arXiv subjects

K. Sethupathi

Publications and source records attributed to K. Sethupathi.

14 recordsLinked to original sources

arXiv2024

Evidence of 3$d$-4$f$ antiferromagnetic coupling in strain-tuned PrCo$_{0.5}$Ni$_{0.5}$O$_{3-\delta}$ epitaxial films

The strong exchange interaction between 3$d$-4$f$ magnetic sublattice in rare-earth perovskites introduces a variety of complex magnetic states hosting fascinating electronic ground states with exotic properties. Especially when it comes to rare-earth nickelate and cobaltite perovskites, tuning their rich magnetic phase diagram and spin-state transitions make them potential candidates for spintronic applications. Here, we report the observation of antiferromagnetic coupling between Pr 4$f$ and Ni/Co 3$d$ magnetic sublattices and its tunability with strain in PrCo$_{0.5}$Ni$_{0.5}$O$_{3-\delta}$ (PCNO) thin films. SQUID magnetization measurements reveal ferromagnetic (FM) ordering around 25 K, followed by a spin glass transition at low temperatures subject to spin reorientation. Competing magnetic interactions arise owing to the 3$d$-4$f$ antiferromagnetic (AFM) coupling between Pr and Co/Ni sublattice as revealed by the X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) at the Pr $M_{4,5}$ and Co/Ni $L_{2,3}$ absorption edges. Strain dependence on these AFM coupling reveals an increase (decrease) in the AFM exchange interaction for tensile (compressive) strained films, leading to a net decrease (increase) in the magnetization of PCNO films at low temperatures. The relative increase in low-temperature negative magnetoresistance for compressively strained films also reflects the enhanced ferromagnetic ordering in the system. The angle-dependent magnetoresistance measurements reveal a two-fold anisotropic magnetoresistance (AMR) in tensile strained PCNO films. In contrast, temperature-dependent switching of AMR accompanied by a two- to four-fold symmetry crossover is observed for LaAlO$_3$-grown compressive strained films.

cond-mat.mtrl-sci↗

arXiv2023

Possible realization of a randomness-driven quantum disordered state in an S = 1/2 antiferromagnet Sr3CuTa2O9

Collective behavior of spins, frustration-induced strong quantum fluctuations, and subtle interplay between competing degrees of freedom in quantum materials can lead to correlated quantum states with exotic excitations that are essential ingredients for establishing paradigmatic models and have immense potential for quantum technologies. Disorder is ubiquitous in real materials, and the detailed insights into the role of disorder on the intriguing ground state borne out of quenched randomness provide a route toward the design and discovery of functional quantum materials. Herein, we report magnetization, specific heat, electron spin resonance, and muon spin resonance studies on a 3d-electron-based antiferromagnet Sr3CuTa2O9. The negative Curie- Weiss temperature value, obtained from the Curie-Weiss fit of high-temperature magnetic susceptibility data, indicates antiferromagnetic interaction between Cu2+ moments. Specific heat data show the absence of long-range magnetic ordering down to 64 mK despite a reasonably strong exchange interaction between Cu2+ (S =1/2) spins as reflected from a Curie-Weiss temperature of -27 K. The power-law behavior and the data collapse of specific heat and magnetization data evince the emergence of a random-singlet state in Sr3CuTa2O9. The power-law-like spin auto-correlation function and the data collapse of muon polarization asymmetry with longitudinal field dependence of t({\mu}0H)^{\gamma} further support credence to the presence of a randomness-induced quantum disordered state. Our results suggest that randomness induced by disorder is an alternate route to realize a quantum disordered state in this antiferromagnet.

cond-mat.str-el↗

arXiv2023

Magnetic properties of a spin-orbit entangled Jeff=1/2 three-dimensional frustrated rare-earth hyperkagome

The interplay between competing degrees of freedom can stabilize non-trivial magnetic states in correlated electron materials. Frustration-induced strong quantum fluctuations can evade long-range magnetic ordering leading to exotic quantum states such as spin liquids in two-dimensional spin-lattices such as triangular and kagome structures. However, the experimental realization of dynamic and correlated quantum states is rare in three-dimensional (3D) frustrated magnets wherein quantum fluctuations are less prominent. Herein, we report the crystal structure, magnetic susceptibility, electron spin resonance (ESR) and specific heat studies accompanied by crystal electric field (CEF) calculations on a 3D frustrated magnet Yb3Sc2Ga3O12. In this material, Yb3+ ions form a three-dimensional network of corner-sharing triangles known as hyperkagome lattice without any detectable anti-site disorder. Our results reveal a low energy state with Jeff = 1/2 degrees of freedom in the Kramers doublet state. The zero field-cooled and field cooled magnetic susceptibility taken in 0.001 T rules out the presence of spin-freezing down to 1.8K. The Curie-Weiss (CW) fit to low-T susceptibility data yields a small and negative CW temperature indicating the presence of a weak antiferromagnetic interaction between Jeff = 1/2 (Yb3+) moments. The Yb-ESR displays a broad line of non-Lorentzian shape that suggests considerable magnetic anisotropy in Yb3Sc2Ga3O12. The CEF calculations suggest that the ground state is well separated from the excited states, which are in good agreement with experimental results. The absence of long-range magnetic ordering indicates a dynamic liquid-like ground state at least down to 130 mK. Furthermore, zero field specific heat shows a broad maximum around 200 mK suggesting the presence of short-range spin correlations in this 3D frustrated antiferromagnet.

cond-mat.str-el↗

arXiv2022

Spin re-orientation induced anisotropic magnetoresistance switching in LaCo$_{0.5}$Ni$_{0.5}$O$_{3-\delta}$ thin films

Realization of novel functionalities by tuning magnetic interactions in rare earth perovskite oxide thin films opens up exciting technological prospects. Strain-induced tuning of magnetic interactions in rare earth cobaltates and nickelates is of central importance due to their versatility in electronic transport properties. Here we reported the spin re-orientation induced switching of anisotropic magnetoresistance (AMR) and its tunability with strain in epitaxial LaCo$_{0.5}$Ni$_{0.5}$O$_{3-\delta}$ thin films across the ferromagnetic transition. Moreover, with strain tuning, we could observe a two-fold to four-fold symmetry crossover in AMR across the magnetic transition temperature. The magnetization measurements revealed an onset of ferromagnetic transition around 50 K, and a further reduction in temperature showed a subtle change in the magnetization dynamics, which reduced the ferromagnetic long-range ordering and introduced glassiness in the system. X-ray absorption and X-ray magnetic circular dichroism spectroscopy measurements over Co and Ni L edges revealed the Co spin state transition below the magnetic transition temperature leading to the AMR switching and also the presence of Ni$^{2+}$ and Co$^{4+}$ ions evidencing the charge transfer from Ni to Co ions. Our work demonstrated the tunability of magnetic interactions mediated electronic transport in cobaltate-nickelate thin films, which is relevant in understanding Ni-Co interactions in oxides for their technological applications such as in AMR sensors.

cond-mat.mtrl-sci↗

arXiv2022

Electronic structure and magnetic properties of 3d-4f double perovskite material

Double perovskite-based magnets wherein frustration and competition between emergent degrees of freedom are at play can lead to novel electronic and magnetic phenomena. Herein, we report the electronic structure and magnetic properties of an ordered double perovskite material Ho2CoMnO6. In the double perovskite with general class A2BB'O6, the octahedral B and B'-site has a distinct crystallographic site. The Rietveld refinement of XRD data reveals that Ho2CoMnO6 crystallizes in the monoclinic P21/n space group. The X-ray photoelectron spectroscopy confirms the charge state of cations present in this material. The temperature dependence of magnetization and specific heat exhibit a long-range ferromagnetic ordering at Tc ~ 76 K owing to the presence of super exchange interaction between Co2+ and Mn4+ moments. Furthermore, the magnetization isotherm at 5 K shows a hysteresis curve that confirms ferromagnetic behavior of this double perovskite. We observed a re-entrant glassy state in the intermediate temperature regime, which is attributed to inherent anti-site disorder and competing interactions. A large magnetocaloric effect has been observed much below the ferromagnetic transition temperature. The temperature-dependent Raman spectroscopy studies support the presence of spin-phonon coupling and short-range order above Tc in this double perovskite. The stabilization of magnetic ordering and charge states is further analyzed through electronic structure calculations. The latter also infers the compound to be a narrow band gap insulator with the gap arising between the lower and upper Hubbard Co-d subbands. Our results demonstrate that anti-site disorder and complex 3d-4f exchange interactions in the spin-lattice account for the observed electronic and magnetic properties in this promising double perovskite material.

cond-mat.mtrl-sci↗

arXiv2021

Signature of a randomness-driven spin-liquid state in a frustrated magnet

Collective behaviour of electrons, frustration induced quantum fluctuations and entanglement in quantum materials underlie some of the emergent quantum phenomena with exotic quasi-particle excitations that are highly relevant for technological applications. Herein, we present our thermodynamic and muon spin relaxation measurements, complemented by ab initio density functional theory and exact diagonalization results, on the recently synthesized frustrated antiferromagnet Li4CuTeO6, in which Cu2+ ions (S = 1/2) constitute disordered spin chains and ladders along the crystallographic [101] direction with weak random inter-chain couplings. Our thermodynamic experiments detect neither long-range magnetic ordering nor spin freezing down to 45 mK despite the presence of strong antiferromagnetic interaction between Cu2+ moments leading to a large effective Curie-Weiss temperature of -154 K. Muon spin relaxation results are consistent with thermodynamic results. The temperature and magnetic field scaling of magnetization and specific heat reveal a data collapse pointing towards the presence of random-singlets within a disorder-driven correlated and dynamic ground-state in this frustrated antiferromagnet.

cond-mat.str-el↗

arXiv2020

Sign reversal of anomalous Hall conductivity and magnetoresistance in cubic non-collinear antiferromagnet Mn$_3$Pt thin films

The two dimensional kagome spin lattice structure of Mn atoms in the family of Mn$_3$X non-collinear antiferromagnets are providing substantial excitement in the exploration of Berry curvature physics and the associated non-trivial magnetotransport responses. Much of these studies are performed in the hexagonal systems, mainly Mn$_3$Sn and Mn$_3$Ge, with the kagome planes having their normal along the [001] direction. In this manuscript, we report our study in the cubic Mn$_3$Pt thin films with their kagome planes normal to the [111] crystal axis. Our studies reveal a hole conduction dominant Hall response with a non-monotonic temperature dependence of anomalous Hall conductivity (AHC), increasing from 9 $\Omega^{-1}$cm$^{-1}$ at room temperature to 29 $\Omega^{-1}$cm$^{-1}$ at 100 K, followed by a drop and unexpected sign-reversal at lower temperatures. Similar sign reversal is also observed in magnetoresistance measurements. We attribute this sign reversal to the transition from a Berry curvature dominated AHC at high temperature to a weak canted ferromagnetic AHC response at lower temperature, below 70 K, caused by the reorientation of Mn moments out of the kagome plane. Our above results in thin films of Mn$_3$Pt make advances in their integration with room temperature antiferromagnetic spintronics.

cond-mat.mtrl-sci↗

arXiv2020

Wohlleben Effect and Emergent Pi junctions in superconducting Boron doped Diamond thin films

Diamond is an excellent band insulator. However, boron (B) doping is known to induce superconductivity. We present two interesting effects in superconducting B doped diamond (BDD) thin films: i) Wohlleben effect (paramagnetic Meissner effect, PME) and ii) a low field spin glass like susceptibility anomaly. We have performed electrical and magnetic measurements (under pressure in one sample) at dopings (1.4 , 2.6 and 3.6) X 1021 cm-3, in a temperature range 2 - 10 K. PME, a low field anomaly in inhomogeneous superconductors could arise from flux trapping, flux compression, or for non-trivial reason such as emergent Josephson Pi junctions. Joint occurrence of PME and spin glass type anomalies points to possible emergence of Pi junctions. BDD is a disordered s-wave superconductor; and Pi junctions could be produced by spin flip scattering of spin half moments when present at weak superconducting regions (Bulaevski et al. 1978). A frustrated network of 0 and Pi junctions will result (Kusmartsev et al. 1992) in a distribution of spontaneous equilibrium supercurrents, a phase glass state. Anderson localized spin half spinons embedded in a metallic fluid (two fluid model of Bhatt et al.) could create Pi junction by spin flip scattering. Our findings are consistent with presence of Pi junctions, invoked to explain their (Bhattacharyya et al.) observation of certain resistance anomaly in BDD.

cond-mat.supr-con↗

arXiv2020

Effect of interfacial oxidation layer in spin pumping experiments on Ni$_{80}$Fe$_{20}$/SrIrO$_3$ heterostructures

SrIrO$_3$ with its large spin-orbit coupling and low charge conductivity has emerged as a potential candidate for efficient spin-orbit torque magnetization control in spintronic devices. We here report on the influence of an interfacial oxide layer on spin pumping experiments in Ni$_{80}$Fe$_{20}$ (NiFe)/SrIrO$_3$ bilayer heterostructures. To investigate this scenario we have carried out broadband ferromagnetic resonance (BBFMR) measurements, which indicate the presence of an interfacial antiferromagnetic oxide layer. We performed in-plane BBFMR experiments at cryogenic temperatures, which allowed us to simultaneously study dynamic spin pumping properties (Gilbert damping) and static magnetic properties (such as the effective magnetization and magnetic anisotropy). The results for NiFe/SrIrO$_3$ bilayer thin films were analyzed and compared to those from a NiFe/NbN/SrIrO$_3$ trilayer reference sample, where a spin-transparent, ultra-thin NbN layer was inserted to prevent oxidation of NiFe. At low temperatures, we observe substantial differences in the magnetization dynamics parameters of these samples, which can be explained by an antiferromagnetic interfacial layer in the NiFe/SrIrO$_3$ bilayers.

cond-mat.mes-hall↗

arXiv2019

Contrasting the magnetism in La$_{2-x}$Sr$_x$FeCoO$_6$ ($x$ = 0, 1, 2) double perovskites: the role of electronic and cationic disorder

The magnetism of the double perovskite compounds \SLFCOx\ ($x$ = 0, 1, 2) are contrasted using magnetization, neutron diffraction and electron paramagnetic resonance with the support from density functional theory calculations. \LFCO\ is identified as a long-range ordered antiferromagnet displaying a near-room temperature transition at $T_N$ = 270~K, accompanied by a low temperature structural phase transition at $T_S$ = 200~K. The structural phase transformation at $T_S$ occurs from $R\overline{3}c$ at 300~K to $Pnma$ at 200~K. The density functional theory calculations support an insulating non-compensated AFM structure. The long-range ordered magnetism of \LFCO\ transforms to short-range glassy magnetism as La is replaced with Sr in the other two compounds. The magnetism of \LFCO\ is differentiated from the non-equilibrium glassy features of \SFCO\ and \SLFCO\ using the {\em cooling-and-heating-in-unequal-fields} (CHUF) magnetization protocols. This contransting magnetism in the \SLFCOx\ series is evidenced in electron paramegnetic resonance studies. The electronic density-of-states estimated using the density functional theory calculations contrast the insulating feature of \LFCO\ from the metallic nature of \SFCO. From the present suite of experimental and computational results on \SLFCOx, it emerges that the electronic degrees of freedom, along with antisite disorder, play an important role in controlling the magnetism observed in double perovskites.

cond-mat.str-el↗

arXiv2018

Hyperfine interaction and electronic spin fluctuation study on Sr$_{2-x}$La$_x$FeCoO$_6$ (x = 0, 1, 2) by high-resolution back-scattering neutron spectroscopy

The study of hyperfine interaction by high-resolution inelastic neutron scattering is not very well known compared to the other competing techniques viz. NMR, Mössbauer, PACS etc. Also the study is limited mostly to magnetically ordered systems. Here we report such study on Sr$_{2-x}$La$_x$FeCoO$_6$ (x = 0, 1, 2) of which first (Sr$_2$FeCoO$_6$ with x = 0) has a canonical spin spin glass, the second (SrLaFeCoO$_6$ with x = 1) has a so-called magnetic glass and the third (La$_2$FeCoO$_6$ with x = 2) has a magnetically ordered ground state. Our present study revealed clear inelastic signal for SrLaFeCoO$_6$, possibly also inelastic signal for Sr$_2$FeCoO$_6$ below the spin freezing temperatures $T_{sf}$ but no inelastic signal at all for for the magnetically ordered La$_2$FeCoO$_6$ in the neutron scattering spectra. The broadened inelastic signals observed suggest hyperfine field distribution in the two disordered magnetic glassy systems and no signal for the third compound suggests no or very small hyperfine field at the Co nucleus due to Co electronic moment. For the two magnetic glassy system apart from the hyperfine signal due only to Co, we also observed electronic spin fluctuations probably from both Fe and Co electronic moments. \end{abstract}

cond-mat.str-el↗

arXiv2017

High-pressure behavior of superconducting boron-doped diamond

This work investigates the high-pressure structure of freestanding superconducting ($T_{c}$ = 4.3\,K) boron doped diamond (BDD) and how it affects the electronic and vibrational properties using Raman spectroscopy and x-ray diffraction in the 0-30\,GPa range. High-pressure Raman scattering experiments revealed an abrupt change in the linear pressure coefficients and the grain boundary components undergo an irreversible phase change at 14\,GPa. We show that the blue shift in the pressure-dependent vibrational modes correlates with the negative pressure coefficient of $T_{c}$ in BDD. The analysis of x-ray diffraction data determines the equation of state of the BDD film, revealing a high bulk modulus of $B_{0}$=510$\pm$28\,GPa. The comparative analysis of high-pressure data clarified that the sp$^{2}$ carbons in the grain boundaries transform into hexagonal diamond.

cond-mat.supr-con↗

arXiv2011

Observation of spin glass state in weakly ferromagnetic Sr$_2$FeCoO$_6$ double perovskite

We report the observation of spin glass state in the double perovskite oxide Sr$_{2}$FeCoO$_{6}$ prepared through sol-gel technique. Initial structural studies using x rays reveal that the compound crystallizes in tetragonal $I 4/m$ structure with lattice parameters, $a$ = 5.4609(2) Åand $c$ = 7.7113(7) Å. The temperature dependent powder x ray studies reveal no structural phase transition in the temperature range 10 -- 300 K. However, the unit cell volume shows an anomaly coinciding with the magnetic transition temperature thereby suggesting a close connection between lattice and magnetism. Neutron diffraction studies and subsequent bond valence sums analysis show that in Sr$_{2}$FeCoO$_{6}$, the $B$ site is randomly occupied by Fe and Co in the mixed valence states of Fe$^{3+}$/Fe$^{4+}$ and Co$^{3+}$/Co$^{4+}$. The random occupancy and mixed valence sets the stage for inhomogeneous magnetic exchange interactions and in turn, for the spin glass like state in this double perovskite which is observed as an irreversibility in temperature dependent dc magnetization at $T_f\sim$ 75 K. Thermal hysteresis observed in the magnetization profile of Sr$_{2}$FeCoO$_{6}$ is indicative of the mixed magnetic phases present. The dynamic magnetic susceptibility displays characteristic frequency dependence and confirms the spin glass nature of this material. Dynamical scaling analysis of $χ'(T)$ yields a critical temperature $T_{ct}$ = 75.14(8) K and an exponent $zν$ = 6.2(2) typical for spin glasses. The signature of presence of mixed magnetic interactions is obtained from the thermal hysteresis in magnetization of Sr$_{2}$FeCoO$_{6}$. Combining the neutron and magnetization results of Sr$_2$FeCoO$_6$, we deduce the spin states of Fe to be in low spin while that of Co to be in low spin and intermediate spin.

cond-mat.str-el↗

arXiv2007

Complex ferromagnetic state and magnetocaloric effect in single crystalline Nd_{0.7}Sr_{0.3}MnO_{3}

The magnetocaloric effect in single crystalline Nd_{0.7}Sr_{0.3}MnO_{3} is investigated by measuring the field-induced adiabatic change in temperature which reveals a single negative peak around 130 K well below the Curie temperature (T_C=203 K). In order to understand this unusual magnetocaloric effect, we invoke the reported {55}^Mn spin-echo nuclear magnetic resonance, electron magnetic resonance and polarized Raman scattering measurements on Nd_{0.7}Sr_{0.3}MnO_{3}. We show that this effect is a manifestation of a competition between the double exchange mechanism and correlations arising from coupled spin and lattice degrees of freedom which results in a complex ferromagnetic state. The critical behavior of Nd_{0.7}Sr_{0.3}MnO_{3} near Curie temperature is investigated to study the influence of the coupled degrees of freedom. We find a complicated behavior at low fields in which the order of the transition could not be fixed and a second-order-like behavior at high fields.

cond-mat.mtrl-sci↗