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11.
Pham TN Griffin JM Masiero S Lena S Gottarelli G Hodgkinson P Filip C Brown SP 《Physical chemistry chemical physics : PCCP》2007,9(26):3416-3423
(2h)J(NN) hydrogen-bond mediated J couplings are measured in the solid state for two synthetic deoxyguanosine derivatives by (15)N MAS NMR spin-echo experiments. The use of rotor-synchronised Hahn-echo pulse train (RS-HEPT) (1)H decoupling, with a duty cycle of 6%, allows spin-echo durations out to 200 ms, hence enabling the accurate determination of J couplings as small as 3.8 Hz. A single-crystal X-ray diffraction structure exists for the shorter alkyl chain derivative dG(C(3))(2): the observation of significantly different (2h)J(NN) couplings, 6.2 +/- 0.4 and 7.4 +/- 0.4 Hz, for the two resolved N7 resonances is to be expected given the NH...N hydrogen-bonding distances of 2.91 and 2.83 A for the two distinct molecules in the asymmetric unit cell. For the longer alkyl chain derivative, dG(C(10))(2), for which there is no single-crystal diffraction structure, a (15)N refocused INADEQUATE spectrum (Pham et al., J. Am. Chem. Soc., 2005, 127, 16018-16019) has demonstrated the presence of N2-H...N7 intermolecular hydrogen-bonds indicative of a quartet-like structure. The (2h)J(NN) hydrogen-bond mediated J coupling of 5.9 +/- 0.2 Hz is at the lower end of the range (5.9-8.2 Hz) of (2h)J(NN) couplings determined from solution-state NMR of guanosine quartets in quadruplex DNA. A full discussion of the determination of error bars on the fitted parameters is given; specifically, error bars determined by a non-linear fitting (using the covariance matrix) or in a Monte-Carlo fashion are found to give effectively identical results. 相似文献
12.
Combating Multidrug‐Resistant Bacteria: Current Strategies for the Discovery of Novel Antibacterials
Dr. Kieron M. G. O'Connell Dr. James T. Hodgkinson Dr. Hannah F. Sore Dr. Martin Welch Prof. George P. C. Salmond Dr. David R. Spring 《Angewandte Chemie (International ed. in English)》2013,52(41):10706-10733
The introduction of effective antibacterial therapies for infectious diseases in the mid‐20th century completely revolutionized clinical practices and helped to facilitate the development of modern medicine. Many potentially life‐threatening conditions became easily curable, greatly reducing the incidence of death or disability resulting from bacterial infections. This overwhelming historical success makes it very difficult to imagine life without effective antibacterials; however, the inexorable rise of antibiotic resistance has made this a very real and disturbing possibility for some infections. The ruthless selection for resistant bacteria, coupled with insufficient investment in antibacterial research, has led to a steady decline in the efficacy of existing therapies and a paucity of novel structural classes with which to replace them, or complement their use. This situation has resulted in a very pressing need for the discovery of novel antibiotics and treatment strategies, the development of which is likely to be a key challenge to 21st century medicinal chemistry. 相似文献
13.
Kenwright JL Galloway WR Blackwell DT Isidro-Llobet A Hodgkinson J Wortmann L Bowden SD Welch M Spring DR 《Chemistry (Weinheim an der Bergstrasse, Germany)》2011,17(10):2981-2986
Herein, a new copper-catalysed strategy for the synthesis of rare nitrogen-linked seven-, eight- and nine-membered biaryl ring systems is described. It is proposed that the reaction proceeds through a highly activated intramolecularly co-ordinated copper catalyst. The process is technically simple, proceeds under relatively mild conditions, displays a broad substrate scope and forms biologically valuable products that are difficult to synthesise by other methods. We envisage that this methodology will prove useful in a wide synthetic context, with possible applications in both target-oriented and diversity-oriented synthesis. 相似文献
14.
W. R. Hodgkinson 《Fresenius' Journal of Analytical Chemistry》1896,35(1):552
Ohne Zusammenfassung 相似文献
15.
16.
Bowmaker GA Harris RK Assadollahzadeh B Apperley DC Hodgkinson P Amornsakchai P 《Magnetic resonance in chemistry : MRC》2004,42(9):819-826
Solid-state cross-polarization magic-angle spinning (CP/MAS) NMR spectra were recorded for the compounds [Ag(NH3)2]2SO4, [Ag(NH3)2]2SeO4 and [Ag(NH3))]NO3, all of which contain the linear or nearly linear two-coordinate [Ag(NH3)2]+ ion. The 109Ag CP/MAS NMR spectra show centrebands and associated spinning sideband manifolds typical for systems with moderately large shielding anisotropy, and splittings due to indirect 1J(109Ag,14N) spin-spin coupling. Spinning sideband analysis was used to determine the 109Ag shielding anisotropy and asymmetry parameters Deltasigma and eta from these spectra, yielding anisotropies in the range 1500-1600 ppm and asymmetry parameters in the range 0-0.3. Spectra were also recorded for 15N and (for the selenate) 77Se. In all cases the number of resonances observed is as expected for the crystallographic asymmetric units. The crystal structure of the selenate is reported for the first time. One-bond (107, 109Ag,15N) coupling constants are found to have magnitudes in the range 60-65 Hz. Density functional calculations of the Ag shielding tensor for model systems yield results that are in good agreement with the experimentally determined shielding parameters, and suggest that in the solid compounds Deltasigma and eta are reduced and increased, respectively, from the values calculated for the free [Ag(NH3)2]+ ion (1920 ppm and 0, respectively), primarily as a result of cation-cation interactions, for which there is evidence from the presence of metal-over-metal stacks of [Ag(NH3)2]+ ions in the solid-state structures of these compounds. 相似文献
17.
Ambichiral layered structures can be designed to function reasonably well as rejection filters for elliptical polarization states, although the proposed design strategy is inadequate for linear and quasilinear polarization states. 相似文献
18.
A kinetic spectrophotometric technique, employing a Q-switched, frequency-doubled ruby laser as the excitation source, has been used to determine the short-lived (S1 → Sp), and long-lived (T1 → Tq) transient absorption spectra of several benzenoid aromatic hydrocarbons. The excited singlet states determined in this way are compared with the singlet states observed by absorption from the ground state (S0 → Sn). Some previously assigned triplet states are reassigned as singlet levels. 相似文献
19.
The accuracy with which distances can be measured using dipolar recoupling experiments in solid-state NMR is investigated. The relative precision of experiments in a three spin system versus an isolated spin pair is found to depend very strongly on the nature of the coupling Hamiltonian. The accuracy of distances measured in even the simplified three spin system is seen to be very poor for existing homonuclear recoupling Hamiltonians. This suggests that it would be difficult to exploit broadband homonuclear recoupling to measure geometrical information reliably in complex spin systems. These conclusions apply equally to both single-crystal studies and powder samples. In contrast, the presence of additional spins has marginal impact on the accuracy when the coupling Hamiltonians commute with each other, as in the case of heteronuclear recoupling. The possibility of creating such a Hamiltonian for homonuclear recoupling using a suitable rotor-synchronized pulse sequence is discussed. 相似文献
20.
L. Calibbi R. N. Hodgkinson J. Jones?Pérez A. Masiero O. Vives 《The European Physical Journal C - Particles and Fields》2012,72(2):1863
The current 7 TeV run of the LHC experiment shall be able to probe gluino and squark masses up to values larger than 1 TeV.
Assuming that hints for SUSY are found in the jets plus missing energy channel by the end of a 5 fb−1 run, we explore the flavour constraints on three models with a CMSSM-like spectrum: the CMSSM itself, a seesaw extension
of the CMSSM, and Flavoured CMSSM. In particular, we focus on decays that might have been measured by the time the run is
concluded, such as B
s
→μμ and μ→eγ. We also analyse constraints imposed by neutral meson bounds and electric dipole moments. The interplay between collider
and flavour experiments is explored through the use of three benchmark scenarios, finding the flavour feedback useful in order
to determine the model parameters and to test the consistency of the different models. 相似文献