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The crystal structure of Nb22O54 is reported for the first time, and the structure of orthorhombic Nb12O29 is reexamined, resolving previous ambiguities. Single crystal X-ray and electron diffraction were employed. These compounds were found to crystallize in the space groups P2/m (, , , β=102.029(3)°) and Cmcm (, , ), respectively and share a common structural unit, a 4×3 block of corner sharing NbO6 octahedra. Despite different constraints imposed by symmetry these blocks are very similar in both compounds. Within a block, it is found that the niobium atoms are not located in the centers of the oxygen octahedra, but rather are displaced inward toward the center of the block forming an apparent antiferroelectric state. Bond valence sums and bond lengths do not show the presence of charge ordering, suggesting that all 4d electrons are delocalized in these compounds at the temperature studied, T=200 K. 相似文献
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Smits R Warner N McQueen JM Cutler A 《The Journal of the Acoustical Society of America》2003,113(1):563-574
We present the results of a large-scale study on speech perception, assessing the number and type of perceptual hypotheses which listeners entertain about possible phoneme sequences in their language. Dutch listeners were asked to identify gated fragments of all 1179 diphones of Dutch, providing a total of 488,520 phoneme categorizations. The results manifest orderly uptake of acoustic information in the signal. Differences across phonemes in the rate at which fully correct recognition was achieved arose as a result of whether or not potential confusions could occur with other phonemes of the language (long with short vowels, affricates with their initial components, etc.). These data can be used to improve models of how acoustic-phonetic information is mapped onto the mental lexicon during speech comprehension. 相似文献
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The crystal structures of the triangular lattice, layered anhydrous alums KCr(SO4)2, RbCr(SO4)2 and KAl(SO4)2 are characterized by X-ray and neutron powder diffraction (NPD) at temperatures between 1.4 and 773 K. The compounds all crystallize in the space group , with octahedral coordination of the trivalent cations. In all cases, small amounts of disorder in the stacking of the triangular layers of corner sharing MO6 octahedra and SO4 tetrahedra is seen, with the MO6−SO4 network rotated in opposite directions between layers. The electron diffraction study of KCr(SO4)2 supports this model, which on an average can be taken to imply trigonal prismatic coordination for the M3+ ions; as was previously reported for the prototype anhydrous alum, KAl(SO4)2. The temperature-dependent magnetic susceptibilities for ACr(SO4)2 (A=K, Rb, Cs) indicate the presence of predominantly ferromagnetic interactions. Low-temperature powder neutron diffraction reveals that the magnetic ordering is ferromagnetic in-plane, with antiferromagnetic ordering between planes below 3 K. 相似文献
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The synthesis and characterization of the pyrochlore solid solutions, Y2Ti2−xNbxO7−y, Lu2Ti2−xNbxO7−y, Y2Ti2−xTaxO7−y and Lu2TiTaO7−y (−0.4<y<0.5), is described. Synthesis at 1600 °C, and 10−5 Torr yields oxygen deficiency in all systems. All compounds are found to be paramagnetic and semiconducting, with the size of the local moments being less, in some cases substantially less, than the expected value for the number of nominally unpaired electrons present. Thermogravimetric analysis (TGA) shows that all compounds can be fully oxidized while retaining the pyrochlore structure, yielding oxygen rich pyrochlores as white powders. Powder neutron diffraction of Y2TiNbO7-based samples was done. Refinement of the data for oxygen deficient Y2TiNbO6.76 indicates the presence of a distribution of oxygen over the 8b and 48f sites. Refinement of the data for oxygen rich Y2TiNbO7.5 shows these sites to be completely filled, with an additional half filling of the 8a site. The magnetic and TGA data strongly suggest a preference for a Ti3+/(Nb,Ta)5+ combination, as opposed to Ti4+/(Nb,Ta)4+, in this pyrochlore family. In addition, the evidence clearly points to Ti3+ as the source of the localized moments, with no evidence for localized Nb4+ moments. 相似文献
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Here, we study the nature of metal-metal bonding in the ThCr(2)Si(2) structure type by probing the rate-limiting steps in the oxidative deintercalation of KNi(2)Se(2). For low extents of oxidation, alkali ions are removed exclusively to form K(1-x)Ni(2)Se(2). For greater extents of oxidation, the rate of the reaction decreases dramatically, concomitant with the extraction of both potassium and nickel to form K(1-x)Ni(2-y)Se(2). The appreciable mobility of transition metal ions is unexpected, but illustrates the relative energy scales of different defects in the ThCr(2)Si(2) structure type. Furthermore, the fully oxidized compounds, K(0.25)Ni(1.5)Se(2), spontaneously convert from the tetrahedral [NiSe(4)]-containing ThCr(2)Si(2) structure to a vacancy-ordered NiAs structure with [NiSe(6)] octahedra. From analysis of the atom positions and kinetic data, we have determined that this transformation occurs by a continuous, low-energy pathway via subtle displacements of Ni atoms and buckling of the Se sublattice. These results have profound implications for our understanding of the stability, mobility, and reactivity of ions in materials. 相似文献