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101.
The rotation of the carboxylate groups in DOTA (DOTA = 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetate) complexes of several lanthanide ions and Sc(3+) was investigated with density functional theory (DFT) calculations and with variable temperature (17)O NMR studies at 4.7-18.8 T. The data obtained show that the rotation is much slower than the other dynamic processes taking place in these complexes. The exchange between the bound and unbound carboxylate oxygen atoms for the largest Ln(3+) ions (La(3+)→Sm(3+)) follows a pathway via a transition state in which both oxygens of the carboxylate group are bound to the Ln(3+) ion, whereas for the smaller metal ions (Tm(3+), Lu(3+), Sc(3+)) the transition state has a fully decoordinated carboxylate group. The activation free energies show a steady increase from about 75 to 125-135 kJ·mol(-1) going from La(3+) to Lu(3+). This computed trend is consistent with the results of the (17)O NMR measurements. Fast exchange between bound and unbound carboxylate oxygen atoms was observed for the diamagnetic La-DOTA, whereas for Pr-, Sm-, Lu-, and Sc-DOTA the exchange was slow on the NMR time scale. The trends in the linewidths for the various metal ions as a function of the temperature agree with trends in the rates as predicted by the DFT calculations. 相似文献
102.
Offermann DA McKendrick JE Sejberg JJ Mo B Holdom MD Helm BA Leatherbarrow RJ Beavil AJ Sutton BJ Spivey AC 《The Journal of organic chemistry》2012,77(7):3197-3214
The disruption of the human immunolobulin E-high affinity receptor I (IgE-FcεRI) protein-protein interaction (PPI) is a validated strategy for the development of anti asthma therapeutics. Here, we describe the synthesis of an array of conformationally constrained cyclic peptides based on an epitope of the A-B loop within the Cε3 domain of IgE. The peptides contain various tolan (i.e., 1,2-biarylethyne) amino acids and their fully and partially hydrogenated congeners as conformational constraints. Modest antagonist activity (IC(50) ~660 μM) is displayed by the peptide containing a 2,2'-tolan, which is the one predicted by molecular modeling to best mimic the conformation of the native A-B loop epitope in IgE. 相似文献
103.
Maxwell D. Cummings Tse‐I Lin Lili Hu Abdellah Tahri David McGowan Katie Amssoms Stefaan Last Benoit Devogelaere Marie‐Claude Rouan Leen Vijgen Jan Martin Berke Pascale Dehertogh Els Fransen Erna Cleiren Liesbet vanderHelm Gregory Fanning Kristof VanEmelen Origne Nyanguile Kenny Simmen Pierre Raboisson Sandrine Vendeville 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2012,124(19):4715-4718
104.
U. Galster P. Kaminski M. Beckert H. Helm U. Müller 《The European Physical Journal D - Atomic, Molecular, Optical and Plasma Physics》2001,17(3):307-318
We have performed kinematically complete investigations of molecular photodissociation of triatomic hydrogen in a fast beam
translational spectrometer recently built in Freiburg. The apparatus allows us to investigate laser-induced dissociation of
neutral molecules into two, three, or more neutral products. The fragments are detected in coincidence and their vectorial
momenta in the center-of-mass frame are determined. We demonstrate the potential of the method at the fragmentation of the
3 s
2
A
1
′
(
N
= 1,
K
= 0) state of triatomic hydrogen. In this state, three-body decay into ground state hydrogen atoms H+H+H, two-body predissociation
into H+H
2
(v
,
J), and photoemission to the H
3
ground state surface with subsequent two-body decay are competing channels. In the case of two-body predissociation, we determine
the rovibrational population in the H
2
(v
,
J) fragment. The vibrational distribution of H
2
is compared with approximate theoretical predictions. For three-body decay, we measure the six-fold differential photodissociation
cross-section. To determine accurate final state distributions, the geometric collection efficiency of the apparatus is calculated
by a Monte Carlo simulation, and the raw data are corrected for apparatus efficiency. The final state momentum distribution
shows pronounced correlation patterns which are characteristic for the dissociation mechanism. For a three-body decay process
with a discrete kinetic energy release we have developed a novel data reduction procedure based on the detection of two fragments.
The final state distribution determined by this independent method agrees extremely well with that observed in the triple-coincidence
data. In addition, this method allows us to fully explore the phase space of the final state and to determine the branching
ratios between the two- and three-body decay processes.
Received 29 March 2001 相似文献
105.
J. Potfajova J.M. Sun B. Schmidt T. Dekorsy W. Skorupa M. Helm 《Journal of luminescence》2006,121(2):290-292
Light emitting pn-diodes were fabricated on a 5.8 μm thick n-type Si device layer of a silicon-on-insulator (SOI) wafer using standard silicon technology and boron implantation. The thickness of the Si device layer was reduced to 1.3 μm, corresponding to a 4λ-cavity for λ=1150 nm light. Electroluminescence spectra of these low Q-factor microcavities are presented. Addition of Si/SiO2 Bragg reflectors on the top and bottom of the device (3.5 and 5.5 pairs, respectively) is predicted to lead to spectral emission enhancement by ∼270. 相似文献
106.
107.
108.
Electron injection through a tunnel barrier into a long period GaAs/AlGaAs superlattice is investigated. Seven negative differential resistance (NDR) regions are observed, resulting from resonant tunneling into the first well of the superlattice. Their positions can be quantitatively accounted for by considering the distribution of the electric field in the depletion region and the tunnel barrier. Upon application of a magnetic field parallel to the layers, the NDR's are shifted and weakened, which can be explained in terms of conservation of energy and canonical momentum. Furthermore, optical phonon generated conductance oscillations are observed although the depletion region is punctuated by the superlattice structure. 相似文献
109.
110.