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Atasi Chakraborty

Publications and source records attributed to Atasi Chakraborty.

23 records · Page 2Linked to original sources

Failure to achieve the $J_{eff}$~=~0 state even in nearly isolated Ir$^{5+}$ in Sr$_3$NaIrO$_6$: are iridates enough for realizing true $j$-$j$ coupling?

Spin-orbit coupling (SOC) often gives rise to interesting electronic and magnetic phases in an otherwise ordinary pool of paramagnetic heavy metal oxides. In presence of strong SOC, assumed to be working in $j$-$j$ coupling regime, 5$d^4$ iridates are generally speculated to possess a nonmagnetic $J_{eff}$~=~0 singlet ground state, which invariably gets masked due to different solid-state effects (e.g. hopping). Here, we try to probe the trueness of the atomic SOC-based proposal in an apparently 1-dimensional system, Sr$_3$NaIrO$_6$, possessing a 2$H$ hexagonal structure with well separated Ir$^{5+}$ (5$d^4$) ions. But all the detailed experimental as well as theoretical characterizations reveal that the ground state of Sr$_3$NaIrO$_6$ is not nonmagnetic, rather accommodating a significantly high effective magnetic moment on Ir$^{5+}$ ion. However our combined dc susceptibility ($χ$), ${}^{23}$Na nuclear magnetic resonance (NMR), muon-spin-relaxation/rotation ($μ$SR) and heat capacity ($C_p$) measurements clearly refute any sign of spin-freezing or ordered magnetism among the Ir$^{5+}$ moments due to geometrical exchange frustration, while in-depth zero-field (ZF) and longitudinal field (LF) $μ$SR investigations strongly point towards inhomogeneous quantum spin-orbital liquid (QSOL)-like ground state. In addition, the linear temperature dependence of both the NMR spin-lattice relaxation rate and the magnetic heat capacity at low temperatures suggest low-lying gapless spin excitations in the QSOL phase of this material. Finally, we conclude that the effective SOC realised in $d^4$ iridates are unlikely to offer a ground state which will be consistent with a purely atomic $j$-$j$ coupling description.

cond-mat.str-el↗

Unusual spin dynamics in the low-temperature magnetically ordered state of Ag$_{3}$LiIr$_{2}$O$_{6}$

Recently, there have been contrary claims of Kitaev spin-liquid behaviour and ordered behavior in the honeycomb compound Ag$_3$LiIr$_2$O$_6$ based on various experimental signatures. Our investigations on this system reveal a low-temperature ordered state with persistent dynamics down to the lowest temperatures. Magnetic order is confirmed by clear oscillations in the muon spin relaxation ($μ$SR) time spectrum below 9 K till 52 mK. Coincidentally in $^7$Li nuclear magnetic resonance, a wipe-out of the signal is observed below $\sim$ 10 K which again strongly indicates magnetic order in the low temperature regime. This is supported by our density functional theory calculations which show an appreciable Heisenberg exchange term in the spin Hamiltonian that favors magnetic ordering. The $^7$Li shift and spin-lattice relaxation rate also show anomalies at $\sim$ 50 K. They are likely related to the onset of dynamic magnetic correlations, but their origin is not completely clear. Detailed analysis of our $μ$SR data is consistent with a co-existence of incommensurate Néel and striped environments. A significant and undiminished dynamical relaxation rate ($\sim 5$ MHz) as seen in $μ$SR deep into the ordered phase indicates enhanced quantum fluctuations in the ordered state.

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Gapless quantum spin liquid in the triangular system Sr$_{3}$CuSb$_{2}$O$_{9}$

We report gapless quantum spin liquid behavior in the layered triangular Sr$_{3}$CuSb$_{2}$O$_{9}$ (SCSO) system. X-ray diffraction shows superlattice reflections associated with atomic site ordering into triangular Cu planes well-separated by Sb planes. Muon spin relaxation ($μ$SR) measurements show that the $S = \frac{1}{2}$ moments at the magnetically active Cu sites remain dynamic down to 65 mK in spite of a large antiferromagnetic exchange scale evidenced by a large Curie-Weiss temperature $θ_{\mathrm{cw}} \simeq $ -143 K as extracted from the bulk susceptibility. Specific heat measurements also show no sign of long-range order down to 0.35 K. The magnetic specific heat ($\mathit{C}$$_{\mathrm{m}}$) below 5 K reveals a $\mathit{C}$$_{\mathrm{m}}$ $=$ $γT$ + $αT$$^{2}$ behavior. The significant $T$$^{2}$ contribution to the magnetic specific heat invites a phenomenology in terms of the so-called Dirac spinon excitations with a linear dispersion. From the low-$T$ specific heat data, we estimate the dominant exchange scale to be $\sim $ 36 K using a Dirac spin liquid ansatz which is not far from the values inferred from microscopic density functional theory calculations ($\sim $ 45 K) as well as high-temperature susceptibility analysis ($\sim$ 70 K). The linear specific heat coefficient is about 18 mJ/mol-K$^2$ which is somewhat larger than for typical Fermi liquids.

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Understanding the Curious Magnetic State of Sr$_{3}$OsO$_{6}$

Motivated by the recent report on high T$_c$ ferromagnetic insulating state of single transition metal containing double perovskite compound, Sr$_3$OsO$_6$ (Wakabayashi et. al., Nature Commun {\bf 10} 535, 2019), we study this curious behavior by employing first-principles calculations in conjunction with exact diagonalization of full $t_{2g}$ multiplet problem of two Os sites. Our analysis highlights the fact that stabilization of Sr$_3$OsO$_6$ in the cubic phase in epitaxially grown thin film is the key to both ferromagnetic correlation and high temperature scale associated to it. This also provides a natural explanation for the sister compound, Ca$_3$OsO$_6$ to exhibit low T$_N$ antiferromagnetism in its monoclinic structure. Further the insulating property is found to be driven by opening of Mott gap in the half filled spin-orbit coupled $j=3/2$ manifold of $d^{2}$ Os. We point out that Sr$_2$CaOsO$_6$ which naturally forms in the cubic phase would be worthwhile to explore as a future candidate to exhibit high T$_c$ ferromagnetic insulating state in bulk form.

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.

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