Magnetic-field-induced phase transitions are investigated in the frustrated gapped quantum paramagnet Rb$_{2}$Cu$_{2}$Mo$_3$O$_{12}$ through dielectric and calorimetric measurements on single-crystal samples. It is clarified that the previously reported dielectric anomaly at 8~K in powder samples is not due to a chiral spin liquid state as has been suggested, but rather to a tiny amount of a ferroelectric impurity phase. Two field-induced quantum phase transitions between paraelectric and paramagnetic and ferroelectric and magnetically ordered states are clearly observed. It is shown that the electric polarization is a secondary order parameter at the lower-field (gap closure) quantum critical point but a primary one at the saturation transition. Having clearly identified the magnetic Bose-Einstein condensation (BEC) nature of the latter, we use the dielectric channel to directly measure the critical divergence of BEC susceptibility. The observed power-law behavior is in very good agreement with theoretical expectations for three-dimensional BEC. Finally, dielectric data reveal magnetic presaturation phases in this compound that may feature exotic order with unconventional broken symmetries.
We consider model of quasi-2D magnetoelectric material as XY model for spin system on a lattice with local multiferroic-like interaction of spin and electric polarization vectors. We calculate the contribution of magnetic (spin) vortex-antivortex pairs (which form electric dipoles) to the dielectric susceptibility of the system. We show that in approximation of non-interacting pairs at $T \rightarrow T_{BKT}$ (Berezinskii-Kosterlitz-Thouless temperature) dielectric susceptibility diverges.
We derive a microscopic expression for the dielectric susceptibility $χ$ of a Coulomb glass, which corresponds to the definition used in classical electrodynamics, the derivative of the polarization with respect to the electric field. The fluctuation-dissipation theorem tells us that $χ$ is a function of the thermal fluctuations of the dipole moment of the system. We calculate $χ$ numerically for three-dimensional Coulomb glasses as a function of temperature and frequency.
The magnetic susceptibility between 1.5 and 800 K, the infrared reflectivity at room temperature and the temperature dependence of the dielectric constant at mm-wavelengths are reported for single crystalline BiFeO3. A well developed anomaly in the magnetic susceptibility signals the onset of antiferromagnetic order close to 640 K. Beside this anomaly, no further indications of phase or spin-glass transitions are found in the susceptibility down to the lowest temperatures. From infrared reflectivity we were able to identify all 9 phonon modes which are expected to be infrared active within the…
We analyze microwave cavity perturbation methods, and show that the technique is an excellent, precision method to study the dynamic magnetic and dielectric response in the $GHz$ frequency range. Using superconducting cavities, we obtain exceptionally high precision and sensitivity for measurements of relative changes. A dynamic electromagnetic susceptibility $\tildeζ(T)=ζ^{\prime}+iζ^{\prime \prime}$ is introduced, which is obtained from the measured parameters: the shift of cavity resonant frequency $δf$ and quality factor $Q$. We focus on the case of a spherical sample placed at the center …
Motivated by recent experiments, we append long ranged Coulomb interactions to dominant strong local correlations and study the resulting $t$-$J$-$V_C$ model for the 2-dimensional cuprate materials. This model includes the effect of short ranged Hubbard-Gutzwiller-Kanamori type correlations and long ranged Coulomb interactions on tight binding electrons. We calculate the $ \{\vec{q},ω\}$ dependent charge density fluctuations in this model using the extremely correlated fermi liquid theory, characterized by quasiparticles with very small weight $Z$. We develop a novel set of formulae to represe…
Dielectric and magnetic properties have been studied for poly-crystalline samples of quasi-one-dimensional frustrated spin-1/2 system Rb$_{2}$(Cu$_{1-x}$M$_{x}$)$_{2}$Mo$_{3}$O$_{12}$(M=Ni and Zn) which does not exhibit a three-dimensional magnetic transition due to quantum spin fluctuation and low dimensionality. A broad peak in the magnetic susceptibility - temperature curves originated from a short range helical ordering at low temperature is suppressed by the Ni and Zn substitution for Cu sites. The capacitance is found to anomalously increase with decreasing T below ~50 K, which is also s…
The recently proposed multiferroic state of the charge-transfer salt κ-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl [P. Lunkenheimer et al., Nature Mater., vol. 11, pp. 755-758, Sept. 2012] has been studied by dc-conductivity, magnetic susceptibility and measurements of the dielectric constant on various, differently prepared single crystals. In the majority of crystals we confirm the existence of an order-disorder-type ferroelectric state which coincides with antiferromagnetic order. This phenomenology rules out scenarios which consider an inhomogeneous, short-range-ordered ferroelectric state. Measurements…
We critically investigate the purported existence of a multiglass state in the quantum paraelectrics SrTiO${_3}$ and KTaO${_3}$ doped with magnetic 3d transition metals. We observe that the transition metals have limited solubility in these hosts, and that traces of impurity magnetic oxides persist even in the most well processed specimens. Our dielectric measurements indicate that the polar nano-regions formed as a consequence of doping appear to lack co-operativity, and the associated relaxation process exhibits a thermally activated Arrhenius form. At lower temperatures, the dielectric susc…
We study the Mott transition as a function of interaction strength in the half-filled Hubbard chain with next-nearest-neighbor hopping t' by calculating the response to an external electric field using the Density Matrix Renormalization Group. The electric susceptibility chi diverges when approaching the critical point from the insulating side. We show that the correlation length xi characterizing this transition is directly proportional to fluctuations of the polarization and that chi ~ xi^2. The critical behavior shows that the transition is infinite-order for all t', whether or not a spin g…
Magnetic dc susceptibility between 1.5 and 800 K, ac susceptibility and magnetization, thermodynamic properties, temperature dependence of radio and audio-wave dielectric constants and conductivity, contact-free dielectric constants at mm-wavelengths, as well as ferroelectric polarization are reported for single crystalline BiFeO3. A well developed anomaly in the magnetic susceptibility signals the onset of antiferromagnetic order close to 635 K. Beside this anomaly no further indications of phase or glass transitions are indicated in the magnetic dc and ac susceptibilities down to the lowest …
We report combined magnetic susceptibility, dielectric constant, nuclear quadruple resonance (NQR) and zero-field nuclear magnetic resonance (NMR) measurements on single crystals of multiferroics CuBr$_2$. High quality of the sample is demonstrated by the sharp magnetic and magnetic-driven ferroelectric transition at $T_N=T_C\approx$ 74~K. The zero-field $^{79}$Br and $^{81}$Br NMR are resolved below $T_N$. The spin-lattice relaxation rates reveal charge fluctuations when cooled below 60~K. Evidences of an increase of NMR linewidth, a reduction of dielectric constant, and an increase of magnet…
Here we calculate the dynamic susceptibility and dynamic correlation function in spin ice using the model of emergent magnetic monopoles. Calculations are based on a method originally suggested for the description of dynamic processes in water ice (non-equilibrium thermodynamics approach). We show that for zero temperature the dynamic correlation function reproduces the transverse dipole correlations (static correlation function) characteristic of spin ice in its ground state. At non-zero temperatures the dynamic correlation function includes an additional longitudinal component which decrease…
Three charge-ordering lanthanum nickelates La2-xAxNiO4, substituted with specific amounts of A = Sr, Ca, and Ba to achieve commensurate charge order, are investigated using broadband dielectric spectroscopy up to GHz frequencies. The transition temperatures of the samples are characterized by additional specific heat and magnetic susceptibility measurements. We find colossal magnitudes of the dielectric constant for all three compounds and strong relaxation features, which partly are of Maxwell-Wagner type arising from electrode polarization. Quite unexpectedly, the temperature-dependent colos…
The lacunar spinel GeV4S8 undergoes orbital and ferroelectric ordering at the Jahn-Teller transition around 30 K and exhibits antiferromagnetic order below about 14 K. In addition to this orbitally driven ferroelectricity, lacunar spinels are an interesting material class, as the vanadium ions form V4 clusters representing stable molecular entities with a common electron distribution and a well-defined level scheme of molecular states resulting in a unique spin state per V4 molecule. Here we report detailed x-ray, magnetic susceptibility, electrical resistivity, heat capacity, thermal expansio…
We report an experimental study of \nco, a Mott insulator containing chains of edge-sharing CuO$_4$ plaquettes, by polarized x-ray absorption spectroscopy (XAS), resonant magnetic x-ray scattering (RMXS), magnetic susceptibility, and pyroelectric current measurements. The XAS data show that the valence holes reside exclusively on the Cu$^{2+}$ sites within the copper-oxide spin chains and populate a $d$-orbital polarized within the CuO$_4$ plaquettes. The RMXS measurements confirm the presence of incommensurate magnetic order below a Néel temperature of $T_N = 11.5$ K, which was previously inf…
We discuss the interplay between anti-ferromagnetic order and polarization fluctuations in a magnetic quantum paraelectric. Using an action where anti-ferromagnetic order parameter couples to the polarization fluctuations and as well as magnetic field, we derive a set of self consistent equations to study both the temperature and the magnetic field dependence of the static dielectric susceptibility. The temperature dependence of dielectric susceptibility near both the anti-ferromagnetic quantum critical point and ferroelectric quantum critical point are described using scaling arguments. Discu…
We investigate magnetic, thermal, and dielectric properties of SrCuTe2O6, which is isostructural to PbCuTe2O6, a recently found, Cu-based 3D frustrated magnet with a corner sharing triangular spin network having dominant first and second nearest neighbor (nn) couplings [B. Koteswararao, et al. Phys. Rev. B 90, 035141 (2014)]. Although SrCuTe2O6 has a structurally similar spin network, but the magnetic data exhibit the characteristic features of a typical quasi -one-dimensional magnet, which mainly resulted from the magnetically dominant third nn coupling, uniform chains. The magnetic propertie…
We present magnetic, thermodynamic, dielectric and structural investigations on the aluminoborate Ni${_2}$AlBO${_5}$, belonging to the ludwigite family. Room temperature structural refinement suggests that the system crystallizes in the orthorhombic $Pbam$ symmetry, in similarity with most members of this material class. Magnetic and thermodynamic measurements shows that the system undergoes a phase transition to an antiferromagnetic state at 38K, signatures of which are also seen in the lattice parameters and the dielectric constant. Short range magnetic correlations appear to persist to much…
The dielectric behavior of the single crystals of the spin-chain system Ca3Co2O6, undergoing geometrically frustrated antiferromagnetic ordering below 25 K, has been investigated as a function of temperature and magnetic field (H) and compared with magnetization (M) behavior. The results provide evidence for anisotropic magnetodielectric (MDE) coupling in this compound. Ac susceptibility exhibits a strong frequency dependence for H parallel c with changes of this feature with the application of external dc magnetic field. No feature in ac susceptibility could be observed for H perpendicular c,…
It was recently observed that materials showing most striking multiferroic phenomena are frustrated spin-density-wave magnets. We present a simple phenomenological theory, which describes the orientation of the induced electric polarization for various incommensurate magnetic states, its dependence on temperature and magnetic field, and anomalies of dielectric susceptibility at magnetic transitions. We show that electric polarization can be induced at domain walls and that magnetic vortices carry electric charge.
We have recently reported that the Haldane spin-chain system, Er2BaNiO5, undergoing antiferromagnetic order below 32 K, is characterized by the onset of ferroelectricity near 60K due to magnetoelectric coupling induced by short-range magnetic-order within spin-chains. We have carried out additional magnetic and dielectric studies to understand the properties well below antiferromagnetic ordering temperature. We emphasize here on the following: (i) A strong frequency dependent behaviors of ac magnetic susceptibility and complex dielectric properties have been observed at much lower temperatures…
Magnetoelectric effect of the spin-1/2 Heisenberg-Ising ladder in a presence of the external electric and magnetic fields is rigorously examined by taking into account Katsura-Nagaosa-Balatsky mechanism. It is shown that the applied electric field may control a quantum phase transition between the Néel (stripy) ordered phase and the disordered paramagnetic phase. The staggered magnetization vanishes according to a power law with the Ising-type critical exponent 1/8, the electric polarization exhibits a weak singularity and the dielectric susceptibility shows a logarithmic divergence at this pa…
We report that the spin-chain compound Dy2BaNiO5 recently proven to exhibit magnetoelectric coupling below its Neel temperature (T_N) of 58 K, exhibits strong frequency-dependent behavior in ac magnetic susceptibility and complex dielectric properties at low temperatures (<10K), mimicking 'reentrant' multiglass phenomenon. Such a behavior is not known among undoped compounds. A new finding in the field of multiferroics is that the characteristic magnetic feature at such low temperatures moves towards higher temperatures in the presence of a magnetic-field (H), whereas the corresponding dielect…
MnSnTeO6, a new chiral antiferromagnet, was prepared both by topotactic transformation of the metastable rosiaite-type polymorph and by direct synthesis from coprecipitated hydroxides. Its structure, static and dynamic magnetic properties were studied comprehensively both experimentally (through X-ray and neutron powder diffraction, magnetization, specific heat, dielectric permittivity and ESR techniques) and theoretically (by means of ab initio density functional theory (DFT) calculations within the spin-polarized generalized gradient approximation). MnSnTeO6 is isostructural with MnSb2O6 (sp…
We develop a theory for the analytic computation of the free energy of band insulators in the presence of a uniform and constant electric field. The two key ingredients are a perturbation-like expression of the Wannier-Stark energy spectrum of electrons and a modified statistical mechanics approach involving a local chemical potential in order to deal with the unbounded spectrum and impose the physically relevant electronic filling. At first order in the field, we recover the result of King-Smith, Vanderbilt and Resta for the electric polarization in terms of a Zak phase - albeit at finite tem…
Tris-sarcosine calcium chloride (TSCC) is a highly uniaxial ferroelectric with a Curie temperature of approximately 130K. By suppressing ferroelectricity with bromine substitution on the chlorine sites, pure single crystals were tuned through a ferroelectric quantum phase transition. The resulting quantum critical regime was investigated in detail - the first time for a uniaxial ferroelectric and for an organic ferroelectric - and was found to persist up to temperatures of at least 30K to 40K. The nature of long-range dipole interactions in uniaxial materials, which lead to non-analytical term…
Twisted van der Waals bilayers provide an ideal platform to study the electron correlation in solids. Of particular interest is the 30 degree twisted bilayer honeycomb lattice system, which possesses an incommensurate moire pattern and uncommon electronic behaviors may appear due to the absence of phase coherence. Such system is extremely sensitive to further twist and many intriguing phenomena will occur. In this work, based on first-principles calculations we show that, for further twist near 30 degree, there could induce dramatically different dielectric behaviors of electron between left a…
The dielectric and magnetic polarizations of quantum paraelectrics and paramagnetic materials have in many cases been found to initially increase with increasing thermal disorder and hence exhibit peaks as a function of temperature. A quantitative description of these examples of 'order-by-disorder' phenomenona has remained elusive in nearly ferromagnetic metals and in dielectrics on the border of displacive ferroelectric transitions. Here we present an experimental study of the evolution of the dielectric susceptibility peak as a function of pressure in the nearly ferroelectric material, stro…
