Search results for "Localized"
showing 10 items of 297 documents
Electrically switchable magnetic exchange in the vibronic model of linear mixed valence triferrocenium complex
2018
In this article, we report our development of a vibronic model for the electric-field control of antiferromagnetic superexchange in the mixed-valence (MV) triferrocenium complex FeIII-FeII-FeIII proposed as a possible candidate for the molecular implementation of a quantum logic gate. Along with the electronic interactions, such as electron transfer between the iron ions in different oxidation degrees and Coulomb repulsion of the extra holes, the proposed model of the triferrocenium complex also takes into account the vibronic coupling as an inherent ingredient of the problem of mixed valency. The latter is described by the conventional Piepho-Krauzs-Shatz (PKS) model adapted to the linear …
Mixed-valence molecular four-dot unit for quantum cellular automata: Vibronic self-trapping and cell-cell response
2015
Our interest in this article is prompted by the vibronic problem of charge polarized states in the four-dot molecular quantum cellular automata (mQCA), a paradigm for nanoelectronics, in which binary information is encoded in charge configuration of the mQCA cell. Here, we report the evaluation of the electronic levels and adiabatic potentials of mixed-valence (MV) tetra-ruthenium (2Ru(ii) + 2Ru(iii)) derivatives (assembled as two coupled Creutz-Taube complexes) for which molecular implementations of quantum cellular automata (QCA) was proposed. The cell based on this molecule includes two holes shared among four spinless sites and correspondingly we employ the model which takes into accoun…
Delocalization of Nonlinear Optical Responses in Plasmonic Nanoantennas
2015
Remote excitation and emission of two-photon luminescence and second-harmonic generation are observed in micrometer long gold rod optical antennas upon local illumination with a tightly focused near-infrared femtosecond laser beam. We show that the nonlinear radiations can be emitted from the entire antenna and the measured far-field angular patterns bear the information regarding the nature and origins of the respective nonlinear processes. We demonstrate that the nonlinear responses are transported by the propagating surface plasmon at excitation frequency, enabling thereby polariton-mediated tailoring and design of nonlinear responses.
Near-field beam displacement at surface plasmon resonance
2011
International audience; A finite-size beam exciting a surface plasmon polariton (SPP) in a prism coupling configuration experiences an in-plane displacement that can be used for the characterization of plasmonic components by means of near-field optical microscopy. We first demonstrate experimentally the existence of this displacement by taking near-field images of finite-width metal strips. Next, the properties of this shift are analyzed in detail. We investigate the dynamic of the near-field shift for an incident Gaussian beam as a function of illumination conditions. For beams with a narrow spectrum, we propose a straightforward derivation showing that the displacement depends on the ave…
Polarizabilities of small annulenes from Cholesky CC2 linear response theory
2004
Using recently developed algorithms based on Cholesky decomposition of two-electron integrals to compute response properties at the correlated level, the static and dynamic (at 589 nm) polarizabilities of [4n + 2]-annulenes (n = 1, 2, 3, 4) have been calculated. The results show that the perpendicular component increases along the series linearly with the number of double bonds. The in-plane static polarizability is also increasing linearly with the area of the aromatic ring in the case of the delocalized species. However, linearity is lost for the localized conformations and for the dynamic polarizability. (C) 2004 Elsevier B.V. All rights reserved.
Coherent Light Harvesting through Strong Coupling to Confined Light
2018
When photoactive molecules interact strongly with confined light modes, new hybrid light–matter states may form: the polaritons. These polaritons are coherent superpositions of excitations of the molecules and of the cavity photon. Recently, polaritons were shown to mediate energy transfer between chromophores at distances beyond the Forster limit. Here we explore the potential of strong coupling for light-harvesting applications by means of atomistic molecular dynamics simulations of mixtures of photoreactive and non-photo-reactive molecules strongly coupled to a single confined light mode. These molecules are spatially separated and present at different concentrations. Our simulations sug…
On the nature of interactions in the F2 OXe(…) NCCH3 complex: Is there the Xe(IV)N bond?
2016
Nature of the bonding in isolated XeOF2 molecule and F2 OXe(…) NCCH3 complexes have been studied in the gas phase (0 K) using Quantum Chemical Topology methods. The wave functions have been approximated at the MP2 and DFT levels of calculations, using the APFD, B3LYP, M062X, and B2PLYP functionals with the GD3 dispersion correction. The nature of the formal XeO bond in the XeOF2 monomer depends on the basis set used (all-electron vs. the ecp-28 approximation for Xe). Within the all-electron basis set approach the bond is represented by two bonding attractors, Vi = 1,2 (Xe,O), with total population of about 1.06e and highly delocalized electron density in both bonding basins. No bonding bas…
Universality classes for wetting in two-dimensional random-bond systems
1991
Interface-unbinding transitions, such as those arising in wetting phenomena, are studied in two-dimensional systems with quenched random impurities and general interactions. Three distinct universality classes or scaling regimes are investigated using scaling arguments and extensive transfer-matrix calculations. Both the critical exponents and the critical amplitudes are determined for the weak- and the strong-fluctuation regime. In the borderline case of the intermediate-fluctuation regime, the asymptotic regime is not accessible to numerical simulations. We also find strong evidence for a nontrivial delocalization transition of an interface that is pinned to a line of defects.
Absence of mutual polariton scattering for strongly coupled surface plasmon polaritons and dye molecules with a large Stokes shift
2013
The understanding and control of the dynamics of hybrid modes consisting of strongly coupled surface plasmon polaritons and molecular excitations of dye molecules is of great timely interest, as it allows one to tailor interactions between optical signals as needed for active all-optical devices. Here we utilize dye molecules with an especially large Stokes shift to demonstrate the absence of mutual scatterings among the strongly coupled hybrid modes. We employ a quantum mechanical three-level model and show that the hybrid modes decay via dephasing and internal relaxation of the molecules to a fluorescing state of the dye, which can be used as a measure for the decay. Our results provide e…
Light trapping by plasmonic nanoparticles
2020
Abstract Metallic nanoparticles sustaining localized surface plasmon resonances are of great interest for enhancing light trapping in thin film photovoltaics. In this chapter, we explore the correlation between the structural and optical properties of self-assembled silver nanostructures fabricated by a solid-state dewetting process on various substrates relevant for silicon photovoltaics and later integrated into plasmonic back reflectors. Our study allows us to optimize the performance of nanostructures by identifying the fabrication conditions in which desirable circular and uniformly spaced nanoparticles are obtained. Second, we introduce a novel optoelectronic spectroscopic method that…