arXiv subjects

T. Fennell

Publications and source records attributed to T. Fennell.

At least 19 recordsLinked to original sources

arXiv2025

Magnetoelastic dynamics of the "spin Jahn-Teller" transition in CoTi$_{2}$O$_{5}$

CoTi$_{2}$O$_{5}$ has the paradox that low temperature static magnetic order is incompatible with the crystal structure owing to a mirror plane that exactly frustrates magnetic interactions. Despite no observable structural distortion with diffraction, CoTi$_{2}$O$_{5}$ does magnetically order below $T_{\rm N}$ $\sim$ 25 K with the breaking of spin ground state degeneracy proposed to be a realization of the spin Jahn-Teller effect in analogy to the celebrated orbital Jahn-Teller transition. We apply neutron and Raman spectroscopy to study the dynamics of this transition in CoTi$_{2}$O$_{5}$. We find anomalous acoustics associated with a symmetry breaking strain that characterizes the spin Jahn-Teller transition. Crucially, the energy of this phonon coincides with the energy scale of the magnetic excitations, and has the same symmetry of an optic mode, observed with Raman spectroscopy, which atypically softens in energy with decreasing temperature. Taken together, we propose that the energetics of the spin Jahn-Teller effect in CoTi$_{2}$O$_{5}$ are related to cooperative magnetoelastic fluctuations as opposed to conventional soft critical dynamics which typically drive large measurable static displacements.

cond-mat.str-el↗

arXiv2024

Excitation Spectrum and Spin Hamiltonian of the Frustrated Quantum Ising Magnet Pr$_3$BWO$_9$

We present a thorough experimental investigation on single crystals of the rare-earth based frustrated quantum antiferromagnet Pr$_3$BWO$_9$, a purported spin-liquid candidate on the breathing kagome lattice. This material possesses a disordered ground state with an unusual excitation spectrum involving a coexistence of sharp spin-waves and broad continuum excitations. Nevertheless, we show through a combination of thermodynamic, magnetometric and spectroscopic probes with detailed theoretical modeling that it should be understood in a completely different framework. The crystal field splits the lowest quasi-doublet states into two singlets moderately coupled through frustrated superexchange, resulting in a simple effective Hamiltonian of an Ising model in a transverse magnetic field. While our neutron spectroscopy data do point to significant correlations within the kagome planes, the dominant interactions are out-of-plane, forming frustrated triangular spin-tubes through two competing ferro-antiferromagnetic bonds. The resulting ground state is a simple quantum paramagnet, but with significant modifications to both thermodynamic and dynamic properties due to small perturbations to the transverse field Ising model in the form of hyperfine enhanced nuclear moments and weak structural disorder.

cond-mat.str-el↗

arXiv2023

Fluctuation-induced spin nematic order in magnetic charge-ice

Disorder in materials may be used to tune their functionalities, but much more strikingly, its presence can entail entirely new behavior. This happens in charge-ice where structural disorder is not weak and local, but strong and long-range correlated. Here, two cations of different charge occupy a pyrochlore lattice, arranging themselves such that all tetrahedra host two cations of each type. The ensuing correlated disorder is characterized by randomly packed loops of a single cation-type. If the cations are magnetic and interact antiferromagnetically, a new type of magnet with strong interactions along the loops, but frustrated interactions between loops, emerges. This results in an ensemble of intertwined Heisenberg spin chains that form an algebraic spin liquid at intermediate temperatures. At lower temperatures, we find these non-local degrees of freedom undergo a discontinuous transition to a spin nematic. While this phase does not break time reversal symmetry, its spin symmetry is reduced resulting in a dramatically slower spin relaxation. The transition is sensitive to the statistics of the cation loops, providing both a direct thermodynamic signature of otherwise elusive structural information and a structural route to engineering nematic phase stability.

cond-mat.stat-mech↗

arXiv2023

Formation of a simple cubic antiferromagnet through charge ordering in a double Dirac material

The appearance of spontaneous charge order in chemical systems is often associated with the emergence of novel, and useful, properties. Here we show through single crystal diffraction that the Eu ions in the mixed valent metal EuPd$_3$S$_4$ undergo long-range charge ordering at $T_{\mathrm{CO}} = 340 \mathrm{~K}$ resulting in simple cubic lattices of Eu$^{2+}$ ($J = 7/2$) and Eu$^{3+}$ ($J = 0$) ions. As only one of the two sublattices has a non-magnetic ground state, the charge order results in the emergence of remarkably simple G-type antiferromagnetic order at $T_{\mathrm{N}} = 2.85(6) \mathrm{~K}$, observed in magnetization, specific heat, and neutron diffraction. Application of a $0.3 \mathrm{~T}$ field is sufficient to induce a spin flop transition to a magnetically polarized, but still charge ordered, state. Density functional theory calculations show that this charge order also modifies the electronic degeneracies present in the material: without charge order, EuPd$_3$S$_4$ is an example of a double Dirac material containing 8-fold degenerate electronic states, greater than the maximum degeneracy of six possible in molecular systems. The symmetry reduction from charge order transmutes 8-fold double Dirac states into 4-fold Dirac states, a degeneracy that can be preserved even in the presence of the magnetic order. Our results show not only how charge order can be used to produce interesting magnetic lattices, but also how it can be used to engineer controlled degeneracies in electronic states.

cond-mat.str-el↗

arXiv2023

Magnetic phase diagram of the breathing-kagome antiferromagnet Nd$_3$BWO$_9$

The highly-frustrated rare-earth based magnet Nd$_3$BWO$_9$ is a promising candidate in the search for proximate spin liquid physics. We present a thorough investigation on single crystals of this material using bulk and microscopic techniques. Magnetization data reveal a fractional magnetization plateau for three different investigated field directions. The magnetic phase diagram is mapped out from calorimetric data and exhibits several domes of magnetic order below 0.3 K. Propagation vectors for all ordered phases are presented. The results suggest complex ordering in this material, and unveil the existence of a commensuration transition of the propagation vector at zero magnetic field. A scenario where interplane exchange interactions are essential to a magnetic model of Nd$_3$BWO$_9$ is discussed.

cond-mat.str-el↗

arXiv2022

Fast broadband cluster spin-glass dynamics in PbFe$_{1/2}$Nb$_{1/2}$O$_{3}$

PbFe$_{1/2}$Nb$_{1/2}$O$_{3}$ (PFN) is a relaxor ferroelectric (T$_{c}$ $\sim$ 400 K) consisting of disordered magnetic Fe$^{3+}$ (S=${5\over2}$, L$\approx$0) ions resulting in a low temperature ``cluster glass" phase (W. Kleemann $\textit{et al.}$ Phys. Rev. Lett. ${\bf{105}}$, 257202 (2010)). We apply neutron scattering to investigate the dynamic magnetism of this phase in a large single crystal which displays a low temperature spin glass transition (T$_{g} \sim$ 15 K), but no observable spatially long-range antiferromagnetic order. The static response in the cluster glass phase (sampled on the timescale set by our resolution) is found to be characterized by an average magnetic spin direction that lacks any preferred direction. The dynamics that drive this phase are defined by a magnetic correlation length that gradually increases with decreasing temperature. However, below $\sim$ 50 K the spatial correlations gradually becoming more short range indicative of increasing disorder on cooling, thereby unravelling magnetism, until the low temperature glass phase sets in at T$_{g}$ $\sim$ 15 K. Neutron spectroscopy is used to characterize the spin fluctuations in the cluster glass phase and are found to be defined by a broadband of frequencies on the scale of $\sim$ THz, termed here ``fast" fluctuations. The frequency bandwidth driving the magnetic fluctuations mimics the correlation length and decreases until $\sim$ 50 K, and then increases again until the glass transition. Through investigating the low-energy acoustic phonons we find evidence of multiple distinct structural regions which form the basis of the clusters, generating a significant amount of local disorder. We suggest that random molecular fields originating from conflicting interactions between clusters is important for the destruction of magnetic order and the eventual formation of the cluster glass in PFN.

cond-mat.mtrl-sci↗

arXiv2022

Thermal Evolution of Dirac Magnons in the Honeycomb Ferromagnet CrBr$_3$

CrBr$_3$ is an excellent realization of the two-dimensional honeycomb ferromagnet, which offers a bosonic equivalent of graphene with Dirac magnons and topological character. We perform inelastic neutron scattering (INS) measurements using state-of-the-art instrumentation to update 50-year-old data, thereby enabling a definitive comparison both with recent experimental claims of a significant gap at the Dirac point and with theoretical predictions for thermal magnon renormalization. We demonstrate that CrBr$_3$ has next-neighbor $J_2$ and $J_3$ interactions approximately 5\% of $J_1$, an ideal Dirac magnon dispersion at the K point, and the associated signature of isospin winding. The magnon lifetime and the thermal band renormalization show the universal $T^2$ evolution expected from an interacting spin-wave treatment, but the measured dispersion lacks the predicted van Hove features, highlighting the need for a deeper theoretical analysis.

cond-mat.str-el↗

arXiv2021

Tunable critical correlations in kagome ice

We present a comprehensive experimental and theoretical study of the kagome ice Coulomb phase, that explores the fine tuning of critical correlations by applied field, temperature and crystal orientation. The continuous modification of algebraic correlations is observed by polarised neutron scattering experiments and is found to be well described by numerical simulations of an idealised model. We further clarify the thermodynamics of field tuned Kasteleyn transitions and demonstrate some dramatic finite size scaling properties that depend on how topological string defects wind around the system boundaries. We conclude that kagome ice is a remarkable example of a critical and topological state in a real system that may be subject to fine experimental control.

cond-mat.stat-mech↗

arXiv2019

Magnetic order and single-ion anisotropy in Tb$_3$Ga$_5$O$_{12}$

Terbium gallium garnet (TGG), Tb$_3$Ga$_5$O$_{12}$, is well known for its applications in laser optics, but also exhibits complex low-temperature magnetism that is not yet fully understood. Its low-temperature magnetic order is determined by means of time-of-flight neutron powder diffraction. It is found to be a multiaxial antiferromagnet with magnetic Tb$^{3+}$ ions forming six sublattices of magnetic moments aligned parallel and anti-parallel to the $\langle100\rangle$ crystallographic directions of the cubic unit cell. The structure displays strong easy-axis anisotropy with respect to a two-fold axis of symmetry in the local orthorhombic environment of the Tb$^{3+}$ sites. The crystal-field splitting within the single-ion ground-state manifold is investigated by inelastic neutron scattering on powder samples. A strong temperature dependence of the quasidoublet ground-state is observed and revised parameters of the crystal-field Hamiltonian are given. The results of bulk magnetic susceptibility and magnetisation measurements are in good agreement with values based on the crystal-field model down to 20~K, where the onset of magnetic correlations is observed.

cond-mat.str-el↗

arXiv2019

Multi-phase competition in quantum $XY$ pyrochlore antiferromagnet CdYb$_{2}$Se$_{4}$: zero and applied magnetic field study

We study magnetic behaviour of the Yb$^{3+}$ ions on a frustrated pyrochlore lattice in the spinel {\CYS}. The crystal-electric field parameters deduced from high-energy inelastic neutron scattering reveal well-isolated ytterbium ground state doublet with a weakly Ising character. Magnetic order studied by powder neutron diffraction evolves from the $XY$-type antiferromagnetic $Γ_5$ state to a splayed ice-like ferromagnet (both with k=0) in applied magnetic field with $B_c$=3 T. Low-energy inelastic neutron scattering identifies weakly dispersive magnetic bands around 0.72 meV starting at $\mid\bf{Q}\mid$ = 1.1 Å$^{-1}$~ at zero field, which diminish with field and vanish above 3 T. We explain the observed magnetic behaviour in framework of the nearest-neighbour anisotropic exchange model for effective $S=1/2$ Kramers doublets on the pyrochlore lattice. The estimated exchanges position the {\CYS} spinel close to the phase boundary between the $Γ_5$ and splayed ferromagnet states, similar to the Yb-pyrochlores suggesting an important role of the competition between these phases.

cond-mat.str-el↗

arXiv2018

Special temperatures in frustrated ferromagnets

The description and detection of unconventional magnetic states such as spin liquids is a recurring topic in condensed matter physics. While much of the efforts have traditionally been directed at geometrically frustrated antiferromagnets, recent studies reveal that systems featuring competing antiferromagnetic and ferromagnetic interactions are also promising candidate materials. We find that this competition leads to the notion of special temperatures, analogous to those of gases, at which the competing interactions balance, and the system is quasi-ideal. Although induced by weak perturbing interactions, these special temperatures are surprisingly high and constitute an accessible experimental diagnostic of eventual order or spin liquid properties. The well characterised Hamiltonian and extended low-temperature susceptibility measurement of the canonical frustrated ferromagnet Dy$_2$Ti$_2$O$_7$ enables us to formulate both a phenomenological and microscopic theory of special temperatures for magnets. Other members of this new class of magnets include kapellasite Cu$_3$Zn(OH)$_6$Cl$_2$ and the spinel GeCo$_2$O$_4$.

cond-mat.str-el↗

arXiv2018

Pauling entropy, metastability and equilibrium in Dy$_2$Ti$_2$O$_7$ spin ice

Determining the fate of the Pauling entropy in the classical spin ice material Dy$_2$Ti$_2$O$_7$ with respect to the third law of thermodynamics has become an important test case for understanding the existence and stability of ice-rule states in general. The standard model of spin ice - the dipolar spin ice model - predicts an ordering transition at $T\approx 0.15$ K, but recent experiments by Pomaranski $et\ al.$ suggest an entropy recovery over long time scales at temperatures as high as $0.5$ K, much too high to be compatible with theory. Using neutron scattering and specific heat measurements at low temperatures and with long time scales ($0.35$ K$/10^6$ s and $0.5$ K$/10^5$ s respectively) on several isotopically enriched samples we find no evidence of a reduction of ice-rule correlations or spin entropy. High-resolution simulations of the neutron structure factor show that the spin correlations remain well described by the dipolar spin ice model at all temperatures. Further, by careful consideration of hyperfine contributions, we conclude that the original entropy measurements of Ramirez $et\ al.$ are, after all, essentially correct: the short-time relaxation method used in that study gives a reasonably accurate estimate of the equilibrium spin ice entropy due to a cancellation of contributions.

cond-mat.str-el↗

arXiv2018

Manifolds of magnetic ordered states and excitations in the almost Heisenberg pyrochlore antiferromagnet MgCr2O4

In spinels ACr2O4 (A=Mg, Zn) realisation of the classical pyrochlore Heisenberg antiferromagnet model is complicated by a strong spin-lattice coupling: the extensive degeneracy of the ground state is lifted by a magneto-structural transition at TN=12.5 K. We study the resulting low-temperature low-symmetry crystal structure by synchrotron x-ray diffraction. The consistent features of x-ray low-temperature patterns are explained by the tetragonal model of Ehrenberg et. al (Pow. Diff. 17, 230( 2002)), while other features depend on sample or cooling protocol. Complex partially ordered magnetic state is studied by neutron diffraction and spherical neutron polarimetry. Multiple magnetic domains of configuration arms of the propagation vectors k1=(1/2 1/2 0), k2=(1 0 1/2) appear. The ordered moment reaches 1.94(3) muB/Cr3+ for k1 and 2.08(3) muB/Cr3+ for k2, if equal amount of the k1 and k2 phases is assumed. The magnetic arrangements have the dominant components along the [110] and [1-10] diagonals and a smaller c-component. By inelastic neutron scattering we investigate the spin excitations, which comprise a mixture of dispersive spin waves propagating from the magnetic Bragg peaks and resonance modes centered at equal energy steps of 4.5 meV. We interpret these as acoustic and optical spin wave branches, but show that the neutron scattering cross sections of transitions within a unit of two corner-sharing tetrahedra match the observed intensity distribution of the resonances. The distinctive fingerprint of cluster-like excitations in the optical spin wave branches suggests that propagating excitations are localized by the complex crystal structure and magnetic orders.

cond-mat.str-el↗

arXiv2016

Magnetic excitations and electronic interactions in Sr$_2$CuTeO$_6$: a spin-1/2 square lattice Heisenberg antiferromagnet

Sr$_2$CuTeO$_6$ presents an opportunity for exploring low-dimensional magnetism on a square lattice of $S=1/2$ Cu$^{2+}$ ions. We employ ab initio multi-reference configuration interaction calculations to unravel the Cu$^{2+}$ electronic structure and to evaluate exchange interactions in Sr$_2$CuTeO$_6$. The latter results are validated by inelastic neutron scattering using linear spin-wave theory and series-expansion corrections for quantum effects to extract true coupling parameters. Using this methodology, which is quite general, we demonstrate that Sr$_2$CuTeO$_6$ is an almost realization of a nearest-neighbor Heisenberg antiferromagnet but with relatively weak coupling of 7.18(5) meV.

cond-mat.str-el↗

arXiv2016

Magnetodielectric detection of magnetic quadrupole order in Ba(TiO)Cu$_4$(PO$_4$)$_4$ with Cu$_4$O$_{12}$ square cupolas

In vortex-like spin arrangements, multiple spins can combine into emergent multipole moments. Such multipole moments have broken space-inversion and time-reversal symmetries, and can therefore exhibit linear magnetoelectric (ME) activity. Three types of such multipole moments are known: toroidal, monopole, and quadrupole moments. So far, however, the ME-activity of these multipole moments has only been established experimentally for the toroidal moment. Here, we propose a magnetic square cupola cluster, in which four corner-sharing square-coordinated metal-ligand fragments form a noncoplanar buckled structure, as a promising structural unit that carries an ME-active multipole moment. We substantiate this idea by observing clear magnetodielectric signals associated with an antiferroic ME-active magnetic quadrupole order in the real material Ba(TiO)Cu$_4$(PO$_4$)$_4$. The present result serves as a useful guide for exploring and designing new ME-active materials based on vortex-like spin arrangements.

cond-mat.str-el↗

arXiv2016

Sample independence of magnetoelastic excitations in the rare earth pyrochlore Tb2Ti2O7

Recent experimental results have emphasized two aspects of Tb2Ti2O7 which have not been taken into account in previous attempts to construct theories of Tb2Ti2O7: the role of small levels of structural disorder, which appears to control the formation of a long-range ordered state of as yet unknown nature; and the importance of strong coupling between spin and lattice degrees of freedom, which results in the hybridization of crystal field excitons and transverse acoustic phonons. In this work we examine the juncture of these two phenomena and show that samples with strongly contrasting behavior vis-a-vis the structural disorder (i.e. with and without the transition to the ordered state), develop identical magnetoelastic coupling. We also show that the comparison between single crystal and powder samples is more complicated than previously thought - the correlation between lattice parameter (as a measure of superstoichiometric Tb$^{3+}$) and the existence of a specific heat peak, as observed in powder samples, does not hold for single crystals.

cond-mat.str-el↗

arXiv2016

Instabilities of Spin-Liquid States in a Quantum Kagome Antiferromagnet

The emergent behavior of spin liquids that are born out of geometrical frustration makes them an intriguing state of matter. We show that in the quantum kagome antiferromagnet ZnCu$_3$(OH)$_6$SO$_4$ several different correlated, yet fluctuating states exist. By combining complementary local-probe techniques with neutron scattering, we discover a crossover from a critical regime into a gapless spin-liquid phase with decreasing temperature. An additional unconventional instability of the latter phase leads to a second, distinct spin-liquid state that is stabilized at the lowest temperatures. We advance such complex behavior as a feature common to different frustrated quantum magnets.

cond-mat.str-el↗

arXiv2014

Magnetoelastic excitations in the pyrochlore spin liquid Tb$_2$Ti$_2$O$_7$

At low temperatures, Tb$_2$Ti$_2$O$_7$ enters a spin liquid state, despite expectations of magnetic order and/or a structural distortion. Using neutron scattering, we have discovered that in this spin liquid state an excited crystal field level is coupled to a transverse acoustic phonon, forming a hybrid excitation. Magnetic and phononlike branches with identical dispersion relations can be identified, and the hybridization vanishes in the paramagnetic state. We suggest that Tb$_2$Ti$_2$O$_7$ is aptly named a "magnetoelastic spin liquid" and that the hybridization of the excitations suppresses both magnetic ordering and the structural distortion. The spin liquid phase of Tb$_2$Ti$_2$O$_7$ can now be regarded as a Coulomb phase with propagating bosonic spin excitations.

cond-mat.str-el↗