Cooperative dynamics in doped manganite films: phonon anomalies in the ferromagnetic state

We present optical measurements of phononic excitations in La$_{2/3}$Ca$_{1/3}$MnO$_{3}$ (LCMO) and La$_{2/3}$Sr$_{1/3}$MnO$_{3}$ (LSMO) thin films covering the full temperature range from the metallic ferromagnetic to the insulating paramagnetic phase. All eight phonons expected for the R$\bar{3}$c symmetry in LSMO and 17 out of the expected 25 phonons for the Pnma symmetry in LCMO have been determined. Close to the ferromagnetic-to-paramagnetic transition both compounds reveal an anomalous behavior but with different characteristics. Anomalies in the phononic spectra are a manifestation of the coupling of lattice degrees of freedom (DOF) to electronic DOF. Specifically, the low-frequency external group proves to be an indicator for lattice modifications induced by electronic correlations. The enhanced electron-phonon coupling in LCMO is responsible for Fano-like interference effects of distinct phonon modes with electronic continuum excitations: we observe asymmetric phonon line shapes, mode splitting and spectral weight transfer between modes.Comment: 10 pages, 10 figure

Large and Small Polaron Excitations in La2/3(Sr/Ca)1/3MnO3 Films

We present detailed optical measurements of the mid-infrared (MIR) excitations in thin films of La2/3Sr1/3MnO3 (LSMO) and La2/3Ca1/3MnO3 (LCMO) across the magnetic transition. The shape of the excitation at about 0.2 eV in both samples is analyzed in terms of polaron models. We propose to identify the MIR resonance in LSMO as the excitation of large polarons and that in LCMO as a small polaron excitation. A scaling behavior for the low-energy side of the polaronic MIR resonance in LSMO is established

Spin-phonon coupling in antiferromagnetic chromium spinels

The temperature dependence of eigenfrequencies and intensities of the IR active modes has been investigated for the antiferromagnetic chromium spinel compounds CdCr2O4, ZnCr2O4, ZnCr2S4, ZnCr2Se4, and HgCr2S4 by IR spectroscopy for temperatures from 5 K to 300 K. At the transition into the magnetically ordered phases, and driven by spin-phonon coupling, most compounds reveal significant splittings of the phonon modes. This is true for geometrically frustrated CdCr2O4, and ZnCr2O4, for bond frustrated ZnCr2S4 and for ZnCr2Se4, which also is bond frustrated, but dominated by ferromagnetic exchange. The pattern of splitting is different for the different compounds and crucially depends on the nature of frustration and of the resulting spin order. HgCr2S4, which is almost ferromagnetic, exhibits no splitting of the eigenfrequencies, but shows significant shifts due to ferromagnetic spin fluctuations.Comment: 15 pages, 6 figure

Coupling of phonons and electromagnons in GdMnO_3

The infrared and Terahertz properties of GdMnO_3 have been investigated as function of temperature and magnetic field, with special emphasis on the phase boundary between the incommensurate and the canted antiferromagnetic structures. The heterogeneous incommensurate phase reveals strong magnetodielectric effects, characterized by significant magnetoelectric contributions to the static dielectric permittivity and by the existence of electrically excited magnons (electromagnons). In the commensurate canted antiferromagnetic phase the magnetoelectric contributions to the dielectric constant and electromagnons are suppressed. The corresponding spectral weight is transferred to the lowest lattice vibration demonstrating the strong coupling of phonons with electromagnons.Comment: 5 pages, 4 figure

Electronic and phonon excitations in {\alpha}-RuCl3_3

We report on THz, infrared reflectivity and transmission experiments for wave numbers from 10 to 8000 cm$^{-1}$ ($\sim$ 1 meV - 1 eV) and for temperatures from 5 to 295 K on the Kitaev candidate material {\alpha}-RuCl$_3$. As reported earlier, the compound under investigation passes through a first-order structural phase transition, from a monoclinic high-temperature to a rhombohedral low-temperature phase. The phase transition shows an extreme and unusual hysteretic behavior, which extends from 60 to 166 K. In passing this phase transition, in the complete frequency range investigated we found a significant reflectance change, which amounts almost a factor of two. We provide a broadband spectrum of dielectric constant, dielectric loss and optical conductivity from the THz to the mid infrared regime and study in detail the phonon response and the low-lying electronic density of states. We provide evidence for the onset of an optical energy gap, which is of order 200 meV, in good agreement with the gap derived from measurements of the DC electrical resistivity. Remarkably, the onset of the gap exhibits a strong blue shift on increasing temperatures.Comment: 18 pages, 7 figure

On Pebble Automata for Data Languages with Decidable Emptiness Problem

In this paper we study a subclass of pebble automata (PA) for data languages for which the emptiness problem is decidable. Namely, we introduce the so-called top view weak PA. Roughly speaking, top view weak PA are weak PA where the equality test is performed only between the data values seen by the two most recently placed pebbles. The emptiness problem for this model is decidable. We also show that it is robust: alternating, nondeterministic and deterministic top view weak PA have the same recognition power. Moreover, this model is strong enough to accept all data languages expressible in Linear Temporal Logic with the future-time operators, augmented with one register freeze quantifier.Comment: An extended abstract of this work has been published in the proceedings of the 34th International Symposium on Mathematical Foundations of Computer Science (MFCS) 2009}, Springer, Lecture Notes in Computer Science 5734, pages 712-72

Unusual Non-Fermi Liquid Behavior of Ce1−x_{1-x}Lax_{x}Ni9_{9}Ge4_4 Analyzed in a Single Impurity Anderson Model with Crystal Field Effects

CeNi$_{9}$Ge$_4$ exhibits unusual non-Fermi liquid behavior with the largest ever recorded value of the electronic specific heat $\Delta C/T \cong 5.5$ JK$^{-2}$mol$^{-1}$ without showing any evidence of magnetic order. Specific heat measurements show that the logarithmic increase of the Sommerfeld coefficient flattens off below 200 mK. In marked contrast, the local susceptibility $\Delta\chi$ levels off well above 200 mK and already becomes constant below 1 K. Furthermore, the entropy reaches 2$R$ln2 below 20 K corresponding to a four level system. An analysis of $C$ and $\chi$ was performed in terms of an $SU(N=4)$ single impurity Anderson model with additional crystal electric field (CEF) splitting. Numerical renormalization group calculations point to a possible consistent description of the different low temperature scales in $\Delta c$ and $\Delta \chi$ stemming from the interplay of Kondo effect and crystal field splitting.Comment: 2 pages, 2 figure

Correlation between magnetic and transport properties of phase separated La0.5_{0.5}Ca0.5_{0.5}MnO3_{3}

The effect of low magnetic fields on the magnetic and electrical transport properties of polycrystalline samples of the phase separated compound La$_{0.5}$Ca$_{0.5}$MnO$_{3}$ is studied. The results are interpreted in the framework of the field induced ferromagnetic fraction enlargement mechanism. A fraction expansion coefficient af, which relates the ferromagnetic fraction f with the applied field H, was obtained. A phenomenological model to understand the enlargement mechanism is worked out.Comment: 3 pages, 3 figures, presented at the Fifth LAW-MMM, to appear in Physica B, Minor change

Broadband dielectric response of CaCu3Ti4O12: From dc to the electronic transition regime

We report on phonon properties and electronic transitions in CaCu3Ti4O12, a material which reveals a colossal dielectric constant at room temperature without any ferroelectric transition. The results of far- and mid-infrared measurements are compared to those obtained by broadband dielectric and millimeter-wave spectroscopy on the same single crystal. The unusual temperature dependence of phonon eigenfrequencies, dampings and ionic plasma frequencies of low lying phonon modes are analyzed and discussed in detail. Electronic excitations below 4 eV are identified as transitions between full and empty hybridized oxygen-copper bands and between oxygen-copper and unoccupied Ti 3d bands. The unusually small band gap determined from the dc-conductivity (~200 meV) compares well with the optical results.Comment: 7 pages, 8 figure