Molecular crystal approach for pi-conjugated polymers: from PPP Hamiltonian to Holstein model for polaron states

Starting from the $\pi$-electron Pariser-Parr-Pople (PPP) Hamiltonian which includes both strong electron-phonon and electron-electron interactions, we propose some strongly correlated wave functions of increasing quality for the ground state of conjugated polymers. These wavefunctions are built by combining different finite sets of local configurations extended at most over two nearest-neighbour monomers. With this picture, the doped case with one additional particle is expressed in terms of quasi-particle. Thus, the polaron formation problem goes back to the study of a Holstein like model.Comment: 27 pages, 6 eps figs, Revtex; enlarged version. Submitted to Journal of Physics: Condensed Matte

Static magneto-polarizability of cylindrical nanostructures

The static polarizability of cylindrical systems is shown to have a strong dependence on a uniform magnetic field applied parallel to the tube axis. This dependence is demonstrated by performing exact numerical diagonalizations of simple cylinders (rolled square lattices), armchair and zig-zag carbon nanotubes (rolled honeycomb lattices) for different electron-fillings. At low temperature, the polarizability as function of the magnetic field has a discontinuous character where plateau-like region are separated by sudden jumps or peaks. A one to one correspondence is pointed out between each discontinuity of the polarizability and the magnetic-field induced cross-over between the ground state and the first excited state. Our results suggest the possibility to use measurements of the static polarizability under magnetic field to get important informations about excited states of cylindrical systems such as carbon nanotubes.Comment: 9 eps fig

Pavlov's dog associative learning demonstrated on synaptic-like organic transistors

In this letter, we present an original demonstration of an associative learning neural network inspired by the famous Pavlov's dogs experiment. A single nanoparticle organic memory field effect transistor (NOMFET) is used to implement each synapse. We show how the physical properties of this dynamic memristive device can be used to perform low power write operations for the learning and implement short-term association using temporal coding and spike timing dependent plasticity based learning. An electronic circuit was built to validate the proposed learning scheme with packaged devices, with good reproducibility despite the complex synaptic-like dynamic of the NOMFET in pulse regime

A simplified picture for Pi electrons in conjugated polymers : from PPP Hamiltonian to an effective molecular crystal approach

An excitonic method proper to study conjugated oligomers and polymers is described and its applicability tested on the ground state and first excited states of trans-polyacetylene, taken as a model. From the Pariser-Parr-Pople Hamiltonian, we derive an effective Hamiltonian based on a local description of the polymer in term of monomers; the relevant electronic configurations are build on a small number of pertinent local excitations. The intuitive and simple microscopic physical picture given by our model supplement recent results, such as the Rice and Garstein ones. Depending of the parameters, the linear absorption appears dominated by an intense excitonic peak.Comment: 41 Pages, 6 postscript figure

Excitonic Strings in one dimensional organic compounds

Important questions concern the existence of excitonic strings in organic compounds and their signatures in the photophysics of these systems. A model in terms of Hard Core Bosons is proposed to study this problem in one dimension. Mainly the cases with two and three particles are studied for finite and infinite lattices, where analytical results are accessible. It is shown that if bi-excitonic states exist, three-excitonic and even, n-excitonic strings, at least in a certain range of parameters, will exist. Moreover, the behaviour of the transitions from one exciton to the biexciton is fully clarified. The results are in agreement with exact finite cluster diagonalizations of several model Hamiltonians.Comment: 36 pages, 4 eps figs. to appear in Phys. Rev.

Optical excitations of Peierls-Mott insulators with bond disorder

The density-matrix renormalization group (DMRG) is employed to calculate optical properties of the half-filled Hubbard model with nearest-neighbor interactions. In order to model the optical excitations of oligoenes, a Peierls dimerization is included whose strength for the single bonds may fluctuate. Systems with up to 100 electrons are investigated, their wave functions are analyzed, and relevant length-scales for the low-lying optical excitations are identified. The presented approach provides a concise picture for the size dependence of the optical absorption in oligoenes.Comment: 12 pages, 13 figures, submitted to Phys. Rev.

Optical excitations in a one-dimensional Mott insulator

The density-matrix renormalization-group (DMRG) method is used to investigate optical excitations in the Mott insulating phase of a one-dimensional extended Hubbard model. The linear optical conductivity is calculated using the dynamical DMRG method and the nature of the lowest optically excited states is investigated using a symmetrized DMRG approach. The numerical calculations agree perfectly with field-theoretical predictions for a small Mott gap and analytical results for a large Mott gap obtained with a strong-coupling analysis. Is is shown that four types of optical excitations exist in this Mott insulator: pairs of unbound charge excitations, excitons, excitonic strings, and charge-density-wave (CDW) droplets. Each type of excitations dominates the low-energy optical spectrum in some region of the interaction parameter space and corresponds to distinct spectral features: a continuum starting at the Mott gap (unbound charge excitations), a single peak or several isolated peaks below the Mott gap (excitons and excitonic strings, respectively), and a continuum below the Mott gap (CDW droplets).Comment: 12 pages (REVTEX 4), 12 figures (in 14 eps files), 1 tabl

Electrostatic potential profiles of molecular conductors

The electrostatic potential across a short ballistic molecular conductor depends sensitively on the geometry of its environment, and can affect its conduction significantly by influencing its energy levels and wave functions. We illustrate some of the issues involved by evaluating the potential profiles for a conducting gold wire and an aromatic phenyl dithiol molecule in various geometries. The potential profile is obtained by solving Poisson's equation with boundary conditions set by the contact electrochemical potentials and coupling the result self-consistently with a nonequilibrium Green's function (NEGF) formulation of transport. The overall shape of the potential profile (ramp vs. flat) depends on the feasibility of transverse screening of electric fields. Accordingly, the screening is better for a thick wire, a multiwalled nanotube or a close-packed self-assembled monolayer (SAM), in comparison to a thin wire, a single-walled nanotube or an isolated molecular conductor. The electrostatic potential further governs the alignment or misalignment of intramolecular levels, which can strongly influence the molecular I-V characteristic. An external gate voltage can modify the overall potential profile, changing the current-voltage (I-V) characteristic from a resonant conducting to a saturating one. The degree of saturation and gate modulation depends on the metal-induced-gap states (MIGS) and on the electrostatic gate control parameter set by the ratio of the gate oxide thickness to the channel length.Comment: to be published in Phys. Rev. B 69, No.3, 0353XX (2004