arXiv subjects

W. J. L. Buyers

Publications and source records attributed to W. J. L. Buyers.

At least 19 recordsLinked to original sources

arXiv2018

Disentangling orbital and spin exchange interactions for Co$^{2+}$ on a rocksalt lattice

Neutron spectroscopy was applied to study the magnetic interactions of orbitally degenerate Co$^{2+}$ on a host MgO rocksalt lattice where no long range spin or orbital order exists. The paramagnetic nature of the substituted monoxide Co$_{0.03}$Mg$_{0.97}$O allows for the disentanglement of spin-exchange and spin-orbit interactions. By considering the prevalent excitations from Co$^{2+}$ spin pairs, we extract 7 exchange constants out to the fourth coordination shell. An antiferromagnetic next nearest neighbor 180$^{\circ}$ exchange interaction is dominant, however dual ferromagnetic and antiferromagnetic interactions are observed for pairings with other pathways. These interactions can be understood in terms of a combination of orbital degeneracy in the $t_{2g}$ channel and the Goodenough-Kanamori-Anderson (GKA) rules. Our work suggests that such a hierarchy of exchange interactions exists in transition metal-based oxides with a $t_{2g}$ orbital degeneracy.

cond-mat.str-el↗

arXiv2017

Early experimental evidence of a topological quantum state: The signature of the Haldane ground state revealed by scattered neutrons

Neutron scattering played an important role in the experimental exploration of the theoretical ideas of Thouless, Haldane, and Kosterlitz, who won the Nobel Prize in Physics in 2016. This article reviews the signatures of Haldane's predicted topological quantum ground state and their observation in early neutron scattering experiments, which overturned the wisdom of the day.

cond-mat.str-el↗

arXiv2017

Gapped Excitations in the High-Pressure Antiferromagnetic Phase of URu$_2$Si$_2$

We report a neutron scattering study of the magnetic excitation spectrum in each of the three temperature and pressure driven phases of URu$_2$Si$_2$. We find qualitatively similar excitations throughout the (H0L) scattering plane in the hidden order and large moment phases, with no changes in the $\hbarω$-widths of the excitations at the $Σ$ = (1.407,0,0) and $Z$ = (1,0,0) points, within our experimental resolution. There is, however, an increase in the gap at the $Σ$ point from 4.2(2) meV to 5.5(3) meV, consistent with other indicators of enhanced antiferromagnetism under pressure.

cond-mat.str-el↗

arXiv2015

Light atom quantum oscillations in UC and US

High energy vibrational scattering in the binary systems UC and US is measured using time-of-flight inelastic neutron scattering. A clear set of well-defined peaks equally separated in energy is observed in UC, corresponding to harmonic oscillations of the light C atoms in a cage of heavy U atoms. The scattering is much weaker in US and only a few oscillator peaks are visible. We show how the difference between the materials can be understood by considering the neutron scattering lengths and masses of the lighter atoms. Monte Carlo ray tracing is used to simulate the scattering, with near quantitative agreement with the data in UC, and some differences with US. The possibility of observing anharmonicity and anisotropy in the potentials of the light atoms is investigated in UC. Overall the observed data is well accounted for by considering each light atom as a single atom isotropic quantum harmonic oscillator.

cond-mat.mtrl-sci↗

arXiv2015

Separation of magnetic and superconducting behaviour in YBCO6.33 (Tc=8.4 K)

Neutron scattering from high-quality YBa2Cu3O6.33 (YBCO6.33) single crystals with a Tc of 8.4 K shows no evidence of a coexistence of superconductivity with long-range antiferromagnetic order at this very low, near-critical doping of p~0.055. However, we find short-range three dimensional spin correlations that develop at temperatures much higher than Tc. Their intensity increases smoothly on cooling and shows no anomaly that might signify a Neel transition. The system remains subcritical with spins correlated over only one and a half unit cells normal to the planes. At low energies the short-range spin response is static on the microvolt scale. The excitations out of this ground state give rise to an overdamped spectrum with a relaxation rate of 3 meV. The transition to the superconducting state below Tc has no effect on the spin correlations. The elastic interplanar spin response extends over a length that grows weakly but fails to diverge as doping is moved towards the superconducting critical point. Any antiferromagnetic critical point likely lies outside the superconducting dome. The observations suggest that conversion from Neel long-range order to a spin glass texture is a prerequisite to formation of paired superconducting charges. We show that while pc =0.052 is a critical doping for superconducting pairing, it is not for spin order.

cond-mat.supr-con↗

arXiv2014

Strict limit on in-plane ordered magnetic dipole moment in URu2Si2

Neutron diffraction is used to examine the polarization of weak static antiferromagnetism in high quality single crystalline URu2Si2. As previously documented, elastic Bragg-like diffraction develops for temperature T<T_{HO}= 17.5 K at q=(100) but not at wave vector transfer q=(001). The peak width indicates correlation lengths ξ_c=230(12) Å\ and ξ_a=240(15) Å. The integrated intensity of the T-dependent peaks corresponds to a sample averaged c-oriented staggered moment of μ_{c}=0.022(1) μ_B at T=1.7 K. The absence of T-dependent diffraction at q=(001) places a limit μ_{\perp}<0.0011 μ_B on an f- or d-orbital based in-plane staggered magnetic dipole moment, which is associated with multipolar orders proposed for URu_2Si_2.

cond-mat.str-el↗

arXiv2013

Magnon breakdown in a two dimensional triangular lattice Heisenberg antiferromagnet of multiferroic LuMnO$_3$

The breakdown of magnons, the quasiparticles of magnetic systems, has rarely been seen. By using an inelastic neutron scattering technique we report the observation of spontaneous magnon decay in multiferroic LuMnO$_3$, a simple two-dimensional Heisenberg triangular lattice antiferromagnet, with large spin, S = 2. The origin of this rare phenomenon lies in the non-vanishing cubic interaction between magnons in the spin Hamiltonian arising from the noncollinear 120$^o$ spin structure. We observed all three key features of the nonlinear effects as theoretically predicted: a roton-like minimum, a flat mode, and a linewidth broadening, in our inelastic neutron scattering measurements of single crystal LuMnO$_3$. Our results show that quasiparticles in a system hitherto thought of as "classical" can indeed break down.

cond-mat.str-el↗

arXiv2013

Neutron scattering measurements of $dd$ and spin-orbit excitations below the Mott-Hubbard gap in CoO

Neutron scattering is used to investigate the single-ion spin and orbital excitations below the Mott-Hubbard gap in CoO. Three excitations are reported at 0.870 $\pm$ 0.009 eV, 1.84 $\pm$ 0.03, and 2.30 $\pm$ 0.15 eV. These were parameterized within a weak crystal field scheme with an intra-orbital exchange of $J(dd)$=1.3 $\pm$ 0.2 eV and a crystal field splitting 10Dq=0.94 $\pm$ 0.10 eV. A reduced spin-orbit coupling of λ=-0.016 $\pm$ 0.003 eV is derived from dilute samples of Mg$_{0.97}$Co$_{0.03}$O, measured to remove complications due to spin exchange and structural distortion parameters which split the cubic phase degeneracy of the orbital excitations complicating the inelastic spectrum. The 1.84 eV, while reported using resonant x-ray and optical techniques, was absent or weak for non resonant x-ray experiments and overlaps with the expected position of a $^{4}A_{2}$ level. This transition is absent in the dipolar approximation but expected to have a finite quadrupolar matrix element that can be observed with neutron scattering techniques at larger momentum transfers. Our results agree with a crystal field analysis (in terms of Racah parameters and Tanabe-Sugano diagrams) and with previous calculations performed using local-density band theory for Mott insulating transition metal oxides. The results also demonstrate the use of neutron scattering for measuring dipole forbidden transitions in transition metal oxide systems.

cond-mat.str-el↗

arXiv2012

Neutron Scattering Study of URu$_{2-x}$Re$_x$Si$_2$ with $x$ = 0.10: Driving Order towards Quantum Criticality

We report inelastic neutron scattering measurements in the hidden order state of URu$_{2-x}$Re$_x$Si$_2$ with $x$ = 0.10. We observe that towards the ferromagnetic quantum critical point induced by the negative chemical pressure of Re-doping, the gapped incommensurate fluctuations are robust and comparable in intensity to the parent material. As the Re doping moves the system toward the quantum critical point, the commensurate spin fluctuations related to hidden order weaken, display a shortened lifetime and slow down. Halfway to the quantum critical point, the hidden order phase survives, albeit weakened, in contrast to its destruction by hydrostatic pressure and by positive chemical pressure from Rh-doping.

cond-mat.str-el↗

arXiv2012

Quantum oscillations of nitrogen atoms in uranium nitride

The vibrational excitations of crystalline solids corresponding to acoustic or optic one phonon modes appear as sharp features in measurements such as neutron spectroscopy. In contrast, many-phonon excitations generally produce a complicated, weak, and featureless response. Here we present time-of-flight neutron scattering measurements for the binary solid uranium nitride (UN), showing well-defined, equally-spaced, high energy vibrational modes in addition to the usual phonons. The spectrum is that of a single atom, isotropic quantum harmonic oscillator and characterizes independent motions of light nitrogen atoms, each found in an octahedral cage of heavy uranium atoms. This is an unexpected and beautiful experimental realization of one of the fundamental, exactly-solvable problems in quantum mechanics. There are also practical implications, as the oscillator modes must be accounted for in the design of generation IV nuclear reactors that plan to use UN as a fuel.

cond-mat.mtrl-sci↗

arXiv2012

Zn-induced spin dynamics in overdoped La$_{2-x}$Sr$_x$Cu$_{1-y}$Zn$_y$O$_4$

Spin fluctuations and the local spin susceptibility in isovalently Zn-substituted La$_{2-x}$Sr$_{x}$Cu$_{1-y}$Zn$_y$O$_4$ ($x=0.25$, $y\approx0.01$) are measured via inelastic neutron scattering techniques. As Zn$^{2+}$ is substituted onto the Cu$^{2+}$-sites, an anomalous enhancement of the local spin susceptibility $χ^{\prime\prime}(ω)$ appears due to the emergence of a commensurate antiferromagnetic excitation centered at wave vector \textbf{Q}$=(π, π, 0)$ that coexists with the known incommensurate SDW excitations at \textbf{Q}$_{HK}=(π\pmδ,π), (π,π\pmδ)$. Our results support a picture of Zn-induced antiferromagnetic (AF) fluctuations appearing through a local staggered polarization of Cu$^{2+}$-spins, and the simultaneous suppression of T$_c$ as AF fluctuations are slowed in proximity to Zn-impurities suggests the continued importance of high energy AF fluctuations at the far overdoped edge of superconductivity in the cuprates.

cond-mat.supr-con↗

arXiv2010

The effect of the pseudogap on suppressing high energy inelastic neutron scattering in superconducting YBa2Cu3O6.5

We have measured the spin fluctuations in the YBa2Cu3O6.5 (YBCO6.5, Tc=59 K) superconductor at high-energy transfers above ~ 100 meV. Within experimental error, the momentum dependence is isotropic at high-energies, similar to that measured in the insulator for two dimensional spin waves, and the dispersion extrapolates back to the incommensurate wave vector at the elastic position. This result contrasts with previous expectations based on measurements around 50 meV which were suggestive of a softening of the spin-wave velocity with increased hole doping. Unlike the insulator, we observe a significant reduction in the intensity of the spin excitations for energy transfers above ~ 100 meV similar to that observed above ~ 200 meV in the YBCO6.35 (Tc=18 K) superconductor as the spin waves approach the zone boundary. We attribute this high energy scale with a second gap and find agreement with measurements of the pseudogap in the cuprates associated with electronic anomalies along the antinodal positions. In addition, we observe a sharp peak at around 400 meV whose energy softens with increased hole doping. We discuss possible origins of this excitation including a hydrogen related molecular excitation and a transition of electronic states between d levels.

cond-mat.supr-con↗

arXiv2010

Magnetic excitations of spin and orbital moments in cobalt oxide

Magnetic and phonon excitations in the antiferromagnet CoO with an unquenched orbital angular momentum are studied by neutron scattering. Results of energy scans in several Brillouin zones in the (HHL) plane for energy transfers up to 16 THz are presented. The measurements were performed in the antiferromagnetic ordered state at 6 K (well below TN~290 K) as well as in the paramagnetic state at 450 K. Several magnetic excitation modes are identified from the dependence of their intensity on wavevector and temperature. Within a Hund's rule model the excitations correspond to fluctuations of coupled orbital and spin degrees of freedom whose bandwidth is controlled by interionic superexchange. The different <111> ordering domains give rise to several magnetic peaks at each wavevector transfer.

cond-mat.str-el↗

arXiv2009

Magnetic field resonantly enhanced free spins in underdoped YBa$_{2}$Cu$_{3}$O$_{6+x}$

Using neutron scattering, we investigate the effect of a magnetic field on the static and dynamic spin response in heavily underdoped superconducting YBa$_{2}$Cu$_{3}$O$_{6+x}$ (YBCO$_{6+x}$) with x=0.33 (T$_{c}$=8 K) and 0.35 (T$_{c}$=18 K). In contrast to the heavily doped and superconducting monolayer cuprates, the elastic central peak characterizing static spin correlations does not respond observably to a magnetic field which suppresses superconductivity. Instead, we find a magnetic field induced resonant enhancement of the spin fluctuations. The energy scale of the enhanced fluctuations matches the Zeeman energy within both the normal and vortex phases while the momentum dependence is the same as the zero field bilayer response. The magnitude of the enhancement is very similar in both phases with a fractional intensity change of $(I/I_{0}-1) \sim 0.1$. We suggest that the enhancement is not directly correlated with superconductivity but is the result of almost free spins located near hole rich regions.

cond-mat.supr-con↗

arXiv2008

Itinerant spin excitations near the hidden order transition in URu2Si2

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$_{0}$. Since the underlying local f-exchange is preserved we expect only the f-d interactions to change across the phase transition and to cause the paramagnetic damping. The damping exhibits single-ion behavior independent of wave vector and vanishes below the hidden order transition. We suggest that this arises from a transition from valence fluctuations to a hybridized f-d state below T$_{0}$. Here we present evidence that the itinerant excitations, like those in chromium, are due to Fermi surface nesting of hole and electron pockets so that the hidden order phase likely originates from a Fermi-surface instability. We identify wave vectors that span nested regions of a band calculation and that match the neutron spin crossover from incommensurate to commensurate on approach to the hidden order phase.

cond-mat.str-el↗

arXiv2008

Incommensurate Spin Ordering and Fluctuations in underdoped La_{2-x}Ba_{x}CuO_{4}

Using neutron scattering techniques, we have studied incommensurate spin ordering as well as low energy spin dynamics in single crystal underdoped \LBCO with x$\sim$0.095 and 0.08; high temperature superconductors with T$_C \sim$ 27 K and 29 K respectively. Static two dimensional incommensurate magnetic order appears below T$_N$=39.5 $\pm$ 0.3 K in \LBCO (x=0.095) and a similar temperature for x=0.08 within the low temperature tetragonal phase. The spin order is unaffected by either the onset of superconductivity or the application of magnetic fields of up to 7 Tesla applied along the c-axis in the x=0.095 sample. Such magnetic field {\it independent} behaviour is in marked contrast with the field induced enhancement of the staggered magnetisation observed in the related \LSCO system, indicating this phenomenon is not a universal property of cuprate superconductors. Surprisingly, we find that incommensurability $δ$ is only weakly dependent on doping relative to \LSCO. Dispersive excitations in \LBCO (x=0.095) at the same incommensurate wavevector persist up to at least 60 K. The dynamical spin susceptibility of the low energy spin excitations saturates below \tc, in a similar manner to that seen in the superconducting state of La$_2$CuO$_{4+y}$.

cond-mat.supr-con↗

arXiv2008

Spin dynamics near the critical doping in weakly-superconducting underdoped YBa2Cu3O6.35 (Tc=18K)

Using neutron scattering we have determined the magnetic structure and fluctuations in the YBa2Cu3O6.35 superconductor (Tc=18 K). The long-range ordered collinear spins of the insulating antiferromagnet are replaced by a commensurate central mode arising from slow, isotropically polarized, short-range spin correlations. The inelastic spectrum up to 30 meV is broad in wave vector and commensurate. In contrast to the the resonance peak of higher Tc superconductors, the spins exhibit a single overdamped spectrum whose rate of relaxation decreases on cooling and saturates at 5 meV below 50 K. As the relaxation rate saturates the quasi-static spin correlations grow and become resolution limited in energy. The spin susceptibility at high temperatures illustrates that the dominant energy scale is set by the temperature. At low temperatures, the scale length is geometric and not linked by velocity to dynamic widths. There is no observable suppression of the spin fluctuations or central mode upon the onset of superconductivity. The spins respond not to coherent charge pairs but to hole doping allowing coexistence of glassy short range spin order with superconductivity. Since the physics of the weakly superconducting system YBCO6.35 must connect continuously with that in more strongly superconducting YBCO6.5, we find that neither incommensurate stripe-like spin modulations nor a well-defined neutron spin resonance are essential for the onset with doping of pairing in a high temperature cuprate superconductor.

cond-mat.supr-con↗

arXiv2007

Gapped itinerant spin excitations account for missing entropy in the hidden order state of URu$_2$Si$_2$

One of the primary goals of modern condensed matter physics is to elucidate the nature of the ground state in various electronic systems. Many correlated electron materials, such as high temperature superconductors, geometrically frustrated oxides, and low-dimensional magnets are still the objects of fruitful study because of the unique properties which arise due to poorly understood many-body effects. Heavy fermion metals - materials which have high effective electron masses due to these effects - represent a class of materials with exotic properties, such as unusual magnetism, unconventional superconductivity, and "hidden order" parameters. The heavy fermion superconductor URu2Si2 has held the attention of physicists for the last two decades due to the presence of a "hidden order" phase below 17.5 K. Neutron scattering measurements indicate that the ordered moment is 0.03 $μ_{B}$, much too small to account for the large heat capacity anomaly at 17.5 K. We present recent neutron scattering experiments which unveil a new piece of this puzzle - the spin excitation spectrum above 17.5 K exhibits well-correlated, itinerant-like spin excitations up to at least 10 meV emanating from incommensurate wavevectors. The gapping of these excitations corresponds to a large entropy release and explains the reduction in the electronic specific heat through the transition.

cond-mat.str-el↗