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11.
Membrane fragments of Heliobacillus (Hc.) mobilis were characterized using resonance Raman (RR) spectroscopy in order to determine the configuration of the neurosporene carotenoid, the pigment-protein interactions of the bacteriochlorophyll (BChl) g molecules, and the Chl a-like chlorin pigments present in the antenna-reaction center complex constituting the photosynthetic apparatus. Using 363.8 nm excitation, the Raman contributions of the BChl g molecules were selectively resonantly enhanced over those of the carotenoid and the Chl a-like chlorin pigments. The RR spectrum of BChl g in these membranes excited at 363.8 nm exhibits bands at 1614 and 1688 cm?1, which correspond to a CaCm methine bridge stretching mode and a keto carbonyl group stretching mode, respectively. Both of these bands are 16 cm?1 wide (full width at half maximum, FWHM), indicating that a sole population of BChl g molecules is being enhanced at this excitation wavelength. The observed frequency of the CaCm stretching mode (1614 cm?1) indicates that the bulk of BChl g molecules is pentacoordinated with only one axial ligand to the central Mg atom while that of the keto carbonyl stretching mode (1668 cm?1) indicates that these groups are engaged in a hydrogen bond. This homogeneous population of BChl g molecules bound to the heliobacterial core polypeptides is in contrast to the heterogeneous population of Chl a molecules bound to the core polypeptides of the reaction center of photosystem I of Synechocystis 6803 as observed by the inhomogeneously broadened C9 keto carbonyl band in its RR spectrum. The RR spectrum of the Chl a-like chlorin pigments in Hc. mobilis excited at 441.6 nm exhibits a broad keto carbonyl band (43 cm?1 FWHM) with components at 1665, 1683 and 1695 cm?1, indicating several populations of these pigments differing in their protein interactions at the level of the keto carbonyl group. Fourier transform (FT) pre-RR spectroscopic measurements of intact whole cells and membrane fragments at room temperature using 1064 nm excitation indicate that high quality vibrational spectra of the BChl g molecules can be obtained with no photodegradation. Low-temperature FT Raman spectra excited at 1064 nm reveals an inhomogeneously broadened 1665 cm?1 band corresponding to the C9 keto carbonyl stretching mode. Spectral deconvolution and second derivative analysis of this band reveal that it is comprised of components at 1665, 1682 and 1695 cm?1, the latter two most likely arising from BChl g photoconversion products. Excitation using 885 nm to enhance the preresonance effect of the BChl g molecules yields an FT Raman spectrum where the keto carbonyl band at 1665 cm?1 is narrow, as is the case in the Soret RR spectra, reflecting a sole population of BChl g molecules, which are engaged in an H bond. The RR spectrum of the neurosporene molecule in Hc. mobilis membranes excited at 496.5 nm is compared to that of 1,2-dihydroneurosporene bound in a cis configuration in reaction centers of Rhodopseudomona viridis and to that of the same carotenoid in its all-trans configuration extracted from these reaction centers in the presence of light. The similarity of this latter RR spectrum with that of neurosporene in the Hc. mobilis membranes indicates that it is bound in an all-trans configuration. 相似文献
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UV.-irradiation of pivalic and isobutyric acid and their methyl esters as well as of α-hydroxy isobutyric and malonic acid in solution lead to chemically induced dynamic nuclear polarization (CIDNP.) of parent compounds and of various reaction products. CIDNP.-effects and product distributions confirm α-cleavage of the C(α), CO bond to be the major mode of photodecomposition. Scavenger experiments indicate that decomposition of the molecules from a triplet excited state is roughly equally or more probable than from a singlet excited state. Quantum yields of educt disappearance are also given for the methyl esters of pivalic and isobutyric acid. 相似文献
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The work function of hydrothermally synthesized UO2 and the implications for semiconductor device fabrication 下载免费PDF全文
Christopher Young James Petrosky J. Matthew Mann Eric M. Hunt David Turner Tony Kelly 《固体物理学:研究快报》2016,10(9):687-690
The photoelectric work function of nearly stoichiometric (111) and (100) hydrothermally grown UO2 was measured to be 6.28 ± 0.36 eV and 5.80 ± 0.36 eV, respectively. Candidate metals for electrical contacts are identified for both rectifying and non‐rectifying contacts based on work function, lattice compatibility, and electrical conductivity. 相似文献
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Seow Jecg Chin Peter Hornsby Damjan Vengust Dragan Mihailović J. Mitra Paul Dawson Tony McNally 《先进技术聚合物》2012,23(2):149-160
Composites of poly(ε‐caprolactone) (PCL) and molybdenum sulfur iodine (MoSI) nanowires were prepared using twin‐screw extrusion. Extensive microscopic examination of the composites revealed the nanowires were well dispersed in the PCL matrix, although bundles of Mo6S3I6 ropes were evident at higher loadings. Secondary electron imaging (SEI) showed the nanowires had formed an extensive network throughout the PCL matrix, resulting in increased electrical conductivity of PCL, by eight orders of magnitude, and an electrical percolation threshold of 6.5 × 10?3 vol%. Thermal analysis (DSC), WAXD, and hot stage polarized optical microscopy (HSPOM) experiments revealed Mo6S3I6 addition altered PCL crystallization kinetics, nucleation density, and crystalline content. A greater number of smaller spherulites were formed via heterogeneous nucleation. The onset of thermal decomposition (TGA) of PCL decreased by 70°C, a consequence of the thermal degradation of Mo6S3I6 to MoO3, which in turn accelerates the formation of volatile gases during the first stage of PCL decomposition. Copyright © 2010 John Wiley & Sons, Ltd. 相似文献
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Tony Chave Sergei I. Nikitenko Dominique Granier Thomas Zemb 《Ultrasonics sonochemistry》2009,16(4):481-487
Herein, we report the sonochemical reactions with MSU-X mesoporous alumina (m-Al2O3) in aqueous solutions. Sonication (f = 20 kHz, I = 30 W cm?2, Waq = 0.67 W mL?1, T = 36–38 °C, Ar) causes significant acceleration of m-Al2O3 dissolution in the pH range of 4–11. Moreover, power ultrasound has a dramatic effect on the textural properties and phase composition of m-Al2O3. Short-time sonication at pH = 4 leads to the formation of nanorods and nanofibers of boehmite, AlO(OH). Prolonged ultrasonic treatment causes high aspect morphology transformation to aggregated nanosheets in weakly acid solutions or plated nanocrystals in alkaline solutions. Sonochemical products in alkaline medium are composed principally from boehmite and small amounts of bayerite, Al(OH)3. Silent hydrolysis of m-Al2O3 yields boehmite at pH = 4 and bayerite at pH = 11. The effect of ultrasound on the textural properties of mesoporous alumina as well as on the transformation of nanosized bayerite to boehmite can be consistently attributed to the transient strong heating of the liquid shell surrounding the cavitation bubble which caused the chemical processes similar to those occurred during hydrothermal treatment. 相似文献
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