214 family which exhibits the largest intervals among the structural, charge ordering (CO), magnetic, and superconducting transition temperatures. By using new dc transport measurements and data in the literature we construct the phase diagram of LESCO between x = 0.8 and 0.20. This phase diagram has been further probed in ac, by measuring the optical conductivity {\sigma}1({\omega}) of three single crystals with x = 0.11, 0.125, and 0.16 between 10 and 300 K in order to associate the extra-Drude peaks often observed in the 214 family with a given phase. The far-infrared peak we detect in underdoped LESCO is the hardest among them, survives up to room temperature and is associated with charge localization rather than with ordering. At the CO transition for the commensurate doping x = 0.125 instead the extra-Drude peak hardens and a pseudogap opens in {\sigma}1({\omega}), approximately as wide as the maximum superconducting gap of LSCO., Comment: 6 pages, 6 figures

We report on an infrared study on the undoped compound BaFe2As2 as a function of both pressure (up to about 10 GPa) at three temperatures (300, 160, and 110 K). The evolution with pressure and temperature of the optical conductivity shows that, by increasing pressure, the mid-infrared absorptions associated with magnetic order are lowered while the Drude term increases, indicating the evolution towards a conventional metallic state. We evaluate the spectral weight dependence on pressure comparing it to that previously found upon doping. The whole optical results indicate that lattice modifications can not be recognized as the only parameter determining the low-energy electrodynamics in these compounds.

We present high-quality optical data and density functional perturbation theory calculations for the vibrational spectrum of solid picene (C$_{22}$H$_{14}$) under pressure up to 8 GPa. First-principles calculations reproduce with a remarkable accuracy the pressure effects on both frequency and intensities of the phonon peaks experimentally observed . Through a detailed analysis of the phonon eigenvectors, We use the projection on molecular eigenmodes to unambiguously fit the experimental spectra, resolving complicated spectral structures, in a system with hundreds of phonon modes. With these projections, we can also quantify the loss of molecular character under pressure. Our results indicate that picene, despite a \sim 20 % compression of the unit cell, remains substantially a molecular solid up to 8 GPa, with phonon modes displaying a smooth and uniform hardening with pressure. The Grueneisen parameter of the 1380 cm^{-1} a_1 Raman peak ($\gamma_p=0.1$) is much lower than the effective value ($\gamma_d=0.8$) due to K doping. This is an indication that the phonon softening in K doped samples is mainly due to charge transfer and electron-phonon coupling., Comment: Replaced with final version (PRB)

The isostructural metal-insulator transition in Cr-doped V2O3 is the textbook example of a Mott-Hubbard transition between a paramagnetic metal and a paramagnetic insulator. We review recent theoretical calculations as well as experimental findings which shed new light on this famous transition. In particular, the old paradigm of a doping-pressure equivalence does not hold, and there is a microscale phase separation for Cr-doped V2O3., Comment: 16 pages, 11 figures, Feature Article which reviews recent calculations and experiments which shed a new light on the famous Mott-Hubbard transition in V2O3. To appear in physica status solidi (b) 2013

Most available theories for correlated electron transport are based on the Hubbard Hamiltonian. In this effective theory, renormalized hopping and interaction parameters only implicitly incorporate the coupling of correlated charge carriers to microscopic degrees of freedom. Unfortunately, no spectroscopy can individually probe such renormalizations, limiting the applicability of Hubbard models. We show here that the role of each individual degree of freedom can be made explicit by using a new experimental technique, which we term 'quantum modulation spectroscopy' and we demonstrate here in the one-dimensional Mott insulator ET-F2TCNQ. We explore the role on the charge hopping of two localized molecular modes, which we drive with a mid infrared optical pulse. Sidebands appear in the modulated optical spectrum, and their linshape is fitted with a model based on the dynamic Hubbard Hamiltonian. A striking asymmetry between the renormalization of doublons and holons is revealed. The concept of quantum modulation spectroscopy can be used to systematically deconstruct Hubbard Hamiltonians in many materials, exposing the role of any mode, electronic or magnetic, that can be driven to large amplitude with a light field., Comment: 20 pages, 5 figures

The ab-plane optical conductivity of eleven single crystals, belonging to the families Sr2-xCuO2Cl2, Y1-xCaxBa2Cu3O6, Bi2Sr2-xLaxCuO6, and Bi2Sr2CaCu2O8 has been measured with hole concentrations p between 0 and 0.18, and for 6 K < T < 500 K to obtain an infrared picture of the p,T phase diagram of the Cu-O plane. At extreme dilution (p = 0.005), a narrow peak is observed at 1570 cm-1 (195 meV), that we assign to a single-hole bound state. For increasing doping, that peak broadens into a far-infrared (FIR) band whose low-energy edge sets the insulating gap. The insulator-to-metal transition (IMT) occurs when the softening of the FIR band closes the gap thus evolving into a Drude term. In the metallic phase, a multi-band analysis identifies a mid-infrared band which weakly depends on temperature and softens for increasing p, while the extended-Drude analysis leads to an optical scattering rate larger than the frequency, as found in other cuprates. The infrared spectral weight W(T) is consistent with a Fermi liquid renormalized by strong correlations, provided that the T^4 term of the Sommerfeld expansion is included above 300 K. In the superconducting phase, the optical response of single-layer Bi2Sr2-xLaxCuO6 at optimum doping is similar to that of the corresponding optimally-doped bilayer Bi2Sr2CaCu2O8., Comment: 28 pages, 14 figures

V2O3 is the prototype system for the Mott transition, one of the most fundamental phenomena of electronic correlation. Temperature, doping or pressure induce a metal to insulator transition (MIT) between a paramagnetic metal (PM) and a paramagnetic insulator (PI). This or related MITs have a high technological potential, among others for intelligent windows and field effect transistors. However the spatial scale on which such transitions develop is not known in spite of their importance for research and applications. Here we unveil for the first time the MIT in Cr-doped V2O3 with submicron lateral resolution: with decreasing temperature, microscopic domains become metallic and coexist with an insulating background. This explains why the associated PM phase is actually a poor metal. The phase separation can be associated with a thermodynamic instability near the transition. This instability is reduced by pressure which drives a genuine Mott transition to an eventually homogeneous metallic state., Comment: Paper plus supplementary material

The optical conductivity and the spectral weight W(T) of two superconducting cuprates at optimum doping, Bi2Sr2-xLaxCuO6 and Bi2Sr2CaCu2O8, have been first measured up to 500 K. Above 300 K, W(T) deviates from the usual T2 behavior in both compounds, even though the zero-frequency extrapolation of the optical conductivity remains larger than the Ioffe-Regel limit. The deviation is surprisingly well described by the T4 term of the Sommerfeld expansion, but its coefficients are enhanced by strong correlation. This renormalization is due to strong correlation, as shown by the good agreement with dynamical mean field calculations., Comment: 5 pages, 3 figures, Physical Review Letters in press

By studying the optical conductivity of BSLCO and YCBCO, we show that the metal-to-insulator transition (MIT) in these hole-doped cuprates is driven by the opening of a small gap at low T in the far infrared. Its width is consistent with the observations of Angle-Resolved Photoemission Spectroscopy in other cuprates, along the nodal line of the k-space. The gap forms as the Drude term turns into a far-infrared absorption, whose peak frequency can be approximately predicted on the basis of a Mott-like transition. Another band in the mid infrared softens with doping but is less sensitive to the MIT., Comment: To be published on Physical Review Letters

The metal to insulator transition in the charge transfer NiS{2-x}Se{x} compound has been investigated through infrared reflectivity. Measurements performed by applying pressure to pure NiS2 (lattice contraction) and by Se-alloying (lattice expansion) reveal that in both cases an anomalous metallic state is obtained. We find that optical results are not compatible with the linear Se-alloying vs Pressure scaling relation previously established through transport, thus pointing out the substantially different microscopic origin of the two transitions., Comment: Accepted for publication in Phys. Rev. B

We present new data on the pressure dependence at 300 K of the optical reflectivity of CeTe$_3$, which undergoes a charge-density-wave (CDW) phase transition well above room temperature. The collected data cover an unprecedented broad spectral range from the infrared up to the ultraviolet, which allows a robust determination of the gap as well as of the fraction of the Fermi surface affected by the formation of the CDW condensate. Upon compressing the lattice there is a progressive closing of the gap inducing a transfer of spectral weight from the gap feature into the Drude component. At frequencies above the CDW gap we also identify a power-law behavior, consistent with findings along the $R$Te$_3$ series (i.e., chemical pressure) and suggestive of a Tomonaga-Luttinger liquid scenario at high energy scales. This newest set of data is placed in the context of our previous investigations of this class of materials and allows us to revisit important concepts for the physics of CDW state in layered-like two-dimensional systems.

We report the pressure dependence of the optical response of LaTe$_2$, which is deep in the charge-density-wave (CDW) ground state even at 300 K. The reflectivity spectrum is collected in the mid-infrared spectral range at room temperature and at pressures between 0 and 7 GPa. We extract the energy scale due to the single particle excitation across the CDW gap and the Drude weight. We establish that the gap decreases upon compressing the lattice, while the Drude weight increases. This signals a reduction in the quality of nesting upon applying pressure, therefore inducing a lesser impact of the CDW condensate on the electronic properties of LaTe$_2$. The consequent suppression of the CDW gap leads to a release of additional charge carriers, manifested by the shift of weight from the gap feature into the metallic component of the optical response. On the contrary, the power-law behavior, seen in the optical conductivity at energies above the gap excitation and indicating a weakly interacting limit within the Tomonaga-Luttinger liquid scenario, seems to be only moderately dependent on pressure.

We report the first optical study of CaAlSi, a superconductor which displays both the crystal structure of MgB2 and the electronic band structure of intercalated graphites. The reflectivity of a CaAlSi single crystal was measured down to sub-THz frequencies and to 3.3 K, with the use of Coherent Synchrotron Radiation. A superconducting gap in the hexagonal planes, two gaps along the c axis were found and measured, as expected from the structure of the CaAlSi Fermi surface. The anisotropic optical parameters of the normal state were also determined., Comment: 4 pages, 4 figures

The infrared conductivity of V2O3 is measured in the whole phase diagram. Quasiparticles appear above the Neel temperature TN and eventually disappear further enhancing the temperature, leading to a pseudogap in the optical spectrum above 425 K. Our calculations demonstrate that this loss of coherence can be explained only if the temperature dependence of lattice parameters is considered. V2O3 is therefore effectively driven from the metallic to the insulating side of the Mott transition as the temperature is increased., Comment: 5 pages, 3 figures

The electrodynamics near the metal-to-insulator transitions (MIT) induced, in V3O5 single crystals, by both temperature (T) and pressure (P) has been studied by infrared spectroscopy. The T- and P-dependence of the optical conductivity may be explained within a polaronic scenario. The insulating phase at ambient T and P corresponds to strongly localized small polarons. Meanwhile the T-induced metallic phase at ambient pressure is related to a liquid of polarons showing incoherent dc transport, in the P-induced metallic phase at room T strongly localized polarons coexist with partially delocalized ones. The electronic spectral weight is almost recovered, in both the T and P induced metallization processes, on an energy scale of 1 eV, thus supporting the key-role of electron-lattice interaction in the V3O5 metal-to-insulator transition., Comment: 7 pages, 5 figures

Raman and combined trasmission and reflectivity mid infrared measurements have been carried out on monoclinic VO$_2$ at room temperature over the 0-19 GPa and 0-14 GPa pressure ranges, respectively. The pressure dependence obtained for both lattice dynamics and optical gap shows a remarkable stability of the system up to P*$\sim$10 GPa. Evidence of subtle modifications of V ion arrangements within the monoclinic lattice together with the onset of a metallization process via band gap filling are observed for P$>$P*. Differently from ambient pressure, where the VO$_2$ metal phase is found only in conjunction with the rutile structure above 340 K, a new room temperature metallic phase coupled to a monoclinic structure appears accessible in the high pressure regime, thus opening to new important queries on the physics of VO$_2$., Comment: 5 pages, 3 figures

We investigate the pressure dependence of the optical properties of CeTe$_3$, which exhibits an incommensurate charge-density-wave (CDW) state already at 300 K. Our data are collected in the mid-infrared spectral range at room temperature and at pressures between 0 and 9 GPa. The energy for the single particle excitation across the CDW gap decreases upon increasing the applied pressure, similarly to the chemical pressure by rare-earth substitution. The broadening of the bands upon lattice compression removes the perfect nesting condition of the Fermi surface and therefore diminishes the impact of the CDW transition on the electronic properties of $R$Te$_3$., Comment: 5 pages, 4 figures

In the mid-infrared absorption of Sr{1-x}Ce{x}MnO{3} at low electron doping (x = 0.05), a band at 0.3 eV is fully replaced by another one at 0.9 eV as the system becomes antiferromagnetic (AF) of type $G$. A weaker effect occurs at x = 0.10 for an AF phase of type $C$. One thus directly measures the electron hopping energies for spin parallel and anti-parallel to that of the host ion. The Hund's, crystal-field, and Jahn-Teller splittings for the Mn{3+} ions in a Mn{4+} matrix, can also be derived., Comment: Includes 8 Postscript figures

The reflectivity $R (\omega)$ of both the $ab$ plane and the c axis of two single crystals of La$_{1.875}$Ba$_{0.125-y}$Sr$_{y}$CuO$_4$ has been measured down to 5 cm$^{-1}$, using coherent synchrotron radiation below 30 cm$^{-1}$. For $y$ = 0.085, a Josephson Plasma Resonance is detected at $T \ll T_c$ = 31 K in $R_{c} (\omega)$, and a far-infrared peak (FIP) appears in the optical conductivity below 50 K, where non-static charge ordering (CO) is reported by X-ray scattering. For $y$ = 0.05 ($T_c$ = 10 K), a FIP is observed in the low-temperature tetragonal phase below the ordering temperature $T_{CO}$. At 1/8 doping the peak frequency scales linearly with $T_{CO}$, confirming that the FIP is an infrared signature of CO, either static or fluctuating., Comment: v2: longer version, 9 pages, 6 color figures

We compare calculations based on the Dynamical Mean-Field Theory of the Hubbard model with the infrared spectral weight $W(\Omega,T)$ of La$_{2-x}$Sr$_x$CuO$_4$ and other cuprates. Without using fitting parameters we show that most of the anomalies found in $W(\Omega,T)$ with respect to normal metals, including the existence of two different energy scales for the doping- and the $T$-dependence of $W(\Omega,T)$, can be ascribed to strong correlation effects., Comment: 4 pages, 3 figures. Minor corrections, corrected some typos and added references

The infrared conductivity of NaxCoO2 is studied as a function of doping and temperature for x between 0.5 and 1. Charge localization in CoO2 layers shows up through a far-infrared peak (FIP) in the infrared conductivity which coexists with a small Drude contribution. Long-range ordering at x = 0.5 is confirmed to create a far-infrared gap, in addition to the FIP. At high x, the formation of a Spin-Density Wave reported below 22 K dramatically shifts the FIP to higher energy when x is incommensurate with the lattice, indicating an abrupt deepening of the localizing potential. The in-plane E1u phonon lifetime is shown to be sensitive to both "freezing" and ordering of the mobile Na+ ions. A comparison with the behavior of the FIP shows that such "freezing" is not the only origin of charge localization in the CoO layers., Comment: 7 pages, 4 figures

By using new and previous measurements of the $ab$-plane conductivity $\sigma_1^{ab} (\omega,T)$ of La$_{2-x}$Sr$_x$CuO$_{4}$ (LSCO) it is shown that the spectral weight $W = \int_0^\Omega {\sigma_1^{ab} (\omega,T) d\omega}$ obeys the same law $W = W_0 - B(\Omega) T^2$ which holds for a conventional metal like gold, for $\Omega$'s below the plasma frequency. However $B(\Omega)$, which measures the "thermal response" of the charge system, in LSCO exhibits a peculiar behavior which points towards correlation effects. In terms of hopping models, $B(\Omega)$ is directly related to an energy scale $t_T$, smaller by one order of magnitude than the full bandwidth $t_0 \sim W_0$., Comment: 4 pages with 3 figs

In their Comment to a recent paper of ours [Lucarelli et al., PRL 92, 037002 (2003)], Tajima et al. (cond-mat 0303493) argue that the samples of La(2-x)Sr(x)CuO(4) where we find far-infrared peaks below 150 cm-1 (which suggest a charge stripe scenario) are not single crystals or are miscut. Here we show that the spectral feature on which this criticism is based was found both in floating-zone-grown crystals where the miscut was negligible, and in flux-grown crystals where the surface is intrinsically a-b. Further arguments are presented to support the validity of our data., Comment: 2 pages, 1 figure, submitted to PRL

Raman and Infrared (IR) spectra of an underdoped La_{1.90}Sr_{0.10}CuO_{4} single crystal have been measured as a function of temperature. Both techniques provide unconventional low-energy spectra. The IR conductivity exhibits features peaked at finite frequencies which do not have a counterpart in the Raman response. Below approximately 100 K a transfer of both Raman and IR spectral weight towards lower energies is found and a new component in the Raman response builds up being characterized by a very long lifetime of electrons propagating along the Cu-O bonds., Comment: 4 pages, 3 eps figures

The infrared absorption of charge density waves coupled to a magnetic background is first observed in two manganites La{1-x}Ca{x}MnO{3} with x = 0.5 and x = 0.67. In both cases a BCS-like gap 2 Delta (T), which for x=0.5 follows the hysteretic ferro-antiferromagnetic transition, fully opens at a finite T{0} < T{Neel}, with 2 Delta(T{0})/kT{c} close to 5. These results may also explain the unusual coexistence of charge ordering and ferromagnetism in La{0.5}Ca{0.5}MnO{3}., Comment: File revtex + 3 figs. in epsf. To appear on Phys. Rev. Lett