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1.
Most known non-radioactive pentafluorides have been examined by molecular-beam mass spectrometry and by the deflection of molecular beams in inhomogeneous electric fields. Extensive association of the vapors occurs for all but the lighter pentafluorides and the interhalogens. The interhalogen pentafluorides are strongly polar, consistent with the accepted C4v symmetry. The transition-metal and Group V pentafluorides are all non-polar, except VF5 and CrF5 for which temperature-dependent polarity is observed. However, uncertainty exists as to whether these observations are applicable to monomeric pentafluorides in all cases. Mass-spectral cracking patterns are presented for all species.  相似文献   
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The initial stages in the oxidation of magnesium, aluminium and magnesium/aluminium alloys have been studied using a photoelectron spectrometer (XPS and exoelectron energy spectra) and the diode technique (surface potentials and volumetric adsorption of oxygen). This paper describes and characterises the exoelectron emission and the visible wavelength photoemission which occurs during oxidation. At low oxygen exposures (< 10 L), exoelectrons with a 4 eV energy spread are emitted in the dark from magnesium and magnesium/aluminium alloy. Aluminium shows no such emission. Another, dark pressure-dependent emission of exoelectrons occurs only on magnesium/aluminium alloy and aluminium at high oxygen exposures. The onset of this emission lies 3 eV higher and it again has a 4 eV spread. When the surface is illuminated, it is possible to distinguish photo/exoelectron emission, which occurs during oxygen uptake, and true photoemission which occurs in vacuo. Both these types of emission, which were only recorded on magnesium, show a resolved triplet. Photoelectric work functions as low as 0.3 eV were observed. A patchy surface evidently develops during oxidation. This process, which may correspond to the nucleation of oxide islands, is slower than the chemisorption of of oxygen. The nature of the low work function patches, which we associate with the electron emissions, is therefore very dependent on the oxygen ambient pressure. A tentative energy scheme is given for such “exopatches” which are neither metal nor oxide and contain a curious energy level that must be situated above the vacuum level of the patch, as well as above the metal Fermi level. The energy with which exoelectrons are emitted derives from the heat of adsorption.  相似文献   
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The a- and b-type rotational transitions of the weakly bound complexes formed by molecular hydrogen and OCS, para-H2-OCS, ortho-H2-OCS, HD-OCS, para-D2-OCS, and ortho-D2-OCS, have been measured by Fourier transform microwave spectroscopy. All five species have ground rotational states with total rotational angular momentum J=0, regardless of whether the hydrogen rotational angular momentum is j=0 as in para-H2, ortho-D2, and HD or j=1 as in ortho-H2 and para-D2. This indicates quenching of the hydrogen angular momentum for the ortho-H2 and para-D2 species by the anisotropy of the intermolecular potential. The ground states of these complexes are slightly asymmetric prolate tops, with the hydrogen center of mass located on the side of the OCS, giving a planar T-shaped molecular geometry. The hydrogen spatial distribution is spherical in the three j=0 species, while it is bilobal and oriented nearly parallel to the OCS in the ground state of the two j=1 species. The j=1 species show strong Coriolis coupling with unobserved low-lying excited states. The abundance of para-H2-OCS relative to ortho-H2-OCS increases exponentially with decreasing normal H2 component in H2He gas mixtures, making the observation of para-H2-OCS in the presence of the more strongly bound ortho-H2-OCS dependent on using lower concentrations of H2. The determined rotational constants are A=22 401.889(4) MHz, B=5993.774(2) MHz, and C=4602.038(2) MHz for para-H2-OCS; A=22 942.218(6) MHz, B=5675.156(7) MHz, and C=4542.960(7) MHz for ortho-H2-OCS; A=15 970.010(3) MHz, B=5847.595(1) MHz, and C=4177.699(1) MHz for HD-OCS; A=12 829.2875(9) MHz, B=5671.3573(7) MHz, and C=3846.7041(6) MHz for ortho-D2-OCS; and A=13 046.800(3) MHz, B=5454.612(2) MHz, and C=3834.590(2) MHz for para-D2-OCS.  相似文献   
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Repeated methanolysis of [Zr(3)O](OPr(n)(10) followed by extraction and crystallization from toluene yields material that is X-ray crystallographically indistinguishable from the compound previously formulated as [Zr(13)O(8)](OMe)(36). Elemental analysis and (1)H solution NMR spectroscopy strongly suggest that this material is a mixture of methyltriskaidecazirconates (MTZ) [Zr(13)O(8)](OMe)(x)(OH)(36)(-)(x), x(av) approximately 20, that readily cocrystallize from hydrocarbon solution. These species have the metal-oxygen framework structure reported for [Zr(13)O(8)](OMe)(36), where the 13 zirconium and 32 bridging oxygen atoms comprise a fragment of the fluorite structure adopted by ZrO(2) at elevated temperatures. Ethanolysis of [Zr(3)O](OPr(n)(10) yields its ethyl analogue, [Zr(3)O](OEt)(10). Both trizirconates display temperature-dependent (1)H solution NMR spectra that are interpreted mechanistically in terms of rearrangement mechanisms involving trigonal twists at the octahedral zirconium centers.  相似文献   
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17O-NMR spectroscopy has found limited application as a structural probe due to the experimental problems associated with a quadrupolar nucleus having low natural abundance. A survey of data obtained from systematic studies of structurally related compounds shows, however, that large chemical shift differences are usually obtained for structurally nonequivalent nuclei, and that characteristic chemical shift values are observed for specific chemical environments. The present day availability of 17O enriched materials and Fourier transform NMR instrumentation should allow extensive application of the 17O-NMR technique to structural problems in the immediate future.  相似文献   
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The electronic structure of the azide ion is investigated using the SCF Xα scattered wave method. Calculated ionization energies are compared with values determined by electron spectroscopy. Transition state calculations for πg → π*u, σu → π*u and σg → π*u single electron transitions yield excitation energies near 5.7, 11.0, and 12.0 eV respectively.  相似文献   
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