Phonon Density of States and Anharmonicity of UO2

Phonon density of states (PDOS) measurements have been performed on polycrystalline UO2 at 295 and 1200 K using time-of-flight inelastic neutron scattering to investigate the impact of anharmonicity on the vibrational spectra and to benchmark ab initio PDOS simulations performed on this strongly correlated Mott-insulator. Time-of-flight PDOS measurements include anharmonic linewidth broadening inherently and the factor of ~ 7 enhancement of the oxygen spectrum relative to the uranium component by the neutron weighting increases sensitivity to the oxygen-dominated optical phonon modes. The first-principles simulations of quasi-harmonic PDOS spectra were neutron-weighted and anharmonicity was introduced in an approximate way by convolution with wavevector-weighted averages over our previously measured phonon linewidths for UO2 that are provided in numerical form. Comparisons between the PDOS measurements and the simulations show reasonable agreement overall, but they also reveal important areas of disagreement for both high and low temperatures. The discrepancies stem largely from an ~ 10 meV compression in the overall bandwidth (energy range) of the oxygen-dominated optical phonons in the simulations. A similar linewidth-convoluted comparison performed with the PDOS spectrum of Dolling et al. obtained by shell-model fitting to their historical phonon dispersion measurements shows excellent agreement with the time-of-flight PDOS measurements reported here. In contrast, we show by comparisons of spectra in linewidth-convoluted form that recent first-principles simulations for UO2 fail to account for the PDOS spectrum determined from the measurements of Dolling et al. These results demonstrate PDOS measurements to be stringent tests for ab initio simulations of phonon physics in UO2 and they indicate further the need for advances in theory to address lattice dynamics of UO2.Comment: Text slightly modified, results unchange

Emergent Spin Topology in Cuprate Superconductors Seen with Neutrons

Peer reviewed: YesNRC publication: Ye

Gapped itinerant spin excitations account for missing entropy in the hidden-order state of URu2Si2

Many correlated electron materials, such as high-temperature superconductors1, geometrically frustrated oxides2 and low-dimensional magnets3, 4, are still objects of fruitful study because of the unique properties that arise owing to poorly understood many-body effects. Heavy-fermion metals5\u2014materials that have high effective electron masses due to those effects\u2014represent a class of materials with exotic properties, ranging from unusual magnetism, unconventional superconductivity and 'hidden' order parameters6. The heavy-fermion superconductor URu2Si2 has held the attention of physicists for the past two decades owing to the presence of a 'hidden-order' phase below 17.5 K. Neutron scattering measurements indicate that the ordered moment is 0.03muB, much too small to account for the large heat-capacity anomaly at 17.5 K. We present recent neutron scattering experiments that unveil a new piece of this puzzle\u2014the 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 large entropy change associated with the presence of an energy gap in the excitations explains the reduction in the electronic specific heat through the transition.NRC publication: Ye