Search results for "Delocalized electron"
showing 10 items of 158 documents
Localization vs. Delocalization in Molecules and Clusters: Electronic and Vibronic Interactions in Mixed Valence Systems
1996
The interplay between electron delocalization and magnetic interactions play a key role in areas as diverse as solid state chemistry (bulk magnetic materials, superconductors,...) [1] and biology (iron-sulfur proteins, manganese-oxo clusters ...) [2]. In molecular inorganic chemistry these two electronic processes have been traditionally studied independently. Thus, the electron dynamics has been extensively investigated in mixedvalence dimers [3] as exemplified by the Creutz-Taube complex [(NH3)5RuII(pyrazine)RuIII(NH3)5]. In this kind of molecular complexes one extra electron is delocalized over two diamagnetic metal sites. Therefore, they constitute model systems for the study of the ele…
Control of Localization and Suppression of Tunneling by Adiabatic Passage
2004
We show that a field of frequency $\ensuremath{\omega}$ combined with its second harmonic $2\ensuremath{\omega}$ driving a double-well potential allows us to localize the wave packet by adiabatic passage, starting from the delocalized ground state. The relative phase of the fields allows us to choose the well of localization. We can suppress (and restore) the tunneling subsequently by switching on (and off) abruptly the fields at well-defined times. The mechanism relies on the fact that the dynamics is driven to an eigenstate of the Floquet Hamiltonian which is a localized state.
Disorder and localization effects on the local spectroscopic and infrared optical properties ofGa1−xMnxAs
2015
We study numerically the influence of disorder and localization effects on the local spectroscopic characteristics and infrared optical properties of ${\text{Ga}}_{1\ensuremath{-}x}{\text{Mn}}_{x}\text{As}$. We treat the band structure and disorder effects at an equal level by using an exact diagonalization supercell simulation method. This method accurately describes the low-doping limit and gives a clear picture of the transition to higher dopings, which captures the localization effects inaccessible to other theoretical methods commonly used. Our simulations capture the rich in-gap localized states observed in scanning tunneling microscopy studies and reproduce the observed features of t…
Control of field-free molecular alignment by phase-shaped laser pulses
2005
We report an experimental study of the control of molecular alignment of ${\mathrm{N}}_{2}$ by use of spectrally modulated pulses at an intensity regime below the intrinsic saturation of the alignment. By manipulating the relative timing of the alignment revival pattern arising from the even subset of the thermal ensemble as compared to the odd subset, we demonstrate that the angular distribution of the aligned molecule can be converted into planar delocalization at specific times. We also show that the angular focusing of the molecular axis can be switched off by applying a specific bipulse.
Comparative study of monotonically convergent optimization algorithms for the control of molecular rotation
2013
We apply two different monotonically convergent optimization algorithms to the control of molecular rotational dynamics by laser pulses. This example represents a quantum control problem where the interaction of the system with the external field is non-linear. We test the validity and accuracy of the two methods on the key control targets of producing molecular orientation and planar delocalization at zero temperature, and maximizing permanent alignment at non-zero temperature.
Electric Field Control of Spin States in Trigonal Two-Electron Quantum Dot Arrays and Mixed-Valence Molecules: II. Vibronic Problem
2018
In this article, the vibronic model for an electric field switchable mixed-valence trimer containing two delocalized electrons or holes is proposed and examined. The role of the vibronic coupling on the electric field effects is analyzed by means of the semiclassical adiabatic approach and, alternatively, with the aid of the numerical analysis of the Schrodinger equation with due allowance for the kinetic energy of the ions (dynamic problem). The adiabatic potential landscapes have been calculated by taking into account the influence of the electric field. As the adiabatic approximation has a limited frame of validity, the study of the electric field effects has also been performed within m…
Correlation gap in the heavy-fermion antiferromagnetUPd2Al3
2002
The optical properties of the heavy-fermion compound ${\mathrm{UPd}}_{2}{\mathrm{Al}}_{3}$ have been measured in a frequency range from 0.04 to 5 meV $(0.3--40{\mathrm{cm}}^{\ensuremath{-}1})$ at temperatures $2\mathrm{K}lTl300\mathrm{K}.$ Below the coherence temperature ${T}^{*}\ensuremath{\approx}50\mathrm{K},$ a hybridization gap opens around 10 meV. As the temperature decreases further $(Tl~20\mathrm{K}),$ a well-pronounced pseudogap of approximately 0.2 meV develops in the optical response; we relate this to the antiferromagnetic ordering which occurs below ${T}_{N}\ensuremath{\approx}14\mathrm{K}.$ The frequency-dependent mass and scattering rate give evidence that the enhancement of …
Electric field controllable magnetic coupling of localized spins mediated by itinerant electrons: a toy model
2017
In this paper, we propose a toy model to describe the magnetic coupling between the localized spins mediated by the itinerant electron in partially delocalized mixed-valence (MV) systems. This minimal model takes into account the key interactions that are common for all such systems, namely, electron transfer in the valence-delocalized moiety and magnetic exchange between the localized spins and the delocalized electrons. The proposed descriptive model is exactly solvable which allows us to qualitatively and quantitatively discuss the main features of the whole class of partially delocalized MV systems. In the case of relatively strong exchange coupling, the combined action of these two int…
Localization–Delocalization in Bridged Mixed-Valence Metal Clusters: Vibronic PKS Model Revisited
2015
Here we describe a new vibronic model of mixed valence (MV) dimer inspired by the conventional Piepho, Krausz, and Schatz (PKS) approach. We attempted to partially lift the main restriction of the PKS model dealing with the vibronically independent moieties of a MV molecule. The refined version of the PKS model in which the bridging ligands are included deals with the three main interactions: electron transfer (integral t0) related to the high-symmetric ligand configuration, on-site vibronic coupling (parameter υ) arising from the modulation of the crystal field on the metal sites by the breathing displacements of their nearest ligand surroundings, and intercenter vibronic coupling (paramet…
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 …