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71.
Xie BP Yang K Shen DW Zhao JF Ou HW Wei J Gu SY Arita M Qiao S Namatame H Taniguchi M Kaneko N Eisaki H Tsuei KD Cheng CM Vobornik I Fujii J Rossi G Yang ZQ Feng DL 《Physical review letters》2007,98(14):147001
In the present photoemission study of a cuprate superconductor Bi1.74Pb0.38Sr1.88CuO6+delta, we discovered a large scale dispersion of the lowest band, which unexpectedly follows the band structure calculation very well. Similar behavior observed in blue bronze and the Mott insulator Ca2CuO2Cl2 suggests that the origin of hopping-dominated dispersion in an overdoped cuprate might be quite complicated. A giant kink in the dispersion is observed, and the complete self-energy containing all interaction information is extracted for a doped cuprate. These results recovered significant missing pieces in our current understanding of the electronic structure of cuprates. 相似文献
72.
In order to resolve the long-standing issue of how itinerant ferromagnetism is affected by lattice structure and Hund's coupling, we compare various three-dimensional lattice structures in the single- and multiorbital Hubbard models with the dynamical mean-field theory with an improved quantum Monte Carlo algorithm that preserves the spin-SU(2) symmetry. The result indicates that both the lattice structure and the d-orbital degeneracy are essential for the ferromagnetism in the parameter region representing a transition metal. Specifically, (a) Hund's coupling, despite the common belief, is important, which is here identified to come from particle-hole scatterings, and (b) the ferromagnetism is a correlation effect (outside the Stoner picture) as indicated from the band-filling dependence. 相似文献
73.
74.
Palladium(0)/PAr3‐Catalyzed Intermolecular Amination of C(sp3)H Bonds: Synthesis of β‐Amino Acids 下载免费PDF全文
Jian He Toshihiko Shigenari Prof. Dr. Jin‐Quan Yu 《Angewandte Chemie (International ed. in English)》2015,54(22):6545-6549
An intermolecular C(sp3)? H amination using a Pd0/PAr3 catalyst was developed. The reaction begins with oxidative addition of R2N? OBz to a Pd0/PAr3 catalyst and subsequent cleavage of a C(sp3)? H bond by the generated Pd? NR2 intermediate. The catalytic cycle proceeds without the need for external oxidants in a similar manner to the extensively studied palladium(0)‐catalyzed C? H arylation reactions. The electron‐deficient triarylphosphine ligand is crucial for this C(sp3)? H amination reaction to occur. 相似文献
75.
Soh N Tanaka M Hirakawa K Zhang R Nakajima H Nakano K Imato T 《Analytical sciences》2011,27(11):1069-1076
Sequential injection immunoassay systems for environmental measurements based on the selective immunoreaction between antigen and antibody were described. A sequential injection analysis (SIA) technique is suitable to be applied for the procedure of enzyme-linked immunosorbent assay (ELISA), because the washing and the addition of reagent solutions can be automated by using a computer-controlled syringe pump and switching valve. We selected vitellogenin (Vg), which is a biomarker for evaluating environmental risk caused by endocrine-disrupting chemicals in the hydrosphere, and linear alkylbenzene sulfonates (LAS) and alkylphenol polyethoxylates (APEO), which are versatile surfactants, as target analytes in the flow immunoassay systems. For Vg monitoring, SIA systems based on spectrophotometric, chemiluminescence, and electrochemical determinations were constructed. On the other hand, chemiluminescence determination was applied to the detection of LAS and APEO. For APEO, an SIA system combined with surface plasmon resonance (SPR) sensor was also developed. These new sequential injection immunoassay systems are expected to be useful systems for environmental analysis. 相似文献
76.
Watanabe M Yamamoto T Yamamoto A Obana E Niiyama K Hada T Ooie T Kataoka M Hori T Houchi H Shinohara Y 《Applied biochemistry and biotechnology》2011,165(2):538-547
The thermogenic function of brown adipose tissue (BAT) is known to be markedly elevated when animals are exposed to the cold, and intensive studies have been carried out to understand the molecular basis enabling effective thermogenesis in cold-exposed animals. In this study, we used microarray analysis to examine the effects of cold exposure of animals on their gene expression profiles in white adipose tissue (WAT), which seems to function as a counterpart tissue of BAT. The results indicate that the effects of cold exposure on the gene expression profiles of WAT were much more moderate than the effects on those of BAT. Possible reasons for the different responses of BAT and WAT to cold exposure are discussed. 相似文献
77.
Ohyanagi T Nagahori N Shimawaki K Hinou H Yamashita T Sasaki A Jin T Iwanaga T Kinjo M Nishimura S 《Journal of the American Chemical Society》2011,133(32):12507-12517
Glycans are expected to be one of the potential signal molecules for controlling drug targeting/delivery or long-term circulation of biopharmaceuticals. However, the effect of the carbohydrates of artificially glycosylated derivatives on in vivo dynamic distribution profiles after intravenous injection of model animals remains unclear due to the lack of standardized methodology and a suitable platform. We report herein an efficient and versatile method for the preparation of multifunctional quantum dots (QDs) displaying common synthetic glycosides with excellent solubility and long-term stability in aqueous solution without loss of quantum yields. Combined use of an aminooxy-terminated thiol derivative, 11,11'-dithio bis[undec-11-yl 12-(aminooxyacetyl)amino hexa(ethyleneglycol)], and a phosphorylcholine derivative, 11-mercaptoundecylphosphorylcholine, provided QDs with novel functions for the chemical ligation of ketone-functionalized compounds and the prevention of nonspecific protein adsorption concurrently. In vivo near-infrared (NIR) fluorescence imaging of phosphorylcholine self-assembled monolayer (SAM)-coated QDs displaying various simple sugars (glyco-PC-QDs) after administration into the tail vein of the mouse revealed that distinct long-term delocalization over 2 h can be achieved in cases of QDs modified with α-sialic acid residue (Neu5Ac-PC-QDs) and control PC-QDs, while QDs bearing other common sugars, such as α-glucose (Glc-PC-QDs), α-mannose (Man-PC-QDs), α-fucose (Fuc-PC-QDs), lactose (Lac-PC-QDs), β-glucuronic acid (GlcA-PC-QDs), N-acetyl-β-D-glucosamine (GlcNAc-PC-QDs), and N-acetyl-β-D-galactosamine (GalNAc-PC-QDs) residues, accumulated rapidly (5-10 min) in the liver. Sequential enzymatic modifications of GlcNAc-PC-QDs gave Galβ1,4GlcNAc-PC-QDs (LacNAc-PC-QDs), Galβ1,4(Fucα1,3)GlcNAc-PC-QDs (Le(x)-PC-QDs), Neu5Acα2,3Galβ1,4GlcNAc-PC-QDs (sialyl LacNAc-PC-QDs), and Neu5Acα2,3Galβ1,4(Fucα1,3)GlcNAc-PC-QDs (sialyl Le(x)-PC-QDs) in quantitative yield as monitored by direct matrix-assisted laser desorption ionization time-of-flight mass spectrometry analyses. Live animal imaging uncovered for the first time that Le(x)-PC-QDs also distributed rapidly in the liver after intravenous injection and almost quenched over 1 h in similar profiles to those of LacNAc-PC-QDs and Lac-PC-QDs. On the other hand, sialyl LacNAc-PC-QDs and sialyl Le(x)-PC-QDs were still retained stably in the whole body after 2 h, while they showed significantly different in vivo dynamics in the tissue distribution, suggesting that structure/sequence of the neighboring sugar residues in the individual sialyl oligosaccharides might influence the final organ-specific distribution. The present results clearly visualize the evidence of an essential role of the terminal sialic acid residue(s) for achieving prolonged in vivo lifetime and biodistribution of various glyco-PC-QDs as a novel class of functional platforms for nanomaterial-based drug targeting/delivery. A standardized protocol using multifunctional PC-QDs should facilitate live animal imaging of ligand-displayed QDs using versatile NIR fluorescence photometry without influence of size-dependent accumulation/excretion pathway for nanoparticles (e.g., viruses) >10 nm in hydrodynamic diameter by the liver. 相似文献
78.
Urita K Shiga Y Fujimori T Iiyama T Hattori Y Kanoh H Ohba T Tanaka H Yudasaka M Iijima S Moriguchi I Okino F Endo M Kaneko K 《Journal of the American Chemical Society》2011,133(27):10344-10347
An outstanding compression function for materials preparation exhibited by nanospaces of single-walled carbon nanohorns (SWCNHs) was studied using the B1-to-B2 solid phase transition of KI crystals at 1.9 GPa. High-resolution transmission electron microscopy and synchrotron X-ray diffraction examinations provided evidence that KI nanocrystals doped in the nanotube spaces of SWCNHs at pressures below 0.1 MPa had the super-high-pressure B2 phase structure, which is induced at pressures above 1.9 GPa in bulk KI crystals. This finding of the supercompression function of the carbon nanotubular spaces can lead to the development of a new compression-free route to precious materials whose syntheses require the application of high pressure. 相似文献
79.
Nagata T Fedorov DG Sawada T Kitaura K Gordon MS 《The Journal of chemical physics》2011,134(3):034110
The gradient for the fragment molecular orbital (FMO) method interfaced with effective fragment potentials (EFP), denoted by FMO∕EFP, was developed and applied to polypeptides solvated in water. The structures of neutral and zwitterionic tetraglycine immersed in water layers of 2.0, 2.5, 3.0, 3.5, 4.0, and 4.5 A? are investigated by performing FMO∕EFP geometry optimizations at the RHF∕cc-pVDZ level of theory for the solutes. The geometries optimized with FMO-RHF∕EFP are compared to those from the conventional RHF∕EFP and are found to be in very close agreement. Using the optimized geometries, the stability of the hydrated zwitterionic and neutral structures is discussed structurally and in terms of energetics at the second-order M?ller-Plesset theory (MP2)∕cc-pVDZ level. To demonstrate the potential of the method for proteins, the geometry of hydrated chignolin (protein data bank ID: 1UAO) was optimized, and the importance of the inclusion of water was examined by comparing the solvated and gas phase structures of chignolin with the experimental NMR structure. 相似文献
80.
The fragmentation pathways of six triterpenoid saponins from Glycyrrhiza radix were investigated using LC-MS/MS. Depending on the structure and the substitution pattern, different molecular adduct ions, [M+NH4]+ or [M+H]+, were observed in the positive ESI spectra. In the positive MSn spectra from the molecular adduct ions, characteristic product ions corresponding to the loss of dehydrated glucuronic acid or glucuronic acid were detected and they indicated the type of substitution and structural modification. Fragment ions originating from the sapogenin moiety in the positive mass spectra were predominantly provided by saponins having an 11-oxo-12-ene structure. On the other hand, the saponins gave fragment ions corresponding to the sugar moiety in the negative mass spectra. These results indicate the specific property of saponins that have the 11-oxo-12-ene structure to localize positive or negative charge in the mass spectrometric ionization and fragmentation process. Information obtained from the present study can be utilized for structural elucidation of triterpenoid saponins in the Glycyrrhiza radix by LC-MS. 相似文献