arXiv subjects

A. Sundaresan

Publications and source records attributed to A. Sundaresan.

At least 37 records · Page 2Linked to original sources

arXiv2019

Muon spin rotation and neutron scattering investigations of the B-site ordered double perovskite Sr2DyRuO6

The magnetic ground state of double perovskite Sr2DyRuO6 has been investigated using muon spin rotation and relaxation (muSR), neutron powder diffraction (NPD) and inelastic neutron scattering (INS), in addition to heat capacity and magnetic susceptibility (ac and dc) measurements. A clear signature of a long-range ordered magnetic ground state has been observed in the heat capacity data, which exhibit two sharp anomalies at 39.5 and 36 K found as well in the magnetic data. Further confirmation of long-range magnetic ordering comes from a sharp drop in the muon initial asymmetry and a peak in the relaxation rate at 40 K, along with a weak anomaly near 36 K. Based on temperature dependent NPD, the low temperature magnetic structure contains two interpenetrating lattices of Dy and Ru5, forming an antiferromagnetic ground state below 39.5 K with magnetic propagation vector k = (0,0,0). The magnetic moments of Dy and Ru at 3.5 K are pointing along the crystallographic b-axis with values of muDy = 4.92(10) muB and muRu = 1.94(7) muB, respectively. The temperature dependence of the Ru moments follows a mean field type behaviour, while that of the Dy moments exhibits a deviation indicating that the primary magnetic ordering is induced by the order of the 4d electrons of Ru rather than that of its proper 4f Dy electrons. The origin of the second anomaly observed in the heat capacity data at 36.5 K must be connected to a very small spin reorientation as the NPD studies do not reveal any clear change in the observed magnetic Bragg peaks positions or intensities between these two transitions. INS measurements reveal the presence of crystal field excitations (CEF) in the paramagnetic state with overall CEF splitting of 73.8 meV, in agreement with the point change model calculations.

cond-mat.str-el↗

arXiv2019

Highly tunable magnetic spirals and electric polarization in Gd$_{0.5}$Dy$_{0.5}$MnO$_3$

Recent progress in the field of multiferroics led to the discovery of many new materials in which ferroelectricity is induced by cycloidal spiral orders. The direction of the electric polarization is typically constrained by spin anisotropies and magnetic field. Here, we report that the mixed rare-earth manganite, Gd$_{0.5}$Dy$_{0.5}$MnO$_3$, exhibits a spontaneous electric polarization along a general direction in the crystallographic ac-plane, which is suppressed below 10 K but re-emerges in an applied magnetic field. Neutron diffraction measurements show that the polarization direction results from a large tilt of the spiral plane with respect to the crystallographic axes and that the suppression of ferroelectricity is caused by the transformation of a cycloidal spiral into a helical one, a unique property of this rare-earth manganite. The freedom in the orientation of the spiral plane allows for a fine magnetic control of ferroelectricity, i.e. a rotation as well as a strong enhancement of the polarization depending on the magnetic field direction. We show that this unusual behavior originates from the coupling between the transition metal and rare-earth magnetic subsystems.

cond-mat.str-el↗

arXiv2019

Evidence of a cluster spin-glass state in the B-site disordered perovskite SrTi0.5Mn0.5O3

SrTi0.5Mn0.5O3 (STMO) is a chemically disordered perovskite having random distribution of Ti and Mn over 1b site. Striking discrepancies about the structural and magnetic properties of STMO demands detailed analysis which is addressed. To explore the magnetic ground state of STMO, static and dynamic magnetic properties were studied over a broad temperature range (2-300 K). The dc, ac magnetization show a cusp like peak at Tf ~ 14 K, which exhibits field and frequency dependence. The thermoremanent magnetization is characterized by using stretched exponential function and characteristic time suggests the existence of spin clusters. Also the other features observed in magnetic memory effect, muon spin resonance/rotation and neutron powder diffraction confirm the existence of cluster spin glass state in STMO, rather than the long range ordered ground state. Intriguingly, the observed spin relaxation can be attributed to the dilute magnetism due to non-magnetic doping at Mn-site and competing antiferromagnetic and ferromagnetic interactions resulting from the site disorder.

cond-mat.mtrl-sci↗

arXiv2018

Linear magnetoelectric effect as a signature of long-range collinear antiferromagnetic ordering in the frustrated spinel CoAl2O4

The ground state of the frustrated A-site magnetic spinel CoAl2O4 has been a controversial issue whether it is a collinear antiferromagnetic ordering or a spiral spin - liquid state, as the ratio of the two competing interactions, J2/J1 lies close to the boundary between these two ground states. Here, we address the magnetic ground state in CoAl2O4 with different amount of Co2+/Al3+ site disorder from the study of magnetoelectric effect and Monte Carlo simulations. CoAl2O4 with low site disorder exhibits linear magnetoelectric effect below the magnetic ordering temperature. With increasing disorder, the magnetoelectric effect is suppressed and the sample with 14% disorder exhibits a spin glass behavior without the magnetoelectric effect. Monte Carlo simulations support the experimental findings and suggest that the site disorder suppresses long - range antiferromagnetic order and induces a spin glass state. Since the linear magnetoelectric effect requires a long - range magnetic ordering, we suggest that the ground state of CoAl2O4 with low site disorder is a collinear antiferromagnet.

cond-mat.str-el↗

arXiv2015

Weak ferromagnetism and magnetization reversal in YFe$_{1-x}$Cr$_x$O$_3$

We present combined experimental and theoretical studies on the magnetic properties of a solid solution between yttrium orthoferrite and yttrium orthochromite systems, YFe$_{1-x}$Cr$_x$O$_3$ (0 $\leq$ x $\leq$ 1) where Fe$^{3+}$ and Cr$^{3+}$ ions are distributed randomly at the same crystallographic site (4b). We found that all the compositions exhibit weak ferromagnetism below the Néel temperature that decreases non-linearly with increasing $x$, while certain intermediate compositions ($x = 0.4,0.5$) show a compensation point and magnetization reversal. This unusual behavior is explained based on a simple model comprising the isotropic superexchange and the antisymmetric Dzyaloshinskii-Moriya interactions. This model explains the magnetization behavior in the entire range of doping and temperature including the magnetization reversal which results from an interplay of various DM interactions such as, Fe-O-Fe, Cr-O-Cr and Fe-O-Cr.

cond-mat.str-el↗

arXiv2015

Structural and magnetic properties of a new and ordered quaternary alloy MnNiCuSb (SG: F-43m)

We have synthesized a new crystallographically ordered quaternary Heusler alloy, MnNiCuSb. The crystal structure of the alloy has been determined by Rietveld refinement of the powder x-ray diffraction data. This alloy crystallizes in the LiMgPdSb type structure with F-43m space group. MnNiCuSb is a ferromagnet with a high TC ~ 690K and magnetic moment of 3.85MuB/f.u. Besides this we have also studied two other off-stoichiometric compositions; one Cu rich and the other Ni rich (MnNi0.9Cu1.1Sb and MnNi1.1Cu0.9Sb) which are also ferromagnets. It must be stressed that MnNiCuSb is one of the very few known, non-Fe containing quaternary Heusler alloys with 1: 1: 1: 1 composition.

cond-mat.mtrl-sci↗

arXiv2015

Possible coexistence of Cycloidal Phases, Magnetic Field Reversal of Polarization and Memory Effect in Multiferroic \emph{R}$_{0.5}$Dy$_{0.5}$MnO$_3$ (\emph{R}=Eu and Gd)

We report the occurrence of both \emph{ab} and \emph{bc} cycloidal ordering of Mn-spins at different temperatures and their possible coexistence at low temperatures in the polycrystalline mixed rare-earth compounds, \emph{R}$_{0.5}$Dy$_{0.5}$MnO$_3$ (\emph{R} = Eu and Gd), which exhibit extraordinary magnetoelectric properties. While the polarization of Gd$_{0.5}$Dy$_{0.5}$MnO$_3$ is comparable to TbMnO$_3$, the compound Eu$_{0.5}$Dy$_{0.5}$MnO$_3$ shows high value of polarization. However, both of them show giant magnetic tunability and exhibit large magnetocapacitance whose sign changes across the two cycloidal ordering temperatures. Intriguingly, the electric polarization can be reversed upon ramping up or ramping down the magnetic field, which has not been observed for any of the \emph{R}MnO$_3$ system. Most strikingly, these compounds show non-volatile ferroelectric memory effect even in the paraelectric and paramagnetic region (T$_C$ $\leq$ T $\leq$ 80 K). We attribute these remarkable properties to the coexistence of \emph{ab} and \emph{bc} cycloidal ordered phases.

cond-mat.mtrl-sci↗

arXiv2015

Effect of internal electric field on ferroelectric polarization in multiferroic TbMnO$_3$

Pyro-current measurements have been widely used to study ferroelectric properties in multiferroic materials. However, determination of intrinsic polarization by this method is not straightforward because of leakage current and trapped charge carriers. Here, we demonstrate the formation of internal electric field due to thermally stimulated charge carriers and its influence on ferroelectric polarization in a polycrystalline sample of the well known multiferroic TbMnO$_3$. While an electric field ($E_{ext}$) poling across the ferroelectric transition ($T_C$ $\sim$ 26 K) is essential to obtain depolarization current at $T_C$, the sample poled only in the paraelectric state ($T_{pole}$ = 130 $-$ 50 K) also exhibits a pyro-current peak at $T_C$ but with the same polarity ($-$ $I_{pyro}$) as that of the external field ($-$ $E_{ext}$). We demonstrate that these unusual behavior of pyro-current are caused by a positive internal electric field ($+$ $E_{int}$) which in turn is created by thermally stimulated free charge carriers during the poling process in the paraelectric state. We also show that a combination of DC-biased current and pyro-current measurements is a promising method to study the intrinsic ferroelectric properties in multiferroic materials.

cond-mat.mtrl-sci↗

arXiv2013

Temperature dependent magnetic, dielectric and Raman studies of partially disordered La2NiMnO6

We report a detailed magnetic, dielectric and Raman studies on partially disordered and biphasic double perovskite La2NiMnO6. DC and AC magnetic susceptibility measurements show two magnetic anomalies at TC1 ~ 270 K and TC2 ~ 240 K, which may indicate the ferromagnetic ordering of the monoclinic and rhombohedral phases, respectively. A broad peak at a lower temperature (Tsg ~ 70 K) is also observed indicating a spin-glass transition due to partial anti-site disorder of Ni2+ and Mn4+ ions. Unlike the pure monoclinic phase, the biphasic compound exhibits a broad but a clear dielectric anomaly around 270 K which is a signature of magneto-dielectric effect. Temperature-dependent Raman studies between the temperature range 12 K to 300 K in a wide spectral range from 220 cm-1 to 1530 cm-1 reveal a strong renormalization of the first as well as second-order Raman modes associated with the (Ni/Mn)O6 octahedra near TC1 implying a strong spin-phonon coupling. In addition, an anomaly is seen in the vicinity of spin-glass transition temperature in the temperature dependence of the frequency of the anti-symmetric stretching vibration of the octahedra.

cond-mat.mtrl-sci↗

arXiv2013

Spin-phonon coupling in multiferroic RCrO$_3$ (R-Y, Lu, Gd, Eu, Sm): A Raman study

Raman study on a select few orthochromites, RCrO$_3$ (R = Y, Lu, Gd, Eu and Sm) shows that the phonon behavior at TN in compounds with magnetic R-ion (Gd and Sm) is remarkably different from that of non-magnetic R-ion (Y, Lu and Eu). While anomalies in most of the observed phonon frequencies in all these compounds may result from the distortion of CrO$_6$ octahedra due to size effect and magnetostriction arising from Cr-ordering, the anomalous behavior of their linewidths observed at TN for the compounds with only magnetic R-ion suggests spin-phonon coupling. The presence of spin-phonon coupling and the anomalies in the low frequency modes related to R-ion motion in orthochromites (R = Gd and Sm) support the suggestion that the coupling between 4f-3d moments play important role in inducing switchable electric polarization.

cond-mat.mtrl-sci↗

arXiv2013

Interplay of 4f-3d Magnetism and Ferroelectricity in DyFeO3

DyFeO3 exhibits a weak ferromagnetism (TNFe ~ 645 K) that disappears below a spin-reorientation (Morin) transition at TSRFe ~ 50 K. It is also known that applied magnetic field induces ferroelectricity at the magnetic ordering temperature of Dy-ions (TNDy ~ 4.5 K). Here, we show that the ferroelectricity exists in the weak ferromagnetic state (TSRFe < T < TN,C) without applying magnetic field, indicating the crucial role of weak ferromagnetism in inducing ferroelectricity. 57Fe Mössbauer studies show that hyperfine field (Bhf) deviates from mean field-like behaviour that is observed in the weak ferromagnetic state and decreases below the onset of spin-reorientation transition (80 K), implying that the Bhf above TSR had additional contribution from Dy-ions due to induced magnetization by the weak ferromagnetic moment of Fe-sublattice and below TSR, this contribution decreases due to collinear ordering of Fe-sublattice. These results clearly demonstrate the presence of magnetic interactions between Dy(4f) and Fe(3d) and their correlation with ferroelectricity in the weak ferromagnetic state of DyFeO3.

cond-mat.mtrl-sci↗

arXiv2012

Ferroelectricity at the Néel Temperature of Chromium in Rare-earth Orthochromites: Interplay of Rare-earth and Cr Magnetism

We report ferroelectricity with fairly large spontaneous polarization (P ~ 0.2 - 0.8 \muC/cm2) below the Néel temperature of chromium (TNCr) in weakly ferromagnetic rare-earth orthochromites, RCrO3 (R=rare-earth) only when the rare-earth ion is magnetic. Intriguingly, the ferroelectricity in ErCrO3 (TC = 133 K) disappears at a spin-reorientation (Morin) transition (TSR ~ 22 K) below which the weak ferromagnetism associated with the Cr-sublattice also disappears, demonstrating the crucial role of weak ferromagnetism in inducing ferroelectricity. Further, the ferroelectric polarization (P) could be reversed by reversing the spontaneous magnetization (M) by changing the polarity of magnetic field, indicating a strong magnetoelectric effect. We suggest that the ferroelectricity occurs in RCrO3, due to the combined effect of poling field that breaks the symmetry and the exchange field on R-ion from Cr-sublattice stabilizes the polar state. We propose that a similar mechanism could work in the isostructural rare-earth orthoferrites, RFeO3 as well.

cond-mat.mtrl-sci↗

arXiv2012

Field-induced Polar Order at the Néel Temperature of Chromium in Rare-earth Orthochromites: Interplay of Rare-earth and Cr Magnetism

We report field-induced switchable polarization (P = 0.2 ~ 0.8 microC/cm2) below the Néel temperature of chromium (TN Cr) in weakly ferromagnetic rareearth orthochromites, RCrO3 (R=rareearth) but only when the rareearth ion is magnetic. Intriguingly, the polarization in ErCrO3 (TC ~ 133 K) disappears at a spin reorientation (Morin) transition (TSR ~ 22 K) below which the weak ferromagnetism associated with the Cr sublattice also disappears, demonstrating the crucial role of weak ferromagnetism in inducing the polar order. Further, the polarization (P) is strongly influenced by applied magnetic field, indicating a strong magneto electric effect. We suggest that the polar order occurs in RCrO3, due to the combined effect of poling field that breaks the symmetry and the exchange field on R ion from Cr sublattice stabilizes the polar state. We propose that a similar mechanism could work in the isostructural rareearth orthoferrites, RFeO3 as well.

cond-mat.mtrl-sci↗

arXiv2012

Multiferroic and magnetoelectric nature of GaFeO3, AlFeO3 and related oxides

GaFeO3, AlFeO3 and related oxides are ferrimagnetic exhibiting magnetodielectric effect. There has been no evidence to date for ferroelectricity and hence multiferroicity in these oxides. We have investigated these oxides as well as oxides of the composition Al1-x-yGaxFe1+yO3 (x = 0.2, y = 0.2) for possible ferroelectricity by carrying out pyroelectric measurements. These measurements establish the occurrence of ferroelectricity at low temperatures below the Nèel temperature in these oxides. They also exhibit significant magnetoelectric effect. We have tried to understand the origin of ferroelectricity based on non-centrosymmetric magnetic ordering and disorder by carrying out first-principles calculations.

cond-mat.mtrl-sci↗

arXiv2012

Coupled Phonons, Magnetic Excitations and Ferroelectricity in AlFeO3: Raman and First-principles Studies

We determine the nature of coupled phonons and magnetic excitations in AlFeO3 using inelastic light scattering from 5 K to 315 K covering a spectral range from 100-2200 cm-1 and complementary first-principles density functional theory-based calculations. A strong spin-phonon coupling and magnetic ordering induced phonon renormalization are evident in (a) anomalous temperature dependence of many modes with frequencies below 850 cm-1, particularly near the magnetic transition temperature Tc ~ 250 K, (b) distinct changes in band positions of high frequency Raman bands between 1100-1800 cm-1, in particular a broad mode near 1250 cm-1 appears only below Tc attributed to the two-magnon Raman scattering. We also observe weak anomalies in the mode frequencies at ~ 100 K, due to a magnetically driven ferroelectric phase transition. Understanding of these experimental observations has been possible on the basis of first-principles calculations of phonons spectrum and their coupling with spins.

cond-mat.str-el↗

arXiv2012

Near room-temperature colossal magnetodielectricity and multiglass properties in partially-disordered La2NiMnO6

We report magnetic, dielectric and magnetodielectric responses of pure monoclinic bulk phase of partially-disordered La2NiMnO6, exhibiting a spectrum of unusual properties and establish that this system intrinsically is a true multiglass with a large magnetodielectric coupling (8-20%) over a wide range of temperatures (150 - 300 K). Specifically, our results establish a unique way to obtain colossal magnetodielectricity, independent of any striction effects, by engineering the asymmetric hopping contribution to the dielectric constant via the tuning of the relative spin orientations between neighboring magnetic ions in a transition metal oxide system. We discuss the role of anti-site (Ni-Mn) disorder in emergence of these unusual properties.

cond-mat.mtrl-sci↗

arXiv2011

119Sn NMR probe of magnetic fluctuations in SnO2 nanoparticles

119Sn nuclear magnetic resonance (NMR) spectra and spin-lattice relaxation rate (1/T1) in SnO2 nanoparticles were measured as a function of temperature and compared with those of SnO2 bulk sample. A 15% loss of 119Sn NMR signal intensity for the nano sample compared to the bulk sample was observed. This is indicative of ferromagnetism from a small fraction of the sample. Another major finding is that the recovery of the 119Sn longitudinal nuclear magnetization in the nano sample follows a stretched exponential behavior, as opposed to that in bulk which is exponential. Further, the 119Sn 1/T1 at room temperature is found to be much higher for the nano sample than for its bulk counterpart. These results indicate the presence of magnetic fluctuations in SnO2 nanoparticles in contrast to the bulk (non-nano) which is diamagnetic. These local moments could arise from surface defects in the nanoparticles.

cond-mat.mtrl-sci↗

arXiv2011

Tuning of dielectric properties and magnetism of SrTiO3 by site-specific doping of Mn

Combining experiments with first principles calculations, we show that site-specific doping of Mn into SrTiO3 has a decisive influence on the dielectric properties of these doped systems. We find that phonon contributions to the dielectric constant invariably decrease sharply on doping at any site. However, a sizable, random dipolar contribution only for Mn at the Sr site arises from a strong off-centric displacement of Mn in spite of Mn being in a non-d0 state; this leads to a large dielectric constant at higher temperatures and gives rise to a relaxor ferroelectric behavior at lower temperatures. We also investigate magnetic properties in detail and critically reevaluate the possibility of a true multi-glass state in such systems.

cond-mat.mtrl-sci↗