Coupled spin-lattice fluctuations in a compound with orbital degrees of freedom: the Cr based dimer system Sr3Cr2O8

We report on an extended fluctuation regime in the spin dimer system Sr3Cr2O8 based on anomalies in Raman active phonons and magnetic scattering. The compound has two characteristic temperatures, TS = 275 K, related to a Jahn-Teller transition with structural distortions and orbital ordering and a second, T*= 150 K, which is due to further changes in the orbital sector. Below TS quasielastic scattering marks strong fluctuations and in addition phonon anomalies are observed. For temperatures below T* we observe an exponential decrease of one phonon linewidth and determine a gap of the orbital excitations. At low temperatures the observation of two- and three-magnon scattering allows the determination of the spin excitation gap.Comment: 7 pages, 4 figures, 1 tabl

Magnetic Structure and Interactions in the Quasi-1D Antiferromagnet CaV2_2O4_4

CaV$_2$O$_4$ is a spin-1 antiferromagnet, where the magnetic vanadium ions are arranged on quasi-one-dimensional (1D) zig-zag chains with potentially frustrated antiferromagnetic exchange interactions. High temperature susceptibility and single-crystal neutron diffraction measurements are used to deduce the non-collinear magnetic structure, dominant exchange interactions and orbital configurations. The results suggest that at high temperatures CaV$_2$O$_4$ behaves as a Haldane chain, but at low temperatures, orbital ordering lifts the frustration and it becomes a spin-1 ladder.Comment: 5 pages, 4 figure

From confined spinons to emergent fermions: Observation of elementary magnetic excitations in a transverse-field Ising chain

We report on spectroscopy study of elementary magnetic excitations in an Ising-like antiferromagnetic chain compound SrCo$_2$V$_2$O$_8$ as a function of temperature and applied transverse magnetic field up to 25 T. An optical as well as an acoustic branch of confined spinons, the elementary excitations at zero field, are identified in the antiferromagnetic phase below the N\'{e}el temperature of 5 K and described by a one-dimensional Schr\"{o}dinger equation. The confinement can be suppressed by an applied transverse field and a quantum disordered phase is induced at 7 T. In this disordered paramagnetic phase, we observe three emergent fermionic excitations with different transverse-field dependencies. The nature of these modes is clarified by studying spin dynamic structure factor of a 1D transverse-field Heisenberg-Ising (XXZ) model using the method of infinite time evolving block decimation. Our work reveals emergent quantum phenomena and provides a concrete system for testifying theoretical predications of one-dimension quantum spin models.Comment: 8 pages and 6 figure

Physical realization of a quantum spin liquid based on a novel frustration mechanism

Unlike conventional magnets where the magnetic moments are partially or completely static in the ground state, in a quantum spin liquid they remain in collective motion down to the lowest temperatures. The importance of this state is that it is coherent and highly entangled without breaking local symmetries. Such phenomena is usually sought in simple lattices where antiferromagnetic interactions and/or anisotropies that favor specific alignments of the magnetic moments are "frustrated" by lattice geometries incompatible with such order e.g. triangular structures. Despite an extensive search among such compounds, experimental realizations remain very few. Here we describe the investigation of a novel, unexplored magnetic system consisting of strong ferromagnetic and weaker antiferromagnetic isotropic interactions as realized by the compound Ca$_{10}$Cr$_7$O$_{28}$. Despite its exotic structure we show both experimentally and theoretically that it displays all the features expected of a quantum spin liquid including coherent spin dynamics in the ground state and the complete absence of static magnetism.Comment: Modified version accepted in Nature Physic

Non-Abelian statistics in light scattering processes across interacting Haldane chains

The $S=1$ Haldane state is constructed from a product of local singlet dimers in the bulk and topological states at the edges of a chain. It is a fundamental representative of topological quantum matter. Its well-known representative, the quasi-one-dimensional SrNi$_2$V$_2$O$_8$ shows both conventional as well as unconventional magnetic Raman scattering. The former is observed as one- and two-triplet excitations with small linewidths and energies corresponding to the Haldane gap $\Delta_H$ and the exchange coupling $J_c$ along the chain, respectively. Well-defined magnetic quasiparticles are assumed to be stabilized by interchain interactions and uniaxial single-ion anisotropy. Unconventional scattering exists as broad continua of scattering with an intensity $I(T)$ that shows a mixed bosonic / fermionic statistic. Such a mixed statistic has also been observed in Kitaev spin liquids and could point to a non-Abelian symmetry. As the ground state in the bulk of SrNi$_2$V$_2$O$_8$ is topologically trivial, we suggest its fractionalization to be due to light-induced interchain exchange processes. These processes are supposed to be enhanced due to a proximity to an Ising ordered state with a quantum critical point. A comparison with SrCo$_2$V$_2$O$_8$, the $S=1/2$ analogue to our title compound, supports these statements.Comment: 3 figures, 1 tabl

Field-induced effects in the spin liquid candidate PbCuTe2_{2}O6_{6}

PbCuTe$_2$O$_6$ is considered as one of the rare candidate materials for a three-dimensional quantum spin liquid (QSL). This assessment was based on the results of various magnetic experiments, performed mainly on polycrystalline material. More recent measurements on single crystals revealed an even more exotic behavior, yielding ferroelectric order below $T_{\text{FE}}\approx 1\,\text{K}$, accompanied by distinct lattice distortions, and a somewhat modified magnetic response which is still consistent with a QSL. Here we report on low-temperature measurements of various thermodynamic, magnetic and dielectric properties of single crystalline PbCuTe$_2$O$_6$ in magnetic fields $B\leq 14.5\,\text{T}$. The combination of these various probes allows us to construct a detailed $B$-$T$ phase diagram including a ferroelectric phase for $B \leq$ $8\,\text{T}$ and a $B$-induced magnetic phase at $B \geq$ $11\,\text{T}$. These phases are preceded by or coincide with a structural transition from a cubic high-temperature phase into a distorted non-cubic low-temperature state. The phase diagram discloses two quantum critical points (QCPs) in the accessible field range, a ferroelectric QCP at $B_{c1}$ = $7.9\,\text{T}$ and a magnetic QCP at $B_{c2}$ = $11\,\text{T}$. Field-induced lattice distortions, observed in the state at $T>$ $1\,\text{K}$ and which are assigned to the effect of spin-orbit interaction of the Cu$^{2+}$-ions, are considered as the key mechanism by which the magnetic field couples to the dielectric degrees of freedom in this material

Spin liquid and ferroelectricity close to a quantum critical point in PbCuTe2O6

Geometrical frustration among interacting spins combined with strong quantum fluctuations destabilize long-range magnetic order in favour of more exotic states such as spin liquids. By following this guiding principle, a number of spin liquid candidate systems were identified in quasi-two-dimensional (quasi-2D) systems. For 3D, however, the situation is less favourable as quantum fluctuations are reduced and competing states become more relevant. Here we report a comprehensive study of thermodynamic, magnetic and dielectric properties on single crystalline and pressed-powder samples of PbCuTe$_2$O$_6$, a candidate material for a 3D frustrated quantum spin liquid featuring a hyperkagome lattice. Whereas the low-temperature properties of the powder samples are consistent with the recently proposed quantum spin liquid state, an even more exotic behaviour is revealed for the single crystals. These crystals show ferroelectric order at $T_{\text{FE}} \approx 1\,\text{K}$, accompanied by strong lattice distortions, and a modified magnetic response -- still consistent with a quantum spin liquid -- but with clear indications for quantum critical behaviour.Comment: 59 pages, 15 figures, This version of the article has been accepted for publication, after peer review but is not the Version of Record and does not reflect post-acceptance improvements, or any corrections. The Version of Record is available onlin

Softened magnetic excitations in the s = 3/2 distorted triangular antiferromagnet alpha-CaCr2O4

The spin dynamics and magnetic excitations of the slightly distorted triangular s = 3/2 system alpha-CaCr2O4 are investigated by means of Raman spectroscopy and electron spin resonance (ESR) to elucidate its peculiar magnetic properties. Two-magnon excitations in circular RL symmetry show a multi-maximum structure with a dominant spectral weight at low energies. The temperature dependence of the ESR linewidth is described by a critical broadening DeltaHpp(T) ~ (T - T_N)^{-p} with the exponent p = 0.30(3) - 0.38(5) for temperatures above T_N = 42.6 K. The exponent is much smaller than that of other s = 3/2 triangular lattices. This is ascribed to soft roton-like modes, indicative of the instability of a helical 120{\deg} phase. As an origin we discuss a complex spin topology formed by four inequivalent nearest neighbor and sizable next-nearest neighbor interactions.Comment: 7 pages, 4 figure