arXiv subjects

E. V. Sampathkumaran

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

At least 37 records · Page 2Linked to original sources

arXiv2019

Extraordinarily large intrinsic magnetodielectric coupling of Tb member within the Haldane spin-chain family, R2BaNiO5

The Haldane spin-chain compound, Tb2BaNiO5, has been known to order antiferromagnetically below (T_N= ) 63 K. The present magnetic studies on the polycrystals bring out that there is another magnetic transition at a lower temperature (T_2= ) 25 K, with a pronounced magnetic-field induced metamagnetic and metaelectric behavior. Multiferroic features are found below T_2 only, and not at T_N. The most intriguing observation is that the observed change of dielectric constant is intrinsic and largest (e.g., about 18% at 15 K) within this Haldane spin-chain family, R2BaNiO5. Taking into account that this trend (the largest change for Tb case within this family) correlates with a similar trend in T_N (with the values of T_N being about 55, 58, 53 and 32 K for Gd, Dy, Ho and Er cases), we believe that an explanation usually offered for this T_N behavior in rare-earth systems is applicable for this behavior as well . That is, single-ion anisotropy following crystal-field splitting is responsible for this extraordinary magnetodielectric effect in this Tb case. To our knowledge, such an observation was not made in the past literature of multiferroics.

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arXiv2019

Existence of a critical canting angle of magnetic moments to induce multiferroicity in the Haldane spin-chain system, Tb2BaNiO5

We report an unusual canted magnetism due to 3d and 4f electrons, occupying two different crystallographic sites, with its consequence to electric dipole order. This is based on neutron powder diffraction measurements on Tb2BaNiO5 (orthorhombic, Immm centrosymmetric space group), exhibiting Neel order below (TN) 63 K, to understand multiferroic behavior below 25 K. The magnetic structure is made up of Ni and Tb magnetic moments, which are found to be mutually canted in the entire temperature range below TN, though collinearity is seen within each sublattice, as known in the past. First-principles density functional theory calculations (GCA plus SO and GCA plus U plus SO approximations) support such a canted ground state. The intriguing finding, being reported here, is that there is a sudden increase in this Tb-Ni relative cantingle angle at the temperature (that is, at 25 K) at which spontaneous electric polarization sets in, with bond distance and bong angle anomalies. This finding emphasizes the need for a new spin-driven polarization mechanism, that is, a critical canting angle coupled with exchangestriction, to induce multiferroicity in magnetic insulators with canted spins.

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arXiv2019

Neutron diffraction study of a metallic kagome lattice, Tb3Ru4Al12

We present the results of neutron diffraction studies on polycrystals of a metallic kagome lattice, Tb3Ru4Al12, reported recently to undergo reentrant magnetism, with the onset of long range antiferromagnetic order below (TN=) 22 K and spin-glass features below about 17 K. The present results reveal long-range antiferromagnetic order of an incommensurate type with the moments oriented along c-axis at all temperatures below TN. There are however notable changes in the T dependence of propagation vector along b-axis across 17 K. An observation of interest is that there is no decrease of intensity of magnetic Bragg peaks on entrance into the glassy phase (that is, below 17 K). This finding suggests that the magnetism of this compound is an exotic one and we wonder whether this compound is an example for dynamical spin-glass freezing phenomenon, as a consequence of geometrical frustration.

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arXiv2019

Anisotropic re-entrant spin-glass features in a metallic kagome lattice, Tb3Ru4Al12

We report the results of ac and dc magnetic susceptibility and isothermal magnetization measurements (T= 2-300 K) on the single crystals of a metallic kagome lattice, Tb3Ru4Al12, reported recently to undergo reentrant magnetism with the onset of long range antiferromagnetic order below (TN=) 22K. The magnetization data obtained on the crystal with the c-axis orientation along magnetic-field reveal spin-glass-like characteristics near 17 K (below TN). However, for the orientation along basal plane, such glassy anomalies are not observable above 2 K. In this respect, this compound behaves like an anisotropic reentrant spin-glass. Possible implications of this finding to the field of geometrically frustrated magnetism is considered.

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arXiv2018

Eu valence transition behavior in the nano form of EuPd2Si2

The compound EuPd2Si2 is a well-known valence-fluctuating compound with a largest variation of Eu valence in a narrow temperature interval (around 150 K). The ball-milled form of this compound was investigated to understand the Eu valence behavior in the nanoform. The compound is found to retain the ThCr2Si2-type tetragonal structure after ball-milling leading to a reduction in particle size, typically falling in the range 10 - 100 nm. We find that there is a qualitative change in the temperature dependence of magnetic susceptibility for such small particles, with respect to that known for bulk form. To understand this microscopically, Mossbauer spectra as a function of temperature were taken. The Mossbauer spectrum of the nanocrystalline compound is essentially divalent-like at room temperature, but becomes distinctly bimodal at all temperatures below 300 K, unlike that of the bulk form. That is, there is a progressive transfer of intensity from divalent position to trivalent position with a gradual decrease of temperature. We attribute it to a first-order valence transition, with extreme broadening by defects in the nano specimen. Thus, there is a qualitative change in the valence behavior in this compound as the particle size is reduced by ball-milling. Such a particle size study is reported for the first time for a Eu-based mixed-valent compound.

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arXiv2018

Multiferroicity in a spin-chain compound, Tb2BaCoO5, with exceptionally large magnetodielectric coupling in polycrystalline form

We report the results of detailed investigations of magnetization, heat-capacity, dielectric, pyrocurrent, and magneto(di)electric measurements on Tb2BaCoO5, belonging to a hither-to-unexplored spin-chain cobaltates family, R2BaCoO5 (R= Rare-earths). The magnetic measurements reveal that this compound exhibits an antiferromagnetic transition at (T_N=) 18.8 K and there is a spin-reorientation beyond 40 kOe below T_N. Dielectric and pyrocurrent data measured as a function of temperature and magnetic-field establish that this compound is a type-II multiferroic material. The most fascinating finding which we would like to emphasize is that the observed value of the magnetodielectric effect beyond the metamagnetic transition field is the largest (close to 55%, below 10 K, for H= 100 kOe) ever reported for polycrystals of a compound in bulk form, thereby offering a hope to find a single-phase polycrystalline compound at room temperature to enable ease of applications.

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arXiv2017

Complex nature of magnetic field-induced ferroelectricity in GdCrTiO5

This work shows an unconventional route for spin-driven ferroelectricity originating from a metastable magnetic field-induced canting of chromium sublattice in the presence of gadolinium moments in GdCrTiO5 at low temperatures. Compared to the isostructural neodymium compound, significant differences of magnetism and magnetoelectric effects are seen. We present the results of thorough investigations of temperature and magnetic field dependent magnetization as well as ac and dc magnetic susceptibility. These bulk measurements are complemented by local-probe spectroscopy utilizing electron-spin resonance and muon-spin rotation/relaxation for probing the chromium moments. Ferroelectric order is inferred from pyro- and magnetocurrent measurements. GdCrTiO5 shows a pyrocurrent signal around 10 K, only if the system is cooled in an applied magnetic field exceeding 10 kOe. A distinct spin-driven ferroelectric order is revealed in this state for temperatures below 10 K, which can be switched by changing magnetic-field direction and the polarity of the electric field. But, the magnetic measurements reveal no clear signature of long-range magnetic ordering. The presence of such meta-magnetoelectric-type behaviour in the absence of any meta-magnetic behavior is rare in the literature. Our microscopic spectroscopy results indicate significant changes of the magnetic properties around 10 K. Probably there is an exchange frustration between Gd and Cr moments, which prevents long-range magnetic ordering at further high temperature. Below 10 K, weak magnetic ordering occurs by minimizing frustration due to lattice distortion, which helps in magnetodielectric coupling. However, the non-polar distortion attains appreciable values after application of magnetic fields above 10 kOe to break the spatial inversion symmetry, which creates ferroelectricity.

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arXiv2017

Dielectric and multiferroic behavior in a Haldane spin-chain compound Sm2BaNiO5 due to an interplay between crystal-field effect and exchange interaction

The Haldane spin-chain (S=1) insulating compound, Sm2BaNiO5, which has been proposed to order antiferromagnetically around (T_N=) 55 K, was investigated for its complex dielectric permittivity, magnetodielectric and pyrocurrent behavior as a function of temperature (T). In order to enable meaningful discussions, the results of ac and dc magnetizatioin and heat-capacity studies are also reported. We emphasize on the following findings: (i) There is a pyrocurrent peak near T_N, but it is shown not to arise from ferroelectricity, but possibly due to 'thermally stimulated depolarization current', unlike in many other members of this rare-earth series, in which case ferroelectric features were reported at or above T_N; (ii) however, the pyrocurrent measured in the presence of a bias electric field (after cooling in zero electric field) as well as dielectric constant reveal a weak peak with increasing T around 22 K - the temperature around which population of the exchange-split excited state of Kramers doublet has been known to occur. This finding suggests that this compound presents a novel situation in which multiferroicity is induced by an interplay between crystal-field effects and exchange interaction. No multiglass features could be observed down to 2 K unlike in many members of this family.

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arXiv2017

Magnetic behavior of new compounds, Gd3RuSn6 and Tb3RuSn6

We report temperature (T) dependence of dc magnetization, electrical resistivity (rho(T)), and heat-capacity of rare-earth (R) compounds, Gd3RuSn6 and Tb3RuSn6, which are found to crystallize in the Yb3CoSn6-type orthorhombic structure (space group: Cmcm). The results establish that there is an onset of antiferromagnetic order near (T_N) 19 and 25 K respectively. In addition, we find that there is another magnetic transition for both the cases around 14 and 17 K respectively. In the case of the Gd compound, the spin-scattering contribution to rho is found to increase below 75 K as the material is cooled towards T_N, thereby resulting in a minimum in the plot of rho(T) unexpected for Gd based systems. Isothermal magnetization at 1.8 K reveals an upward curvature around 50 kOe. Isothermal magnetoresistance plots show interesting anomalies in the magnetically ordered state. There are sign reversals in the plot of isothermal entropy change versus T in the magnetically ordered state, indicating subtle changes in the spin reorientation with T. The results reveal that these compounds exhibit interesting magnetic properties.

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arXiv2017

Magnetic behavior of metallic kagome lattices, Tb3Ru4Al12 and Er3Ru4Al12

We report magnetic behavior of two intermetallics-based kagome lattices, Tb3Ru4Al12 and Er3Ru4Al12, crystallizing in the Gd3Ru4Al12-type hexagonal crystal structure, by measurements in the range 1.8-300 K with bulk experimental techniques (ac and dc magnetization, heat-capacity and magnetoresistance). The main finding is that the Tb compound, known to order antiferromagnetically below (T_N=) 22 K, shows glassy characteristics at lower temperatures (<15K), thus characterizing this compound as a re-entrant spin-glass. The data reveal that glassy phase is quite complex and is of a cluster type. Since the glassy behavior was not seen for the Gd analogue in the past literature, this finding for the Tb compound emphasizes that this kagome family could provide an opportunity to explore the role of higher order (such as quadrupole) in bringing out magnetic frustration. Additional findings reported here for this compound are: (i) The temperature dependence of magnetic susceptibility and electrical resistivity in the range 12 - 20 K are found to be hysteretic leading to a magnetic phase in this temperature range, mimicking disorder-induced first-order magnetic phase-transition. (ii) Features attributable to an interesting magnetic phase co-existence phenomenon in the magnetoresistance in zero field, after cycling across metamagnetic transition fields, are observed. With respect to the Er compound, we do not find any evidence for long-range magnetic ordering down to 2 K, but this appears to be on the verge of magnetic order at 2 K.

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arXiv2017

Relaxor ferroelectric behavior and intrinsic magnetodielectric behavior near room temperature in Li2Ni2Mo3O12, a compound with distorted honeycomb and spin-chains

Keeping current interests to identify materials with intrinsic magnetodielectric behavior near room temperature and with novel pyroelectric current anomalies, we report temperature and magnetic-field dependent behavior of complex dielectric permittivity and pyroelectric current for an oxide, Li2Ni2Mo3O12, containing magnetic ions with (distorted) honey-comb and chain arrangement and ordering magnetically below 8 K. The dielectric data reveal the existence of relaxor ferroelectricity behavior in the range 160-240 K and there are corresponding Raman mode anomalies as well in that temperature range. Pyrocurrent behavior is also consistent with this interpretation, with the pyrocurrent peak-temperature interestingly correlating with the poling temperature. 7Li NMR offer an evidence for crystallographic disorder intrinsic to this compound and we therefore conclude that such a disorder is apparently responsible for the randomness of local electric field leading to relaxor ferroelectric property. Another observation of emphasis is that there is a notable decrease in the dielectric constant with the application of magnetic field to the tune of about -2.4% at 300 K, with the magnitude varying mariginally with temperature. Small loss factor values validate intrinsic behavior of the magnetodielectric effect at room temperature.

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arXiv2017

Re-entrant spin-glass freezing and magneto-dielectric behavior of Li3NiRuO6, a layered rock-salt related oxide

We report the results of neutron diffraction, ac and dc magnetization, heat-capacity, complex permittivity, and pyrocurrent measurements on an oxide, Li3NiRuO5, hitherto not paid much attention in the literature, except for a previous report on its promising electrochemical performance. We emphasize on the following findings: (i) Observation of re-entrant spin-glass behavior; that is, this oxide undergoes ferrilmagnetic ordering below 8- K, entering spin-glass regime around 12 K. (ii) There is no prominent feature in the complex dielectric permittivity (in particular, at the magnetic transitions) in the absence of external magnetic field, indicative of the absence of ferroelectricity. However, there is a distinct evidence for magneto-dielectric (MDE) coupling. The sign of MDE coupling also changes as the sample is cooled from ferrimagnetic state to spin-glass regime. (iii) There are pyroelectric anomalies in the vicinity of 30-70 K, presumably from thermally stimulated depolarization current.

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arXiv2016

Effect of rare-earth (Er and Gd) substitution on the magnetic and multiferroic properties of DyFe0.5Cr0.5O3

We report the results of our investigations on the influence of partial substitution of Er and Gd for Dy on the magnetic and magnetoelectric properties of DyFe0.5Cr0.5O3, which is known to be a multiferroic system. Magnetic susceptibility and heat capacity data, apart from confirming the occurrence of magnetic transitions at ~ 121 and 13 K in DyFe0.5Cr0.5O3, bring out that the lower transition temperature only is suppressed by rare-earth substitution. Multiferroic behavior is found to persist in Dy0.4Ln0.6Fe0.5Cr0.5O3 (Ln= Er and Gd). There is an evidence for magnetoelectric coupling in all these materials with qualitative differences in its behavior as the temperature is changed across these two transitions. Remnant electric polarization is observed for all the compounds. The most notable observation is that electric polarization is seen to get enhanced as a result of rare-earth substitution with respect to that in DyFe0.5Cr0.5O3. Interestingly, similar trend is seen in magnetocaloric effect, consistent with the existence of magnetoelectric coupling. The results thus provide evidence for the tuning of magnetoelectric coupling by rare-earth substitution in this family of oxides.

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arXiv2016

Spin-glass behavior and pyroelectric anomalies in a new lithium-based oxide, Li3FeRuO5

The results of dc and ac magnetization, heat-capacity, 57Fe Moessbauer spectroscopy, dielectric, pyroelectric current and isothermal magneto-capacitance measurements on a recently reported lithium-based oxide, Li3FeRuO6, related to LiCoO2-type rhombohedral structure (space group, R-3m) are presented. The results reveal that the compound undergoes spin-glass freezing below 15 K. There is a peak around 34 K in pyroelectric data, which can not be attributed to ferroelectricity, but to the phenomenon of thermally stimulated depolarization current. As revealed by magnetocapacitance data above and below magnetic ordering temperature, magnetic and electric dipoles appear to be coupled, thereby offering evidence for magnetodielectric coupling.

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arXiv2016

A rock-salt type Li-based oxide, Li3Ni2RuO6, exhibiting a chaotic ferrimagnetism with cluster spin-glass dynamics and thermally frozen charge carriers

The area of research to discover new Li containing materials and to understand their physical properties has been of constant interest due to applications potential for rechargeable batteries. Here, we present the results of magnetic investigations on a Li compound, Li3Ni2RuO6, which was believed to be a ferrimagnet below 80K. While our neutron diffraction (ND) and isothermal magnetization (M) data support ferrimagnetism, more detailed magnetic studies establish that this ferrimagnetic phase exhibits some features similar to spin-glasses. In addition, we find another broad magnetic anomaly around 40-55 K in magnetic susceptibility, attributable to cluster spin-glass phenomenon. Gradual dominance of cluster spin-glass dynamics with a decrease of temperature (T) and the apparent spread in freezing temperature suggest that the ferrimagnetism of this compound is a chaotic one. The absence of a unique freezing temperature for a crystalline material is interesting. In addition, pyroelectric current data reveals a feature in the range 40-50 K, attributable to thermally stimulated depolarization current. We hope this finding motivates future work to explore whether there is any intriguing correlation of such a feature with spin-glass dynamics. We attribute these magnetic and electric dipole anomalies to the crystallographic disorder intrinsic to this compound.

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arXiv2016

Magnetism of a rhombohedral-type pyrochlore-derived Kagome series, Mn2R3Sb3O14 (R= Rare-earths)

The results of magnetic investigations on a new series of compounds, Mn2R3Sb3O14, containing 2-dimensional Kagome lattice of R ions and belonging to pyrochlore series, are presented. Crystallographic features of light R members (R= La, Pr and Nd) of this family, as established in the recent literature, have been reported to be novel in many respects, in particular, the rhomohedral nature of the structure which is rare among pyrochlores. It was also reported that, as the R becomes heavier, beyond R= Sm, the fraction of well-known cubic pyrochlore phase tends to gradually dominate. Here, we report that we are able to form the Gd member in the rhombohedral form without noticeable admixture from the cubic phase. With respect to magnetic behavior, our magnetization measurements on the La member reveal that Mn exists in divalent state without any evidence for long range magnetic ordering down to 2 K (that is, suppressed magnetism), which is not so common for Mn based oxides, though antiferromagnerism below 2 K is not ruled out. Nd and Gd members, are however, found to show distinct features above 2 K in magnetic susceptibility and heat-capacity, attributable to long-range magnetic ordering from respective rare-earth sublattice. The experimental results with respect to magnetism are found to be consistent with the results from ab initio band structure calculations performed for the La case. The calculations imply that electron correlation is important to describe insulating behavior.

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arXiv2016

Magnetic behavior of Gd3Ru4Al12, a layered compound with a distorted Kagome net

The magnetic behavior of the compound, Gd3Ru4Al12, which has been reported to crystallize in a hexagonal structure about two decades ago, had not been investigated in the past literature despite interesting structural features (that is, magnetic layers and triangles as well as Kagome-lattice features favouring frustrated magnetism) characterizing this compound. We report here the results of magnetization, heat-capacity, and magnetoresistance studies in the temperature (T) range 1.8-300 K. The results establish that there is a long-range magnetic order of an antiferromagnetic type below (TN= ) 18.5 K, despite a much large value (about 80 K) of paramagnetic Curie temperature with a positive sign characteristic of ferromagnetic interaction. We attribute this to geometric frustration. The most interesting finding is that there is an additional magnetic anomaly below about 55 K before the onset of long range order in the magnetic susceptibility data. Concurrent with this observation, the sign of isothermal entropy change remains positive above TN with a broad peak above TN. This observation indicates the presence of ferromagnetic clusters before the onset of long range magnetic order. Thus, this compound may serve as an example for a situation in which magnetic frustration due to geometrical reasons is faced by competition with such precursor effects. There is also a reversal of the sign of entropy-change in the curves for lower final fields (for H less than 30 kOe) on entering into magnetically ordered state consistent with the entrance into antiferromagnetic state. The magnetoresistance behavior is consistent with above conclusions.

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arXiv2016

Insight into the magnetism of a distorted Kagome lattice, Dy3Ru4Al12, based on polycrystalline studies

The layered compound with distorted Kagome nets, Dy3Ru4Al12, was previously reported to undergo antiferromagnetic ordering below (TN=) 7 K, based on investigations on single crystals. Here, we report the results of our investigation of ac and dc magnetic susceptibility (\c{hi}), isothermal remnant magnetization (MIRM), heat-capacity, magnetocaloric effect and magnetoresistance measurements on polycrystals. The present results reveal that there is an additional magnetic anomaly around 20 K, as though the Néel order is preceded by the formation of ferromagnetic clusters. We attribute this feature to geometric frustration of magnetism. In view of the existence of this phase, the interpretation of the linear-term in the heat-capacity in terms of spin-fluctuations from the Ru 4d band needs to be revisited. Additionally, in the vicinity of TN, AC \c{hi} shows a prominent frequency dependence and, below TN, MIRM exhibits a slow decay with time. This raises a question whether the antiferromagnetic structure in this compound is characterized by spin-glass-like dynamics. In contrast to what was reported earlier, there is a change in the sign of the magnetoresistance (MR) at the metamagnetic transition. A butter-fly-shaped (isothermal) MR loop (interestingly spanning over all the four quadrants) is observed at 2 K with distinct evidence for the magnetic phase co-existence phenomenon in zero field after travelling through metamagnetic transition field. The results on polycrystals thus provide additional information about the magnetism of this compound, revealing that the magnetism of this compound is more complex than what is believed, due to geometric frustration intrinsic to Kagome net.

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