arXiv subjects

P. Lemmens

Publications and source records attributed to P. Lemmens.

At least 37 records · Page 2Linked to original sources

arXiv2011

Tuning the spin dynamics of kagome systems

Despite the conceptional importance of realizing spin liquids in solid states only few compounds are known. On the other side the effect of lattice distortions and anisotropies on the magnetic exchange topology and the fluctuation spectrum are an interesting problem. We compare the excitation spectra of the two s=1/2 kagome lattice compounds volborthite and vesignieite using Raman scattering. We demonstrate that even small modifications of the crystal structure may have a huge effect on the phonon spectrum and low temperature properties.

cond-mat.str-el↗

arXiv2011

Helical fluctuations in the Raman response of the topological insulator Bi2Se3

The topological insulator Bi2Se3 shows a Raman scattering response related to topologically protected surface states amplified by a resonant interband transition. Most significantly this signal has a characteristic Lorentzian lineshape and spin-helical symmetry due to collision dominated scattering of Dirac states at the Fermi level E_F on bulk valence states. Its resonance energy, temperature and doping dependence points to a high selectivity of this process. Its scattering rate (Gamma=40 cm-1=5 meV) is comparable to earlier observations, e.g. in spin-polaron systems. Although the observation of topological surface states in Raman scattering is limited to resonance conditions, this study represents a quite clean case which is not polluted by symmetry forbidden contributions from the bulk

cond-mat.str-el↗

arXiv2011

Magnetic properties of the antiferromagnetic spin-1/2 chain system $β$-TeVO$_{4}$

The magnetic susceptibility and magnetization of high quality single crystal beta-TeVO4 are reported. We show that this compound, made of weakly coupled infinite chains of VO5 pyramids sharing corners, behaves as a S = 1/2 one-dimensional Heisenberg antiferromagnet. From magnetic experiments we deduce the intrachain antiferromagnetic coupling constant J/kB = 21.4 $\pm$ 0.2 K. Below 5 K a series of three phase transitions at 2.26, 3.28 and 4.65 K is observed.

cond-mat.str-el↗

arXiv2011

Anomalous low-energy phonons in nearly tetragonal BiFeO3 thin films

We present evidence for a concomitant structural and ferroelectric transformation around $T_S\sim 360$ K in multiferroic BiFeO$_3$/LaAlO$_3$ thin films close to the tetragonal phase. Phonon excitations are investigated by using Raman scattering as a function of temperature. The low-energy phonon modes at 180-260 cm$^{-1}$ related to the FeO$_6$ octahedron tilting show anomalous behaviors upon cooling through $T_S$; (i) a large hardening amounting to 15 cm$^{-1}$, (ii) an increase of intensity by one order of magnitude, and (iii) an appearance of a dozen new modes. In contrast, the high-frequency modes exhibit only weak anomalies. This suggests an intimate coupling of octahedron tilting to ferroelectricity leading to a simultaneous change of structural and ferroelectric properties.

cond-mat.str-el↗

arXiv2011

Magneto-structural transitions in a frustrated magnet at high fields

Ultrasound and magnetization studies of bond-frustrated ZnCr2S4 spinel are performed in static magnetic fields up to 18 T and in pulsed fields up to 62 T. At temperatures below the antiferromagnetic transition at T_N1 14 K the sound velocity as function of magnetic field reveals a sequence of steps followed by plateaus indicating a succession of crystallographic structures with constant stiffness. At the same time, the magnetization evolves continuously with field up to full magnetic polarization without any plateaus in contrast to geometrically frustrated chromium oxide spinels. The observed high-field magneto-structural states are discussed within a H-T phase diagram taking into account the field and temperature evolution of three coexisting spin structures and subsequent lattice transformations induced by magnetic field.

cond-mat.str-el↗

arXiv2011

Evidence for local lattice distortions in giant magnetocapacitive CdCr2S4

Raman scattering experiments on CdCr2S4 single crystals show pronounced anomalies in intensity and frequency of optical phonon modes with an onset temperature T*=130 K that coincides with the regime of giant magnetocapacitive effects. A loss of inversion symmetry and Cr off-centering are deduced from the observation of longitudinal optical and formerly infrared active modes for T<T_c=84 K. The intensity anomalies are attributed to the enhanced electronic polarizability of displacements that modulate the Cr-S distance and respective hybridization. Photo doping leads to an annihilation of the symmetry reduction. Our scenario of multiferroic effects is based on the near degeneracy of polar and nonpolar modes and the additional low energy scale due to hybridization.

cond-mat.str-el↗

arXiv2011

Interplay of Spin and Lattice Degrees of Freedom in the Frustrated Antiferromagnet CdCr_2O_4: High-field and Temperature Induced Anomalies of the Elastic Constants

Temperature and magnetic field studies of the elastic constants of the chromium spinel CdCr_2O_4 show pronounced anomalies related to strong spin-phonon coupling in this frustrated antiferromagnet. A detailed comparison of the longitudinal acoustic mode propagating along the [111] direction with theory based on an exchange-striction mechanism leads to an estimate of the strength of the magneto-elastic interaction. The derived spin-phonon coupling constant is in good agreement with previous determinations based on infrared absorption. Further insight is gained from intermediate and high magnetic field experiments in the field regime of the magnetization plateau. The role of the antisymmetric Dzyaloshinskii-Moriya interaction discussed and we compare the spin-phonon coupling in CdCr_2O_4 in both the ordered and disordered states.

cond-mat.str-el↗

arXiv2011

Anomalous optical phonons in FeTe pnictides: spin state, magnetic order, and lattice anharmonicity

Polarized Raman-scattering spectra of non-superconducting, single-crystalline FeTe are investigated as function of temperature. We have found a relation between the magnitude of ordered magnetic moments and the linewidth of A1g phonons at low temperatures. This relation is attributed to the intermediate spin state (S=1) and the orbital degeneracy of the Fe ions. Spin-phonon coupling constants have been estimated based on microscopic modeling using density-functional theory and analysis of the local spin density. Our observations show the importance of orbital degrees of freedom for the Fe-based superconductors with large ordered magnetic moments, while small magnetic moment of Fe ions in some iron pnictides reflects the low spin state of Fe ions in those systems.

cond-mat.str-el↗

arXiv2010

Dynamical Dzyaloshinsky-Moriya interaction in KCuF3: Raman evidence for an antiferrodistortive lattice instability

In the orbitally ordered, quasi-one dimensional Heisenberg antiferromagnet KCuF3 the low-energy Eg and B1g phonon modes show an anomalous softening (25% and 13%) between room temperature and the characteristic temperature T_S = 50 K. In this temperature range a freezing-in of F ion dynamic displacements is proposed to occur. In addition, the Eg mode at about 260 cm-1 clearly splits below T_S. The width of the phonon lines above T_S follows an activated behavior with an activation energy of about 50 K. Our observations clearly evidence a reduction of the structural symmetry below T_S and indicate a strong coupling of lattice and spin fluctuations for T>T_S.

cond-mat.str-el↗

arXiv2009

Stabilization of charge and orbital ordered states by antiferromagnetism in the A-site ordered YBaMn2O6

We report on Raman scattering measurements of the A-site ordered YBaMn2O6 in the wide temperature range of 10-650K. Upon cooling almost all phonon modes show pronounced temperature dependencies of frequency, linewidth, and scattering intensity. This suggests that the octahedra tilting, Mn-O bond angles and lengths vary with temperature in a concerted way. The remarkable feature is that the high-temperature metallic and the charge and orbital ordered (CO-OO) states coexist down to T_N=195K. In the antiferromagnetic state zone-folded modes are induced by the CO-OO superstructure and the phonon modes undergo an anomalous softening and narrowing. Our results evidence that the CO-OO state is stabilized by the spin ordering for temperatures below T_N.

cond-mat.str-el↗

arXiv2009

Self-energy effects and electron-phonon coupling in Fe-As superconductors

We report on Raman scattering experiments of the undoped SrFe2As2 and superconducting Sr0.85K0.15Fe2As2 (Tc=28K) and Ba0.72K0.28Fe2As2 (Tc=32K) single crystals. The frequency and linewidth of the B1g mode at 210 cm-1 exhibits an appreciable temperature dependence induced by the superconducting and spin density wave transitions. We give estimates of the electron-phonon coupling related to this renormalization. In addition, we observe a pronounced quasi-elastic Raman response for the undoped compound, suggesting persisting magnetic fluctuations to low temperatures. In the superconducting state the renormalization of an electronic continuum is observed with a threshold energy of 61cm-1.

cond-mat.supr-con↗

arXiv2009

Optical phonons, spin correlations, and spin-phonon coupling in the frustrated pyrochlore magnets CdCr2O4 and ZnCr2O4

We report on infrared, Raman, magnetic susceptibility, and specific heat measurements on CdCr2O4 and ZnCr2O4 single crystals. We estimate the nearest-neighbor and next-nearest neighbor exchange constants from the magnetic susceptibility and extract the spin-spin correlation functions obtained from the magnetic susceptibility and the magnetic contribution to the specific heat. By comparing with the frequency shift of the infrared optical phonons above TN , we derive estimates for the spin-phonon coupling constants in these systems. The observation of phonon modes which are both Raman and infrared active suggest the loss of inversion symmetry below the Neel temperature in CdCr2O4 in agreement with theoretical predictions by Chern and coworkers [Phys. Rev. B 74, 060405 (2006)]. In ZnCr2O4 several new modes appear below TN, but no phonon modes could be detected which are both Raman and infrared active indicating the conservation of inversion symmetry in the low temperature phase.

cond-mat.str-el↗

arXiv2009

Iron pnictides: Single crystal growth and effect of doping on structural, transport and magnetic properties

We demonstrate the preparation of large, free standing iron pnictide single crystals with a size up to 20 x 10 x 1 mm3 using solvents in zirconia crucibles under argon atmosphere. Transport and magnetic properties are investigated to study the effect of potassium doping on the structural and superconducting property of the compounds. The spin density wave (SDW) anomaly at Ts ~138 K in BaFe2As2 single crystals from self-flux shifts to Ts ~85 K due to Sn solvent growth. We show direct evidence for an incorporation of Sn on the Fe site. The electrical resistivity data show a sharp superconducting transition temperature Tc~38.5 K for the single crystal of Ba0.68K0.32Fe2As2. A nearly 100% shielding fraction and bulk nature of the superconductivity for the single crystal were confirmed by magnetic susceptibility data. A sharp transition Tc~25 K occurred for the single crystal of Sr0.85K0.15Fe2As2. There is direct evidence for a coexistence of the SDW and superconductivity in the low doping regime of Sr1-xKxFe2As2 single crystals. Structural implications of the doping effects as well as the coexistence of the two order parameters are discussed.

cond-mat.supr-con↗

arXiv2009

Spectral sensitive phonon wipeout due to a fluctuating spin state in a Fe2+ coordination polymer

Raman scattering in the spin-crossover system [Fe(pmd)(H2O){Au(CN)2}2]*H2O reveals a complex three-phase spin-state transition in contrast to earlier observations in magnetization measurements. We observe different spin state phases as function of temperature and electromagnetic radiation in the visible spectral range. There exists a fluctuating spin state phase with an unexpected wipeout of the low frequency phonon scattering intensity. Furthermore we observe one phase with reduced symmetry that is attributed to a cooperative Jahn-Teller effect. Pronounced electron-phonon interaction manifests itself as a strong Fano-resonance of phonons related to {FeN6} and {FeN4O2} coordination octahedra. Density functional theory supports this interpretation.

cond-mat.str-el↗

arXiv2008

Lattice and electronic anomalies of CaFe_2As_2 studied by Raman spectroscopy

We report inelastic light scattering experiments on CaFe_2As_2 in the temperature range of 4 to 290 K. In in-plane polarizations two Raman-active phonon modes are observed at 189 and 211 cm-1, displaying A_1g and B_1g symmetries, respectively. Upon heating through the tetragonal-to-orthorhombic transition at about T_S=173 K, the B_1g phonon undergoes a discontinuous drop of the frequency by 4 cm-1 whereas the A_1g phonon shows a suppression of the integrated intensity. Their linewidth increases strongly with increasing temperature and saturates above T_S. This suggests (i) a first-order structural phase transition and (ii) a drastic change of charge distribution within the FeAs plane through T_S.

cond-mat.supr-con↗

arXiv2008

Magnetic crossover and complex excitation spectrum of the ferromagnetic/antiferromagnetic spin-1/2 chain system alpha-TeVO4

We report magnetic susceptibility, specific heat, and Raman scattering investigations of alpha-TeVO4 containing V-O edge-sharing chains. These chains promote a system of ferromagnetic/antiferromagnetic spin-1/2 Heisenberg alternating exchange chains with pronounced spin frustration. The magnetic susceptibility and Raman scattering evidence a crossover at T* = 85 K with different slopes of the reciprocal susceptibility and a magnetic phase transition into a long-range-ordered state at Tc = 16 K. From Raman scattering data a strong mutual coupling between lattice and magnetic degrees of freedom is deduced. A comparison to model calculations and prior Raman scattering on other chain systems yield a plausible interpretation of the microscopic mechanism for the crossover behavior.

cond-mat.str-el↗

arXiv2008

Microscopic Evidence of Spin State Order and Spin State Phase Separation in Layered Cobaltites RBaCo2O5.5 with R=Y, Tb, Dy, and Ho

We report muon spin relaxation measurements on the magnetic structures of RBaCo_2O_5.5 with R=Y, Tb, Dy, and Ho. Three different phases, one ferrimagnetic and two antiferromagnetic, are identified below 300 K. They consist of different ordered spin state arrangements of high-, intermediate-, and low-spin Co^3+ of CoO_6 octahedra. Phase separation into well separated regions with different spin state order is observed in the antiferromagnetic phases. The unusual strongly anisotropic magnetoresistance and its onset at the FM-AFM phase boundary is explained.

cond-mat.str-el↗

arXiv2008

Electron-phonon interaction in the lamellar cobaltate Na$_x$CoO$_2$

We study theoretically and experimentally the dependence of the electron-phonon interaction in Na$_x$CoO$_2$ on the sodium concentration $x$. For the two oxygen phonon modes found in Raman experiments, $A_{1g}$ and $E_{1g}$, we calculate the matrix elements of the electron-phonon interaction. Analyzing the feedback effect of the conduction electrons on the phonon frequency we compare the calculated and experimentally observed doping dependence of the $A_{1g}$ mode. Furthermore, due to the momentum dependence of the electron-phonon coupling for the $E_{1g}$ symmetry we find no renormalization of the corresponding phonon frequency which agrees with experiment. Our results shed light on the possible importance of the electron-phonon interaction in this system.

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