arXiv subjects

P. Lemmens

Publications and source records attributed to P. Lemmens.

At least 55 records · Page 3Linked to original sources

arXiv2007

Comment on "Raman spectroscopy study of NaxCoO2 and superconducting NaxCoO2 yH2O"

The effect of surface degradation of the thermolectric cobaltite on Raman spectra is discussed and compared to experimental results from Co3O4 single crystals. We conclude that on NaCl flux grown NaxCoO2 crystals a surface layer of Co3O4 easily forms that leads to the observation of an intense phonon around 700 cm-1 [Phys. Rev. B 70, 052502 (2004)]. Raman spectra on freshly cleaved crystals from optical floating zone ovens do not show such effects and have a high frequency phonon cut-off at approximately 600 cm -1 [Phys. Rev. Lett 96, 167204 (2006)]. We discuss the relation of structural dimensionality, electronic correlations and the high frequency phonon cut-off of the thermolectric cobaltite.

cond-mat.str-el↗

arXiv2006

Structural and magnetic dimers in the spin-gapped system CuTe2O5

We investigated the magnetic properties of the system CuTe2O5 by susceptibility and electron spin resonance measurements. The anisotropy of the effective g-factors and the ESR linewidth indicates that the anticipated structural dimer does not correspond to the singlet-forming magnetic dimer. Moreover, the spin susceptibility of CuTe2O5 can only be described by taking into account interdimer interactions of the same order of magnitude than the intradimer coupling. Analyzing the exchange couplings in the system we identify the strongest magnetic coupling between two Cu ions to be mediated by super-super exchange interaction via a bridging Te ligand, while the superexchange coupling between the Cu ions of the structural dimer only results in the second strongest coupling.

cond-mat.str-el↗

arXiv2006

Comparative investigation of the coupled-tetrahedra quantum spin systems Cu2Te2O5X2, X=Cl, Br and Cu4Te5O12Cl4

We present a comparative study of the coupled-tetrahedra quantum spin systems Cu2Te2O5X2, X=Cl, Br (Cu-2252(X)) and the newly synthesized Cu4Te5O12Cl4 (Cu-45124(Cl)) based on ab initio Density Functional Theory calculations. The magnetic behavior of Cu-45124(Cl) with a phase transition to an ordered state at a lower critical temperature T$_c$=13.6K than in Cu-2252(Cl) (T$_c$=18K) can be well understood in terms of the modified interaction paths. We identify the relevant structural changes between the two systems and discuss the hypothetical behavior of the not yet synthesized Cu-45124(Br) with an ab initio relaxed structure using Car-Parrinello Molecular Dynamics.

cond-mat.str-el↗

arXiv2006

Approaching the ground state of the kagome antiferromagnet

Y{0.5}$Ca{0.5}BaCo4O7 contains kagome layers of Co ions, whose spins are strongly coupled according to a Curie-Weiss temperature of -2200 K. At low temperatures, T = 1.2 K, our diffuse neutron scattering study with polarization analysis reveals characteristic spin correlations close to a predicted two-dimensional coplanar ground state with staggered chirality. The absence of three dimensional long-range AF order proves negligible coupling between the kagome layers. The scattering intensities are consistent with high spin S=3/2 states of Co2+ in the kagome layers and low spin S=0 states for Co3+ ions at interlayer sites. Our observations agree with previous Monte Carlo simulations indicating a ground state of only short range chiral order.

cond-mat.str-el↗

arXiv2006

Charge density waves in Sr_14-xCa_xCu_24O_41: electron correlations vs. structural effects

We report inelastic light scattering experiments in the spin-chain and ladder system Sr_14-xCa_xCu_24O_41. A depletion of an electronic background is observed for 0 < x < 5 at low temperatures and with light polarization both parallel to the leg and rung directions. This points to the formation of 2D charge density wave in the ladders. Furthermore, the Ca-substitution dependence of the 305- and 249-cm-1 modes, sensitive to the lattice modulations of the respective chain and ladder system, suggests that the charge dynamics in the ladders is strongly influenced by the structural incommensurability.

cond-mat.str-el↗

arXiv2006

Low temperature mixed spin state of Co3+ in LaCoO3 evidenced from Jahn-Teller lattice distortions

One- and multi-phonon excitations of the single crystalline LaCoO3 were studied using Raman spectroscopy in the temperature region of 5 K - 300 K. First-order Raman spectra show a larger number of phonon modes than allowed for the rhombohedral structure. Additional phonon modes are interpreted in terms of activated modes due to lattice distortions, arising from the Jahn-Teller (JT) activity of the intermediate-spin (IS) state of Co3+ ions. In particular, the 608-cm-1 stretching-type mode shows anomalous behavior in peak energy and scattering intensity as a function of temperature. The anomalous temperature dependence of the second-order phonon excitations spectra is in accordance with the Franck-Condon mechanism that is characteristic for a JT orbital order.

cond-mat.str-el↗

arXiv2005

Magnetic excitations and phonons in the spin-chain compound NaCu2O2

We report an inelastic light scattering study of single-crystalline NaCu$_2$O$_2$, a spin-chain compound known to exhibit a phase with helical magnetic order at low temperatures. Phonon excitations were studied as a function of temperature and light polarization, and the phonon frequencies are compared to the results of ab-initio lattice dynamical calculations, which are also reported here. The good agreement between the observed and calculated modes allows an assignment of the phonon eigenvectors. Two distinct high-energy two-magnon features as well as a sharp low-energy one-magnon peak were also observed. These features are discussed in terms of the magnon modes expected in a helically ordered state. Their polarization dependence provides evidence of substantial exchange interactions between two closely spaced spin chains within a unit cell. At high temperatures, the spectral features attributable to magnetic excitations are replaced by a broad, quasielastic mode due to overdamped spin excitations.

cond-mat.str-el↗

arXiv2005

Anomalous electronic Raman scattering in Na_xCoO_2 H_2O

Raman scattering experiments on Na_{x}CoO_2 yH_2O single crystals show a broad electronic continuum with a pronounced peak around 100 cm-1 and a cutoff at approximately 560 cm-1over a wide range of doping levels. The electronic Raman spectra in superconducting and non-superconducting samples are similar at room temperature, but evolve in markedly different ways with decreasing temperature. For superconducting samples, the low-energy spectral weight is depleted upon cooling below T* sim 150K, indicating a opening of a pseudogap that is not present in non-superconducting materials. Weak additional phonon modes observed below T* suggest that the pseudogap is associated with charge ordering.

cond-mat.str-el↗

arXiv2005

Hole stripe and orbital fluctuating state in LaMnO$_{3+δ}$ ($0.085\leq δ\leq0.125$) unveiled by Raman spectroscopy

Giant softening by 30 cm$^{-1}$ of the 490- and 620-cm$^{-1}$ modes is observed by Raman scattering measurements below the Curie temperature of single crystalline LaMnO$_{3+δ}$ ($0.085\leq δ\leq0.125$). A pseudogap-like electronic continuum and a Fano antiresonance at 144 cm$^{-1}$ appear below the charge ordering temperature. This gives evidence for the presence of an orbital fluctuating state and the formation of a hole stripe, respectively. This is further corroborated by a unstructured broadening and shifting of multiphonon features with increasing doping $δ$. Our study suggests the significance of double exchange mechanism in the charged ordered insulating state.

cond-mat.str-el↗

arXiv2005

Orbiton-mediated multi-phonon scattering in La$_{1-x}$Sr$_x$MnO$_3$

We report on Raman scattering measurements of single crystalline La$_{1-x}$Sr$_x$MnO$_3$ ($x$=0, 0.06, 0.09 and 0.125), focusing on the high frequency regime. We observe multi-phonon scattering processes up to fourth-order which show distinct features: (i) anomalies in peak energy and its relative intensity and (ii) a pronounced temperature-, polarization-, and doping-dependence. These features suggest a mixed orbiton-phonon nature of the observed multi-phonon Raman spectra.

cond-mat.str-el↗

arXiv2005

Study of intercalation and deintercalation of Na_xCoO_2 yH_2O single crystals

Single crystals of NaxCoO2 with beta-phase (x=0.55, 0.60 and 0.65), alpha'-phase (x=0.75) and alpha-phase (x=0.9, 1.0) have been grown by the floating zone technique. The Na-extraction and hydration were carried out for the alpha'-sample to get superconducting phase of NaxCoO2.yH2O (x~0.3, y~1.3). Hydrated single crystals exhibit cracked layers perpendicular to the c-axis due to a large expansion when the water is inserted into the structure. A study of intercalation/deintercalation was performed to determine the stability of the hydrated phase and effects of hydration on the structure of the compound. X-ray diffraction and Thermogravimetric experiments are used to monitor the process of water molecules accommodated in and removed from the crystal lattice. The initial intercalation process takes place with two-water molecules corresponding to y=0.6) inserted in a formula unit, followed by a group of four (y=1.3) to form a cluster of Na(H2O)4. Thermogravimetric analysis suggests that the deintercalation occurs with the removal of the water molecules one by one from the hydrated cluster at elevated temperatures of approximately 50, 100, 200 and 300 C, respectively. Our investigations reveal that the hydration process is dynamic and that water molecule inter- and deintercalation follow different reaction paths in an irreversible way.

cond-mat.str-el↗

arXiv2005

Spin gap formation in the quantum spin systems TiOX, X=Cl and Br

In the layered quantum spin systems TiOCl and TiOBr the magnetic susceptibility shows a very weak temperature dependence at high temperatures and transition-induced phenomena at low temperatures. There is a clear connection of the observed transition temperatures to the distortion of the octahedra and the layer separation. Band structure calculations point to a relation of the local coordinations and the dimensionality of the magnetic properties. While from magnetic Raman scattering only a small decrease of the magnetic exchange by -5-10% is derived comparing TiOCl with TiOBr, the temperature dependence of the magnetic susceptibility favors a much bigger change.

cond-mat.str-el↗

arXiv2005

Unusual criticality of Cu2Te2O5Br2 under pressure

We present measurements of the magnetic susceptibility chi(T) on Cu2Te2O5Br2 under externally applied pressure. From our data we extract the pressure response of the antiferromagnetic phase transition at T0 = 11.6 K and of the overall magnetic coupling strength. Our experiments indicate that with pressure the overall magnetic coupling strength increases by about 25% with applied pressure of only 8 kbar. In contrast, the phase transition temperature T0 is significantly suppressed and not observable anymore at a pressure of already 8.2 kbar.

cond-mat.other↗

arXiv2004

Phonon scattering and stability of Na_0.5CoO_2

Raman scattering experiments have been performed on Na_xCoO_2 as function of temperature at the composition x=0.5 where a structural instability and a metal-insulator transition have been observed. Three additional phonon modes are observed compared to samples with larger x. An in-situ annealing study (T_max=550 K) with the initial presence of water vapor at ambient conditions reveals an irreversible structural instability of this composition.

cond-mat.str-el↗

arXiv2004

Analysis of the phonon spectrum in the titanium oxyhalide TiOBr

We present the electrodynamic response of TiOBr, which undergoes a transition to a spin-singlet ground state for temperatures below T$_{C1}=28$ K. The temperature evolution of the phonon anomalies indicates, like in \cl, an extended fluctuation regime, extending well above T$_{C1}$. At low frequencies, the spectral weight is progressively suppressed by decreasing the temperature, suggesting the formation of a spin-gap and a considerable electron-phonon coupling. A comparison of the two oxyhalides shows a weaker interplane coupling and reduced dimensionality for TiOBr that enhances fluctuations and shifts the ordering temperatures to lower values. In the fluctuation regime the temperature dependencies of some phonon parameters track the temperature evolution of the magnetic susceptibility.

cond-mat.mtrl-sci↗

arXiv2004

Bulk antiferromagnetism in $\bf Na_{0.82}CoO_2$ single crystals

Susceptibility, specific heat, and muon spin rotation measurements on high-quality single crystals of $\rm Na_{0.82}CoO_2$ have revealed bulk antiferromagnetism with Néel temperature $\rm T_N = 19.8 \pm 0.1$ K and an ordered moment perpendicular to the $\rm CoO_2$ layers. The magnetic order encompasses nearly 100% of the crystal volume. The susceptibility exhibits a broad peak around 30 K, characteristic of two-dimensional antiferromagnetic fluctuations. The in-plane resistivity is metallic at high temperatures and exhibits a minimum at $\rm T_N$.

cond-mat.str-el↗

arXiv2004

The crystal growth and characterization of NaxCoO2 and NaxCoO2yH2O

A systematic study of NaxCoO2 (x=0.50 - 0.90) and NaxCoO2 yH(D)2O (x=0.26 - 0.42, y=1.3) has been performed to determine phase stability and the effect of hydration on the structural and superconducting properties of this system. We show that a careful control of the Na deintercalation process and hydration dynamics is possible in single crystals of this system. Furthermore, we give experimental evidence that the dependence of the superconducting transition temperature on Na content is much weaker than reported earlier. Implications of this effect for the understanding of the superconducting phase diagram are discussed.

cond-mat.supr-con↗

arXiv2004

Interplay of structural and electronic phase separation in single crystalline La(2)CuO(4.05) studied by neutron and Raman scattering

We report a neutron and Raman scattering study of a single-crystal of La(2)CuO(4.05) prepared by high temperature electrochemical oxidation. Elastic neutron scattering measurements show the presence of two phases, corresponding to the two edges of the first miscibility gap, all the way up to 300 K. An additional oxygen redistribution, driven by electronic energies, is identified at 250 K in Raman scattering (RS) experiments by the simultaneous onset of two-phonon and two-magnon scattering, which are fingerprints of the insulating phase. Elastic neutron scattering measurements show directly an antiferromagnetic ordering below a Néel temperature of T_N =210K. The opening of the superconducting gap manifests itself as a redistribution of electronic Raman scattering below the superconducting transition temperature, T_c = 24K. A pronounced temperature-dependent suppression of the intensity of the (100) magnetic Bragg peak has been detected below T_c. We ascribe this phenomenon to a change of relative volume fraction of superconducting and antiferromagnetic phases with decreasing temperature caused by a form of a superconducting proximity effect.

cond-mat.supr-con↗