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51.
Hüsken N G?bala M Battistel A La Mantia F Schuhmann W Metzler-Nolte N 《Chemphyschem》2012,13(1):131-139
Gold‐surface grafted peptide nucleic acid (PNA) strands, which carry a redox‐active ferrocene tag, present unique tools to electrochemically investigate their mechanical bending elasticity based on the kinetics of electron‐transfer (ET) processes. A comparative study of the mechanical bending properties and the thermodynamic stability of a series of 12‐mer Fc‐PNA?DNA duplexes was carried out. A single basepair mismatch was integrated at all possible strand positions to provide nanoscopic insights into the physicochemical changes provoked by the presence of a single basepair mismatch with regard to its position within the strand. The ET processes at single mismatch Fc‐PNA?DNA modified surfaces were found to proceed with increasing diffusion limitation and decreasing standard ET rate constants k0 when the single basepair mismatch was dislocated along the strand towards its free‐dangling Fc‐modified end. The observed ET characteristics are considered to be due to a punctual increase in the strand elasticity at the mismatch position. The kinetic mismatch discrimination with respect to the fully‐complementary duplex presents a basis for an electrochemical DNA sensing strategy based on the Fc‐PNA?DNA bending dynamics for loosely packed monolayers. In a general sense, the strand elasticity presents a further physicochemical property which is affected by a single basepair mismatch which may possibly be used as a basis for future DNA sensing concepts for the specific detection of single basepair mismatches. 相似文献
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We study the electron transport in three terminal junctions and quantum rings looking for the classical deflection of electron trajectories in the presence of intersubband scattering. We indicate that although the Aharonov-Bohm oscillations and the Lorentz force effects co-exist in the low subband transport, for higher Fermi energies a simultaneous observation of both effects is difficult and calls for carefully formed structures. In particular, in quantum rings with channels wider than the input lead the Lorentz force is well resolved but the Aharonov-Bohm periodicity is lost in chaotic scattering events. In quantum rings with equal lengths of the channels and T-shaped junctions the Aharonov-Bohm oscillations are distinctly periodic but the Lorentz force effects are not well pronounced. We find that systems with wedge-shaped junctions allow for observation of both the periodic Aharonov-Bohm oscillations and the magnetic deflection. 相似文献
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First-principles calculations are performed to obtain the dielectric function and loss spectra of bulk PdH(x). Hydrogen concentrations between x = 0 and 1 are considered. The calculated spectra are dominated by a broad peak that redshifts in energy with x. The obtained bulk dielectric function is employed to compute the loss spectra of PdH(x) spherical nanoparticles as a function of x. The dominant plasmon peak in the spherical nanoparticle is lowered in energy with respect to the bulk case. However, the dependence of the resonance energy on the hydrogen concentration is roughly similar to that in bulk. 相似文献
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We study theoretically the spin dynamics of a magnetic dimer serving as a contact between two electrodes. We find that the spin-spin coupling in the dimer can be dramatically modified from its equilibrium value. We show that the interaction can be tuned in such a way that it effectively changes its sign. The calculations show that, for large enough bias, the exchange interaction can even be changed from antiferromagnetic to ferromagnetic. The physical principles behind this result can be used as a new tool to achieve magneto-electric effects in molecular magnet systems. 相似文献
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Because of the spin and Dirac-valley degrees of freedom, graphene allows the observation of one-, two- or four-component fractional quantum Hall effects in different parameter regions. We address the stability of various states in the SU(2) and SU(4) limits. In the SU(4) limit, we predict that new low-energy Goldstone modes determine the stability of the fractional quantum Hall states at 2/5, 3/7, etc; SU(4) skyrmions are not found to be relevant for the low-energy physics. These results are discussed in light of experiments. 相似文献
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Structural properties and energetics of Cr-based Z-phases (CrNbN, Cr(Nb,V)N and CrVN) were investigated using the Vienna ab?initio simulation package (VASP) code employing the projector augmented wave (PAW) pseudopotentials by means of both local density approximation (LDA) and generalized gradient approximation (GGA) for the exchange and correlation term. The geometry of all studied phases including NbN, VN and elemental constituents (nonmagnetic bcc Nb and V and antiferromagnetic bcc Cr) was fully relaxed, providing the equilibrium structure parameters and total energies. The calculated lattice parameters of Z-phases correspond very well to the experimental data and decrease with increasing molar fraction of vanadium. Enthalpies of formation show that all three Z-phases are stable at T?=?0?K. The electronic structures of Z-phases including densities of states and charge densities were analysed. The calculated bulk moduli and elastic constants were used to evaluate stability conditions and elastic anisotropy ratios. It was confirmed that Z-phases are mechanically stable. Additional information on ductility was obtained from Cauchy pressures, Pugh ratios, Young moduli, and Poisson ratios. The ductility evaluated using the Pugh ratio decreases with number of vanadium atoms. 相似文献