arXiv subjects

B. Roessli

Publications and source records attributed to B. Roessli.

At least 19 recordsLinked to original sources

arXiv2024

Field-Induced Magnon Decay, Magnon Shadows, and Roton-like Excitations in the Honeycomb Antiferromagnet YbBr$_3$

Although the search for quantum many-body phenomena in magnetic materials has a strong focus on highly frustrated systems, even unfrustrated quantum magnets show a multitude of unconventional phenomena in their spin excitation spectra. YbBr$_3$ is an excellent realization of the $S = 1/2$ antiferromagnetic Heisenberg model on the honeycomb lattice, and we have performed detailed spectroscopic experiments with both unpolarized and polarized neutrons at all applied magnetic fields up to saturation. We observe extensive excitation continua, which cause strong renormalization and the decay of single magnons at higher fields, while coherent features include field-induced ``shadows'' of the single magnons and the spectacular emergence of a roton-like excitation. To guide and interpret our experiments, we performed systematic calculations by the method of cylinder matrix-product states that provide quantitative agreement with the neutron scattering data and a qualitative benchmark for the spectral signatures of strong quantum fluctuations even in the absence of magnetic frustration.

cond-mat.str-el↗

arXiv2024

Magnetic skin effect in Pb(Fe$_{1/2}$Nb$_{1/2}$)O$_3$

Relaxor-ferroelectrics display exceptional dielectric properties resulting from the underlying random dipolar fields induced by strong chemical inhomogeneity. An unusual structural aspect of relaxors is a skin-effect where the near-surface region in single crystals exhibit structures and critical phenomena that differ from the bulk. Relaxors are unique in that this skin effect extends over a macroscopic lengthscale of $\sim$ 100$\mu$m whereas usual surface layers only extend over a few unit cells (or $\sim$ nm). We present a muon spectroscopy study of Pb(Fe$_{1/2}$Nb$_{1/2}$)O$_{3}$ (PFN) which displays ferroelectric order, including many relaxor-like dielectric properties such as a frequency broadened dielectric response, and antiferromagnetism with spatially short-range polar correlations and hence can be termed a multiferroic. In terms of the magnetic behavior determined by the Fe$^{3+}$ ($S=5/2$, $L\approx0$) ions, PFN has been characterized as a unique example of a "cluster spin-glass". We use variable momentum muon spectroscopy to study the depth dependence of the slow magnetic relaxations in a large 1 cm$^{3}$ crystal of PFN. Zero-field positive muon spin relaxation is parameterized using a stretched exponential, indicative of a distribution of relaxation rates of the Fe$^{3+}$ spins. This bandwidth of frequencies changes as a function of muon momentum, indicative of a change in the Fe$^{3+}$ relaxation rates as a function of muon implantation depth in our single crystal. Using negative muon elemental analysis, we find small-to-no measurable change in the Fe$^{3+}$/Nb$^{5+}$ concentration with depth implying that chemical concentration alone cannot account for the change in the relaxational dynamics. PFN displays an analogous magnetic skin effect reported to exist in the structural properties of relaxor-ferroelectrics.

cond-mat.str-el↗

arXiv2023

Spin-orbital correlations from complex orbital order in MgV$_{2}$O$_{4}$

MgV$_{2}$O$_{4}$ is a spinel based on magnetic V$^{3+}$ ions which host both spin ($S=1$) and orbital ($l_{eff}=1$) moments. Owing to the underlying pyrochlore coordination of the magnetic sites, the spins in MgV$_{2}$O$_{4}$ only antiferromagnetically order once the frustrating interactions imposed by the $Fd\overline{3}m$ lattice are broken through an orbitally-driven structural distortion at T$_{S}$ $\simeq$ 60 K. Consequently, a Néel transition occurs at T$_{N}$ $\simeq$ 40 K. Low temperature spatial ordering of the electronic orbitals is fundamental to both the structural and magnetic properties, however considerable discussion on whether it can be described by complex or real orbital ordering is ambiguous. We apply neutron spectroscopy to resolve the nature of the orbital ground state and characterize hysteretic spin-orbital correlations using x-ray and neutron diffraction. Neutron spectroscopy finds multiple excitation bands and we parameterize these in terms of a multi-level (or excitonic) theory based on the orbitally degenerate ground state. Meaningful for the orbital ground state, we report an "optical-like" mode at high energies that we attribute to a crystal-field-like excitation from the spin-orbital $j_{eff}$=2 ground state manifold to an excited $j_{eff}$=1 energy level. We parameterize the magnetic excitations in terms of a Hamiltonian with spin-orbit coupling and local crystalline electric field distortions resulting from deviations from perfect octahedra surrounding the V$^{3+}$ ions. We suggest that this provides compelling evidence for complex orbital order in MgV$_{2}$O$_{4}$. We then apply the consequences of this model to understand hysteretic effects in the magnetic diffuse scattering where we propose that MgV$_{2}$O$_{4}$ displays a high temperature orbital memory of the low temperature spin order.

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

Spin Density Wave versus Fractional Magnetization Plateau in a Triangular Antiferromagnet

We report an excellent realization of the highly non-classical incommensurate spin-density wave (SDW) state in the quantum frustrated antiferromagnetic insulator Cs$_2$CoBr$_4$. In contrast to the well-known Ising spin chain case, here the SDW is stabilized by virtue of competing planar in-chain anisotropies and frustrated interchain exchange. Adjacent to the SDW phase is a broad $m = 1/3$ magnetization plateau that can be seen as a commensurate locking of the SDW state into the up-up-down (UUD) spin structure. This represents the first example of long-sought SDW-UUD transition in triangular-type quantum magnets.

cond-mat.str-el↗

arXiv2022

Dipolar spin-waves and tunable band gap at the Dirac points in the 2D magnet ErBr3

Topological magnon insulators constitute a growing field of research for their potential use as information carriers without heat dissipation. We report an experimental and theoretical study of the magnetic ground-state and excitations in the van der Waals two-dimensional honeycomb magnet ErBr3. We show that the magnetic properties of this compound are entirely governed by the dipolar interactions which generate a continuously degenerate non-collinear ground-state on the honeycomb lattice with spins confined in the plane. We find that the magnon dispersion exhibits Dirac-like cones when the magnetic moments in the ground-state are related by time-reversal and inversion symmetries associated with a Berry phase πas in single-layer graphene. A magnon band gap opens when the dipoles are rotated away from this state, entailing a finite Berry curvature in the vicinity of the K and K' Dirac points. Our results illustrate that the spin-wave dispersion of dipoles on the honeycomb lattice can be reversibly controlled from a magnetic phase with Dirac cones to a topological antiferromagnetic insulator with non-trivial valley Chern number.

cond-mat.str-el↗

arXiv2020

Observation of plaquette fluctuations in the spin-1/2 honeycomb lattice

Quantum spin liquids are materials that feature quantum entangled spin correlations and avoid magnetic long-range order at T = 0 K. Particularly interesting are two-dimensional honeycomb spin lattices where a plethora of exotic quantum spin liquids have been predicted. Here, we experimentally study an effective S=1/2 Heisenberg honeycomb lattice with competing nearest and next-nearest neighbor interactions. We demonstrate that YbBr$_3$ avoids order down to at least T=100 mK and features a dynamic spin-spin correlation function with broad continuum scattering typical of quantum spin liquids near a quantum critical point. The continuum in the spin spectrum is consistent with plaquette type fluctuations predicted by theory. Our study is the experimental demonstration that strong quantum fluctuations can exist on the honeycomb lattice even in the absence of Kitaev-type interactions, and opens a new perspective on quantum spin liquids.

cond-mat.str-el↗

arXiv2020

Broadband critical dynamics in disordered lead-based perovskites

Materials based on the cubic perovskite unit cell continue to provide the basis for technologically important materials with two notable recent examples being lead-based relaxor piezoelectrics and lead-based organic-inorganic halide photovoltaics. These materials carry considerable disorder, arising from site substitution in relaxors and molecular vibrations in the organic-inorganics, yet much of our understanding of these systems derives from the initial classic work of Prof. Roger A. Cowley, who applied both theory and neutron scattering methods while at Chalk River Laboratories to the study of lattice vibrations in SrTiO$_{3}$. Neutron scattering continues to play a vital role in characterizing lattice vibrations in perovskites owing to the simple cross section and the wide range of energy resolutions achievable with current neutron instrumentation. We discuss the dynamics that drive the phase transitions in the relaxors and organic-inorganic lead-halides in terms of neutron scattering and compare them to those in phase transitions associated with a ``central peak" and also a soft mode. We review some of the past experimental work on these materials and present new data from high-resolution time-of-flight backscattering spectroscopy taken on organic-inorganic perovskites. We will show that the structural transitions in disordered lead-based perovskites are driven by a broad frequency band of excitations.

cond-mat.mtrl-sci↗

arXiv2019

Dual nature of magnetism in MnSi

The temperature dependence of the manganese magnetic moment and the spin-lattice relaxation rate measured by the muon spin relaxation technique in the magnetically ordered phase of the chiral intermetallic cubic MnSi system are both explained in terms of helimagnon excitations of a localized spin model. The two free parameters characterizing the helimagnon dispersion relation are determined. A combined analysis of the two data sets cannot be achieved using the self-consistent renormalization theory of spin fluctuations which assumes the magnetism of MnSi to arise uniquely from electronic bands. As a result of this work, MnSi is proposed to be a dual electronic system composed of localized and itinerant magnetic electrons. Finally we note that the analysis framework can be applied to other helimagnets such as the magnetoelectric compound Cu2OSeO3.

cond-mat.str-el↗

arXiv2019

Lifetime-shortened acoustic phonons and static order at the Brillouin zone boundary in the organic-inorganic perovskite CH$_3$NH$_3$PbCl$_3$

Lead halide hybrid perovskites consist of an inorganic framework hosting a molecular cation located in the interstitial space. These compounds have been extensively studied as they have been identified as promising materials for photovoltaic applications with the interaction between the molecular cation and the inorganic framework implicated as influential for the electronic properties. CH3NH3PbCl3 undergoes two structural transitions from a high temperature cubic unit cell to a tetragonal phase at 177 K and an orthorhombic transition at 170 K. We have measured the low-frequency lattice dynamics using neutron spectroscopy and observe an energy broadening in the acoustic phonon linewidth towards the symmetry point QX =(2,1/2,0) when approaching the transitions. Concomitant with these zone boundary anomalies is a hardening of the entire acoustic phonon branch measured near the (2, 0, 0) Bragg position with decreasing temperature. Measurements of the elastic scattering at the Brillouin zone edges QX = (2,1/2,0), QM = (3/2,1/2,0), and QR = (3/2,3/2,5/2) show Bragg peaks appearing below these structural transitions. Based on selection rules of neutron scattering, we suggest that the higher 177 K transition is displacive with a distortion of the local octahedral environment and the lower transition is a rigid tilt transition of the octahedra. We do not observe any critical broadening in energy or momentum, beyond resolution, of these peaks near the transitions. We compare these results to the critical properties reported near the structural transitions in other perovskites. We suggest that the simultaneous onset of static resolution-limited Bragg peaks at the zone boundaries and the changes in acoustic phonon energies near the zone center is evidence of a coupling between the inorganic framework and the molecular cation.

cond-mat.mtrl-sci↗

arXiv2018

On the robustness of the MnSi magnetic structure determined by muon spin rotation

Muon spin rotation (muSR) spectra recorded for manganese silicide MnSi and interpreted in terms of a quantitative analysis constrained by symmetry arguments were recently published. The magnetic structures of MnSi in zero-field at low temperature and in the conical phase near the magnetic phase transition were shown to substantially deviate from the expected helical and conical structures. Here, we present material backing the previous results obtained in zero-field. First, from simulations of the field distributions experienced by the muons as a function of relevant parameters we confirm the uniqueness of the initial interpretation and illustrate the remarkable complementarity of neutron scattering and muSR for the MnSi magnetic structure determination. Second we present the result of a muSR experiment performed on MnSi crystallites grown in a Zn-flux and compare it with the previous data recorded with a crystal obtained from Czochralski pulling. We find the magnetic structure for the two types of crystals to be identical within experimental uncertainties. We finally address the question of a possible muon-induced effect by presenting transverse field muSR spectra recorded in a wide range of temperature and field intensity. The field distribution parameters perfectly scale with the macroscopic magnetization, ruling out a muon-induced effect.

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↗

arXiv2017

Transverse acoustic phonon anomalies at intermediate wavevectors in MgV$_{2}$O$_{4}$

Magnetic spinels (with chemical formula $AX_{2}$O$_{4}$, with $X$ a 3$d$ transition metal ion) that also have an orbital degeneracy are Jahn-Teller active and hence possess a coupling between spin and lattice degrees of freedom. At high temperatures, MgV$_{2}$O$_{4}$ is a cubic spinel based on V$^{3+}$ ions with a spin $S$=1 and a triply degenerate orbital ground state. A structural transition occurs at T$_{OO}$=63 K to an orbitally ordered phase with a tetragonal unit cell followed by an antiferromagnetic transition of T$_{N}$=42 K on cooling. We apply neutron spectroscopy in single crystals of MgV$_{2}$O$_{4}$ to show an anomaly for intermediate wavevectors at T$_{OO}$ associated with the acoustic phonon sensitive to the shear elastic modulus $\left(C_{11}-C_{12}\right)/2$. On warming, the shear mode softens for momentum transfers near close to half the Brillouin zone boundary, but recovers near the zone centre. High resolution spin-echo measurements further illustrate a temporal broadening with increased temperature over this intermediate range of wavevectors, indicative of a reduction in phonon lifetime. A subtle shift in phonon frequencies over the same range of momentum transfers is observed with magnetic fields. We discuss this acoustic anomaly in context of coupling to orbital and charge fluctuations.

cond-mat.str-el↗

arXiv2017

Long-range dynamical magnetic order and spin tunneling in the cooperative paramagnetic states of the pyrochlore analogous spinel antiferromagnets CdYb2X4 (X = S, Se)

Magnetic systems with spins sitting on a lattice of corner sharing regular tetrahedra have been particularly prolific for the discovery of new magnetic states for the last two decades. The pyrochlore compounds have offered the playground for these studies, while little attention has been comparatively devoted to other compounds where the rare earth R occupies the same sub-lattice, e.g. the spinel chalcogenides CdR2X4 (X = S, Se). Here we report measurements performed on powder samples of this series with R = Yb using specific heat, magnetic susceptibility, neutron diffraction and muon-spin-relaxation measurements. The two compounds are found to be magnetically similar. They long-range order into structures described by the Γ_5 irreducible representation. The magnitude of the magnetic moment at low temperature is 0.77 (1) and 0.62 (1) mu_B for X = S and Se, respectively. Persistent spin dynamics is present in the ordered states. The spontaneous field at the muon site is anomalously small, suggesting magnetic moment fragmentation. A double spin-flip tunneling relaxation mechanism is suggested in the cooperative paramagnetic state up to 10 K. The magnetic space groups into which magnetic moments of systems of corner-sharing regular tetrahedra order are provided for a number of insulating compounds characterized by null propagation wavevectors.

cond-mat.str-el↗

arXiv2017

Magnetic structure of Ba(TiO)Cu$_4$(PO$_4$)$_4$ probed using spherical neutron polarimetry

The antiferromagnetic compound Ba(TiO)Cu$_4$(PO$_4$)$_4$ contains square cupola of corner-sharing CuO$_4$ plaquettes, which were proposed to form effective quadrupolar order. To identify the magnetic structure, we have performed spherical neutron polarimetry measurements. Based on symmetry analysis and careful measurements we conclude that the orientation of the Cu$^{2+}$ spins form a non-collinear in-out structure with spins approximately perpendicular to the CuO$_4$ motif. Strong Dzyaloshinskii-Moriya interaction naturally lends itself to explain this phenomenon. The identification of the ground state magnetic structure should serve well for future theoretical and experimental studies into this and closely related compounds.

cond-mat.str-el↗

arXiv2017

Complementary response of static spin-stripe order and superconductivity to non-magnetic impurities in cuprates

We report muon-spin rotation and neutron-scattering experiments on non-magnetic Zn impurity effects on the static spin-stripe order and superconductivity of the La214 cuprates. Remarkably, it was found that, for samples with hole doping x = 1/8, the spin-stripe ordering temperature T_so decreases linearly with Zn doping y and disappears at around y = 4\%, demonstrating a high sensitivity of static spin-stripe order to impurities within a CuO_2 plane. Moreover, T_so is suppressed by Zn in the same manner as is the superconducting transition temperature T_c for samples near optimal hole doping. This surprisingly similar sensitivity suggests that the spin-stripe order is dependent on intertwining with superconducting correlations.

cond-mat.supr-con↗

arXiv2017

Coupled multiferroic domain switching in the canted conical spin spiral system Mn$_{2}$GeO$_{4}$

Despite remarkable progress in developing multifunctional materials, spin-driven ferroelectrics featuring both spontaneous magnetization and electric polarization are still rare. Among such ferromagnetic ferroelectrics are conical spin spiral magnets with a simultaneous reversal of magnetization and electric polarization that is still little understood. Such materials can feature various multiferroic domains that complicates their study. Here we study the multiferroic domains in ferromagnetic ferroelectric Mn$_{2}$GeO$_{4}$ using neutron diffraction, and show that it features a double-Q conical magnetic structure that, apart from trivial 180 degree commensurate magnetic domains, can be described by ferromagnetic and ferroelectric domains only. We show unconventional magnetoelectric couplings such as the magnetic-field-driven reversal of ferroelectric polarization with no change of spin-helicity, and present a phenomenological theory that successfully explains the magnetoelectric coupling. Our measurements establish Mn$_{2}$GeO$_{4}$ as a conceptually simple multiferroic in which the magnetic-field-driven flop of conical spin spirals leads to the simultaneous reversal of magnetization and electric polarization.

cond-mat.str-el↗

arXiv2017

Magnetic structure of the MnGe helimagnet and representation analysis

In the light of recent results obtained for the prototype helimagnet MnSi we examine the possible magnetic structures of compounds of the same family, consistent with the crystal symmetries when the magnetic propagation vector is parallel to the [001] axis. The analysis of a published muon spin rotation spectrum recorded in MnGe [Phys. Rev. B 93, 174405 (2016)] shows no deviation from the canonical helimagnetic structure, unlike in MnSi. This qualitative difference calls for further theoretical works on chiral magnets.

cond-mat.str-el↗