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Tusharkanti Dey

Publications and source records attributed to Tusharkanti Dey.

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Interplay of magnetic order and ferroelasticity in the spin-orbit coupled antiferromagnet K$_2$ReCl$_6$

The magnetic and structural phase transitions occurring in K$_2$ReCl$_6$ were studied by macroscopic and microscopic techniques. Structural phase transitions associated with rotations of the ReCl$_6$ octahedra lower the symmetry from cubic to monoclinic, form ferroelastic domains, and are visible in susceptibility, specific heat and thermal expansion measurements. In the antiferromagnetically ordered state slightly below $T_{\rm N}$=12\,K these domains can be rearranged by a magnetic field inducing a relative elongation of the polydomain crystal parallel to the field of 0.6\%. At zero field the magnetic structure in K$_2$ReCl$_6$ does not exhibit a weak ferromagnetic component, but at large magnetic field a distinct magnetic structure with a finite weak ferromagnetic component is stabilized. High magnetic fields rearrange the domains in the crystal to align the weak ferromagnetic moment parallel to the field. The altered domain structure with the crystal elongation is abruptly suppressed at lower temperature but persists upon heating to well above $T_{\rm N}$. However, heating above the lowest structural phase transition and successive cooling restore the initial shape.

cond-mat.str-el

Observation of E8 Particles in an Ising Chain Antiferromagnet

Near the transverse-field induced quantum critical point of the Ising chain, an exotic dynamic spectrum consisting of exactly eight particles was predicted, which is uniquely described by an emergent quantum integrable field theory with the symmetry of the $E_8$ Lie algebra, but rarely explored experimentally. Here we use high-resolution terahertz spectroscopy to resolve quantum spin dynamics of the quasi-one-dimensional Ising antiferromagnet BaCo$_2$V$_2$O$_8$ in an applied transverse field. By comparing to an analytical calculation of the dynamical spin correlations, we identify $E_8$ particles as well as their two-particle excitations.

cond-mat.str-el

Persistent spin dynamics in the pressurized spin-liquid candidate YbMgGaO$_4$

Single-crystal x-ray diffraction, density-functional band-structure calculations, and muon spin relaxation ($μ$SR) are used to probe pressure evolution of the triangular spin-liquid candidate YbMgGaO$_4$. The rhombohedral crystal structure is retained up to at least 10 GPa and shows a nearly uniform compression along both in-plane and out-of-plane directions, whereas local distortions caused by the random distribution of Mg$^{2+}$ and Ga$^{3+}$ remain mostly unchanged. The $μ$SR data confirm persistent spin dynamics up to 2.6 GPa and down to 250 mK with no change in the muon relaxation rate. Longitudinal-field $μ$SR reveals power-law behavior of the spin-spin autocorrelation function, both at ambient pressure and upon compression.

cond-mat.str-el

Soft and anisotropic local moments in 4$d$ and 5$d$ mixed-valence M$_2$O$_9$ dimers

We investigate via exact diagonalization of finite clusters the electronic structure and magnetism of M$_2$O$_9$ dimers in the mixed-valence hexagonal perovskites A$_3$B'M$_2$O$_9$ for various different fillings of 4$d$ and 5$d$ transition-metal M ions. We find that the magnetic moments of such dimers are determined by a subtle interplay of spin-orbit coupling, Hund's coupling, and Coulomb repulsion, as well as the electron filling of the M ions. Most importantly, the magnetic moments are anisotropic and temperature-dependent. This behavior is a result of spin-orbit coupling, magnetic field effects, and the existence of several nearly-degenerate electronic configurations whose proximity allows occupation of excited states already at room temperature. This analysis is consistent with experimental susceptibility measurements for a variety of dimer-based materials. Furthermore, we perform a survey of A$_3$B'M$_2$O$_9$ materials and propose ground-state phase diagrams for the experimentally relevant M fillings of $d^{4.5}$, $d^{3.5}$ and $d^{2.5}$. Finally, our results show that the usually applied Curie-Weiss law with a constant magnetic moment cannot be used in these spin-orbit-coupled materials.

cond-mat.str-el

Structural, thermodynamic, and local probe investigations of a honeycomb material Ag$_{3}$LiMn$_{2}$O$_{6}$

The system Ag[Li$_{1/3}$Mn$_{2/3}$]O$_{2}$ belongs to a quaternary 3R-delafossite family and crystallizes in a monoclinic symmetry with space group $C\,2/m$ and the magnetic Mn$^{4+}$($S=3/2$) ions form a honeycomb network in the $ab$-plane. An anomaly around 50 K and the presence of antiferromagnetic (AFM) coupling (Curie-Weiss temperature $θ_{CW}\sim-51$ K) were inferred from our magnetic susceptibility data. The magnetic specific heat clearly manifests the onset of magnetic ordering in the vicinity of 48\,K and the recovered magnetic entropy, above the ordering temperature, falls short of the expected value, implying the presence of short-range magnetic correlations. The (ESR) line broadening on approaching the ordering temperature $T_{\rm N}$ could be described in terms of a Berezinski-Kosterlitz-Thouless (BKT) scenario with $T_{\rm KT}=40(1)$ K. $^{7}$Li NMR line-shift probed as a function of temperature tracks the static susceptibility (K$_{iso}$) of magnetically coupled Mn$^{4+}$ ions. The $^{7}$Li spin-lattice relaxation rate (1/$T$$_{1}$) exhibits a sharp decrease below about 50 K. Combining our bulk and local probe measurements, we establish the presence of an ordered ground state for the honeycomb system Ag$_{3}$LiMn$_{2}$O$_{6}$.Our ab-initio electronic structure calculations suggest that in the $ab$-plane, the nearest neighbor (NN) exchange interaction is strong and AFM, while the next NN and the third NN exchange interactions are FM and AFM respectively. In the absence of any frustration the system is expected to exhibit long-range, AFM order, in agreement with experiment.

cond-mat.str-el

Unconventional magnetism in the 4d$^{4}$ based ($S=1$) honeycomb system Ag$_{3}$LiRu$_{2}$O$_{6}$

We have investigated the thermodynamic and local magnetic properties of the Mott insulating system Ag$_{3}$LiRu$_{2}$O$_{6}$ containing Ru$^{4+}$ (4$d$$^{4}$) for novel magnetism. The material crystallizes in a monoclinic $C2/m$ structure with RuO$_{6}$ octahedra forming an edge-shared two-dimensional honeycomb lattice with limited stacking order along the $c$-direction. The large negative Curie-Weiss temperature ($θ_{CW}$ = -57 K) suggests antiferromagnetic interactions among Ru$^{4+}$ ions though magnetic susceptibility and heat capacity show no indication of magnetic long-range order down to 1.8 K and 0.4 K, respectively. $^{7}$Li nuclear magnetic resonance (NMR) shift follows the bulk susceptibility between 120-300 K and levels off below 120 K. Together with a power-law behavior in the temperature dependent spin-lattice relaxation rate between 0.2 and 2 K, it suggest dynamic spin correlations with gapless excitations. Electronic structure calculations suggest an $S = 1$ description of the Ru-moments and the possible importance of further neighbour interactions as also bi-quadratic and ring-exchange terms in determining the magnetic properties. Analysis of our $μ$SR data indicates spin freezing below 5 K but the spins remain on the borderline between static and dynamic magnetism even at 20 mK.

cond-mat.str-el

Persistent low-temperature spin dynamics in the mixed-valence iridate Ba$_{3}$InIr$_{2}$O$_{9}$

Using thermodynamic measurements, neutron diffraction, nuclear magnetic resonance, and muon spin relaxation, we establish putative quantum spin-liquid behavior in Ba$_3$InIr$_2$O$_9$, where unpaired electrons are localized on mixed-valence Ir$_2$O$_9$ dimers with Ir$^{4.5+}$ ions. Despite the antiferromagnetic Curie-Weiss temperature on the order of 10 K, neither long-range magnetic order nor spin freezing are observed down to at least 20 mK, such that spins are short-range correlated and dynamic over nearly three decades in temperature. Quadratic power-law behavior of both the spin-lattice relaxation rate and specific heat indicates the gapless nature of the ground state. We envisage that this exotic behavior may be related to an unprecedented combination of the triangular and buckled honeycomb geometries of nearest-neighbor exchange couplings in the mixed-valence setting.

cond-mat.str-el

Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$(M = Ir, Rh): A family of 5\textit{\textcolor{black}{d}}/4\textit{\textcolor{black}{d}}-based, diluted quantum spin liquids

We report the structural and magnetic properties of the 4}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Rh) based and 5}\textit{\textcolor{black}{d }}\textcolor{black}{(M = Ir) based systems Ba$_{3}$M$_{x}$Ti$_{3-x}$O$_{9}$ (nominally $x$ = 0.5, 1). The studied compositions were found to crystallize in a hexagonal structure with the centrosymmetric space group }$P6_{3}/mmc$.\textcolor{black}{{} The structures comprise of A$_{2}$O$_{9}$ polyhedra (with the A site (possibly) statistically occupied by M and Ti) in which pairs of transition metal ions are stacked along the crystallographic }\textit{\textcolor{black}{c}}\textcolor{black}{-axis. These pairs form triangular bilayers in the $ab$-plane. The magnetic Rh and Ir ions occupy these bilayers, diluted by Ti ions even for $x$ = 1. These bilayers are separated by a triangular layer which is dominantly occupied by Ti ions. From magnetization measurements we infer strong antiferromagnetic couplings for all of the materials but the absence of any spin-freezing or spin-ordering down to 2~K. Further, specific heat measurements down to 0.35~K show no sign of a phase transition for any of the compounds. Based on these thermodynamic measurements we propose the emergence of a quantum spin liquid ground state for Ba$_{3}$Rh$_{0.5}$Ti$_{2.5}$O$_{9}$, and Ba$_{3}$Ir$_{0.5}$Ti$_{2.5}$O$_{9}$, in addition to the already reported Ba$_{3}$IrTi$_{2}$O$_{9}$. }

cond-mat.str-el

Unconventional magnetism in the spin-orbit driven Mott insulators Ba3MIr2O9 (M=Sc,Y)

We have carried out detailed bulk and local probe studies on the hexagonal oxides Ba3MIr2O9 (M=Sc,Y) where Ir is expected to have a fractional oxidation state of +4.5. In the structure, Ir-Ir dimers are arranged in an edge shared triangular network parallel to the ab plane. Whereas only weak anomalies are evident in the susceptibility data, clearer anomalies are present in the heat capacity data. Our 45Sc nuclear magnetic resonance (NMR) lineshape (first order quadrupole split) is symmetric at room temperature but becomes progressively asymmetric with decreasing temperatures. This is suggestive of distortions in the structure which could arise from progressive tilt/rotation of the IrO6 octahedra with a decrease in temperature T. The 45Sc NMR spectral weight shifts near the reference frequency with decreasing T indicating the development of magnetic singlet regions. Around 10K, a significant change in the spectrum takes place with a large intensity appearing near the reference frequency but with the spectrum remaining multi-peak. It appears from our 45Sc NMR data that in Ba3ScIr2O9 significant disorder is still present below 10K. In the case of Ba3YIr2O9, the 89Y NMR spectral lines are asymmetric at high temperatures but become nearly symmetric (single magnetic environment) below T~70K. Our 89Y spectra and T1 measurements confirm the onset of long range ordering (LRO) from a bulk of the sample at 4K in this compound. Our results suggest that Ba3YIr2O9 might be structurally distorted at room temperature (via, for example, tilt/rotations of the IrO6 octahedra) but becomes progressively a regular triangular lattice with decreasing T. The effective magnetic moments and magnetic entropy changes are strongly reduced in Ba3YIr2O9 as compared to those expected for a S=1/2 system. Similar effects have been found in other iridates which naturally have strong spin-orbit coupling (SOC).

cond-mat.str-el

Possible spin-orbit driven spin-liquid ground state in the double perovskite phase of Ba3YIr2O9

We report the structural transformation of hexagonal Ba3YIr2O9 to a cubic double perovskite form (stable in ambient conditions) under an applied pressure of 8GPa at 1273K. While the ambient pressure (AP) synthesized sample undergoes long-range magnetic ordering at 4K, the high pressure(HP) synthesized sample does not order down to 2K as evidenced from our susceptibility, heat capacity and nuclear magnetic resonance (NMR) measurements. Further, for the HP sample, our heat capacity data have the form gamma*T+beta*T3 in the temperature (T) range of 2-10K with the Sommerfeld coefficient gamma=10mJ/mol-Ir K2. The 89Y NMR shift has no T-dependence in the range of 4-120K and its spin-lattice relaxation rate varies linearly with T in the range of 8-45K (above which it is T-independent). Resistance measurements of both the samples confirm that they are semiconducting. Our data provide evidence for the formation of a 5d based, gapless, quantum spin-liquid (QSL) in the cubic (HP) phase of Ba3YIr2O9. In this picture, the T term in the heat capacity and the linear variation of 89Y 1/T1 arises from excitations out of a spinon Fermi surface. Our findings lend credence to the theoretical suggestion [G. Chen, R. Pereira, and L. Balents, Phys. Rev. B 82, 174440 (2010)] that strong spin-orbit coupling can enhance quantum fluctuations and lead to a QSL state in the double perovskite lattice.

cond-mat.str-el

75As NMR local probe study of magnetism in (Eu1-xKx)Fe2As2

75As NMR measurements were performed as a function of temperature and doping in (Eu1-xKx)Fe2As2 (x=0,0.38,0.5,0.7) samples. The large Eu2+ moments and their fluctuations are found to dominate the 75As NMR properties. The 75As nuclei close to the Eu2+ moments likely have a very short spin-spin relaxation time (T2) and are wiped out of our measurement window. The 75As nuclei relatively far from Eu2+ moments are probed in this study. Increasing the Eu content progressively decreases the signal intensity with no signal found for the full-Eu sample (x=0). The large 75As NMR linewidth arises from an inhomogeneous magnetic environment around them. The spin lattice relaxation rate (1/T1) for x=0.5 and 0.7 samples is nearly independent of temperature above 100K and results from a coupling to paramagnetic fluctuations of the Eu2+ moments. The behavior of 1/T1 at lower temperatures has contributions from the antiferromagnetic fluctuations of the Eu2+ moments as also the fluctuations intrinsic to the FeAs planes and from superconductivity.

cond-mat.supr-con

Frustration induced disordered magnetism in Ba3RuTi2O9

The title compound Ba3RuTi2O9 crystallizes with a hexagonal unit cell. It contains layers of edge shared triangular network of Ru4+ (S=1) ions. Magnetic susceptibility chi(T) and heat capacity data show no long range magnetic ordering down to 1.8K. A Curie-Weiss (CW) fitting of chi(T) yields a large antiferromagnetic CW temperature theta_CW=-166K. However, in low field, a splitting of zero field cooled (ZFC) and field cooled (FC) chi(T) is observed below ~30K. Our measurements suggest that Ba3RuTi2O9 is a highly frustrated system but only a small fraction of the spins in this system undergo a transition to a frozen magnetic state below ~30K.

cond-mat.str-el

Spin liquid behaviour in Jeff=1/2 triangular lattice Ba3IrTi2O9

Ba3IrTi2O9 crystallizes in a hexagonal structure consisting of a layered triangular arrangement of Ir4+ (Jeff=1/2). Magnetic susceptibility and heat capacity data show no magnetic ordering down to 0.35K inspite of a strong magnetic coupling as evidenced by a large Curie-Weiss temperature=-130K. The magnetic heat capacity follows a power law at low temperature. Our measurements suggest that Ba3IrTi2O9 is a 5d, Ir-based (Jeff=1/2), quantum spin liquid on a 2D triangular lattice.

cond-mat.str-el

75As NMR probe of antiferromagnetic fluctuations in Ba(Fe1-xRux)2As2

The evolution of 75As NMR parameters with composition and temperature was probed in the Ba(Fe1-xRux)2As2 system where Fe is replaced by isovalent Ru. While the Ru-end member was found to be a conventional Fermi liquid, the composition (x=0.5) corresponding to the highest Tc (20K) in this system shows an upturn in 75As 1/T1T below about 80 K evidencing the presence of antiferromagnetic (AFM) fluctuations. These results are similar to those obtained in another system with isovalent substitution BaFe2(As1-xPx)2 [Y. Nakai, T. Iye, S. Kitagawa, K. Ishida, H. Ikeda, S. Kasahara, H. Shishido, T. Shibauchi, Y. Matsuda, and T. Terashima, Phys. Rev. Lett. 105, 107003 (2010)] and point to the possible role of AFM fluctuations in driving superconductivity.

cond-mat.supr-con

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