Quantum kinetic theory of confined electrons in a strong time dependent field

A gauge-invariant Green’s function approach to the quantum transport of spatially confined electrons in strong electromagnetic fields is presented. The theory includes mean field and exchange effects, as well as collisions and initial correlations. It allows for a self-consistent treatment of spectral properties and collective effects (plasmons), on one hand, and nonlinear field phenomena, such as harmonic generation and multiphoton absorption, on the other. It is equally applicable to electrons in quantum dots, ultracold ions in traps and valence electrons of metal clusters.     

Theory of ferromagnetism in doped excitonic condensates

Nesting in a semimetal can lead to an excitonic-insulator state with spontaneous coherence between conduction and valence bands and a gap for charged excitations. We present a theory of the ferromagnetic state that occurs when the density of electrons in the conduction band and holes in the valence band differ. We find an unexpectedly rich doping-field phase diagram and an unusual collective excitation spectrum that includes two gapless collective modes. We predict regions of doping and external field in which phase-separated condensates of electrons and holes with parallel spins and opposing spins coexist.     

Electron states in metal clusters

Radiative transitions in metal clusters are analyzed in terms of quantum transitions of valence electrons that interact with surrounding valence electrons and ion cores. The analysis is based on the solution of the Thomas-Fermi equation for valence electrons in a spherical cluster. The quantum states of valence electrons and the energy and the dipole moments of transitions are determined in the quasiclassical approximation. It is shown that the frequencies of dipole oscillations and the dipole moments of the transitions strongly depend on the size of a cluster.     

Statistical measures and magic numbers in metal clusters

In this work, a shell model for metal clusters up to 220 valence electrons is used to obtain the fractional occupation probabilities of the electronic orbitals. Then, the calculation of a statistical measure of complexity and the Fisher-Shannon information is carried out. An increase of both magnitudes with the number of valence electrons is observed. The shell structure is reflected by the behavior of the statistical complexity. The magic numbers are indicated by the Fisher-Shannon information. So, as in the case of atomic nuclei, the study of statistical indicators also unveil the existence of magic numbers in metal clusters.     

Radiative transition mechanisms in metal clusters

Experimental data on the absorption of radiation by cold lithium, potassium, and silver clusters and on the emission of radiation by hot niobium and tungsten clusters are analyzed within the scope of two interpretive schemes of radiative transitions in clusters. The first scheme comprises plasmon model of light absorption by valence electrons of metal clusters. The second scheme treats radiative transitions in metal clusters as transitions of valence electrons interacting with surrounding electrons and atomic cores. The experimental data exhibit better agreement with the second interpretation. Zh. éksp. Teor. Fiz. 116, 1903–1911 (December 1999)     

Twist mode in spherical alkali metal clusters

A remarkable orbital quadrupole magnetic resonance, so-called twist mode, is predicted in alkali metal clusters where it is represented by Ipi = 2(-) low-energy excitations of valence electrons with strong M2 transitions to the ground state. We treat the twist by both macroscopic and microscopic ways. In the latter case, the shell structure of clusters is fully exploited, which is crucial for the considered size region ( 8相似文献   

Collective electronic excitations in clusters in the vicinity of metal surfaces

We study the collective excitations of metal clusters approaching a metal surface. Using a simple model for the frequency-dependent dielectric constant ε(ω) and the multiple scattering method, we numerically investigate the shift in the plasmon resonance due to the coupling of the collective modes of the sphere with those of its mirror image. Results of the model calculation are verified by means of ab initio theory. As a prototype system we study Na₉ ⁺ cluster on the Cu(100) surface. The representation of the solid surface by a cluster of several, typically 54 substrate atoms, is used in combination with a high level configuration interaction (CI) calculation. PACS 31.15.Dv; 36.40.Gk; 73.20.-f     

Towards spectral pattern of spin polarized sodium clusters: The example of Na

We investigate spin modes in the ground state and the polarized first isomer of the Na₁₂ cluster describing the valence electrons in time-dependent local-spin-density approximation (TDLSDA) and the detailed ionic background using local pseudopotentials. The spin modes show a collective redshift compared to the unperturbed particle-hole excitations. They are strongly fragmented and the average energy of the modes along the principal axes are related to the underlying geometry (triaxial or axially symmetric). For the polarized isomer, we find significant cross talk between the spin modes and the dipole plasmon, which hints at a possible spectroscopic identification. Received: 22 June 1998 / Accepted: 29 July 1998     

Resonance and composition effects on the Raman scattering from silver-gold alloy clusters

Low-frequency Raman scattering experiments have been performed on thin films consisting of pure gold or gold-silver alloy clusters embedded in alumina matrix. It is clearly shown that the quadrupolar vibrational modes are observed by Raman scattering because of the effect of resonance with the excitation of the electronic surface dipolar plasmon. This is due to the strong coupling between the collective electronic dipolar excitation and the quadrupolar vibrational modes. This effect of resonance does not exist with the core electron excitations. The mixing of the conduction electron dipolar excitation (surface plasmon) with the core electrons leads to the quenching of the resonant Raman scattering. Received 16 November 2000     

SU(2) gauge theory of the Hubbard model: emergence of an anomalous metallic phase near the Mott critical point

We propose one possible mechanism for an anomalous metallic phase appearing frequently in two spatial dimensions, that is, local pairing fluctuations. Introducing a pair-rotor representation to decompose bare electrons into collective pairing excitations and renormalized electrons, we derive an SU(2) gauge theory of the Hubbard model as an extended version of its U(1) gauge theory. Since our effective SU(2) gauge theory admits two kinds of collective bosons corresponding to pair excitations and density fluctuations, respectively, an intermediate phase appears naturally between the spin liquid Mott insulator and Fermi liquid metal of the U(1) gauge theory, characterized by softening of density-fluctuation modes as the Fermi liquid, but gapping of pair-excitation modes. We show that this intermediate phase is identified with an anomalous metallic phase because there are no electronlike quasiparticles although it is metallic.     

Electron localization and the non-metal-metal transition in alkali-alkali-halide solutions

Summary We evaluate and extend an earlier proposal for a microscopic theory of the non-metal-to-metal (NM-M) transition which occurs on dissolving an alkali metal in it molten halide. The transition is viewed as involving a balance between the free-energy gain from the binding of valence electrons into localization centres and the excess free energy of the ionic assembly screened by the electrons. Using parameters estimated for solutions of potassium in potassium chloride and assuming that the elementary process of electronic trapping is the formation ofF-centre-like clusters, Thomas-Fermi screening by metallic electrons is shown to lead to a very sharp NM-M transition at a concentration in the range of 25–30% added metal. Thermally activated hopping of the localized electrons and the evolution of the localization centres with composition are next crudely taken into account by allowing for an additional contribution to the inverse screening length, which is estimated from the electronic localization length. This is shown to lead to a progressive break-up of the localization clusters, accelerating into a NM-M transition in the same concentration range. This simplified theoretical scenario is consistent with the available experimental evidence.     

Anomalous multiphoton photoelectric effect in ultrashort time scales

In a multiphoton photoelectric process, an electron needs to absorb a given number of photons to escape the surface of a metal. It is shown for the first time that this number is not a constant depending only on the characteristics of the metal and light, but varies with the interaction duration in ultrashort time scales. The phenomenon occurs when electromagnetic energy is transferred, via ultrafast excitation of electron collective modes, to conduction electrons in a duration less than the electron energy damping time. It manifests itself through a dramatic increase of electron production.     

Ionization potentials in alkali-metal clusters

The ionization potentials in alkali metal clusters are calculated using a jellium-background model for positive-ion cores and the local-spin-density functional approximation for valence electrons. The computed results compare reasonably with previous experimental and theoretical values in the cases of Li, Na, K and Cs.     

Theory of oxidation/reduction-induced valence transformations of metal ion dopants in oxide crystals mediated by oxide-vacancy diffusion: I. Thermodynamic analysis

We consider theoretically valence transformations of doping metal ions in oxide crystals induced by oxidation and reduction obtained by changes in the ambient oxygen partial pressure. Three types of oxygen vacancies are assumed to mediate transformations: neutral, singly ionized, and doubly ionized. We provide thermodynamic equilibrium analyses, yielding concentration relations among the oxygen vacancy, metal ions, holes and electrons as functions of the ambient oxygen pressure. The results suggest that experimental study of different species concentrations at thermodynamic equilibrium as functions of pressure and temperature should allow assessment of various reversible reaction constants controlling the process. In the Part II companion paper, the kinetic (diffusion) characteristics are considered in detail.     

X-ray photoelectron emission from iron metal

XPS-spectra of iron metal with special emphasis on the valence band region are reported. The valence band spectrum is in qualitative agreement with that obtained from UPS measurements with 21 eV photons. A comparison with theoretical density of states curves shows reasonable agreement, if the matrix element modulation, lifetime broadening, the inelastic scattering of electrons, the production of electron hole pairs by the photohole, and the instrumental resolution are taken into account. The production of electron hole pairs by a photohole in the valence band seems to be smaller than by a photohole in a core level. This is not unexpected in view of the delocalized nature of these valence electrons.     

Stability patterns of transition metal doped silver clusters: Dopant- and size-dependent electron delocalization

The stability of cationic silver clusters doped with a 3d transition metal atom (Sc, Ti, V, Cr, Mn, Ni, Cu) is investigated by mass spectrometric analysis of fragments resulting from high fluence irradiation of a cluster beam. The mass spectra show enhanced stabilities that correspond to closed shells of valence electrons. Dopant- and size-dependent delocalization of 4s and 3d electrons is discussed based on spherical shell model considerations. Contrary to doped gold clusters, no evidence was found for the existence of 2D electronic shell closures.     

Collective modes and dynamic structure factor of a two-dimensional electron fluid

The electrons bound to the surface of liquid dielectrics by image forces are described as a two-dimensional, classical, one-component plasma with inverse distance interactions. Exact expressions for the collective modes and the dynamic structure factor are obtained from first principles in the limit of long wavelengths. The differences and analogies with uncharged particle fluids and with the three-dimensional one-component plasma are explicitly displayed. The previously used mean-field approximation is shown not to describe weakly coupled systems and to be inadequate in the long-wavelength region.     

Ionization dynamics of simple metal clusters in intense fields by the Thomas-Fermi-Vlasov method

The time-dependent response of simple metal clusters to femtosecond laser pulses is investigated using the semiclassical theory based on the Vlasov equation. Starting from a Thomas-Fermi ground state the dynamics are calculated by use of the pseudoparticle method. Systems studied here are sodium clusters containing up to 147 atoms. Both, the energy transfer to the cluster, which is largely affected by the plasmon enhanced absorption, and the following release of energy to the ions are examined in detail. During the laser excitation the feedback of the absorption to the development of the plasmon energy is controlled by competing mechanisms: ionization and cluster expansion. Characteristics of the Coulomb explosion are studied as function of photon energy and cluster size, particularly with regard to the dynamical influence of collective excitations of the electrons. We also predict features in the angular distribution of the ions that could be measured to test the calculated dynamics.Received: 9 December 2003, Published online: 16 March 2004PACS: 52.50.Jm Plasma production and heating by laser beams (laser-foil, laser-cluster, etc.) - 36.40.Vz Optical properties of clusters - 36.40.Gk Plasma and collective effects in clusters