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M. P. Saravanan

Publications and source records attributed to M. P. Saravanan.

14 recordsLinked to original sources

Microscopic Origin of Random Singlet Behavior in B-site Disordered Spin-1/2 Perovskite BaCu_1/3Nb_2/3O_3 Revealed by EXAFS and Thermodynamics

We report a combined structural and thermodynamic study of the ABO$_3$-type disordered perovskite BaCu$_{1/3}$Nb$_{2/3}$O$_3$ (BCNO), whose B site is jointly occupied by Cu and Nb in the $1:2$ ratio. Using synchrotron powder x-ray diffraction (XRD) and x-ray absorption fine structure (XAFS) spectroscopy, we investigate the microscopic nature of Cu$^{2+}$/Nb$^{5+}$ disorder on the pseudo-cubic B-sublattice and its relation to the emergent random-singlet (RS) behavior evidenced at low temperatures. While XRD reveals no long-range Cu/Nb ordering and average site occupancy consistent with stoichiometry, XAFS reveals a peculiar local chemical order characterized by preferential heteroatomic Cu$:$Nb correlations. This local arrangement strongly suppresses direct Cu$:$Cu linkages, despite the Cu concentration being close to the percolation threshold of a cubic lattice. The resulting exchange network explains the absence of spin-glass freezing or long-range magnetic order in the presence of substantial antiferromagnetic interactions, as indicated by a Curie-Weiss temperature $Θ_{CW}\approx -50$ K. Instead, the magnetic susceptibility $χ(T)$ and specific heat $c_p(T)$ exhibit power-law behavior and characteristic single-parameter $T/H$ scaling over broad temperature and magnetic-field ranges, consistent with random-singlet phenomenology. Notably, at very low temperatures, the specific heat behavior transitions from $T^{1-γ}$ ($γ\approx 0.6$ from the $T/H$ scaling) in zero-field to a T-linear dependence under high field, indicating a crossover to a distinct low-energy regime whose microscopic origin remains to be established.

cond-mat.str-el

Spin-orbit-entangled frustrated magnetism in fcc Ba$_2$(Yb,Nd)NbO$_6$ double perovskites

The search for candidate Kitaev materials has largely focused on 4$d$ and 5$d$ transition-metal compounds with various lattice geometries. In contrast, investigations of rare-earth 4$f$ systems have thus far been restricted mainly to honeycomb and triangular lattices. In this work, we investigate the rare-earth-based double perovskites Ba$_2$YbNbO$_6$ and Ba$_2$NdNbO$_6$, which crystallize in a face-centered cubic structure. Magnetization and heat-capacity measurements establish isolated ${j_{\rm eff}} = 1/2$ Kramers doublet ground states arising from strong spin-orbit coupling (SOC) and crystal electric-field effects, which are further supported by density-functional theory calculations. Millikelvin-temperature thermodynamic measurements reveal long-range magnetic order with moderate frustration in both compounds. The emergence of magnetic order may be understood within an order-by-disorder scenario, as theoretically proposed for rare-earth fcc lattices with finite Kitaev interactions. Our results thus identify Ba$_2$YbNbO$_6$ and Ba$_2$NdNbO$_6$ as promising rare-earth spin-orbit-entangled magnets and motivate further experimental and theoretical investigations aimed at determining the complete exchange tensor to elucidate the microscopic origin of the underlying magnetic interactions.

cond-mat.str-el

Novel Quantum Spin Liquid States in the $S = {\frac{1}{2}}$ Three-Dimensional Compound Y$_{3}$Cu$_{2}$Sb$_{3}$O$_{14}$

The three-dimensional $S = {\frac{1}{2}}$ system Y$_{3}$Cu$_{2}$Sb$_{3}$O$_{14}$ consists of two inequivalent Cu$^{2+}$ sites, each forming an edge shared triangular lattice. Our magnetic susceptibility $χ(T)$, specific heat $C_p(T)$, $^{89}$Y nuclear magnetic resonance (NMR), muon spin relaxation ($\upmu\mathrm{SR}$), and electron spin resonance (ESR) measurements on this system confirm the absence of any long-range magnetic ordering and the persistence of spin dynamics down to 0.077 K. In $^{89}$Y NMR we find an anomaly at about 120 K which we suggest arises from a fraction of the spins condensing into a singlet (a valence bond solid VBS) state. A plateau in the muon relaxation rate is observed between 60 K and 10 K (signifying the VBS state from a fraction of the spins) followed by an increase and another plateau below about 1 K (presumably signifying the quantum spin liquid state from all the spins). Our density functional theory calculations find a dominant antiferromagnetic interaction along the body diagonal with inequivalent Cu(1) and Cu(2) ions alternately occupying the corners of the cube. All other near-neighbour interactions between the Cu ions are also found to be antiferromagnetic and are thought to drive the frustration.

cond-mat.str-el

Crystal electric field excitations and spin dynamics in a spin-orbit coupled distorted honeycomb magnet BiErGeO$_5$

The magnetic properties and crystal electric field (CEF) scheme of BiErGeO$_5$ are investigated via magnetization, heat capacity, muon spin relaxation (muSR), and inelastic neutron scattering (INS) experiments on a polycrystalline sample. The Er$^{3+}$ ions form a quasi-two-dimensional distorted honeycomb network with a Kramers doublet ground state. Magnetic susceptibility and heat capacity reveal short-range antiferromagnetic correlations, manifested as a broad maximum around 1.4 K. Heat-capacity data further confirm the onset of a magnetic long-range order at $T_ N = 0.4$ K. The INS spectra exhibit eight CEF excitations and the CEF analysis yields the $g$-factor anisotropy with $g_{xy}/g_{z} = 1.38$ and exchange anisotropy with $J_{xy} = 2.96$ K and $J_{z} = 1.56$ K. The experimental temperature and field dependent magnetization and heat capacity are also reproduced by the simulation using CEF energy scheme. Zero-field muSR measurements down to 30 mK, do not exhibit coherent oscillations or a static 1/3 tail. The spectra are well described by two exponential relaxation components, indicating two magnetically inequivalent muon environments. The relaxation rates display a nearly temperature-independent plateau below $T_{\rm N}$ and follow an Orbach-type activated behavior at higher temperatures involving excited CEF levels, consistent with the INS results. Longitudinal-field $μ$SR measurements reveal only weak decoupling up to 1.5 T, indicating persistent slow spin fluctuations below $T_{\rm N}$.

cond-mat.mtrl-sci

Emergent Random Spin Singlets in Disordered Spin-1/2 perovskite BaCu$_{1/3}$Ta$_{2/3}$O$_3$

We investigate the disordered perovskite BaCu$_{1/3}$Ta$_{2/3}$O$_3$, where Cu (spin-1/2) and Ta randomly occupy a pseudo-cubic lattice. Synchrotron X-ray diffraction and X-ray absorption spectroscopy establish the local nature of the disorder, revealing the presence of structurally constrained magnetic exchange paths. No magnetic ordering or spin freezing is observed down to 0.1 K. The low-temperature magnetic and thermodynamic behavior is captured by a broad but non-singular distribution $P(J)$ of exchange couplings $J$. These results open the possibility of realizing a disordered quantum ground state where the exchange randomness is broad yet intrinsically bounded, departing from the conventional infinite-randomness fixed point driven random-singlet phase.

cond-mat.str-el

Proximate spin-liquid behavior in the double trillium lattice antiferromagnet K$_2$Co$_2$(SO$_4$)$_3$

We report proximate quantum spin liquid behavior in K$_2$Co$_2$(SO$_4$)$_3$ with the magnetic Co$^{2+}$ ions embedded on a highly frustrated three-dimensional double trillium lattice. Single-crystal and high-resolution synchrotron powder x-ray diffraction experiments reveal a structural phase transition at $T_{\rm t} \simeq 125$ K from high-temperature cubic to low-temperature monoclinic phase with the three-fold superstructure. Magnetization and heat capacity consistently show the formation of the $J_{\rm eff} =1/2$ state of Co$^{2+}$ below 50 K. In zero field, K$_2$Co$_2$(SO$_4$)$_3$ shows signatures of static magnetic order formed below $T^* \simeq 0.6$ K, but muon spin relaxation experiments reveal a large fluctuating component that persists down to at least 50 mK, reminiscent of quantum spin liquid (QSL). Static order is completely suppressed in the small magnetic field of $\sim 1$ T, and low-temperature heat capacity demonstrates the $T^2$ behavior above this field, another fingerprint of QSL. Ab initio calculations show a competition of several antiferromagnetic couplings that render K$_2$Co$_2$(SO$_4$)$_3$ a promising pseudospin-$\frac12$ material for studying quantum magnetism in the double trillium lattice geometry.

cond-mat.mtrl-sci

Tomonaga-Luttinger liquid and quantum criticality in spin-1/2 antiferromagnetic Heisenberg chain C14H18CuN4O10 via Wilson ratio

The ground state of a one-dimensional spin-1/2 uniform antiferromagnetic Heisenberg chain (AfHc) is a Tomonaga-Luttinger liquid which is quantum-critical with respect to applied magnetic fields upto a saturation field Hs beyond which it transforms to a fully polarised state. Wilson ratio has been predicted to be a good indicator for demarcating these phases [Phys. Rev. B 96, 220401 (2017)]. From detailed temperature and magnetic field dependent magnetisation, magnetic susceptibility and specific heat measurements in a metalorganic complex and comparisons with field theory and quantum transfer matrix method calculations, the complex was found to be a very good realisation of a spin-1/2 AfHc. Wilson ratio obtained from experimentally obtained magnetic susceptibility and magnetic contribution of specific heat values was used to map the magnetic phase diagram of the uniform spin-1/2 AfHc over large regions of phase space demarcating Tomonaga-Luttinger liquid, saturation field quantum critical, and fully polarised states. Luttinger parameter and spinon velocity were found to match very well with the values predicted from conformal field theory.

cond-mat.str-el

Atypical antiferromagnetic ordering in single crystalline quasi-2D honeycomb magnet YbI$_3$

Here, we study YbI$_3$, a quasi-2D layered material with Yb atoms arranged on an ideal honeycomb network of edge-sharing YbI$_6$ octahedra, analogous to the low-temperature phase of $α-$RuCl$_3$. High quality single crystals of YbI$_3$ are grown from Yb and I as starting precursors, using the vapor transport technique. The grown crystals are characterized by single crystal x-ray diffraction, Raman spectroscopy, magnetization, and heat capacity probes. The crystal-field split ground state of Yb$^{3+}$ in \Yb~ is a well-isolated Kramers doublet with an effective moment $\rm J_{eff} = 1/2$. Upon cooling, the low-temperature heat capacity of \Yb~ reveals a broad peak at $\rm T_1 = 0.95$~K due to short-range ordering of the Yb moments, followed by a sharp peak at $\rm T_2 = T_N = 0.6$~K due to long-range ordering. The magnetic behavior is found to be weakly anisotropic with $χ^\parallel > χ^\perp$, where $χ^\parallel$ and $χ^\perp$ refers to the in-plane ($H \parallel ab$) and out-of-plane ($H \perp ab$) susceptibilities. The 2~K isothermal magnetization saturates at $\rm \approx~1.5~μ_B/Yb^{3+}$ (in-plane) and $\rm \approx~1~μ_B/Yb^{3+}$ (out-of-plane), suggesting the anisotropy to be easy-plane type. Low-temperature heat capacity, well below T$_N$, is found to vary as T$^α$ with $α~\approx~2.5$, indicating a possible unconventional magnetic ground state for YbI$_3$.

cond-mat.str-el

Emergence of quantum Griffiths singularity in disordered TiN thin films

The association of quantum Griffiths singularity (QGS) to the magnetic-field-induced superconductor-metal transition predicts the unconventional diverging behaviour of dynamical critical exponent in low disorder crystalline two-dimensional superconductors. But whether this state exists in the superconducting systems exhibiting superconductor-insulator transition remains elusive. Here, we report the emergence of quantum Griffiths singularity in ultrathin disordered TiN thin films with more than two orders of magnitude variation in their normal state resistance. For both superconductor-metal transition and superconductor-insulator transition types, a diverging critical exponent is observed while approaching the quantum phase transition. Further, the magnetoresistance isotherms obey a direct activated scaling governed by an infinite-randomness fixed critical point. Finally, this work establishes the robustness of the QGS phenomenon towards a wide range of temperature and also towards a wide range of disorder strength as correlated with the normal state resistance.

cond-mat.supr-con

Disordered ground state in the spin-orbit coupled $J_{\rm eff}= 1/2$ cobalt-based metal-organic framework magnet with orthogonal spin dimers

We present the magnetic properties of a strongly spin-orbit coupled quantum dimer magnet based on Co$^{2+}$. The metal-organic framework compound Co$_2$(BDC)$_2$(DPTTZ)$_2$$\cdot$DMF features Co$^{2+}$ dimers arranged nearly orthogonal to each other, similar to the Shastry-Sutherland lattice. Our assessment based on the magnetization and heat capacity experiments reveals that the magnetic properties at low temperatures can be described by an effective $J_{\rm eff} = 1/2$ Kramers doublet and the ground state is a singlet with a tiny spin gap. Although the magnetic susceptibility could be analyzed in terms of the interacting dimer model with an isotropic intradimer coupling $J_0/k_{\rm B} \simeq 7.6$ K, this model fails to reproduce the shape of magnetization isotherm and heat capacity data. A model of isolated spin dimers with the anisotropic exchange couplings $J_{xy} \simeq 3.5$ K and $J_{z} \simeq 11$ K provides an adequate description to the magnetic susceptibility, magnetization isotherm, and heat capacity data at low temperatures. Interestingly, no field-induced quantum phase phase is detected down to 100~mK around the critical field of gap closing, suggesting the absence of Bose-Einstein condensation of triplons and establishing isolated dimers with a negligible interdimer coupling.

cond-mat.str-el

Double magnetic transitions and exotic field induced phase in the triangular lattice antiferromagnets Sr$_3$Co(Nb,Ta)$_2$O$_9$

Two triangular lattice antiferromagnets Sr$_3$Co(Nb,Ta)$_2$O$_9$ with an effective $j_{\rm eff}=1/2$ of Co$^{2+}$ are synthesized and their magnetic properties are investigated via magnetization and heat capacity measurements. The leading in-plane antiferromagnetic exchange coupling is estimated to be $J/k_{\rm B} \simeq 4.7$ K and 5.8 K, respectively. Both the compounds feature two-step magnetic transitions at low temperatures [($T_{\rm N1} \simeq 1.47$ K and $T_{\rm N2} \simeq 1.22$ K) and ($T_{\rm N1} \simeq 0.88$ K and $T_{\rm N2} \simeq 0.67$ K), respectively], driven by weak easy-axis anisotropy. Under magnetic field Sr$_3$CoNb$_2$O$_9$ evinces a plateau at $1/3$ magnetization. Interestingly, the high field magnetization of Sr$_3$CoTa$_2$O$_9$ reveals an exotic regime (between $H_{\rm S1}$ and $H_{\rm S2}$), below the fully polarized state in which the heat capacity at low temperatures is governed by a power law ($C_{\rm p} \propto T^α$) with a reduced exponent $α\simeq 2$. These results demonstrate an unusual field induced state with gapless excitations in the strongly frustrated magnet Sr$_3$CoTa$_2$O$_9$. The complete $T-H$ phase diagram is discussed for both the compounds.

cond-mat.str-el

Probing electron-electron interaction along with superconducting fluctuations in disordered TiN thin films

Here, we demonstrate an interplay between superconducting fluctuations and electron-electron interaction (EEI) by low temperature magnetotransport measurements for a set of 2D disordered TiN thin films. While cooling down the sample, a characteristic temperature T* is obtained from the R(T) at which superconducting fluctuations start to appear. The upturn in R(T) above T* corresponds to weak localization (WL) and/or EEI. By the temperature and field dependences of the observed resistance, we show that the upturn in R(T) originates mainly from EEI with a negligible contribution from WL. Further, we have used the modified Larkins electron-electron attraction strength beta(T/Tc), containing a field induced pair breaking parameter, in the Maki-Thompson (MT) superconducting fluctuation term. Here, the temperature dependence of the beta(T/Tc) obtained from the magnetoresistance analysis shows a diverging behavior close to Tc and it remains almost constant at higher temperature within the limit of ln(T/Tc) < 1. Interestingly, the variation of beta(T/Tc) on the reduced temperature (T/Tc) offers a common trend which has been closely followed by all the concerned samples presented in this study. Finally, the temperature dependence of inverse phase scattering time , as obtained from the magnetoresistance analysis, clearly shows two different regimes; the first one close to Tc follows the Ginzburg-Landau relaxation rate , whereas, the second one at high temperature varies almost linearly with temperature indicating the dominance of inelastic electron-electron scattering for the dephasing mechanism. These two regimes are followed in a generic way by all the samples in spite of being grown under different growth conditions.

cond-mat.supr-con

Large exchange bias and low temperature glassy state in frustrated triangular-lattice antiferromagnet Ba$_3$NiIr$_2$O$_9$

Here, we report both ac and dc magnetization, thermodynamic and electric properties of hexagonal Ba$_3$NiIr$_2$O$_9$. The Ni$^{2+}$ (spin-1) forms layered triangular-lattice and interacts antiferromagnetically while Ir$^{5+}$ is believed to act as magnetic link between the layers. This complex magnetic interaction results in magnetic frustration leading to a spin-glass transition at $T_f$ $\sim$ 8.5 K. The observed magnetic relaxation and aging effect also confirms the nonequilibrium ground state. The system further shows large exchange bias which is tunable with cooling field. Below the Curie-Weiss temperature $θ_{CW}$ ($\sim$ -29 K), the magnetic specific heat $C_m$ displays a broad hump and at low temperature follows $C_m = γT^α$ dependence where both $γ$ and $α$ show dependence on temperature and magnetic field. A sign change in magnetoresistace is observed which is due to an interplay among magnetic moment, field and spin-orbit coupling.

cond-mat.str-el

A Robust nitridation technique for fabrication of disordered superconducting TiN thin films featuring phase slip events

Disorder induced phase slip (PS) events appearing in the current voltage characteristics (IVCs) are reported for two-dimensional TiN thin films produced by a robust substrate mediated nitridation technique. Here, high temperature annealing of Ti/Si3N4 based metal/substrate assembly is the key to produce majority phase TiN accompanied by TiSi2 and elemental Si as minority phases. The method itself introduces different level of disorder intrinsically by tuning the amount of the non-superconducting minority phases that are controlled by annealing temperature (Ta) and the film thickness. The superconducting critical temperature (Tc) strongly depends on Ta and the maximum Tc obtained from the demonstrated technique is about 4.8 K for the thickness range of about 12 nm and above. Besides, the dynamics of IVCs get modulated by the appearance of intermediated resistive steps for decreased Ta and the steps get more prominent for reduced thickness. Further, the deviation in the temperature dependent critical current (Ic) from the Ginzburg-Landau theoretical limit varies strongly with the thickness. Finally, the Tc, intermediate resistive steps in the IVCs and the depairing current are observed to alter in a similar fashion with Ta and the thickness indicating the robustness of the synthesis process to fabricate disordered nitride-based superconductor.

cond-mat.supr-con