arXiv subjects

L. Baldassarre

Publications and source records attributed to L. Baldassarre.

At least 19 recordsLinked to original sources

arXiv2015

Optical properties of V2O3 in its whole phase diagram

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.

cond-mat.str-el↗

arXiv2015

Pressure dependent relaxation in the photo-excited Mott insulator ETF2TCNQ: Influence of hopping and correlations on quasiparticle recombination rates

Femtosecond relaxation of photo-excited quasiparticles in the one dimensional Mott insulator ET-F2TCNQ are measured as a function of external pressure, which is used to tune the electronic structure. By fitting the static optical properties and measuring femtosecond decay times at each pressure value, we correlate the relaxation rates with the electronic bandwidth t and on the intersite correlation energy V. The scaling of relaxation times with microscopic parameters is different than for metals and semiconductors. The competition between localization and delocalization of the Mott-Hubbard exciton dictates the efficiency of the decay, as exposed by a fit based on the solution of the time-dependent extended Hubbard Hamiltonian.

cond-mat.str-el↗

arXiv2014

Infrared phonon spectrum of the tetragonal helimagnet Ba$_2$CuGe$_2$O$_7$

The lattice dynamics of Ba$_2$CuGe$_2$O$_7$, a compound which develops Dzyaloshinsky-Moriya (DM) helical magnetism below $T_N$ = 3.2 K, has been studied by measuring the infrared reflectivity of a single crystal with the radiation polarized both in the $ab$ plane and along the $c$ axis of its tetragonal cell, from 7 K to 300 K. In this compound, where the unit cell has no inversion symmetry, fourteen $E$ phonon modes of the $ab$ plane, out of the eighteen predicted, and all the ten $B_2$ modes of the $c$ axis, have been observed. They have been assigned to the atomic motions by a comparison with shell-model calculations, which provided vibrational frequencies in good agreement with the experiment, while most calculated intensities turned to be much lower than the experimental values. This discrepancy has been tentatively explained by assuming strong electron-phonon interactions, a hypothesis supported by the failure of the $f$- sum rule if restricted to the phonon region. Indeed, we observe a remarkable increase in the oscillator strengths at $T$'s low but higher than $T_N$, which suggests that the dielectric constant of Ba$_2$CuGe$_2$O$_7$ may increase at those temperatures.

cond-mat.mtrl-sci↗

arXiv2014

Evolution of optical properties of chromium spinels CdCr$_2$O$_4$, HgCr$_2$S$_4$, and ZnCr$_2$Se$_4$ under high pressure

We report pressure-dependent reflection and transmission measurements on ZnCr$_2$Se$_4$, HgCr$_2$S$_4$, and CdCr$_2$O$_4$ single crystals at room temperature over a broad spectral range 200-24000 cm$^{-1}$. The pressure dependence of the phonon modes and the high-frequency electronic excitations indicates that all three compounds undergo a pressure-induced structural phase transition with the critical pressure 15 GPa, 12 GPa, and 10 GPa for CdCr$_2$O$_4$, HgCr$_2$S$_4$, and ZnCr$_2$Se$_4$, respectively. The eigenfrequencies of the electronic transitions are very close to the expected values for chromium crystal-field transitions. In the case of the chalcogenides pressure induces a red shift of the electronic excitation which indicates a strong hybridization of the Cr d-bands with the chalcogenide bands.

cond-mat.mtrl-sci↗

arXiv2013

A combined experimental and computational study of the pressure dependence of the vibrational spectrum of solid picene C_22H_14

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 ($γ_p=0.1$) is much lower than the effective value ($γ_d=0.8$) 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.

cond-mat.supr-con↗

arXiv2013

Electrodynamics of BaFe2As2 from infrared measurements under pressure

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.

cond-mat.str-el↗

arXiv2012

Pressure dependence of the Verwey transition in magnetite: an infrared spectroscopic point of view

We investigated the electronic and vibrational properties of magnetite at temperatures from 300 K down to 10 K and for pressures up to 10 GPa by far-infrared reflectivity measurements. The Verwey transition is manifested by a drastic decrease of the overall reflectance and the splitting of the phonon modes as well as the activation of additional phonon modes. In the whole studied pressure range the down-shift of the overall reflectance spectrum saturates and the maximum number of phonon modes is reached at a critical temperature, which sets a lower bound for the Verwey transition temperature T$_{\mathrm{v}}$. Based on these optical results a pressure-temperature phase diagram for magnetite is proposed.

cond-mat.str-el↗

arXiv2012

Optical conductivity of Bismuth-based topological insulator

The optical conductivity and the spectral weight of four topological insulators with increasing chemical compensation (Bi2Se3, Bi2-xCaxSe3, Bi2Se2Te, Bi2Te2Se) have been measured from 5 to 300 K and from sub-THz to visible frequencies. The effect of compensation is clearly observed in the infrared spectra, through the suppression of an extrinsic Drude term and the appearance of strong absorption peaks, that we assign to electronic transitions among localized states. From the far-infrared spectral weight of the most compensated sample (Bi2Te2Se) one can estimate a density of charge-carriers in the order of 10^17/cm^3 in good agreement with transport data. Those results demonstrate that the low-energy electrodynamics in single crystals of topological insulators, even at the highest degree of compensation presently achieved, is still affected by extrinsic charge excitations.

cond-mat.mtrl-sci↗

arXiv2012

Universal conductivity and the electrodynamics of graphite at high pressures

We address the in-plane pressure-dependent electrodynamics of graphite through synchrotron based infrared spectroscopy and ab initio Density Functional Theory calculations. The Drude term remarkably increases upon pressure application, as a consequence of an enhancement of both electron and hole charge densities. This is due to the growth of the band dispersion along the k_z direction between the K and H points of the Brillouin zone. On the other hand, the mid-infrared optical conductivity between 800 and 5000 cm-1 is almost flat, and very weakly pressure dependent, at least up to 7 GPa. This demonstrates a surprising robustness of the graphene-like universal quantum conductance of graphite, even when the interlayer distance is significantly reduced.

cond-mat.mtrl-sci↗

arXiv2012

Polaron physics and crossover transition in magnetite probed by pressure-dependent infrared spectroscopy

The optical properties of magnetite at room temperature were studied by infrared reflectivity measurements as a function of pressure up to 8 GPa. The optical conductivity spectrum consists of a Drude term, two sharp phonon modes, a far-infrared band at around 600 cm$^{-1}$, and a pronounced mid-infrared absorption band. With increasing pressure both absorption bands shift to lower frequencies and the phonon modes harden in a linear fashion. Based on the shape of the MIR band, the temperature dependence of the dc transport data, and the occurrence of the far-infrared band in the optical conductivity spectrum the polaronic coupling strength in magnetite at room temperature should be classified as intermediate. For the lower-energy phonon mode an abrupt increase of the linear pressure coefficient occurs at around 6 GPa, which could be attributed to minor alterations of the charge distribution among the different Fe sites.

cond-mat.str-el↗

arXiv2012

Vibrational spectrum of solid picene (C_22H_14)

Recently, Mitsuhashi et al., have observed superconductivity with transition temperature up to 18 K in potassium doped picene (C22H14), a polycyclic aromatic hydrocarbon compound [Nature 464 (2010) 76]. Theoretical analysis indicate the importance of electron-phonon coupling in the superconducting mechanisms of these systems, with different emphasis on inter- and intra-molecular vibrations, depending on the approximations used. Here we present a combined experimental and ab-initio study of the Raman and infrared spectrum of undoped solid picene, which allows us to unanbiguously assign the vibrational modes. This combined study enables the identification of the modes which couple strongly to electrons and hence can play an important role in the superconducting properties of the doped samples.

cond-mat.mtrl-sci↗

arXiv2010

Optical Properties of (SrMnO3)n/(LaMnO3)2n superlattices: an insulator-to-metal transition observed in the absence of disorder

We measure the optical conductivity of (SrMnO3)n/(LaMnO3)2n superlattices (SL) for n=1,3,5, and 8 and 10 < T < 400 K. Data show a T-dependent insulator to metal transition (IMT) for n \leq 3, driven by the softening of a polaronic mid-infrared band. At n = 5 that softening is incomplete, while at the largest-period n=8 compound the MIR band is independent of T and the SL remains insulating. One can thus first observe the IMT in a manganite system in the absence of the disorder due to chemical doping. Unsuccessful reconstruction of the SL optical properties from those of the original bulk materials suggests that (SrMnO3)n/(LaMnO3)2n heterostructures give rise to a novel electronic state.

cond-mat.mtrl-sci↗

arXiv2010

A Microscopic View on the Mott transition in Chromium-doped V2O3

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.

cond-mat.str-el↗

arXiv2010

Far infrared properties of the rare-earth scandate DyScO3

We present reflectance measurements in the infrared region on a single crystal the rare earth scandate DyScO3. Measurements performed between room temperature and 10 K allow to determine the frequency of the infrared-active phonons, never investigated experimentally, and to get information on their temperature dependence. A comparison with the phonon peak frequency resulting from ab-initio computations is also provided. We finally report detailed data on the frequency dependence of the complex refractive index of DyScO3 in the terahertz region, which is important in the analysis of terahertz measurements on thin films deposited on DyScO3.

cond-mat.mtrl-sci↗

arXiv2010

Multi-gap superconductivity in a BaFe1.84Co0.16As2 film from optical measurements at terahertz frequencies

We measured the THz reflectance properties of a high quality epitaxial thin film of the Fe-based superconductor BaFe$_{1.84}$Co$_{0.16}$As$_2$ with T$_c$=22.5 K. The film was grown by pulsed laser deposition on a DyScO$_3$ substrate with an epitaxial SrTiO$_3$ intermediate layer. The measured $R_S/R_N$ spectrum, i.e. the reflectivity ratio between the superconducting and normal state reflectance, provides clear evidence of a superconducting gap $Δ_A$ close to 15 cm$^{-1}$. A detailed data analysis shows that a two-band, two-gap model is absolutely necessary to obtain a good description of the measured $R_S/R_N$ spectrum. The low-energy $Δ_A$ gap results to be well determined ($Δ_A$=15.5$\pm$0.5 cm$^{-1}$), while the value of the high-energy gap $Δ_B$ is more uncertain ($Δ_B$=55$\pm$7 cm$^{-1}$). Our results provide evidence of a nodeless isotropic double-gap scenario, with the presence of two optical gaps corresponding to 2$Δ/kT_c$ values close to 2 and 7.

cond-mat.supr-con↗

arXiv2010

Metal-insulator transition in NiS$_{2-x}$Se$_x$

The origin of the gap in NiS2 as well as the pressure- and doping-induced metal-insulator transition in the NiS2-xSex solid solutions are investigated both theoretically using the first-principles band structures combined with the dynamical mean-field approximation for the electronic correlations and experimentally by means of infrared and x-ray absorption spectroscopies. The bonding-antibonding splitting in the S-S (Se-Se) dimer is identified as the main parameter controlling the size of the charge gap. The implications for the metal-insulator transition driven by pressure and Se doping are discussed.

cond-mat.str-el↗

arXiv2009

Far-infrared absorption and the metal-to-insulator transition in hole-doped cuprates

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.

cond-mat.supr-con↗

arXiv2009

Magnetic order induced crystal symmetry lowering in ACr$_2$O$_4$ ferrimagnetic spinels

We demonstrate that the onset of complex spin orders in ACr$_2$O$_4$ spinels with magnetic A$=$Co, Fe and Cu ions lowers the lattice symmetry. This is clearly indicated by the emergence of anisotropic lattice dynamics -- as evidenced by the pronounced phonon splittings -- even when experiments probing static distortions fail. We show that the crystal symmetry in the magnetic phase is reduced from tetragonal to orthorhombic for FeCr$_2$O$_4$ and CuCr$_2$O$_4$ with Jahn-Teller active A-site ions. The conical spin structure in FeCr$_2$O$_4$ is also manifested in the phonon frequencies. In contrast, the multiferroic CoCr$_2$O$_4$ with no orbital degrees of freedom remains nearly cubic in its ground state.

cond-mat.str-el↗