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A. Loidl

Publications and source records attributed to A. Loidl.

At least 199 records · Page 11Linked to original sources
arXiv2007

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.

cond-mat.str-el↗
arXiv2007

Polar phonons and spin-phonon coupling in HgCr2S4 and CdCr2S4

Polar phonons of HgCr2S4 and CdCr2S4 are studied by far-infrared spectroscopy as a function of temperature and external magnetic field. Eigenfrequencies, damping constants, effective plasma frequencies and Lyddane-Sachs-Teller relations, and effective charges are determined. Ferromagnetic CdCr2S4 and antiferromagnetic HgCr2S4 behave rather similar. Both compounds are dominated by ferromagnetic exchange and although HgCr2S4 is an antiferromagnet, no phonon splitting can be observed at the magnetic phase transition. Temperature and magnetic field dependence of the eigenfrequencies show no anomalies indicating displacive polar soft mode behavior. However, significant effects are detected in the temperature dependence of the plasma frequencies indicating changes in the nature of the bonds and significant charge transfer. In HgCr2S4 we provide experimental evidence that the magnetic field dependence of specific polar modes reveal shifts exactly correlated with the magnetization showing significant magneto-dielectric effects even at infrared frequencies.

cond-mat.str-el↗
arXiv2007

Terahertz spectroscopy of electromagnons in Eu_{1-x}Y_xMnO_3

Dielectric permittivity spectra of yttrium-doped EuMnO$_3$ in the composition range 0 =< x =< 0.5 have been investigated in the terahertz frequency range. Magnetoelectric contributions to the permittivity were observed in all compositions for ac electric fields parallel to the crystallographic a-axis. Well defined electromagnons exist for x >= 0.2 close to ν~ 20 cm^{-1} and with dielectric strength strongly increasing on doping. In addition to electromagnons, a broad contribution of magnetoelectric origin is observed for all compositions. For Eu_{0.8}Y_{0.2}MnO_3 the electromagnons can be suppressed by external magnetic fields which induce a canted antiferromagnetic phase. Magnetoelectric effects in the different doping regimes are discussed in detail.

cond-mat.str-el↗
arXiv2007

Broadband dielectric spectroscopy on single-crystalline and ceramic CaCu3Ti4O12

We present dielectric measurements of the colossal dielectric constant material CaCu3Ti4O12 extending up to 1.3 GHz also covering so far only rarely investigated single crystalline samples. Special emphasis is put on the second relaxation reported in several works on polycrystals, which we detect also in single crystals. For polycrystalline samples we provide a recipe to achieve values of the dielectric constant as high as in single crystals.

cond-mat.mtrl-sci↗
arXiv2007

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.

cond-mat.str-el↗
arXiv2006

Broadband dielectric spectroscopy and aging of glass formers

We present the results of aging experiments on a variety of glass formers, including xylitol, glycerol, propylene carbonate, and [Ca(NO3)2]0.4[KNO3]0.6 (CKN). In addition, broadband dielectric spectra of xylitol and CKN are provided. We demonstrate that, irrespective of which dielectric quantities (dielectric constant, loss and modulus) are analyzed, and irrespective of the spectral region where they have been measured, the aging-time dependence always is governed by the structural rearrangements constituting the alpha-relaxation. If the time dependence of the structural relaxation time during aging is taken into account, relaxation times and stretching parameters, fully consistent with equilibrium data, are obtained. In CKN, both the structural relaxation time and the strongly decoupled conductivity relaxation time are deduced from the same dielectric aging experiment.

cond-mat.dis-nn↗
arXiv2006

7Li NMR, magnetic susceptibility, and heat capacity studies on the triangular lattice system LiCrO2

We report 7Li NMR, magnetic susceptibility, and heat capacity measurements on the triangular lattice Heisenberg antiferromagnet compound LiCrO2. We find that in contrast to NaCrO2, magnetic properties of LiCrO2 have a more pronounced three dimensional character with sharp anomalies in the temperature variation of the 7Li NMR intensity and the NMR spin-lattice relaxation rate 1/T1. From heat capacity measurements we find that the total entropy related to the magnetic transition is in agreement with expectations. However, we find a significant contribution to the magnetic entropy in the range from the ordering temperature T_N to nearly 4T_N. This suggests the existence of magnetic correlations at temperatures well above T_N which might be due to the frustrated nature of the system. Based on the temperature dependence of 1/T1, we discuss the possible occurrence of a Kosterlitz-Thouless-Berezinskii transition taking place at T_KTB = 55 K in LiCrO2. Lithium depletion has no significant effect on the magnetic properties and the behaviour of Li0.5CrO2 is nearly unchanged from that of LiCrO2.

cond-mat.str-el↗
arXiv2006

Spin-phonon coupling in ZnCr2Se4

Spin-phonon coupling and magnetodielectric effects of ZnCr2Se4 were investigated by means of infrared (IR) spectroscopy as a function of temperature and magnetic field. ZnCr2Se4 is dominated by ferromagnetic exchange but undergoes antiferromagnetic order at T = 21 K. In the magnetically ordered phase the low-frequency IR active phonon splits, indicating strong dynamic anisotropy via magnetic exchange interactions. Antiferromagnetic order and concomitantly the phonon splitting is wiped out by external magnetic fields. Hence, ZnCr2Se4 is a prominent example of a spin-driven Jahn-Teller effect which can be fully suppressed in external magnetic fields.

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

Multiferroicity and colossal magneto-capacitance in Cr-thiospinels

The sulfur based Cr-spinels RCr2S4 with R = Cd and Hg exhibit the coexistence of ferromagnetic and ferroelectric properties together with a pronounced magnetocapacitive coupling. While in CdCr2S4 purely ferromagnetic order is established, in HgCr2S4 a bond-frustrated magnetic ground state is realized, which, however, easily can be driven towards a ferromagnetic configuration in weak magnetic fields. This paper shall review our recent investigation for both compounds. Besides the characterization of the magnetic properties, the complex dielectric permittivity was studied by means of broadband dielectric spectroscopy as well as measurements of polarization hysteresis and pyro-currents. The observed colossal magneto-capacitive effect at the magnetic transition seems to be driven by an enormous variation of the relaxation dynamics.

cond-mat.str-el↗
arXiv2006

Colossal magnetostriction and negative thermal expansion in the frustrated antiferromagnet ZnCr2Se4

A detailed investigation of ZnCr2Se4 is presented which is dominated by strong ferromagnetic exchange but orders antiferromagnetically at T_N = 21 K. Specific heat C and thermal expansion Delta L/L exhibit sharp first-order anomalies at the antiferromagnetic transition. T_N is strongly reduced and shifted to lower temperatures by external magnetic fields and finally is fully suppressed suggesting a field induced quantum critical behavior close to 60 kOe. Delta L/L(T) is unusually large and exhibits negative thermal expansion below 75 K down to T_N indicating strong frustration of the lattice. Magnetostriction Delta L/L(H) reveals colossal values (0.5x10^{-3}) comparable to giant magnetostriction materials. Electron-spin resonance, however, shows negligible spin-orbital coupling excluding orbitally induced Jahn-Teller distortions. The obtained results point to a spin-driven origin of the structural instability at T_N explained in terms of competing ferromagnetic and antiferromagnetic exchange interactions yielding strong bond frustration.

cond-mat.mtrl-sci↗
arXiv2006

Apparent giant dielectric constants, dielectric relaxation, and ac-conductivity of hexagonal perovskites La1.2Sr2.7BO7.33 (B = Ru, Ir)

We present a thorough dielectric investigation of the hexagonal perovskites La1.2Sr2.7IrO7.33 and La1.2Sr2.7RuO7.33 in a broad frequency and temperature range, supplemented by additional infrared measurements. The occurrence of giant dielectric constants up to 10^5 is revealed to be due to electrode polarization. Aside of dc and ac conductivity contributions, we detect two intrinsic relaxation processes that can be ascribed to ionic hopping between different off-center positions. In both materials we find evidence for charge transport via hopping of localized charge carriers. In the infrared region, three phonon bands are detected, followed by several electronic excitations. In addition, these materials provide further examples for the occurrence of a superlinear power law in the broadband ac conductivity, which recently was proposed to be a universal feature of all disordered matter.

cond-mat.str-el↗
arXiv2006

Spin-driven Phonon Splitting in Bond-frustrated ZnCr2S4

Utilizing magnetic susceptibility, specific heat, thermal expansion and IR spectroscopy we provide experimental evidence that the two subsequent antiferromagnetic transitions in ZnCr_2S_4 at T_N1 = 15 K and T_N2= 8 K are accompanied by significant thermal and phonon anomalies. The anomaly at T_N2 reveals a strong temperature hysteresis typical for a first-order transformation. Due to strong spin-phonon coupling both magnetic phase transitions induce a splitting of phonon modes, where at T_N1 the high-frequency and at T_N2 the low-frequency modes split. The anomalies and phonon splitting observed at T_N2 are strongly suppressed by magnetic field. Regarding the small positive Curie-Weiss temperature Theta= 8 K, we argue that this scenario of two different magnetic phases with concomitant different magneto-elastic couplings results from the strong competition of ferromagnetic and antiferromagnetic exchange of equal strength.

cond-mat.str-el↗
arXiv2006

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.

cond-mat.str-el↗
arXiv2006

Scaling of THz-conductivity at metal-insulator transition in doped manganites

Magnetic field and temperature dependence of the Terahertz conductivity and permittivity of the colossal magnetoresistance manganite Pr_{0.65}Ca_{0.28}Sr_{0.07}MnO_3 (PCSMO) is investigated approaching the metal-to-insulator transition (MIT) from the insulating side. In the charge-ordered state of PCSMO both conductivity and dielectric permittivity increase as function of magnetic field and temperature. Universal scaling relationships between the changes in permittivity and conductivity are observed in a broad range of temperatures and magnetic fields. Similar scaling is also seen in La_{1-x}Sr_xMnO_3 for different doping levels. The observed proportionality points towards the importance of pure ac-conductivity and phononic energy scale at MIT in manganites.

cond-mat.str-el↗
arXiv2006

Experimental evidence for competition of antiferromagnetic and ferromagnetic correlations in HgCr2S4

A detailed study of poly- and single crystalline samples of the normal spinel HgCr2S4 is reported. The structural refinement reveals enhanced values of the atomic displacements suggesting closeness to a structural instability. Magnetization, electron-spin resonance and specific-heat studies document strong ferromagnetic fluctuations close to 50 K and the occurrence of complex antiferromagnetic order at TN = 22 K. We found highly unconventional behavior resembling properties of a non-collinear antiferromagnet and soft ferromagnet dependent on temperature and magnetic field. Even weak external magnetic fields disturb the antiferromagnetic order and strongly enhance the ferromagnetic correlations. The conductivity shows an insulating character with non-monotonous temperature behavior and a metal-to-insulator like transition at 80 K well above the magnetic transition. The observed anomalies are related to bond frustration due to competing magnetic exchange interactions between the Cr ions.

cond-mat.mtrl-sci↗
arXiv2006

The multiferroic phases of (Eu:Y)MnO3

We report on structural, magnetic, dielectric, and thermodynamic properties of (Eu:Y)MnO3 for Y doping levels 0 <= x < 1. This system resembles the multiferroic perovskite manganites RMnO3 (with R= Gd, Dy, Tb) but without the interference of magnetic contributions of the 4f-ions. In addition, it offers the possibility to continuously tune the influence of the A-site ionic radii. For small concentrations x <= 0.1 we find a canted antiferromagnetic and paraelectric groundstate. For higher concentrations x <= 0.3 ferroelectric polarization coexists with the features of a long wavelength incommensurate spiral magnetic phase analogous to the observations in TbMnO3. In the intermediate concentration range around x = 0.2 a multiferroic scenario is realized combining weak ferroelectricity and weak ferromagnetism, presumably due to a canted spiral magnetic structure.

cond-mat.str-el↗