Topological magnon band structure of emergent Landau levels in a skyrmion lattice.

The motion of a spin excitation across topologically nontrivial magnetic order exhibits a deflection that is analogous to the effect of the Lorentz force on an electrically charged particle in an orbital magnetic field. We used polarized inelastic neutron scattering to investigate the propagation of magnons (i.e., bosonic collective spin excitations) in a lattice of skyrmion tubes in manganese silicide. For wave vectors perpendicular to the skyrmion tubes, the magnon spectra are consistent with the formation of finely spaced emergent Landau levels that are characteristic of the fictitious magnetic field used to account for the nontrivial topological winding of the skyrmion lattice. This provides evidence of a topological magnon band structure in reciprocal space, which is borne out of the nontrivial real-space topology of a magnetic order.

Low-energy spin dynamics in rare-earth perovskite oxides.

We review recent studies of spin dynamics in rare-earth orthorhombic perovskite oxides of the type RMO3, where R is a rare-earth ion and M is a transition-metal ion, using single-crystal inelastic neutron scattering (INS). After a short introduction to the magnetic INS technique in general, the results of INS experiments on both transition-metal and rare-earth subsystems for four selected compounds (YbFeO3, TmFeO3, YFeO3, YbAlO3) are presented. We show that the spectrum of magnetic excitations consists of two types of collective modes that are well separated in energy: gapped magnons with a typical bandwidth of <70 meV, associated with the antiferromagnetically (AFM) ordered transition-metal subsystem, and AFM fluctuations of <5 meV within the rare-earth subsystem, with no hybridization of those modes. We discuss the high-energy conventional magnon excitations of the 3dsubsystem only briefly, and focus in more detail on the spectacular dynamics of the rare-earth sublattice in these materials. We observe that the nature of the ground state and the low-energy excitation strongly depends on the identity of the rare-earth ion. In the case of non-Kramers ions, the low-symmetry crystal field completely eliminates the degeneracy of the multiplet state, creating a rich magnetic field-temperature phase diagram. In the case of Kramers ions, the resulting ground state is at least a doublet, which can be viewed as an effective quantum spin-1/2. Equally important is the fact that in Yb-based materials the nearest-neighbor exchange interaction dominates in one direction, despite the three-dimensional nature of the orthoperovskite crystal structure. The observation of a fractional spinon continuum and quantum criticality in YbAlO3demonstrates that Kramers rare-earth based magnets can provide realizations of various aspects of quantum low-dimensional physics.

Van Hove singularity in the magnon spectrum of the antiferromagnetic quantum honeycomb lattice.

In quantum magnets, magnetic moments fluctuate heavily and are strongly entangled with each other, a fundamental distinction from classical magnetism. Here, with inelastic neutron scattering measurements, we probe the spin correlations of the honeycomb lattice quantum magnet YbCl3. A linear spin wave theory with a single Heisenberg interaction on the honeycomb lattice, including both transverse and longitudinal channels of the neutron response, reproduces all of the key features in the spectrum. In particular, we identify a Van Hove singularity, a clearly observable sharp feature within a continuum response. The demonstration of such a Van Hove singularity in a two-magnon continuum is important as a confirmation of broadly held notions of continua in quantum magnetism and additionally because analogous features in two-spinon continua could be used to distinguish quantum spin liquids from merely disordered systems. These results establish YbCl3 as a benchmark material for quantum magnetism on the honeycomb lattice.

Extended anharmonic collapse of phonon dispersions in SnS and SnSe.

The lattice dynamics and high-temperature structural transition in SnS and SnSe are investigated via inelastic neutron scattering, high-resolution Raman spectroscopy and anharmonic first-principles simulations. We uncover a spectacular, extreme softening and reconstruction of an entire manifold of low-energy acoustic and optic branches across a structural transition, reflecting strong directionality in bonding strength and anharmonicity. Further, our results solve a prior controversy by revealing the soft-mode mechanism of the phase transition that impacts thermal transport and thermoelectric efficiency. Our simulations of anharmonic phonon renormalization go beyond low-order perturbation theory and capture these striking effects, showing that the large phonon shifts directly affect the thermal conductivity by altering both the phonon scattering phase space and the group velocities. These results provide a detailed microscopic understanding of phase stability and thermal transport in technologically important materials, providing further insights on ways to control phonon propagation in thermoelectrics, photovoltaics, and other materials requiring thermal management.

Order out of a Coulomb Phase and Higgs Transition: Frustrated Transverse Interactions of Nd_{2}Zr_{2}O_{7}.

The pyrochlore material Nd_{2}Zr_{2}O_{7} with an "all-in-all-out" (AIAO) magnetic order shows novel quantum moment fragmentation with gapped flat dynamical spin ice modes. The parametrized spin Hamiltonian with a dominant frustrated ferromagnetic transverse term reveals a proximity to a U(1) spin liquid. Here we study the magnetic excitations of Nd_{2}Zr_{2}O_{7} above the ordering temperature (T_{N}) using high-energy-resolution inelastic neutron scattering. We find strong spin ice correlations at zero energy with the disappearance of gapped magnon excitations of the AIAO order. It seems that the gap to the dynamical spin ice closes above T_{N} and the system enters a quantum spin ice state competing with and suppressing the AIAO order. Classical Monte Carlo simulations, molecular dynamics, and quantum boson calculations support the existence of a Coulombic phase above T_{N}. Our findings relate the magnetic ordering of Nd_{2}Zr_{2}O_{7} with the Higgs mechanism and provide explanations for several previously reported experimental features.

Tomonaga-Luttinger liquid behavior and spinon confinement in YbAlO3.

Low dimensional quantum magnets are interesting because of the emerging collective behavior arising from strong quantum fluctuations. The one-dimensional (1D) S = 1/2 Heisenberg antiferromagnet is a paradigmatic example, whose low-energy excitations, known as spinons, carry fractional spin S = 1/2. These fractional modes can be reconfined by the application of a staggered magnetic field. Even though considerable progress has been made in the theoretical understanding of such magnets, experimental realizations of this low-dimensional physics are relatively rare. This is particularly true for rare-earth-based magnets because of the large effective spin anisotropy induced by the combination of strong spin-orbit coupling and crystal field splitting. Here, we demonstrate that the rare-earth perovskite YbAlO3 provides a realization of a quantum spin S = 1/2 chain material exhibiting both quantum critical Tomonaga-Luttinger liquid behavior and spinon confinement-deconfinement transitions in different regions of magnetic field-temperature phase diagram.

Evidence for the confinement of magnetic monopoles in quantum spin ice.

Magnetic monopoles are hypothesised elementary particles connected by Dirac strings that behave like infinitely thin solenoids (Dirac 1931 Proc. R. Soc. A 133 60). Despite decades of searching, free magnetic monopoles and their Dirac strings have eluded experimental detection, although there is substantial evidence for deconfined magnetic monopole quasiparticles in spin ice materials (Castelnovo et al 2008 Nature 326 411). Here we report the detection of a hierarchy of unequally-spaced magnetic excitations via high resolution inelastic neutron spectroscopic measurements on the quantum spin ice candidate [Formula: see text] [Formula: see text] [Formula: see text]. These excitations are well-described by a simple model of monopole pairs bound by a linear potential (Coldea et al Science 327 177) with an effective tension of 0.642(8) K [Formula: see text] at 1.65 K. The success of the linear potential model suggests that these low energy magnetic excitations are direct spectroscopic evidence for the confinement of magnetic monopole quasiparticles in the quantum spin ice candidate [Formula: see text] [Formula: see text] [Formula: see text].

Scaling of Memories and Crossover in Glassy Magnets.

Glassiness is ubiquitous and diverse in characteristics in nature. Understanding their differences and classification remains a major scientific challenge. Here, we show that scaling of magnetic memories with time can be used to classify magnetic glassy materials into two distinct classes. The systems studied are high temperature superconductor-related materials, spin-orbit Mott insulators, frustrated magnets, and dilute magnetic alloys. Our bulk magnetization measurements reveal that most densely populated magnets exhibit similar memory behavior characterized by a relaxation exponent of [Formula: see text]. This exponent is different from [Formula: see text] of dilute magnetic alloys that was ascribed to their hierarchical and fractal energy landscape, and is also different from [Formula: see text] of the conventional Debye relaxation expected for a spin solid, a state with long range order. Furthermore, our systematic study on dilute magnetic alloys with varying magnetic concentration exhibits crossovers among the two glassy states and spin solid.

Observation of dynamic atom-atom correlation in liquid helium in real space.

Liquid 4He becomes superfluid and flows without resistance below temperature 2.17 K. Superfluidity has been a subject of intense studies and notable advances were made in elucidating the phenomenon by experiment and theory. Nevertheless, details of the microscopic state, including dynamic atom-atom correlations in the superfluid state, are not fully understood. Here using a technique of neutron dynamic pair-density function (DPDF) analysis we show that 4He atoms in the Bose-Einstein condensate have environment significantly different from uncondensed atoms, with the interatomic distance larger than the average by about 10%, whereas the average structure changes little through the superfluid transition. DPDF peak not seen in the snap-shot pair-density function is found at 2.3 Å, and is interpreted in terms of atomic tunnelling. The real space picture of dynamic atom-atom correlations presented here reveal characteristics of atomic dynamics not recognized so far, compelling yet another look at the phenomenon.

The cold neutron chopper spectrometer at the Spallation Neutron Source-A review of the first 8 years of operation.

The first eight years of operation of the Cold Neutron Chopper Spectrometer (CNCS) at the Spallation Neutron Source in Oak Ridge is being reviewed. The instrument has been part of the facility user program since 2009, and more than 250 individual user experiments have been performed to date. CNCS is an extremely powerful and versatile instrument and offers leading edge performance in terms of beam intensity, energy resolution, and flexibility to trade one for another. Experiments are being routinely performed with the sample at extreme conditions: T ≲ 0.05 K, p ≳ 2 GPa, and B = 8 T can be achieved individually or in combination. In particular, CNCS is in a position to advance the state of the art with inelastic neutron scattering under pressure, and some of the recent accomplishments in this area will be presented in more detail.

Orbital-exchange and fractional quantum number excitations in an f-electron metal, Yb2Pt2Pb.

Exotic quantum states and fractionalized magnetic excitations, such as spinons in one-dimensional chains, are generally expected to occur in 3d transition metal systems with spin 1/2. Our neutron-scattering experiments on the 4f-electron metal Yb2Pt2Pb overturn this conventional wisdom. We observe broad magnetic continuum dispersing in only one direction, which indicates that the underlying elementary excitations are spinons carrying fractional spin-1/2. These spinons are the emergent quantum dynamics of the anisotropic, orbital-dominated Yb moments. Owing to their unusual origin, only longitudinal spin fluctuations are measurable, whereas the transverse excitations such as spin waves are virtually invisible to magnetic neutron scattering. The proliferation of these orbital spinons strips the electrons of their orbital identity, resulting in charge-orbital separation.

Static and Dynamical Properties of the Spin-1/2 Equilateral Triangular-Lattice Antiferromagnet Ba_{3}CoSb_{2}O_{9}.

We present single-crystal neutron scattering measurements of the spin-1/2 equilateral triangular-lattice antiferromagnet Ba_{3}CoSb_{2}O_{9}. Besides confirming that the Co^{2+} magnetic moments lie in the ab plane for zero magnetic field and then determining all the exchange parameters of the minimal quasi-2D spin Hamiltonian, we provide conclusive experimental evidence of magnon decay through observation of intrinsic line broadening. Through detailed comparisons with the linear and nonlinear spin-wave theories, we also point out that the large-S approximation, which is conventionally employed to predict magnon decay in noncollinear magnets, is inadequate to explain our experimental observation. Thus, our results call for a new theoretical framework for describing excitation spectra in low-dimensional frustrated magnets under strong quantum effects.

Damped spin waves in the intermediate ordered phases in Ni3V2O8.

Spin dynamics in the intermediate ordered phases (between 4 and 9 K) in Ni3V2O8 have been studied with inelastic neutron scattering. It is found that the spin waves are very diffuse, indicative of short lived correlations and the coexistence of paramagnetic moments with the long-range ordered state.

Painting biological low-frequency vibrational modes from small peptides to proteins.

Protein low-frequency vibrational modes are an important portion of a proteins' dynamical repertoire. Yet, it is notoriously difficult to isolate specific vibrational features in the spectra of proteins. Given an appropriately chosen model peptide, and using different experimental conditions, we can simplify the system and gain useful insights into the protein vibrational properties. Combining neutron scattering, depolarized light scattering, and molecular dynamics simulations, we analyse the low frequency vibrations of biological molecules, comparing the results from a small globular protein, lysozyme, and an amphiphilic peptide, NALMA, both in solution and in powder states. Lysozyme and NALMA present similar spectral features in the frequency range between 1 and 10 THz. With the aid of MD simulations, we assign the spectral features to methyl groups' librations (1-5 THz) and hindered torsions (5-10 THz) in NALMA. Our data also show that, while proteins display boson peak vibrations in both powder and solution forms, NALMA exhibits boson peak vibrations in powder form only. This provides insight into the nature of this feature, suggesting a connection of BP collective motions to a characteristic length scale of heterogeneities present in the system. These results provide context for the use of model peptide systems to study protein dynamics; demonstrating both their utility, and the great care that has to be used in extrapolating results observed in powder to solutions.

Quantum critical fluctuations in the heavy fermion compound Ce(Ni0.935Pd0.065)2Ge2.

Electric resistivity, specific heat, magnetic susceptibility, and inelastic neutron scattering experiments were performed on a single crystal of the heavy fermion compound Ce(Ni0.935Pd0.065)2Ge2 in order to study the spin fluctuations near an antiferromagnetic (AF) quantum critical point (QCP). The resistivity and the specific heat coefficient for T ⩽ 1 K exhibit the power law behavior expected for a 3D itinerant AF QCP (ρ(T) ∼ T(3/2) and γ(T) ∼ γ0 - bT(1/2)). However, for 2 ⩽ T ⩽ 10 K, the susceptibility and specific heat vary as log T and the resistivity varies linearly with temperature. Furthermore, despite the fact that the resistivity and specific heat exhibit the non-Fermi liquid behavior expected at a QCP, the correlation length, correlation time, and staggered susceptibility of the spin fluctuations remain finite at low temperature. We suggest that these deviations from the divergent behavior expected for a QCP may result from alloy disorder.

Magnitude of the magnetic exchange interaction in the heavy-fermion antiferromagnet CeRhIn5.

We have used high-resolution neutron spectroscopy experiments to determine the complete spin wave spectrum of the heavy-fermion antiferromagnet CeRhIn5. The spin wave dispersion can be quantitatively reproduced with a simple frustrated J1-J2 model that also naturally explains the magnetic spin-spiral ground state of CeRhIn5 and yields a dominant in-plane nearest-neighbor magnetic exchange constant J0=0.74(3) meV. Our results pave the way to a quantitative understanding of the rich low-temperature phase diagram of the prominent CeTIn5 (T=Co, Rh, Ir) class of heavy-fermion materials.

From spin glass to quantum spin liquid ground states in molybdate pyrochlores.

We present new magnetic heat capacity and neutron scattering results for two magnetically frustrated molybdate pyrochlores: S=1 oxide Lu_{2}Mo_{2}O_{7} and S=1/2 oxynitride Lu_{2}Mo_{2}O_{5}N_{2}. Lu_{2}Mo_{2}O_{7} undergoes a transition to an unconventional spin glass ground state at T_{f}∼16 K. However, the preparation of the corresponding oxynitride tunes the nature of the ground state from spin glass to quantum spin liquid. The comparison of the static and dynamic spin correlations within the oxide and oxynitride phases presented here reveals the crucial role played by quantum fluctuations in the selection of a ground state. Furthermore, we estimate an upper limit for a gap in the spin excitation spectrum of the quantum spin liquid state of the oxynitride of Δ∼0.05 meV or Δ/|θ|∼0.004, in units of its antiferromagnetic Weiss constant θ∼-121 K.

Phonon self-energy and origin of anomalous neutron scattering spectra in SnTe and PbTe thermoelectrics.

The anharmonic lattice dynamics of rock-salt thermoelectric compounds SnTe and PbTe are investigated with inelastic neutron scattering (INS) and first-principles calculations. The experiments show that, surprisingly, although SnTe is closer to the ferroelectric instability, phonon spectra in PbTe exhibit a more anharmonic character. This behavior is reproduced in first-principles calculations of the temperature-dependent phonon self-energy. Our simulations reveal how the nesting of phonon dispersions induces prominent features in the self-energy, which account for the measured INS spectra and their temperature dependence. We establish that the phase space for three-phonon scattering processes, combined with the proximity to the lattice instability, is the mechanism determining the complex spectrum of the transverse-optic ferroelectric mode.

A comparison of four direct geometry time-of-flight spectrometers at the Spallation Neutron Source.

The Spallation Neutron Source at Oak Ridge National Laboratory now hosts four direct geometry time-of-flight chopper spectrometers. These instruments cover a range of wave-vector and energy transfer space with varying degrees of neutron flux and resolution. The regions of reciprocal and energy space available to measure at these instruments are not exclusive and overlap significantly. We present a direct comparison of the capabilities of this instrumentation, conducted by data mining the instrument usage histories, and specific scanning regimes. In addition, one of the common science missions for these instruments is the study of magnetic excitations in condensed matter systems. We have measured the powder averaged spin wave spectra in one particular sample using each of these instruments, and use these data in our comparisons.

A detailed study of the magnetic phase transition in CuCrO2.

The phase transition in CuCrO2 to an ordered magnetic state is studied with bulk measurements and elastic and inelastic neutron scattering techniques. The reported onset of spontaneous electric polarization at T = 23.5 K coincides with the appearance, on cooling, of elastic magnetic scattering. At higher temperatures long range magnetic correlations gradually develop but they are dynamic. The ground state is characterized by three-dimensional long range magnetic ordering but along the c direction the correlation length remains limited to ∼200 Å.