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Quantum Spin Liquid in a depleted triangular lattice Iridate K$_x$Ir$_y$O$_2$

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 Added by Yogesh Singh
 Publication date 2019
  fields Physics
and research's language is English




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We report discovery of a new iridate family K$_x$Ir$_y$O$_2$ with depleted triangular lattice planes made up of edge sharing IrO$_6$ octahedra separated by K planes. Such a material interpolates between the triangular and honeycomb lattices and is a new playground for Kitaev physics. The materials are Mott insulators with $y = 1 - x/4$. Physical property measurements for the $x approx 0.85$ material are reported. Using magnetic susceptibility $chi$ versus temperature $T$ measurements we find $S_{eff} = 1/2$ moments interacting strongly with a Weiss temperature $theta approx - 180$~K and no magnetic order or spin freezing down to $T = 1.8$~K@. Heat capacity shows a broad maximum around $30$~K which is insensitive to magnetic fields and a $T$-linear low temperature behaviour with $gamma sim 10$~mJ/mol~K$^2$. These results are consistent with a gapless QSL state in K$_{0.85}$Ir$_{0.79}$O$_2$.



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We report on thermodynamic, magnetization, and muon spin relaxation measurements of the strong spin-orbit coupled iridate Ba$_3$IrTi$_2$O$_9$, which constitutes a new frustration motif made up a mixture of edge- and corner-sharing triangles. In spite of strong antiferromagnetic exchange interaction of the order of 100~K, we find no hint for long-range magnetic order down to 23 mK. The magnetic specific heat data unveil the $T$-linear and -squared dependences at low temperatures below 1~K. At the respective temperatures, the zero-field muon spin relaxation features a persistent spin dynamics, indicative of unconventional low-energy excitations. A comparison to the $4d$ isostructural compound Ba$_3$RuTi$_2$O$_9$ suggests that a concerted interplay of compass-like magnetic interactions and frustrated geometry promotes a dynamically fluctuating state in a triangle-based iridate.
A quantum spin liquid (QSL) is an exotic state of matter in which electrons spins are quantum entangled over long distances, but do not show symmetry-breaking magnetic order in the zero-temperature limit. The observation of QSL states is a central aim of experimental physics, because they host collective excitations that transcend our knowledge of quantum matter; however, examples in real materials are scarce. Here, we report neutron-scattering measurements on YbMgGaO4, a QSL candidate in which Yb3+ ions with effective spin-1/2 occupy a triangular lattice. Our measurements reveal a continuum of magnetic excitations - the essential experimental hallmark of a QSL - at very low temperature (0.06 K). The origin of this peculiar excitation spectrum is a crucial question, because isotropic nearest-neighbor interactions do not yield a QSL ground state on the triangular lattice. Using measurements of the magnetic excitations close to the field-polarized state, we identify antiferromagnetic next-nearest-neighbor interactions in the presence of planar anisotropy as key ingredients for QSL formation in YbMgGaO4.
Platelike high-quality NaYbS$_{2}$ rhombohedral single crystals with lateral dimensions of a few mm have been grown and investigated in great detail by bulk methods like magnetization and specific heat, but also by local probes like nuclear magnetic resonance (NMR), electron-spin resonance (ESR), muon-spin relaxation ($mu$SR), and inelastic neutron scattering (INS) over a wide field and temperature range. Our single-crystal studies clearly evidence a strongly anisotropic quasi-2D magnetism and an emerging spin-orbit entangled $S=1/2$ state of Yb towards low temperatures together with an absence of long-range magnetic order down to 260~mK. In particular, the clear and narrow Yb ESR lines together with narrow $^{23}$Na NMR lines evidence an absence of inherent structural distortions in the system, which is in strong contrast to the related spin-liquid candidate YbMgGaO$_{4}$ falling within the same space group $Roverline{3}m$. This identifies NaYbS$_{2}$ as a rather pure spin-1/2 triangular lattice magnet and a new putative quantum spin liquid.
Frustrated quantum magnets are expected to host many exotic quantum spin states like quantum spin liquid (QSL), and have attracted numerous interest in modern condensed matter physics. The discovery of the triangular lattice spin liquid candidate YbMgGaO$_4$ stimulated an increasing attention on the rare-earth-based frustrated magnets with strong spin-orbit coupling. Here we report the synthesis and characterization of a large family of rare-earth chalcogenides AReCh$_2$ (A = alkali or monovalent ions, Re = rare earth, Ch = O, S, Se). The family compounds share the same structure (R$bar{3}$m) as YbMgGaO$_4$, and antiferromagnetically coupled rare-earth ions form perfect triangular layers that are well separated along the $c$-axis. Specific heat and magnetic susceptibility measurements on NaYbO$_2$, NaYbS$_2$ and NaYbSe$_2$ single crystals and polycrystals, reveal no structural or magnetic transition down to 50mK. The family, having the simplest structure and chemical formula among the known QSL candidates, removes the issue on possible exchange disorders in YbMgGaO$_4$. More excitingly, the rich diversity of the family members allows tunable charge gaps, variable exchange coupling, and many other advantages. This makes the family an ideal platform for fundamental research of QSLs and its promising applications.
Rare-earth delafossites were recently proposed as promising candidates for the realization of an effective $S$=1/2 quantum spin liquid (QSL) on the triangular lattice. In contrast to the most actively studied triangular-lattice antiferromagnet YbMgGaO$_4$, which is known for considerable structural disorder due to site intermixing, NaYbS$_2$ delafossite realizes structurally ideal triangular layers. We present detailed $mu$SR studies on this regular (undistorted) triangular Yb sublattice based system with effective spin $J_{mathrm{eff}}=1/2$ in the temperature range 0.05 - 40 K. Zero-field (ZF) and longitudinal field (LF) $mu$SR studies confirm the absence of any long range magnetic order state down to 0.05K ($sim J$/80). Current $mu$SR results together with the so far available bulk characterization data suggest that NaYbS$_2$ is an ideal candidate to identify QSL ground state.
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