Local Moment Instability of Os in Honeycomb Li2.15Os0.85O3.

Compounds with honeycomb structures occupied by strong spin orbit coupled (SOC) moments are considered to be candidate Kitaev quantum spin liquids. Here we present the first example of Os on a honeycomb structure, Li2.15(3)Os0.85(3)O3 (C2/c, a = 5.09 Å, b = 8.81 Å, c = 9.83 Å, β = 99.3°). Neutron diffraction shows large site disorder in the honeycomb layer and X-ray absorption spectroscopy indicates a valence state of Os (4.7 ± 0.2), consistent with the nominal concentration. We observe a transport band gap of Δ = 243 ± 23 meV, a large van Vleck susceptibility, and an effective moment of 0.85 μB, much lower than expected from 70% Os(+5). No evidence of long range order is found above 0.10 K but a spin glass-like peak in ac-susceptibility is observed at 0.5 K. The specific heat displays an impurity spin contribution in addition to a power law ∝T(0.63±0.06). Applied density functional theory (DFT) leads to a reduced moment, suggesting incipient itineracy of the valence electrons, and finding evidence that Li over stoichiometry leads to Os(4+)-Os(5+) mixed valence. This local picture is discussed in light of the site disorder and a possible underlying quantum spin liquid state

Emergent excitations in a geometrically frustrated magnet

Frustrated systems are ubiquitous and interesting because their behavior is difficult to predict. Magnetism offers extreme examples in the form of spin lattices where all interactions between spins cannot be simultaneously satisfied. Such geometrical frustration leads to macroscopic degeneracies, and offers the possibility of qualitatively new states of matter whose nature has yet to be fully understood. Here we have discovered how novel composite spin degrees of freedom can emerge from frustrated interactions in the cubic spinel ZnCr2O4. Upon cooling, groups of six spins self-organize into weakly interacting antiferromagnetic loops whose directors, defined as the unique direction along which the spins are aligned parallel or antiparallel, govern all low temperature dynamics. The experimental evidence comes from a measurement of the magnetic form factor by inelastic neutron scattering. While the data bears no resemblance to the atomic form factor for chromium, they are perfectly consistent with the form factor for hexagonal spin loop directors. The hexagon directors are to a first approximation decoupled from each other and hence their reorientations embody the long-sought local zero energy modes for the pyrochlore lattice.Comment: 10 pages, 4 figures upon reques

Low-temperature muon spin rotation studies of the monopole charges and currents in Y doped Ho2Ti2O7

In the ground state of Ho2Ti2O7 spin ice, the disorder of the magnetic moments follows the same rules as the proton disorder in water ice. Excitations take the form of magnetic monopoles that interact via a magnetic Coulomb interaction. Muon spin rotation has been used to probe the low-temperature magnetic behaviour in single crystal Ho2−xYxTi2O7 (x = 0, 0.1, 1, 1.6 and 2). At very low temperatures, a linear field dependence for the relaxation rate of the muon precession λ(B), that in some previous experiments on Dy2Ti2O7 spin ice has been associated with monopole currents, is observed in samples with x = 0, and 0.1. A signal from the magnetic fields penetrating into the silver sample plate due to the magnetization of the crystals is observed for all the samples containing Ho allowing us to study the unusual magnetic dynamics of Y doped spin ice

Hidden Orbital Order in URu2Si2URu_{2}Si_{2}

When matter is cooled from high temperatures, collective instabilities develop amongst its constituent particles that lead to new kinds of order. An anomaly in the specific heat is a classic signature of this phenomenon. Usually the associated order is easily identified, but sometimes its nature remains elusive. The heavy fermion metal $URu_2Si_2$ is one such example, where the order responsible for the sharp specific heat anomaly at $T_0=17 K$ has remained unidentified despite more than seventeen years of effort. In $URu_{2}Si_{2}$, the coexistence of large electron-electron repulsion and antiferromagnetic fluctuations in $URu_2Si_2$ leads to an almost incompressible heavy electron fluid, where anisotropically paired quasiparticle states are energetically favored. In this paper we use these insights to develop a detailed proposal for the hidden order in $URu_2Si_2$. We show that incommensurate orbital antiferromagnetism, associated with circulating currents between the uranium ions, can account for the local fields and entropy loss observed at the $17 K$ transition; furthermore we make detailed predictions for neutron scattering measurements

Quantum spin liquid states in the two dimensional kagome antiferromagnets, ZnxCu4-x(OD)6Cl2

A three-dimensional system of interacting spins typically develops static long-range order when it is cooled. If the spins are quantum (S = 1/2), however, novel quantum paramagnetic states may appear. The most highly sought state among them is the resonating valence bond (RVB) state in which every pair of neighboring quantum spins form entangled spin singlets (valence bonds) and the singlets are quantum mechanically resonating amongst all the possible highly degenerate pairing states. Here we provide experimental evidence for such quantum paramagnetic states existing in frustrated antiferromagnets, ZnxCu4-x(OD)6Cl2, where the S = 1/2 magnetic Cu2+ moments form layers of a two-dimensional kagome lattice. We find that in Cu4(OD)6Cl2, where distorted kagome planes are weakly coupled to each other, a dispersionless excitation mode appears in the magnetic excitation spectrum below ~ 20 K, whose characteristics resemble those of quantum spin singlets in a solid state, known as a valence bond solid (VBS), that breaks translational symmetry. Doping nonmagnetic Zn2+ ions reduces the distortion of the kagome lattice, and weakens the interplane coupling but also dilutes the magnetic occupancy of the kagome lattice. The VBS state is suppressed and for ZnCu3(OD)6Cl2 where the kagome planes are undistorted and 90% occupied by the Cu2+ ions, the low energy spin fluctuations in the spin liquid phase become featureless

Spin-lattice instability to a fractional magnetization state in the spinel HgCr2O4

Magnetic systems are fertile ground for the emergence of exotic states when the magnetic interactions cannot be satisfied simultaneously due to the topology of the lattice - a situation known as geometrical frustration. Spinels, AB2O4, can realize the most highly frustrated network of corner-sharing tetrahedra. Several novel states have been discovered in spinels, such as composite spin clusters and novel charge-ordered states. Here we use neutron and synchrotron X-ray scattering to characterize the fractional magnetization state of HgCr2O4 under an external magnetic field, H. When the field is applied in its Neel ground state, a phase transition occurs at H ~ 10 Tesla at which each tetrahedron changes from a canted Neel state to a fractional spin state with the total spin, Stet, of S/2 and the lattice undergoes orthorhombic to cubic symmetry change. Our results provide the microscopic one-to-one correspondence between the spin state and the lattice distortion

Order by disorder and spiral spin liquid in frustrated diamond lattice antiferromagnets

Frustration refers to competition between different interactions that cannot be simultaneously satisfied, a familiar feature in many magnetic solids. Strong frustration results in highly degenerate ground states, and a large suppression of ordering by fluctuations. Key challenges in frustrated magnetism are characterizing the fluctuating spin-liquid regime and determining the mechanism of eventual order at lower temperature. Here, we study a model of a diamond lattice antiferromagnet appropriate for numerous spinel materials. With sufficiently strong frustration a massive ground state degeneracy develops amongst spirals whose propagation wavevectors reside on a continuous two-dimensional ``spiral surface'' in momentum space. We argue that an important ordering mechanism is entropic splitting of the degenerate ground states, an elusive phenomena called order-by-disorder. A broad ``spiral spin-liquid'' regime emerges at higher temperatures, where the underlying spiral surface can be directly revealed via spin correlations. We discuss the agreement between these predictions and the well characterized spinel MnSc2S4

Spin chirality on a two-dimensional frustrated lattice

The collective behavior of interacting magnetic moments can be strongly influenced by the topology of the underlying lattice. In geometrically frustrated spin systems, interesting chiral correlations may develop that are related to the spin arrangement on triangular plaquettes. We report a study of the spin chirality on a two-dimensional geometrically frustrated lattice. Our new chemical synthesis methods allow us to produce large single crystal samples of KFe3(OH)6(SO4)2, an ideal Kagome lattice antiferromagnet. Combined thermodynamic and neutron scattering measurements reveal that the phase transition to the ordered ground-state is unusual. At low temperatures, application of a magnetic field induces a transition between states with different non-trivial spin-textures.Comment: 7 pages, 4 figure

Pinwheel VBS state and triplet excitations in the two-dimensional deformed kagome lattice

Determining ground states of correlated electron systems is fundamental to understanding novel phenomena in condensed matter physics. A difficulty, however, arises in a geometrically frustrated system in which the incompatibility between the global topology of an underlying lattice and local spin interactions gives rise to macroscopically degenerate ground states, potentially prompting the emergence of quantum spin states, such as resonating valence bond (RVB) and valence bond solid (VBS). Although theoretically proposed to exist in a kagome lattice -- one of the most highly frustrated lattices in two dimensions (2D) being comprised of corner-sharing triangles -- such quantum-fluctuation-induced states have not been observed experimentally. Here we report the first realization of the "pinwheel" VBS ground state in the S=1/2 deformed kagome lattice antiferromagnet Rb2Cu3SnF12. In this system, a lattice distortion breaks the translational symmetry of the ideal kagome lattice and stabilizes the VBS state.Comment: 10 pages, 4 figures and Supplemental Informatio

Oxygen-related band gap state in single crystal rubrene

A molecular exciton signature is established and investigated under different ambient conditions in rubrene single crystals. An oxygen-related band gap state is found to form in the ambient atmosphere. This state acts as an acceptor center and assists in the fast dissociation of excitons, resulting in a higher dark and photoconductivity of oxidized rubrene. The band gap state produces a well-defined photoluminescence band at an energy 0.25 eV below the energy of the 0-0 molecular exciton transition. Two-photon excitation spectroscopy shows that the states are concentrated near the surface of naturally oxidized rubrene