Current Enhancement In Three Dmensional MetalWaterMetal 在三维metalwatermetal电流增强.pptVIP

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Current Enhancement In Three Dmensional MetalWaterMetal 在三维metalwatermetal电流增强.ppt

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Current Enhancement In Three Dmensional MetalWaterMetal 在三维metalwatermetal电流增强

Electronic Tunneling through Dissipative Molecular Bridges Uri Peskin Department of Chemistry, Technion - Israel Institute of Technology Outline Motivation: Controlled electron transport in molecular devices and in biological systems. Background: ET in Donor-Acceptor complexes: The Golden Rule, the Condon approximaton and the spin-boson Hamiltonian. ET in Donor-Bridge-Acceptor complexes: McConnell’s formula for the tunneling matrix elements. The problem: Electronic-nuclear coupling at the molecular bridge and the breakdown of the Condon approximation. The model system: Generalized spin-boson Hamiltonians for dissipative through-bridge tunneling. Results: The weak coupling limit: Langevin-Schroedinger formulation, simulations and interpretation of ET through a dissipative bridge Beyond the weak coupling limit: An analytic formula for the tunneling matrix element in the deep tunneling regime. Conclusions: Promotion of tunneling through molecular barriers by electronic-nuclear coupling. The effect of molecular rigidity. Controlled tunneling through molecules? Long Range Electronic Tunneling McConnell’s Formula:A tight binding model Superexchange dynamics througha symmetric uniform bridge Deep tunneling through a molecular bridge The role of bridge nuclear modes? Validity of the Condon approximation? Electronic nuclear coupling at the bridge: Structural (promoting) bridge modes: Numerical Simulations: Weak e-n coupling Interpretation: a time-dependent Hamiltonian Interpretation: a time-dependent Hamiltonian A dissipative-acceptor model: A Rigorous Formulation Introducing vibrational eigenstates: In the absence of electronic coupling the ground state is degenerate: Interpretation: Summation over vibronic tunneling pathways: An example (N=8) The “slow electron” adiabatic limit Flexible vs. Rigid molecular bridges Langevin-Schroedinger simulations: A rigorous treatment:The “slow electron” limit Summary and Conclusions A rigorous calculation