Structure and melting of dipole clusters

Two-dimensional microclusters made up of particles repelled by the dipole law and confined by an external quadratic potential are considered. The model describes a number of physical systems, in particular, electrons in semiconductor structures near a metallic electrode, indirect excitons in coupled semiconductor dots etc. Two competing types of particle ordering in clusters have been revealed: formation of a triangular lattice and of a shell structure. Equilibrium configurations of clusters with N=1–40 particles are calculated. Temperature dependences of the structure, potential energy, and mean-square radial and angular displacements are studied. These characteristics are used to investigate cluster melting. Melting occurs in one or two stages, depending on N. Melting of a two-shell microcluster takes place in two stages: at low temperatures—from the frozen phase to a state with rotationally reoriented “crystalline” shells with respect to one another, followed by a transition involving breakdown of radial order. Melting in a cluster made up of a larger number of shells occurs in one stage. This is due to the fact that the potential barrier to intershell rotation is substantially lower than that to particle jumping from one shell to another for small N, and of the same order of magnitude for large N. A method is proposed for predicting the character of melting in shell clusters by comparing the potential barriers for shell rotation and intershell particle jumping. Fiz. Tverd. Tela (St. Petersburg) 40, 1379–1386 (July 1998)     

Structure, melting, and potential barriers in mesoscopic clusters of repulsive particles

This paper discusses two-dimensional mesoscopic clusters of particles that repel according to dipole, Coulomb, and logarithmic laws and are confined by an external parabolic potential. These models describe a number of physical systems, in particular, electrons in semiconductor structures or on a liquid-helium surface allowing for image forces, indirect excitons in coupled semi-conductor dots, and a small number of vortices in an island of a second-order superconductor or in superfluid helium. Two competing forms of ordering are detected in the particles in the mesoscopic clusters-the formation of a triangular lattice or of a shell structure. The temperature dependences of the potential energy, the mean-square radial and angular deviations, the radial and angular distributions of the particles, and the distribution of the particles over the local minima are studied. Melting in mesoscopic clusters occurs in two stages: at lower temperatures, there is orientation melting, from the frozen phase into a phase with rotational reorientation of “crystalline” shells with respect to each other; subsequently, a transition occurs in which the radial order disappears. Melting in dipole macroclusters occurs in a single stage. However, in Coulomb and logarithmic macroclusters, orientation melting occurs only for the outer pairs of shells. Orientation melting is also detected in three-dimensional Coulomb clusters. A connection is established between the character of the melting and the ratio of the energy barriers that describe the breakdown of the orientational and radial structure of a cluster. Zh. éksp. Teor. Fiz. 116, 2012–2037 (December 1999)     

Melting properties of two-dimensional multi-species colloidal systems in a parabolic trap

The angular and radial melting properties of two-dimensional classical systems consisting of different types of particles confined in a parabolic trap are studied through modified Monte Carlo simulations. A universal behavior of the angular melting process is found, which occurs in multiple steps due to shell depended melting temperatures. The melting sequence of the different shells is determined by two major factors: (1) the confinement strength which each shell is subjected to, and (2) the specific structure of each shell. Further, a continuous radial disordering of the particle types forming a single circular shell is found and analyzed. This phenomenon has never been observed before in two-dimensional mono-dispersive systems. This continuous radial disordering results from the high energy barrier between different particle types in multi-species systems.     

Coulomb clusters: melting and potential barriers

The melting of two-dimensional and three-dimensional Coulomb micro- and macroclusters is studied. Temperature dependences of radial and angular square deviations of particles are investigated. The melting of microclusters has two stages: at lower temperature there is a transition from a frozen phase to a state with a rotatory reorientation of “crystalline” shells relative to each other, different pairs of shells melting at different temperatures. In the case of large N and high triangular symmetry inside the cluster, orientational melting takes place only for external pairs of shells. In this case external shells lose their order. At higher temperature a transition with a loss of radial shell order occurs. The origin of two-stage melting is in the smallness of the barrier energy relative to the rotation of shells in comparison with the barrier corresponding to the radial disordering of shells. It is shown also that the temperatures of orientational and total melting are at 5–15 times lower than the temperatures of disappearance of corresponding potential barriers. The influence of confinement anisotropy on the character of cluster melting is considered. It is found that at some degree of anisotropy the melting becomes one stage. The last is connected with an increase of the ratios of barriers of intershell rotation to barriers of jumps of a particle between the shells.     

Two-dimensional Abrikosov-vortex microclusters: Shell structure and melting

Melting of two-dimensional Abrikosov-vortex microclusters in a type-II superconductor island with thickness less than the coherence length has been studied. Equilibrium configurations corresponding to local and global minima of potential energy for clusters with N=1–50 particles are calculated. The temperature dependences of the structure and of mean-square radial and angular vortex displacements are investigated. It is shown that vortex microclusters melt in two stages: first the frozen-out phase transfers to a state corresponding to rotational reorientation of crystalline shells with respect to one another, followed by a transition to a state with no radial order at a substantially higher temperature. The reason for this is that the barrier to shell rotation is significantly lower than that to radial breakdown of shells. Fiz. Tverd. Tela (St. Petersburg) 39, 1005–1010 (June 1997)     

Two-dimensional mesoscopic vortex clusters in a superconducting ring: Shell structure and melting

The structure and phase transitions in the mesoscopic system of vortices in a quasi-two-dimensional superconducting ring are investigated. The shell structure of the mesoscopic system of vortices is studied, and its variation with the number of vortices and the parameters of the superconducting ring is analyzed. Two mechanisms of formation of new shells in vortex clusters with an increasing number of vortices in an increasing magnetic field are discovered: the generation of a new shell in a cluster and the splitting of the internal shell into two shells. The melting of vortex clusters and their thermodynamic parameters are analyzed using the Monte Carlo method. It is found that the melting of shell-type clusters occurs in two stages, orientation melting taking place at the lower temperature (during which nearly crystalline adjacent shells start rotating relative to each other) and blurring of the vortex structure occurring at the higher temperature. The shells obtained by splitting upon an increase in the number of vortices do not participate in orientational melting. The two-stage form of melting is associated with the smaller height of potential barriers being surmounted during the rotation of shells relative to one another as compared to the barrier for vortices jumping from one shell to another.     

Mesoscopic and macroscopic dipole clusters: Structure and phase transitions

A two dimensional (2D) classical system of dipole particles confined by a quadratic potential is studied. This system can be used as a model for rare electrons in semiconductor structures near a metal electrode, indirect excitons in coupled quantum dots etc. For clusters of N ≤ 80 particles ground state configurations and appropriate eigenfrequencies and eigenvectors for the normal modes are found. Monte-Carlo and molecular dynamic methods are used to study the order-disorder transition (the “melting” of clusters). In mesoscopic clusters (N < 37) there is a hierarchy of transitions: at lower temperatures an intershell orientational disordering of pairs of shells takes place; at higher temperatures the intershell diffusion sets in and the shell structure disappears. In “macroscopic” clusters (N > 37) an orientational “melting” of only the outer shell is possible. The most stable clusters (having both maximal lowest nonzero eigenfrequencies and maximal temperatures of total melting) are those of completed crystal shells which are concentric groups of nodes of 2D hexagonal lattice with a number of nodes placed in the center of them. The picture of disordering in clusters is compared with that in an infinite 2D dipole system. The study of the radial diffusion constant, the structure factor, the local minima distribution and other quantities shows that the melting temperature is a nonmonotonic function of the number of particles in the system. The dynamical equilibrium between “solid-like” and “orientationally disordered” forms of clusters is considered.     

Characteristic features of the melting of two-dimensional mesoscopic Wigner clusters

Two-dimensional Wigner microclusters in a semiconductor dot are studied. Their melting is investigated in detail and it is shown that, for typical mesoscopic clusters possessing a shell structure, melting occurs in two stages: orientational melting (rotation of the shells relative to one another) and total melting, where the shells start to overlap with one another and exchange particles. An example of a “magic” microstructure which has a triangular structure and melts in a single stage is presented. For this, the temperature dependences of various quantities characterizing cluster structure are investigated. The change in the distribution of cluster configurations over local minima of the potential energy with increasing temperature is investigated. At temperatures below the temperature of total melting, a cluster is always located near the configuration of a global minimum and, at temperatures above the temperature of complete melting, a cluster can be located with finite probability near configurations corresponding to various local minima of the potential energy. Fiz. Tverd. Tela (St. Petersburg) 41, 1499–1504 (August 1999)     

Two-dimensional microclusters of vortices: Shell structure and melting

The melting of two-dimensional microclusters of “particles” which repel one another according to a logarithmic law and are confined by an external quadratic potential is investigated. The model describes Abrikosov vortices in a superconducting island of vortices in a rotating superfluid liquid and electrons in a semiconductor nanostructure surrounded by a low-permittivity medium. The structure of clusters and its dependence on temperature and melting are investigated. The melting of microclusters of vortices proceeds in two stages: 1. A transition from a frozen phase into a state corresponding to rotational reorientation of crystal shells relative to one another. 2. At a higher temperature, the radial order vanishes. This is connected with the fact that the barrier for rotation of the shells is much lower than the barrier for radial breakup of the shells. Pis’ma Zh. éksp. Teor. Fiz. 65, No. 3, 268–273 (10 February 1997)     

Structures of energy spectrum and persistent currents in mesoscopic rings with radial potential barrier in magnetic field

The energy spectrum and the persistent currents are calculated for finite-width mesoscopic annular structures with radial potential barrier in the presence of a magnetic field. The introduction of the tunneling barrier leads to the creation of extra edge states around the barrier and the occurrence of oscillatory structures superimposed on the bulk Landau level plateaus in the energy spectrum. We found that the Fermi energy E _F increases with the number of electrons N emerging many kinks. The single eigenstate persistent current exhibits complicated structures with vortex-like texture, “bifurcation”, and multiple “furcation” patterns as N is increased. The total currents versus N display wild fluctuations.     

Spectres Auger sous bombardement d'ions Ar+ de 60 keV de quelques éléments purs et de composés binaires

Auger spectra of different elements, alloys and compounds excited by 60 keV argon ions have been obtained. These spectra show a detailed structure with, in particular, a sharp Auger peak. This peak is interpreted as a superposition of two kinds of Auger transitions: the first one occurs with two electrons of the electronic band, the second, takes place from electrons situated on “quasi-atomic” outer shells. On the low energy side of Auger line, two equidistant peaks attributed to Auger electrons having suffered energy losses by ionization of electronic outer shell of target-atoms were observed. From Mg, Al, Si, P and S Auger transitions due to initial double L_ii,iii level ionization were detected. The interpretation of the creation of a vacancy in electronic inner shell at the origin of Auger effect by ionic bombardment is given from the electronic promotion model of Fano and Lichten.     

Molecular dynamics study of orientational melting and thermodynamic properties of C<Subscript>60</Subscript>@C<Subscript>240</Subscript> nanoparticles

The barriers to relative shell rotation and other energy characteristics of C₆₀@C₂₄₀ two-shell carbon nanoparticles (“onions”) with outer shells of different shapes are calculated. The disturbance of the orientational order in the mutual arrangement of shells with an increase in temperature (orientational melting) is studied by the molecular dynamics method. The intershell orientational diffusion is represented by the Arrhenius relationship, and the Arrhenius parameters are calculated numerically. A definition is proposed for the temperature of short-range order disturbance in systems that undergo melting without structural change. The calculated temperature of orientational melting of the C₆₀@C₂₄₀ nanoparticle is approximately equal to 60 K.     

The direct exchange interaction for weakly delocalized multielectron systems in crystals

The multielectron theory of exchange interactions taking into account both electrostatic interactions between electrons (“potential” exchange) and electron transfer between magnetic centers (“kinetic” exchange) has been developed on the basis of Bogolubov's procedure using double irreducible operators. The final hamiltonian contains a number of isotropic and anisotropic terms. The exchange interaction parameter variations with the distance have been calculated. The terms determining the dependence on the occupancy of magnetic shells are shown to be of the same order of magnitude as the “potential” exchange and two orders of magnitude less than the “kinetic” exchange. It is shown that in the model adopted the mechanisms of direct exchange interactions always favour the antiferromagnetic spin ordering     

Melting behavior of large disordered sodium clusters

The melting-like transition in disordered sodium clusters Na₉₂ and Na₁₄₂ is studied by performing density functional constant-energy molecular dynamics simulations. The orbital-free version of the density functional formalism is used. In Na₁₄₂ the atoms are distributed in two distinct shells (surface and inner shells) and this cluster melts in two steps: the first one, at ≈130 K, is characterized by the development of a high intrashell atomic mobility, and the second, homogeneous melting at ≈270 K, involves diffusive motion of all the atoms across the whole cluster volume. On the contrary, the melting of Na₉₂ proceeds smoothly over a very broad temperature interval, without any abrupt change in the thermal or structural indicators. The occurrence of two steps in the melting transition is suggested to be related to the existence of a grouping of the atoms in radial shells, even if those shells present a large degree of internal disorder. It then appears that a cluster can be considered fully amorphous (totally disordered) only when there are no radial regions of low atomic density separating shells. The isomer of Na₉₂ studied here fulfills this criterion and its thermal behavior can be considered as representative of that expected for fully amorphous clusters. Disordered Na₁₄₂, on the other hand, that has a discernible structure of an inner and a surface shell, should be considered as not fully disordered. The thermal behavior of these two clusters is also compared to that of icosahedral (totally ordered) sodium clusters of the same sizes. Received 5 February 2001 and Received in final form 21 May 2001     

Cohesive energy of small metallic particles

The cohesive energy of sodium microparticles is calculated using the density functional formalism. The model particles are formed by a central atom surrounded by successive coordination shells of first neighbours, second neighbours, etc. Maxima in the cohesive energy per atom are obtained for particles with filled coordination shells. The sublimation energy is also studied. Insight is gained on the nature of “magic numbers” observed in the experimental size distribution.     

Calculation of the equation of state of a dense hydrogen plasma by the Feynman path integral method

A method is developed for calculating the equation of state of a system of quantum particles at a finite temperature, based on the Feynman formulation of quantum statistics. A general analytical expression is found for the virial estimator for the kinetic energy of a system with rigid boundaries at a finite pressure. An effective method is developed for eliminating the unphysical singularity in the electrostatic potential between a discretized Feynman path of an electron and a proton. It is shown that the “refinement” of an expansion of a quantum-mechanical propagator by addition of high powers of time exacerbates, rather than eliminates, the divergence of a Feynman path integral. A brief summary of the current status of the problem is presented. The proposed new approaches are presented in relation to progress made in this field. Path integral Monte Carlo simulations are performed for nonideal hydrogen plasmas in which both indistinguishability and spin of electrons are taken into account under conditions preceding the formation of the electron shells of atoms. The electron permutation symmetry is represented in terms of Young operators. It is shown that, owing to the singularity of the Coulomb potential, quantum effects on the behavior of the electron component cannot be reduced to small corrections even if the system must be treated as a classical system according to the formal de Broglie criterion. Quantum-mechanical delocalization of electrons substantially weakens the repulsion between electrons as compared to protons. In relatively cold plasmas, many-body correlations lead to complex behavior of the potential of the average force between particles and give rise to repulsive forces acting between protons and electrons at distances of about 5 angstroms. Plasma pressure drops with decreasing plasma temperature as the electron shells of atoms begin to form, and the electron kinetic energy reaches a minimum at a temperature of about 31000 K. The minimum point weakly depends on plasma density. Owing to quantum effects, the electron component is “heated” well before electrons are completely bound in the field of protons.     

Mechanisms for second harmonic generation in the interaction of a superintense ultrashort laser pulse with cluster plasma

The effects of the interaction of an intense femtosecond laser pulse with large atomic clusters are considered. The pulse intensity is of the order of 10¹⁸ W cm^?2. New effects appear when the magnetic component of the Lorentz force is taken into account. The second harmonic of laser radiation is generated. The second harmonic generation (SHG) efficiency is proportional to the square of the number of atoms in a cluster and the square of the laser radiation intensity. The resonance increase in the SHG efficiency at the Mie frequencies (both at the second harmonic frequency and fundamental frequency) proved to be insignificant because of the fast passage through the resonance during cluster expansion. The mechanisms of the expansion and accumulation of energy by electrons and ions in the cluster are discussed in detail. The energy accumulation by electrons mainly occurs due to stimulated inverse bremsstrahlung upon elastic reflection of the electrons from the cluster surface. The equations describing the cluster expansion take into account both the hydrodynamic pressure of heated electrons and the Coulomb explosion of the ionized cluster caused by outer shell ionization. It is assumed that both inner shell and outer shell ionization is described by the over barrier mechanism. It is shown that atomic clusters are more attractive for the generation of even harmonics than compared to solid and gas targets.     

Control of electron correlations in a spherical quantum dot

Spherical quantum dots containing several electrons are considered for different values of the total spin. Numerical calculations are carried out using the quantum path-integral Monte Carlo method. The dependence of the electron correlations on the dimensionless control quantum parameter q associated with the steepness of the confinement potential is studied. The quantum transition from a Wigner crystal-like state (i.e., from the regime of strongly correlated electrons) to a Fermi-liquid state (“cold” melting) driven by the parameter q is studied in detail. The behavior of the radial and pair correlation functions, which characterize quantum delocalization of the electrons, is considered.