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Terahertz (THz) magnonics represent the notion of mathematical algebraic operations of magnons such as addition and subtraction in THz regime which is an emergent dissipationless ultrafast alternative to existing data processing technologies. Spin waves on antiferromagnets with a twist in spin order host such magnons in THz regime, which possess advantage of higher processing speeds, additional polarization degree of freedom and longer propagation lengths compared to that of gigahertz magnons in ferromagnets. While interaction among THz magnons is the crux of algebra operations, it requires magnetic orders with closely spaced magnon modes for easier experimental realization of their interactions. Herein, rich wealth of magnons spanning a narrow energy range of 0.4 to 10 meV is unraveled in Co4Ta2O9 using magneto-THz spectroscopy. Rare multitude of ten excitation modes, either of magnons or hybrid magnon-phonon modes is presented. Among other attributes, spin lattice interaction suggests a correlation among spin and local lattice distortion, magnetostriction, and magnetic exchange interaction signifying a THz magnetoelectric effect. This unification of structural, magnetic and dielectric facets, and their magnetic field control in a narrow spectrum unwinds the mechanism underneath the system's complexity while the manifestation of multitude of spin excitation modes is a potential source to design multiple channels in spin-wave computing based devices.

Fe doping into BaTiO3, stabilizes the paraelectric hexagonal phase in place of the ferroelectric tetragonal one [P. Pal et al. Phys. Rev. B, 101, 064409 (2020)]. We show that simultaneous doping of Bi along with Fe into BaTiO3 effectively enhances the magnetoelectric (ME) multiferroic response (both ferromagnetism and ferroelectricity) at room-temperature, through careful tuning of Fe valency along with the controlled-recovery of ferroelectric-tetragonal phase. We also report systematic increase in large dielectric constant values as well as reduction in loss tangent values with relatively moderate temperature variation of dielectric constant around room-temperature with increasing Bi doping content in Ba1-xBixTi0.9Fe0.1O3 (0

The effect of Sr doping in BaTiO3 (BTO) with nominal compositions Ba0.80Sr0.20TiO3 (BSTO) have been explored in its structural, lattice vibration, dielectric, ferroelectric and electrocaloric properties. The temperature dependent dielectric results elucidate the enhancement in dielectric constant and exhibit three frequency independent transitions around 335, 250 and 185 K which are related to different structural transitions. All these transitions occur at lower temperature as compared with pristine BTO, however; remnant electric polarization (P) of BSTO is much higher than in BTO. The value of P is around 5 microC/cm2 at room temperature and the maximum P around 8 microC/cm2 is observed at tetragonal to orthorhombic and orthorhombic to rhombohedral transitions. The electro-caloric effect shows the maximum adiabatic change in temperature deltaT approx 0.24 K at cubic to tetragonal transition. The temperature dependent synchrotron X-ray diffraction and Raman results shows correlations between P, crystal structure and lattice vibrations. Our results demonstrate the enhancement in ferroelectric properties of BTO with Sr doping. The origin of the enhancement in ferroelectric property is also discussed which is related to the appearance of superlattice peak around room temperature due to TiO6 octahedral distortion. These enhanced properties would be useful to design lead free high quality ferroelectric and piezoelectric materials., Comment: 22 pages, 7 figures

The effect of Cr doping with nominal compositions Mn2-xCrxO3 (0 less than equal to x less than equal to 0.10) has been undertaken to investigate its effect on structural, magnetic, dielectric and magnetoelectric properties. The Cr doping transformed the room temperature crystal structure from orthorhombic to cubic symmetry. Similar to alpha-Mn2O3, two magnetic transitions have been observed in the Cr doped samples. The effect of Cr doping is significant on the low temperature transition i.e. the lower magnetic transition shifted towards higher temperature (25 K for pristine to 40 K for x=0.10) whereas the high temperature transition decreases slightly with increasing Cr content. A clear frequency independent transition is observed in complex dielectric measurements for all compositions around high temperature magnetic ordering. Interestingly, the magnetodielectric behaviour enhanced enormously approx 21% with Cr substitution as compared to pristine Mn2O3., Comment: 13 pages, 2 tables, 4 figures

Simultaneous co-existence of room-temperature(T) ferromagnetism and ferroelectricity in Fe doped BaTiO$_3$ (BTO) is intriguing, as such Fe doping into tetragonal BTO, a room-T ferroelectric (FE), results in the stabilization of its hexagonal polymorph which is FE only below $\sim$80K. Here, we investigate its origin and show that Fe-doped BTO has a mixed-phase room-temperature multiferroicity, where the ferromagnetism comes from the majority hexagonal phase and a minority tetragonal phase gives rise to the observed weak ferroelectricity. In order to achieve majority tetragonal phase (responsible for room-T ferroelectricity) in Fe-doped BTO, we investigate the role of different parameters which primarily control the PE hexagonal phase stability over the FE tetragonal one and identify three major factors namely, the effect of ionic size, Jahn-Teller (J-T) distortions and oxygen vacancies (OVs), to be primarily responsible. The effect of ionic size which can be qualitatively represented using the Goldschmidt's tolerance (GT) factor seems to be the major dictating factor for the hexagonal phase stability. The understanding of these factors not only enables us to control them but also, achieve suitable co-doped BTO compound with enhanced room-T multiferroic properties., Comment: 15 pages, 17 figures

Multiferroics where at least two primary ferroic orders are present and coupled in a single system constitute an important class of materials. They attracted special consideration as they present both intriguing fundamental physics problems and technological importance for potential multifunctional devices. Here, we present the evidence of multiferroicity and magnetoelectric (ME) coupling in alpha-Mn2O3; a unique binary perovskite. Corresponding to the antiferromagnetic (AFM) ordering around 80K, a clear frequency independent transition is observed in the dielectric permittivity. We showed that electric polarization emerges near AFM regime that can be modulated with magnetic field. The detailed structural analysis using synchrotron radiation X-ray diffraction demonstrates the increase in structural distortion with decreasing temperature, as well as changes in the unit cell parameters and bond lengths across the ferroelectric and magnetic ordering temperatures. This observation of multiferroicity and magnetoelastic coupling in alpha-Mn2O3 provides insights for the exploration of ME coupling in related materials., Comment: Page 20 and 6 figures

The temperature (T) dependent x-ray diffraction (XRD) and resistivity measurements of La0.175Pr0.45Ca0.375MnO3 (LPCMO) have been performed down to 2K to understand the structural and transport properties. From room temperature down to 220K, LPCMO exists in orthorhombic phase with Pnma structure and at 220K, it transforms to charge ordered (CO) monoclinic phase with P21/m structure and remains as it is down to 2K. The CO phase is evident from the occurrence of weak but well defined superlattice peaks in the XRD pattern. This structural transformation is of first order in nature as evident from the phase coexistence across the transition region. These results thus clearly illustrate that LPCMO undergoes a first order structural phase transition from charge disordered orthorhombic phase to CO monoclinic phase at 220K, consistent with temperature dependent resistivity results. Our structural analysis of T dependent XRD data using Rietveld refinement infers that below 220K, LPCMO forms commensurate CO monoclinic P21/m structure with four times structural modulation., Comment: 2 pages, 3 figure, accepted in AIP conference procceding

The low-temperature and high-magnetic field (2K, 8T) powder x-ray diffraction (LTHM-XRD) measurements have been carried out at different temperatures (T) and magnetic fields (H) to investigate the structural phase diagram for phase separated La0.175Pr0.45Ca0.375MnO3 (LPCMO) manganite. The antiferromagnetic (AFM) P21/m insulating phase undergoes field induced transformation to ferromagnetic (FM) Pnma metallic ground state below its AFM ordering temperature (220K) in zero-field cooling (ZFC) from room temperature. At temperature greater than 25K, the field induced FM Pnma phase remained irreversible even after complete removal of field. However, for T ( 39-65K), the field induced transformation is partially reversible. This behaviour has been attributed to magnetic field induced devitrification of the glass-like arrested AFM P21/m phase to FM Pnma equilibrium phase. The devitrified FM Pnma phase starts transforming back to AFM P21/m phase around ~39K on heating the sample under zero field. Our results corroborate the evidence of strong magneto-structural coupling in this system. An H-T phase-diagram has been constructed based on LTHM-XTD data, which resembles with the one made from magnetic measurements. These results have been explained on the basis of kinetic arrest of first order phase transition and field induced devitrification of the arrested phase., Comment: 16pages, 6 figures, ON page no 5, line number 16 has been modified as, "The FM Pnma phase transforms back to AFM P21/m phase on heating"

We have carried out dc magnetization (M), heat-capacity (C) and dielectric studies down to 2K for the compound GdCrTiO5, crystallizing in orthorhombic Pbam structure, in which well-known multiferroics RMn2O5 (R= Rare-earths) form. The points of emphasis are: (i) The magnetic ordering temperature of Cr appears to be suppressed compared to that in isostructural Nd counterpart, NdCrTiO5, for which the Neel temperature is about 21 K. This finding on the Gd compound suggests that Nd 4f orbital plays a role on the magnetism of Cr in contrast to a proposal long ago. (ii) Dielectric constant does not exhibit any notable feature below about 30 K in the absence of external magnetic field, but a peak appears and gets stronger with the application of external magnetic fields, supporting the existence of magnetodielectric coupling. (iii) The dielectric anomalies appear even near 100 K, which can be attributed to short-range magnetic-order. We also observe a gain in spectral weight below about 150 K in Raman spectra in the frequency range 150 to 400 cm-1, which could be magnetic in origin supporting short-range magnetic order. It is of interest to explore whether geometrically frustration plays any role on the dielectric properties of this family, as in the case of RMn2O5., Comment: 15 pages, 6 figures, manuscript submitted

We report the existence of ferromagnetic correlations (FMC) in paramagnetic (PM) matrix of cubic La1-xSrxMnO3-{\delta} (x = 0.80, 0.85) well above its coupled structural, magnetic and electronic phase transitions. The dc-magnetization vs temperature [M(T)] behaviour under different magnetic fields (from 100 Oe to 70 kOe) shows the presence of short range magnetic correlations up to (TFMC ~) 365 K, far above the antiferromagnetic ordering temperatures (TN =) 260 K and 238 K for x=0.80 and 0.85, respectively. More importantly the observed short-range FMC survive even up to 70 kOe, which indicates their robust nature. The temperature region between TN to TFMC is dominated by the presence of correlated ferromagnetic (FM) entities within the PM matrix and stabilized due to A-site chemical disorder. Our results further illustrate that for the studied compositions, the oxygen off-stoichiometry does not have any significant effect on the nature and strength of these FM entities; however, FM interactions increase in the oxygen deficient samples. These compositions are the unique examples, where the presence of FMC is observed in an undistorted basic cubic perovskite lattice well above TN and therefore are novel to understand the physics behind the colossal magneto-resistance effect., Comment: Accepted in Physica status solidi (b), 19 Page, 5 figures

We report the magnetic, heat-capacity, dielectric and magnetodielectric (MDE) behaviour of a Haldane spin-chain compound containing light rare-earth ion, Nd2BaNiO5, in detail, as a function of temperature (T) and magnetic field (H) down to 2 K. In addition to the well-known long range antiferromagnetic order setting in at (T_N=) 48 K as indicated in dc magnetization (M), we have observed another magnetic transition near 10 K; this transition appears to be of a glassy-type which vanishes with a marginal application of external magnetic field (even H= 100 Oe). There are corresponding anomalies in dielectric constant as well with variation of T. The isothermal M(H) curves at 2 and 5 K reveal the existence of a magnetic-field induced transition around 90 kOe; the isothermal H-dependent dielectric constant also tracks such a metamagnetic transition. These results illustrate the MDE coupling in this compound. Additionally, we observe a strong frequency dependence of a step in T-dependent dielectric constant with this feature appearing around 25-30 K for the lowest frequency of 1 kHz, far below T_N. This is attributed to interplay between crystal-field effect and exchange interaction between Nd and Ni, which establishes the sensitivity of dielectric measurements to detect such effects. Interestingly enough, the observed dispersions of the T-dependent dielectric constant curves is essentially H-independent in the entire T-range of measurement, despite the existence of MDE coupling, which is in sharp contrast with other heavy rare-earth members in this series., Comment: AIP Advances, in Press. Supplementary Material is included

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 (below 8 K), that is, reentrant multiglass-like phenomenon, naturally suggesting the existence of an additional transition well below Neel temperature; ii) Magnetoelectric phase coexistence is observed at very low temperature (e.g., T =2K), where the high-field magnetoelectric phase is partially arrested on returning to zero magnetic field after a cycling through metamagnetic transition., Comment: J. Applied Physics, in press

We have investigated the magnetic, dielectric and magnetodielectric (MDE) behavior of a geometrically frustrated spin-chain system, Ca3Co1.4Rh0.6O6, in the single crystalline form for different orientations. The results bring out that the magnetic behavior of this compound is by itself interesting in the sense that this compound exhibits an anisotropic glassy-like magnetic behavior with a huge frequency dependence of ac susceptibility peak for an orientation along the spin-chain in the range 30-60 K; this behavior is robust to applications of large external magnetic fields (H) unlike in canonical spin-glasses. The temperature dependence of dielectric constant also shows strong frequency dependence with similar robustness to H. The isothermal H-dependent dielectric results at low temperatures establishes anisotropic MDE coupling. It is intriguing to note that there is a 'step' roughly at one-third of saturation values as in the case of isothermal magnetization curves for same temperatures (for orientation along spin-chain), a correlation hitherto unrealized for geometrically frustrated systems., Comment: Applied Physics Letters, in press. Supplementary Material is included

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 dielectric feature shifts towards lower temperatures with H, unlike the situation near T_N. This observation indicates that the alignment of spins by external magnetic fields tends to inhibit glassy-like slow electric-dipole dynamics, at least in this system, possibly arising from peculiarities in the magnetic structure., Comment: 11 pages, 5 figueres, JPCM (Fast Track Communication), in press

We bring out novel dielectric behavior of a spin-chain compound, Ca3Co2O6, undergoing Neel order at (T_N=) 24 K. It is found that the virgin curve in the plot of isothermal dielectric constant versus magnetic-field lies outside the 'butterfly-shaped' envelope curve well below T_N (e.g., 2.6 K), with a signature of a partial arrest of the high-field magnetoelectric ME) phase in zero-field after travelling through magnetic-field-induced magnetic transitions. This behavior is in contrast to that observed in the isothermal magnetization data. Thus, this work brings out a novel case for 'phase-coexistence phenomenon' due to ME coupling. Another strange finding is that there is a weak, but a broad, peak in dielectric constant around 85 - 115 K well above T_N, attributable to incipient spin-chain magnetic ordering. This finding should inspire further work to study ME coupling on artificial assemblies of magnetic chains, also keeping in mind miniaturization required for possible applications., Comment: Scientific Reports, 31st October 2013

We report the results of various measurements, namely magnetization, complex dielectric permittivity and electric polarization (P) on Dy2BaNiO5 as a function of temperature (T) and magnetic-field (H), apart from heat-capacity (C), with the primary motivation of exploring the existence of magnetoelectric (ME) coupling among Haldane spin-chain systems. The M(T) and C(T) data establish long range magnetic ordering at 58K. The most noteworthy observations are: (i) Distinct anomalies are observed in dielectric constant ({\epsilon}') vs T and loss (tan{\delta}) vs T at different temperatures, i.e. 12.5, 30, 50 and 58K; at low temperatures, three magnetic-field-induced transitions are observed in {\epsilon}' vs H at 6, 40 and 60 kOe. These transition temperatures and critical magnetic fields track those obtained from magnetization data. This establishes the existence of strong magnetoelectric coupling in this compound. (ii) Correspondingly, electric polarization could be observed as a function of T and H in the magnetically ordered state, thereby indicating magnetism-induced ferroelectricity in this compound; this result suggests that this compound is a possible new multiferroic material among spin = 1 (nickel containing) compounds with successive magnetic transitions and strong magnetoelectric coupling., Comment: 22 pages, 5 figures Accepted in Physical Rev. B

Ferroelectricity in the incommensurate helical magnetic phase (below TN, 43K) of alpha CaCr2O4 has been confirmed by pyroelectric measurements. Magnetoelectric and magnetodielectric coupling exist below TN and are proportional to the square of magnetic field. From symmetry analysis, we suggest that the presence of an external electric field destabilizes the symmetrical 2221' phase and stabilizes 21' symmetry. This provides a unique system in which polarization varies as the fourth-degree of the order-parameter amplitude and exhibit a vanishingly small value below the first-order transition at TN, as observed experimentally., Comment: 14 pages, 4 figures

Dielectric response has been studied for a new manganocuprate, Gd3Ba2Mn2Cu2O12 (Gd3222) as a function of temperature (100 - 300 K) and frequency (75 kHz to 1 MHz). The dielectric constant (e) exhibits a two step increase (two peaks) in e(T) with increasing temperature from 100 to 300 K. The first peak is seen around 150 K and the second one around 210 K (both for 75 kHz). Increasing frequency shifts both the peaks to higher temperature side. The behavior of dielectric constant (e) and dielectric loss (tan_delta) matches with glassy behavior observed in many dipolar molecules., Comment: 1 PDF file, Submitted

The manganocuprate compound Gd3Ba2Mn2Cu2O12 (Gd-3222) has been synthesized by conventional solid state reaction method and its magnetic behavior has been studied by dc and ac magnetization (M) and heat capacity (C) measurements as a function of temperature (T). This compound crystallizes in a tetragonal structure (space group I4/mmm). We find that this compound exhibits three magnetic transitions, around 2.5, 4.8 and 9 K, as inferred from dc and ac magnetic susceptibility (chi) data. However, no evidence for a well-defined lambda-anomaly is found in C(T) above 1.8 K, though there is a gradual upturn below about 10 K. An application of a magnetic field results in a peak around 5K, while ac chi appears to show a very weak frequency dependence below 9 K. Isothermal M curve at 1.8 K exhibits a weak hysteresis without any evidence for saturation even at fields as high as 120 kOe. These results imply that this compound undergoes a spin-glass-like freezing at low temperatures, though the exact nature of the magnetic transition at 10 K is not clear. The magnitude of the magnetocaloric effect, as inferred from M and C data, is quite large over a wide temperature range below 50 K peaking around 4 K., Comment: 1 PDF file, 8 Figures, 18 pages