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R. Moessner

Publications and source records attributed to R. Moessner.

At least 19 recordsLinked to original sources

Observation of Dipolar Spin-ice--like Correlations in the Quantum Spin Ice Candidate Ce$_2$Sn$_2$O$_7$

We report diffuse scattering measurements on the dipolar-octupolar pyrochlore, Ce$_2$Sn$_2$O$_7$, to elucidate its magnetic correlations within the correlated paramagnetic regime above its ordering temperature, $\mathrm{T_N}\sim 40~$mK. The magnetic transition at $\mathrm{T_N}$, observed in recent specific heat measurements, has been interpreted within the nearest-neighbor XYZ model as a transition into an all-in-all-out (AIAO) magnetic order. However, the observed diffuse scattering above $\mathrm{T_N}$ argues against an AIAO magnetic order by exhibiting $no$ short-range order at the AIAO wave-vectors, inconsistent with the nearest neighbor model. Instead, the observed diffuse scattering strongly resembles that observed in classical dipolar spin ice, Dy$_2$Ti$_2$O$_7$, and suggests the presence of short-range correlated structures such as chains, or clusters in the low energy manifold of Ce$_2$Sn$_2$O$_7$, favored by further neighbor interactions. We discuss how chain-like states qualitatively account for the observed H-T phase diagram under a [1,1,0]-field.

cond-mat.str-el

Intermediate Field Spin(on) Dynamics in $\alpha$-RuCl$_3$

We present comprehensive inelastic neutron spectroscopic maps of the magnetic field-induced disordered phase of the Kitaev quantum spin liquid candidate material $\alpha$-RuCl$_3$. For fields along both in-plane high-symmetry directions we observe that the spin excitation spectrum at and above a magnetic field of 8~T is gapped. Excitation modes then sharpen for increasing field but are consistently broader than experimental resolution even at 13.5~T. The out-of-plane dispersion diminishes in the 7-10~T regime, signifying enhanced two-dimensional behavior as the in-plane liquid correlations are established. In this regime, excitations are very broad and largely flat for all accessible energy-momenta, which is kinematically at odds with a magnon-decay picture. By contrast, a continuum of fractionalized excitations naturally yields a broad continuum response, which crucially may be accompanied by sharper modes of bound states of fractionalized excitations. Their damping by the continuum accounts for the observed spectral broadening and field dependence. Our results provide strong evidence for the existence of fractionalized excitations in $\alpha$-RuCl$_3$ in a magnetic field.

cond-mat.str-el

Two-Peak Heat Capacity Accounts for $R\ln(2)$ Entropy and Ground State Access in the Dipole-Octupole Pyrochlore Ce$_2$Hf$_2$O$_7$

Magnetic heat capacity measurements of a high-quality single crystal of the dipole-octupole pyrochlore Ce$_2$Hf$_2$O$_7$ down to a temperature of $T = 0.02$ K are reported. These show a two-peaked structure, with a Schottky-like peak at $T_1 \sim 0.065$ K, similar to what is observed in its sister Ce-pyrochlores Ce$_2$Zr$_2$O$_7$ and Ce$_2$Sn$_2$O$_7$. However, a second sharper peak is observed at $T_2 \sim 0.025$ K, signifying the entrance to the ground state. The ground state appears to have gapped excitations, as even the most abrupt extrapolation to $C_P=0$ at $T = 0$ K fully accounts for the $R\ln(2)$ entropy associated with the pseudospin-1/2 doublet for Ce$^{3+}$ in this environment. The ground state could be conventionally ordered, although theory predicts a much larger anomaly in $C_P$ at much higher temperatures than the measured $T_2$ for expectations from an all-in all-out ground state of the XYZ Hamiltonian for Ce$_2$Hf$_2$O$_7$. The sharp low-temperature peak could also signify a cross-over from a classical spin liquid to a quantum spin liquid (QSL). For both scenarios, comparison of the measured $C_P$ with NLC calculations suggests that weak interactions beyond the nearest-neighbor XYZ Hamiltonian become relevant below $T \sim 0.25$ K. The diffuse magnetic neutron scattering observed from Ce$_2$Hf$_2$O$_7$ at low temperatures between $T_2$ and $T_1$ resembles that observed from Ce$_2$Zr$_2$O$_7$, which is well established as a $\pi$-flux quantum spin ice (QSI). Together with the peak in the heat capacity at $T_2$, this diffuse scattering from Ce$_2$Hf$_2$O$_7$ is suggestive of a classical spin liquid regime above $T_2$ that is distinct from the zero-entropy quantum ground state below $T_2$.

cond-mat.str-el

The landscape of symmetry enhancement in tight-binding models

Band structures are ubiquitous in condensed matter physics and their symmetries constrain possible degeneracies, topology and response functions across a broad range of different systems. Here we address the question: given a parent crystal, what is the symmetry of hopping models on that lattice at a given shell number? We find that the parent structure does not, in general, determine the symmetry of the tight-binding model. Instead, the symmetry is dependent on the hopping range. The key to symmetry breakdown on the lattice is the existence of different {\it bond equivalence classes} whose number is related to group-subgroup indices for a broad classes of cases. We find all bond equivalence classes for $s$-wave hopping out to 20th neighbor across the different space groups and Wyckoff positions and the symmetries of the associated tight-binding models. These observations naturally lead to the definition of a {\it bond complex} $-$ the possible classes of networks of bonds to which symmetries may be enhanced from a given parent structure.

cond-mat.str-el

Single Crystal Diffuse Neutron Scattering Study of the Dipole-Octupole Quantum Spin Ice Candidate Ce$_2$Zr$_2$O$_7$: No Apparent Octupolar Correlations Above $T = 0.05$ K

The insulating magnetic pyrochlore Ce$_2$Zr$_2$O$_7$ has gained attention as a quantum spin ice candidate with dipole-octupole character arising from the crystal electric field ground state doublet for the Ce$^{3+}$ ion. This permits both spin ice phases based on magnetic dipoles and those based on more-exotic octupoles. We report low-temperature neutron diffraction measurements on single crystal Ce$_2$Zr$_2$O$_7$ with $Q$-coverage both at low $Q$ where the magnetic form factor for dipoles is near maximal and at high $Q$ where the magnetic form factor for Ce$^{3+}$ octupoles is near maximal. This study was motivated by recent powder neutron diffraction studies of other Ce-based dipole-octupole pyrochlores, Ce$_2$Sn$_2$O$_7$ and Ce$_2$Hf$_2$O$_7$, which each showed temperature-dependent diffuse diffraction at high $Q$ that was interpreted as arising from octupolar correlations. Our measurements use an optimized single crystal diffuse scattering instrument that allows us to screen against strong Bragg scattering from Ce$_2$Zr$_2$O$_7$. The temperature-difference neutron diffraction reveals a low-$Q$ peak consistent with dipolar spin ice correlations reported in previous work, and an alternation between positive and negative net intensity at higher $Q$. These features are consistent with our numerical-linked-cluster calculations using pseudospin interaction parameters previously reported for Ce$_2$Zr$_2$O$_7$, Ce$_2$Sn$_2$O$_7$, and Ce$_2$Hf$_2$O$_7$. Importantly, neither the measured data nor any of the NLC calculations show evidence for increased scattering at high $Q$ resulting from octupolar correlations. We conclude that at the lowest attainable temperature for our measurements ($T = 0.05$ K), scattering from octupolar correlations in Ce$_2$Zr$_2$O$_7$ is not present in the neutron diffraction signal on the level of our observation threshold of ~ 0.1 % of the low-$Q$ dipole scattering.

cond-mat.str-el

Tomographic Imaging of Orbital Vortex Lines in Three-Dimensional Momentum Space

We report the experimental discovery of orbital vortex lines in the three-dimensional (3D) band structure of a topological semimetal. Combining linear and circular dichroism in soft x-ray angle-resolved photoemission (SX-ARPES) with first-principles theory, we image the winding of atomic orbital angular momentum, thereby revealing - and determining the location of - lines of vorticity in full 3D momentum space. Our observation of momentum-space vortex lines with quantized winding number establishes an analogue to real-space quantum vortices, for instance, in type-II superconductors and certain non-collinear magnets. These results establish multimodal dichroism in SX-ARPES as an approach to trace 3D orbital textures. Our present findings particularly constitute the first imaging of non-trivial quantum-phase winding at line nodes and may pave the way to new orbitronic phenomena in quantum materials

cond-mat.str-el

Quantum Spin Ice Response to a Magnetic Field in the Dipole-Octupole Pyrochlore Ce$_2$Zr$_2$O$_7$

We report new heat capacity measurements on single crystal Ce$_2$Zr$_2$O$_7$ down to $\sim$ 0.1 K in a magnetic field along the $[1,\bar{1}, 0]$ direction. These new measurements show that the broad hump in the zero-field heat capacity moves higher in temperature with increasing field strength and is split into two humps by the $[1,\bar{1}, 0]$ field at $\sim$ 2 T. These separate features are due to the decomposition of the pyrochlore lattice into effectively decoupled chains for fields in this direction: one set of chains ($\alpha$-chains) is polarized by the field while the other ($\beta$-chains) remains free. Our theoretical modelling suggests that the $\beta$-chains are close to a critical state, with nearly-gapless excitations. We also report new elastic and inelastic neutron scattering measurements on single crystal Ce$_2$Zr$_2$O$_7$ in $[1, \bar{1}, 0]$ and $[0, 0, 1]$ magnetic fields at temperatures down to 0.03 K. The elastic scattering behaves consistently with the formation of independent chains for a $[1, \bar{1}, 0]$ field, while the $[0, 0, 1]$ field produces a single field-induced magnetic Bragg peak at $(0, 2, 0)$ and equivalent wavevectors, indicating a polarized spin ice for fields above $\sim$ 3 T. For both $[1, \bar{1}, 0]$ and $[0, 0, 1]$ fields, our inelastic neutron scattering results show an approximately-dispersionless continuum of scattering that increases in both energy and intensity with increasing field strength. By modelling the complete set of experimental data using numerical linked cluster and semiclassical molecular dynamics calculations, we demonstrate the dominantly multipolar nature of the exchange interactions in Ce$_2$Zr$_2$O$_7$ and the smallness of the parameter $\theta$ which controls the mixing between dipolar and octupolar degrees of freedom. These results support previous estimates of the microscopic exchange parameters.

cond-mat.str-el

Adiabaticity enhancement in the classical transverse field Ising chain, and its effective non-Hermitian description

We analyse the near-adiabatic dynamics in a ramp through the critical point (CP) of the classical transverse field Ising chain. This is motivated, conceptually, by the fact that this CP -- unlike its quantum counterpart -- experiences no thermal or quantum fluctuations, and technically by the tractability of its effective model. For a `half-ramp' from ferromagnet to CP, the longitudinal and transverse magnetization scale as $\tau^{-1/3}$ and $\tau^{-2/3}$, respectively, with $1/\tau$ the ramp rate, in accord with Kibble-Zurek theory. For ferro- to paramagnetic ramps across the CP, however, they stay closer, $\tau^{-1/2}$ and $\tau^{-1}$, to adiabaticity. This adiabaticity enhancement compared to the half ramp is understood by casting the dynamics in the paramagnet in the form of a non-hermitian Dirac Hamiltonian, with the CP playing the role of an exceptional point, opening an additional decay channel.

cond-mat.stat-mech

Dipolar spin ice regime proximate to an all-in-all-out N\'{e}el ground state in the dipolar-octupolar pyrochlore Ce$_2$Sn$_2$O$_7$

The dipolar-octupolar (DO) pyrochlores, R$_2$M$_2$O$_7$ (R = Ce, Sm, Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce$_2$Sn$_2$O$_7$, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce$_2$Sn$_2$O$_7$ using the near-neighbor $XYZ$ model Hamiltonian associated with DO pyrochlores. Utilizing quantum numerical linked cluster expansion fits to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples, we place Ce$_2$Sn$_2$O$_7$'s ground state within the ordered dipolar all-in-all-out (AIAO) N\'{e}el phase, with quantum Monte Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce$_2$Sn$_2$O$_7$ powders show a broad signal at low scattering wave vectors, reminiscent of a \textit{dipolar} spin ice, in striking contrast from previous powder neutron diffraction on samples grown from solid-state synthesis, which found diffuse scattering at high scattering wave vectors associated with magnetic {\it octupoles} and suggested an octupolar quantum spin ice state. We conclude that new hydrothermally grown Ce$_2$Sn$_2$O$_7$ samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO N\'{e}el order.

cond-mat.str-el

Field-tunable Berezinskii-Kosterlitz-Thouless correlations in a Heisenberg magnet

We report the manifestation of field-induced Berezinskii-Kosterlitz-Thouless (BKT) correlations in the weakly coupled spin-1/2 Heisenberg layers of the molecular-based bulk material [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$. Due to the moderate intralayer exchange coupling of $J/k_\mathrm{B} = 6.8$ K, the application of laboratory magnetic fields induces a substantial $XY$ anisotropy of the spin correlations. Crucially, this provides a significant BKT regime, as the tiny interlayer exchange $J^\prime / k_\mathrm{B} \approx 1$ mK only induces 3D correlations upon close approach to the BKT transition with its exponential growth in the spin-correlation length. We employ nuclear magnetic resonance and $\mu^{+}$SR measurements to probe the spin correlations that determine the critical temperatures of the BKT transition as well as that of the onset of long-range order. Further, we perform stochastic series expansion quantum Monte Carlo simulations based on the experimentally determined model parameters. Finite-size scaling of the in-plane spin stiffness yields excellent agreement of critical temperatures between theory and experiment, providing clear evidence that the nonmonotonic magnetic phase diagram of [Cu(pz)$_2$(2-HOpy)$_2$](PF$_6$)$_2$ is determined by the field-tuned $XY$ anisotropy and the concomitant BKT physics.

cond-mat.str-el

Topological Electrostatics

We present a theory of optimal topological textures in nonlinear sigma-models with degrees of freedom living in the Grassmannian $\mathrm{Gr}(M,N)$ manifold. These textures describe skyrmion lattices of $N$-component fermions in a quantising magnetic field, relevant to the physics of graphene, bilayer and other multicomponent quantum Hall systems near integer filling factors $\nu>1$. We derive analytically the optimality condition, minimizing topological charge density fluctuations, for a general Grassmannian sigma model $\mathrm{Gr}(M,N)$ on a sphere and a torus, together with counting arguments which show that for any filling factor and number of components there is a critical value of topological charge $d_c$ above which there are no optimal textures. Below $d_c$ a solution of the optimality condition on a torus is unique, while in the case of a sphere one has, in general, a continuum of solutions corresponding to new {\it non-Goldstone} zero modes, whose degeneracy is not lifted (via a order from disorder mechanism) by any fermion interactions depending only on the distance on a sphere. We supplement our general theoretical considerations with the exact analytical results for the case of $\mathrm{Gr}(2,4)$, appropriate for recent experiments in graphene.

cond-mat.mes-hall

Dynamics and thermodynamics of a topological transition in spin ice materials under strain

We study single crystals of Dy$_2$Ti$_2$O$_7$ and Ho$_2$Ti$_2$O$_7$ under magnetic field and stress applied along their [001] direction. We find that many of the features that the emergent gauge field of spin ice confers to the macroscopic magnetic properties are preserved in spite of the finite temperature. The magnetisation vs. field shows an upward convexity within a broad range of fields, while the static and dynamic susceptibilities present a peculiar peak. Following this feature for both compounds, we determine a single experimental transition curve: that for the Kasteleyn transition in three dimensions, proposed more than a decade ago. Additionally, we observe that compression up to $-0.8\%$ along [001] does not significantly change the thermodynamics. However, the dynamical response of Ho$_2$Ti$_2$O$_7$ is quite sensitive to changes introduced in the ${\rm Ho}^{3+}$ environment. Uniaxial compression can thus open up experimental access to equilibrium properties of spin ice at low temperatures.

cond-mat.stat-mech

Spin-Space Groups and Magnon Band Topology

Band topology is both constrained and enriched by the presence of symmetry. The importance of anti-unitary symmetries such as time reversal was recognized early on leading to the classification of topological band structures based on the ten-fold way. Since then, lattice point group and non-symmorphic symmetries have been seen to lead to a vast range of possible topologically nontrivial band structures many of which are realized in materials. In this paper we show that band topology is further enriched in many physically realizable instances where magnetic and lattice degrees of freedom are wholly or partially decoupled. The appropriate symmetry groups to describe general magnetic systems are the spin-space groups. Here we describe cases where spin-space groups are essential to understand the band topology in magnetic materials. We then focus on magnon band topology where the theory of spin-space groups has its simplest realization. We consider magnetic Hamiltonians with various types of coupling including Heisenberg and Kitaev couplings revealing a hierarchy of enhanced magnetic symmetry groups depending on the nature of the lattice and the couplings. We describe, in detail, the associated representation theory and compatibility relations thus characterizing symmetry-enforced constraints on the magnon bands revealing a proliferation of nodal points, lines, planes and volumes.

cond-mat.str-el

Butterfly Effect and Spatial Structure of Information Spreading in a Chaotic Cellular Automaton

Inspired by recent developments in the study of chaos in many-body systems, we construct a measure of local information spreading for a stochastic Cellular Automaton in the form of a spatiotemporally resolved Hamming distance. This decorrelator is a classical version of an Out-of-Time-Order Correlator studied in the context of quantum many-body systems. Focusing on the one-dimensional Kauffman Cellular Automaton, we extract the scaling form of our decorrelator with an associated butterfly velocity $v_b$ and a velocity-dependent Lyapunov exponent $\lambda(v)$. The existence of the latter is not a given in a discrete classical system. Second, we account for the behaviour of the decorrelator in a framework based solely on the boundary of the information spreading, including an effective boundary random walk model yielding the full functional form of the decorrelator. In particular, we obtain analytic results for $v_b$ and the exponent $\beta$ in the scaling ansatz $\lambda(v) \sim \mu (v - v_b)^\beta$, which is usually only obtained numerically. Finally, a full scaling collapse establishes the decorrelator as a unifying diagnostic of information spreading.

cond-mat.stat-mech

Emergent moments and random singlet physics in a Majorana spin liquid

We exhibit an exactly solvable example of a SU(2) symmetric Majorana spin liquid phase, in which quenched disorder leads to random-singlet phenomenology. More precisely, we argue that a strong-disorder fixed point controls the low temperature susceptibility $\chi(T)$ of an exactly solvable $S=1/2$ model on the decorated honeycomb lattice with quenched bond disorder and/or vacancies, leading to $\chi(T) = {\mathcal C}/T+ {\mathcal D} T^{\alpha(T) - 1}$ where $\alpha(T) \rightarrow 0$ as $T \rightarrow 0$. The first term is a Curie tail that represents the emergent response of vacancy-induced spin textures spread over many unit cells: it is an intrinsic feature of the site-diluted system, rather than an extraneous effect arising from isolated free spins. The second term, common to both vacancy and bond disorder (with different $\alpha(T)$ in the two cases) is the response of a random singlet phase, familiar from random antiferromagnetic spin chains and the analogous regime in phosphorus-doped silicon (Si:P).

cond-mat.str-el

Quantum spin liquid at finite temperature: proximate dynamics and persistent typicality

Quantum spin liquids are long-range entangled states of matter with emergent gauge fields and fractionalized excitations. While candidate materials, such as the Kitaev honeycomb ruthenate $\alpha$-RuCl$_3$, show magnetic order at low temperatures $T$, here we demonstrate numerically a dynamical crossover from magnon-like behavior at low $T$ and frequencies $\omega$ to long-lived fractionalized fermionic quasiparticles at higher $T$ and $\omega$. This crossover is akin to the presence of spinon continua in quasi-1D spin chains. It is further shown to go hand in hand with persistent typicality down to very low $T$. This aspect, which has also been observed in the spin-1/2 kagome Heisenberg antiferromagnet, is a signature of proximate spin liquidity and emergent gauge degrees of freedom more generally, and can be the basis for the numerical study of many finite-$T$ properties of putative spin liquids.

cond-mat.str-el

Probing spin correlations using angle resolved photoemission in a coupled metallic/Mott insulator system

A nearly free electron metal and a Mott insulating state can be thought of as opposite ends of possibilities for the motion of electrons in a solid. In the magnetic oxide metal PdCrO$_{2}$, these two coexist as alternating layers. Using angle resolved photoemission, we surprisingly find sharp band-like features in the one-electron removal spectral function of the correlated subsystem. We show that these arise because a hole created in the Mott layer moves to and propagates in the metallic layer while retaining memory of the Mott layer's magnetism. This picture is quantitatively supported by a strong coupling analysis capturing the physics of PdCrO$_{2}$ in terms of a Kondo lattice Hamiltonian. Our findings open new routes to use the non-magnetic probe of photoemission to gain insights into the spin-susceptibility of correlated electron systems.

cond-mat.str-el

Zero point fluctuations for magnetic spirals and Skyrmions, and the fate of the Casimir energy in the continuum limit

We study the role of zero-point quantum fluctuations in a range of magnetic states which on the classical level are close to spin-aligned ferromagnets. These include Skyrmion textures characterized by non-zero topological charge, and topologically-trivial spirals arising from the competition of the Heisenberg and Dzyaloshinskii-Moriya interactions. For the former, we extend our previous results on quantum exactness of classical Bogomolny-Prasad-Sommerfield (BPS) ground-state degeneracies to the general case of K\"ahler manifolds, with a specific example of Grassmann manifolds $\mathrm{Gr(M,N)}$. These are relevant to quantum Hall ferromagnets with $\mathrm{N}$ internal states and integer filling factor $\mathrm{M}$. A promising candidate for their experimental implementation is monolayer graphene with $\mathrm{N=4}$ corresponding to spin and valley degrees of freedom at the charge neutrality point with $\mathrm{M=2}$ filled Landau levels. We find that the vanishing of the zero-point fluctuations in taking the continuum limit occurs differently in the case of BPS states compared to the case of more general smooth textures, with the latter exhibiting more pronounced lattice effects. This motivates us to consider the vanishing of zero-point fluctuations in such near-ferromagnets more generally. We present a family of lattice spin models for which the vanishing of zero-point fluctuations is evident, and show that some spirals can be thought of as having nonzero but weak zero-point fluctuations on account of their closeness to this family. Between them, these instances provide concrete illustrations of how the Casimir energy, dependent on the full UV-structure of the theory, evolves as the continuum limit is taken.

cond-mat.str-el