207 research outputs found
Dissipative Effects in the Electronic Transport through DNA Molecular Wires
We investigate the influence of a dissipative environment which effectively
comprises the effects of counterions and hydration shells, on the transport
properties of short \DNA wires. Their electronic structure is captured by a
tight-binding model which is embedded in a bath consisting of a collection of
harmonic oscillators. Without coupling to the bath a temperature independent
gap opens in the electronic spectrum. Upon allowing for electron-bath
interaction the gap becomes temperature dependent. It increases with
temperature in the weak-coupling limit to the bath degrees of freedom. In the
strong-coupling regime a bath-induced {\it pseudo-gap} is formed. As a result,
a crossover from tunneling to activated behavior in the low-voltage region of
the - characteristics is observed with increasing temperature. The
temperature dependence of the transmission near the Fermi energy, , manifests an Arrhenius-like behavior in agreement with recent transport
experiments. Moreover, shows a weak exponential dependence on
the wire length, typical of strong incoherent transport. Disorder effects smear
the electronic bands, but do not appreciably affect the pseudo-gap formation
Overcoming the Exciton Binding Energy in Two-Dimensional Perovskite Nanoplatelets by Attachment of Conjugated Organic Chromophores
In this work we demonstrate a novel approach to achieve efficient charge separation in dimensionally and dielectrically confined two-dimensional perovskite materials. Two-dimensional perovskites generally exhibit large exciton binding energies that limit their application in optoelectronic devices that require charge separation such as solar cells, photo-detectors and in photo-catalysis. Here, we show that by incorporating a strongly electron accepting moiety, perylene diimide organic chromophores, on the surface of the two-dimensional perovskite nanoplatelets it is possible to achieve efficient formation of mobile free charge carriers. These free charge carriers are generated with ten times higher yield and lifetimes of tens of microseconds, which is two orders of magnitude longer than without the peryline diimide acceptor. This opens a novel synergistic approach, where the inorganic perovskite layers are combined with functional organic chromophores in the same material to tune the properties for specific applications. Functionalizing two-dimensional (2D) hybrid perovskites with organic chromophores is a novel approach to tune their optoelectronic properties. Here, the authors report efficient charge separation and conduction in 2D hybrid perovskite nanoplatelets by incorporating an electron acceptor chromophoreThis work has received funding from the European Research Council Horizon 2020 ERC Grant Agreement No. 648433
Tuning of the excited state properties of phenylenevinylene oligomers:A time-dependent density functional theory study
This paper discusses a time-dependent density functional theory study of the effect of molecular structure on the excited state polarizability of conjugated molecules. A short phenylenevinylene oligomer containing three phenyl rings (PV2, distyryl benzene) is taken as a model system. Introduction of methyl substituents is shown to have only a small influence on the increase in polarizability upon excitation (the excess polarizability, Delta(alpha) over bar). Methoxy groups have a much larger effect but in this case Delta(alpha) over bar depends strongly on the dihedral angle between the side chain and the backbone of the molecule. If the central phenyl ring of PV2 has a meta-configuration rather than para, both the optical absorption spectrum and the excess polarizability change considerably. (C) 2003 American Institute of Physics
Tight-binding parameters for charge transfer along DNA
We systematically examine all the tight-binding parameters pertinent to
charge transfer along DNA. The molecular structure of the four DNA bases
(adenine, thymine, cytosine, and guanine) is investigated by using the linear
combination of atomic orbitals method with a recently introduced
parametrization. The HOMO and LUMO wavefunctions and energies of DNA bases are
discussed and then used for calculating the corresponding wavefunctions of the
two B-DNA base-pairs (adenine-thymine and guanine-cytosine). The obtained HOMO
and LUMO energies of the bases are in good agreement with available
experimental values. Our results are then used for estimating the complete set
of charge transfer parameters between neighboring bases and also between
successive base-pairs, considering all possible combinations between them, for
both electrons and holes. The calculated microscopic quantities can be used in
mesoscopic theoretical models of electron or hole transfer along the DNA double
helix, as they provide the necessary parameters for a tight-binding
phenomenological description based on the molecular overlap. We find that
usually the hopping parameters for holes are higher in magnitude compared to
the ones for electrons, which probably indicates that hole transport along DNA
is more favorable than electron transport. Our findings are also compared with
existing calculations from first principles.Comment: 15 pages, 3 figures, 7 table
Long-range corrected DFT calculations of charge-transfer integrals in model metal-free phthalocyanine complexes
An assessment of several widely used exchange--correlation potentials in computing charge-transfer integrals is performed. In particular, we employ the recently proposed Coulomb-attenuated model which was proven by other authors to improve upon conventional functionals in the case of charge-transfer excitations. For further validation, two distinct approaches to compute the property in question are compared for a phthalocyanine dimer
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