54 research outputs found
Cubic lead perovskite PbMoO3 with anomalous metallic behavior
A previously unreported Pb-based perovskite PbMoO is obtained by
high-pressure and high-temperature synthesis. This material crystallizes in the
cubic structure at room temperature, making it distinct from
typical Pb-based perovskite oxides with a structural distortion. PbMoO
exhibits a metallic behavior down to 0.1 K with an unusual -sub linear
dependence of the electrical resistivity. Moreover, a large specific heat is
observed at low temperatures accompanied by a peak in around 10 K, in
marked contrast to the isostructural metallic system SrMoO. These transport
and thermal properties for PbMoO, taking into account anomalously large Pb
atomic displacements detected through diffraction experiments, are attributed
to a low-energy vibrational mode, associated with incoherent off-centering of
lone pair Pb cations. We discuss the unusual behavior of the electrical
resistivity in terms of a polaron-like conduction, mediated by the strong
coupling between conduction electrons and optical phonons of the local
low-energy vibrational mode.Comment: 5 pages, 5 figure
Ultrafast Vibrational Dynamics of Water Disentangled by Reverse Nonequilibrium Ab Initio Molecular Dynamics Simulations
Water is a unique solvent with strong, yet highly dynamic, intermolecular interactions. Many insights into this distinctive liquid have been obtained using ultrafast vibrational spectroscopy of water’s O-H stretch vibration. However, it has been challenging to separate the different contributions to the dynamics of the O-H stretch vibration in H_{2}O. Here, we present a novel nonequilibrium molecular dynamics (NEMD) algorithm that allows for a detailed picture of water vibrational dynamics by generating nonequilibrium vibrationally excited states at targeted vibrational frequencies. Our ab initio NEMD simulations reproduce the experimentally observed time scales of vibrational dynamics in H_{2}O. The approach presented in this work uniquely disentangles the effects on the vibrational dynamics of four contributions: the delocalization of the O-H stretch mode, structural dynamics of the hydrogen bonded network, intramolecular coupling within water molecules, and intermolecular coupling between water molecules (near-resonant energy transfer between O-H groups). Our results illustrate that intermolecular energy transfer and the delocalization of the O-H stretch mode are particularly important for the spectral diffusion in H_{2}O
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