arXiv subjects

S. Rayaprol

Publications and source records attributed to S. Rayaprol.

At least 19 recordsLinked to original sources

arXiv2025

Quantum spin liquid ground state in a rare-earth triangular antiferromagnet SmTa$_7$O$_{19}$

The rare-earth-based geometrically frustrated triangular magnets have attracted considerable attention due to the intricate interplay between strong spin-orbit coupling and the crystal electric field (CEF), which often leads to effective spin-1/2 degrees of freedom and therefore promotes strong quantum fluctuations at low temperatures, thus offering an excellent route to stabilize a quantum spin liquid (QSL) ground state. We have investigated the ground state magnetic properties of a polycrystalline sample of $\text{SmTa}_7\text{O}_{19}$ which we propose to have a gapless QSL ground state by employing powder X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), DC and AC-magnetic susceptibility, $M$ vs. $H$ isotherm, specific heat, and muon spin rotation/relaxation measurements ($\mu$SR) down to 30 mK. The combined structural and electronic studies reveal the formation of an edge-sharing equilateral triangular lattice of Sm$^{3+}$ ions in $ab$ plane. The DC, AC magnetic susceptibility, and heat capacity measurements reveal that $\text{SmTa}_7\text{O}_{19}$ does not exhibit any long-range magnetic ordering transition down to 50 mK. The zero-field (ZF)-$\mu$SR study strongly refutes the long-range magnetically ordered ground state and/or any partial spin-freezing down to at least 30 mK. The ZF-muon-spin relaxation rate is weakly temperature dependent between 50 and 20 K, rapidly increases below $\sim$20 K and saturates at low temperatures between 2 K and 30 mK, which has been attributed to a characteristic signature of QSL systems. Further, our longitudinal-field (LF)-$\mu$SR measurements at 0.1 K reveal a dynamic nature of the magnetic ground state. In addition, our high-field specific heat data suggest a gapless nature of spin excitations in this compound.

cond-mat.str-el↗

arXiv2024

Magnetic ground state and excitations in mixed 3$d$-4$d$ quasi-1D spin-chain oxide Sr$_3$NiRhO$_6$

Entanglement of spin and orbital degrees of freedom, via relativistic spin-orbit coupling, in 4$d$ transition metal oxides can give rise to a variety of novel quantum phases. A previous study of mixed 3$d$-4$d$ quasi-1D spin-chain oxide Sr$_3$NiRhO$_6$ using the magnetization measurements by Mohapatra et al. [Phys. Rev. B 75, 214422 (2007)] revealed a partially disordered antiferromagnetic (PDA) structure below 50 K [Mohapatra et al, Phys. Rev. B 75, 214422 (2007)]. We here report the magnetic ground state and spin-wave excitations in Sr$_3$NiRhO$_6$, using muon spin rotation and relaxation ($\mu$SR), and neutron (elastic and inelastic) scattering techniques. Our neutron diffraction study reveals that in the magnetic structure of Sr$_3$NiRhO$_6$, Rh$^{4+}$ and Ni$^{2+}$ spins are aligned ferromagnetically in a spin-chain, with moments along the crystallographic $c$-axis. However, spin-chains are coupled antiferromanetically in the $ab$-plane. $\mu$SR reveals the presence of oscillations in the asymmetry-time spectra below 50 K, supporting the long-range magnetically ordered ground state. Our inelastic neutron scattering study reveals gapped quasi-1D magnetic excitations with a large ratio of gap to exchange interaction. The observed spin-wave spectrum could be well fitted with a ferromagnetic isotropic exchange model (with $J = 3.7 $ meV) and single ion anisotropy ($D=10$ meV) on the Ni$^{2+}$ site. The magnetic excitations survive up to 85 K, well above the magnetic ordering temperature of $\sim 50$ K, also indicating a quasi-1D nature of the magnetic interactions in Sr$_3$NiRhO$_6$.

cond-mat.str-el↗

arXiv2024

Emergent Griffiths-phase-like behavior in the ball-milled nanocrystalline Dy4RhAl and its implication

We report the results of dc susceptibility and heat capacity measurements on the (ball-milled) nanocrystalline rare-earth (R) ternary compound, crystallizing in Gd4RhIn type, cubic Dy4RhAl compound. The bulk form of this compound has been known to undergo antiferromagnetic ordering at (TN=) 18 K with concomitant cluster spin glass anomalies. The present studies on the nano-form obtained by ball milling reveal that this antiferromagnetic ordering is suppressed with the reduction of particle size with no feature attributable to a well defined long-range magnetic ordering down to 1.8 K, but showing an inhomogeneous magnetism below 10 K. The point being stressed is that the results show the dominance of a feature around 30 K in the magnetic susceptibility data (well above TN of the bulk form) mimicking Griffiths phase. We infer that surface magnetism dominates before long range magnetic ordering occurs in this material.

cond-mat.str-el↗

arXiv2023

Role of crystal field ground state in the classical spin-liquid behavior of a quasi-one dimensional spin-chain system Sr3NiPtO6

The spin-chain compound Sr3NiPtO6 is known to have a nonmagnetic ground state. We have investigated the nature of ground state of Sr3NiPtO6 using magnetic susceptibility $\chi(T)$, heat capacity $C_{\rm p}(T)$, muon spin relaxation ($\mu$SR) and inelastic neutron scattering (INS) measurements. The $\chi(T)$ and $C_{\rm p}(T)$ do not exhibit any pronounced anomaly that can be associated with a phase transition to a magnetically ordered state. Our $\mu$SR data confirm the absence of long-range magnetic ordering down to 0.04 K. Furthermore, the muon spin relaxation rate increases below 20 K and exhibits temperature independent behavior at low temperature, very similar to that observed in a quantum spin-liquid system. The INS data show a large excitation near 8~meV, and the analysis of the INS data reveals a singlet CEF ground state with a first excited CEF doublet state at $\Delta_{\rm CEF}$ = 7.7 meV. The estimated CEF parameters reveal a strong planar anisotropy in the calculated $\chi(T)$, consistent with the reported behavior of the $\chi(T)$ of single crystal Sr3NiPtO6. We propose that the nonmagnetic singlet ground state and a large $\Delta_{\rm CEF}$ (much larger than the exchange interaction $\mathcal{J}_{\rm ex}$) are responsible for the absence of long-range magnetic ordering and can mimic a classical spin-liquid behavior in this quasi-1D spin chain system Sr3NiPtO6. The classical spin-liquid ground state observed in Sr3NiPtO6 is due to the single-ion property, which is different from the quantum spin-liquid ground state observed in geometrically frustrated systems, where two-ion exchanges play an important role.

cond-mat.str-el↗

arXiv2023

Canting angle behavior of magnetic moments in Y- substituted Tb2BaNiO5 and its relevance for magnetoelectric coupling

The Haldane-spin chain compound, Tb2BaNiO5, has been known to be an exotic multiferroic system, exhibiting antiferromagnetic anomalies at T_N1= 63 K and T_N2= 25 K, with ferroelectricity appearing below T_N2 only. Previous reports in addition established that, interestingly, Tb ions play a direct and decisive role to lead to multiferroic properties with a critical canting angle of magnetic moments, unlike other well-known multiferroics. Here, we report the results of temperature dependent neutron powder diffraction studies on Tb_2-x Y_x BaNiO_5, to get an insight into the critical canting angle for multiferroic behavior. While multiferroic transition temperature decreases linearly with Y concentration, there is an abrupt drop of relative canting angle (of Tb and Ni magnetic moments) with respect to that in parent compound for an initial substitution ofx = 0.5 in the multiferroic region, without any notable change thereafter. We therefore infer that this critical canting angle is made up of two components - cooperative (long-range) and local (short-range) contributions.

cond-mat.str-el↗

arXiv2022

Magnetic-field induced melting of long-range magnetic order akin to Kitaev insulators in the metallic compound Tb5Si3

There have been constant efforts to find exotic quantum spin-liquid (QSL) materials. Some of the transition metal insulators dominated by the direction dependent anisotropic exchange interaction (Kitaev model for honeycomb network of magnetic ions) are considered to be promising cases for the same. In such Kitaev insulators, QSL is achieved from the zero-field antiferromagnetic state by the application of magnetic field, suppressing other exchange interactions responsible for magnetic order. Here, we show that the features attributable to long-range magnetic ordering of the intermetallic compound, Tb5Si3 (T_N= 69 K), containing honey-comb network of Tb ions, are completely suppressed by a critical applied field, H_cr, in heat-capacity and magnetization data, mimicking the behavior of Kitaev physics candidates. The neutron diffraction patterns as a function of H reveal that it is an incommensurate magnetic structure that gets suppressed, showing peaks arising from multiple wave vectors beyond Hcr. Increasing magnetic entropy as a function of H with a peak in the magnetically ordered state is in support of some kind of magnetic disorder in a narrow field range after H_cr. Such a high-field behavior for a metallic heavy rare-earth system to our knowledge has not been reported in the past and therefore is intriguing.

cond-mat.str-el↗

arXiv2021

Structure-property relations characterizing the devitrification of Ni-Zr glassy alloy thin films

The investigation of devitrification in thermally annealed nanodimensional glassy alloy thin films provides a comprehensive understanding of their thermal stability, which can be used to explore potential applications. The amorphous to crystalline polymorphous transformation of cosputtered NiZr alloy (Ni78Zr22 at%) films, with a thickness lower than the reported critical limit of devitrification, was studied through detailed structural characterization and molecular dynamics (MD) simulations. Devitrification to a nanocrystalline state (Ni7Zr2 structure) was observed at 800 degC, with an increase in density (approx 3.6%) much higher than that achieved in bulk alloys. Variation in the magnetic property of the films and the overall physical structure including morphology and composition were examined before and after annealing. MD simulations were employed to effectively elucidate not only the high densification but also the increased magnetic moment after annealing, which was correlated with the simulated change in the coordination number around Ni atoms. The structural relaxation process accompanying devitrification was described as a disorder-to-order transformation while highlighting the crucial role played by chemical short range order prevalent in glassy materials.

cond-mat.mtrl-sci↗

arXiv2021

Pressure-induced anomalies in the magnetic transitions of the exotic multiferroic material, Tb2BaNiO5

We have studied the influence of external pressure up to 1 GPa on the magnetic transitions of the orthorhombic Haldane-spin chain compound Tb2BaNiO5 an exotic multiferroic material. This parent compound is known to undergo N\'eel ordering at TN1= 63 K and another magnetic transition at TN2= 25K at which ferroelectricity sets in, however, without any change in the magnetic symmetry, but with only a sharp change in the canting angle of Tb 4f and Ni 3d magnetic moments. There is a subtle difference in the antiferromagnetic state above and below TN2, which is supported by the fact that there is a metamagnetic transition below TN2only (for 5 K, at about 60 kOe). We report here that, with the application of external pressure, there is an upward shift of TN1, while TN2 shifts towards lower temperatures. It is interesting that the two magnetic transitions in the same compound behave differently under pressure and the opposite behavior at TN2 is attributed to local distortion leading to ferroelectricity. The results are augmented by temperature dependent x-ray diffraction and positive chemical pressure studies. The chemical pressure caused by the isoelectronic doping at Ba site by Sr reduces both the transition temperatures. Clearly, the external pressure favors antiferromagnetic coupling (that is, leading to TN1 enhancement), whereas the chemical pressure reduces TN1, suggesting important role of the changes in local hybridization induced by doping on magnetism in this material.

cond-mat.str-el↗

arXiv2020

Origin of destruction of multiferroicity in Tb2BaNiO5 by Sr doping and its implications

The orthorhombic Haldane spin chain compound Tb2BaNiO5 (Neel order, TN1= 63 K) has been shown to be an exotic multiferroic system below (TN2) 25 K due to various fascinating features, pointing to a strong potential for the advancement of concepts in this field. In particular, the rare-earth ions play a direct decisive role unlike in many other well known multiferroic materials and there appears to be a critical canting angle, developing below TN2, subtended by Tb 4f and Ni 3d moments to trigger this cross coupling phenomenon. However, for a small replacement of Sr for Ba, viz. in Tb2Ba0.9Sr0.1NiO5, ferroelectricity was reported to get destroyed, but retaining magnetic features at (TN1) 55 K and (TN2) 14 K. In this article, we address the origin of suppression of multiferrocity in this Sr doped system through neutron diffraction studies and density functional theory calculations. We find that, unlike in Tb2BaNiO5, there is no pronounced change in the relative canting angle of the magnetic moments around TN2 and that the absolute value of this parameter down to 2 K fails to exceed the critical value noted for the parent, thereby explaining the origin of destruction of magnetoelectric coupling in the Sr doped material. This finding renders strong support to the proposal of possible existence of critical canting angle, at least in some cases, to induce multiferroicity, apart from serving as a route to engineer multiferroic materials for applications.

cond-mat.str-el↗

arXiv2019

Magnetic order in Nd$_2$PdSi$_3$ investigated using neutron scattering and muon spin relaxation

The rare-earth based ternary intermetallic compounds $R_2TX_3$ ($R$ = rare-earth, $T$ = transition-metal, $X$ = Si, Ge, Ga, In) have attracted considerable interest due to a wide range of interesting low temperature properties. Here we investigate the magnetic state of Nd$_{2}$PdSi$_{3}$ using neutron diffraction, muon spin relaxation ($\mu$SR) and inelastic neutron scattering (INS). This compound appears anomalous among the $R_{2}$PdSi$_{3}$ series, since it was proposed to order ferromagnetically, whereas others in this series are antiferromagnets. Although some members of the $R_2TX_3$ series have been reported to form ordered superstructures, our data are well described by Nd$_{2}$PdSi$_{3}$ adopting the AlB$_2$-type structure with a single Nd site, and we do not find evidence for superlattice peaks in neutron diffraction. Our results confirm the onset of long range magnetic order below $T_0=17$~K, where the whole sample enters the ordered state. Neutron diffraction measurements establish the presence of a ferromagnetic component in this compound, as well as an antiferromagnetic one which has a propagation vector $\mathbf{k_2}=(1/2,1/2,1/4-\delta)$ with a temperature dependent $\delta\approx0.02-0.04$, and moments orientated exclusively along the $c$-axis. $\mu$SR measurements suggest that these components coexist on a microscopic level, and therefore the magnetic structure of Nd$_{2}$PdSi$_{3}$ is predominantly ferromagnetic, with a sinusoidally modulated antiferromagnetic contribution which reaches a maximum amplitude at 11~K, and becomes smaller upon further decreasing the temperature. INS results show the presence of crystalline-electric field (CEF) excitations above $T_0$, and from our analysis we propose a CEF level scheme.

cond-mat.str-el↗

arXiv2017

Spin reorientation and disordered rare earth magnetism in Ho$_2$FeCoO$_6$

We report the experimental observation of spin reorientation in the double perovskite Ho$_2$FeCoO$_6$. The magnetic phase transitions in this compound are characterized and studied through magnetization and specific heat, and the magnetic structures are elucidated by neutron powder diffraction. Two magnetic phase transitions are observed in this compound - one at $T_\mathrm{N1} \approx$ 250~K, from paramagnetic to antiferromagnetic, and the other at $T_\mathrm{N2} \approx$ 45~K, from a phase with mixed magnetic structures to a single phase through a spin reorientation process. The magnetic structure in the temperature range 200~K - 45~K is a mixed phase of the irreducible representations $\Gamma_1$ and $\Gamma_3$, both of which are antiferromagnetic. The phase with mixed magnetic structures that exists in Ho$_2$FeCoO$_6$ gives rise to a large thermal hysteresis in magnetization that extends from 200~K down to the spin reorientation temperature. At $T_\mathrm{N2}$, the magnetic structure transforms to $\Gamma_1$. Though long-range magnetic order is established in the transition metal lattice, it is seen that only short-range magnetic order prevails in Ho$^{3+}$ - lattice. Our results should motivate further detailed studies on single crystals in order to explore spin reorientation process, spin switching and the possibility of anisotropic magnetic interactions giving rise to electric polarization in Ho$_2$FeCoO$_6$.

cond-mat.mtrl-sci↗

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.

cond-mat.str-el↗

arXiv2016

Non-collinear Order and Spin-Orbit Coupling in Sr$_3$ZnIrO$_6$

Sr$_{3}$ZnIrO$_{6}$ is an effective spin one-half Mott insulating iridate belonging to a family of magnets which includes a number of quasi-one dimensional systems as well as materials exhibiting three dimensional order. Here we present the results of an extensive investigation into the magnetism including heat capacity, a.c. susceptibility, muon spin rotation ($\mu$SR), neutron diffraction and inelastic neutron scattering on the same sample. It is established that the material exhibits a transition at about $17$ K into a three-dimensional antiferromagnetic structure with propagation vector $\boldsymbol{k}=(0,\frac{1}{2},1)$ in the hexagonal setting of R$\bar{3}$c and non-collinear moments of $0.87$$\mu_B$ on Ir$^{4+}$ ions. Further we have observed a well defined powder averaged spin wave spectrum with zone boundary energy of $\sim 5$ meV at $5$ K. We stress that a theoretical analysis shows that the observed non-collinear magnetic structure arises from anisotropic inter- and intra- chain exchange which has its origin in significant spin-orbit coupling. The model can satisfactorily explain the observed spin wave excitations.

cond-mat.str-el↗

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.

cond-mat.str-el↗

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

Correlation of exchange bias with magneto-structural effects across the compensation temperature of Co(Cr$_{1-x}$Fe$_{x}$)$_2$O$_4$ (x = 0.05 and 0.075)

A small amount of Fe (5% and 7.5%) substitution in the Cr-site of the multiferroic compound CoCr2O4 leads to a magnetization reversal. In these compounds, we report a sign change in the exchange bias across the compensation temperature, accompanied by a non-monotonic change in the local moments across the compensation temperature. Such non-monotonic change in the magnetic moments is triggered by a similar change in the lattice structure. We relate here the sign change of exchange bias with that of the crystalline energy of the lattice and the Zeeman energy term arising from the anti-site disorder.

cond-mat.str-el↗

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↗

arXiv2012

Magnetic behavior of Ba_{3}Cu_{3}Sc_{4}O_{12}

The chain-like system Ba_{3}Cu_{3}Sc_4O_{12} has potentially interesting magnetic properties due to the presence of Cu^{2+} and a structure-suggested low-dimensionality. We present magnetization M versus magnetic field H and temperature T, T- and H-dependent heat-capacity C_{p}, ^{45}Sc nuclear magnetic resonance (NMR), muon spin rotation ({\mu}SR), neutron diffraction measurements and electronic structure calculations for Ba_{3}Cu_{3}Sc_{4}O_{12}. The onset of magnetic long-range antiferromagnetic order at T_{N} ~16 K is consistently evidenced from the whole gamut of our data. A significant sensitivity of T_{N} to the applied magnetic field H (T_{N}~0 K for H=70 kOe) is also reported. Coupled with a ferromagnetic Curie-Weiss temperature ({\theta}_{CW}~65 K) in the susceptibility (from a 100 K-300 K fit), it is indicative of competing ferromagnetic and antiferromagnetic interactions. These indications are corroborated by our density functional theory based electronic structure calculations where we find the presence of significant ferromagnetic couplings between some copper ions whereas AF couplings were present between some others. Our experimental data, backed by our theoretical calculations, rule out one-dimensional magnetic behaviour suggested by the structure and the observed long-range order is due to the presence of non-negligible magnetic interactions between adjacent as well as next-nearest chains.

cond-mat.str-el↗