arXiv subjects

E. V. Sampathkumaran

Publications and source records attributed to E. V. Sampathkumaran.

At least 55 records · Page 3Linked to original sources

arXiv2016

Frustrated Ising chains on the triangular lattice in Sr$_3$NiIrO$_6$

Inelastic neutron scattering study on the spin-chain compound Sr$_3$NiIrO$_6$ reveals gapped quasi-1D magnetic excitations. The observed one-magnon band between 29.5 and 39 meV consists of magnon modes of the Ni$^{2+}$ ions. The fitting of the spin wave spectrum reveals strongly coupled Ising-like chains along the $c$-axis that are weakly coupled into a frustrated triangular lattice in the $ab$-plane. The magnetic excitations survive up to 200 K well above the magnetic ordering temperature of $T_N \sim 75$ K, also indicating a quasi-1D nature of the magnetic interactions in Sr$_3$NiIrO$_6$. Our microscopic model is in good agreement with ab initio electronic structure calculations and explains the giant spin flip field observed in bulk magnetization measurements.

cond-mat.str-el↗

arXiv2016

Dielectric anomalies and magnetodielectric coupling behavior of single crystalline Ca3Co2O6, a geometrically frustrated magnetic spin-chain system

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, thereby providing evidence for strong anisotropic spin-glass behavior. Interestingly, the strong frequency dependence in dielectric is present for both the crystallographic directions (E parallel c and E perpendicular c where E is the electric field) with a negligible influence of H, despite the existence of MDE coupling. This result appears to suggest different dynamics of electric dipole and spin-glass, although they are coupled with each other. In addition, interestingly, there is also a step at one-third of high-(magnetic) field value of MDE at some temperatures tracking a similar step in M(H). This work also confirms following unusual features reported on polycrystals, when measured along c-axis. The dielectric constant exhibits a broad peak around 50-130 K when the electric field is applied along the spin-chain (crystallographic c direction); however this feature is essentially absent for the perpendicular orientation. This finding supports the role of incipient spin-chain ordering to induce magnetodielectric coupling. There is a signature of magnetoelectric phase coexistence when the magnetic field is applied along the spin-chain irrespective of the direction of applied electric field.

cond-mat.mtrl-sci↗

arXiv2015

Complex dielectric and impedance behavior of magnetoelectric Fe2TiO5

We have investigated the complex dielectric and impedance properties of magnetoelectric compound Fe2TiO5 (FTO) as a function of temperature (T) and frequency (f) to understand the grain (G) and grain boundary (Gb) contributions to its dielectric response. The temperature and frequency dependent dielectric permittivity data shows a sharp increase in permittivity above 200K accompanied with a frequency dependent peak in loss. At T less than 175K, only G contribution dominates even at lower frequency (nearly 100Hz), but for T greater than 175K, the Gb contribution starts appearing at low frequency. The value of critical frequency distinguishing these two contributions increases with increasing temperature. The observed non-Debye dielectric relaxation follows thermally activated process and is attributed to polaron hopping. Further the frequency dependence of ac conductivity follows the Jonscher power-law. The temperature dependency of critical exponent s shows that the correlated barrier hopping model is appropriate to define the conductivity mechanism of FTO in the studied temperature regime.

cond-mat.mtrl-sci↗

arXiv2015

Magnetic and magnetotransport behavior of RFe5Al7 (R= Gd and Dy): Observation of re-entrant inverse-magnetocaloric phenomenon and asymmetric magnetoresistance behavior

We have compared and contrasted magnetic, magnetocaloric and magnetoresistive properties of Gd and Dy members of the rare-earth (R) series RFe5Al7, crystallizing in ThMn12 structure, known to order antiferromagnetically. Among other observations, we would like to emphasize on the following novel findings: (i) There are multiple sign-crossovers in the temperature (T) dependence of isothermal entropy change (DeltaS) in the case of Dy compound; in addition to nil DeltaS at the magnetic compensation point known for two-magnetic-sublattice systems, there is an additional sign-crossover at low temperatures, as though there is a re-entrant inverse magnetocaloric phenomenon. Corresponding sign reversals could also be observed in the magnetoresistance data. (ii) The plots of magnetoresistance versus magnetic field are found to be highly asymmetric with the reversal of the direction of magnetic-field (H) well below TN for both compounds, similar to that known for an antiferromagnetic tunnel junctions. We attribute these to subtle changes in spin orientations of R and Fe moments induced by T and H.

cond-mat.str-el↗

arXiv2015

Implications of magnetic and magnetodielectric behavior of GdCrTiO5

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.

cond-mat.mtrl-sci↗

arXiv2015

Magnetic and magnetodielectric coupling anomalies in the Haldane spin-chain system Nd2BaNiO5

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.

cond-mat.mtrl-sci↗

arXiv2015

Giant gap in the magnon excitations of the quasi-1D chain compound Sr3NiIrO6

Inelastic neutron scattering on the spin-chain compound Sr$_3$NiIrO$_6$ reveals gapped quasi-1D magnetic excitations. The observed one-magnon band between 29.5 and 39 meV consists of two dispersive modes. The spin wave spectrum could be well fitted with an antiferromagnetic anisotropic exchange model and single ion anisotropy on the Ni site. The extracted dominant anisotropic antiferromagnetic intra-chain exchange interaction between Ir and Ni ions are $J_z=19.5$ meV and $J_{xy}=12.1$ meV. These values justify previous electronic structure calculations, showing the importance of Ir spin orbit coupling on the electron correlations. The magnetic excitations survive up to 200 K well above the magnetic ordering temperature of $T_N \sim 70$ K, also indicating a quasi-1D nature of the magnetic interactions in Sr$_3$NiIrO$_6$. Our results not only support the idea of the existence of a new temperature scale well above $T_N$, but also emphasize the need to consider new exchange paths complicated by the SOC, resulting in additional characteristic temperatures in such spin-chain systems.

cond-mat.str-el↗

arXiv2014

Electronic structure of La(2)CoSi(3) - a non-Kondo analogue of a Kondo lattice, Ce(2)CoSi(3)

We study the electronic structure of a Pauli paramagnetic compound, La(2)CoSi(3) using photoemission spectroscopy and ab initio band structure calculations. Experimental valence band spectra exhibit signature of electron correlation induced feature around 2.5 eV - the correlation strength among Co 3d electrons is estimated to be close to 3 eV. The Co 2p core level spectra also exhibit correlation induced satellite features consistent with the scenario in the valence band spectra suggesting importance of conduction electron correlation in addition to the local moment in Kondo lattice systems. The La(2)CoSi(3) valence band spectra could be utilized to extract Ce 4f related spectral features and thus provide a good reference to study Kondo lattice systems in this class of materials. Temperature evolution of various core level spectra is found to be complex revealing deviations from a typical Fermi liquid behavior and emergence of distinct surface-bulk difference in the electronic structure at finite temperature.

cond-mat.str-el↗

arXiv2014

Multiglass properties and magnetoelectric coupling in uniaxial anisotropic spin-cluster-glass Fe2TiO5

The compound, Fe2TiO5 (FTO)is a well-known uniaxial anisotropic spin-glass insulator with two successive glassy freezing temperatures i.e. transverse (TTF= 9K) and longitudinal (TLF= 55 K). In this article, we present the results of measurements of complex dielectric behavior, electric polarization as a function of temperature (T), in addition to characterization by magnetic susceptibility and heat-capacity, primarily to explore magnetoelectric (ME) coupling and multiglass properties in uniaxial anisotropic spin cluster-glass FTO. The existence of two magnetic transitions is reflected in the isothermal magnetodielectric (MD) behavior in the sense that the sign of MD is different in the T regime T TTF.The data in addition provide evidence for the glassy dynamics of electric-dipoles; interestingly, this occurs at much higher temperature (~100-150 K) than TLF with high remnant polarization at 10 K( 4000 micro C/m2) attributable to short-range magnetic correlations, thereby offering a route to attain ME coupling above 77 K.

cond-mat.mtrl-sci↗

arXiv2014

Magnetic and dielectric behavior of the spin-chain compound Er2BaNiO5 well below its Néel temperature

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.

cond-mat.str-el↗

arXiv2014

Anisotropic magnetodielectric coupling behavior of Ca3Co1.4Rh0.6O6 due to geometrically frustrated magnetism

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.

cond-mat.str-el↗

arXiv2014

Multiferroicity and magneto-electric effect in Gd$_2$BaNiO$_5$

We report the observation of electric polarization in the magnetically ordered state of the Haldane chain compound, Gd$_2$BaNiO$_5$, with strongly correlated magnetic and dielectric properties. The results of dc magnetic susceptibility and heat capacity measurements indicate two magnetic transitions,one corresponding to the anti-ferromagnetic order at T$_N$ around 55 K and the other to spin-reorientation transition at T$_{SR}$ around 24 K. The dielectric permittivity ($ε'$) and loss (tan$δ$) also exhibit anomalies in the vicinity of T$_{SR}$ and T$_N$ respectively. Below the spin-reorientation transition, concurrently magnetic-field-induced spin-flop and the meta-electric transitions are observed at a critical magnetic field in isothermal magnetization and magneto-dielectric results respectively. Another interesting finding is that the change in dielectric constant changes its sign at the critical magnetic field. The origin of the observed magneto-electric effect is discussed on the basis of spin-phonon coupling.

cond-mat.mtrl-sci↗

arXiv2014

Displacive-type ferroelectricity from magnetic correlations within spin-chain

Observation of ferroelectricity among non-d0 systems, which was believed for a long time an unrealistic concept, led to various proposals for the mechanisms to explain the same (i.e. magnetically induced ferroelectricity) during last decade. Here, we provide support for ferroelectricity of a displacive-type possibly involving magnetic ions due to short-range magnetic correlations within a spin-chain, through the demonstration of magnetoelectric coupling in a Haldane spin-chain compound Er2BaNiO5 well above its Néel temperature of (TN=) 32K. There is a distinct evidence for electric polarization setting in near 60 K around which there is an evidence for short-range magnetic correlations from other experimental methods. Raman studies also establish a softening of phonon modes in the same temperature (T) range and T-dependent x-ray diffraction (XRD) patterns also reveal lattice parameters anomalies. Density-functional theory based calculations establish a displacive component (similar to d0-ness) as the root-cause of ferroelectricity from (magnetic) NiO6 chain, thereby offering a new route to search for similar materials near room temperature to enable applications.

cond-mat.str-el↗

arXiv2014

Magnetic order in the frustrated Ising-like chain compound Sr$_3$NiIrO$_6$

We have studied the field and temperature dependence of the magnetization of single crystals of Sr3NiIrO6. These measurements evidence the presence of an easy axis of anisotropy and two anomalies in the magnetic susceptibility. Neutron powder diffraction realized on a polycrystalline sample reveals the emergence of magnetic reflections below 75 K with magnetic propagation vector k ~ (0, 0, 1), undetected in previous neutron studies [T.N. Nguyen and H.-C zur Loye, J. Solid State Chem., 117, 300 (1995)]. The nature of the magnetic ground state, and the presence of two anomalies common to this family of material, are discussed on the basis of the results obtained by neutron diffraction, magnetization measurements, and symmetry arguments.

cond-mat.str-el↗

arXiv2014

A reentrant phenomenon in magnetic and dielectric properties of Dy2BaNiO5 and an intriguing influence of external magnetic field

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.

cond-mat.str-el↗

arXiv2013

Novel dielectric anomalies due to spin-chains above and below Neel temperature in Ca3Co2O6

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.

cond-mat.mtrl-sci↗

arXiv2013

Modifications in the frustrated magnetism, oxidation state of Co and magnetoelectric coupling effects induced by a partial replacement of Ca by Gd in the spin chain compound Ca3Co2O6

We have systematically investigated the influence of gradual replacement of Ca by Gd on the magnetic and complex dielectric properties of the well-known geometrically frustrated spin-chain system, Ca3Co2O6 (T_N= 24 K with additional magnetic transitions below 12K), by studying the series, Ca3-xGdxCo2O6 (x less than 0.7), down to 1.8K. Heat capacity measurements establish that the reduction of T_N with Gd substitution is much less as compared to that by Y substitution. The magnetic moment data reveal that there are changes in the oxidation state of Co as well, unlike for Y-substitution, beyond x= 0.2. Thus, despite being isovalent, both these substitutions interestingly differ in changing these magnetic properties in these oxides. We propose that the valence electrons of Y and those of R ions play different roles on deciding these magnetic characteristics of these mixed oxides. It is observed that a small amount (x= 0.3) of Gd substitution for Ca is enough to suppress glassy ac magnetic susceptibility behavior for the peak around 12 K. An additional low-temperature magnetic anomaly close to 5 K gets more prominent with increasing Gd concentration as revealed by heat-capacity data. Trends in temperature dependence of complex dielectric behavior were also tracked with varying composition and a frequency dependence is observed, not only for the transition in the region around 10 K (for some compositions), but also for the 5 K transition which is well-resolved for a higher concentration of Gd. Thus, Gd-substituted Ca3Co2O6 series is shown to reveal interesting magnetic and dielectric behavior of this family of oxides.

cond-mat.str-el↗

arXiv2013

Magnetoelectric coupling in Haldane spin chain system, Dy2BaNiO5

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 (ε') vs T and loss (tanδ) vs T at different temperatures, i.e. 12.5, 30, 50 and 58K; at low temperatures, three magnetic-field-induced transitions are observed in ε' 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.

cond-mat.mtrl-sci↗