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Crucial Role of Nuclear Dynamics for Electron Injection in a Dye–Semiconductor Complex
journal contribution
posted on 2015-12-17, 08:28 authored by Adriano Monti, Christian
F. A. Negre, Victor S. Batista, Luis G. C. Rego, Huub J. M. de Groot, Francesco BudaWe investigate the electron injection
from a terrylene-based chromophore
to the TiO2 semiconductor bridged by a recently proposed
phenyl-amide-phenyl molecular rectifier. The mechanism of electron
transfer is studied by means of quantum dynamics simulations using
an extended Hückel Hamiltonian. It is found that the inclusion
of the nuclear motion is necessary to observe the photoinduced electron
transfer. In particular, the fluctuations of the dihedral angle between
the terrylene and the phenyl ring modulate the localization and thus
the electronic coupling between the donor and acceptor states involved
in the injection process. The electron propagation shows characteristic
oscillatory features that correlate with interatomic distance fluctuations
in the bridge, which are associated with the vibrational modes driving
the process. The understanding of such effects is important for the
design of functional dyes with optimal injection and rectification
properties.
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Keywords
oscillatory featuresCrucial RoleTiO 2 semiconductor bridgeddihedral angleNuclear Dynamicselectron transferinteratomic distance fluctuationsvibrational modesElectron Injectionquantum dynamics simulationselectron injectionelectron propagationrectification propertiesinjection processphenyl ringacceptor statesphotoinduced electron transfer
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