arXiv subjects

Matthew B. Stone

Publications and source records attributed to Matthew B. Stone.

86 records · Page 5Linked to original sources

arXiv2018

Two-dimensional spin liquid behaviour in the triangular-honeycomb antiferromagnet TbInO$_3$

Spin liquid ground states are predicted to arise within several distinct scenarios in condensed matter physics. The observation of these disordered magnetic states is particularly pervasive amongst a class of materials known as frustrated magnets, in which the competition between various magnetic exchange interactions prevents the system from adopting long-range magnetic order at low temperatures. Spin liquids continue to be of great interest due to their exotic nature and the possibility that they may support fractionalised excitations, such as Majorana fermions. Systems that allow for such phenomena are not only fascinating from a fundamental perspective but may also be practically significant in future technologies based on quantum computation. Here we show that the underlying antiferromagnetic sublattice in TbInO$_3$ undergoes a crystal field induced triangular-to-honeycomb dilution at low temperatures. The absence of a conventional magnetic ordering transition at the lowest measurable temperatures indicates that another critical mechanism must govern in the ground state selection of TbInO$_3$. We propose that anisotropic exchange interactions, mediated through strong spin-orbit coupling on the emergent honeycomb lattice of TbInO$_3$, give rise to a highly frustrated spin liquid.

cond-mat.str-el↗

arXiv2018

Quantum Spin Fragmentation in Kagome Ice Ho3Mg2Sb3O14

A promising route to realize entangled magnetic states combines geometrical frustration with quantum-tunneling effects. Spin-ice materials are canonical examples of frustration, and Ising spins in a transverse magnetic field are the simplest many-body model of quantum tunneling. Here, we show that the tripod kagome lattice material Ho3Mg2Sb3O14 unites an ice-like magnetic degeneracy with quantum-tunneling terms generated by an intrinsic splitting of the Ho3+ ground-state doublet, realizing a frustrated transverse Ising model. Using neutron scattering and thermodynamic experiments, we observe a symmetry-breaking transition at T*~0.32 K to a remarkable quantum state with three peculiarities: a continuous magnetic excitation spectrum down to T~0.12K; a macroscopic degeneracy of ice-like states; and a fragmentation of the spin into periodic and aperiodic components strongly affected by quantum fluctuations. Our results establish that Ho3Mg2Sb3O14 realizes a spin-fragmented state on the kagome lattice, with intrinsic quantum dynamics generated by a homogeneous transverse field.

cond-mat.str-el↗

arXiv2017

Crystal field excitations from $\mathrm{Yb^{3+}}$ ions at defective sites in highly stuffed $\rm Yb_2Ti_2O_7$

The pyrochlore magnet $\rm Yb_2Ti_2O_7$ has been proposed as a quantum spin ice candidate, a spin liquid state expected to display emergent quantum electrodynamics with gauge photons among its elementary excitations. However, $\rm Yb_2Ti_2O_7$'s ground state is known to be very sensitive to its precise stoichiometry. Powder samples, produced by solid state synthesis at relatively low temperatures, tend to be stoichiometric, while single crystals grown from the melt tend to display weak "stuffing" wherein $\mathrm{\sim 2\%}$ of the $\mathrm{Yb^{3+}}$, normally at the $A$ site of the $A_2B_2O_7$ pyrochlore structure, reside as well at the $B$ site. In such samples $\mathrm{Yb^{3+}}$ ions should exist in defective environments at low levels, and be subjected to crystalline electric fields (CEFs) very different from those at the stoichiometric $A$ sites. New neutron scattering measurements of $\mathrm{Yb^{3+}}$ in four compositions of $\rm Yb_{2+x}Ti_{2-x}O_{7-y}$, show the spectroscopic signatures for these defective $\mathrm{Yb^{3+}}$ ions and explicitly demonstrate that the spin anisotropy of the $\mathrm{Yb^{3+}}$ moment changes from XY-like for stoichiometric $\mathrm{Yb^{3+}}$, to Ising-like for "stuffed" $B$ site $\mathrm{Yb^{3+}}$, or for $A$ site $\mathrm{Yb^{3+}}$ in the presence of an oxygen vacancy.

cond-mat.str-el↗

arXiv2017

Spin wave damping arising from phase coexistence below $T_c$ in colossal magnetoresistive La$_{0.7}$Ca$_{0.3}$MnO$_3$

While the spin dynamics of La$_{0.7}$Ca$_{0.3}$MnO$_3$ in the ferromagnetic phase are known to be unconventional, previous measurements have yielded contradictory results regarding the damping of spin wave excitations. Neutron spectroscopy measurements on a sample with a transition temperature of $T_c$=257 K, higher than most single crystals, unambiguously reveal an anomalous increase in spin wave damping for excitations approaching the Brillouin zone boundary along the [$100$] direction that cannot be explained as an artifact due to a noninteracting phonon branch. Spin waves throughout the ($HK0$) plane display a common trend where the spin wave damping is dependent upon the excitation energy, increasing for energies above roughly 15 meV and reaching a full width at half maximum of at least 20 meV. The results are consistent with a model of intrinsic spatial inhomogeneity with phase separated regions approximately 18 Å in size persisting over a large range of temperatures below $T_c$.

cond-mat.str-el↗

arXiv2016

Combining micro- and macroscopic probes to untangle single-ion and spatial exchange anisotropies in a $S = 1$ quantum antiferromagnet

The magnetic ground state of the quasi-one-dimensional spin-1 antiferromagnetic chain is sensitive to the relative sizes of the single-ion anisotropy ($D$) and the intrachain ($J$) and interchain ($J'$) exchange interactions. The ratios $D/J$ and $J'/J$ dictate the material's placement in one or other of three competing phases: a Haldane gapped phase, a quantum paramagnet and an XY-ordered state, with a quantum critical point at their junction. We have identified [Ni(HF)$_2$(pyz)$_2]$SbF$_6$, where pyz = pyrazine, as a candidate in which this behavior can be explored in detail. Combining neutron scattering (elastic and inelastic) in applied magnetic fields of up to 10~tesla and magnetization measurements in fields of up to 60~tesla with numerical modeling of experimental observables, we are able to obtain accurate values of all of the parameters of the Hamiltonian [$D = 13.3(1)$~K, $J = 10.4(3)$~K and $J' = 1.4(2)$~K], despite the polycrystalline nature of the sample. Density-functional theory calculations result in similar couplings ($J = 9.2$~K, $J' = 1.8$~K) and predict that the majority of the total spin population of resides on the Ni(II) ion, while the remaining spin density is delocalized over both ligand types. The general procedures outlined in this paper permit phase boundaries and quantum-critical points to be explored in anisotropic systems for which single crystals are as yet unavailable.

cond-mat.mes-hall↗

arXiv2016

Band Excitations in CePd$_3$: A Comparison of Neutron Scattering and ab initio Theory

Intermediate valence compounds containing rare earth or actinide ions are archetypal systems for the investigation of strong electron correlations. Their effective electron masses of 10 to 50 times the free electron mass result from a hybridization of the highly localized $f$-electrons with the more itinerant $d$-electrons, which is strong enough that their properties are dominated by on-site electron correlations. To a remarkable degree, this can be modeled by the Anderson Impurity Model, even though the $f$-electrons are situated on a periodic lattice. However, in recent years, there has been increasing evidence that the dynamic magnetic susceptibility of intermediate valence compounds is not purely local, but shows variations across the Brillouin zone that have been ascribed to $f$-band coherence. So far, this has been based on simplified qualitative models. In this article, we present a quantitative comparison of inelastic neutron scattering from a single crystal of CePd$_3$, measured in four-dimensional (Q,$ω$)-space, with ab initio calculations, which are in excellent agreement on an absolute scale. Our results establish that the Q-dependence of the scattering is caused by particle-hole excitations within $f$-$d$ hybridized bands that grow in coherence with decreasing temperature.

cond-mat.str-el↗

arXiv2016

Neutron tomography of magnetic Majorana fermions in a proximate quantum spin liquid

Quantum matter provides an effective vacuum out of which arise emergent particles not corresponding to any experimentally detected elementary particle. Topological quantum materials in particular have become a focus of intense research in part because of the remarkable possibility to realize Majorana fermions, with their potential for new, decoherence-free quantum computing architectures. In this paper we undertake a study on high-quality single crystal of $α-RuCl_3$ which has been identified as a material realizing a proximate Kitaev state, a topological quantum state with magnetic Majorana fermions. Four-dimensional tomographic reconstruction of dynamical correlations measured using neutrons is uniquely powerful for probing such magnetic states. We discover unusual signals, including an unprecedented column of scattering over a large energy interval around the Brillouin zone center which is remarkably stable with temperature. This is straightforwardly accounted for in terms of the Majorana excitations present in Kitaev's topological quantum spin liquid. Other, more delicate, features in the scattering can be transparently associated with perturbations to an ideal model. This opens a window on emergent magnetic Majorana fermions in correlated materials.

cond-mat.mtrl-sci↗

arXiv2013

Transport, Thermal, and Magnetic Properties of the Narrow-Gap Semiconductor CrSb2

Resistivity, Hall effect, Seebeck coefficient, thermal conductivity, heat capacity, and magnetic susceptibility data are reported for CrSb2 single crystals. In spite of some unusual features in electrical transport and Hall measurements below 100 K, only one phase transition is found in the temperature range from 2 to 750 K corresponding to long-range antiferromagnetic order below T_N ~ 273 K. Many of the low temperature properties can be explained by the thermal depopulation of carriers from the conduction band into a low mobility band located approximately 16 meV below the conduction band edge, as deduced from the Hall effect data. In analogy with what occurs in Ge, the low mobility band is likely an impurity band. The Seebeck coefficient, S, is large and negative for temperatures from 2 to 300 K ranging from ~ -70\muV/K at 300 K to -4500\muV/K at 18 K. A large maximum in |S| at 18 K is likely due to phonon drag with the abrupt drop in |S| below 18 K due to the thermal depopulation of the high mobility conduction band. The large thermal conductivity between 10 and 20 K (~350 W/m/K) is consistent with this interpretation, as are detailed calculations of the Seebeck coefficient made using the complete calculated electronic structure. These data are compared to data reported for FeSb2, which crystallizes in the same marcasite structure, and FeSi, another unusual narrow-gap semiconductor.

cond-mat.str-el↗

arXiv2012

Paramagnetic Spin Correlations in Colossal Magnetoresistive La0.7Ca0.3MnO3

Neutron spectroscopy measurements reveal dynamic spin correlations throughout the Brillouin zone in the colossal magnetoresistive material La0.7Ca0.3MnO3 at 265 K (approximately 1.03 Tc). The long-wavelength behavior is consistent with spin diffusion, yet an additional and unexpected component of the scattering is also observed in low-energy constant-E measurements, which takes the form of ridges of strong quasielastic scattering running along (H 0 0) and equivalent directions. Well-defined Q-space correlations are observed in constant-E scans at energies up to at least 28 meV, suggesting robust short-range spin correlations in the paramagnetic phase.

cond-mat.str-el↗

arXiv2012

Lattice dynamics reveals a local symmetry breaking in the emergent dipole phase of PbTe

Local symmetry breaking in complex materials is emerging as an important contributor to materials properties but is inherently difficult to study. Here we follow up an earlier structural observation of such a local symmetry broken phase in the technologically important compound PbTe with a study of the lattice dynamics using inelastic neutron scattering (INS). We show that the lattice dynamics are responsive to the local symmetry broken phase, giving key insights in the behavior of PbTe, but also revealing INS as a powerful tool for studying local structure. The new result is the observation of the unexpected appearance on warming of a new zone center phonon branch in PbTe. In a harmonic solid the number of phonon branches is strictly determined by the contents and symmetry of the unit cell. The appearance of the new mode indicates a crossover to a dynamic lower symmetry structure with increasing temperature. No structural transition is seen crystallographically but the appearance of the new mode in inelastic neutron scattering coincides with the observation of local Pb off-centering dipoles observed in the local structure. The observation resembles relaxor ferroelectricity but since there are no inhomogeneous dopants in pure PbTe this anomalous behavior is an intrinsic response of the system. We call such an appearance of dipoles out of a non-dipolar ground-state "emphanisis" meaning the appearance out of nothing. It cannot be explained within the framework of conventional phase transition theories such as soft-mode theory and challenges our basic understanding of the physics of materials.

cond-mat.mtrl-sci↗

arXiv2012

Anharmonic Phonons and Magnons in BiFeO3

The phonon density of states (DOS) and magnetic excitation spectrum of polycrystalline BiFeO$_3$ were measured for temperatures $200 \leq T \leq 750\,$K, using inelastic neutron scattering (INS). Our results indicate that the magnetic spectrum of BiFeO$_3$ closely resembles that of similar Fe perovskites, such as LaFeO$_3$, despite the cycloid modulation in BiFeO$_3$. We do not find any evidence for a spin gap. A strong $T$-dependence of the phonon DOS was found, with a marked broadening of the whole spectrum, providing evidence of strong anharmonicity. This anharmonicity is corroborated by large-amplitude motions of Bi and O ions observed with neutron diffraction. These results highlight the importance of spin-phonon coupling in this material.

cond-mat.mtrl-sci↗

arXiv2011

Spin Waves and magnetic exchange interactions in insulating Rb$_{0.89}$Fe$_{1.58}$Se$_2$

The discovery of alkaline iron selenide $A$Fe$_{1.6+x}$Se$_2$ ($A=$ K, Rb, Cs) superconductors has generated considerable excitement in the condensed matter physics community because superconductivity in these materials may have a different origin from the sign reversed s-wave electron pairing mechanism, a leading candidate proposed for all other Fe-based superconductors. Although $A$Fe$_{1.6+x}$Se$_2$ are isostructural with the metallic antiferromagnetic (AF) iron pnictides such as (Ba,Ca,Sr)Fe$_2$As$_2$, they are insulators near $x=0$ and form a $\sqrt{5}\times\sqrt{5}$ blocked AF structure (Fig. 1a) completely different from the iron pnictides. If magnetism is responsible for superconductivity of all iron-based materials, it is important to determine their common magnetic features. Here we use neutron scattering to map out spin waves in the AF insulating Rb$_{0.89}$Fe$_{1.58}$Se$_2$. We find that although Rb$_{0.89}$Fe$_{1.58}$Se$_2$ has a N$\rm \acute{e}$el temperature ($T_N=475$ K) much higher than that of the iron pnictides ($T_N\leq 220$ K), spin waves for both classes of materials have similar zone boundary energies. A comparison of the fitted effective exchange couplings using a local moment Heisenberg Hamiltonian in Rb$_{0.89}$Fe$_{1.58}$Se$_2$, (Ba,Ca,Sr)Fe$_2$As$_2$, and iron chalcogenide Fe$_{1.05}$Te reveals that their next nearest neighbor (NNN) exchange couplings are similar. Therefore, superconductivity in all Fe-based materials may have a common magnetic origin that is intimately associated with the NNN magnetic exchange interactions, even though they have metallic or insulating ground states, different AF orders and electronic band structures.

cond-mat.supr-con↗

arXiv2011

Unconventional temperature enhanced magnetism in iron telluride

Highly energetic magnetic fluctuations, discovered in high-temperature superconductors (HTSC) by inelastic neutron scattering (INS), are now widely believed to be vital for the superconductivity. In two competing scenarios, they either originate from local atomic spins, or are a property of cooperative spin-density-wave (SDW) behavior of conduction electrons. Both assume clear partition into localized electrons, giving rise to local spins, and itinerant ones, occupying well-defined, rigid conduction bands. Here, by performing an INS study of spin dynamics in iron telluride, a parent material of one of the iron-based HTSC families, we have discovered that this very assumption fails, and that conduction and localized electrons are fundamentally entangled. We find that the real-space structure of magnetic correlations can be explained by a simple local-spin plaquette model. However, the effective spin implicated in such a model, appears to increase with the increasing temperature. Thus, we observe a remarkable redistribution of magnetism between the two groups of electrons, which occurs in the temperature range relevant for the superconductivity. The analysis of magnetic spectral weight shows that the effective spin per Fe at T \approx 10 K, in the antiferromagnetic phase, corresponds to S \approx 1, consistent with the recent analyses that emphasize importance of Hund's intra-atomic exchange. However, it grows to S \approx 3/2 in the disordered phase, a result that profoundly challenges the picture of rigid bands, broadly accepted for HTSC.

cond-mat.str-el↗

arXiv2005

Quasiparticle breakdown in a quantum spin liquid

Much of modern condensed matter physics is understood in terms of elementary excitations, or quasiparticles - fundamental quanta of energy and momentum. Various strongly-interacting atomic systems are successfully treated as a collection of quasiparticles with weak or no interactions. However, there are interesting limitations to this description: the very existence of quasiparticles cannot be taken for granted in some systems. Like unstable elementary particles, quasiparticles cannot survive beyond a threshold where certain decay channels become allowed by conservation laws - their spectrum terminates at this threshold. This regime of quasiparticle failure was first predicted for an exotic state of matter, super-fluid helium-4 at temperatures close to absolute zero - a quantum Bose-liquid where zero-point atomic motion precludes crystallization. Using neutron scattering, here we show that it can also occur in a quantum magnet and, by implication, in other systems with Bose-quasiparticles. We have measured spin excitations in a two dimensional (2D) quantum-magnet, piperazinium hexachlorodicuprate (PHCC) in which spin-1/2 copper ions form a non-magnetic quantum spin liquid (QSL), and find remarkable similarities with excitations measured in superfluid 4He. There is a threshold momentum beyond which the quasiparticle peak merges with the two-quasiparticle continuum. It then acquires a finite energy width and becomes indistinguishable from a leading-edge singularity, so that lowest excited states occupy a wide band of energy. Our findings have important ramifications for understanding phenomena involving excitations with gapped spectra in many condensed matter systems, including high-transition-temperature superconductors.

cond-mat.str-el↗