arXiv subjects

S-W. Cheong

Publications and source records attributed to S-W. Cheong.

At least 55 records · Page 3Linked to original sources

arXiv2008

Complex Spin Structures and Origin of the Magneto-Electric Coupling in YMn2O5

By combining neutron four-circle diffraction and polarized neutron diffraction techniques we have determined the complex spin structures of a multiferroic, YMn2O5, that exhibits two ferroelectric phases at low temperatures. The obtained magnetic structure has spiral components in both the low temperature ferroelectric phases that are magnetically commensurate and incommensurate, respectively. Among proposed microscopic theories for the magneto-electric coupling, our results are consistent with both the spin-current model that requires a magnetic transverse (cycloidal) spiral structure in order to induce a spontaneous electric polarization and the magneto-restriction model. Our results also explain why the electric polarization changes at the commensurate-to-incommensurate phase transition.

cond-mat.str-el↗

arXiv2008

Spin phonon coupling in frustrated magnet CdCr$_2$O$_4$

The infrared phonon spectrum of the spinel CdCr2O4 is measured as a function temperature from 6 K to 300K. The triply degenerate Cr phonons soften in the paramagnetic phase as temperature is lowered below 100 K and then split into a singlet and doublet in the low T antiferromagnetic phase which is tetragonally distorted to relieve the geometric frustration in the pyrochlore lattice of Cr$^{3+}$ ions. The phonon splitting is inconsistent with the simple increase (decrease) in the force constants due to deceasing (increasing) bond lengths in the tetragonal phase. Rather they correspond to changes in the force constants due to the magnetic order in the antiferromagnetic state. The phonon splitting in this system is opposite of that observed earlier in ZnCr2O4 as predicted by theory. The magnitude of the splitting gives a measure of the spin phonon coupling strength which is smaller than in the case of ZnCr2O4.

cond-mat.mtrl-sci↗

arXiv2008

Raman scattering studies of temperature- and field-induced melting of charge order in (La,Pr,Ca)MnO$_{3}$

We present Raman scattering studies of the structural and magnetic phases that accompany temperature- and field-dependent melting of charge- and orbital-order (COO) in La0.5Ca0.5MnO3 and La0.25Pr0.375Ca0.375MnO3. Our results show that thermal and field-induced COO melting in La0.5Ca0.5MnO3 exhibits three stages in a heterogeneous melting process associated with a structural change: a long-range, strongly JT distorted/COO regime; a coexistence regime; and weakly JT distorted/PM or FM phase. We provide a complete structural phase diagram of La0.5Ca0.5MnO3 for the temperature and field ranges 6<=T<=170 K and 0<=H<=9 T. We also investigate thermal and field-induced melting in La0.25Pr0.375Ca0.375MnO3 to elucidate the role of disorder in melting of COO. We find that while thermal melting of COO in La0.25Pr0.375Ca0.375MnO3 is quite similar to that in La0.5Ca0.5MnO3, the field-induced transition from the COO phase to the weakly JT-distorted/FM phase in La0.25Pr0.375Ca0.375MnO3 is very abrupt, and occurs at significantly lower fields (H~2 T at T~0 K) than in La0.5Ca0.5MnO3 (H~30 T at T=0 K). Moreover, the critical field H_c increases with increasing temperature in La0.25Pr0.375Ca0.375MnO3 in contrast to La0.5Ca0.5MnO3. To explain these differences, we propose that field-induced melting of COO in La0.25Pr0.375Ca0.375MnO3 is best described as the field-induced percolation of FM domains, and we suggest that Griffiths phase physics may be an appropriate theoretical model for describing the unusual temperature- and field- dependent transitions observed in La0.25Pr0.375Ca0.375MnO3.

cond-mat.str-el↗

arXiv2007

Neel to Spin-Glass-like Phase Transition versus Dilution in Geometrically Frustrated ZnCr_{2-2x}Ga_{2x}O_4

ZnCr2O4 undergoes a first order spin-Peierls-like phase transition at 12.5 K from a cubic spin liquid phase to a tetragonal Neel state. Using powder diffraction and single crystal polarized neutron scattering, we determined the complex spin structure of the Neel phase. This phase consisted of several magnetic domains with different characteristic wave vectors. This indicates that the tetragonal phase of ZnCr2O4 is very close to a critical point surrounded by many different Neel states. We have also studied, using elastic and inelastic neutron scattering techniques, the effect of nonmagnetic dilution on magnetic correlations in ZnCr_{2-2x}Ga_{2x}O_4 (x=0.05 and 0.3). For x=0.05, the magnetic correlations do not change qualitatively from those in the pure material, except that the phase transition becomes second order. For x= 0.3, the spin-spin correlations become short range. Interestingly, the spatial correlations of the frozen spins in the x=0.3 material are the same as those of the fluctuating moments in the pure and the weakly diluted materials.

cond-mat.str-el↗

arXiv2007

Direct observation of oxygen superstructures in manganites

We report the observation of superstructures associated with the oxygen 2p-states in two prototypical manganites using x-ray diffraction at the oxygen K-edge. We determine the nature of the orderings and discuss our picture with respect to novel theoretical models. In the stripe order system Bi0.31 Ca0.69 MnO3, hole-doped O states are found to be orbitally ordered, at the same propagation vector as the Mn orbital ordering, but no evidence is found to support a picture of oxygen charge stripes at this periodicity. In La 7/8 Sr 1/8 MnO3, we observe a 2p charge ordering described by alternating hole-poor and hole-rich MnO planes that is consistent with recent predictions.

cond-mat.str-el↗

arXiv2007

Pressure induced enhancement of ferroelectricity in multiferroic $R$Mn$_2$O$_5$($R$=Tb,Dy, and Ho)

Measurements of ferroelectric polarization and dielectric constant were done on $R$Mn$_2$O$_5$ ($R$=Tb, Dy, and Ho) with applied hydrostatic pressures of up to 18 kbar. At ambient pressure, distinctive anomalies were observed in the temperature profile of both physical properties at critical temperatures marking the onset of long range AFM order (T$_{N1}$), ferroelectricity (T$_{C1}$) as well as at temperatures when anomalous changes in the polarization, dielectric constant and spin wave commensurability have been previously reported. In particular, the step in the dielectric constant at low temperatures (T$_{C2}$), associated with both a drop in the ferroelectric polarization and an incommensurate magnetic structure, was shown to be suddenly quenched upon passing an $R$-dependent critical pressure. This was shown to correlate with the stabilization of the high ferroelectric polarization state which is coincident with the commensurate magnetic structure. The observation is suggested to be due to a pressure induced phase transition into a commensurate magnetic structure as exemplified by the pressure-temperature ($p$-$T$) phase diagrams constructed in this work. The $p$-$T$ phase diagrams are determined for all three compounds.

cond-mat.str-el↗

arXiv2007

Universality in one dimensional orbital wave ordering in spinel and related compounds: an experimental perspective

Recent state-of-the-art crystallographic investigations of transition metal spinel compounds have revealed that the d- orbital charge carriers undergo ordering transitions with the formation of local "molecular bonding" units such as dimers in MgTi2O4, octomers in CuIr2S4, and heptamers in AlV2O4. Herein, we provide a unifying scheme involving one- dimensional orbital wave ordering applicable to all of these spinels. The relative phase of the orbitals in the chains is shown to be crucial to the formation of different local units, and thus both the amplitude and phase of the orbital wave play important roles. Examination of Horibe et al.'s [1] structure for AlV2O4 serves as the vehicle for developing the general behavior for such orbital wave ordering. Ordered AlV2O4 will be seen to organize into three equivalent chains in 2D Kagome planes coupled so as to form units of three dimer bonds. Three additional equivalent chains manifest a more complex tetramerization with three different charge states and two different bonding schemes. The orbital wave ordering scheme developed is extended to other spinel and related compounds with local triangular transition metal coordination and partial filling of the t2g-d orbitals.

cond-mat.str-el↗

arXiv2007

Symmetry of Multiferroicity in a Frustrated Magnet TbMn$_2$O$_5$

Based on measurements of soft x-ray magnetic scattering and symmetry considerations, we demonstrate that the magnetoelectric effect in TbMn$_2$O$_5$ arises from an internal field determined by $\vec{S}_{\vec{q}} \times {\vec{S}_{-\vec{q}}}$ with $\vec{S}_{\vec{q}}$ being the magnetization at modulation vector $\vec{q}$, whereas the magneto-elastic effect in the exchange energy governs the response to external electric fields. Our results set fundamental symmetry constraints on the microscopic mechanism of multiferroicity in frustrated magnets.

cond-mat.str-el↗

arXiv2006

Electromagnons in multiferroic YMn2O5 and TbMn2O5

Based on temperature dependent far infrared transmission spectra of YMn2O5 and TbMn2O5 single crystals, we report the observation of electric dipole-active magnetic excitations, or electromagnons, in these multiferroics. Electromagnons are found to be directly responsible for the step-like anomaly of the static dielectric constant at the commensurate--incommensurate magnetic transition and are the origin of the colossal magneto-dielectric effect reported in these multiferroics.

cond-mat.str-el↗

arXiv2006

IR Phonon signatures of multiferroicity in TbMn$_{2}$O$_{5}$

The infrared (IR) active phonons in multiferroic TbMn$_2$O$_5$ are studied as a function of temperature. Most of the symmetry allowed IR modes polarized along the \textit{a} and \textit{b} crystal axes are observed and the behavior of several \textit{b} polarized phonons is correlated with the magnetic and ferroelectric transitions. A high frequency \textit{b} polarized phonon only Raman allowed in the paraelectric phase becomes IR active at the ferroelectric transition. The IR strength of this mode is proportional to the square of the ferroelectric order parameter and gives a sensitive measure of the symmetry lowering lattice distortions in the ferroelectric phase.

cond-mat.mtrl-sci↗

arXiv2006

Evidences of a consolute critical point in the Phase Separation regime of La(5/8-y)Pr(y)Ca(3/8)MnO(3) (y = 0.4) single crystals

We report on DC and pulsed electric field sensitivity of the resistance of mixed valent Mn oxide based La(5/8-y)Pr(y)Ca(3/8)MnO(3) (y = 0.4) single crystals as a function of temperature. The low temperature regime of the resistivity is highly current and voltage dependent. An irreversible transition from high (HR) to a low resistivity (LR) is obtained upon the increase of the electric field up to a temperature dependent critical value (V_c). The current-voltage characteristics in the LR regime as well as the lack of a variation in the magnetization response when V_c is reached indicate the formation of a non-single connected filamentary conducting path. The temperature dependence of V_c indicates the existence of a consolute point where the conducting and insulating phases produce a critical behavior as a consequence of their separation.

cond-mat.str-el↗

arXiv2006

Structural Anomalies at the Magnetic and Ferroelectric Transitions in $RMn_2O_5$ (R=Tb, Dy, Ho)

Strong anomalies of the thermal expansion coefficients at the magnetic and ferroelectric transitions have been detected in multiferroic $RMn_2O_5$. Their correlation with anomalies of the specific heat and the dielectric constant is discussed. The results provide evidence for the magnetic origin of the ferroelectricity mediated by strong spin-lattice coupling in the compounds. Neutron scattering data for $HoMn_2O_5$ indicate a spin reorientation at the two low-temperature phase transitions.

cond-mat.str-el↗

arXiv2006

Relating supercooling and glass-like arrest of kinetics for phase separated systems: studies on doped CeFe$_2$ and (La,Pr,Ca)MnO$_3$

Coexisting ferromagnetic and antiferromagnetic phases over a range of temperature as well as magnetic field have been reported in many materials of current interest, showing disorder-broadened 1st order transitions. Anomalous history effects observed in magnetization and resistivity are being explained invoking the concepts of kinetic arrest akin to glass transitions. From magnetization measurements traversing novel paths in field-temperature space, we obtain the intriguing result that the regions of the sample which can be supercooled to lower temperatures undergo kinetic-arrest at higher temperatures, and vice versa. Our results are for two diverse systems viz. the inter-metallic doped CeFe$_2$ which has an antiferromagnetic ground state, and the oxide La-Pr-Ca-Mn-O which has a ferromagnetic ground state, indicating the possible universality of this effect of disorder on the widely encountered phenomenon of glass-like arrest of kinetics.

cond-mat.str-el↗

arXiv2005

Ferroelectricity induced by acentric spin-density waves in YMn$_2$O$_5$

The commensurate and incommensurate magnetic structures of the magnetoelectric system YMn$_{2}$O$_{5}$, as determined from neutron diffraction, were found to be spin-density waves lacking a global center of symmetry. We propose a model, based on a simple magneto-elastic coupling to the lattice, which enables us to predict the polarization based entirely on the observed magnetic structure. Our data accurately reproduce the temperature-dependence of the spontaneous polarization, in particular its sign reversal at the commensurate-incommensurate transition.

cond-mat.mtrl-sci↗

arXiv2005

Polarized resonant inelastic x-ray scattering as an ultra-fine probe of excited states in La2CuO4

X-ray absorption is the standard method to probe the unoccupied density of states at a given edge. Here we show that polarized Resonant Inelastic X-Ray Scattering in La2CuO4 at the Cu K-edge is extremely sensitive to the environment of the Cu atom and the fine structure in the Cu 4p density of states. Combined ab initio and many-body cluster calculations, used for the first time in such a context, show remarkable agreement with experiment. In particular we identify a non-local effect namely a transition to off-site Cu 3d states.

cond-mat.str-el↗

arXiv2005

The charge ordered state in half-doped Bi-based manganites studied by $^{17}$O and $^{209}$Bi NMR

We present a $^{209}$Bi and $^{17}$O NMR study of the Mn electron spin correlations developed in the charge ordered state of Bi$_{0.5}$Sr$_{0.5}$MnO$_{3}$ and Bi$_{0.5}$Ca$_{0.5}$MnO$_{3}$. The unusually large local magnetic field $^{209}H_{loc}$ indicates the dominant $6s^{2}$ character of the lone electron pair of Bi$^{3+}$-ions in both compounds. The mechanism connecting the $s$ character of the lone pairs to the high temperature of charge ordering $T_{CO}$ is still not clarified. The observed difference in $^{209}H_{loc}$ for Bi$_{0.5}$Sr$_{0.5}$MnO$_{3}$ to Bi$_{0.5}$Ca$_{0.5}$MnO$_{3}$ is probably due to a decrease in the canting of the staggered magnetic moments of Mn$^{3+}$-ions from. The modification of the $^{17}$O spectra below $T_{CO}$ demonstrates that the line due to the apical oxygens is a unique local tool to study the development of the Mn spin correlations. In the AF state the analysis of the $^{17}$O spectrum of Pr$_{0.5}$Ca$_{0.5}$MnO$_{3}$ and Bi$_{0.5}$Sr$_{0.5}$MnO$_{3}$ prompts us to try two different theoretical descriptions of the charge-ordered state, a site-centered model for the first manganite and a bond-centered model for the second one.

cond-mat.str-el↗

arXiv2005

Spin structure and magnetic frustration in multiferroic RMn2O5 (R = Tb, Ho, Dy)

We have studied the crystal and magnetic structures of the magnetoelectric materials RMn2O5 (R = Tb, Ho, Dy) using neutron diffraction as a function of temperature. All three materials display incommensurate antiferromagnetic ordering below 40 K, becoming commensurate on further cooling. For R = Tb, Ho, a commensurate-incommensurate transition takes place at low temperatures. The commensurate magnetic structures have been solved and are discussed in terms of competing exchange interactions. The spin configuration within the ab plane is essentially the same for each system, and the radius of R determines the sign of the magnetic exchange between adjacent planes. The inherent magnetic frustration in these materials is lifted by a small lattice distortion, primarily involving shifts of the Mn3+ cations and giving rise to a canted antiferroelectric phase.

cond-mat.str-el↗

arXiv2004

Uncorrelated and correlated nanoscale lattice distortions in the paramagnetic phase of magnetoresistive manganites

Neutron scattering measurements on a magnetoresistive manganite La$_{0.75}$(Ca$_{0.45}$Sr$_{0.55}$)$_{0.25}$MnO$_3$ show that uncorrelated dynamic polaronic lattice distortions are present in both the orthorhombic (O) and rhombohedral (R) paramagnetic phases. The uncorrelated distortions do not exhibit any significant anomaly at the O-to-R transition. Thus, both the paramagnetic phases are inhomogeneous on the nanometer scale, as confirmed further by strong damping of the acoustic phonons and by the anomalous Debye-Waller factors in these phases. In contrast, recent x-ray measurements and our neutron data show that polaronic correlations are present only in the O phase. In optimally doped manganites, the R phase is metallic, while the O paramagnetic state is insulating (or semiconducting). These measurements therefore strongly suggest that the {\it correlated} lattice distortions are primarily responsible for the insulating character of the paramagnetic state in magnetoresistive manganites.

cond-mat.str-el↗