Molecular dynamics simulation of dielectric constant and cluster structure of liquid methanol: the role of cluster–cluster dipole correlations

A molecular dynamics simulation of liquid methanol at ambient conditions with two different three-site potential models was performed and the evaluated dielectric constant was discussed in the light of the cluster structure of the liquid. The distribution of the pair interaction energy of molecules and the cluster size distribution were calculated. An aggregation contribution to dielectric constant was defined and calculated as a function of the threshold H-bond energy using energetic criterion of H-bond. The structural information on dipole–dipole correlations of molecules incorporated in the size and structure distribution of aggregates proved to cover about 80% of the calculated dielectric constant of methanol. The other 20% should be attributed to the cluster–cluster dipole correlations.     

Generation of multiple-particle cluster state via cavity QED

This paper proposes schemes for generating multiple-photon and multiple-atom cluster states, respectively. The schemes are based on the cavity input-output process and atomic or photonic states measurement, and the successful probabilities approach unity in the ideal case. The numerical simulations show that the produced multiple-particle cluster states have high fidelity even if the Lamb-Dicke condition is not satisfied. Some practical imperfections, such as atomic spontaneous emission and output coupling inefficiency, only decrease the success probability but exert no influence on the fidelity of generated multiple-particle cluster states. From the experimental point of view, smaller operation number and lack of need for individual addressing keeps the schemes easy to implement. These schemes may offer a promising approach to the generation of a large-scale cluster state.     

Dynamics of aggregation－annihilation process with cluster removals

We have studied the kinetic behaviours of irreversible aggregation－annihilation models with cluster removals. In the models, an irreversible aggregation reaction occurs between any two clusters of the same species and an irreversible annihilation reaction occurs simultaneously between two different species; meanwhile, the clusters of large size are gradually removed from the system. In a mean-field limit, we obtain the general solutions of the cluster-mass distributions for the cases with an arbitrary removal probability. We found that the cluster-mass distribution of either species satisfies a generalized or modified scaling form. The results also indicate that the evolution behaviours of the systems depend strongly on the details of the reaction events.     

Post-deposition dynamics of multiple cluster aggregation on liquid surfaces

A comprehensive simulation model---deposition, diffusion, rotation and aggregation---is presented to demonstrate the post-deposition phenomena of multiple cluster growth on liquid surfaces, such as post-deposition nucleation, post-deposition growth and post-deposition coalescence. Emphasis is placed on the relaxations of monomer density, dimer density and cluster density as well as combined cluster-plus-monomer density with time after deposition ending. It is shown that post-deposition coalescence largely takes place after deposition due to the large mobility of clusters on liquid surfaces, while the post-deposition nucleation is only possible before the saturation cluster density is reached at the end of the deposition. The deposition flux and the moment of deposition ending play important roles in the post-deposition dynamics.     

Local structure changes of Cu55 cluster during heating

The structural relaxation of a cluster containing 55 atoms at elevated temperatures is simulated by molecular dynamics. The interatomic interactions are given by using the embedded atom method （EAM） potential. By decomposing the peaks of the radial distribution functions （RDFs） according to the pair analysis technique, the local structural patterns are identified for this cluster. During increasing temperature, structural changes of different shells determined by atom density profiles result in an abrupt increase in internal energy. The simulations show how local structural changes can strongly cause internal energy to change accordingly.     

Relativistic coupled cluster calculation of Mössbauer isomer shifts of iodine compounds

ABSTRACT

Mössbauer isomer shifts of ¹²⁹I and ¹²⁷I in the ICl, IBr and I₂ molecules are studied. Filatov's formulation is used, based on calculating the electronic energy change of the two systems involved in the Mössbauer γ transition, the source and absorber. The energy difference between the transitions in the two systems determines the shift. The effects of relativity and electron correlation on the shifts are investigated. The exact two-component (X2C) and the four-component relativistic schemes give virtually identical results; the non-relativistic approach yields about 50% of the relativistic shifts. Electron correlation is included by coupled-cluster singles-and-doubles with perturbative triples [CCSD(T)]; it reduces Hartree–Fock shifts by 15%–20%. Basis sets are increased until the isomer shifts converge. The final results, calculated with the converged basis in the framework of the X2C Hamiltonian and CCSD(T) correlation, give an agreement of 10% or better with experimental data.     

Robust H_∞ cluster synchronization analysis of Lurie dynamical networks

The cluster synchronization problem of complex dynamical networks with each node being a Lurie system with exter- nal disturbances and time-varying delay is investigated in this paper. Some criteria for cluster synchronization with desired H∞ performance are presented by using a local linear control scheme. Firstly, sufficient conditions are established to realize cluster synchronization of the Lurie dynamical networks without time delay. Then, the notion of the cluster synchronized region is introduced, and some conditions guaranteeing the cluster synchronized region and unbounded cluster synchro- nized region are derived. Furthermore, the cluster synchronization and cluster synchronized region in the Lurie dynamical networks with time-varying delay are considered. Numerical examples are finally provided to verify and illustrate the theoretical results.     

Effects of charge on the structures and spin moments of Nil3 cluster

The structural stability and magnetic properties of the icosahedral Ni13, Ni13^＋1 and Ni13^-1 clusters have been obtained by utilizing all-electron density functional theory with the generalized gradient approximations for the exchange-correlation energy. The calculated results show that the ground states of neutral and charged clusters all favour a D3d structure, a distorted icosahedron, due to the Jahn-Teller effect. The radial distortions caused by doping one electron and by doping one hole are opposite to each other. Doping one electron will result in a 1/2 decrease and doping one hole will result in a 1/2 increase of the total spin. Both increasing interatomic spacing and decreasing coordination will lead to an enhancement of the spin magnetic moments for Nil3 clusters.     

DFT study on the structure and spectra of GasP5 cluster

In this paper, possible structures of GasP5 cluster were optimized by using density functional method with generalized gradient correction （B3LYP）. The electronic structure of the isomers with lower energy was studied. The most stable structure obtained for GasP5 is a distorted pentaprism. The Ga-P bond formed in the cluster is strongly ionic. Based on NBO analysis, an average value of 0.59 electron transfers from Gallium to Phosphorus. The bond length 2.33-2.43 is around the value in bulk GaP. The HOMO-LUMO gap is about 2.2 eV. The dipole moment and polarizability are calculated, and the IR and Raman spectra are also presented.     

Thermodynamics of a 1—d fermion system by cluster expansions

The thermodynamics of a 1—d fermion system can be perfectly mapped onto the thermodynamics of a two-component classical real gas on the surface of a cylinder. The latter system is studied by a modified Mayer cluster expansion method (Debye-Hückel theory and corrections to it). Simple reinterpretation of thermodynamic variables then leads to an exponentially activated behavior of the fermions' specific heat (spin density contribution). The exponent in Luther's recent gap formula is obtained as well as Zittartz's structure of the ground state energy. The method is applied to the case of strongly attractive spin-non-flip coupling (–1< <–3/5) when the spin-flip coupling is small. For large there is a gap everywhere.Abbreviated version of the author'sHabilitationsschrift     

Cluster–cluster fusion

An experimental study of molecular fusion in fullerene–fullerene collisions is presented and the theoretical interpretation of the cross section is reconsidered in terms of phase space arguments and competition with direct collision induced dissociation. The form and absolute magnitude of the cross sections for C⁺₆₀+C₇₀ (or C⁺₇₀+C₆₀) and C⁺₇₀+C₇₀ can be understood, however, the much smaller cross section for C⁺₆₀+C₆₀ remains a puzzle. The fragmentation behaviour of the hot fusion product is well described by a maximal entropy model indicating equipartition of the centre of mass collision energy followed by statistical fragmentation. To cite this article: E.E.B. Campbell et al., C. R. Physique 3 (2002) 341–352.     

Pervasiveness of cluster excitations as seen in the Mössbauer spectra of magnetic materials

Magnetic cluster excitations in various physical systems (e.g., soliton bearing one-dimensional solids, metallic alloys, amorphous materials, small particle aggregates, magnetically ordered substances near T_C, transition metal di-chloride graphite intercalation compounds, etc.) are described. Use of Fe-57 Mössbauer effect spectroscopy as a probe of the spin dynamics for inverse autocorrelation times between 10⁷Hz to 10¹⁰ Hz is emphasized. Particular attention is given to systems which exhibit local or long range magnetic order and whose Mössbauer spectra must therefore be described by more than one autocorrelation (or dwell) time for fluctuations between different allowed hyperfine field directions on a given site.     

Role of the chemical ordering on the magnetic properties of Fe–Ni cluster alloys

The spin and orbital moments of fcc Fe-Ni cluster alloys are determined within the framework of a d-band Hamiltonian including the spin-orbit coupling non perturbatively. Different sizes (up to 321 atoms), compositions, and chemical configurations (random alloys as well as core-shell arrays of iron and nickel atoms) are considered in order to reveal the crucial role played by local order and stoichiometry on the magnetic moments of the clusters. Interestingly, we have found considerably reduced average magnetizations for Fe-Ni clusters with Fe cores compared to that of the bulk alloy with the same composition. Indeed, in these configurations not only antiparallel arrangements between the local moments of some Fe atoms within the iron core are found, but also the total magnetization of the surface Ni atoms is significantly quenched. On the opposite, the disordered and Ni-core cluster alloys are characterized by high magnetizations resulting from saturated-like contributions from both Ni and Fe atoms, in agreement with recent ab-initio calculations. In general, the local orbital magnetic moments are strongly enhanced with respect to their bulk values. Finally, the variation of the orbital-to-spin moment ratio with the chemical order is discussed.     

“Magic numbers” in the melting of a cluster of point charges on a sphere

The thermodynamic properties of a cluster of point Coulomb charges on a sphere have been analyzed using the Monte Carlo method for the number of charges 20 ≤ N ≤ 90. The ground state of the system of charges is described in the model of a closed quasi-two-dimensional triangular lattice with topological defects. We have determined the dependence of the Lindeman parameter δ_L of this system on N and on the dimensionless parameter $ \tilde T $ \tilde T , which is proportional to the temperature T and to the radius R of the cluster: $ \tilde T = {{k_B T\varepsilon R} \mathord{\left/ {\vphantom {{k_B T\varepsilon R} {e^2 }}} \right. \kern-\nulldelimiterspace} {e^2 }} $ \tilde T = {{k_B T\varepsilon R} \mathord{\left/ {\vphantom {{k_B T\varepsilon R} {e^2 }}} \right. \kern-\nulldelimiterspace} {e^2 }} , where ∈ is the dielectric constant of the medium and e is the charge of a particle. The “magic numbers,” i.e., the N values, for which the melting point of the closed triangular lattice of charges is much higher than those for neighboring N values, have been found. The evolution of the lattice-melting mechanisms with an increase in the number of charges N in a mesoscopic cluster has been analyzed. For N ≤ 32, the melting of the lattice does not involve dislocations (nontopological melting); this behavior of the mesoscopic system of charges on the sphere differs from the behavior of the extended planar two-dimensional system. At N ≳ 50, melting is accompanied by the formation of dislocations. The mechanism of dislocation-free non-topological melting of a closed lattice, which occurs at small N values and is associated with the cooperative rotational motion of “rings” of particles, has been analyzed. The model has various implementations in the mesoscopic region; in particular, it describes the system of electrons over the liquid-helium cluster, the liquid-helium cluster with incorporated charged particles, a multielectron bubble in liquid helium, a charged quantum dot, etc.     

Effects of vibrational averaging on coupled cluster calculations of spin–spin coupling constants for hydrocarbons

We present vibrationally corrected nuclear spin–spin coupling constants for four hydrocarbons with different types of carbon–carbon bonds calculated with coupled cluster (CC) theory. First, we perform a systematic basis set investigation on acetylene for all of the four contributions (Fermi-contact, spin-dipole, para- and diamagnetic spin–orbit) to the spin–spin coupling constants and subsequently choose basis sets of sufficient flexibility to describe converged electronic properties. Then, in order to describe the effects of vibrational motion for the studied molecules we perform a Taylor expansion in the normal coordinates up to second order – a method that is well known for both its quality and efficiency – and rigorously estimate the resulting contribution for all types of spin–spin coupling constants. Combined, this allows us to obtain highly accurate benchmark estimates of the spin–spin coupling constants for acetylene, ethylene, ethane, and cyclopropane. This work provides one of the first systematic benchmarks of zero-point vibrational contributions to spin–spin coupling constants in poly-atomic molecules using the reliable CC theory and it is thus an important reference for further research within in-silico spin–spin coupling constant determination. We note that earlier computational estimates of zero-point vibrational effects agree well with those presented here (for acetylene, ethylene, and cyclopropane) while vibrational corrections for ethane are reported for the first time.     

Photon-trap spectroscopy of size-selected free cluster ions: “direct” measurement of optical absorption of Ag+ 9

An absorption spectrum of size-selected free cluster ions has been measured “directly” via extinction of light without relying on photodepletion/dissociation spectroscopy. The novel technique employs an ion trap and an optical cavity; cluster ions stored in an ion trap interact with photons trapped in a cavity. The storage lifetime of photons in the cavity provides “direct” observation of extinction of light (photon-trap spectroscopy, which is a generalized scheme of cavity ring-down spectroscopy). The first measurement is performed on ultraviolet absorption of Ag₉ ⁺. Temperature dependence of the spectrum is presented by cooling the ion trap down to 10 K.     

Efficient scheme of quantum SWAP gate and multi-atom cluster state via cavity QED

In this paper, we propose a physical scheme to realize quantum SWAP gate by using a large-detuned single-mode cavity field and two identical Rydberg atoms. It is shown that the scheme can also be used to create multi-atom cluster state. During the interaction between atom and cavity, the cavity is only virtually excited and thus the scheme is insensitive to the cavity field states and cavity decay. With the help of our scheme it is very simple to prepare the N-atom cluster state with perfect fidelity and probability. The practical feasibility of this method is also discussed.