Spinon confinement and a sharp longitudinal mode in Yb2Pt2Pb in magnetic fields.

The fundamental excitations in an antiferromagnetic chain of spins-1/2 are spinons, de-confined fractional quasiparticles that when combined in pairs, form a triplet excitation continuum. In an Ising-like spin chain the continuum is gapped and the ground state is Néel ordered. Here, we report high resolution neutron scattering experiments, which reveal how a magnetic field closes this gap and drives the spin chains in Yb2Pt2Pb to a critical, disordered Luttinger-liquid state. In Yb2Pt2Pb the effective spins-1/2 describe the dynamics of large, Ising-like Yb magnetic moments, ensuring that the measured excitations are exclusively longitudinal, which we find to be well described by time-dependent density matrix renormalization group calculations. The inter-chain coupling leads to the confinement of spinons, a condensed matter analog of quark confinement in quantum chromodynamics. Insensitive to transverse fluctuations, our measurements show how a gapless, dispersive longitudinal mode arises from confinement and evolves with magnetic order.

Frustrated magnetic interactions in an S = 3/2 bilayer honeycomb lattice compound Bi3Mn4O12(NO3).

An inelastic neutron scattering study has been performed in an S = 3/2 bilayer honeycomb lattice compound Bi3Mn4O12(NO3) at ambient and high magnetic fields. Relatively broad and monotonically dispersive magnetic excitations were observed at ambient field, where no long-range magnetic order exists. In the magnetic-field-induced long-range ordered state at 10 T, the magnetic dispersions become slightly more intense, albeit still broad as in the disordered state, and two excitation gaps, probably originating from an easy-plane magnetic anisotropy and intrabilayer interactions, develop. Analyzing the magnetic dispersions using the linear spin-wave theory, we estimated the intraplane and intrabilayer magnetic interactions, which are almost consistent with those determined by ab initio density functional theory calculations [M. Alaei et al., Phys. Rev. B 96, 140404(R) (2017)], except the third and fourth neighbor intrabilayer interactions. Most importantly, as predicted by the theory, there is no significant frustration in the honeycomb plane but frustrating intrabilayer interactions probably give rise to the disordered ground state.

Nanoscopic length scale dependence of hydrogen bonded molecular associates' dynamics in methanol.

In a recent paper [C. E. Bertrand et al., J. Chem. Phys. 145, 014502 (2016)], we have shown that the collective dynamics of methanol shows a fast relaxation process related to the standard density-fluctuation heat mode and a slow non-Fickian mode originating from the hydrogen bonded molecular associates. Here we report on the length scale dependence of this slow relaxation process. Using quasielastic neutron scattering and molecular dynamics simulations, we show that the dynamics of the slow process is affected by the structuring of the associates, which is accessible through polarized neutron diffraction experiments. Using a series of partially deuterated samples, the dynamics of the associates is investigated and is found to have a similar time scale to the lifetime of hydrogen bonding in the system. Both the structural relaxation and the dynamics of the associates are thermally activated by the breaking of hydrogen bonding.

Disordered Route to the Coulomb Quantum Spin Liquid: Random Transverse Fields on Spin Ice in Pr_{2}Zr_{2}O_{7}.

Inelastic neutron scattering reveals a broad continuum of excitations in Pr_{2}Zr_{2}O_{7}, the temperature and magnetic field dependence of which indicate a continuous distribution of quenched transverse fields (Δ) acting on the non-Kramers Pr^{3+} crystal field ground state doublets. Spin-ice correlations are apparent within 0.2 meV of the Zeeman energy. A random phase approximation provides an excellent account of the data with a transverse field distribution ρ(Δ)∝(Δ^{2}+Γ^{2})^{-1}, where Γ=0.27(1) meV. Established during high temperature synthesis due to an underlying structural instability, it appears disorder in Pr_{2}Zr_{2}O_{7} actually induces a quantum spin liquid.

Dynamic signature of molecular association in methanol.

Quasielastic neutron scattering measurements and molecular dynamics simulations were combined to investigate the collective dynamics of deuterated methanol, CD3OD. In the experimentally determined dynamic structure factor, a slow, non-Fickian mode was observed in addition to the standard density-fluctuation heat mode. The simulation results indicate that the slow dynamical process originates from the hydrogen bonding of methanol molecules. The qualitative behavior of this mode is similar to the previously observed α-relaxation in supercooled water [M. C. Bellissent-Funel et al., Phys. Rev. Lett. 85, 3644 (2000)] which also originates from the formation and dissolution of hydrogen-bonded associates (supramolecular clusters). In methanol, however, this mode is distinguishable well above the freezing transition. This finding indicates that an emergent slow mode is not unique to supercooled water, but may instead be a general feature of hydrogen-bonding liquids and associating molecular liquids.

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.

Order by disorder spin wave gap in the XY pyrochlore magnet Er2Ti2O7.

The recent determination of a robust spin Hamiltonian for the antiferromagnetic XY pyrochlore Er2Ti2O7 reveals a most convincing case of the "Order-by-Quantum-Disorder" mechanism for ground state selection. This mechanism relies on quantum fluctuations to remove an accidental symmetry of the magnetic ground state, and selects a particular ordered spin structure below TN=1.2 K. The removal of the continuous degeneracy results in an energy gap in the spectrum of spin wave excitations, long wavelength pseudo-Goldstone modes. We have measured the Order-by-Quantum-Disorder spin wave gap at a zone center in Er2Ti2O7, using low incident energy neutrons and the time-of-flight inelastic scattering method. We report a gap of Δ=0.053±0.006 meV, which is consistent with upper bounds placed on it from heat capacity measurements and roughly consistent with the theoretical estimate of ∼0.02 meV, further validating the spin Hamiltonian that led to that prediction. The gap is observed to vary with the square of the order parameter, and goes to zero for T∼TN.

Successive phase transitions and extended spin-excitation continuum in the S=1/2 triangular-lattice antiferromagnet Ba3CoSb2O9.

Using magnetic, thermal, and neutron measurements on single-crystal samples, we show that Ba3CoSb2O9 is a spin-1/2 triangular-lattice antiferromagnet with the c axis as the magnetic easy axis and two magnetic phase transitions bracketing an intermediate up-up-down phase in magnetic field applied along the c axis. A pronounced extensive neutron-scattering continuum above spin-wave excitations, observed below T(N), implies that the system is in close proximity to one of two spin-liquid states that have been predicted for a 2D triangular lattice.

Spin liquid state in the S = 1/2 triangular lattice Ba3CuSb2O9.

The synthesis and characterization of Ba3CuSb2O9, which has a layered array of Cu2+ spins in a triangular lattice, are reported. The magnetic susceptibility and neutron scattering experiments of this material show no magnetic ordering down to 0.2 K with a θ(CW) = -55 K. The magnetic specific heat reveals a T-linear dependence with a γ = 43.4 mJ K(-2) mol(-1) below 1.4 K. These observations suggest that Ba3CuSb2O9 is a new quantum spin liquid candidate with a S = 1/2 triangular lattice.

Chemical pressure induced spin freezing phase transition in kagome pr langasites.

The 2D kagome system Pr3Ga5SiO14 has been previously identified as a spin-liquid candidate in zero field, displaying no magnetic long-ranged order down to at least 35 mK. Perturbations upon such systems, either under applied fields or applied pressure, should induce a spin freezing phase transition, but there are very few experimental realizations of this phenomena other than the well-studied 3D pyrochlore Tb2Ti2O7. In this Letter, we report the observation of a spin freezing phase transition in Pr3Ga5SiO14 through the application of chemical pressure--that is, through a systematic substitution on the Si site with larger ions and an elongation of the nearest-neighbor Pr-Pr distance in the kagome lattice. This results in a suppression of the T2 component of the heat capacity, and the reduction of the exchange constant eventually leads to dipolar-driven spin freezing.

Itinerant spin excitations near the hidden order transition in URu(2)Si(2).

By means of neutron scattering we show that the high temperature precursor to the hidden order state of the heavy fermion superconductor URu(2)Si(2) exhibits heavily damped incommensurate paramagnons whose strong energy dispersion is very similar to that of the long-lived longitudinal f spin excitations that appear below T(0). This suggests that there is a strongly hybridized character to the itinerant excitations observed previously above the hidden order transition. Here we present evidence that the itinerant excitations, like those in chromium, are due to Fermi surface nesting of hole and electron pockets; hence the hidden order phase probably originates from a Fermi surface instability. We identify wavevectors that span nested regions of a f-d hybridized band calculation and that match the neutron spin crossover from incommensurate to commensurate on approach to the hidden order phase.

Two-dimensional kagome correlations and field induced order in the ferromagnetic XY pyrochlore Yb2Ti2O7.

Neutron scattering measurements show the ferromagnetic XY pyrochlore Yb2Ti2O7 to display strong quasi-two-dimensional (2D) spin correlations at low temperature, which give way to long range order (LRO) under the application of modest magnetic fields. Rods of scattering along 111 directions due to these 2D spin correlations imply a magnetic decomposition of the cubic pyrochlore system into decoupled kagome planes. A magnetic field of approximately 0.5 T applied along the [110] direction induces a transition to a 3D LRO state characterized by long-lived, dispersive spin waves. Our measurements map out a complex low temperature-field phase diagram for this exotic pyrochlore magnet.

Dynamic spin ice: Pr2Sn2O7.

In this Letter, we report a new spin ice--Pr2Sn2O7--which appears to have enhanced residual entropy due to the dynamic nature of the spins. Neutron scattering experiments show that at 200 mK, there is a significant amount of magnetic diffuse scattering which can be fit to the dipolar spin-ice model. However, these short-ranged ordered spins have a quasielastic response that is atypical of the canonical spin ices, and suggests that the ground state is dynamic (i.e., composed of locally ordered two-in-two-out spin configurations that can tunnel between energetically equivalent orientations). We report this as an example of a dynamic spin ice down to 200 mK.

Spin waves and quantum criticality in the frustrated XY pyrochlore antiferromagnet Er2Ti2O7.

We report detailed measurements of the low temperature magnetic phase diagram of Er2Ti2O7. Heat capacity and time-of-flight neutron scattering studies of single crystals reveal unconventional low-energy states. Er3+ magnetic ions reside on a pyrochlore lattice in Er2Ti2O7, where local XY anisotropy and antiferromagnetic interactions give rise to a unique frustrated system. In zero field, the ground state exhibits coexisting short and long-range order, accompanied by soft collective spin excitations previously believed to be absent. The application of finite magnetic fields tunes the ground state continuously through a landscape of noncollinear phases, divided by a zero temperature phase transition at micro{0}H{c} approximately 1.5 T. The characteristic energy scale for spin fluctuations is seen to vanish at the critical point, as expected for a second order quantum phase transition driven by quantum fluctuations.

Quantum oscillations of the total spin in a heterometallic antiferromagnetic ring: evidence from neutron spectroscopy.

Using inelastic neutron scattering and applied fields up to 11.4 T, we have studied the spin dynamics of the Cr7Ni antiferromagnetic ring in the energy window 0.05-1.6 meV. We demonstrate that the external magnetic field induces an avoided crossing (anticrossing) between energy levels with different total-spin quantum numbers. This corresponds to quantum oscillations of the total spin of each molecule. The inelastic character of the observed excitation and the field dependence of its linewidth indicate that molecular spins oscillate coherently for a significant number of cycles. Precise signatures of the anticrossing are also found at higher energy, where measured and calculated spectra match very well.

Comparative study of normal and branched alkane monolayer films adsorbed on a solid surface. II. Dynamics.

The dynamics of monolayer films of the n-alkane tetracosane (n-C24H52) and the branched alkane squalane (C30H62) adsorbed on graphite have been studied by quasielastic and inelastic neutron scattering and molecular dynamics (MD) simulations. Both molecules have 24 carbon atoms along their carbon backbone, and squalane has an additional six methyl side groups symmetrically placed along its length. The authors' principal objective has been to determine the influence of the side groups on the dynamics of the squalane monolayer and thereby assess its potential as a nanoscale lubricant. To investigate the dynamics of these monolayers they used both the disk chopper spectrometer (DCS) and the high flux backscattering spectrometer (HFBS) at the National Institute of Standards and Technology. These instruments made it possible to study dynamical processes such as molecular diffusive motions and vibrations on very different time scales: 1-40 ps (DCS) and 0.1-4 ns (HFBS). The MD simulations were done on corresponding time scales and were used to interpret the neutron spectra. The authors found that the dynamics of the two monolayers are qualitatively similar on the respective time scales and that there are only small quantitative differences that can be understood in terms of the different masses and moments of inertia of the two molecules. In the course of this study, the authors developed a procedure to separate out the low-frequency vibrational modes in the spectra, thereby facilitating an analysis of the quasielastic scattering. They conclude that there are no major differences in the monolayer dynamics caused by intramolecular branching. It remains to be seen whether this similarity in monolayer dynamics also holds for the lubricating properties of these molecules in confined geometries.

Partial field-induced magnetic order in the spin-liquid kagomé Nd3Ga5SiO14.

The distorted kagomé system Nd3Ga5SiO14 has been investigated with neutron scattering down to 0.046 K with no evidence of magnetic long range order of the Nd3+ moments in a zero field. Substantial diffuse scattering is observed which is in agreement with nearest-neighbor correlations between the fluctuating spins. Upon the application of a field in the c direction, the diffuse scattering is reduced in intensity while the magnetic Bragg peaks grow in intensity to saturate by 1 T to 1/2 of the expected magnetization. These measurements suggest that a unique spin-liquid state develops in Nd3Ga5SiO14 with a frustration index of f approximately |theta|/T_{C}> or =1300.

Field-induced order and spin waves in the pyrochlore antiferromagnet Tb2Ti207.

High resolution time-of-flight neutron scattering measurements on Tb(2)Ti(2)0(7) reveal a rich low temperature phase diagram in the presence of a magnetic field applied along [110]. In zero field at T = 0.4 K, Tb(2)Ti(2)0(7) is a highly correlated cooperative paramagnet with disordered spins residing on a pyrochlore lattice of corner-sharing tetrahedra. Application of a small field condenses much of the magnetic diffuse scattering, characteristic of the disordered spins, into a new Bragg peak characteristic of a polarized paramagnet. At higher fields, a magnetically ordered phase is induced, which supports spin wave excitations indicative of continuous, rather than Ising-like, spin degrees of freedom.

Nanomagnetic droplets and implications to orbital ordering in LA(1-x)Sr(x)CoO3.

Inelastic cold-neutron scattering on LaCoO3 provided evidence for a distinct low energy excitation at 0.6 meV coincident with the thermally induced magnetic transition. Coexisting strong ferromagnetic (FM) and weaker antiferromagnetic correlations that are dynamic follow the activation to the excited state, identified as the intermediate S = 1 spin triplet. This is indicative of dynamical orbital ordering favoring the observed magnetic interactions. With hole doping as in La(1-x)Sr(x)CoO3 , the FM correlations between Co spins become static and isotropically distributed due to the formation of FM droplets. The correlation length and condensation temperature of these droplets increase rapidly with metallicity due to the double exchange mechanism.