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71.
The electronic structures of a series of polythiaadamantanes from thiaadamantane through 2,4,6,8,9,10-hexathiaadamantane (HTA) have been analyzed using density functional theory calculations in conjunction with Hückel and natural bond orbital analysis. The effects of multiple sulfur p-type lone-pair orbital interactions on ionization potentials, hole mobilities, and electronic coupling have been determined. An overall increase in the average energy of the lone-pair orbitals as the number of sulfur atoms increases is predicted, with the exact positioning of the HOMO depending on specific lone-pair interactions. Separation of through-bond (TB) and through-space (TS) interactions between intramolecular sulfur atoms has been performed using localized molecular orbitals and model systems based on interacting hydrogen sulfide molecules. TB interations were found to reduce orbital splitting, while TS interactions were found to increase orbital splitting. TS interactions were more or less constant from one polythiaadamantane to the next, and the contributions of TB effects to individual orbital energies vary depending on the relative orientation of sulfur atoms as determined by the sigma molecular framework. Electronic coupling between intermolecular sulfur lone-pair orbitals was determined by investigating unique dimer pairs observed in the crystal structure of HTA. Electronic coupling is not as strong as expected given the short intermolecular S-S distances observed in the crystal structure. In general, B3LYP/6-31G(d) and B3LYP/6-311+G(d,p) give very similar orbital energies and splittings. 相似文献
72.
M. J. Petrasiunas E. W. Streed T. J. Weinhold B. G. Norton D. Kielpinski 《Applied physics. B, Lasers and optics》2012,107(4):1053-1059
The metastable 2F7/2 and 2D3/2 states of Yb+ are of interest for applications in metrology and quantum information and also act as dark states in laser cooling. These metastable states are commonly repumped to the ground state via the 638.6 nm 2F7/2–1D[5/2]5/2 and 935.2?nm 2D3/2–3D[3/2]1/2 transitions. We have performed optogalvanic spectroscopy of these transitions in Yb+ ions generated in a discharge. We measure the pressure broadening coefficient for the 638.6 nm transition to be 70±10?MHz?mbar?1. We place an upper bound of 375 MHz/nucleon on the 638.6 nm isotope splitting and show that our observations are consistent with theory for the hyperfine splitting. Our measurements of the 935.2 nm transition extend those made by Sugiyama et al., showing well-resolved isotope and hyperfine splitting (Sugiyama and Yoda in IEEE Trans. Instrum. Meas. 44: 140, 1995). We obtain high signal-to-noise, sufficient for laser stabilisation applications (Streed et al. in Appl. Phys. Lett. 93: 071103, 2008). 相似文献
73.
Norton M. Hintz 《Physics in Perspective (PIP)》2012,14(2):196-238
I sketch my life as an experimental nuclear physicist, beginning as a graduate student at Harvard University from 1948 to 1951, then as a postdoctoral fellow at the Cavendish Laboratory from 1951 to 1952, and finally as a faculty member at the University of Minnesota from 1952 until my retirement in 1991. I also carried out research at the Niels Bohr Institute in Copenhagen, Indiana University, and Los Alamos National Laboratory, and I participated in a number of summer schools and international conferences on nuclear physics. I also have worked in photography and opera. Over the years, I met and collaborated with many people in many walks of life who became friends for life. 相似文献
74.
The effect of surfactants' type and concentration on the interfacial tension and contact angle in the presence of hydrophilic silica particles was investigated. Silica particles have been shown to have an antagonistic effect on interfacial tension and contact angle in the presence of both W/O and O/W surfactants. Silica particles, combined with W/O surfactant, have no effect on interfacial tension, which is only dictated by the surfactant concentration, while they strongly affect interfacial tension when combined with O/W surfactants. At low O/W surfactant, both particles and surfactant are adsorbed at the interface, modifying the interface structure. At higher concentration, interfacial tension is only dictated by the surfactant. By increasing the surfactant concentration, the contact angle that a drop of aqueous phase assumes on a glass substrate placed in oil media decreases or increases depending on whether the surfactant is of W/O or O/W type, respectively. This is due to the modification of the wettability of the glass by the oil or water induced by the surfactants. Regardless of the surfactant's type, the contact angle profile was dictated by both particles and surfactant at low surfactant concentration, whereas it is dictated by the surfactant only at high concentration. 相似文献
75.
76.
The adhesion of a Mg:Ag cathode to the tris-(8-hydroxyquinoline) aluminum (Alq3) in organic light emitting devices (OLEDs) can be greatly enhanced by a remote plasma treatment of the Alq3 layer using either air or N2 prior to metal deposition. The altered surface properties which lead to increased sticking coefficients of Mg and Ag, as well as enhanced adhesion, are attributed to the introduction of new functional groups into the organic layer, as observed by X-ray photoelectron spectroscopy (XPS). The storage life of the plasma treated devices in air without any capping treatment, as judged by a visible deterioration of the cathode, was increased by approximately five to six times compared to untreated OLEDs. Current–voltage characteristics and EL efficiency, however, were shown to deteriorate for devices incorporating either an air or an N2 plasma treated Alq3 layer. For OLEDs subjected to short treatment times with an N2 plasma, only a very slight increase in the turn-on voltage, of about 0.2 V, was observed. An investigation of black spot formation revealed that an air plasma treatment resulted in a five-fold decrease in the time required for 50% of the device to become non-emissive. N2 treated devices on the other hand, developed black spots at a comparable rate to the non-treated devices. Thus, a short N2 plasma treatment of the Alq3 layer prior to metal deposition improves the adhesion at the interface, thereby reducing the oxidation and degradation of the device through exposure to ambient conditions, particularly in storage. 相似文献
77.
78.
79.
The cyclization of o-aminobenzoylhydrazine ( 1a ) and its 5-methyl derivative 1b with four equivalents and with one equivalent of triethyl orthoacetate (TEOA) was studied. 3-Amino-2-methyl-4(3H)-quinazolinone ( 2a ), 3,4-dihydro-2-methyl-5H-1,3,4-benzotriazepin-5-one ( 3a ) and an imino ether derivative of 2a , N-[2-methyl-4-oxo-3(4H)quinazolinyl]ethanimidic acid ethyl ester ( 4a ) were obtained from the reaction of 1a with four equivalents of TEOA. These results were compared with those of Merour [1] who isolated 2a and 3a using the same conditions. When 1a was treated with one equivalent of TEOA, 2a, 3a , and a new product, 2-(5-methyl-1,3,4-oxadiazol-2-yl)benzenamine ( 5a ) were produced, and 4a was not. Similar results were obtained with the reactions of 1b with TEOA. Authentic samples of oxadiazoles 5a and b were prepared by alternate routes. Novel acid-catalyzed rearrangements of benzotriazepinones 3a and b , to mixtures of aminoquinazolinones 2a and b and oxadiazoles 5a and b , respectively, were found. The different relative amounts of aminoquinazolinones 2 and oxadiazoles 5 which were produced from these rearrangements allowed us to choose between two potential mechanisms for these interesting rearrangements. Treatment of 5-nitrobenzoylhydrazine ( 37 ) with four equivalents of TEOA gave three products which were characterized, but did not lead to benzotriazepinone formation. 相似文献
80.
8-Hydroxyquinoline ( 9 ) was converted to 8 -aminequinoline ( 10 ) in a one-pot procedure involving alleviation with 2-bromo-2-methylpropionamide ( 2 ) followed by Smiles rearrangement and hydrolysis, in 41% yield. The scope and limitations of this new procedure were explored with additional hydroxyquinolines. 相似文献