Ho$_3$ScO$_6$ harbours a frustrated Maple Leaf Lattice (MLL). It crystalizes in the Mg$_3$TeO$_6$-type structure, and has a centrosymmetric trigonal space group (R$\bar{3}$). This system contains stacked layers of magnetic rings along the c-axis consisting of six magnetic Ho$^{3+}$ ions forming Ho hexagons, which are connected into a 2-dimensional network by equilateral and isosceles triangles to form a rare example of a MLL. Long range magnetic order is reached below $T_N=4.1$ K with a 120$^\circ$ spin arrangement on the equilateral triangles resulting in a positive vector chirality ground state configuration.
This study explores the bulk crystal growth, structural characterization, and physical property measurements of the cubic double perovskite Ba_2CoWO_6(BCWO). In BCWO, Co+2 ions form a face-centered cubic (FCC) lattice with non-distorted cobalt octahedra. The compound exhibits long-range antiferromagnetic order below TN = 14 K. Magnetization data indicated a slight anisotropy along with a spin-flop transition at 10 kOe , a saturation field of 310 kOe and an ordered moment of 2.17 Mu_B at T = 1.6 K. Heat capacity measurements indicate an effective j = 1/2 ground state configuration, resulting from the combined effects of the crystal electric field and spin-orbit interaction. Surface photovoltage analysis reveals two optical gaps in the UV-Visible region, suggesting potential applications in photocatalysis and photovoltaics. The magnetic and optical properties highlight the significant role of orbital contributions within BCWO, indicating various other potential applications.
J. Philippe, F. Elson, M. P. N. Casati, S. Sanz, M. Metzelaars, O. Shliakhtun, O. K. Forslund, J. Lass, T. Shiroka, A. Linden, D. G. Mazzone, J. Ollivier, S. Shin, M. Medarde, B. Lake, M. Mansson, M. Bartkowiak, B. Normand, P. Kögerler, Y. Sassa, et al (2) Low-dimensional quantum magnets are a versatile materials platform for studying the emergent many-body physics and collective excitations that can arise even in systems with only short-range interactions. Understanding their low-temperature structure and spin Hamiltonian is key to explaining their magnetic properties, including unconventional quantum phases, phase transitions, and excited states. We study the metal-organic coordination compound (C$_5$H$_9$NH$_3$)$_2$CuBr$_4$ and its deuterated counterpart, which upon its discovery was identified as a candidate two-leg quantum ($S = 1/2$) spin ladder in the strong-leg coupling regime. By growing large single crystals and probing them with both bulk and microscopic techniques, we deduce that two previously unknown structural phase transitions take place between 136 K and 113 K. The low-temperature structure has a monoclinic unit cell giving rise to two inequivalent spin ladders. We further confirm the absence of long-range magnetic order down to 30 mK and discuss the implications of this two-ladder structure for the magnetic properties of (C$_5$H$_9$NH$_3$)$_2$CuBr$_4$.
Quantum spin liquids (QSL) are novel phases of matter which remain quantum disordered even at the lowest temperature. They are characterized by emergent gauge fields and fractionalized quasiparticles. Here we show that the sub-Kelvin thermal transport of the three-dimensional $S=1/2$ hyper-hyperkagome quantum magnet PbCuTe$_2$O$_6$ is governed by a sizeable charge-neutral fermionic contribution which is compatible with the itinerant fractionalized excitations of a spinon Fermi surface. We demonstrate that this hallmark feature of the QSL state is remarkably robust against sample crystallinity, large magnetic field, and field-induced magnetic order, ruling out the imitation of QSL features by extrinsic effects. Our findings thus reveal the characteristic low-energy features of PbCuTe$_2$O$_6$ which qualify this compound as a true QSL material.
The effective spin-1/2 antiferromagnetic Heisenberg-Ising chain materials, ACo$_2$V$_2$O$_8$, A = Sr, Ba, are a rich source of exotic fundamental phenomena and have been investigated for their model magnetic properties both in zero and non-zero magnetic fields. Here we investigate a new member of the family, namely PbCo$_2$V$_2$O$_8$. We synthesize powder and single crystal samples of PbCo$_2$V$_2$O$_8$ and determine its magnetic structure using neutron diffraction. Furthermore, the magnetic field/temperature phase diagrams for magnetic field applied along the c, a, and [110] crystallographic directions in the tetragonal unit cell are determined via magnetization and heat capacity measurements. A complex series of phases and quantum phase transitions are discovered that depend strongly on both the magnitude and direction of the field. Our results show that \pcvo is an effective spin-1/2 antiferromagnetic Heisenberg-Ising chain with properties that are in general comparable to those of SrCo$_2$V$_2$O$_8$ and BaCo$_2$V$_2$O$_8$. One interesting departure from the results of these related compounds, is however, the discovery of a new field-induced phase for the field direction $H\|$[110] which has not been previously observed.
In this article, we report on inelastic neutron scattering measurements on a quasi-1D antiferromagnet BaCo$_2$V$_2$O$_8$ under a transverse magnetic field applied along the (0,1,0) direction. Combining results of inelastic neutron scattering experiments, analytical analysis, and numerical simulations, we precisely studied the $E_8$ excitations appearing in the whole Brillouin zone at $B_c^{1D}\approx 4.7$ T. The energy scan at $Q=(0,0,2)$ reveals a match between the data and the theoretical prediction of energies of multiple $E_8$ excitations. Furthermore, dispersions of the lightest three $E_8$ particles have been clearly observed, confirming the existence of the $E_8$ particles in BaCo$_2$V$_2$O$_8$. Our results lay down a concrete ground to systematically study the physics of the exotic $E_8$ particles.
We investigate classical Heisenberg models on the distorted windmill lattice and discuss their applicability to the spin-$1/2$ spin liquid candidate PbCuTe$_2$O$_6$. We first consider a general Heisenberg model on this lattice with antiferromagnetic interactions $J_n$ ($n=1,2,3,4$) up to fourth neighbors. Setting $J_1=J_2$ (as approximately realized in PbCuTe$_2$O$_6$) we map out the classical ground state phase diagram in the remaining parameter space and identify a competition between $J_3$ and $J_4$ that opens up interesting magnetic scenarios. Particularly, these couplings tune the ground states from coplanar commensurate or non-coplanar incommensurate magnetically ordered states to highly degenerate ground state manifolds with subextensive or extensive degeneracies. In the latter case, we uncover an unusual classical spin liquid defined on a lattice of corner sharing octahedra. We then focus on the particular set of interaction parameters $J_n$ that has previously been proposed for PbCuTe$_2$O$_6$ and investigate the system's incommensurate magnetic ground state order and finite temperature multistage ordering mechanism. We perform extensive finite temperature simulations of the system's dynamical spin structure factor and compare it with published neutron scattering data for PbCuTe$_2$O$_6$ at low temperatures. Our results demonstrate that thermal fluctuations in the classical model can largely explain the signal distribution in the measured spin structure factor but we also identify distinct differences. Our investigations make use of a variety of different analytical and numerical approaches for classical spin systems, such as Luttinger-Tisza, classical Monte Carlo, iterative minimization, and molecular dynamics simulations.
The magnetic excitation spectrum and Hamiltonian of the quantum magnet BaCuTe2O6 is studied by inelastic neutron scattering (INS) and density functional theory (DFT). INS on powder and single crystal samples reveals overlapping spinon continuua - the spectrum of an antiferromagnetic spin-1/2 spin chain - due to equivalent chains running along the a, b, and c directions. Long-range magnetic order onsets below TN = 6.3 K due to interchain interactions, and is accompanied by the emergence of sharp spin-wave excitations which replace the continuua at low energies. The spin-wave spectrum is highly complex and was successfully modelled achieving excellent agreement with the data. The extracted interactions reveal an intrachain interaction, J3 = 2.9 meV, while the antiferromagnetic hyperkagome interaction J2, is the sub-leading interaction responsible for coupling the chains together in a frustrated way. DFT calculations reveal a similar picture for BaCuTe2O6 of dominant J3 and sub-leading J2 antiferromagnetic interactions and also indicate a high sensitivity of the interactions to small changes of structure which could explain the very different Hamiltonians observed in the sister compounds SrCuTe2O6 and PbCuTe2O6.
Paul Eibisch, Christian Thurn, Arif Ata, Ulrich Tutsch, Yohei Saito, Steffi Hartmann, Bernd Wolf, Abanoub R. N. Hanna, A. T. M. Nazmul Islam, Shravani Chillal, Bella Lake, Michael Lang 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.
Aimed at a more realistic classical description of natural quantum systems, we present a two-dimensional tensor network algorithm to study finite temperature properties of frustrated model quantum systems and real quantum materials. For this purpose, we introduce the infinite projected entangled simplex operator ansatz to study thermodynamic properties. To obtain state-of-the-art benchmarking results, we explore the highly challenging spin-1/2 Heisenberg anti-ferromagnet on the Kagome lattice, a system for which we investigate the melting of the magnetization plateaus at finite magnetic field and temperature. Making close connection to actual experimental data of real quantum materials, we go on to studying the finite temperature properties of Ca$_{10}$Cr$_7$O$_{28}$. We compare the magnetization curve of this material in the presence of an external magnetic field at finite temperature with classically simulated data. As a first theoretical tool that incorporates both thermal fluctuations as well as quantum correlations in the study of this material, our work contributes to settling the existing controversy between the experimental data and previous theoretical works on the magnetization process.
While it is established that the pinch point scattering pattern in spin ice arises from an emergent coulomb phase associated with magnetic moment that is divergence-free, more complex Hamiltonians can introduce a divergence-full part. If these two parts remain decoupled, they give rise to the co-existence of distinct features. Here we show that the moment in ${\rm Nd_2Hf_2O_7}$ forms a static long-range ordered ground state, a flat, gapped pinch point excitation and dispersive excitations. These results confirm recent theories which predict that the dispersive modes, which arise from the divergence-full moment, host a pinch point pattern of their own, observed experimentally as `half-moons'.
The interplay of interactions and disorder in a quantum many body system may lead to the elusive phenomenon of many body localization (MBL). It has been observed under precisely controlled conditions in synthetic quantum many-body systems, but to detect it in actual quantum materials seems challenging. In this work, we present a path to synthesize real materials that show signatures of many body localization by mixing different species of materials in the laboratory. To provide evidence for the functioning of our approach, we perform a detailed tensor-network based numerical analysis to study the effects of various doping ratios of the constituting materials. Moreover, in order to provide guidance to experiments, we investigate different choices of actual candidate materials. To address the challenge of how to achieve stability under heating, we study the effect of the electron-phonon coupling, focusing on effectively one dimensional materials embedded in one, two and three dimensional lattices. We analyze how this coupling affects the MBL and provide an intuitive microscopic description of the interplay between the electronic degrees of freedom and the lattice vibrations. Our work provides a guideline for the necessary conditions on the properties of the ingredient materials and, as such, serves as a road map to experimentally synthesizing real quantum materials exhibiting signatures of MBL.
Traditional spectroscopy, by its very nature, characterizes properties of physical systems in the momentum and frequency domains. The most interesting and potentially practically useful quantum many-body effects however emerge from the deep composition of local, short-time correlations. Here, using inelastic neutron scattering and methods of integrability, we experimentally observe and theoretically describe a local, coherent, long-lived, quasiperiodically oscillating magnetic state emerging out of the distillation of propagating excitations following a local quantum quench in a Heisenberg antiferromagnetic chain. This "quantum wake" displays similarities to Floquet states, discrete time crystals and nonlinear Luttinger liquids.
Single crystals of the three-dimensional frustrated magnet and spin liquid candidate compound PbCuTe$_2$O$_6$ were grown using both the Travelling Solvent Floating Zone (TSFZ) and the Top-Seeded Solution Growth (TSSG) techniques. The growth conditions were optimized by investigating the thermal properties. The quality of the crystals was checked by polarized optical microscopy, X-ray Laue and X-ray powder diffraction, and compared to the polycrystalline samples. Excellent quality crystals were obtained by the TSSG method. Magnetic measurements of these crystals revealed a small anisotropy for different crystallographic directions in comparison with the previously reported data. The heat capacity of both single crystal and powder samples reveal a transition anomaly around 1 K. Curiously the position and magnitude of the transition are strongly dependent on the crystallite size and it is almost entirely absent for the smallest crystallites. A structural transition is suggested which accompanies the reported ferroelectric transition, and a scenario whereby it becomes energetically unfavourable in small crystallites is proposed.
The magnetic Hamiltonian of the Heisenberg quantum antiferromagnet SrCuTe$_{2}$O$_{6}$ is studied by inelastic neutron scattering technique on powder and single crystalline samples above and below the magnetic transition temperatures at 8 K and 2 K. The high temperature spectra reveal a characteristic diffuse scattering corresponding to a multi-spinon continuum confirming the dominant quantum spin-chain behavior due to the third neighbour interaction J$_{intra}$ = 4.22 meV (49 K). The low temperature spectra exhibits sharper excitations at energies below 1.25 meV which can be explained by considering a combination of weak antiferromagnetic first nearest neighbour interchain coupling J$_1$ = 0.17 meV (1.9 K) and even weaker ferromagnetic second nearest neighbour J$_2$ = -0.037 meV (-0.4 K) or a weak ferromagnetic J$_2$ = -0.11 meV (-1.3 K) and antiferromagnetic J$_6$ = 0.16 meV (1.85 K) giving rise to the long-range magnetic order and spin-wave excitations at low energies. These results suggest that SrCuTe$_{2}$O$_{6}$ is a highly one-dimensional Heisenberg system with three mutually perpendicular spin-chains coupled by a weak ferromagnetic J$_2$ in addition to the antiferromagnetic J$_1$ or J$_6$ presenting a contrasting scenario from the highly frustrated hyper-hyperkagome lattice (equally strong antiferromagnetic J$_1$ and J$_2$) found in the iso-structural PbCuTe$_{2}$O$_{6}$.
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.
Alsu Gazizulina, Diana Lucia Quintero-Castro, Zhe Wang, Fabienne Duc, Frederic Bourdarot, Karel Prokes, Wolfgang Schmidt, Ramzy Daou, Sergei Zherlitsyn, Nazmul Islam, Nils Henrik Kolnes, Abhijit Bhat Kademane, Andreas Schilling, Bella Lake In this work, we investigate the evolution and settling of magnon condensation in the spin-1/2 dimer system Sr$_{3}$Cr$_{2}$O$_{8}$ using a combination of magnetostriction in pulsed fields and inelastic neutron scattering in a continuous magnetic field. The magnetic structure in the Bose-Einstein condensation (BEC) phase was probed by neutron diffraction in pulsed magnetic fields up to 39~T. The magnetic structure in this phase was confirmed to be an XY-antiferromagnetic structure validated by irreducible representational analysis. The magnetic phase diagram as a function of an applied magnetic field for this system is presented. Furthermore, zero-field neutron diffraction results indicate that dimerization plays an important role in stabilizing the low-temperature crystal structure.
Christian Thurn, Paul Eibisch, Arif Ata, Maximilian Winkler, Peter Lunkenheimer, István Kézsmárki, Ulrich Tutsch, Yohei Saito, Steffi Hartmann, Jan Zimmermann, Abanoub R. N. Hanna, A. T. M. Nazmul Islam, Shravani Chillal, Bella Lake, Bernd Wolf, Michael Lang 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.
Walter Schnelle, Beluvalli E. Prasad, Claudia Felser, Martin Jansen, Evgenia V. Komleva, Sergey V. Streltsov, Igor I. Mazin, Dmitry Khalyavin, Pascal Manuel, Sukanya Pal, D. V. S. Muthu, A. K. Sood, Ekaterina S. Klyushina, Bella Lake, Jean-Christophe Orain, Hubertus Luetkens The silver ruthenium oxide AgRuO$_3$ consists of honeycomb [Ru$_2^{5+}$O$_6^{2-}$] layers, and can be considered an analogue of SrRu$_2$O$_6$ with a different intercalation stage. We present measurements of magnetic susceptibility and specific heat on AgRuO$_3$ single crystals which reveal a sharp antiferromagnetic transition at 342(3)K. The electrical transport in single crystals of AgRuO$_3$ is determined by a combination of activated conduction over an intrinsic semiconducting gap of $\approx$ 100 meV and carriers trapped and thermally released from defects. From powder neutron diffraction data a Néel-type antiferromagnetic structure with the Ru moments along the $c$ axis is derived. Raman and muon spin rotation spectroscopy measurements on AgRuO$_3$ powder samples indicate a further weak phase transition or a crossover in the temperature range 125-200 K. The transition does not show up in magnetic susceptibility and its origin is argued to be related to defects but cannot be fully clarified. The experimental findings are complemented by DFT-based electronic structure calculations. It is found that the magnetism in AgRuO$_3$ is similar to that of SrRu$_2$O$_6$, however with stronger intralayer and weaker interlayer magnetic exchange interactions.
We demonstrate how quantum entanglement can be directly witnessed in the quasi-1D Heisenberg antiferromagnet KCuF$_3$. We apply three entanglement witnesses --- one-tangle, two-tangle, and quantum Fisher information --- to its inelastic neutron spectrum, and compare with spectra simulated by finite-temperature density matrix renormalization group (DMRG) and classical Monte Carlo methods. We find that each witness provides direct access to entanglement. Of these, quantum Fisher information is the most robust experimentally, and indicates the presence of at least bipartite entanglement up to at least 50 K, corresponding to around 10% of the spinon zone-boundary energy. We apply quantum Fisher information to higher spin-S Heisenberg chains, and show theoretically that the witnessable entanglement gets suppressed to lower temperatures as the quantum number increases. Finally, we outline how these results can be applied to higher dimensional quantum materials to witness and quantify entanglement.
We investigate the structural and magnetic properties of the new quantum magnet BaCuTe$_2$O$_6$. This compound is synthesized for the first time in powder and single crystal form. Synchrotron X-ray and neutron diffraction reveal a cubic crystal structure (P4$_1$32) where the magnetic Cu$^{2+}$ ions form a complex network. Physical properties measurements suggest the presence of antiferromagnetic interactions with a Curie-Weiss temperature of -33K, while long-range magnetic order occurs at the much lower temperature of ~6.3K. The magnetic structure, solved using neutron diffraction, reveals antiferromagnetic order along chains parallel to the a, b and c crystal axes. This is consistent with the magnetic excitations which resemble the multispinon continuum typical of the spin-1/2 Heisenberg antiferromagnetic chain. A consistent intrachain interaction value of ~34K is achieved from the various techniques. Finally the magnetic structure provides evidence that the chains are coupled together in a non-colinear arrangement by a much weaker antiferromagnetic, frustrated hyperkagome interaction.
We investigate the critical properties of the spin-$1$ honeycomb antiferromagnet BaNi$_2$V$_2$O$_8$, both below and above the ordering temperature $T_N$ using neutron diffraction and muon spin rotation measurements. Our results characterize BaNi$_2$V$_2$O$_8$ as a two-dimensional (2D) antiferromagnet across the entire temperature range, displaying a series of crossovers from 2D Ising-like to 2D XY and then to 2D Heisenberg behavior with increasing temperature. In particular, the extracted critical exponent of the order parameter reveals a narrow temperature regime close to $T_N$, in which the system behaves as a 2D XY antiferromagnet. Above $T_N$, evidence for Berezinsky-Kosterlitz-Thouless behavior driven by vortex excitations is obtained from the scaling of the correlation length. Our experimental results are in accord with classical and quantum Monte Carlo simulations performed for microscopic magnetic model Hamiltonians for BaNi$_2$V$_2$O$_8$.
S.Chillal, E.Schierle, E.Weschke, F.Yokaichiya, J.-U.Hoffmann, O.S.Volkova, A.N.Vasiliev, A.A.Sinchenko, P.Lejay, A.Hadj-Azzem, P.Monceau, B.Lake We report a ground state with strongly coupled magnetic and charge density wave orders mediated via orbital ordering in the layered compound \tbt. In addition to the commensurate antiferromagnetic (AFM) and charge density wave (CDW) orders, new magnetic peaks are observed whose propagation vector equals the sum of the AFM and CDW propagation vectors, revealing an intricate and highly entwined relationship. This is especially interesting given that the magnetic and charge orders lie in different layers of the crystal structure where the highly localized magnetic moments of the Tb$^{3+}$ ions are netted in the Tb-Te stacks, while the charge order is formed by the conduction electrons of the adjacent Te-Te layers. Our results, based on neutron diffraction and resonant x-ray scattering reveal that the charge and magnetic subsystems mutually influence each other via the orbital ordering of Tb$^{3+}$ ions.
S. Wimmer, J. Sánchez-Barriga, P. Küppers, A. Ney, E. Schierle, F. Freyse, O. Caha, J. Michalicka, M. Liebmann, D. Primetzhofer, M. Hoffmann, A. Ernst, M. M. Otrokov, G. Bihlmayer, E. Weschke, B. Lake, E. V. Chulkov, M. Morgenstern, G. Bauer, G. Springholz, et al (1) Ferromagnetic topological insulators exhibit the quantum anomalous Hall effect that might be used for high precision metrology and edge channel spintronics. In conjunction with superconductors, they could host chiral Majorana zero modes which are among the contenders for the realization of topological qubits. Recently, it was discovered that the stable 2+ state of Mn enables the formation of intrinsic magnetic topological insulators with A1B2C4 stoichiometry. However, the first representative, MnBi2Te4, is antiferromagnetic with 25 K Néel temperature and strongly n-doped. Here, we show that p-type MnSb2Te4, previously considered topologically trivial, is a ferromagnetic topological insulator in the case of a few percent of Mn excess. It shows (i) a ferromagnetic hysteresis with record high Curie temperature of 45-50 K, (ii) out-of-plane magnetic anisotropy and (iii) a two-dimensional Dirac cone with the Dirac point close to the Fermi level which features (iv) out-of-plane spin polarization as revealed by photoelectron spectroscopy and (v) a magnetically induced band gap that closes at the Curie temperature as demonstrated by scanning tunneling spectroscopy. Moreover, it displays (vi) a critical exponent of magnetization beta~1, indicating the vicinity of a quantum critical point. Ab initio band structure calculations reveal that the slight excess of Mn that substitutionally replaces Sb atoms provides the ferromagnetic interlayer coupling. Remaining deviations from the ferromagnetic order, likely related to this substitution, open the inverted bulk band gap and render MnSb2Te4 a robust topological insulator and new benchmark for magnetic topological insulators.
T. Nomura, Y. Skourski, D. L. Quintero-Castro, A.A. Zvyagin, A. V. Suslov, D. Gorbunov, S. Yasin, J. Wosnitza, K. Kindo, A. T. M. N. Islam, B. Lake, Y. Kohama, S. Zherlitsyn, M. Jaime Combined experimental and modeling studies of the magnetocaloric effect, ultrasound, and magnetostriction were performed on single-crystal samples of the spin-dimer system Sr$_3$Cr$_2$O$_8$ in large magnetic fields, to probe the spin-correlated regime in the proximity of the field-induced XY-type antiferromagnetic order also referred to as a Bose-Einstein condensate of magnons. The magnetocaloric effect, measured under adiabatic conditions, reveals details of the field-temperature ($H,T$) phase diagram, a dome characterized by critical magnetic fields $H_{c1}$ = 30.4 T, $H_{c2}$ = 62 T, and a single maximum ordering temperature $T_{{\rm max}}(45~$T$)\simeq$8 K. The sample temperature was observed to drop significantly as the magnetic field is increased, even for initial temperatures above $T_{{\rm max}}$, indicating a significant magnetic entropy associated to the field-induced closure of the spin gap. The ultrasound and magnetostriction experiments probe the coupling between the lattice degrees of freedom and the magnetism in Sr$_3$Cr$_2$O$_8$. Our experimental results are qualitatively reproduced by a minimalistic phenomenological model of the exchange-striction by which sound waves renormalize the effective exchange couplings.
SrCuTe$_2$O$_6$ consists of a 3-dimensional arrangement of spin-$\frac{1}{2}$ Cu$^{2+}$ ions. The 1st, 2nd and 3rd neighbor interactions respectively couple Cu$^{2+}$ moments into a network of isolated triangles, a highly frustrated hyperkagome lattice consisting of corner sharing triangles and antiferromagnetic chains. Of these, the chain interaction dominates in SrCuTe$_2$O$_6$ while the other two interactions lead to frustrated inter-chain coupling giving rise to long range magnetic order at suppressed temperatures. In this paper, we investigate the magnetic properties in SrCuTe$_2$O$_6$ using muon relaxation spectroscopy and neutron diffraction and present the low temperature magnetic structure.
Anup Kumar Bera, Jianda Wu, Wang Yang, Zhe Wang, Robert Bewley, Martin Boehm, Maciej Bartkowiak, Oleksandr Prokhnenko, Bastian Klemke, A. T. M. Nazmul Islam, Joseph Mathew Law, Bella Lake Complex bound states of magnetic excitations, known as Bethe string, were predicted almost a century ago to exist in one-dimensional quantum magnets 1. The dispersions of the string states have so far remained the subject of intensive theoretical studies 2-7. By performing neutron scattering experiments on the one-dimensional Heisenberg-Ising antiferromagnet SrCo2V2O8 in high longitudinal magnetic fields, we reveal in detail the dispersion relations of the string states over the full Brillouin zone, as well as their magnetic field dependences. Furthermore the characteristic energy, the scattering intensity and linewidth of the observed string states exhibit excellent agreement with our precise Bethe Ansatz calculations. Our results establish the important role of string states in the quantum spin dynamics of one-dimensional systems, and will invoke studies of their dynamical properties in more general many-body systems.
The pyrochlore material Nd$_2$Zr$_2$O$_7$ with an "all-in-all-out" (AIAO) magnetic order shows novel quantum moment fragmentation with gapped flat dynamical spin ice modes. The parameterized spin Hamiltonian with a dominant frustrated ferromagnetic transverse term reveals a proximity to a U(1) spin liquid. Here we study magnetic excitations of Nd$_2$Zr$_2$O$_7$ above the ordering temperature ($T_\text{N}$) using high-energy-resolution inelastic neutron scattering. We find strong spin ice correlations at zero energy with the disappearance of gapped magnon excitations of the AIAO order. It seems that the gap to the dynamical spin ice closes above $T_\text{N}$ and the system enters a quantum spin ice state competing with and suppressing the AIAO order. Classical Monte Carlo, molecular dynamics and quantum boson calculations support the existence of a Coulombic phase above $T_\text{N}$. Our findings relate the magnetic ordering of Nd$_2$Zr$_2$O$_7$ with the Higgs mechanism and provide explanations for several previously reported experimental features.
We study the magnetocaloric effect and critical behavior of Co$_2$Cr$_{1-x}$Mn$_x$Al ($x=$ 0.25, 0.5, 0.75) Heusler alloys across the ferromagnetic (FM) transition (T$_{\rm C}$). The Rietveld refinement of x-ray diffraction patterns exhibit single phase cubic structure for all the samples. The temperature dependent magnetic susceptibility $\chi$(T) data show a systematic enhancement in the Curie temperature and effective magnetic moment with Mn concentration, which is consistent with the Slater-Pauling behavior. The M(H) isotherms also exhibit the FM ordering and the analysis of $\chi$(T) data indicates the nature of the phase transition to be a second order, which is further supported by scaling of the entropy curves and Arrott plot. Interestingly, the Mn substitution causes an increase in the magnetic entropy change and hence large relative cooling power for multi-stage magnetic refrigerator applications. In order to understand the nature of the magnetic phase transition we examine the critical exponents $\beta$, $\gamma$, $\delta$ for the $x=$ 0.75 sample by the modified Arrott plot and the critical isotherm analysis, which is further confirmed by Kouvel-Fisher method and Widom scaling relation, respectively. The estimated values of $\beta=$ 0.507, $\gamma=$ 1.056, $\delta=$ 3.084 are found to be close to the mean field theoretical values. The renormalized isotherms (m vs h) corresponding to these exponent values collapse into two branches, above and below T$_{\rm C}$ that validates our analysis. Our results suggest for the existence of long-range FM interactions, which decays slower than power law as $J(r)\sim r^{-4.5}$ for a 3 dimensional mean field theory.
We present new experimental low-temperature heat capacity and detailed dynamical spin-structure factor data for the quantum spin liquid candidate material Ca$_{10}$Cr$_7$O$_{28}$. The measured heat capacity shows an almost perfect linear temperature dependence in the range $0.1$ K $\lesssim T\lesssim0.5$ K, reminiscent of fermionic spinon degrees of freedom. The spin structure factor exhibits two energy regimes of strong signal which display rather different but solely diffuse scattering features. We theoretically describe these findings by an effective spinon hopping model which crucially relies on the existence of strong ferromagnetically coupled triangles in the system. Our spinon theory is shown to naturally reproduce the overall weight distribution of the measured spin structure factor. Particularly, we argue that various different observed characteristic properties of the spin structure factor and the heat capacity consistently indicate the existence of a spinon Fermi surface. A closer analysis of the heat capacity at the lowest accessible temperatures hints towards the presence of weak $f$-wave spinon pairing terms inducing a small partial gap along the Fermi surface (except for discrete nodal Dirac points) and suggesting an overall $\mathbb{Z}_2$ quantum spin liquid scenario for Ca$_{10}$Cr$_7$O$_{28}$.
J. Xu, Owen Benton, V. K. Anand, A. T. M. N. Islam, T. Guidi, G. Ehlers, E. Feng, Y. Su, 6 A. Sakai, P. Gegenwart, B. Lake We present thermodynamic and neutron scattering measurements on the quantum spin ice candidate Nd$_2$Zr$_2$O$_7$. The parameterization of the anisotropic exchange Hamiltonian is refined based on high-energy-resolution inelastic neutron scattering data together with thermodynamic data using linear spin wave theory and numerical linked cluster expansion. Magnetic phase diagrams are calculated using classical Monte Carlo simulations with fields along \mbox[100], \mbox[110] and \mbox[111] crystallographic directions which agree qualitatively with the experiment. Large hysteresis and irreversibility for \mbox[111] is reproduced and the microscopic mechanism is revealed by mean field calculations to be the existence of metastable states and domain inversion. Our results shed light on the explanations of the recently observed dynamical kagome ice in Nd$_2$Zr$_2$O$_7$ in \mbox[111] fields.
Quantum spin liquids are exotic quantum phases of matter that do not order even at zero temperature. While there are several toy models and simple Hamiltonians that could host a quantum spin liquid as their ground state, it is very rare to find actual, realistic materials that exhibits their properties. At the same time, the classical simulation of such instances of strongly correlated systems is intricate and reliable methods are scarce. In this work, we investigate the quantum magnet Ca$_{10}$Cr$_7$O$_{28}$ that has recently been discovered to exhibit properties of a quantum spin liquid in inelastic neutron scattering experiments. This compound has a distorted bilayer Kagome lattice crystal structure consisting of Cr$^{5+}$ ions with spin-$1/2$ moments. Coincidentally, the lattice structure renders a tensor network algorithm in 2D applicable that can be seen as a new variant of a projected entangled simplex state algorithm in the thermodynamic limit. In this first numerical investigation of this material that takes into account genuine quantum correlations, good agreement with the experimental findings is found. We argue that this is one of the very first studies of physical materials in the laboratory with tensor network methods, contributing to uplifting tensor networks from conceptual tools to methods to describe real two-dimensional quantum materials.
We report the optimized conditions for growing the high quality single crystals of candidate quantum spin-ice Pr2Hf2O7 using the optical floating-zone method. Large single crystals of Pr2Hf2O7 have been grown under different growth conditions using a four-mirror type optical floating-zone furnace and their microscopic structural differences have been probed by high-resolution synchrotron x-ray diffraction (SXRD). The SXRD data reveal that the crystals grown under fowing argon (~ 2 L/h) atmosphere with slightly off-stoichiometric (optimized) starting composition yields the highest quality crystals. The magnetic susceptibility, isothermal magnetization and heat capacity data of optimally grown crystals are presented.
Superconductivity in the pseudo-binary pnictides Ru0.55Rh0.45P and Ru0.75Rh0.25As is probed by muon spin relaxation and rotation (muSR) measurements in conjuction with magnetic susceptibility, heat capacity and electrical resistivity measurements. Powder x-ray diffraction confirmed the MnP-type orthorhombic structure (space group Pnma) and showed a nearly single phase nature with small impurity phase(s) of about 5% for both the samples. The occurence of bulk superconductivity is confirmed with Tc = 3.7 K for Ru0.55Rh0.45P and T = 1.6 K for Ru0.75Rh0.25As. The superconducting state electronic heat capacity data reveal weak-coupling single-band isotropic s-wave gap BCS superconductivity. Various normal and superconducting state parameters are determined which reveal a weak-coupling electron-phonon driven type-II dirty-limit superconductivity for both the compounds. The upper critical field shows a linear temperature dependence down to the lowest measured temperatures which is quite unusual for a single-band superconductor. The muSR data confirm the conventional type-II behavior, and show evidence for a single-band s-wave singlet pairing superconductivity with a preserved time reversal symmetry for both the compounds.
Calcium vanadate CaV$_2$O$_4$ has a crystal structure of quasi-one-dimensional zigzag chains composed of orbital-active V$^{3+}$ ions and undergoes successive structural and antiferromagnetic phase transitions at $T_s\sim 140$ K and $T_N \sim 70$ K, respectively. We perform ultrasound velocity measurements on a single crystal of CaV$_2$O$_4$. The temperature dependence of its shear elastic moduli exhibits huge Curie-type softening upon cooling that emerges above and below $T_s$ depending on the elastic mode. The softening above $T_s$ suggests the presence of either onsite Jahn-Teller-type or intersite ferro-type orbital fluctuations in the two inequivalent V$^{3+}$ zigzag chains. The softening below $T_s$ suggests the occurrence of a dimensional spin-state crossover, from quasi-one to three, that is driven by the spin-lattice coupling along the inter-zigzag-chain orthogonal direction. The successive emergence of the orbital- and spin-driven lattice instabilities above and below $T_s$, respectively, is unique to the orbital-spin zigzag chain system of CaV$_2$O$_4$.
V. K. Anand, L. Opherden, J. Xu, D. T. Adroja, A. D. Hillier, P. K. Biswas, T. Herrmannsdörfer, M. Uhlarz, J. Hornung, J. Wosnitza, E. Canevet, B. Lake We report the physical properties of Tb2Hf2O7 based on ac magnetic susceptibility \chi_ac(T), dc magnetic susceptibility \chi(T), isothermal magnetization M(H), and heat capacity C_p(T) measurements combined with muon spin relaxation (\muSR) and neutron powder diffraction measurements. No evidence for long-range magnetic order is found down to 0.1 K. However, \chi_ac(T) data present a frequency-dependent broad peak (near 0.9 K at 16 Hz) indicating slow spin dynamics. The slow spin dynamics is further evidenced from the \muSR data (characterized by a stretched exponential behavior) which show persistent spin fluctuations down to 0.3 K. The neutron powder diffraction data collected at 0.1 K show a broad peak of magnetic origin (diffuse scattering) but no magnetic Bragg peaks. The analysis of the diffuse scattering data reveals a dominant antiferromagnetic interaction in agreement with the negative Weiss temperature. The absence of long-range magnetic order and the presence of slow spin dynamics and persistent spin fluctuations together reflect a dynamical ground state in Tb2Hf2O7.
Magnetic remanence - found in bar magnets or magnetic storage devices - is probably the oldest and most ubiquitous phenomenon underpinning technological applications of magnetism. It is a macroscopic non-equilibrium phenomenon: a remanent magnetisation appears when a magnetic field is applied to an initially unmagnetised ferromagnet, and then taken away. Here, we present an inverted magnetic hysteresis loop in the pyrochlore compound Nd$_2$Hf$_2$O$_7$: the remanent magnetisation points in a direction opposite to the applied field. This phenomenon is exquisitely tunable as a function of the protocol in field and temperature, and it is reproducible as in a quasi-equilibrium setting. We account for this phenomenon in considerable detail in terms of the properties of non-equilibrium population of domain walls which exhibit a magnetic moment between domains of an ordered antiferromagnetic state which itself has zero net magnetisation. Properties and (non-equilibrium) dynamics of topological defects play an important role in modern spintronics, and our study adds an instance where a uniform field couples selectively to domain walls rather than the bulk.
The magnetic properties of the two-dimensional, S=1 honeycomb antiferromagnet BaNi$_2$V$_2$O$_8$ have been comprehensively studied using DC susceptibility measurements and inelastic neutron scattering techniques. The magnetic excitation spectrum is found to be dispersionless within experimental resolution between the honeycomb layers, while it disperses strongly within the honeycomb plane where it consists of two gapped spin-wave modes. The magnetic excitations are compared to linear spin-wave theory allowing the Hamiltonian to be determined. The first- and second-neighbour magnetic exchange interactions are antiferromagnetic and lie within the ranges 10.90meV$\le$J$_n$$\le$13.35 meV and 0.85meV$\le$J$_{nn}$$\le$1.65 meV respectively. The interplane coupling J$_{out}$ is four orders of magnitude weaker than the intraplane interactions, confirming the highly two-dimensional magnetic behaviour of this compound. The sizes of the energy gaps are used to extract the magnetic anisotropies and reveal substantial easy-plane anisotropy and a very weak in-plane easy-axis anisotropy. Together these results reveal that BaNi$_2$V$_2$O$_8$ is a candidate compound for the investigation of vortex excitations and Berezinsky-Kosterliz-Thouless phenomenona.
S. Chillal, Y. Iqbal, H. O. Jeschke, J. A. Rodriguez-Rivera, R. Bewley, P. Manuel, D. Khalyavin, P. Steffens, R. Thomale, A. T. M. N. Islam, J. Reuther, B. Lake The quantum spin liquid (QSL) is a highly entangled magnetic state characterized by the absence of static magnetism in its ground state. Instead, the spins fluctuate in a highly correlated way down to the lowest temperatures. The QSL is very rare and is confined to a few specific cases where the interactions between the magnetic ions cannot be simultaneously satisfied (known as frustration). Lattices with magnetic ions in triangular or tetrahedral arrangements which interact via isotropic antiferromagnetic interactions can generate such a frustration. Three-dimensional isotropic spin liquids have mostly been sought in materials where the magnetic ions form pyrochlore or hyperkagome lattices. Here we present a three-dimensional lattice called the hyper-hyperkagome that enables spin liquid behaviour and manifests in the compound PbCuTe$_{2}$O$_{6}$. Using a combination of experiment and theory we show that this system exhibits signs of being a quantum spin liquid with no detectable static magnetism together with the presence of diffuse continua in the magnetic spectrum suggestive of fractional spinon excitations.
Nd2Hf2O7, belonging to the family of geometrically frustrated cubic rare earth pyrochlore oxides, was recently identified to order antiferromagnetically below T_N = 0.55 K with an all-in/all-out arrangement of Nd3+ moments, however with a much reduced ordered state moment. Herein we investigate the spin dynamics and crystal field states of Nd2Hf2O7 using muon spin relaxation (muSR) and inelastic neutron scattering (INS) measurements. Our muSR study confirms the long range magnetic ordering and shows evidence for coexisting persistent dynamic spin fluctuations deep inside the ordered state down to 42 mK. The INS data show the crytal electric field (CEF) excitations due to the transitions both within the ground state multiplet and to the first excited state multiplet. The INS data are analyzed by a model based on CEF and crystal field states are determined. Strong Ising-type anisotropy is inferred from the ground state wavefunction. The CEF parameters indicate the CEF-split Kramers doublet ground state of Nd3+ to be consistent with the dipolar-octupolar character.
Zhe Wang, Jianda Wu, Wang Yang, Anup Kumar Bera, Dmytro Kamenskyi, A.T.M. Nazmul Islam, Shenglong Xu, Joseph Matthew Law, Bella Lake, Congjun Wu, Alois Loidl Almost one century ago, string states - complex bound states (Wellenkomplexe) of magnetic excitations - have been predicted to exist in one-dimensional quantum magnets and since then become a subject of intensive theoretical study. However, experimental realization and identification of string states in condensed-matter systems remains an unsolved challenge up to date. Here we use high-resolution terahertz spectroscopy to identify string states in the antiferromagnetic Heisenberg-Ising chain SrCo2V2O8 in strong longitudinal magnetic fields. We observe complex bound states (strings) and fractional magnetic excitations (psinons and antipsinons) in the field-induced critical regime, which are precisely described by the Bethe ansatz. Our study reveals that two-string and three-string states govern the quantum spin dynamics close to the quantum criticality, while the fractional excitations are dominant at low energies, reflecting the antiferromagnetic quantum fluctuations.
Confinement is a process by which particles with fractional quantum numbers bind together to form quasiparticles with integer quantum numbers. The constituent particles are confined by an attractive interaction whose strength increases with increasing particle separation and as a consequence, individual particles are not found in isolation. This phenomenon is well known in particle physics where quarks are confined in baryons and mesons. An analogous phenomenon occurs in certain magnetic insulators; weakly coupled chains of spins S=1/2. The collective excitations in these systems is spinons (S=1/2). At low temperatures weak coupling between chains can induce an attractive interaction between pairs of spinons that increases with their separation and thus leads to confinement. In this paper, we employ inelastic neutron scattering to investigate the spinon confinement in the quasi-1D S=1/2 XXZ antiferromagnet SrCo2V2O8. Spinon excitations are observed above TN in quantitative agreement with established theory. Below TN the pairs of spinons are confined and two sequences of meson-like bound states with longitudinal and transverse polarizations are observed. Several theoretical approaches are used to explain the data. A new theoretical technique based on Tangent-space Matrix Product States gives a very complete description of the data and provides good agreement not only with the energies of the bound modes but also with their intensities. We also successfully explained the effect of temperature on the excitations including the experimentally observed thermally induced resonance between longitudinal modes below TN ,and the transitions between thermally excited spinon states above TN. In summary, our work establishes SrCo2V2O8 as a beautiful paradigm for spinon confinement in a quasi-1D quantum magnet and provides a comprehensive picture of this process.
We report the observation of magnetic domains in the exotic, antiferromagnetically ordered all-in-all-out state of Nd$_2$Zr$_2$O$_7$, induced by spin canting. The all-in-all-out state can be realized by Ising-like spins on a pyrochlore lattice and is established in Nd$_2$Zr$_2$O$_7$ below 0.31 K for external magnetic fields up to 0.14 T. Two different spin arrangements can fulfill this configuration which leads to the possibility of magnetic domains. The all-in-all-out domain structure can be controlled by an external magnetic field applied parallel to the [111] direction. This is a result of different spin canting mechanism for the two all-in-all-out configurations for such a direction of the magnetic field. The change of the domain structure is observed through a hysteresis in the magnetic susceptibility. No hysteresis occurs, however, in case the external magnetic field is applied along [100].
The physical properties of an intermetallic compound CeRh2Ga2 have been investigated by magnetic susceptibility \chi(T), isothermal magnetization M(H), heat capacity C_p(T), electrical resistivity \rho(T), thermal conductivity \kappa(T) and thermopower S(T) measurements. CeRh2Ga2 is found to crystallize with CaBe2Ge2-type primitive tetragonal structure (space group P4/nmm). No evidence of long range magnetic order is seen down to 1.8 K. The \chi(T) data show paramagnetic behavior with an effective moment \mu_eff ~ 2.5 \mu_B/Ce indicating Ce^3+ valence state of Ce ions. The \rho(T) data exhibit Kondo lattice behavior with a metallic ground state. The low-T C_p(T) data yield an enhanced Sommerfeld coefficient \gamma = 130(2) mJ/mol K^2 characterizing CeRh2Ga2 as a moderate heavy fermion system. The high-T C_p(T) and \rho(T) show an anomaly near 255 K, reflecting a phase transition. The \kappa(T) suggests phonon dominated thermal transport with considerably higher values of Lorenz number L(T) compared to the theoretical Sommerfeld value L_0.
V. K. Anand, L. Opherden, J. Xu, D. T. Adroja, A. T. M. N. Islam, T. Herrmannsdörfer, J. Hornung, R. Schönemann, M. Uhlarz, H. C. Walker, N. Casati, B. Lake Physical properties of a pyrohafnate compound Pr2Hf2O7 have been investigated by ac magnetic susceptibility \chi_ ac(T), dc magnetic susceptibility \chi(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements on polycrystalline as well as single crystal samples combined with high-resolution synchrotron x-ray diffraction (XRD) for structural characterization and inelastic neutron scattering (INS) to determine the crystal field energy level scheme and wave functions. Synchrotron XRD data confirm the ordered cubic pyrochlore (Fd-3m) structure without any noticeable site mixing or oxygen deficiency. No clear evidence of long range magnetic ordering is observed down to 90 mK, however the \chi_ac(T) evinces slow spin dynamics revealed by a frequency dependent broad peak associated with spin freezing. The INS data reveal the expected five well defined magnetic excitations due to crystal field splitting of the J = 4 ground state multiplet of the Pr^3+. The crystal field parameters and ground state wavefunction of Pr^3+ have been determined. The Ising anisotropic nature of magnetic ground state is inferred from the INS as well as \chi(T) and M(H) data. Together these properties make Pr2Hf2O7 a candidate compound for quantum spin-ice behavior.
A spin liquid is a new state of matter with topological order where the spin moments continue to fluctuate coherently down to the lowest temperatures rather than develop static long-range magnetic order as found in conventional magnets. For spin liquid behavior to arise in a material the magnetic Hamiltonian must be "frustrated" where the combination of lattice geometry, interactions and anisotropies gives rise to competing spin arrangements in the ground state. Theoretical Hamiltonians which produce spin liquids are spin ice, the Kitaev honeycomb model and the Heisenberg kagome antiferromagnet. Spin liquid behavior however in real materials is rare because they can only approximate these Hamiltonians and often have weak higher order terms that destroy the spin liquid state. Ca10Cr7O28 is a new quantum spin liquid with magnetic Cr5+ ions that possess quantum spin number S=1/2. The spins are entirely dynamic in the ground state and the excitation spectrum is broad and diffuse as is typical of spinons which are the excitations of a spin liquid. In this paper we determine the Hamiltonian of Ca10Cr7O28 using inelastic neutron scattering under high magnetic field to induce a ferromagnetic ground state and spin-wave excitations that can be fitted to extract the interactions. We further explore the phase diagram by using inelastic neutron scattering and heat capacity measurements and establish the boundaries of the spin liquid phase as a function of magnetic field and temperature. Our results show that Ca10Cr7O28 consists of distorted kagome bilayers with several isotropic ferromagnetic and antiferromagnetic interactions where unexpectedly the ferromagnetic interactions are stronger than the antiferromagnetic ones. This complex Hamiltonian does not correspond to any known spin liquid model and points to new directions in the search for quantum spin liquid behavior.
A detailed diffraction study of Ca10Cr7O28 is presented which adds significant new insights into the structural and magnetic properties of this compound. A new crystal structure type was used where the a and b axes are doubled compared to previous models providing a more plausible structure where all crystallographic sites are fully occupied. The presence of two different valences of chromium was verified and the locations of the magnetic Cr5+ and non-magnetic Cr6+ ions were identified. The Cr5+ ions have spin-1/2 and form distorted kagome bilayers which are stacked in an ABC arrangement along the c axis. These results lay the foundation for understanding of the quantum spin liquid behavior in Ca10Cr7O28 which has recently been reported in [C. Balz et al., Nature Physics, 12, 942 (2016)].
We present a muon spin relaxation study on the Ising pyrochlore Nd$_2$Zr$_2$O$_7$ which develops an "all-in-all-out" magnetic order below 0.4~K. At 20~mK far below the ordering transition temperature, the zero-field muon spin relaxation spectra show no static features and can be well described by a dynamical Gaussian-broadened Gaussian Kubo-Toyabe function indicating strong fluctuations of the ordered state. The spectra of the paramagnetic state (below 4.2~K) reveal anomalously slow paramagnetic spin dynamics and show only small difference with the spectra of the ordered state. We find that the fluctuation rate decreases with decreasing temperature and becomes nearly temperature independent below the transition temperature indicating persistent slow spin dynamics in the ground state. The field distribution width shows a small but sudden increase at the transition temperature and then becomes almost constant. The spectra in applied longitudinal fields are well fitted by the conventional dynamical Gaussian Kubo-Toyabe function, which further supports the dynamical nature of the ground state. The fluctuation rate shows a peak as a function of external field which is associated with a field-induced spin-flip transition. The strong dynamics in the ordered state are attributed to the transverse coupling of the Ising spins introduced by the multipole interactions.
Christian Balz, Bella Lake, Johannes Reuther, Hubertus Luetkens, Rico Schönemann, Thomas Herrmannsdörfer, Yogesh Singh, A.T.M. Nazmul Islam, Elisa M. Wheeler, Jose A. Rodriguez-Rivera, Tatiana Guidi, Giovanna G. Simeoni, Chris Baines, Hanjo Ryll 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.
Unlike most quantum systems which rapidly become incoherent as temperature is raised, strong correlations persist at elevated temperatures in $S=1/2$ dimer magnets, as revealed by the unusual asymmetric lineshape of their excitations at finite temperatures. Here we quantitatively explore and parameterize the strongly correlated magnetic excitations at finite temperatures using the high resolution inelastic neutron scattering on the model compound BaCu$_2$V$_2$O$_8$ which we show to be an alternating antiferromagnetic-ferromagnetic spin$-1/2$ chain. Comparison to state of the art computational techniques shows excellent agreement over a wide temperature range. Our findings hence demonstrate the possibility to quantitatively predict coherent behavior at elevated temperatures in quantum magnets.
Zhe Wang, Jianda Wu, Shenglong Xu, Wang Yang, Congjun Wu, Anup Kumar Bera, A. T. M. Nazmul Islam, Bella Lake, Dmytro Kamenskyi, Papori Gogoi, Hans Engelkamp, Nanlin Wang, Joachim Deisenhofer, Alois Loidl 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 Néel temperature of 5 K and described by a one-dimensional Schrödinger 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.
We present synchrotron x-ray diffraction, neutron powder diffraction and time-of-flight inelastic neutron scattering measurements on the rare earth pyrochlore oxide Nd2Zr2O7 to study the ordered state magnetic structure and cystal field states. The structural characterization by high-resolution synchrotron x-ray diffraction confirms that the pyrochlore structure has no detectable O vacancies or Nd/Zr site mixing. The neutron diffraction reveals long range all-in/all-out antiferromagnetic order below T_N ~ 0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) \mu_B/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65 \mu_B/Nd for the local <111> Ising ground state of Nd3+ (J=9/2) suggesting that the ordering is partially suppressed by quantum fluctuations. The strong Ising anisotropy is further confirmed by the inelastic neutron scattering data which reveals a well-isolated dipolar-octupolar type Kramers doublet ground state. The crystal field level scheme and ground state wavefunction have been determined.
We have investigated the physical properties of a pyrochlore hafnate Nd2Hf2O7 using ac magnetic susceptibility \chi_ac(T), dc magnetic susceptibility \chi(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements, and determined the magnetic ground state by neutron powder diffraction study. An upturn is observed below 6 K in C_p(T)/T, however both C_p(T) and \chi(T) do not show any clear anomaly down to 2 K. The \chi_ac(T) shows a well pronounced anomaly indicating an antiferromagnetic transition at T_N = 0.55 K. The long range antiferromagnetic ordering is confirmed by neutron diffraction. The refinement of neutron diffraction pattern reveals an all-in/all-out antiferromagnetic structure, where for successive tetrahedra, the four Nd3+ magnetic moments point alternatively all-into or all-out-of the tetrahedron, with an ordering wavevector k = (0, 0, 0) and an ordered state magnetic moment of m = 0.62(1) \mu_B/Nd at 0.1 K. The ordered moment is strongly reduced reflecting strong quantum fluctuations in ordered state.
Physical properties of partially Ca substituted hole-doped Dy2Ti2O7 have been investigated by ac magnetic susceptibility \chi_ac(T), dc magnetic susceptibility \chi(T), isothermal magnetization M(H) and heat capacity C_p(T) measurements on Dy1.8Ca0.2Ti2O7. The spin-ice system Dy2Ti2O7 exhibits a spin-glass type freezing behavior near 16 K. Our frequency dependent \chi_ac(T) data of Dy1.8Ca0.2Ti2O7 show that the spin-freezing behavior is significantly influenced by Ca substitution. The effect of partial nonmagnetic Ca2+ substitution for magnetic Dy3+ is similar to the previous study on nonmagnetic isovalent Y3+ substituted Dy2-xYxTi2O7 (for low levels of dilution), however the suppression of spin-freezing behavior is substantially stronger for Ca than Y. The Cole-Cole plot analysis reveals semicircular character and a single relaxation mode in Dy1.8Ca0.2Ti2O7 as for Dy2Ti2O7. No noticeable change in the insulating behavior of Dy2Ti2O7 results from the holes produced by 10% Ca2+ substitution for Dy3+ ions.
Effects of interchain couplings and anisotropy on a Haldane chain have been investigated by single crystal inelastic neutron scattering and density functional theory (DFT) calculations on the model compound SrNi$_2$V$_2$O$_8$. Significant effects on low energy excitation spectra are found where the Haldane gap ($\Delta_0 \approx 0.41J$; where $J$ is the intrachain exchange interaction) is replaced by three energy minima at different antiferromagnetic zone centers due to the complex interchain couplings. Further, the triplet states are split into two branches by single-ion anisotropy. Quantitative information on the intrachain and interchain interactions as well as on the single-ion anisotropy are obtained from the analyses of the neutron scattering spectra by the random phase approximation (RPA) method. The presence of multiple competing interchain interactions is found from the analysis of the experimental spectra and is also confirmed by the DFT calculations. The interchain interactions are two orders of magnitude weaker than the nearest-neighbour intrachain interaction $J$ = 8.7~meV. The DFT calculations reveal that the dominant intrachain nearest-neighbor interaction occurs via nontrivial extended superexchange pathways Ni--O--V--O--Ni involving the empty $d$ orbital of V ions. The present single crystal study also allows us to correctly position SrNi$_2$V$_2$O$_8$ in the theoretical $D$-$J_{\perp}$ phase diagram [T. Sakai and M. Takahashi, Phys. Rev. B 42, 4537 (1990)] showing where it lies within the spin-liquid phase.
For quasi-one dimensional quantum spin systems theory predicts the occurrence of a confinement of spinon excitation due to interchain couplings. Here we investigate the system SrCo2V2O8, a realization of the weakly-coupled Ising-like XXZ antiferromagnetic chains, by terahertz spectroscopy with and without applied magnetic field. At low temperatures a series of excitations is observed, which split in a Zeeman-like fashion in an applied magnetic field. These magnetic excitations are identified as the theoretically predicted spinon-pair excitations. Using a one dimensional Schrödinger equation with a linear confinement potential imposed by weak interchain couplings, the hierarchy of the confined spinons can be fully described.
Magnetic correlations of two iso-structural quasi-one-dimensional (1D) antiferromagnetic spin-chain compounds Sr$M_2$V$_2$O$_8$ ($M$ = Co, Mn) have been investigated by magnetization and powder neutron diffraction. Two different collinear antiferromagnetic (AFM) structures, characterized by the propagation vectors, $k$ = (0 0 1) and $k$ = (0 0 0), have been found below $\sim$ 5.2 K and $\sim$ 42.2 K for the Co- and Mn-compounds, respectively. For the Mn-compound, AFM chains (along the $c$ axis) order ferromagnetically within the $ab$ plane, whereas, for the Co-compound, AFM chains order ferro-/antiferromagnetically along the $a/b$ direction. The critical exponent study confirms that the Co- and Mn-compounds belong to the Ising and Heisenberg universality classes, respectively. For both compounds, short-range spin-spin correlations are present over a wide temperature range above $T_N$. The reduced ordered moments at base temperature (1.5 K) indicate the presence of quantum fluctuations in both compounds due to the quasi-1D magnetic interactions.
C. Balz, B. Lake, H. Luetkens, C. Baines, T. Guidi, M. Abdel-Hafiez, A.U.B. Wolter, B. Büchner, I.V. Morozov, E.B. Deeva, O.S. Volkova, A.N. Vasiliev It is well established that long-range magnetic order is suppressed in magnetic systems whose interactions are low-dimensional. The prototypical example is the S-1/2 Heisenberg antiferromagnetic chain (S-1/2 HAFC) whose ground state is quantum critical. In real S-1/2 HAFC compounds interchain coupling induces long-range magnetic order although with a suppressed ordered moment and reduced Néel temperature compared to the Curie-Weiss temperature. Recently, it was suggested that order can also be suppressed if the interchain interactions are frustrated, as for the Nersesyan-Tsvelik model. Here, we study the new S-1/2 HAFC, (NO)[Cu(NO3)3]. This material shows extreme suppression of order which furthermore is incommensurate revealing the presence of frustration consistent with the Nersesyan-Tsvelik model.
Ultrasound velocity measurements of the orbital-degenerate frustrated spinel MgV$_2$O$_4$ are performed in the high-purity single crystal which exhibits successive structural and antiferromagnetic phase transitions, and in the disorder-introduced single crystal which exhibits spin-glass-like behavior. The measurements reveal that two-types of unusual temperature dependence of the elastic moduli coexist in the cubic paramagnetic phase, which are resolved by magnetic-field and disorder sensitivities: huge Curie-type softening with decreasing temperature, and concave temperature dependence with a characteristic minimum. These elastic anomalies suggest the coupling of lattice to coexisting orbital fluctuations and orbital-spin-coupled excitations.
Linear spin wave theory provides the leading term in the calculation of the excitation spectra of long-range ordered magnetic systems as a function of $1/\sqrt{S}$. This term is acquired using the Holstein-Primakoff approximation of the spin operator and valid for small $\delta S$ fluctuations of the ordered moment. We propose an algorithm that allows magnetic ground states with general moment directions and single-Q incommensurate ordering wave vector using a local coordinate transformation for every spin and a rotating coordinate transformation for the incommensurability. Finally we show, how our model can determine the spin wave spectrum of the magnetic C-site langasites with incommensurate order.
Zhe Wang, D. Kamenskyi, O. Cépas, M. Schmidt, D. L. Quintero-Castro, A. T. M. N. Islam, B. Lake, A. A. Aczel, H. A. Dabkowska, A. B. Dabkowski, G. M. Luke, Yuan Wan, A. Loidl, M. Ozerov, J. Wosnitza, S. A. Zvyagin, J. Deisenhofer Magnetic excitations in the isostructural spin-dimer systems Sr3Cr2O8 and Ba3Cr2O8 are probed by means of high-field electron spin resonance at sub-terahertz frequencies. Three types of magnetic modes were observed. One mode is gapless and corresponds to transitions within excited states, while two other sets of modes are gapped and correspond to transitions from the ground to the first excited states. The selection rules of the gapped modes are analyzed in terms of a dynamical Dzyaloshinskii-Moriya interaction, suggesting the presence of phonon-assisted effects in the low-temperature spin dynamics of Sr3Cr2O8 and Ba3Cr2O8
Field-induced magnetic ordering in the Haldane chain compound SrNi$_{2}$V$_{2}$O$_{8}$ and effect of anisotropy have been investigated using single crystals. Static susceptibility, inelastic neutron scattering, high-field magnetization, and low temperature heat-capacity studies confirm a non-magnetic spin-singlet ground state and a gap between the singlet ground state and triplet excited states. The intra-chain exchange interaction is estimated to be $J \sim 8.9{\pm}$0.1 meV. Splitting of the dispersions into two modes with minimum energies 1.57 and 2.58 meV confirms the existence of single-ion anisotropy $D(S^z){^2}$. The value of \it D is estimated to be $-0.51{\pm}0.01$ meV and the easy axis is found to be along the crystallographic \it c-axis. Field-induced magnetic ordering has been found with two critical fields [$\mu_0H_c^{\perp c} = 12.0{\pm}$0.2 T and $\mu_0H_c^{\parallel c} = 20.8{\pm}$0.5 T at 4.2 K]. Field-induced three-dimensional magnetic ordering above the critical fields is evident from the heat-capacity, susceptibility, and high-field magnetization study. The Phase diagram in the \it H-T plane has been obtained from the high-field magnetization. The observed results are discussed in the light of theoretical predictions as well as earlier experimental reports on Haldane chain compounds.
The space- and time-dependent response of many-body quantum systems is the most informative aspect of their emergent behaviour. The dynamical structure factor, experimentally measurable using neutron scattering, can map this response in wavevector and energy with great detail, allowing theories to be quantitatively tested to high accuracy. Here, we present a comparison between neutron scattering measurements on the one-dimensional spin-1/2 Heisenberg antiferromagnet KCuF3, and recent state-of-the-art theoretical methods based on integrability and density matrix renormalization group simulations. The unprecedented quantitative agreement shows that precise descriptions of strongly correlated states at all distance, time and temperature scales are now possible, and highlights the need to apply these novel techniques to other problems in low-dimensional magnetism.
Multi-frequency electron spin resonance (ESR) transmission spectra have been measured as function of temperature and magnetic field on single crystals of the quasi-one-dimensional spin-1 chain compound SrNi2V2O8 in the GHz frequency range. Magnetic resonance modes above 50 K have been observed with an effective g-factor of 2.24 at 100 K. Below 30 K, intra-triplet excitations have been observed in the ESR spectra, which reveal the presence of single-ion anisotropy with D = -0.29 meV.
We report on optical transmission spectroscopy of the Cr-based frustrated triangular antiferromagnets CuCrO2 and alpha-CaCr2O4, and the spinels CdCr2O4 and ZnCr2O4 in the near-infrared to visible-light frequency range. We explore the possibility to search for spin correlations far above the magnetic ordering temperature and for anomalies in the magnon lifetime in the magnetically ordered state by probing exciton-magnon sidebands of the spin-forbidden crystal-field transitions of the Cr3+ ions (spin S = 3/2). In CuCrO2 and alpha-CaCr2O4 the appearance of fine structures below T_N is assigned to magnon sidebands by comparison with neutron scattering results. The temperature dependence of the line width of the most intense sidebands in both compounds can be described by an Arrhenius law. For CuCrO2 the sideband associated with the 4A2 -> 2T2 transition can be observed even above T_N. Its line width does not show a kink at the magnetic ordering temperature and can alternatively be described by a Z2 vortex scenario proposed previously for similar materials. The exciton-magnon features in alpha-CaCr2O4 are more complex due to the orthorhombic distortion. While for CdCr2O4 magnon sidebands are identified below T_N and one sideband excitation is found to persist across the magnetic ordering transition, only a weak fine structure related to magnetic ordering has been observed in ZnCr2O4.
It is widely believed that magnetic excitations become increasingly incoherent as temperature is raised due to random collisions which limit their lifetime. This picture is based on spin-wave calculations for gapless magnets in 2 and 3 dimensions and is observed experimentally as a symmetric Lorentzian broadening in energy. Here, we investigate a three-dimensional dimer antiferromagnet and find unexpectedly that the broadening is asymmetric - indicating that far from thermal decoherence, the excitations behave collectively like a strongly correlated gas. This result suggests that a temperature activated coherent state of quasi-particles is not confined to special cases like the highly dimerized spin-1/2 chain but is found generally in dimerized antiferromagnets of all dimensionalities and perhaps gapped magnets in general.
In this paper we explore the phase diagram and excitations of a distorted triangular lattice antiferromagnet. The unique two-dimensional distortion considered here is very di?erent from the 'isosceles'-type distortion that has been extensively investigated. We show that it is able to stabilize a 120\deg spin structure for a large range of exchange interaction values, while new structures are found for extreme distortions. A physical realization of this model is \alpha-CaCr2O4 which has 120\deg structure but lies very close to the phase boundary. This is veri?ed by inelastic neutron scattering which reveals unusual roton-like minima at reciprocal space points di?erent from those corresponding to the magnetic order.
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.
S. E. Dissanayake, C. Chan, S. Ji, J. Lee, Y. Qiu, K. C. Rule, B. Lake, M. Green, M. Hagihala, X. G. Zheng, T. K. Ng, S.-H. Lee Using elastic and inelastic neutron scattering techniques with and without application of an external magnetic field $H$, the magnetic ground states of Zn$_x$Co$_{4-x}$(OD)$_6$Cl$_2$ ($x=0,1$) were studied. Our results show that for $x=0$, the ground state is a magnetic long-range ordered (LRO) state where each tetrahedron forms an "umbrella"-type structure. On the other hand, for $x=1$, no static ordering was observed down to 1.5 K, which resembles the behavior found in the isostructural quantum system Zn$_x$Cu$_{4-x}$(OD)$_6$Cl$_2$. When $H$ field is applied, however the $x=1$ system develops the same LRO state as $x=0$. This indicates that the $x=1$ disordered state is in the vicinity of the $x=0$ ordered state.
BaMn2As2 is unique among BaT2As2 compounds crystallizing in the body-centered-tetragonal ThCr2Si2 structure, which contain stacked square lattices of 3d transition metal T atoms, since it has an insulating large-moment (3.9 muB/Mn) G-type (checkerboard) antiferromagnetic AF ground state. We report measurements of the anisotropic magnetic susceptibility chi versus temperature T from 300 to 1000 K of single crystals of BaMn2As2, and magnetic inelastic neutron scattering measurements at 8 K and 75As NMR measurements from 4 to 300 K of polycrystalline samples. The Neel temperature determined from the chi(T) measurements is TN = 618(3) K. The measurements are analyzed using the J1-J2-Jc Heisenberg model. Linear spin wave theory for G-type AF ordering and classical and quantum Monte Carlo simulations and molecular field theory calculations of chi(T) and of the magnetic heat capacity Cmag(T) are presented versus J1, J2 and Jc. We also obtain band theoretical estimates of the exchange couplings in BaMn2As2. From analyses of our chi(T), NMR, neutron scattering, and previously published heat capacity data for BaMn2As2 on the basis of the above theories for the J1-J2-Jc Heisenberg model and our band-theoretical results, our best estimates of the exchange constants in BaMn2As2 are J1 = 13 meV, J2/J1 = 0.3 and Jc/J1 = 0.1, which are all antiferromagnetic. From our classical Monte Carlo simulations of the G-type AF ordering transition, these exchange parameters predict TN = 640 K for spin S = 5/2, in close agreement with experiment. Using spin wave theory, we also utilize these exchange constants to estimate the suppression of the ordered moment due to quantum fluctuations for comparison with the observed value and again obtain S = 5/2 for the Mn spin.