arXiv subjects

A. Loidl

Publications and source records attributed to A. Loidl.

At least 181 records · Page 10Linked to original sources

arXiv2009

Optical properties of ZnCr2Se4 - Spin-phonon coupling and electronic d-d-like excitations

We studied the optical properties of antiferromagnetic ZnCr2Se4 by infrared spectroscopy up to 28,000 cm-1 and for temperatures from 5 to 295 K. At the magnetic phase transition at 21 K, one of the four phonon modes reveals a clear splitting of 3 cm-1 as a result of spin-phonon coupling, the other three optical eigenmodes only show shifts of the eigenfrequencies. The antiferromagnetic ordering and the concomitant splitting of the phonon mode can be suppressed in a magnetic field of 7 T. At higher energies we observed a broad excitation band which is dominated by a two-peak-structure at about 18,000 cm-1 and 22,000 cm-1, respectively. These energies are in good agreement with the expected spin-allowed crystal-field transition of the Cr3+ ions. The unexpected strength of these forbidden onsite d-d transitions is attributed to a considerable hybridization of the selenium p with the chromium d orbitals.

cond-mat.str-el↗

arXiv2009

Magnetic and magnetoelectric excitations in TbMnO$_3$

Magnetic and magnetoelectric excitations in the multiferroic TbMnO_3 have been investigated at terahertz frequencies. Using different experimental geometries we can clearly separate the electro-active excitations (electromagnons) from the magneto-active modes, i.e. antiferromagnetic resonances (AFMR). Two AFMR resonances were found to coincide with electromagnons. This indicates that both excitations belong to the same mode and the electromagnons can be excited by magnetic ac-field as well. In external magnetic fields and at low temperatures distinct fine structure of the electromagnons appears. In spite of the 90^o rotation of the magnetic structure, the electromagnons are observable for electric ac-fields parallel to the a-axis only. Contrary to simple expectations, the response along the c-axis remains purely magnetic in nature.

cond-mat.str-el↗

arXiv2008

Colossal dielectric constant up to GHz at room temperature

The search for new materials with extremely high ("colossal") dielectric constants, required for future electronics, is one of the most active fields of modern materials science. However, the applicability of the colossal-epsilon' materials, discovered so far, suffers from the fact that their dielectric constant, epsilon', only is huge in a limited frequency range below about 1 MHz. In the present report, we show that the dielectric properties of La15/8Sr1/8NiO4 surpass those of other materials. Especially, epsilon' retains its colossal magnitude of >10000 well into the GHz range. This material is prone to charge order and this spontaneous ordering process of the electronic subsystem can be assumed to play an important role in the generation of the observed unusual dielectric properties.

cond-mat.mtrl-sci↗

arXiv2008

Spin-driven Phase Transitions in ZnCr$_2$Se$_4$ and ZnCr$_2$S$_4$ Probed by High Resolution Synchrotron X-ray and Neutron Powder Diffraction

The crystal and magnetic structures of the spinel compounds ZnCr$_2$S$_4$ and ZnCr$_2$Se$_4$ were investigated by high resolution powder synchrotron and neutron diffraction. ZnCr$_2$Se$_4$ exhibits a first order phase transition at $T_N=21$ K into an incommensurate helical magnetic structure. Magnetic fluctuations above $T_N$ are coupled to the crystal lattice as manifested by negative thermal expansion. Both, the complex magnetic structure and the anomalous structural behavior can be related to magnetic frustration. Application of an external magnetic field shifts the ordering temperature and the regime of negative thermal expansion towards lower temperatures. Thereby, the spin ordering changes into a conical structure. ZnCr$_2$S$_4$ shows two magnetic transitions at $T_{N1}=15$ K and $T_{N2}=8$ K that are accompanied by structural phase transitions. The crystal structure transforms from the cubic spinel-type (space group $Fd$\={3}$m$) at high temperatures in the paramagnetic state, via a tetragonally distorted intermediate phase (space group $I4_1$ / $amd$) for $T_{N2} < T < T_{N1}$ into a low temperature orthorhombic phase (space group $I m m a$) for $T < T_{N2}$. The cooperative displacement of sulfur ions by exchange striction is the origin of these structural phase transitions. The low temperature structure of ZnCr$_2$S$_4$ is identical to the orthorhombic structure of magnetite below the Verwey transition. When applying a magnetic field of 5 T the system shows an induced negative thermal expansion in the intermediate magnetic phase as observed in ZnCr$_2$Se$_4$.

cond-mat.str-el↗

arXiv2008

Glassy dynamics in mono-, di-, and tri-propylene glycol: From the alpha- to the fast beta-relaxation

We present a thorough characterization of the glassy dynamics of three propylene glycols (mono-, di- and trimer) by broadband dielectric spectroscopy. By covering a frequency range of more than 15 decades, we have access to the entire variety of dynamic processes typical for glassy dynamics. These results add three more molecular glass formers to the sparse list of materials for which real broadband spectra, including the region of the fast beta-process, are available. Some first analyses of the various observed dynamic processes are provided.

cond-mat.soft↗

arXiv2008

Colossal magnetocapacitive effect in differently synthesized and doped CdCr2S4

In the present work, we address the question of an impurity-related origin of the colossal magnetocapacitive effect in the spinel system CdCr2S4. We demonstrate that a strong variation in the dielectric constant below the magnetic transition temperature or in external magnetic fields also arises in crystals prepared without chlorine. This excludes that an inhomogeneous distribution of chlorine impurities at the surface or in the bulk material gives rise to the unusual effects in the spinel multiferroics. In addition, we show that colossal magnetocapacitive effects can be also generated in chlorine-free ceramic samples of CdCr2S4, doped with indium.

cond-mat.mtrl-sci↗

arXiv2008

Electron Spin Resonance across the Charge-ordering Transition in YBaMn2O6

We investigated the metal-ordered manganite system YBaMn2O6 using electron spin resonance (ESR) in the paramagnetic regime across the charge-ordering and structural phase transition at T_CO = 480 K and T_t = 520 K, respectively. All ESR parameters exhibit jump-like changes at T_t while the charge-ordering at T_CO manifests itself only as a weak and broad anomaly. Above T_t the ESR spin susceptibility is reduced with respect to the dc-susceptibility, indicating that only the t_2g-core spins of Mn ions contribute to the resonance absorption. The contribution of the e_g-spins is suppressed by the time scale of the polaronic hopping process of the e_g-electrons. The linewidth in this regime is reminiscent of a Korringa-type relaxation behavior. In this picture the ESR properties below T_t are dominated by the slowing down of the polaronic hopping process. The charge fluctuations persist down to the temperature T* ~ 410 K, below which the system can be described as a charge-ordered assembly of Mn$^{3+}$ and Mn$^{4+}$ spins.

cond-mat.str-el↗

arXiv2008

Optical Spectroscopy in CoO: Phonons, Electric, and Magnetic Excitations

The reflectivity of single-crystalline CoO has been studied by optical spectroscopy for wave numbers ranging from 100 to 28,000\wn and for temperatures 8 $< T <$ 325 K\@. A splitting of the cubic IR-active phonon mode on passing the antiferromagnetic phase transition at $T_N$ = 289 K has been observed. At low temperatures the splitting amounts to 15.0\wn. In addition, we studied the splitting of the cubic crystal field ground state of the Co$^{2+}$ ions due to spin-orbit coupling, a tetragonal crystal field, and exchange interaction. Below $T_N$, magnetic dipole transitions between the exchange-split levels are identified and the energy-level scheme can be well described with a spin-orbit coupling $λ= 151.1\wn$, an exchange constant $J = 17.5\wn$, and a tetragonal crystal-field parameter $D = -47.8\wn$. Already in the paramagnetic state electric quadrupole transitions between the spin-orbit split level have been observed. At high frequencies, two electronic levels of the crystal-field-split $d$-manifold were identified at 8,000 and 18,500\wn.

cond-mat.str-el↗

arXiv2008

Chain Formation by Spin Pentamers in eta-Na9V14O35

The nature of the gapped ground state in the quasi-one-dimensional compound eta-Na9V14O35 cannot easily be understood, if one takes into account the odd number of spins on each structural element. Combining the results of specific heat, susceptibility and electron spin resonance measurements we show that eta-Na9V14O35 exhibits a novel ground state where multi-spin objects build up a linear chain. These objects - pentamers - consist of five antiferromagnetically arranged spins with effective spin 1/2. Their spatial extent results in an exchange constant along the chain direction comparable to the one in the high-temperature state.

cond-mat.str-el↗

arXiv2008

Dynamical Dzyaloshinsky-Moriya Interaction in KCuF3

The spin dynamics of the prototypical quasi one-dimensional antiferromagnetic Heisenberg spin S=1/2 chain KCuF3 is investigated by electron spin resonance spectroscopy. Our analysis shows that the peculiarities of the spin dynamics require a new dynamical form of the antisymmetric anisotropic spin-spin interaction. This dynamical Dzyaloshinsky-Moriya interaction is related to strong oscillations of the bridging fuorine ions perpendicular to the crystallographic c axis. This new mechanism allows to resolve consistently the controversies in observation of the magnetic and structural properties of this orbitally ordered perovskite compound.

cond-mat.str-el↗

arXiv2008

Evidence for orthorhombic distortions in the ordered state of ZnCr$_2$O$_4$: A magnetic resonance study

We present an elaborate electron-spin resonance study of the low-energy dynamics and magnetization in the ordered phase of the magnetically frustrated spinel ZnCr$_2$O$_4$. We observe several resonance modes corresponding to different structural domains and found that the number of domains can be easily reduced by field-cooling the sample through the transition point. To describe the observed antiferromagnetic resonance spectra it is necessary to take into account an orthorhombic lattice distortion in addition to the earlier reported tetragonal distortion which both appear at the antiferromagnetic phase transition.

cond-mat.str-el↗

arXiv2008

Dielectric and conductivity relaxation in mixtures of glycerol with LiCl

We report a thorough dielectric characterization of the alpha relaxation of glass forming glycerol with varying additions of LiCl. Nine salt concentrations from 0.1 - 20 mol% are investigated in a frequency range of 20 Hz - 3 GHz and analyzed in the dielectric loss and modulus representation. Information on the dc conductivity, the dielectric relaxation time (from the loss) and the conductivity relaxation time (from the modulus) is provided. Overall, with increasing ion concentration, a transition from reorientationally to translationally dominated behavior is observed and the translational ion dynamics and the dipolar reorientational dynamics become successively coupled. This gives rise to the prospect that by adding ions to dipolar glass formers, dielectric spectroscopy may directly couple to the translational degrees of freedom determining the glass transition, even in frequency regimes where usually strong decoupling is observed.

cond-mat.soft↗

arXiv2008

Broadband dielectric spectroscopy on benzophenone: alpha relaxation, beta relaxation, and mode coupling theory

We have performed a detailed dielectric investigation of the relaxational dynamics of glass-forming benzophenone. Our measurements cover a broad frequency range of 0.1 Hz to 120 GHz and temperatures from far below the glass temperature well up into the region of the small-viscosity liquid. With respect to the alpha relaxation this material can be characterized as a typical molecular glass former with rather high fragility. A good agreement of the alpha relaxation behavior with the predictions of the mode coupling theory of the glass transition is stated. In addition, at temperatures below and in the vicinity of Tg we detect a well-pronounced beta relaxation of Johari-Goldstein type, which with increasing temperature develops into an excess wing. We compare our results to literature data from optical Kerr effect and depolarized light scattering experiments, where an excess-wing like feature was observed in the 1 - 100 GHz region. We address the question if the Cole-Cole peak, which was invoked to describe the optical Kerr effect data within the framework of the mode coupling theory, has any relation to the canonical beta relaxation detected by dielectric spectroscopy.

cond-mat.dis-nn↗

arXiv2007

Switching the Ferroelectric Polarization by External Magnetic Fields in the Spin = 1/2 Chain Cuprate LiCuVO4

We present a detailed study of complex dielectric constant and ferroelectric polarization in multiferroic LiCuVO4 as function of temperature and external magnetic field. In zero external magnetic field, spiral spin order with an ab helix and a propagation vector along the crystallographic b direction is established, which induces ferroelectric order with spontaneous polarization parallel to a. The direction of the helix can be reoriented by an external magnetic field and allows switching of the spontaneous polarization. We find a strong dependence of the absolute value of the polarization for different orientations of the spiral plane. Above 7.5 T, LiCuVO4 reveals collinear spin order and remains paraelectric for all field directions. Thus this system is ideally suited to check the symmetry relations for spiral magnets as predicted theoretically. The strong coupling of ferroelectric and magnetic order is documented and the complex (B,T) phase diagram is fully explored.

cond-mat.str-el↗

arXiv2007

Spin Frustration and Magnetic Exchange in Cobalt Aluminum Oxide Spinels

We report on x-ray diffraction, magnetic susceptibility, electron- spin resonance and heat- capacity studies of Co[Al_1-xCo_x]_2O_4 for Co concentrations 0 10 indicates the presence of strong spin frustration at least for x < 0.6. The frustration mechanism is attributed to competing nearest neighbor and next-nearest neighbor superexchange interactions between the A-site Co^2+ ions.

cond-mat.mtrl-sci↗

arXiv2007

Magnetic-order induced phonon splitting in MnO from far-infrared spectroscopy

Detailed far-infrared spectra of the optical phonons are reported for antiferromagnetic MnO. Eigenfrequencies, phonon damping and effective plasma frequencies are studied as a function of temperature. Special attention is paid to the phonon splitting at the antiferromagnetic phase transition. The results are compared to recent experimental and theoretical studies of the spin-phonon coupling in frustrated magnets, which are explained in terms of a spin-driven Jahn-Teller effect, and to ab initio and model calculations, which predict phonon splitting induced by magnetic order.

cond-mat.str-el↗

arXiv2007

Colossal dielectric constants in single-crystalline and ceramic CaCu3Ti4O12 investigated by broadband dielectric spectroscopy

In the present work the authors report results of broadband dielectric spectroscopy on various samples of CaCu3Ti4O12, including so far only rarely investigated single crystalline material. The measurements extend up to 1.3 GHz, covering more than nine frequency decades. We address the question of the origin of the colossal dielectric constants and of the relaxational behavior in this material, including the second relaxation reported in several recent works. For this purpose, the dependence of the temperature- and frequency-dependent dielectric properties on different tempering and surface treatments of the samples and on ac-field amplitude are investigated. Broadband spectra of a single crystal are analyzed by an equivalent circuit description, assuming two highly resistive layers in series to the bulk. Good fits could be achieved, including the second relaxation, which also shows up in single crystals. The temperature- and frequency-dependent intrinsic conductivity of CCTO is consistent with the Variable Range Hopping model. The second relaxation is sensitive to surface treatment and, in contrast to the main relaxation, also is strongly affected by the applied ac voltage. Concerning the origin of the two insulating layers, we discuss a completely surface-related mechanism assuming the formation of a metal-insulator diode and a combination of surface and internal barriers.

cond-mat.mtrl-sci↗

arXiv2007

Dielectric spectroscopy in benzophenone: The beta relaxation and its relation to the mode-coupling Cole-Cole peak

We report a thorough characterization of the glassy dynamics of benzophenone by broadband dielectric spectroscopy. We detect a well pronounced beta relaxation peak developing into an excess wing with increasing temperature. A previous analysis of results from Optical-Kerr-effect measurements on this material within the mode coupling theory revealed a high-frequency Cole-Cole peak. We address the question if this phenomenon also may explain the Johari-Goldstein beta relaxation, a so far unexplained spectral feature inherent to glass-forming matter, mainly observed in dielectric spectra. Our results demonstrate that according to the present status of theory, both spectral features seem not to be directly related.

cond-mat.dis-nn↗