ABSTRACT
Establishing the physical mechanism governing exchange interactions is fundamental for exploring exotic phases such as quantum spin liquids in real materials. In this Letter, we address exchange interactions in Sr_{2}CuTe_{x}W_{1-x}O_{6}, a series of double perovskites that realize a spin-1/2 square lattice and are suggested to harbor a quantum spin liquid ground state arising from the random distribution of nonmagnetic ions. Our ab initio multireference configuration interaction calculations show that replacing Te atoms with W atoms changes the dominant couplings from nearest to next-nearest neighbor due to the crucial role of unoccupied states of the nonmagnetic ions in the super-superexchange mechanism. Combined with spin-wave theory simulations, our calculated exchange couplings provide an excellent description of the inelastic neutron scattering spectra of the parent compounds, as well as explaining that the magnetic excitations in Sr_{2}CuTe_{0.5}W_{0.5}O_{6} emerge from bond-disordered exchange couplings. Our results demonstrate the crucial role of the nonmagnetic cations in exchange interactions paving the way to further explore quantum spin liquid phases in bond-disordered materials.
ABSTRACT
We present a compact nuclear magnetic resonance (NMR) probe which is compatible with a magnet of a commercial superconducting quantum interference device magnetometer and demonstrate its application to the study of a quantum magnet. We employ trimmer chip capacitors to construct an NMR tank circuit for low temperature measurements. Using a magnetic insulator MoOPO4 with S = 1/2 (Mo5+) as an example, we show that the T-dependence of the circuit is weak enough to allow the ligand-ion NMR study of magnetic systems. Our 31P NMR results are compatible with previous bulk susceptibility and neutron scattering experiments and furthermore reveal unconventional spin dynamics.
ABSTRACT
Sr_{2}CuTeO_{6} presents an opportunity for exploring low-dimensional magnetism on a square lattice of S=1/2 Cu^{2+} ions. We employ ab initio multireference configuration interaction calculations to unravel the Cu^{2+} electronic structure and to evaluate exchange interactions in Sr_{2}CuTeO_{6}. The latter results are validated by inelastic neutron scattering using linear spin-wave theory and series-expansion corrections for quantum effects to extract true coupling parameters. Using this methodology, which is quite general, we demonstrate that Sr_{2}CuTeO_{6} is an almost ideal realization of a nearest-neighbor Heisenberg antiferromagnet but with relatively weak coupling of 7.18(5) meV.
ABSTRACT
In vortex-like spin arrangements, multiple spins can combine into emergent multipole moments. Such multipole moments have broken space-inversion and time-reversal symmetries, and can therefore exhibit linear magnetoelectric (ME) activity. Three types of such multipole moments are known: toroidal; monopole; and quadrupole moments. So far, however, the ME activity of these multipole moments has only been established experimentally for the toroidal moment. Here we propose a magnetic square cupola cluster, in which four corner-sharing square-coordinated metal-ligand fragments form a noncoplanar buckled structure, as a promising structural unit that carries an ME-active multipole moment. We substantiate this idea by observing clear magnetodielectric signals associated with an antiferroic ME-active magnetic quadrupole order in the real material Ba(TiO)Cu4(PO4)4. The present result serves as a useful guide for exploring and designing new ME-active materials based on vortex-like spin arrangements.
ABSTRACT
Recent experiments indicate that static stripe-like charge order is generic to the hole-doped copper oxide superconductors and competes with superconductivity. Here we show that a similar type of charge order is present in La5/3Sr1/3CoO4, an insulating analogue of the copper oxide superconductors containing cobalt in place of copper. The stripe phase we have detected is accompanied by short-range, quasi-one-dimensional, antiferromagnetic order, and provides a natural explanation for the distinctive hourglass shape of the magnetic spectrum previously observed in neutron-scattering measurements of La2-xSrxCoO4 and many hole-doped copper oxide superconductors. The results establish a solid empirical basis for theories of the hourglass spectrum built on short-range, quasi-static, stripe correlations.
ABSTRACT
We report ac susceptibility, specific heat, and neutron scattering measurements on a dipolar-coupled antiferromagnet LiYbF_{4}. For the thermal transition, the order-parameter critical exponent is found to be 0.20(1) and the specific-heat critical exponent -0.25(1). The exponents agree with the 2D XY/h_{4} universality class despite the lack of apparent two-dimensionality in the structure. The order-parameter exponent for the quantum phase transitions is found to be 0.35(1) corresponding to (2+1)D. These results are in line with those found for LiErF_{4} which has the same crystal structure, but largely different T_{N}, crystal field environment and hyperfine interactions. Our results therefore experimentally establish that the dimensional reduction is universal to quantum dipolar antiferromagnets on a distorted diamond lattice.
ABSTRACT
Superconductivity in layered copper oxide compounds emerges when charge carriers are added to antiferromagnetically ordered CuO(2) layers. The carriers destroy the antiferromagnetic order, but strong spin fluctuations persist throughout the superconducting phase and are intimately linked to superconductivity. Neutron scattering measurements of spin fluctuations in hole-doped copper oxides have revealed an unusual 'hour-glass' feature in the momentum-resolved magnetic spectrum that is present in a wide range of superconducting and non-superconducting materials. There is no widely accepted explanation for this feature. One possibility is that it derives from a pattern of alternating spin and charge stripes, and this idea is supported by measurements on stripe-ordered La(1.875)Ba(0.125)CuO(4) (ref. 15). Many copper oxides without stripe order, however, also exhibit an hour-glass spectrum. Here we report the observation of an hour-glass magnetic spectrum in a hole-doped antiferromagnet from outside the family of superconducting copper oxides. Our system has stripe correlations and is an insulator, which means that its magnetic dynamics can conclusively be ascribed to stripes. The results provide compelling evidence that the hour-glass spectrum in the copper oxide superconductors arises from fluctuating stripes.
ABSTRACT
We have used inelastic neutron scattering and muon-spin rotation to compare the low energy magnetic excitations in single crystals of superconducting Fe(1.01)Se(0.50)Te(0.50) and non-superconducting Fe(1.10)Se(0.25)Te(0.75). We confirm the existence of a spin resonance in the superconducting phase of Fe(1.01)Se(0.50)Te(0.50), at an energy of 7 meV and a wavevector of (1/2, 1/2, 0). The non-superconducting sample exhibits two incommensurate magnetic excitations at (1/2, 1/2, 0) ± (0.18, - 0.18, 0) which rise steeply in energy, but no resonance is observed at low energies. A strongly dispersive low energy magnetic excitation is also observed in Fe(1.10)Se(0.25)Te(0.75) close to the commensurate antiferromagnetic ordering wavevector (1/2 - δ, 0, 1/2), where δ≈0.03. The magnetic correlations in both samples are found to be quasi-two-dimensional in character and persist well above the magnetic (Fe(1.10)Se(0.25)Te(0.75)) and superconducting (Fe(1.01)Se(0.50)Te(0.50)) transition temperatures.
