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The effect of electronic-nuclear coupling on electronic transport through a complex molecular network is studied. Electronic tunneling dynamics in a network of N donor/acceptor sites, connected by molecular bridges, is shown to be controlled by electronic-nuclear coupling at the bridges. Particularly, electronic coupling to an accepting nuclear mode at the contact site between the donor and the rest of the network is shown to affect the tunneling path selection to specific acceptors. In the "deep" tunneling regime, the network is mapped onto an N-level system using a recursive perturbation expansion, enabling analytical treatment of the electronic dynamics. The analytic formulation is applied for two model systems, demonstrating site-directed tunneling by electronic-nuclear coupling. Numerical simulations suggest that this phenomenon is not limited to the deep tunneling regime. 相似文献
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Electronic tunneling in a complex molecular network of N(>2) donor/acceptor sites, connected by molecular bridges, is analyzed. The "deep" tunneling dynamics is formulated using a recursive perturbation expansion, yielding a McConnell-type reduced N-level model Hamiltonian. Applications to models of molecular junctions demonstrate that the donor-bridge contact parameters can be tuned in order to control the tunneling dynamics and particularly to direct the tunneling pathway to either one of the various acceptors. 相似文献
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F. Caspary 《Mathematische Annalen》1887,28(4):493-498
Ohne Zusammenfassung 相似文献
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The avalanche energy transfer in highly thulium doped fiber amplifiers (TDFA) pumped at 1056 nm with laser diodes was investigated. Amplified spontaneous emission (ASE) at 800 nm and 1470 nm as well as the remaining pump power were measured as function of the pump power to explain the efficiency of the energy transfer between thulium ions. As proof of our theory, fiber amplifiers based on self-made fluoride fibers doped with 2000 and 5000 ppm thulium were realized and their gain and noise figure was measured. A gain of more than 25 dB and a noise figure of less than 4 dB was achieved at a pump power of 210 mW in a TDFA using the 5000 ppm thulium fiber, whereas a gain maximum of only 5.6 dB was observed with the 2000 ppm TDF. These investigations are of special importance since until now almost all TDFAs have used 2000 ppm fibers. PACS 83.80.Ab; 32.80.Bx; 42.65.Yj 相似文献
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The ability to control electronic tunneling in complex molecular networks of multiple donor/acceptor sites is studied theoretically. Our past analysis, demonstrating the phenomenon of site-directed transport, was limited to the coherent tunneling regime. In this work we consider electronic coupling to a dissipative molecular environment including the effect of decoherence. The nuclear modes are classified into two categories. The first kind corresponds to the internal molecular modes, which are coupled to the electronic propagation along the molecular bridges. The second kind corresponds to the external solvent modes, which are coupled to the electronic transport between different segments of the molecular network. The electronic dynamics is simulated within the effective single electron picture in the framework of the tight binding approximation. The nuclear degrees of freedom are represented as harmonic modes and the electronic-nuclear coupling is treated within the time-dependent Redfield approximation. Our results demonstrate that site-directed tunneling prevails in the presence of dissipation, provided that the decoherence time is longer than the time period for tunneling oscillations (e.g., at low temperatures). Moreover, it is demonstrated that the strength of electronic coupling to the external nuclear modes (the solvent reorganization energy) controls the coherent intramolecular tunneling dynamics at short times and may be utilized for the experimental control of site-directed tunneling in a complex network. 相似文献
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The Landauer-type formulation of current through a molecular junction with electronic-nuclear coupling introduced by Troisi et al. [J. Chem. Phys. 118, 6072 (2003)] is generalized to account for the dependence of the molecule-leads coupling terms on the nuclear coordinates. Although this electronic-nuclear coupling is external to the molecule there is no need to extend the molecular subspace when projection operators are employed for calculations of the current through the junction. A test case of a conductor with vibrating contacts to the leads is studied numerically. It is demonstrated that contact vibrations lead to inelastic contributions to the current and to characteristic features in the I-V curve and its derivatives, similar to the ones observed for internal (molecular) electronic-nuclear coupling. 相似文献
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